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Chem. Theory Comput.}\ }\textbf {\bibinfo {volume} {10}},\ - \bibinfo {pages} {4795} (\bibinfo {year} {2014})}\BibitemShut {NoStop}% -\bibitem [{\citenamefont {Burton}\ \emph - {et~al.}(2019{\natexlab{b}})\citenamefont {Burton}, \citenamefont {Thom},\ - and\ \citenamefont {Loos}}]{Burton_2019a}% - \BibitemOpen - \bibfield {author} {\bibinfo {author} {\bibfnamefont {H.~G.~A.}\ - \bibnamefont {Burton}}, \bibinfo {author} {\bibfnamefont {A.~J.~W.}\ - \bibnamefont {Thom}}, \ and\ \bibinfo {author} {\bibfnamefont {P.-F.}\ - \bibnamefont {Loos}},\ }\href {\doibase 10.1021/acs.jctc.9b00289} {\bibfield - {journal} {\bibinfo {journal} {J. Chem. Theory Comput.}\ }\textbf {\bibinfo - {volume} {15}},\ \bibinfo {pages} {4374} (\bibinfo {year} - {2019}{\natexlab{b}})}\BibitemShut {NoStop}% -\bibitem [{\citenamefont {Slater}(1960)}]{SlaterBook}% - \BibitemOpen - \bibfield {author} {\bibinfo {author} {\bibfnamefont {J.~C.}\ \bibnamefont - {Slater}},\ }\href@noop {} {\emph {\bibinfo {title} {{Quantum Theory of - Atomic Structure}}}}\ (\bibinfo {publisher} {McGraw-Hill},\ \bibinfo {year} - {1960})\BibitemShut {NoStop}% \end{thebibliography}% diff --git a/Manuscript/EPAWTFT.bib b/Manuscript/EPAWTFT.bib index 164073e..f9cbd97 100644 --- a/Manuscript/EPAWTFT.bib +++ b/Manuscript/EPAWTFT.bib @@ -1,948 +1,1056 @@ %% This BibTeX bibliography file was created using BibDesk. %% http://bibdesk.sourceforge.net/ -%% Created for Pierre-Francois Loos at 2020-08-22 22:23:12 +0200 +%% Created for Pierre-Francois Loos at 2020-11-12 10:02:40 +0100 %% Saved with string encoding Unicode (UTF-8) +@article{Nesbet_1955, + abstract = { A systematic method is developed for estimating or calculating corrections for configuration interaction in atomic, molecular and nuclear wave-function calculations. Solutions of the Hartree-Fock equations for a single Slater determinant or approximate Hartree-Fock solutions obtained by Roothaan's iterative procedure have special properties which are used to simplify the matrix of the many-particle Hamiltonian. A restricted self-consistent field method is proposed for treating states of low symmetry. This method avoids the off-diagonal Lagrange multipliers encountered in previous methods and is adapted to configuration interaction calculations. }, + author = {Nesbet, R. K. and Hartree, Douglas Rayner}, + date-added = {2020-11-12 10:01:40 +0100}, + date-modified = {2020-11-12 10:02:40 +0100}, + doi = {10.1098/rspa.1955.0134}, + journal = {Proc. R. Soc. Lond. A}, + number = {1182}, + pages = {312-321}, + title = {Configuration interaction in orbital theories}, + volume = {230}, + year = {1955}, + Bdsk-Url-1 = {https://royalsocietypublishing.org/doi/abs/10.1098/rspa.1955.0134}, + Bdsk-Url-2 = {https://doi.org/10.1098/rspa.1955.0134}} + +@article{Epstein_1926, + author = {Epstein, Paul S.}, + date-added = {2020-11-12 10:00:50 +0100}, + date-modified = {2020-11-12 10:01:10 +0100}, + doi = {10.1103/PhysRev.28.695}, + issue = {4}, + journal = {Phys. Rev.}, + month = {Oct}, + numpages = {0}, + pages = {695--710}, + publisher = {American Physical Society}, + title = {The Stark Effect from the Point of View of Schroedinger's Quantum Theory}, + url = {https://link.aps.org/doi/10.1103/PhysRev.28.695}, + volume = {28}, + year = {1926}, + Bdsk-Url-1 = {https://link.aps.org/doi/10.1103/PhysRev.28.695}, + Bdsk-Url-2 = {https://doi.org/10.1103/PhysRev.28.695}} + +@article{Gill_1994, + author = {P. M. W. Gill}, + date-added = {2020-11-12 09:57:40 +0100}, + date-modified = {2020-11-12 09:57:40 +0100}, + doi = {10.1016/S0065-3276(08)60019-2}, + journal = {Adv. Quantum Chem.}, + pages = {141--205}, + title = {Molecular Integrals Over Gaussian Basis Functions}, + volume = {25}, + year = {1994}, + Bdsk-Url-1 = {https://doi.org/10.1016/S0065-3276(08)60019-2}} + +@article{Mihalka_2017b, + author = {Mih{\'a}lka,Zsuzsanna {\'E}. and Szabados,{\'A}gnes and Surj{\'a}n,P{\'e}ter R.}, + date-added = {2020-11-12 09:31:14 +0100}, + date-modified = {2020-11-12 09:33:15 +0100}, + doi = {10.1063/1.4978898}, + journal = {J. Chem. Phys.}, + number = {12}, + pages = {124121}, + title = {Effect of partitioning on the convergence properties of the Rayleigh-Schr{\"o}dinger perturbation series}, + volume = {146}, + year = {2017}, + Bdsk-Url-1 = {https://doi.org/10.1063/1.4978898}} + +@article{Mihalka_2019, + author = {Mih{\'a}lka,Zsuzsanna {\'E}. and Szabados,{\'A}gnes and Surj{\'a}n,P{\'e}ter R.}, + date-added = {2020-11-12 09:29:42 +0100}, + date-modified = {2020-11-12 09:33:07 +0100}, + doi = {10.1063/1.5083191}, + journal = {J. Chem. Phys.}, + number = {3}, + pages = {031101}, + title = {Application of the Cauchy integral formula as a tool of analytic continuation for the resummation of divergent perturbation series}, + volume = {150}, + year = {2019}, + Bdsk-Url-1 = {https://doi.org/10.1063/1.5083191}} + +@article{Mihalka_2017a, + author = {Mih\'alka, Zsuzsanna \'E. and Surj\'an, P\'eter R.}, + date-added = {2020-11-12 09:28:43 +0100}, + date-modified = {2020-11-12 09:30:45 +0100}, + doi = {10.1103/PhysRevA.96.062106}, + issue = {6}, + journal = {Phys. Rev. A}, + month = {Dec}, + numpages = {5}, + pages = {062106}, + publisher = {American Physical Society}, + title = {Analytic-continuation approach to the resummation of divergent series in Rayleigh-Schr\"odinger perturbation theory}, + url = {https://link.aps.org/doi/10.1103/PhysRevA.96.062106}, + volume = {96}, + year = {2017}, + Bdsk-Url-1 = {https://link.aps.org/doi/10.1103/PhysRevA.96.062106}, + Bdsk-Url-2 = {https://doi.org/10.1103/PhysRevA.96.062106}} + +@article{Berry_2011, + abstract = {For non-Hermitian Hamiltonians with an isolated degeneracy (`exceptional point'), a model for cycling around loops that enclose or exclude the degeneracy is solved exactly in terms of Bessel functions. Floquet solutions, returning exactly to their initial states (up to a constant) are found, as well as exact expressions for the adiabatic multipliers when the evolving states are represented as a superposition of eigenstates of the instantaneous Hamiltonian. Adiabatically (i.e. for slow cycles), the multipliers of exponentially subdominant eigenstates can vary wildly, unlike those driven by Hermitian operators, which change little. These variations are explained as an example of the Stokes phenomenon of asymptotics. Improved (superadiabatic) approximations tame the variations of the multipliers but do not eliminate them.}, + author = {M V Berry and R Uzdin}, + date-added = {2020-11-12 09:14:42 +0100}, + date-modified = {2020-11-12 09:20:26 +0100}, + doi = {10.1088/1751-8113/44/43/435303}, + journal = {J. Phys. A Math. Theor.}, + month = {oct}, + number = {43}, + pages = {435303}, + publisher = {{IOP} Publishing}, + title = {Slow non-Hermitian cycling: exact solutions and the Stokes phenomenon}, + url = {https://doi.org/10.1088%2F1751-8113%2F44%2F43%2F435303}, + volume = {44}, + year = 2011, + Bdsk-Url-1 = {https://doi.org/10.1088%2F1751-8113%2F44%2F43%2F435303}, + Bdsk-Url-2 = {https://doi.org/10.1088/1751-8113/44/43/435303}} + @book{BenderPTBook, - Author = {C. M. Bender}, - Date-Added = {2020-08-22 22:22:25 +0200}, - Date-Modified = {2020-08-22 22:22:25 +0200}, - Publisher = {World Scientific}, - Title = {{{\cal PT}}-Symmetry in Quantum and Classical Physics}, - Year = {2019}} + author = {C. M. Bender}, + date-added = {2020-08-22 22:22:25 +0200}, + date-modified = {2020-08-22 22:22:25 +0200}, + publisher = {World Scientific}, + title = {{{\cal PT}}-Symmetry in Quantum and Classical Physics}, + year = {2019}} @article{Benda_2018, - Author = {Zsuzsanna Benda and Thomas-C. Jagau}, - Date-Added = {2020-08-22 22:03:56 +0200}, - Date-Modified = {2020-08-22 22:04:59 +0200}, - Doi = {10.1021/acs.jpclett.8b03228}, - Journal = {J. Phys. Chem. Lett.}, - Pages = {6978--6984}, - Title = {Locating Exceptional Points on Multidimensional Complex-Valued Potential Energy Surfaces}, - Volume = {9}, - Year = {2018}, + author = {Zsuzsanna Benda and Thomas-C. Jagau}, + date-added = {2020-08-22 22:03:56 +0200}, + date-modified = {2020-08-22 22:04:59 +0200}, + doi = {10.1021/acs.jpclett.8b03228}, + journal = {J. Phys. Chem. Lett.}, + pages = {6978--6984}, + title = {Locating Exceptional Points on Multidimensional Complex-Valued Potential Energy Surfaces}, + volume = {9}, + year = {2018}, Bdsk-Url-1 = {https://doi.org/10.1021/acs.jpclett.8b03228}} @book{BenderBook, - Author = {C. M. Bender and S. A. Orszag}, - Date-Added = {2020-07-28 09:59:40 +0200}, - Date-Modified = {2020-07-28 09:59:40 +0200}, - Publisher = {Springer}, - Title = {Advanced Mathematical Methods for Scientists and Engineers: Asymptotics Methods and Perturbation Theory}, - Year = {1978}} + author = {C. M. Bender and S. A. Orszag}, + date-added = {2020-07-28 09:59:40 +0200}, + date-modified = {2020-07-28 09:59:40 +0200}, + publisher = {Springer}, + title = {Advanced Mathematical Methods for Scientists and Engineers: Asymptotics Methods and Perturbation Theory}, + year = {1978}} @article{Gill_1986, - Author = {Gill, Peter M. W. and Radom, Leo}, - Date = {1986-11-28}, - Date-Modified = {2020-08-22 22:12:45 +0200}, - Doi = {10.1016/0009-2614(86)80686-8}, - Journal = {Chem. Phys. Lett.}, - Number = {1}, - Pages = {16--22}, - Title = {Deceptive convergence in {M{\o}ller-Plesset} perturbation energies}, - Volume = {132}, - Year = {1986}, + author = {Gill, Peter M. W. and Radom, Leo}, + date = {1986-11-28}, + date-modified = {2020-08-22 22:12:45 +0200}, + doi = {10.1016/0009-2614(86)80686-8}, + journal = {Chem. Phys. Lett.}, + number = {1}, + pages = {16--22}, + title = {Deceptive convergence in {M{\o}ller-Plesset} perturbation energies}, + volume = {132}, + year = {1986}, Bdsk-Url-1 = {https://doi.org/10.1016/0009-2614(86)80686-8}} @article{Gill_1988, - Author = {Gill, Peter M. W. and Pople, John A. and Radom, Leo and Nobes, Ross H.}, - Date = {1988-12-15}, - Date-Modified = {2020-08-22 22:12:52 +0200}, - Doi = {10.1063/1.455312}, - Journal = {J. Chem. Phys.}, - Number = {12}, - Pages = {7307--7314}, - Title = {Why does unrestricted {M{\o}ller-Plesset} perturbation theory converge so slowly for spin‐contaminated wave functions?}, - Volume = {89}, - Year = {1988}, + author = {Gill, Peter M. W. and Pople, John A. and Radom, Leo and Nobes, Ross H.}, + date = {1988-12-15}, + date-modified = {2020-08-22 22:12:52 +0200}, + doi = {10.1063/1.455312}, + journal = {J. Chem. Phys.}, + number = {12}, + pages = {7307--7314}, + title = {Why does unrestricted {M{\o}ller-Plesset} perturbation theory converge so slowly for spin‐contaminated wave functions?}, + volume = {89}, + year = {1988}, Bdsk-Url-1 = {https://doi.org/10.1063/1.455312}} @article{Sergeev_2005, - Author = {Sergeev, Alexey V. and Goodson, David Z. and Wheeler, Steven E. and Allen, Wesley D.}, - Date-Modified = {2020-08-22 22:13:37 +0200}, - Doi = {10.1063/1.1991854}, - Journal = {J. Chem. Phys.}, - Number = {6}, - Pages = {064105}, - Title = {On the nature of the {M{\o}ller-Plesset} critical point}, - Volume = {123}, - Year = {2005}, + author = {Sergeev, Alexey V. and Goodson, David Z. and Wheeler, Steven E. and Allen, Wesley D.}, + date-modified = {2020-08-22 22:13:37 +0200}, + doi = {10.1063/1.1991854}, + journal = {J. Chem. Phys.}, + number = {6}, + pages = {064105}, + title = {On the nature of the {M{\o}ller-Plesset} critical point}, + volume = {123}, + year = {2005}, Bdsk-Url-1 = {https://doi.org/10.1063/1.1991854}} @article{Sergeev_2006, - Author = {Sergeev, Alexey V. and Goodson, David Z.}, - Date-Modified = {2020-08-22 22:13:42 +0200}, - Doi = {10.1063/1.2173989}, - Journal = {J. Chem. Phys.}, - Number = {9}, - Pages = {094111}, - Title = {Singularities of {M{\o}ller-Plesset} energy functions}, - Volume = {124}, - Year = {2006}, + author = {Sergeev, Alexey V. and Goodson, David Z.}, + date-modified = {2020-08-22 22:13:42 +0200}, + doi = {10.1063/1.2173989}, + journal = {J. Chem. Phys.}, + number = {9}, + pages = {094111}, + title = {Singularities of {M{\o}ller-Plesset} energy functions}, + volume = {124}, + year = {2006}, Bdsk-Url-1 = {https://doi.org/10.1063/1.2173989}} @article{Stillinger_2000, - Author = {Stillinger, Frank H.}, - Date = {2000-05-31}, - Date-Modified = {2020-08-22 22:14:50 +0200}, - Doi = {10.1063/1.481608}, - Journal = {J. Chem. Phys.}, - Number = {22}, - Pages = {9711--9715}, - Title = {{M{\o}ller-Plesset} convergence issues in computational quantum chemistry}, - Volume = {112}, - Year = {2000}, + author = {Stillinger, Frank H.}, + date = {2000-05-31}, + date-modified = {2020-08-22 22:14:50 +0200}, + doi = {10.1063/1.481608}, + journal = {J. Chem. Phys.}, + number = {22}, + pages = {9711--9715}, + title = {{M{\o}ller-Plesset} convergence issues in computational quantum chemistry}, + volume = {112}, + year = {2000}, Bdsk-Url-1 = {https://doi.org/10.1063/1.481608}} @article{Olsen_1996, - Author = {Olsen, Jeppe and Christiansen, Ove and Koch, Henrik and J{\o}rgensen, Poul}, - Date = {1996-09-01}, - Doi = {10.1063/1.472352}, - Journal = {J. Chem. Phys.}, - Pages = {5082--5090}, - Title = {Surprising cases of divergent behavior in {M{\o}ller-Plesset} perturbation theory}, - Volume = {105}, + author = {Olsen, Jeppe and Christiansen, Ove and Koch, Henrik and J{\o}rgensen, Poul}, + date-modified = {2020-11-12 09:19:06 +0100}, + doi = {10.1063/1.472352}, + journal = {J. Chem. Phys.}, + pages = {5082--5090}, + title = {Surprising cases of divergent behavior in {M{\o}ller-Plesset} perturbation theory}, + volume = {105}, + year = {1996}, Bdsk-Url-1 = {https://doi.org/10.1063/1.472352}} @article{Olsen_2000, - Author = {Olsen, Jeppe and J{\o}rgensen, Poul and Helgaker, Trygve and Christiansen, Ove}, - Date = {2000-05-31}, - Doi = {10.1063/1.481611}, - Journal = {J. Chem. Phys.}, - Number = {22}, - Pages = {9736--9748}, - Title = {Divergence in {M{\o}ller-Plesset} theory: {A} simple explanation based on a two-state model}, - Volume = {112}, + author = {Olsen, Jeppe and J{\o}rgensen, Poul and Helgaker, Trygve and Christiansen, Ove}, + date-modified = {2020-11-12 09:19:09 +0100}, + doi = {10.1063/1.481611}, + journal = {J. Chem. Phys.}, + pages = {9736--9748}, + title = {Divergence in {M{\o}ller-Plesset} theory: {A} simple explanation based on a two-state model}, + volume = {112}, + year = {2000}, Bdsk-Url-1 = {https://doi.org/10.1063/1.481611}} @article{Olsen_2019, - Author = {Olsen, Jeppe and J{\o}rgensen, Poul}, - Date-Modified = {2020-08-22 22:21:37 +0200}, - Doi = {10.1063/1.5110554}, - Journal = {J. Chem. Phys.}, - Number = {8}, - Pages = {084108}, - Title = {Convergence patterns and rates in two-state perturbation expansions}, - Volume = {151}, - Year = {2019}, + author = {Olsen, Jeppe and J{\o}rgensen, Poul}, + date-modified = {2020-08-22 22:21:37 +0200}, + doi = {10.1063/1.5110554}, + journal = {J. Chem. Phys.}, + number = {8}, + pages = {084108}, + title = {Convergence patterns and rates in two-state perturbation expansions}, + volume = {151}, + year = {2019}, Bdsk-Url-1 = {https://doi.org/10.1063/1.5110554}} @article{Leininger_2000, - Author = {Leininger, Matthew L. and Allen, Wesley D. and Schaefer, Henry F. and Sherrill, C. David}, - Date = {2000-05-17}, - Doi = {10.1063/1.481764}, - Journal = {J. Chem. Phys.}, - Number = {21}, - Pages = {9213--9222}, - Title = {Is {M{\o}ller-Plesset} perturbation theory a convergent ab initio method?}, - Volume = {112}, + author = {Leininger, Matthew L. and Allen, Wesley D. and Schaefer, Henry F. and Sherrill, C. David}, + date = {2000-05-17}, + doi = {10.1063/1.481764}, + journal = {J. Chem. Phys.}, + number = {21}, + pages = {9213--9222}, + title = {Is {M{\o}ller-Plesset} perturbation theory a convergent ab initio method?}, + volume = {112}, Bdsk-Url-1 = {https://doi.org/10.1063/1.481764}} @article{Moller_1934, - Author = {M{\o}ller, Chr. and Plesset, M. S.}, - Date = {1934-10-01}, - Date-Modified = {2020-08-22 22:12:33 +0200}, - Doi = {10.1103/PhysRev.46.618}, - Journal = {Phys. Rev.}, - Number = {7}, - Pages = {618--622}, - Title = {Note on an {Approximation Treatment for Many-Electron Systems}}, - Volume = {46}, - Year = {1934}, + author = {M{\o}ller, Chr. and Plesset, M. S.}, + date = {1934-10-01}, + date-modified = {2020-08-22 22:12:33 +0200}, + doi = {10.1103/PhysRev.46.618}, + journal = {Phys. Rev.}, + number = {7}, + pages = {618--622}, + title = {Note on an {Approximation Treatment for Many-Electron Systems}}, + volume = {46}, + year = {1934}, Bdsk-Url-1 = {https://doi.org/10.1103/PhysRev.46.618}} @article{Handy_1985, - Author = {Handy, N. C. and Knowles, P. J. and Somasundram, K.}, - Date-Modified = {2020-08-22 22:13:56 +0200}, - Doi = {10.1007/BF00698753}, - Journal = {Theoret. Chim. Acta}, - Number = {1}, - Pages = {87--100}, - Title = {On the convergence of the {M{\o}ller-Plesset} perturbation series}, - Volume = {68}, - Year = {1985}, + author = {Handy, N. C. and Knowles, P. J. and Somasundram, K.}, + date-modified = {2020-08-22 22:13:56 +0200}, + doi = {10.1007/BF00698753}, + journal = {Theoret. Chim. Acta}, + number = {1}, + pages = {87--100}, + title = {On the convergence of the {M{\o}ller-Plesset} perturbation series}, + volume = {68}, + year = {1985}, Bdsk-Url-1 = {https://doi.org/10.1007/BF00698753}} @article{Christiansen_1996, - Author = {Christiansen, Ove and Olsen, Jeppe and J{\o}rgensen, Poul and Koch, Henrik and Malmqvist, Per-{\AA}ke}, - Date = {1996-10-18}, - Date-Modified = {2020-08-22 22:14:27 +0200}, - Doi = {10.1016/0009-2614(96)00974-8}, - Journal = {Chem. Phys. Lett.}, - Number = {3}, - Pages = {369--378}, - Title = {On the inherent divergence in the {M{\o}ller-Plesset} series. {The} neon atom --- a test case}, - Urldate = {2020-07-07}, - Volume = {261}, - Year = {1996}, + author = {Christiansen, Ove and Olsen, Jeppe and J{\o}rgensen, Poul and Koch, Henrik and Malmqvist, Per-{\AA}ke}, + date = {1996-10-18}, + date-modified = {2020-08-22 22:14:27 +0200}, + doi = {10.1016/0009-2614(96)00974-8}, + journal = {Chem. Phys. Lett.}, + number = {3}, + pages = {369--378}, + title = {On the inherent divergence in the {M{\o}ller-Plesset} series. {The} neon atom --- a test case}, + urldate = {2020-07-07}, + volume = {261}, + year = {1996}, Bdsk-Url-1 = {https://doi.org/10.1016/0009-2614(96)00974-8}} @incollection{Goodson_2004, - Author = {Goodson, David Z. and Sergeev, Alexey V.}, - Booktitle = {Adv. 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Commun.}, + month = dec, + number = {1}, + pages = {2182}, + title = {{Observation of an Anti-PT-Symmetric Exceptional Point and Energy-Difference Conserving Dynamics in Electrical Circuit Resonators}}, + volume = {9}, + year = {2018}, Bdsk-Url-1 = {https://doi.org/10.1038/s41467-018-04690-y}} @article{El-Ganainy_2018, - Author = {El-Ganainy, Ramy and Makris, Konstantinos G. and Khajavikhan, Mercedeh and Musslimani, Ziad H. and Rotter, Stefan and Christodoulides, Demetrios N.}, - Date-Added = {2019-01-30 12:10:10 +0100}, - Date-Modified = {2019-01-30 12:10:10 +0100}, - Doi = {10.1038/nphys4323}, - Journal = {Nat. 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Scr.}, + number = {11}, + pages = {114015}, + title = {Excited-state quantum phase transitions in finite many-body systems}, + volume = {90}, + year = {2015}, Bdsk-Url-1 = {https://doi.org/10.1088/0031-8949/90/11/114015}} @article{Cejnar_2009, - Author = {Cejnar, Pavel and Jolie, Jan}, - Date-Modified = {2020-08-22 22:16:10 +0200}, - Doi = {10.1016/j.ppnp.2008.08.001}, - Journal = {Prog. Part. Nucl. Phys.}, - Number = {1}, - Pages = {210--256}, - Title = {Quantum phase transitions in the interacting boson model}, - Volume = {62}, - Year = {2009}, + author = {Cejnar, Pavel and Jolie, Jan}, + date-modified = {2020-08-22 22:16:10 +0200}, + doi = {10.1016/j.ppnp.2008.08.001}, + journal = {Prog. Part. Nucl. 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Phys.}, - Month = jan, - Number = {4}, - Pages = {041103}, - Title = {Complex adiabatic connection: {A} hidden non-{Hermitian} path from ground to excited states}, - Volume = {150}, - Year = {2019}, + author = {Burton, Hugh G. A. and Thom, Alex J. W. and Loos, Pierre-Fran{\c c}ois}, + doi = {10.1063/1.5085121}, + journal = {J. Chem. Phys.}, + month = jan, + number = {4}, + pages = {041103}, + title = {Complex adiabatic connection: {A} hidden non-{Hermitian} path from ground to excited states}, + volume = {150}, + year = {2019}, Bdsk-Url-1 = {https://doi.org/10.1063/1.5085121}} @article{Burton_2019a, - Author = {Burton, Hugh G. A. and Thom, Alex J. W. and Loos, Pierre-Fran{\c c}ois}, - Doi = {10.1021/acs.jctc.9b00289}, - Journal = {J. Chem. Theory Comput.}, - Month = aug, - Number = {8}, - Pages = {4374--4385}, - Title = {Parity-{Time} {Symmetry} in {Hartree}--{Fock} {Theory}}, - Volume = {15}, - Year = {2019}, + author = {Burton, Hugh G. A. and Thom, Alex J. W. and Loos, Pierre-Fran{\c c}ois}, + doi = {10.1021/acs.jctc.9b00289}, + journal = {J. Chem. Theory Comput.}, + month = aug, + number = {8}, + pages = {4374--4385}, + title = {Parity-{Time} {Symmetry} in {Hartree}--{Fock} {Theory}}, + volume = {15}, + year = {2019}, Bdsk-Url-1 = {https://doi.org/10.1021/acs.jctc.9b00289}} @article{Hiscock_2014, - Author = {Hiscock, Hamish G. and Thom, Alex J. W.}, - Doi = {10.1021/ct5007696}, - Journal = {J. Chem. Theory Comput.}, - Month = nov, - Number = {11}, - Pages = {4795--4800}, - Title = {Holomorphic {Hartree}--{Fock} {Theory} and {Configuration} {Interaction}}, - Volume = {10}, - Year = {2014}, + author = {Hiscock, Hamish G. and Thom, Alex J. W.}, + doi = {10.1021/ct5007696}, + journal = {J. Chem. Theory Comput.}, + month = nov, + number = {11}, + pages = {4795--4800}, + title = {Holomorphic {Hartree}--{Fock} {Theory} and {Configuration} {Interaction}}, + volume = {10}, + year = {2014}, Bdsk-Url-1 = {https://doi.org/10.1021/ct5007696}} @article{Seidl_2018, - Author = {Seidl, Michael and Giarrusso, Sara and Vuckovic, Stefan and Fabiano, Eduardo and Gori-Giorgi, Paola}, - Doi = {10.1063/1.5078565}, - Journal = {J. Chem. Phys.}, - Month = dec, - Number = {24}, - Pages = {241101}, - Title = {Communication: {Strong}-interaction limit of an adiabatic connection in {Hartree}-{Fock} theory}, - Volume = {149}, - Year = {2018}, + author = {Seidl, Michael and Giarrusso, Sara and Vuckovic, Stefan and Fabiano, Eduardo and Gori-Giorgi, Paola}, + doi = {10.1063/1.5078565}, + journal = {J. Chem. Phys.}, + month = dec, + number = {24}, + pages = {241101}, + title = {Communication: {Strong}-interaction limit of an adiabatic connection in {Hartree}-{Fock} theory}, + volume = {149}, + year = {2018}, Bdsk-Url-1 = {https://doi.org/10.1063/1.5078565}} @book{GiulianiBook, - Author = {Giuliani, Gabriele and Vignale, Giovanni}, - Doi = {10.1017/CBO9780511619915}, - Isbn = {978-0-521-52796-5}, - Publisher = {Cambridge University Press}, - Title = {Quantum {Theory} of the {Electron} {Liquid}}, - Urldate = {2020-07-21}, - Year = {2005}, + author = {Giuliani, Gabriele and Vignale, Giovanni}, + doi = {10.1017/CBO9780511619915}, + isbn = {978-0-521-52796-5}, + publisher = {Cambridge University Press}, + title = {Quantum {Theory} of the {Electron} {Liquid}}, + urldate = {2020-07-21}, + year = {2005}, Bdsk-Url-1 = {https://doi.org/10.1017/CBO9780511619915}} @book{AngularBook, - Author = {Edmonds, A. R.}, - Isbn = {978-0-691-02589-6}, - Publisher = {Princeton University Press}, - Title = {Angular {Momentum} in {Quantum} {Mechanics}}, - Year = {1996}} + author = {Edmonds, A. R.}, + isbn = {978-0-691-02589-6}, + publisher = {Princeton University Press}, + title = {Angular {Momentum} in {Quantum} {Mechanics}}, + year = {1996}} @book{SlaterBook, - Author = {Slater, John Clarke}, - Publisher = {McGraw-Hill}, - Title = {{Quantum Theory of Atomic Structure}}, - Year = {1960}} + author = {Slater, John Clarke}, + publisher = {McGraw-Hill}, + title = {{Quantum Theory of Atomic Structure}}, + year = {1960}} @article{Loos_2009, - Author = {Loos, Pierre-Fran{\c c}ois and Gill, Peter M. W.}, - Doi = {10.1103/PhysRevA.79.062517}, - Journal = {Phys. Rev. A}, - Month = jun, - Number = {6}, - Pages = {062517}, - Title = {Ground state of two electrons on a sphere}, - Volume = {79}, - Year = {2009}, + author = {Loos, Pierre-Fran{\c c}ois and Gill, Peter M. W.}, + doi = {10.1103/PhysRevA.79.062517}, + journal = {Phys. Rev. A}, + month = jun, + number = {6}, + pages = {062517}, + title = {Ground state of two electrons on a sphere}, + volume = {79}, + year = {2009}, Bdsk-Url-1 = {https://doi.org/10.1103/PhysRevA.79.062517}} @book{Ushveridze_1994, - Author = {Ushveridze, Alexander G}, - Isbn = {978-0-7503-0266-1}, - Publisher = {Institute of Physics Publishing}, - Title = {Quasi-exactly solvable models in quantum mechanics}, - Year = {1994}} + author = {Ushveridze, Alexander G}, + isbn = {978-0-7503-0266-1}, + publisher = {Institute of Physics Publishing}, + title = {Quasi-exactly solvable models in quantum mechanics}, + year = {1994}} @article{Lipkin_1965, - Author = {Lipkin, H. J. and Meshkov, N. and Glick, A. J.}, - Doi = {10.1016/0029-5582(65)90862-X}, - Journal = {Nucl. Phys.}, - Language = {en}, - Month = feb, - Number = {2}, - Pages = {188--198}, - Title = {Validity of many-body approximation methods for a solvable model: ({I}). {Exact} solutions and perturbation theory}, - Volume = {62}, - Year = {1965}, + author = {Lipkin, H. J. and Meshkov, N. and Glick, A. J.}, + doi = {10.1016/0029-5582(65)90862-X}, + journal = {Nucl. Phys.}, + language = {en}, + month = feb, + number = {2}, + pages = {188--198}, + title = {Validity of many-body approximation methods for a solvable model: ({I}). {Exact} solutions and perturbation theory}, + volume = {62}, + year = {1965}, Bdsk-Url-1 = {https://doi.org/10.1016/0029-5582(65)90862-X}} @article{Wigner_1934, - Author = {Wigner, E.}, - Doi = {10.1103/PhysRev.46.1002}, - Journal = {Phys. Rev.}, - Month = dec, - Number = {11}, - Pages = {1002--1011}, - Title = {On the {Interaction} of {Electrons} in {Metals}}, - Volume = {46}, - Year = {1934}, + author = {Wigner, E.}, + doi = {10.1103/PhysRev.46.1002}, + journal = {Phys. Rev.}, + month = dec, + number = {11}, + pages = {1002--1011}, + title = {On the {Interaction} of {Electrons} in {Metals}}, + volume = {46}, + year = {1934}, Bdsk-Url-1 = {https://doi.org/10.1103/PhysRev.46.1002}} @article{Thompson_2005, - Author = {Thompson, David C. and Alavi, Ali}, - Doi = {10.1063/1.1869978}, - Issn = {0021-9606}, - Journal = {J. Chem. Phys.}, - Month = mar, - Number = {12}, - Pages = {124107}, - Title = {A comparison of {Hartree}--{Fock} and exact diagonalization solutions for a model two-electron system}, - Volume = {122}, - Year = {2005}, + author = {Thompson, David C. and Alavi, Ali}, + doi = {10.1063/1.1869978}, + issn = {0021-9606}, + journal = {J. Chem. Phys.}, + month = mar, + number = {12}, + pages = {124107}, + title = {A comparison of {Hartree}--{Fock} and exact diagonalization solutions for a model two-electron system}, + volume = {122}, + year = {2005}, Bdsk-Url-1 = {https://doi.org/10.1063/1.1869978}} @article{Seidl_2007, - Author = {Seidl, Michael}, - Doi = {10.1103/PhysRevA.75.062506}, - Journal = {Phys. Rev. A}, - Month = jun, - Number = {6}, - Pages = {062506}, - Title = {Adiabatic connection in density-functional theory: {Two} electrons on the surface of a sphere}, - Volume = {75}, - Year = {2007}, + author = {Seidl, Michael}, + doi = {10.1103/PhysRevA.75.062506}, + journal = {Phys. Rev. A}, + month = jun, + number = {6}, + pages = {062506}, + title = {Adiabatic connection in density-functional theory: {Two} electrons on the surface of a sphere}, + volume = {75}, + year = {2007}, Bdsk-Url-1 = {https://doi.org/10.1103/PhysRevA.75.062506}} @article{Loos_2009b, - Author = {Loos, Pierre-Fran{\c c}ois and Gill, Peter M. W.}, - Doi = {10.1103/PhysRevLett.103.123008}, - Journal = {Phys. Rev. Let.}, - Month = sep, - Number = {12}, - Pages = {123008}, - Title = {Two {Electrons} on a {Hypersphere}: {A} {Quasiexactly} {Solvable} {Model}}, - Volume = {103}, - Year = {2009}, + author = {Loos, Pierre-Fran{\c c}ois and Gill, Peter M. W.}, + doi = {10.1103/PhysRevLett.103.123008}, + journal = {Phys. Rev. Let.}, + month = sep, + number = {12}, + pages = {123008}, + title = {Two {Electrons} on a {Hypersphere}: {A} {Quasiexactly} {Solvable} {Model}}, + volume = {103}, + year = {2009}, Bdsk-Url-1 = {https://doi.org/10.1103/PhysRevLett.103.123008}} diff --git a/Manuscript/EPAWTFT.blg b/Manuscript/EPAWTFT.blg index 81a86b0..727fbc2 100644 --- a/Manuscript/EPAWTFT.blg +++ b/Manuscript/EPAWTFT.blg @@ -23,46 +23,45 @@ Control: production of article title (-1) disabled Control: page (0) single Control: year (1) truncated Control: production of eprint (0) enabled -Warning--empty year in Coulson_1949 -You've used 76 entries, +You've used 72 entries, 5847 wiz_defined-function locations, - 2147 strings with 28164 characters, -and the built_in function-call counts, 72588 in all, are: -= -- 4650 -> -- 1882 -< -- 494 -+ -- 601 -- -- 459 -* -- 11148 -:= -- 7202 -add.period$ -- 74 -call.type$ -- 76 -change.case$ -- 298 -chr.to.int$ -- 80 -cite$ -- 77 -duplicate$ -- 6786 -empty$ -- 5460 -format.name$ -- 1102 -if$ -- 14470 -int.to.chr$ -- 5 -int.to.str$ -- 83 -missing$ -- 887 -newline$ -- 274 -num.names$ -- 222 -pop$ -- 2827 + 2133 strings with 28024 characters, +and the built_in function-call counts, 70033 in all, are: += -- 4473 +> -- 1850 +< -- 481 ++ -- 585 +- -- 453 +* -- 10828 +:= -- 6899 +add.period$ -- 70 +call.type$ -- 72 +change.case$ -- 282 +chr.to.int$ -- 78 +cite$ -- 72 +duplicate$ -- 6517 +empty$ -- 5216 +format.name$ -- 1078 +if$ -- 13975 +int.to.chr$ -- 3 +int.to.str$ -- 79 +missing$ -- 860 +newline$ -- 262 +num.names$ -- 210 +pop$ -- 2686 preamble$ -- 1 -purify$ -- 367 +purify$ -- 350 quote$ -- 0 -skip$ -- 2666 +skip$ -- 2570 stack$ -- 0 -substring$ -- 1918 -swap$ -- 6353 -text.length$ -- 222 +substring$ -- 1863 +swap$ -- 6176 +text.length$ -- 219 text.prefix$ -- 0 top$ -- 10 -type$ -- 1036 -warning$ -- 2 -while$ -- 223 +type$ -- 993 +warning$ -- 1 +while$ -- 215 width$ -- 0 -write$ -- 633 -(There were 2 warnings) +write$ -- 606 +(There was 1 warning) diff --git a/Manuscript/EPAWTFT.log b/Manuscript/EPAWTFT.log index 685dbfc..f63c5bc 100644 --- a/Manuscript/EPAWTFT.log +++ b/Manuscript/EPAWTFT.log @@ -1,4 +1,4 @@ -This is pdfTeX, Version 3.14159265-2.6-1.40.21 (TeX Live 2020) (preloaded format=pdflatex 2020.6.14) 24 AUG 2020 11:00 +This is pdfTeX, Version 3.14159265-2.6-1.40.21 (TeX Live 2020) (preloaded format=pdflatex 2020.6.14) 12 NOV 2020 12:04 entering extended mode restricted \write18 enabled. file:line:error style messages enabled. @@ -587,55 +587,55 @@ Package uniquecounter Info: New unique counter `rerunfilecheck' on input line 2 \Hy@SectionHShift=\skip78 ) Class revtex4-1 Info: Unrecognized array package. 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PDF statistics: - 743 PDF objects out of 1000 (max. 8388607) - 656 compressed objects within 7 object streams - 170 named destinations out of 1000 (max. 500000) - 59112 words of extra memory for PDF output out of 61914 (max. 10000000) + 457 PDF objects out of 1000 (max. 8388607) + 430 compressed objects within 5 object streams + 120 named destinations out of 1000 (max. 500000) + 47241 words of extra memory for PDF output out of 51595 (max. 10000000) diff --git a/Manuscript/EPAWTFT.out b/Manuscript/EPAWTFT.out index 6f335e0..97cf40c 100644 --- a/Manuscript/EPAWTFT.out +++ b/Manuscript/EPAWTFT.out @@ -1,4 +1,4 @@ -\BOOKMARK [0][-]{section*.2}{Perturbation theory in the complex plane}{}% 2 +\BOOKMARK [0][-]{section*.2}{Perturbation theory in the complex plane: Exceptional points and where to find them}{}% 2 \BOOKMARK [1][-]{section*.1}{Abstract}{section*.2}% 1 \BOOKMARK [1][-]{section*.3}{Introduction}{section*.2}% 3 \BOOKMARK [2][-]{section*.4}{Background}{section*.3}% 4 @@ -7,16 +7,11 @@ \BOOKMARK [2][-]{section*.7}{Rayleigh-Schr\366dinger perturbation theory}{section*.6}% 7 \BOOKMARK [2][-]{section*.8}{The Hartree-Fock Hamiltonian}{section*.6}% 8 \BOOKMARK [2][-]{section*.9}{M\370ller-Plesset perturbation theory}{section*.6}% 9 -\BOOKMARK [2][-]{section*.10}{Alternative partitioning}{section*.6}% 10 -\BOOKMARK [1][-]{section*.11}{Historical overview}{section*.2}% 11 -\BOOKMARK [2][-]{section*.12}{Behavior of the M\370ller-Plesset series}{section*.11}% 12 -\BOOKMARK [2][-]{section*.13}{Cases of divergence}{section*.11}% 13 -\BOOKMARK [2][-]{section*.14}{The singularity structure}{section*.11}% 14 -\BOOKMARK [2][-]{section*.15}{The physics of quantum phase transition}{section*.11}% 15 -\BOOKMARK [1][-]{section*.16}{The spherium model}{section*.2}% 16 -\BOOKMARK [1][-]{section*.17}{Radius of convergence and exceptional points}{section*.2}% 17 -\BOOKMARK [2][-]{section*.18}{Evolution of the radius of convergence}{section*.17}% 18 -\BOOKMARK [2][-]{section*.19}{Exceptional points in the UHF formalism}{section*.17}% 19 -\BOOKMARK [1][-]{section*.20}{Conclusion}{section*.2}% 20 -\BOOKMARK [1][-]{section*.21}{Acknowledgments}{section*.2}% 21 -\BOOKMARK [1][-]{section*.22}{References}{section*.2}% 22 +\BOOKMARK [1][-]{section*.10}{Historical overview}{section*.2}% 10 +\BOOKMARK [2][-]{section*.11}{Behavior of the M\370ller-Plesset series}{section*.10}% 11 +\BOOKMARK [2][-]{section*.12}{Cases of divergence}{section*.10}% 12 +\BOOKMARK [2][-]{section*.13}{The singularity structure}{section*.10}% 13 +\BOOKMARK [2][-]{section*.14}{The physics of quantum phase transitions}{section*.10}% 14 +\BOOKMARK [1][-]{section*.15}{Conclusion}{section*.2}% 15 +\BOOKMARK [1][-]{section*.16}{Acknowledgments}{section*.2}% 16 +\BOOKMARK [1][-]{section*.17}{References}{section*.2}% 17 diff --git a/Manuscript/EPAWTFT.pdf b/Manuscript/EPAWTFT.pdf index 1fc8170..cdbe9ec 100644 Binary files a/Manuscript/EPAWTFT.pdf and b/Manuscript/EPAWTFT.pdf differ diff --git a/Manuscript/EPAWTFT.synctex.gz b/Manuscript/EPAWTFT.synctex.gz index 72ccb1f..998e2eb 100644 Binary files a/Manuscript/EPAWTFT.synctex.gz and b/Manuscript/EPAWTFT.synctex.gz differ diff --git a/Manuscript/EPAWTFT.tex b/Manuscript/EPAWTFT.tex index 286abe8..63c150d 100644 --- a/Manuscript/EPAWTFT.tex +++ b/Manuscript/EPAWTFT.tex @@ -31,6 +31,7 @@ % operators \newcommand{\bH}{\mathbf{H}} +\newcommand{\bV}{\mathbf{V}} \newcommand{\bh}{\mathbf{h}} \newcommand{\bQ}{\mathbf{Q}} \newcommand{\bSig}{\mathbf{\Sigma}} @@ -72,32 +73,35 @@ \newcommand{\VU}{Department of Theoretical Chemistry and Amsterdam Center for Multiscale Modeling, FEW, Vrije Universiteit, De Boelelaan 1083, 1081HV Amsterdam, The Netherlands.} \begin{document} -\title{Perturbation theory in the complex plane} -%\title{Exceptional points and where to find them} +\title{Perturbation theory in the complex plane: Exceptional points and where to find them} \author{Antoine \surname{Marie}} \affiliation{\LCPQ} \author{Hugh G.~A.~\surname{Burton}} \affiliation{\UCAM} -\author{Paola \surname{Gori-Giorgi}} -\affiliation{\VU} +%\author{Paola \surname{Gori-Giorgi}} +%\affiliation{\VU} \author{Pierre-Fran\c{c}ois \surname{Loos}} \email{loos@irsamc.ups-tlse.fr} \affiliation{\LCPQ} \begin{abstract} -In this work, we explore the extension of quantum chemistry in the complex plane. We observe that the physics of a quantum system is intimately connected to the position of the energy singularities in the complex plane. After a brief presentation of the fundamental notions of quantum chemistry and perturbation theory in the complex plane, we provide a historical overview of the various research activities that have been performed on the physic of singularities. Then we connect and further discuss these different aspects using the spherium model (\ie, two opposite-spin electrons restricted to remain on the surface of a sphere) as a theoretical playground. In particular, we explore various perturbative partitioning strategies and the effects of symmetry breaking on the singularity structure of the electronic energy. This provides fundamental insights on the location of these singularities in the complex plane (that one calls exceptional points) and, specifically, on the magnitude of the radius of convergence associated with the perturbative treatment. +In this review, we explore the extension of quantum chemistry in the complex plane. +We observe that the physics of a quantum system is intimately connected to the position of the energy singularities in the complex plane. +After a presentation of the fundamental notions of quantum chemistry and perturbation theory in the complex plane, we provide a historical overview of the various research activities that have been performed on the physic of singularities. \end{abstract} \maketitle -%============================================================% +%%%%%%%%%%%%%%%%%%%%%%% \section{Introduction} \label{sec:intro} -%============================================================% +%%%%%%%%%%%%%%%%%%%%%%% +%======================% \subsection{Background} +%=======================% Due to the ubiquitous influence of processes involving electronic excited states in physics, chemistry, and biology, their faithful description from first principles has been one of the grand challenges faced by theoretical chemists since the dawn of computational chemistry. Accurately predicting ground- and excited-state energies (hence excitation energies) is particularly valuable in this context, and it has concentrated most of the efforts within the community. @@ -111,24 +115,26 @@ However, one can gain a different perspective on quantization extending quantum In a non-Hermitian complex picture, the energy levels are \textit{sheets} of a more complicated topological manifold called \textit{Riemann surface}, and they are smooth and continuous \textit{analytic continuation} of one another. In other words, our view of the quantized nature of conventional Hermitian quantum mechanics arises only from our limited perception of the more complex and profound structure of its non-Hermitian variant. \cite{MoiseyevBook,BenderPTBook} The realization that ground and excited states both emerge from one single mathematical structure with equal importance suggests that excited-state energies can be computed from first principles in their own right. -One could then exploit the structure of these Riemann surfaces to develop methods that directly target excited-state energies without needing ground-state information. \cite{Burton_2019} +One could then exploit the structure of these Riemann surfaces to develop methods that directly target excited-state energies without needing ground-state information. \cite{Burton_2019,Burton_2019a} By analytically continuing the electronic energy $E(\lambda)$ in the complex domain (where $\lambda$ is a coupling parameter), the ground and excited states of a molecule can be smoothly connected. This connection is possible because by extending real numbers to the complex domain, the ordering property of real numbers is lost. Hence, electronic states can be interchanged away from the real axis since the concept of ground and excited states has been lost. -Amazingly, this smooth and continuous transition from one state to another has recently been experimentally realized in physical settings such as electronics, microwaves, mechanics, acoustics, atomic systems and optics. \cite{Bittner_2012, Chong_2011, Chtchelkatchev_2012, Doppler_2016, Guo_2009, Hang_2013, Liertzer_2012, Longhi_2010, Peng_2014, Peng_2014a, Regensburger_2012, Ruter_2010, Schindler_2011, Szameit_2011, Zhao_2010, Zheng_2013, Choi_2018, El-Ganainy_2018} +Amazingly, this smooth and continuous transition from one state to another has recently been experimentally realized in physical settings such as electronics, microwaves, mechanics, acoustics, atomic systems and optics. \cite{Bittner_2012,Chong_2011,Chtchelkatchev_2012,Doppler_2016,Guo_2009,Hang_2013,Liertzer_2012,Longhi_2010,Peng_2014, Peng_2014a,Regensburger_2012,Ruter_2010,Schindler_2011,Szameit_2011,Zhao_2010,Zheng_2013,Choi_2018,El-Ganainy_2018} -Exceptional points (EPs) are branch point singularities where two (or more) states become exactly degenerate. \cite{Heiss_1990,Heiss_1999,Heiss_2012,Heiss_2016} +Exceptional points (EPs) are branch point singularities where two (or more) states become exactly degenerate. \cite{MoiseyevBook,Heiss_1988,Heiss_1990,Heiss_1999,Berry_2011,Heiss_2012,Heiss_2016,Benda_2018} They are the non-Hermitian analogs of conical intersections, \cite{Yarkony_1996} which are ubiquitous in non-adiabatic processes and play a key role in photo-chemical mechanisms. In the case of auto-ionizing resonances, EPs have a role in deactivation processes similar to conical intersections in the decay of bound excited states. \cite{Benda_2018} Although Hermitian and non-Hermitian Hamiltonians are closely related, the behavior of their eigenvalues near degeneracies is starkly different. -For example, encircling non-Hermitian degeneracies at EPs leads to an interconversion of states, and two loops around the EP are necessary to recover the initial energy. +For example, encircling non-Hermitian degeneracies at EPs leads to an interconversion of states, and two loops around the EP are necessary to recover the initial energy. \cite{MoiseyevBook,Heiss_2016,Benda_2018} Additionally, the wave function picks up a geometric phase (also known as Berry phase \cite{Berry_1984}) and four loops are required to recover the initial wave function. In contrast, encircling Hermitian degeneracies at conical intersections only introduces a geometric phase while leaving the states unchanged. More dramatically, whilst eigenvectors remain orthogonal at conical intersections, at non-Hermitian EPs the eigenvectors themselves become equivalent, resulting in a \textit{self-orthogonal} state. \cite{MoiseyevBook} -More importantly here, although EPs usually lie off the real axis, these singular points are intimately related to the convergence properties of perturbative methods and avoided crossing on the real axis are indicative of singularities in the complex plane. \cite{BenderBook,Olsen_1996,Olsen_2000,Olsen_2019} +More importantly here, although EPs usually lie off the real axis, these singular points are intimately related to the convergence properties of perturbative methods and avoided crossing on the real axis are indicative of singularities in the complex plane. \cite{BenderBook,Olsen_1996,Olsen_2000,Olsen_2019,Mihalka_2017a,Mihalka_2017b,Mihalka_2019} +%===================================% \subsection{An illustrative example} +%===================================% In order to highlight the general properties of EPs mentioned above, we propose to consider the following $2 \times 2$ Hamiltonian commonly used in quantum chemistry \begin{equation} @@ -180,53 +186,16 @@ and we have E_{\pm}(4\pi) & = E_{\pm}(0). \notag \end{align} This evidences that encircling non-Hermitian degeneracies at EPs leads to an interconversion of states, and two loops around the EP are necessary to recover the initial energy. -Additionally, the wave function picks up a geometric phase (also known as Berry phase \cite{Berry_1984}) and four loops are required to recover the starting wave function. +Additionally, the wave function picks up a geometric phase and four loops are required to recover the starting wave function. \cite{MoiseyevBook} -%The eigenvectors associated to the eigenenergies \eqref{eq:E_2x2} are -%\begin{equation}\label{eq:phi_2x2} -%\begin{split} -% \phi_{\pm} -% & = -% \begin{pmatrix} -% (\epsilon_1 - \epsilon_2 \pm \sqrt{(\epsilon_1 - \epsilon_2)^2 + 4\lambda^2})/2\lambda -% \\ -% 1 -% \end{pmatrix} -% \\ -% = -% \begin{pmatrix} -% (\epsilon_1-\epsilon_2)/2\lambda \pm \sqrt{2\lambda_\text{EP}} \sqrt{\lambda - \lambda_\text{EP}}/\lambda -% \\ -% 1 -% \end{pmatrix}, -%\end{split} -%\end{equation} -%and, for $\lambda=\lambda_\text{EP}$, they become -%\begin{equation} -% \phi_{\pm} = \begin{pmatrix} \mp i \\ 1\end{pmatrix}, -%\end{equation} -%which are clearly self-orthogonal, \ie, their norm is equal to zero. -% -%As branch point (square-root) singularities, EPs inherit their topology from the multi-valued function $\sqrt{\lambda - \lambda_\text{EP}}$. -%Then, if the eigenvectors are properly normalized, they behave as $(\lambda - \lambda_\text{EP})^{-1/4}$, which gives the following pattern when looping around one EP: -%\begin{align} -% \phi_{\pm}(2\pi) & = \phi_{\mp}(0), -% & -% \phi_{\pm}(4\pi) & = -\phi_{\pm}(0), \notag -% \\ -% \phi_{\pm}(6\pi) & = -\phi_{\mp}(0), -% & -% \phi_{\pm}(8\pi) & = \phi_{\pm}(0).\notag -%\end{align} -%In plain words, four loops around the EP are necessary to recover the initial state. -%We can also see that looping the other way around leads to a different pattern. - -%============================================================% +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% \section{Perturbation theory} -%============================================================% +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% +%============================================================% \subsection{Rayleigh-Schr\"odinger perturbation theory} +%============================================================% Within the Born-Oppenheimer approximation, \begin{equation}\label{eq:ExactHamiltonian} @@ -246,7 +215,7 @@ is recast as \end{equation} where $\hH^{(0)}$ is the zeroth-order Hamiltonian and $\hV = \hH - \hH^{(0)}$ is the so-called perturbation. The ``physical'' system of interest is recovered by setting the coupling parameter $\lambda$ to unity. -This decomposition is obviously non-unique and motivated by several factors as discussed below. +This decomposition is obviously non-unique and motivated by several factors as discussed below. \cite{Mihalka_2017b} Accordingly to Eq.~\eqref{eq:SchrEq-PT}, the energy can then be written as a power series of $\lambda$ \begin{equation} \label{eq:Elambda} @@ -265,8 +234,9 @@ This theorem means that the radius of convergence of the perturbation series is \end{equation} This function is smooth for $x \in \mathbb{R}$ and infinitely differentiable in $\mathbb{R}$. One would expect that the Taylor series of such a function would be convergent $\forall x \in \mathbb{R}$. However this series is divergent for $x \ge 1$. This is because the function has four singularities in the complex plane ($x = e^{i\pi/4}$, $e^{-i\pi/4}$, $e^{i3\pi/4}$, and $e^{-i3\pi/4}$) with a modulus equal to $1$. This simple yet powerful example emphasizes the importance of the singularities in the complex plane to understand the convergence properties on the real axis. - +%============================================================% \subsection{The Hartree-Fock Hamiltonian} +%============================================================% In the Hartree-Fock (HF) approximation, the many-electron wave function is approximated as a single Slater determinant $\Psi^{\text{HF}}(\vb{x}_1,\ldots,\vb{x}_n)$ [where $\vb{x} = (\sigma,\vb{r})$ is a composite vector gathering spin and spatial coordinates] defined as an antisymmetric combination of $n$ (real-valued) one-electron spin-orbitals $\phi_p(\vb{x})$, which are, by definition, eigenfunctions of the one-electron Fock operator \begin{equation}\label{eq:FockOp} @@ -291,14 +261,13 @@ is the HF mean-field potential with \end{gather} \end{subequations} being the Coulomb and exchange operators (respectively) in the spin-orbital basis. \cite{SzaboBook} -If the spatial part of the spin-orbitals are restricted to be the same for spin-up and spin-down electrons, one talks about restricted HF (RHF) theory, whereas if one does not enforce this constrain it leads to the so-called unrestricted HF (UHF) theory. +If the spatial part of the spin-orbitals are restricted to be the same for spin-up and spin-down electrons, one talks about restricted HF (RHF) theory, whereas if one does not enforce this constrain it leads to the so-called unrestricted HF (UHF) theory. From hereon, $i$ and $j$ are occupied orbitals, $a$ and $b$ are unoccupied (or virtual) orbitals, while $p$, $q$, $r$, and $s$ indicate arbitrary orbitals. Rather than solving Eq.~\eqref{eq:SchrEq}, HF theory uses the variational principle to find an approximation of $\Psi$ as a single Slater determinant. Hence a Slater determinant is not an eigenfunction of the exact Hamiltonian $\hH$. However, it is, by definition, an eigenfunction of the so-called (approximated) HF many-electron Hamiltonian defined as the sum of the one-electron Fock operators \begin{equation}\label{eq:HFHamiltonian} \hH^{\text{HF}} = \sum_{i} f(\vb{x}_i). \end{equation} -%Note that the lowest eigenvalue of the Hamiltonian \eqref{eq:HFHamiltonian} is not the HF energy but the sum of the eigenvalues associated with the occupied eigenvalues (see below). \subsection{M{\o}ller-Plesset perturbation theory} @@ -329,9 +298,9 @@ The MP2 energy reads \end{equation} with $\mel{pq}{}{rs} = \braket{pq}{rs} - \braket{pq}{sr}$, and where \begin{equation} - \braket{pq}{rs} = \iint \dd\vb{x}_1\dd\vb{x}_2\phi_p(\vb{x}_1)\phi_q(\vb{x}_2)\frac{1}{\abs{\vb{r}_1 - \vb{r}_2}}\phi_r(\vb{x}_1)\phi_s(\vb{x}_2) + \braket{pq}{rs} = \iint \dd\vb{x}_1\dd\vb{x}_2\frac{\phi_p(\vb{x}_1)\phi_q(\vb{x}_2)\phi_r(\vb{x}_1)\phi_s(\vb{x}_2)}{\abs{\vb{r}_1 - \vb{r}_2}} \end{equation} -is a two-electron integral in the spin-orbital basis. +are two-electron integral in the spin-orbital basis. \cite{Gill_1994} As mentioned earlier, there is, \textit{a priori}, no guarantee that the MP$m$ series converges to the exact energy when $m \to \infty$. In fact, it is known that when the HF wave function is a poor approximation to the exact wave function, for example in multi-reference systems, the MP method yields deceptive results. \cite{Gill_1986, Gill_1988, Handy_1985, Lepetit_1988} @@ -344,22 +313,19 @@ In order to better understand the behavior of the MP series and how it is connec For small systems, one can access the whole terms of the series using full configuration interaction (FCI). If the Hamiltonian $H(\lambda)$ is diagonalized in the FCI space, one gets the exact energies (in this finite Hilbert space) and the Taylor expansion with respect to $\lambda$ allows to access the MP perturbation series at any order. -\subsection{Alternative partitioning}\label{sec:AlterPart} +Obviously, although practically convenient for electronic structure calculations, the MP partitioning is not the only possibility, and alternative partitioning have been proposed in the literature: +i) the Epstein-Nesbet (EN) partitioning which consists in taking the diagonal elements of $\hH$ as the zeroth-order Hamiltonian. \cite{Nesbet_1955,Epstein_1926} +Hence, the off-diagonal elements of $\hH$ are the perturbation operator, +ii) the weak correlation partitioning in which the one-electron part is consider as the unperturbed Hamiltonian $\hH^{(0)}$ and the two-electron part is the perturbation operator $\hV$, and +iii) the strong coupling partitioning where the two operators are inverted compared to the weak correlation partitioning. \cite{Seidl_2018} -Obviously, although practically convenient for electronic structure calculations, the MP partitioning is not the only possibility. -Here, we will consider three alternative partitioning schemes: -\begin{itemize} - \item The Epstein-Nesbet (EN) partitioning which consists in taking the diagonal elements of $\hH$ as the zeroth-order Hamiltonian. - Hence, the off-diagonal elements of $\hH$ are the perturbation operator. - \item The weak correlation (WC) partitioning in which the one-electron part is consider as the unperturbed Hamiltonian $\hH^{(0)}$ and the two-electron part is the perturbation operator $\hV$. - \item The strong coupling (SC) partitioning where the two operators are inverted compared to the WC partitioning. \cite{Seidl_2018} -\end{itemize} - -%============================================================% +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% \section{Historical overview} -%============================================================% +%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% +%=====================================================% \subsection{Behavior of the M{\o}ller-Plesset series} +%=====================================================% When one relies on MP perturbation theory (and more generally on any perturbative partitioning), it would be reasonable to ask for a systematic improvement of the energy with respect to the perturbative order, \ie, one would expect that the more terms of the perturbative series one can compute, the closer the result from the exact energy. %In other words, each time a higher-order term is computed, one would like to obtained an overall result closer to the exact energy. @@ -369,23 +335,23 @@ In Ref.~\onlinecite{Gill_1986}, the authors showed that the RMP series is conver On the other hand, the UMP series is monotonically convergent (except for the first few orders) but very slowly. Thus, one cannot practically use it for systems where only the first terms can be computed. -When a bond is stretched, in most cases the exact wave function becomes more and more multi-reference. Yet the HF wave function is restricted to be a single Slater determinant. -Thus, it is inappropriate to model (even qualitatively) stretched systems. Nevertheless, the HF wave function can undergo a symmetry breaking to lower its energy by sacrificing one of the symmetry of the exact wave function during the process (see for example the case of \ce{H2} in Ref.~\onlinecite{SzaboBook}). -One could then potentially claim that the RMP series exhibits deceptive convergence properties as the RHF Slater determinant is a poor approximation of the exact wave function for stretched system. However, even in the unrestricted formalism which clearly represents a better description of a stretched system, the UMP series does not have the smooth and rapidly converging behavior that one would wish for. +When a bond is stretched, in most cases the exact wave function becomes more and more of multi-reference nature. +Yet the HF wave function is restricted to be a single Slater determinant. +It is then inappropriate to model (even qualitatively) stretched systems. Nevertheless, the HF wave function can undergo symmetry breaking to lower its energy by sacrificing one of the symmetry of the exact wave function in the process (see for example the case of \ce{H2} in Ref.~\onlinecite{SzaboBook}). +One could then potentially claim that the RMP series exhibits deceptive convergence properties as the RHF Slater determinant is a poor approximation of the exact wave function for stretched system. However, even in the unrestricted formalism which clearly represents a better description of a stretched system, the UMP series does not have the smooth and rapidly convergent behavior that one would wish for. In the unrestricted framework the singlet ground state wave function is allowed to mix with triplet wave functions, leading to the so-called spin contamination issue. Gill \textit{et al.}~highlighted the link between slow convergence of the UMP series and spin contamination for \ce{H2} in a minimal basis. \cite{Gill_1988} -Handy and coworkers reported the same behavior of the series (oscillatory and slowly monotonically convergent) in stretched \ce{H2O} and \ce{NH2} systems. \cite{Handy_1985} Lepetit \textit`{et al.}~analyzed the difference between the MP and EN partitioning for the UHF reference. \cite{Lepetit_1988} +Handy and coworkers reported the same behavior of the series (oscillatory and slowly monotonically convergent) in stretched \ce{H2O} and \ce{NH2}. \cite{Handy_1985} Lepetit \textit{et al.}~analyzed the difference between the MP and EN partitioning for the UHF reference. \cite{Lepetit_1988} They concluded that the slow convergence is due to the coupling of the singly- and doubly-excited configurations. Cremer and He analyzed 29 atomic and molecular systems at the FCI level \cite{Cremer_1996} and grouped them in two classes: i) the \textit{class A} systems where one observes a monotonic convergence to the FCI energy, and ii) the \textit{class B} systems for which convergence is erratic after initial oscillations. Their system set contains stretched molecules as well as molecules at their equilibrium geometry for various basis sets. They highlighted that \cite{Cremer_1996} -\begin{quote} - \textit{``Class A systems are characterized by electronic structures with well-separated electron pairs while class B systems are characterized by electronic structures with electron clustering in one or more regions.''} -\end{quote} +\textit{``Class A systems are characterized by electronic structures with well-separated electron pairs while class B systems are characterized by electronic structures with electron clustering in one or more regions.''} As one can only compute the first terms of the MP series, a smart way of getting more accurate results is to use extrapolation formula, \ie, estimating the limit of the series with only few terms. -Cremer and He proved that using specific extrapolation formulas of the MP series for class A and class B systems improves the precision of the results compared to the formula used without classes. The mean deviation from FCI correlation energies is $0.3$ millihartree with the adapted formula whereas with the formula that do not distinguish the systems it is 12 millihartree. -Even if there were still shaded areas and that this classification was incomplete, this work showed that understanding the origin of the different modes of convergence would lead to a more rationalized use of the MP perturbation theory and to more accurate correlation energies. - +Cremer and He proved that using specific extrapolation formulas of the MP series for class A and class B systems improves the precision of the results compared to the formula used without resorting to classes. The mean absolute deviation taking the FCI correlation energies as reference is $0.3$ millihartree with the class-specific formula whereas the deviation increases to 12 millihartree using the general formula. +Even if there were still shaded areas in their analysis and that their classification was incomplete, the work of Cremer and He clearly evidenced that understanding the origin of the different modes of convergence could potentially lead to a more rationalized use of MP perturbation theory and, hence, to more accurate correlation energy estimates. +%===============================% \subsection{Cases of divergence} +%===============================% In the late 90's, Olsen \textit{et al.}~discovered an even more preoccupying behavior of the MP series. \cite{Olsen_1996} They showed that the series could be divergent even in systems that they considered as well understood like \ce{Ne} and \ce{HF}. \cite{Olsen_1996, Christiansen_1996} Cremer and He had already studied these two systems and classified them as \textit{class B} systems. However, the analysis of Olsen and coworkers was performed in larger basis sets containing diffuse functions. In these basis sets, they found that the series become divergent at (very) high order. @@ -394,24 +360,24 @@ The discovery of this divergent behavior is worrying as in order to get meaningf \textit{``In the limit of large order, the series coefficients become equivalent to the Taylor series coefficients of the singularity closest to the origin. Following the result of this theorem, the convergence patterns of the MP series can be explained by looking at the dominant singularity.''} \end{quote} -A singularity in the unit circle is designated as an intruder state, more precisely as a front-door (respectively back-door) intruder state if the real part of the singularity is positive (respectively negative). Their method consists in performing a scan of the real axis to detect the avoided crossing responsible for the pair of dominant singularities. Then, by modeling this avoided crossing via a two-state Hamiltonian one can get an approximation of the dominant conjugate pair of singularities by finding the EPs of the following $2\times2$ Hamiltonian +A singularity in the unit circle is designated as an intruder state, more precisely as a front-door (respectively back-door) intruder state if the real part of the singularity is positive (respectively negative). Their method consists in performing a scan of the real axis to detect the avoided crossing responsible for the pair of dominant singularities. Then, by modeling this avoided crossing via a two-state Hamiltonian one can get an approximation of the dominant conjugate pair of singularities by finding the EPs of the following $2\times2$ matrix \begin{equation} -\underbrace{\mqty(\alpha & \delta \\ \delta & \beta)}_{\hH} = \underbrace{\mqty(\alpha + \alpha_s & 0 \\ 0 & \beta + \beta_s )}_{\hH^{(0)}} + \underbrace{\mqty(- \alpha_s & \delta \\ \delta & - \beta_s)}_{\hV}, +\underbrace{\mqty(\alpha & \delta \\ \delta & \beta)}_{\bH} = \underbrace{\mqty(\alpha + \alpha_s & 0 \\ 0 & \beta + \beta_s )}_{\bH^{(0)}} + \underbrace{\mqty(- \alpha_s & \delta \\ \delta & - \beta_s)}_{\bV}, \end{equation} -where the diagonal matrix is the unperturbed Hamiltonian and the other matrix is the perturbation. +where the diagonal matrix is the unperturbed Hamiltonian matrix $\bH^{(0)}$ and the second matrix in the right-hand-side $\bV$ is the perturbation. See also Ref.~\onlinecite{Olsen_2019} where the present model is generalized to a non-symmetric (i.e, non-Hermitian) Hamiltonian. They first studied molecules with low-lying doubly-excited states of the same spatial and spin symmetry. -% \titou{because in those systems the HF wave function is a bad approximation.} -The exact wave function has a non-negligible contribution from the doubly-excited states, so these low-lying excited states were good candidates for being intruder states. For \ce{CH_2} in a large basis set, the series is convergent up to the 50th order. They showed that the dominant singularity lies outside the unit circle but close to it causing the slow convergence. +The exact wave function has a non-negligible contribution from the doubly-excited states, so these low-lying excited states were good candidates for being intruder states. \titou{For \ce{CH_2} in a large basis set, the series is convergent up to the 50th order. They showed that the dominant singularity lies outside the unit circle but close to it causing the slow convergence.} Then they demonstrated that the divergence for \ce{Ne} is due to a back-door intruder state. When the basis set is augmented with diffuse functions, the ground state undergo sharp avoided crossings with highly diffuse excited states leading to a back-door intruder state. They used their two-state model on this avoided crossings and the model was actually predicting the divergence of the series. %They concluded that the divergence of the series was due to the interaction with a highly diffuse excited state. Moreover they proved that the extrapolation formulas of Cremer and He \cite{Cremer_1996} cannot be used for all systems, and that these formulas were not mathematically motivated when looking at the singularity causing the divergence. For example, the hydrogen fluoride molecule contains both back-door intruder states and low-lying doubly-excited states which results in alternated terms up to 10th order. For higher orders, the series is monotonically convergent. This surprising behavior is due to the fact that two pairs of singularities are approximately at the same distance from the origin. +%======================================= \subsection{The singularity structure} - +%======================================= In the 2000's, Sergeev and Goodson \cite{Sergeev_2005, Sergeev_2006} analyzed this problem from a more mathematical point of view by looking at the whole singularity structure where Olsen and collaborators were trying to find the dominant singularity causing the divergence. They regrouped singularities in two classes: i) $\alpha$ singularities which have ``large'' imaginary parts, and ii) $\beta$ singularities which have very small imaginary parts. Singularities of type $\alpha$ are related to large avoided crossing between the ground and low-lying excited states, whereas $\beta$ singularities come from a sharp avoided crossing between the ground state and a highly diffuse state. They succeeded to explain the divergence of the series caused by $\beta$ singularities following previous work of Stillinger. \cite{Stillinger_2000} To understand the convergence properties of the perturbation series at $\lambda=1$, one must look at the whole complex plane, in particular, for negative (\ie, real) values of $\lambda$. If $\lambda$ is negative, the Coulomb interaction becomes attractive but the mean field (which has been computed at $\lambda = 1$) remains repulsive as it is proportional to $(1-\lambda)$: @@ -421,311 +387,321 @@ To understand the convergence properties of the perturbation series at $\lambda= \hH(\lambda) = \sum_{i}^{n} \Bigg[ \overbrace{-\frac{1}{2}\grad_i^2 - - \sum_{A}^{N} \frac{Z_A}{\abs{\vb{r}_i-\vb{R}_A}}}^{\text{Independent of $\lambda$}} + - \sum_{A}^{N} \frac{Z_A}{\abs{\vb{r}_i-\vb{R}_A}}}^{\text{independent of $\lambda$}} \\ - + \underbrace{(1-\lambda)v^{\text{HF}}(\vb{x}_i)}_{\text{Repulsive for $\lambda < 1$}} - + \underbrace{\lambda\sum_{i3/2$ the sb-UHF solution is the global minimum of the HF equations and the RHF solution presented before is a local minimum. This solution corresponds to the configuration with the spin-up electron in an orbital on one side of the sphere and the spin-down electron in a miror-image orbital on the opposite side and the configuration the other way round. The electrons can be on opposite sides of the sphere because the choice of p\textsubscript{z} as a basis function induced a privileged axis on the sphere for the electrons. For $R>3/2$, this solution has the energy -\begin{equation}\label{eq:EsbUHF} - E_{\text{sb-UHF}}=-\frac{75}{112R^3}+\frac{25}{28R^2}+\frac{59}{84R}. -\end{equation} - -The exact solution for the ground state is a singlet. The spherical harmonics are eigenvectors of $\hS^2$ (the spin operator) and they are associated to different eigenvalues. Yet, the symmetry-broken orbitals are linear combinations of $Y_0$ and $Y_1$. Hence, the symmetry-broken orbitals are not eigenvectors of $\hS^2$. However, this solution gives lower energies than the RHF one at large $R$ as shown in Table \ref{tab:ERHFvsEUHF} even if it does not have the exact spin symmetry. In fact, at the Coulson-Fischer point, it becomes more effective to minimize the Coulomb repulsion than the kinetic energy in order to minimize the total energy. Thus, within the HF approximation, the variational principle is allowed to break the spin symmetry because it yields a more effective minimization of the Coulomb repulsion. This type of symmetry breaking is called a spin density wave because the system oscillates between the two symmetry-broken configurations. \cite{GiulianiBook} - -\begin{table*} -\caption{RHF and sb-UHF energies in the minimal basis and exact energies (in the complete basis) for various $R$. -\label{tab:ERHFvsEUHF}} -\begin{ruledtabular} -\begin{tabular}{ccccccccc} -$R$ & 0.1 & 1 & 2 & 3 & 5 & 10 & 100 & 1000 \\ -\hline -RHF & 10.00000 & 1.000000 & 0.500000 & 0.333333 & 0.200000 & 0.100000 & 0.010000 & 0.001000 \\ -UHF & 10.00000 & 1.000000 & 0.490699 & 0.308532 & 0.170833 & 0.078497 & 0.007112 & 0.000703 \\ -Exact & 9.783874 & 0.852781 & 0.391959 & 0.247898 & 0.139471 & 0.064525 & 0.005487 & 0.000515 \\ -\end{tabular} -\end{ruledtabular} -\end{table*} - -There is also another symmetry-broken solution for $R>75/38$ but this one corresponds to a maximum of the HF equations. This solution is associated with another type of symmetry breaking somewhat less known. It corresponds to a configuration where both electrons are on the same side of the sphere, in the same spatial orbital. This solution is called symmetry-broken RHF (sb-RHF). The reasoning is counter-intuitive because the electrons tends to maximize their energy. The p\textsubscript{z} orbital is symmetric with respect to the center of the sphere. If the orbitals are symmetric, the maximum is when the two electrons are in the p\textsubscript{z} orbital because it maximizes the kinetic energy. At the critical value of $R$, placing the two electrons in the same symmetry-broken orbital \ie, on the same side of the sphere gives a superior energy than the p\textsubscript{z}\textsuperscript{2} state. Adding a s orbital on one side of the p\textsubscript{z} orbital to form a symmetry-broken orbital reduce the kinetic energy but increase the repulsion energy as the two electrons are more localized on one side of the sphere. It becomes more efficient to maximize the repulsion energy than the kinetic energy for $R>75/38$. This configuration breaks the spatial symmetry of charge. Hence this symmetry breaking is associated with a charge density wave, the system oscillates between the situations with the two electrons on each side. \cite{GiulianiBook} -The energy associated with this sb-RHF solution reads -\begin{equation} -E_{\text{sb-RHF}}=\frac{75}{88R^3}+\frac{25}{22R^2}+\frac{91}{66R}. -\end{equation} -\begin{figure} - \includegraphics[width=\linewidth]{EsbHF.pdf} - \caption{Energies of the five solutions of the HF equations (multiplied by $R^2$). The dotted curves correspond to the analytic continuation of the symmetry-broken solutions.} - \label{fig:SpheriumNrj} -\end{figure} - -We can also consider negative values of $R$, which corresponds to the situation where one of the electrons is replaced by a positron (the anti-particle of the electron) as readily seen in Eq.~\eqref{eq:H-sph-omega}. For negative $R$ values, there are also a sb-RHF ($R<-3/2$) and a sb-UHF ($R<-75/38$) solution for negative values of $R$ (see Fig.~\ref{fig:SpheriumNrj}) but in this case the sb-RHF solution is a minimum and the sb-UHF is a maximum of the HF equations. Indeed, the sb-RHF state minimizes the attraction energy by placing the electron and the positron on the same side of the sphere. And the sb-UHF state maximizes the energy because the two attracting particles are on opposite sides of the sphere. - -In addition, we can also consider the symmetry-broken solutions beyond their respective Coulson-Fischer points by analytically continuing their respective energies leading to the so-called holomorphic solutions. \cite{Hiscock_2014, Burton_2019, Burton_2019a} All those energies are plotted in Fig.~\ref{fig:SpheriumNrj}. The dotted curves corresponds to the holomorphic domain of the energies. - - -\section{Radius of convergence and exceptional points} - -\subsection{Evolution of the radius of convergence} - -In this subsection, we investigate how the partitioning of $\hH(\lambda)$ influence the radius of convergence of the perturbation series. Let us remind the reader that the radius of convergence is equal to the distance of the closest singularity to the origin of $E(\lambda)$. Hence, we have to determine the locations of the EPs to obtain information on the convergence properties of the perturbative series. To find them we solve simultaneously the following equations: \cite{Cejnar_2007} -\begin{subequations} -\begin{align} - \label{eq:PolChar} - \det[E\hI-\hH(\lambda)] & = 0, - \\ - \label{eq:DPolChar} - \pdv{E}\det[E\hI-\hH(\lambda)] & = 0, -\end{align} -\end{subequations} -where $\hI$ is the identity operator. -Equation \eqref{eq:PolChar} is the well-known secular equation providing us with the (eigen)energies of the system. If an energy is also solution of Eq.~\eqref{eq:DPolChar}, then this energy is, at least two-fold degenerate. In this case the energies obtained are dependent of $\lambda$. Thus, solving these equations with respect to $E$ and $\lambda$ gives the value of $\lambda$ where two energies are degenerate. These degeneracies can be conical intersections between two states with different symmetry for real values of $\lambda$ \cite{Yarkony_1996} or EPs between two states with the same symmetry for complex values of $\lambda$. - -Let us assume that electron 1 is spin-up and electron 2 is spin-down. -Hence, we can forget about the spin part of the spin-orbitals and from now on we will work with spatial orbitals. In the restricted formalism the spatial orbitals are the same so the two-electron basis set can be defined as - -\begin{align}\label{eq:rhfbasis} - \psi_1 & =Y_{0}(\theta_1)Y_{0}(\theta_2), - & - \psi_2 & =Y_{0}(\theta_1)Y_{1}(\theta_2),\\ - \psi_3 & =Y_{1}(\theta_1)Y_{0}(\theta_2), - & - \psi_4 & =Y_{1}(\theta_1)Y_{1}(\theta_2). -\end{align} -The Hamiltonian $\hH(\lambda)$ is block diagonal in this basis because of its symmetry, \ie, $\psi_1$ only interacts with $\psi_4$, and $\psi_2$ with $\psi_3$. The two singly-excited states yield, after diagonalization, a spatially anti-symmetric singlet $sp_z$ and a spatially symmetric triplet sp\textsubscript{z} state. Hence those states do not have the same symmetry as the spatially symmetric singlet ground state. Thus, these states cannot be involved in an avoided crossing with the ground state as can be seen in Fig.~\ref{fig:RHFMiniBas} and, \textit{a fortiori} cannot be involved in an EP with the ground state. However there is an avoided crossing between the s\textsuperscript{2} and p\textsubscript{z}\textsuperscript{2} states which gives two EPs in the complex plane. - -\begin{figure} - \includegraphics[width=\linewidth]{EMP_RHF_R10.pdf} - \caption{Energies $E(\lambda)$ in the restricted basis set \eqref{eq:rhfbasis} with $R=10$. - One can clearly see the avoided crossing between the s\textsuperscript{2} and p\textsubscript{z}\textsuperscript{2} states around $\lambda = 1$.} - \label{fig:RHFMiniBas} -\end{figure} - -To simplify the problem, it is convenient to only consider basis functions of a given symmetry. Such basis functions are called configuration state functions (CSFs). It simplifies greatly the problem because, with such a basis set, one only gets the degeneracies of interest associated with the convergence properties, \ie, the EPs between states with the same symmetry as the ground state. In the present context, the ground state is a totally symmetric singlet. According to angular momentum theory, \cite{AngularBook, SlaterBook, Loos_2009} we expand the exact wave function in the following two-electron basis: -\begin{equation} -\Phi_\ell(\omega)=\frac{\sqrt{2\ell+1}}{4\pi R^2}P_\ell(\cos\omega), -\end{equation} -where $P_\ell$ are Legendre polynomials. - -Then, using this basis set we can compare the different partitioning of Sec.~\ref{sec:AlterPart}. Figure \ref{fig:RadiusPartitioning} shows the evolution of the radius of convergence $R_{\text{CV}}$ as a function of $R$ for the MP, the EN, the WC and the SC partitioning in a minimal basis (\ie, consisting of $P_0$ and $P_1$) of size $K = 2$, and in the same basis augmented with $P_2$ ($K = 3$). We see that, for the SC partitioning, $R_{\text{CV}}$ increases with $R$ whereas it is decreasing for the three others partitioning. This result is expected because the MP, EN, and WC partitioning use a weakly correlated reference so $\hH^{(0)}$ is a good approximation for small $R$. On the contrary, the SC partitioning consider naturally a strongly correlated reference so the SC series converges far better when the electron are strongly correlated, \ie, when $R$ is large in the spherium model. - -Interestingly, the radius of convergence associated with the SC partitioning is greater than one for a greater range of radii for $K = 2$ than $K = 3$. - -\begin{figure} - \includegraphics[width=0.49\textwidth]{PartitioningRCV2.pdf} - \includegraphics[width=0.49\textwidth]{PartitioningRCV3.pdf} - \caption{Radius of convergence $R_{\text{CV}}$ for two (left) and three (right) basis functions for various partitionings.} - \label{fig:RadiusPartitioning} -\end{figure} - -The MP partitioning is always better than WC in Fig.~\ref{fig:RadiusPartitioning}. In the WC partitioning the powers of $R$ (the zeroth-order scales as $R^{-2}$ while the perturbation scales as $R^{-1}$) are well-separated so each term of the series has a well-defined power of $R$. This is not the case for the MP series. -Interestingly, it can be proved that the $m$th order energy of the WC series can be obtained as a Taylor series of MP$m$ with respect to $R$. -It seems that the EN is better than MP for very small $R$ in the minimal basis. In fact, it is just an artefact of the minimal basis because, for $K = 3$, the MP series has a greater radius of convergence for all values of $R$. It holds true for $K>3$. - - -Figure \ref{fig:RadiusBasis} shows that the radius of convergence is not very sensitive to the size of the basis set. The CSFs have all the same spin and spatial symmetries so we expect that the singularities obtained within this basis set will be $\alpha$ singularities. Table \ref{tab:SingAlpha} shows that the singularities considered in this case are indeed $\alpha$ singularities. This is consistent with the observation of Goodson and Sergeev \cite{Goodson_2004} who stated that $\alpha$ singularities are relatively insensitive to the basis set size. The discontinuities observed in Fig.~\ref{fig:RadiusBasis} for the MP partitioning are due to changes in dominant singularity. We can observe this change in Table \ref{tab:SingAlpha}, the value for $R=1$ and $R=2$ are respectively in the positive and negative planes. - -\begin{figure} - \includegraphics[width=0.49\textwidth]{MPlargebasis.pdf} - \includegraphics[width=0.49\textwidth]{WCElargebasis.pdf} - \caption{Radius of convergence $R_{\text{CV}}$ in the CSF basis with $K$ basis functions for the MP (left) and WC (right) partitioning.} - \label{fig:RadiusBasis} -\end{figure} - -\begin{table} -\footnotesize -\caption{Dominant singularity in the CSF basis set ($K=8$) for various value of $R$ in the MP and WC partitioning.} -\begin{tabular}{cccccccc} -\hline -\hline -$R$ & 0.1 & 1 & 2 & 3 & 5 & 10 & 100 \\ -\hline -MP & $+14.1-10.9\,i$ & $+2.38-1.47\,i$ & $-0.67-1.30\,i$ & $-0.49-0.89\,i$ & $-0.33-0.55\,i$ & $-0.22-0.31\,i$ & $+0.03-0.05\,i$ \\ -WC & $-9.6-10.7\,i$ & $-0.96-1.07\,i$ & $-0.48-0.53\,i$ & $-0.32-0.36\,i$ & $-0.19-0.21\,i$ & $-0.10-0.11\,i$ & $-0.01-0.01\,i$ \\ -\hline -\hline -\end{tabular} -\label{tab:SingAlpha} -\end{table} - -\subsection{Exceptional points in the UHF formalism}\label{sec:uhfSing} - -Now, we investigate the differences in the singularity structure between the RHF and UHF formalism. To do so, we use the symmetry-broken orbitals discussed in Sec.~\ref{sec:spherium}. Thus, the UHF two-electron basis is -\begin{align}\label{eq:uhfbasis} - \psi_1 & =\phi_{\alpha,1}(\theta_1)\phi_{\beta,1}(\theta_2), - & - \psi_2 & =\phi_{\alpha,1}(\theta_1)\phi_{\beta,2}(\theta_2),\\ - \psi_3 & =\phi_{\alpha,2}(\theta_1)\phi_{\beta,1}(\theta_2), - & - \psi_4 & =\phi_{\alpha,2}(\theta_1)\phi_{\beta,2}(\theta_2). -\end{align} -with the symmetry-broken orbitals -\begin{subequations} -\begin{align}\label{eq:uhforbitals} - \phi_{\alpha,1}(\theta) - & =\frac{\sqrt{75+62R}}{4\sqrt{7R}} Y_{0}(\theta) - + \frac{5\sqrt{-3+2R}}{4\sqrt{7R}} Y_{1}(\theta), - \\ - \phi_{\beta,1}(\theta) - & =\frac{\sqrt{75+62R}}{4\sqrt{7R}} Y_{0}(\theta) - - \frac{5\sqrt{-3+2R}}{4\sqrt{7R}} Y_{1}(\theta), - \\ - \phi_{\alpha,2}(\theta) - & = - \frac{5\sqrt{-3+2R}}{4\sqrt{7R}} Y_{0}(\theta) - + \frac{\sqrt{75+62R}}{4\sqrt{7R}} Y_{1}(\theta), - \\ - \phi_{\beta,2}(\theta) - & =\frac{5\sqrt{-3+2R}}{4\sqrt{7R}} Y_{0}(\theta) - +\frac{\sqrt{75+62R}}{4\sqrt{7R}} Y_{1}(\theta). -\end{align} -\end{subequations} - -In the UHF formalism the Hamiltonian $\hH(\lambda)$ is no more block diagonal, $\psi_4$ can interact with $\psi_2$ and $\psi_3$. The matrix elements of the Hamiltonian corresponding to this interaction are -\begin{equation}\label{eq:MatrixElem} - H_{24}=H_{34}=H_{42}=H_{43}=\sqrt{R-\frac{3}{2}}\sqrt{R+\frac{75}{62}}\qty(R+\frac{25}{2})\frac{\sqrt{31}}{70R^3} -\end{equation} - -For $R=3/2$ the Hamiltonian is block diagonal because the matrix elements \eqref{eq:MatrixElem} are equal to zero so this is equivalent to the RHF case but for $R>3/2$ the matrix elements become real. This interaction corresponds to the spin contamination of the wave function. For $R<3/2$ the matrix elements are complex, this corresponds to the holomorphic solution of Fig.~\ref{fig:SpheriumNrj}, the singularities in this case will be treated later. The matrix elements become real again for $R<-75/62$, this corresponds to the sb-UHF solution for negative value of $R$ observed in Sec.~\ref{sec:spherium}. We will refer to the domain where the matrix elements are complex as the holomorphic domain. - -The singularity structure in this case is more complex because of the spin contamination of the wave function. We can not use CSFs in this case. So when one compute all the degeneracies using Eqs.~\eqref{eq:PolChar} and \eqref{eq:DPolChar} some correspond to EPs and some correspond to conical intersections. The numerical distinction of those singularities is very difficult. We will first look at the energies $E(\lambda)$ obtained with this basis set to attribute a physical signification to the singularities obtained numerically. -Figure \ref{fig:UHFMiniBas} is the analog of Fig.~\ref{fig:RHFMiniBas} in the UHF formalism. We see that in this case the sp\textsubscript{z} triplet interacts with the s\textsuperscript{2} and the p\textsubscript{z}\textsuperscript{2} singlets. Those avoided crossings are due to the spin contamination of the wave function. - -\begin{figure} - \includegraphics[width=\linewidth]{EMP_UHF_R10.pdf} - \caption{Energies $E(\lambda)$ in the unrestricted basis set \eqref{eq:uhfbasis} with $R=10$.} - \label{fig:UHFMiniBas} -\end{figure} - -Within the RHF formalism, we have observed only $\alpha$ singularities and large avoided crossings but one can see in Fig.~\ref{fig:UHFMiniBas} that in the UHF case there are sharp avoided crossings which are known to be connected to $\beta$ singularities. For example at $R=10$ the pair of singularities connected to the avoided crossing between s\textsuperscript{2} and sp\textsubscript{z} $^{3}P$ is $0.999\pm0.014\,i$. And the one between sp\textsubscript{z} $^{3}P$ and p\textsubscript{z}\textsuperscript{2} is connected with the singularities $2.207\pm0.023\,i$. However, in spherium, the electrons cannot be ionized so those singularities cannot be the same $\beta$ singularities as the ones highlighted by Sergeev and Goodson. \cite{Sergeev_2005} We can see in Fig.~\ref{fig:UHFEP} that the s\textsuperscript{2} singlet and the sp\textsubscript{z} triplet states are degenerated for $R=3/2$. For $R>3/2$, it becomes an avoided crossing on the real axis and the degeneracies are $moved$ in the complex plane. The wave function is spin contaminated by $Y_1$ for $R>3/2$ this is why the s\textsuperscript{2} singlet energy cannot cross the sp\textsubscript{z} triplet curves anymore. When $R$ increases this avoided crossing becomes sharper. As presented before $\beta$ singularities are linked to quantum phase transition so it seems that this singularity is linked to the spin symmetry breaking of the UHF wave function. The fact that a similar pair of $\beta$ singularities appears for $R<-75/62$ confirms this assumption. The sharp avoided crossing between sp\textsubscript{z} $^{3}P$ and p\textsubscript{z}\textsuperscript{2} is not present on Fig. \ref{fig:UHFEP}. The second pair of $\beta$ singularities resulting from this avoided crossing appears for $R\gtrsim 2.5$, this is probably due to an excited-state quantum phase transition but this still need to be investigated. - -\begin{figure} - \includegraphics[width=0.45\textwidth]{UHFCI.pdf} - \includegraphics[width=0.45\textwidth]{UHFEP.pdf} - \caption{Energies $E(\lambda)$ in the unrestricted basis set \eqref{eq:uhfbasis} for $R=1.5$ (left) and $R=1.51$ (right).} - \label{fig:UHFEP} -\end{figure} - -As shown before, some matrix elements of the Hamiltonian become complex in the holomorphic domain. Therefore the Hamiltonian becomes non-Hermitian for these values of $R$. In Ref.~\onlinecite{Burton_2019a}, Burton \textit{et al.}~proved that for the \ce{H_2} molecule the unrestricted Hamiltonian is not \pt -symmetric in the holomorphic domain. An analog reasoning can be done with the spherium model to prove the same result. The \pt -symmetry (invariance with respect to combined space reflection $\mathcal{P}$ and time reversal $\mathcal{T}$) is a property which ensures that a non-Hermitian Hamiltonian has a real energy spectrum. \cite{BenderPTBook} Thus \pt -symmetric Hamiltonians can be seen as an intermediate class between Hermitian and non-Hermitian Hamiltonians. - -Figure \ref{fig:UHFPT} shows that for the spherium model a part of the energy spectrum becomes complex when $R$ is in the holomorphic domain. The domain of values where the energy becomes complex is called the broken \pt-symmetry region. This is consistent with the fact that in the holomorphic domain the Hamiltonian is no more \pt -symmetric. - -For a non-Hermitian Hamiltonian the EPs can lie on the real axis. In particular, at the point of {\pt} transition (the point where the energies become complex) the two energies are degenerate resulting in such an EP on the real axis. This degeneracy can be seen in Fig.~\ref{fig:UHFPT}. - -\begin{figure}[h!] - \includegraphics[width=0.45\textwidth]{ReNRJPT.pdf} - \includegraphics[width=0.45\textwidth]{ImNRJPT.pdf} - \caption{Real part (left) and imaginary part (right) of $E(\lambda)$ in the unrestricted basis set \eqref{eq:uhfbasis} for $R=1$.} - \label{fig:UHFPT} -\end{figure} +%%============================================================% +%\section{The spherium model} +%\label{sec:spherium} +%%============================================================% +% +%Simple systems that are analytically solvable (or at least quasi-exactly solvable, \ie, models for which it is possible to obtain a finite portion of the exact solutions of the Schr{\"o}dinger equation \cite{Ushveridze_1994}) are of great importance in theoretical chemistry. +%These systems are very useful to perform benchmark studies in order to test new methods as the mathematics are easier than in realistic systems (such as molecules or solids) but retain much of the key physics. +%To investigate the physics of EPs we consider one such system named \textit{spherium}. +%It consists of two electrons confined to the surface of a sphere interacting through the long-range Coulomb potential. \cite{Thompson_2005, Seidl_2007, Loos_2009b} +%Thus, the Hamiltonian is +%\begin{equation} +% \hH = -\frac{\grad_1^2 + \grad_2^2}{2} + \frac{1}{r_{12}}, +%\end{equation} +%or +%\begin{equation} \label{eq:H-sph-omega} +% \hH = -\frac{1}{R^2} \qty( \pdv[2]{}{\omega} + \cot \omega \pdv{}{\omega}) + \frac{1}{R \sqrt{2 - 2 \cos \omega}}, +%\end{equation} +%in term of the interelectronic angle $\omega$. +%The Laplace operators are the kinetic operators for each electron and $r_{12}^{-1} = \abs{\vb{r}_1 - \vb{r}_2}^{-1}$ is the Coulomb operator. +%Note that, as readily seen by the definition of the interelectronic distance $r_{12}$, the electrons interact through the sphere. +%The radius of the sphere $R$ dictates the correlation regime. \cite{Loos_2009} +%In the weak correlation regime (\ie, small $R$), the kinetic energy (which scales as $R^{-2}$) dominates and the electrons are delocalized over the sphere. +%For large $R$ (or strong correlation regime), the electron repulsion term (which scales as $R^{-1}$) drives the physics and the electrons localize on opposite side of the sphere to minimize their Coulomb repulsion. +%This phenomenon is sometimes referred to as a Wigner crystallization. \cite{Wigner_1934} +% +%We will use this model in order to rationalize the effects of the parameters that may influence the physics of EPs: +%i) Partitioning of the Hamiltonian and the actual zeroth-order reference: weak correlation reference (RHF or UHF references, MP or EN partitioning), or strongly correlated reference. +%ii) Basis set: minimal basis or infinite (\ie, complete) basis. +%iii) Radius of the sphere that ultimately dictates the correlation regime. +% +%In the RHF formalism, the two electrons are restricted to ``live'' in the same spatial orbital. +%The spatial part of the RHF wave function is then +%\begin{equation}\label{eq:RHF_WF} +% \Psi_{\text{RHF}}(\theta_1,\theta_2) = Y_0(\theta_1) Y_0(\theta_2), +%\end{equation} +%where $\theta_i$ is the polar angle of the $i$th electron and $Y_{\ell}(\theta)$ is a zonal spherical harmonic. +%Because $Y_0(\theta) = 1/\sqrt{4\pi}$, it is clear that the RHF wave function yields a uniform one-electron density. +% +%The RHF wave function cannot model properly the physics of the system at large $R$ because the spatial orbitals are restricted to be the same, and, \textit{a fortiori}, it cannot represent two electrons on opposite side of the sphere. +%Within the UHF formalism, there is a critical value of $R$, called Coulson-Fischer point, \cite{Coulson_1949} at which a UHF solution appears and is lower in energy than the RHF one. +%The UHF solution has broken symmetry because the two electrons tends to localize on opposite sides of the sphere. +%The spatial part of the UHF wave function is defined as +%\begin{equation}\label{eq:UHF_WF} +% \Psi_{\text{UHF}}(\theta_1,\theta_2)=\phi_\alpha(\theta_1)\phi_\beta(\theta_2), +%\end{equation} +%where $\phi_\sigma(\theta)$ is the spatial orbital associated with the spin-$\sigma$ electrons ($\sigma = \alpha$ for spin-up electrons and $\sigma = \beta$ for spin-down electrons). +%These one-electron orbitals are expanded in the basis of zonal spherical harmonics +%\begin{equation} +% \phi_\sigma(\theta)=\sum_{\ell=0}^{\infty}C_{\sigma,\ell}Y_{\ell}(\theta). +%\end{equation} +%It is possible to obtain the formula for the HF energy in this basis set: \cite{Loos_2009} +%\begin{equation} +% E_{\text{HF}} = T_{\text{HF}} + V_{\text{HF}}, +%\label{eq:EHF} +%\end{equation} +%where the kinetic and potential energies are, respectively, +%\begin{align} +% T_{\text{HF}} & = \frac{1}{R^2} \sum_{\sigma=\alpha,\beta} \sum_{\ell=0}^{\infty} C_{\sigma,\ell}^2 \, \ell(\ell+1), +% & +% V_{\text{HF}} & = \frac{1}{R} \sum_{L=0}^{\infty} +% v^\alpha_{L} v^\beta_{L}, +%\end{align} +%and +%\begin{equation} +% v^\sigma_{L} +% = \sum_{\ell_1,\ell_2} \sqrt{(2\ell_1+1)(2\ell_2+1)} C_{\sigma,\ell_1}C_{\sigma,\ell_2} +% \begin{pmatrix} +% \ell_1 & L & \ell_2 +% \\ +% 0 & 0 & 0 +% \end{pmatrix}^2 +%\end{equation} +%is expressed in terms of the Wigner 3j-symbols. \cite{AngularBook} +% +%The general method is to use a self-consistent field procedure as described in Ref.~\onlinecite{SzaboBook} to get the coefficients of the HF wave function corresponding to stationary solutions with respect to the coefficients $C_{\sigma,\ell}$, \ie, +%\begin{equation} +% \pdv{E_{\text{HF}}}{C_{\sigma,\ell}} = 0. +%\end{equation} +%Here, we work in a minimal basis, composed of $Y_{0}$ and $Y_{1}$, or equivalently, a $s$ and $p_{z}$ orbital, to illustrate the difference between the RHF and UHF solutions. In this basis there is a shortcut to find the stationary solutions and ensure normalization of the orbitals. One can define the one-electron orbitals as +%\begin{equation} +% \phi_\sigma(\theta)= \cos(\chi_\sigma)Y_{0}(\theta) + \sin(\chi_\sigma)Y_{1}(\theta), +%\end{equation} +%using a mixing angle $\chi_\sigma$ between the two basis functions for each spin manifold. +%Hence, one has just to minimize/maximize the energy with respect to the two mixing angles $\chi_\alpha$ and $\chi_\beta$. +% +%This process provides the three following solutions valid for all value of $R$, which are respectively a minimum, a maximum and a saddle point of the HF equations: +%i) the two electrons are in the $s$ orbital which is a RHF solution. This solution is associated with the energy $1/R$; +%ii) the two electrons are in the $p_{z}$ orbital which is a RHF solution. This solution is associated with the energy $2/R^{2}+ 29/(25R)$; +%iii) one electron is in the $s$ orbital and the other is in the $p_{z}$ orbital which is a UHF solution. This solution is associated with the energy $1/R^{2} + 1/R$. +% +%In addition, the minimization process gives also the well-known symmetry-broken UHF (sb-UHF) solution. In this case the Coulson-Fischer point associated to this solution is $R=3/2$. +%For $R>3/2$, the sb-UHF solution is the global minimum of the HF equations and the RHF solution presented before is a local minimum. This solution corresponds to the configuration with the spin-up electron in an orbital on one side of the sphere and the spin-down electron in a miror-image orbital on the opposite side and the configuration the other way round. The electrons can be on opposite sides of the sphere because the choice of $p_{z}$ as a basis function induced a privileged axis on the sphere for the electrons. For $R>3/2$, this solution has the energy +%\begin{equation}\label{eq:EsbUHF} +% E_{\text{sb-UHF}}=-\frac{75}{112R^3}+\frac{25}{28R^2}+\frac{59}{84R}. +%\end{equation} +% +%The exact solution for the ground state is a singlet. The spherical harmonics are eigenvectors of $\hS^2$ (the spin operator) and they are associated to different eigenvalues. +%Yet, the symmetry-broken orbitals are linear combinations of $Y_0$ and $Y_1$. +%Hence, the symmetry-broken orbitals are not eigenvectors of $\hS^2$. +%However, this solution gives lower energies than the RHF one at large $R$, even if it does not have the exact spin symmetry. +%In fact, at the Coulson-Fischer point, it becomes more effective to minimize the Coulomb repulsion than the kinetic energy in order to minimize the total energy. +%Thus, within the HF approximation, the variational principle is allowed to break the spin symmetry because it yields a more effective minimization of the Coulomb repulsion. +%This type of symmetry breaking is also called a spin-density wave in the physics community as the system ``oscillates'' between the two symmetry-broken configurations. \cite{GiulianiBook} +% +%There is also another symmetry-broken solution for $R>75/38$ but this one corresponds to a maximum of the HF equations. +%This solution is associated with another type of symmetry breaking somewhat less known. +%It corresponds to a configuration where both electrons are on the same side of the sphere, in the same spatial orbital. +%This solution is called symmetry-broken RHF (sb-RHF). The reasoning is counter-intuitive because the electrons tends to maximize their energy. +%The $sp_{z}$ orbital is symmetric with respect to the center of the sphere. +%If the orbitals are symmetric, the maximum is when the two electrons are in the $p_{z}$ orbital because it maximizes the kinetic energy. +%At the critical value of $R$, placing the two electrons in the same symmetry-broken orbital \ie, on the same side of the sphere gives a superior energy than the $p_{z}^2$ state. Adding a s orbital on one side of the $p_{z}$ orbital to form a symmetry-broken orbital reduce the kinetic energy but increase the repulsion energy as the two electrons are more localized on one side of the sphere. +%It becomes more efficient to maximize the repulsion energy than the kinetic energy for $R>75/38$. +%This configuration breaks the spatial symmetry of charge. +%Hence this symmetry breaking is associated with a charge-density wave as the system oscillates between the situations where the two electrons are one side or the other. \cite{GiulianiBook} +%The energy associated with this sb-RHF solution reads +%\begin{equation} +%E_{\text{sb-RHF}}=\frac{75}{88R^3}+\frac{25}{22R^2}+\frac{91}{66R}. +%\end{equation} +%\begin{figure} +% \includegraphics[width=\linewidth]{EsbHF.pdf} +% \caption{Energies of the five solutions of the HF equations (multiplied by $R^2$). The dotted curves correspond to the analytic continuation of the symmetry-broken solutions.} +% \label{fig:SpheriumNrj} +%\end{figure} +% +%We can also consider negative values of $R$, which corresponds to the situation where one of the electrons is replaced by a positron as readily seen in Eq.~\eqref{eq:H-sph-omega}. +%For negative $R$ values, there are also a sb-RHF ($R<-3/2$) and a sb-UHF ($R<-75/38$) solution for negative values of $R$ (see Fig.~\ref{fig:SpheriumNrj}) but in this case the sb-RHF solution is a minimum and the sb-UHF is a maximum of the HF equations. +%Indeed, the sb-RHF state minimizes the attraction energy by placing the electron and the positron on the same side of the sphere. +%And the sb-UHF state maximizes the energy because the two attracting particles are on opposite sides of the sphere. +% +%In addition, we can also consider the symmetry-broken solutions beyond their respective Coulson-Fischer points by analytically continuing their respective energies leading to the so-called holomorphic solutions. \cite{Hiscock_2014, Burton_2019, Burton_2019a} All those energies are plotted in Fig.~\ref{fig:SpheriumNrj}. The dotted curves corresponds to the holomorphic domain of the energies. +% +% +%\section{Radius of convergence and exceptional points} +% +%\subsection{Evolution of the radius of convergence} +% +%In this subsection, we investigate how the partitioning of $\hH(\lambda)$ influence the radius of convergence of the perturbation series. Let us remind the reader that the radius of convergence is equal to the distance of the closest singularity to the origin of $E(\lambda)$. Hence, we have to determine the locations of the EPs to obtain information on the convergence properties of the perturbative series. To find them we solve simultaneously the following equations: \cite{Cejnar_2007} +%\begin{subequations} +%\begin{align} +% \label{eq:PolChar} +% \det[E\hI-\hH(\lambda)] & = 0, +% \\ +% \label{eq:DPolChar} +% \pdv{E}\det[E\hI-\hH(\lambda)] & = 0, +%\end{align} +%\end{subequations} +%where $\hI$ is the identity operator. +%Equation \eqref{eq:PolChar} is the well-known secular equation providing us with the (eigen)energies of the system. If an energy is also solution of Eq.~\eqref{eq:DPolChar}, then this energy is, at least, two-fold degenerate. In this case the energies obtained are $\lambda$-dependent. +%Thus, solving these equations with respect to $E$ and $\lambda$ gives the value of $\lambda$ where two energies are degenerate. +%These degeneracies can be conical intersections between two states with different symmetries for real values of $\lambda$ \cite{Yarkony_1996} or EPs between two states with the same symmetry for complex values of $\lambda$. +% +%Let us assume that electron 1 is spin-up and electron 2 is spin-down. +%Hence, we can forget about the spin part of the spin-orbitals and from now on we will work with spatial orbitals. In the restricted formalism the spatial orbitals are the same so the two-electron basis set can be defined as +% +%\begin{align}\label{eq:rhfbasis} +% \psi_1 & =Y_{0}(\theta_1)Y_{0}(\theta_2), +% & +% \psi_2 & =Y_{0}(\theta_1)Y_{1}(\theta_2),\\ +% \psi_3 & =Y_{1}(\theta_1)Y_{0}(\theta_2), +% & +% \psi_4 & =Y_{1}(\theta_1)Y_{1}(\theta_2). +%\end{align} +%The Hamiltonian $\hH(\lambda)$ is block diagonal in this basis because of its symmetry, \ie, $\psi_1$ only interacts with $\psi_4$, and $\psi_2$ with $\psi_3$. The two singly-excited states yield, after diagonalization, a spatially anti-symmetric singlet $sp_z$ and a spatially symmetric triplet $sp_{z}$ state. +%Hence those states do not have the same symmetry as the spatially symmetric singlet ground state. +%Thus, these states cannot be involved in an avoided crossing with the ground state as can be seen in Fig.~\ref{fig:RHFMiniBas} and, \textit{a fortiori} cannot be involved in an EP with the ground state. +%However there is an avoided crossing between the $s^{2}$ and $p_{z}^{2}$ states which gives two EPs in the complex plane. +% +%\begin{figure} +% \includegraphics[width=\linewidth]{EMP_RHF_R10.pdf} +% \caption{Energies $E(\lambda)$ in the restricted basis set \eqref{eq:rhfbasis} with $R=10$. +% One can clearly see the avoided crossing between the $s^{2}$ and $p_{z}^{2}$ states around $\lambda = 1$.} +% \label{fig:RHFMiniBas} +%\end{figure} +% +%To simplify the problem, it is convenient to only consider basis functions of a given symmetry. Such basis functions are called configuration state functions (CSFs). It simplifies greatly the problem because, with such a basis set, one only gets the degeneracies of interest associated with the convergence properties, \ie, the EPs between states with the same symmetry as the ground state. In the present context, the ground state is a totally symmetric singlet. According to angular momentum theory, \cite{AngularBook, SlaterBook, Loos_2009} we expand the exact wave function in the following two-electron basis: +%\begin{equation} +%\Phi_\ell(\omega)=\frac{\sqrt{2\ell+1}}{4\pi R^2}P_\ell(\cos\omega), +%\end{equation} +%where $P_\ell$ are Legendre polynomials. +% +%Then, using this basis set we can compare the different partitioning of Sec.~\ref{sec:AlterPart}. Figure \ref{fig:RadiusPartitioning} shows the evolution of the radius of convergence $R_{\text{CV}}$ as a function of $R$ for the MP, the EN, the WC and the SC partitioning in a minimal basis (\ie, consisting of $P_0$ and $P_1$) of size $K = 2$, and in the same basis augmented with $P_2$ ($K = 3$). We see that, for the SC partitioning, $R_{\text{CV}}$ increases with $R$ whereas it is decreasing for the three others partitioning. This result is expected because the MP, EN, and WC partitioning use a weakly correlated reference so $\hH^{(0)}$ is a good approximation for small $R$. On the contrary, the SC partitioning consider naturally a strongly correlated reference so the SC series converges far better when the electron are strongly correlated, \ie, when $R$ is large in the spherium model. +% +%Interestingly, the radius of convergence associated with the SC partitioning is greater than one for a greater range of radii for $K = 2$ than $K = 3$. +% +%\begin{figure} +% \includegraphics[width=0.49\textwidth]{PartitioningRCV2.pdf} +% \includegraphics[width=0.49\textwidth]{PartitioningRCV3.pdf} +% \caption{Radius of convergence $R_{\text{CV}}$ for two (left) and three (right) basis functions for various partitionings.} +% \label{fig:RadiusPartitioning} +%\end{figure} +% +%The MP partitioning is always better than WC in Fig.~\ref{fig:RadiusPartitioning}. In the WC partitioning the powers of $R$ (the zeroth-order scales as $R^{-2}$ while the perturbation scales as $R^{-1}$) are well-separated so each term of the series has a well-defined power of $R$. This is not the case for the MP series. +%Interestingly, it can be proved that the $m$th order energy of the WC series can be obtained as a Taylor series of MP$m$ with respect to $R$. +%It seems that the EN is better than MP for very small $R$ in the minimal basis. In fact, it is just an artefact of the minimal basis because, for $K = 3$, the MP series has a greater radius of convergence for all values of $R$. It holds true for $K>3$. +% +% +%Figure \ref{fig:RadiusBasis} shows that the radius of convergence is not very sensitive to the size of the basis set. The CSFs have all the same spin and spatial symmetries so we expect that the singularities obtained within this basis set will be $\alpha$ singularities. Table \ref{tab:SingAlpha} shows that the singularities considered in this case are indeed $\alpha$ singularities. This is consistent with the observation of Goodson and Sergeev \cite{Goodson_2004} who stated that $\alpha$ singularities are relatively insensitive to the basis set size. The discontinuities observed in Fig.~\ref{fig:RadiusBasis} for the MP partitioning are due to changes in dominant singularity. We can observe this change in Table \ref{tab:SingAlpha}, the value for $R=1$ and $R=2$ are respectively in the positive and negative planes. +% +%\begin{figure} +% \includegraphics[width=0.49\textwidth]{MPlargebasis.pdf} +% \includegraphics[width=0.49\textwidth]{WCElargebasis.pdf} +% \caption{Radius of convergence $R_{\text{CV}}$ in the CSF basis with $K$ basis functions for the MP (left) and WC (right) partitioning.} +% \label{fig:RadiusBasis} +%\end{figure} +% +%\begin{table*} +%\caption{Dominant singularity in the CSF basis set ($K=8$) for various value of $R$ in the MP and WC partitioning.} +%\begin{ruledtabular} +%\begin{tabular}{cccccccc} +%$R$ & 0.1 & 1 & 2 & 3 & 5 & 10 & 100 \\ +%\hline +%MP & $+14.1-10.9\,i$ & $+2.38-1.47\,i$ & $-0.67-1.30\,i$ & $-0.49-0.89\,i$ & $-0.33-0.55\,i$ & $-0.22-0.31\,i$ & $+0.03-0.05\,i$ \\ +%WC & $-9.6-10.7\,i$ & $-0.96-1.07\,i$ & $-0.48-0.53\,i$ & $-0.32-0.36\,i$ & $-0.19-0.21\,i$ & $-0.10-0.11\,i$ & $-0.01-0.01\,i$ \\ +%\end{tabular} +%\end{ruledtabular} +%\label{tab:SingAlpha} +%\end{table*} +% +%\subsection{Exceptional points in the UHF formalism}\label{sec:uhfSing} +% +%Now, we investigate the differences in the singularity structure between the RHF and UHF formalism. To do so, we use the symmetry-broken orbitals discussed in Sec.~\ref{sec:spherium}. Thus, the UHF two-electron basis is +%\begin{align}\label{eq:uhfbasis} +% \psi_1 & =\phi_{\alpha,1}(\theta_1)\phi_{\beta,1}(\theta_2), +% & +% \psi_2 & =\phi_{\alpha,1}(\theta_1)\phi_{\beta,2}(\theta_2),\\ +% \psi_3 & =\phi_{\alpha,2}(\theta_1)\phi_{\beta,1}(\theta_2), +% & +% \psi_4 & =\phi_{\alpha,2}(\theta_1)\phi_{\beta,2}(\theta_2). +%\end{align} +%with the symmetry-broken orbitals +%\begin{subequations} +%\begin{align}\label{eq:uhforbitals} +% \phi_{\alpha,1}(\theta) +% & =\frac{\sqrt{75+62R}}{4\sqrt{7R}} Y_{0}(\theta) +% + \frac{5\sqrt{-3+2R}}{4\sqrt{7R}} Y_{1}(\theta), +% \\ +% \phi_{\beta,1}(\theta) +% & =\frac{\sqrt{75+62R}}{4\sqrt{7R}} Y_{0}(\theta) +% - \frac{5\sqrt{-3+2R}}{4\sqrt{7R}} Y_{1}(\theta), +% \\ +% \phi_{\alpha,2}(\theta) +% & = - \frac{5\sqrt{-3+2R}}{4\sqrt{7R}} Y_{0}(\theta) +% + \frac{\sqrt{75+62R}}{4\sqrt{7R}} Y_{1}(\theta), +% \\ +% \phi_{\beta,2}(\theta) +% & =\frac{5\sqrt{-3+2R}}{4\sqrt{7R}} Y_{0}(\theta) +% +\frac{\sqrt{75+62R}}{4\sqrt{7R}} Y_{1}(\theta). +%\end{align} +%\end{subequations} +% +%In the UHF formalism the Hamiltonian $\hH(\lambda)$ is no more block diagonal, $\psi_4$ can interact with $\psi_2$ and $\psi_3$. The matrix elements of the Hamiltonian corresponding to this interaction are +%\begin{equation}\label{eq:MatrixElem} +% H_{24}=H_{34}=H_{42}=H_{43}=\sqrt{R-\frac{3}{2}}\sqrt{R+\frac{75}{62}}\qty(R+\frac{25}{2})\frac{\sqrt{31}}{70R^3} +%\end{equation} +% +%For $R=3/2$ the Hamiltonian is block diagonal because the matrix elements \eqref{eq:MatrixElem} are equal to zero so this is equivalent to the RHF case but for $R>3/2$ the matrix elements become real. This interaction corresponds to the spin contamination of the wave function. For $R<3/2$ the matrix elements are complex, this corresponds to the holomorphic solution of Fig.~\ref{fig:SpheriumNrj}, the singularities in this case will be treated later. The matrix elements become real again for $R<-75/62$, this corresponds to the sb-UHF solution for negative value of $R$ observed in Sec.~\ref{sec:spherium}. We will refer to the domain where the matrix elements are complex as the holomorphic domain. +% +%The singularity structure in this case is more complex because of the spin contamination of the wave function. We can not use CSFs in this case. So when one compute all the degeneracies using Eqs.~\eqref{eq:PolChar} and \eqref{eq:DPolChar} some correspond to EPs and some correspond to conical intersections. The numerical distinction of those singularities is very difficult. We will first look at the energies $E(\lambda)$ obtained with this basis set to attribute a physical signification to the singularities obtained numerically. +%Figure \ref{fig:UHFMiniBas} is the analog of Fig.~\ref{fig:RHFMiniBas} in the UHF formalism. We see that in this case the $sp_{z}$ triplet interacts with the $s^{2}$ and the $p_{z}^{2}$ singlets. Those avoided crossings are due to the spin contamination of the wave function. +% +%\begin{figure} +% \includegraphics[width=\linewidth]{EMP_UHF_R10.pdf} +% \caption{Energies $E(\lambda)$ in the unrestricted basis set \eqref{eq:uhfbasis} with $R=10$.} +% \label{fig:UHFMiniBas} +%\end{figure} +% +%Within the RHF formalism, we have observed only $\alpha$ singularities and large avoided crossings but one can see in Fig.~\ref{fig:UHFMiniBas} that in the UHF case there are sharp avoided crossings which are known to be connected to $\beta$ singularities. For example at $R=10$ the pair of singularities connected to the avoided crossing between $s^{2}$ and $sp_{z}$ $^{3}P$ is $0.999\pm0.014\,i$. And the one between $sp_{z}$ $^{3}P$ and $p_{z}^{2}$ is connected with the singularities $2.207\pm0.023\,i$. However, in spherium, the electrons cannot be ionized so those singularities cannot be the same $\beta$ singularities as the ones highlighted by Sergeev and Goodson. \cite{Sergeev_2005} We can see in Fig.~\ref{fig:UHFEP} that the $s^{2}$ singlet and the $sp_{z}$ triplet states are degenerated for $R=3/2$. For $R>3/2$, it becomes an avoided crossing on the real axis and the degeneracies are $moved$ in the complex plane. The wave function is spin contaminated by $Y_1$ for $R>3/2$ this is why the $s^{2}$ singlet energy cannot cross the $sp_{z}$ triplet curves anymore. When $R$ increases this avoided crossing becomes sharper. As presented before $\beta$ singularities are linked to quantum phase transition so it seems that this singularity is linked to the spin symmetry breaking of the UHF wave function. The fact that a similar pair of $\beta$ singularities appears for $R<-75/62$ confirms this assumption. The sharp avoided crossing between $sp_{z}$ $^{3}P$ and $p_{z}^{2}$ is not present on Fig. \ref{fig:UHFEP}. The second pair of $\beta$ singularities resulting from this avoided crossing appears for $R\gtrsim 2.5$, this is probably due to an excited-state quantum phase transition but this still need to be investigated. +% +%\begin{figure} +% \includegraphics[width=0.45\textwidth]{UHFCI.pdf} +% \includegraphics[width=0.45\textwidth]{UHFEP.pdf} +% \caption{Energies $E(\lambda)$ in the unrestricted basis set \eqref{eq:uhfbasis} for $R=1.5$ (left) and $R=1.51$ (right).} +% \label{fig:UHFEP} +%\end{figure} +% +%As shown before, some matrix elements of the Hamiltonian become complex in the holomorphic domain. Therefore the Hamiltonian becomes non-Hermitian for these values of $R$. In Ref.~\onlinecite{Burton_2019a}, Burton \textit{et al.}~proved that for the \ce{H_2} molecule the unrestricted Hamiltonian is not \pt -symmetric in the holomorphic domain. An analog reasoning can be done with the spherium model to prove the same result. The \pt -symmetry (invariance with respect to combined space reflection $\mathcal{P}$ and time reversal $\mathcal{T}$) is a property which ensures that a non-Hermitian Hamiltonian has a real energy spectrum. \cite{BenderPTBook} Thus \pt -symmetric Hamiltonians can be seen as an intermediate class between Hermitian and non-Hermitian Hamiltonians. +% +%Figure \ref{fig:UHFPT} shows that for the spherium model a part of the energy spectrum becomes complex when $R$ is in the holomorphic domain. The domain of values where the energy becomes complex is called the broken \pt-symmetry region. This is consistent with the fact that in the holomorphic domain the Hamiltonian is no more \pt -symmetric. +% +%For a non-Hermitian Hamiltonian the EPs can lie on the real axis. In particular, at the point of {\pt} transition (the point where the energies become complex) the two energies are degenerate resulting in such an EP on the real axis. This degeneracy can be seen in Fig.~\ref{fig:UHFPT}. +% +%\begin{figure}[h!] +% \includegraphics[width=0.45\textwidth]{ReNRJPT.pdf} +% \includegraphics[width=0.45\textwidth]{ImNRJPT.pdf} +% \caption{Real part (left) and imaginary part (right) of $E(\lambda)$ in the unrestricted basis set \eqref{eq:uhfbasis} for $R=1$.} +% \label{fig:UHFPT} +%\end{figure} \section{Conclusion} @@ -743,13 +719,13 @@ The $\beta$ singularities, which constitutes the second family, are artifacts ge These singularities are close to the real axis and connected with sharp avoided crossing between the ground state and a highly diffuse state. We have found that the $\beta$ singularities modeling the ionization phenomenon described by Sergeev and Goodson are actually part of a more general class of singularities. Indeed, those singularities close to the real axis are connected to quantum phase transition and symmetry breaking, and theoretical physics have demonstrated that the behavior of the EPs depends of the type of transitions from which the EPs result (first or higher orders, ground state or excited state transitions). -In this work, we have shown that $\beta$ singularities are involved in the spin symmetry breaking of the UHF wave function. -This confirms that $\beta$ singularities can occur for other types of transition and symmetry breaking than just the formation of a bound cluster of electrons. -It would be interesting to investigate the difference between the different type of symmetry breaking and how it affects the singularity structure. -Moreover the singularity structure in the non-Hermitian case still need to be investigated. -In the holomorphic domain, some singularities lie on the real axis and it would also be interesting to look at the differences between the different symmetry breaking and their respective holomorphic domain. -Furthermore, in this study we have used spherical harmonics (or combination of spherical harmonics) as basis functions which have a delocalized nature. It would also be interesting to investigate the use of localized basis functions \cite{Seidl_2018} (for example gaussians) because these functions would be more adapted to describe the strongly correlated regime. %More generally, to investigate the effect of the type of basis on the physics of EPs. -To conclude, this work shows that our understanding of the singularity structure of the energy is still incomplete but we hope that it opens new perspectives for the understanding of the physics of EPs in electronic structure theory. +%In this work, we have shown that $\beta$ singularities are involved in the spin symmetry breaking of the UHF wave function. +%This confirms that $\beta$ singularities can occur for other types of transition and symmetry breaking than just the formation of a bound cluster of electrons. +%It would be interesting to investigate the difference between the different type of symmetry breaking and how it affects the singularity structure. +%Moreover the singularity structure in the non-Hermitian case still need to be investigated. +%In the holomorphic domain, some singularities lie on the real axis and it would also be interesting to look at the differences between the different symmetry breaking and their respective holomorphic domain. +%Furthermore, in this study we have used spherical harmonics (or combination of spherical harmonics) as basis functions which have a delocalized nature. It would also be interesting to investigate the use of localized basis functions \cite{Seidl_2018} (for example gaussians) because these functions would be more adapted to describe the strongly correlated regime. %More generally, to investigate the effect of the type of basis on the physics of EPs. +%To conclude, this work shows that our understanding of the singularity structure of the energy is still incomplete but we hope that it opens new perspectives for the understanding of the physics of EPs in electronic structure theory. %%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%%% diff --git a/References/Altland_1997.pdf b/References/Altland_1997.pdf new file mode 100644 index 0000000..a1198e9 Binary files /dev/null and b/References/Altland_1997.pdf differ diff --git a/References/Anandan_1990.pdf b/References/Anandan_1990.pdf new file mode 100644 index 0000000..615ed46 Binary files /dev/null and b/References/Anandan_1990.pdf differ diff --git a/References/Baker_1971.pdf 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/DeviceRGB +/Filter /FlateDecode + +>> +stream +xwTSϽ7" %z ;HQIP&vDF)VdTG"cE b PQDE݌k 5ޚYg}׺PtX4X\XffGD=HƳ.d,P&s"7C$ +E6<~&S2)212 "įl+ɘ&Y4Pޚ%ᣌ\%g|eTI(L0_&l2E9r9hxgIbטifSb1+MxL 0oE%YmhYh~S=zU&ϞAYl/$ZUm@O ޜl^ ' lsk.+7oʿ9V;?#I3eE妧KD d9i,UQ h +A1vjpԁzN6p\W p G@ +K0ށiABZyCAP8C@&*CP=#t] 4}a ٰ;GDxJ>,_“@FXDBX$!k"EHqaYbVabJ0՘cVL6f3bձX'?v 6-V``[a;p~\2n5׌ &x*sb|! +ߏƿ' Zk! $l$T4QOt"y\b)AI&NI$R$)TIj"]&=&!:dGrY@^O$ _%?P(&OJEBN9J@y@yCR nXZOD}J}/G3ɭk{%Oחw_.'_!JQ@SVF=IEbbbb5Q%O@%!BӥyҸM:e0G7ӓ e%e[(R0`3R46i^)*n*|"fLUo՝mO0j&jajj.ϧwϝ_4갺zj=U45nɚ4ǴhZ ZZ^0Tf%9->ݫ=cXgN].[7A\SwBOK/X/_Q>QG[ `Aaac#*Z;8cq>[&IIMST`ϴ kh&45ǢYYF֠9<|y+ =X_,,S-,Y)YXmĚk]c}džjcΦ浭-v};]N"&1=xtv(}'{'IߝY) Σ -rqr.d._xpUەZM׍vm=+KGǔ ^WWbj>:>>>v}/avO8 +FV> 2 u/_$\BCv< 5 ]s.,4&yUx~xw-bEDCĻHGKwFGEGME{EEKX,YFZ ={$vrK +.3\rϮ_Yq*©L_wד+]eD]cIIIOAu_䩔)3ѩiB%a+]3='/40CiU@ёL(sYfLH$%Y jgGeQn~5f5wugv5k֮\۹Nw]m mHFˍenQQ`hBBQ-[lllfjۗ"^bO%ܒY}WwvwXbY^Ю]WVa[q`id2JjGէ{׿m>PkAma꺿g_DHGGu;776ƱqoC{P38!9 ҝˁ^r۽Ug9];}}_~imp㭎}]/}.{^=}^?z8hc' +O*?f`ϳgC/Oϩ+FFGGόzˌㅿ)ѫ~wgbk?Jި9mdwi獵ޫ?cǑOO?w| x&mf +endstream + +endobj +772 0 obj +[ /PDF ] +endobj +773 0 obj +<< +/Cs1 787 0 R + +>> + +endobj +774 0 obj +<< +/Gs1 788 0 R + +>> + +endobj +775 0 obj +<< +/Length 2612 +/N 3 +/Alternate /DeviceRGB +/Filter /FlateDecode + +>> +stream +xwTSϽ7" %z ;HQIP&vDF)VdTG"cE b PQDE݌k 5ޚYg}׺PtX4X\XffGD=HƳ.d,P&s"7C$ +E6<~&S2)212 "įl+ɘ&Y4Pޚ%ᣌ\%g|eTI(L0_&l2E9r9hxgIbטifSb1+MxL 0oE%YmhYh~S=zU&ϞAYl/$ZUm@O ޜl^ ' lsk.+7oʿ9V;?#I3eE妧KD d9i,UQ h +A1vjpԁzN6p\W p G@ +K0ށiABZyCAP8C@&*CP=#t] 4}a ٰ;GDxJ>,_“@FXDBX$!k"EHqaYbVabJ0՘cVL6f3bձX'?v 6-V``[a;p~\2n5׌ &x*sb|! +ߏƿ' Zk! $l$T4QOt"y\b)AI&NI$R$)TIj"]&=&!:dGrY@^O$ _%?P(&OJEBN9J@y@yCR nXZOD}J}/G3ɭk{%Oחw_.'_!JQ@SVF=IEbbbb5Q%O@%!BӥyҸM:e0G7ӓ e%e[(R0`3R46i^)*n*|"fLUo՝mO0j&jajj.ϧwϝ_4갺zj=U45nɚ4ǴhZ ZZ^0Tf%9->ݫ=cXgN].[7A\SwBOK/X/_Q>QG[ `Aaac#*Z;8cq>[&IIMST`ϴ kh&45ǢYYF֠9<|y+ =X_,,S-,Y)YXmĚk]c}džjcΦ浭-v};]N"&1=xtv(}'{'IߝY) Σ -rqr.d._xpUەZM׍vm=+KGǔ ^WWbj>:>>>v}/avO8 +FV> 2 u/_$\BCv< 5 ]s.,4&yUx~xw-bEDCĻHGKwFGEGME{EEKX,YFZ ={$vrK +.3\rϮ_Yq*©L_wד+]eD]cIIIOAu_䩔)3ѩiB%a+]3='/40CiU@ёL(sYfLH$%Y jgGeQn~5f5wugv5k֮\۹Nw]m mHFˍenQQ`hBBQ-[lllfjۗ"^bO%ܒY}WwvwXbY^Ю]WVa[q`id2JjGէ{׿m>PkAma꺿g_DHGGu;776ƱqoC{P38!9 ҝˁ^r۽Ug9];}}_~imp㭎}]/}.{^=}^?z8hc' +O*?f`ϳgC/Oϩ+FFGGόzˌㅿ)ѫ~wgbk?Jި9mdwi獵ޫ?cǑOO?w| x&mf +endstream + +endobj +776 0 obj +[ /PDF ] +endobj +777 0 obj +<< +/Cs1 789 0 R + +>> + +endobj +778 0 obj +<< +/Gs1 790 0 R + +>> + +endobj +779 0 obj +<< +/Length 2612 +/N 3 +/Alternate /DeviceRGB +/Filter /FlateDecode + +>> +stream +xwTSϽ7" %z ;HQIP&vDF)VdTG"cE b PQDE݌k 5ޚYg}׺PtX4X\XffGD=HƳ.d,P&s"7C$ +E6<~&S2)212 "įl+ɘ&Y4Pޚ%ᣌ\%g|eTI(L0_&l2E9r9hxgIbטifSb1+MxL 0oE%YmhYh~S=zU&ϞAYl/$ZUm@O ޜl^ ' lsk.+7oʿ9V;?#I3eE妧KD d9i,UQ h +A1vjpԁzN6p\W p G@ +K0ށiABZyCAP8C@&*CP=#t] 4}a ٰ;GDxJ>,_“@FXDBX$!k"EHqaYbVabJ0՘cVL6f3bձX'?v 6-V``[a;p~\2n5׌ &x*sb|! +ߏƿ' Zk! $l$T4QOt"y\b)AI&NI$R$)TIj"]&=&!:dGrY@^O$ _%?P(&OJEBN9J@y@yCR nXZOD}J}/G3ɭk{%Oחw_.'_!JQ@SVF=IEbbbb5Q%O@%!BӥyҸM:e0G7ӓ e%e[(R0`3R46i^)*n*|"fLUo՝mO0j&jajj.ϧwϝ_4갺zj=U45nɚ4ǴhZ ZZ^0Tf%9->ݫ=cXgN].[7A\SwBOK/X/_Q>QG[ `Aaac#*Z;8cq>[&IIMST`ϴ kh&45ǢYYF֠9<|y+ =X_,,S-,Y)YXmĚk]c}džjcΦ浭-v};]N"&1=xtv(}'{'IߝY) Σ -rqr.d._xpUەZM׍vm=+KGǔ ^WWbj>:>>>v}/avO8 +FV> 2 u/_$\BCv< 5 ]s.,4&yUx~xw-bEDCĻHGKwFGEGME{EEKX,YFZ ={$vrK +.3\rϮ_Yq*©L_wד+]eD]cIIIOAu_䩔)3ѩiB%a+]3='/40CiU@ёL(sYfLH$%Y jgGeQn~5f5wugv5k֮\۹Nw]m mHFˍenQQ`hBBQ-[lllfjۗ"^bO%ܒY}WwvwXbY^Ю]WVa[q`id2JjGէ{׿m>PkAma꺿g_DHGGu;776ƱqoC{P38!9 ҝˁ^r۽Ug9];}}_~imp㭎}]/}.{^=}^?z8hc' +O*?f`ϳgC/Oϩ+FFGGόzˌㅿ)ѫ~wgbk?Jި9mdwi獵ޫ?cǑOO?w| x&mf +endstream + +endobj +780 0 obj +[ /PDF ] +endobj +781 0 obj +<< +/Cs1 791 0 R + +>> + +endobj +782 0 obj +<< +/Gs1 792 0 R + +>> + +endobj +783 0 obj +<< +/Length 2612 +/N 3 +/Alternate /DeviceRGB +/Filter /FlateDecode + +>> +stream +xwTSϽ7" %z ;HQIP&vDF)VdTG"cE b PQDE݌k 5ޚYg}׺PtX4X\XffGD=HƳ.d,P&s"7C$ +E6<~&S2)212 "įl+ɘ&Y4Pޚ%ᣌ\%g|eTI(L0_&l2E9r9hxgIbטifSb1+MxL 0oE%YmhYh~S=zU&ϞAYl/$ZUm@O ޜl^ ' lsk.+7oʿ9V;?#I3eE妧KD d9i,UQ h +A1vjpԁzN6p\W p G@ +K0ށiABZyCAP8C@&*CP=#t] 4}a ٰ;GDxJ>,_“@FXDBX$!k"EHqaYbVabJ0՘cVL6f3bձX'?v 6-V``[a;p~\2n5׌ &x*sb|! +ߏƿ' Zk! $l$T4QOt"y\b)AI&NI$R$)TIj"]&=&!:dGrY@^O$ _%?P(&OJEBN9J@y@yCR nXZOD}J}/G3ɭk{%Oחw_.'_!JQ@SVF=IEbbbb5Q%O@%!BӥyҸM:e0G7ӓ e%e[(R0`3R46i^)*n*|"fLUo՝mO0j&jajj.ϧwϝ_4갺zj=U45nɚ4ǴhZ ZZ^0Tf%9->ݫ=cXgN].[7A\SwBOK/X/_Q>QG[ `Aaac#*Z;8cq>[&IIMST`ϴ kh&45ǢYYF֠9<|y+ =X_,,S-,Y)YXmĚk]c}džjcΦ浭-v};]N"&1=xtv(}'{'IߝY) Σ -rqr.d._xpUەZM׍vm=+KGǔ ^WWbj>:>>>v}/avO8 +FV> 2 u/_$\BCv< 5 ]s.,4&yUx~xw-bEDCĻHGKwFGEGME{EEKX,YFZ ={$vrK +.3\rϮ_Yq*©L_wד+]eD]cIIIOAu_䩔)3ѩiB%a+]3='/40CiU@ёL(sYfLH$%Y jgGeQn~5f5wugv5k֮\۹Nw]m mHFˍenQQ`hBBQ-[lllfjۗ"^bO%ܒY}WwvwXbY^Ю]WVa[q`id2JjGէ{׿m>PkAma꺿g_DHGGu;776ƱqoC{P38!9 ҝˁ^r۽Ug9];}}_~imp㭎}]/}.{^=}^?z8hc' +O*?f`ϳgC/Oϩ+FFGGόzˌㅿ)ѫ~wgbk?Jި9mdwi獵ޫ?cǑOO?w| x&mf +endstream + +endobj +784 0 obj +[ /PDF ] +endobj +785 0 obj +<< +/Cs1 793 0 R + +>> + +endobj +786 0 obj +<< +/Gs1 794 0 R + +>> + +endobj +787 0 obj +[ /ICCBased 795 0 R ] +endobj +788 0 obj +<< +/Type /ExtGState +/BM /Multiply + +>> + +endobj +789 0 obj +[ /ICCBased 796 0 R ] +endobj +790 0 obj +<< +/Type /ExtGState +/BM /Multiply + +>> + +endobj +791 0 obj +[ /ICCBased 797 0 R ] +endobj +792 0 obj +<< +/Type /ExtGState +/BM /Multiply + +>> + +endobj +793 0 obj +[ /ICCBased 798 0 R ] +endobj +794 0 obj +<< +/Type /ExtGState +/BM /Multiply + +>> + +endobj +795 0 obj +<< +/Length 2612 +/N 3 +/Alternate /DeviceRGB +/Filter /FlateDecode + +>> +stream +xwTSϽ7" %z ;HQIP&vDF)VdTG"cE b PQDE݌k 5ޚYg}׺PtX4X\XffGD=HƳ.d,P&s"7C$ +E6<~&S2)212 "įl+ɘ&Y4Pޚ%ᣌ\%g|eTI(L0_&l2E9r9hxgIbטifSb1+MxL 0oE%YmhYh~S=zU&ϞAYl/$ZUm@O ޜl^ ' lsk.+7oʿ9V;?#I3eE妧KD d9i,UQ h +A1vjpԁzN6p\W p G@ +K0ށiABZyCAP8C@&*CP=#t] 4}a ٰ;GDxJ>,_“@FXDBX$!k"EHqaYbVabJ0՘cVL6f3bձX'?v 6-V``[a;p~\2n5׌ &x*sb|! +ߏƿ' Zk! $l$T4QOt"y\b)AI&NI$R$)TIj"]&=&!:dGrY@^O$ _%?P(&OJEBN9J@y@yCR nXZOD}J}/G3ɭk{%Oחw_.'_!JQ@SVF=IEbbbb5Q%O@%!BӥyҸM:e0G7ӓ e%e[(R0`3R46i^)*n*|"fLUo՝mO0j&jajj.ϧwϝ_4갺zj=U45nɚ4ǴhZ ZZ^0Tf%9->ݫ=cXgN].[7A\SwBOK/X/_Q>QG[ `Aaac#*Z;8cq>[&IIMST`ϴ kh&45ǢYYF֠9<|y+ =X_,,S-,Y)YXmĚk]c}džjcΦ浭-v};]N"&1=xtv(}'{'IߝY) Σ -rqr.d._xpUەZM׍vm=+KGǔ ^WWbj>:>>>v}/avO8 +FV> 2 u/_$\BCv< 5 ]s.,4&yUx~xw-bEDCĻHGKwFGEGME{EEKX,YFZ ={$vrK +.3\rϮ_Yq*©L_wד+]eD]cIIIOAu_䩔)3ѩiB%a+]3='/40CiU@ёL(sYfLH$%Y jgGeQn~5f5wugv5k֮\۹Nw]m mHFˍenQQ`hBBQ-[lllfjۗ"^bO%ܒY}WwvwXbY^Ю]WVa[q`id2JjGէ{׿m>PkAma꺿g_DHGGu;776ƱqoC{P38!9 ҝˁ^r۽Ug9];}}_~imp㭎}]/}.{^=}^?z8hc' +O*?f`ϳgC/Oϩ+FFGGόzˌㅿ)ѫ~wgbk?Jި9mdwi獵ޫ?cǑOO?w| x&mf +endstream + +endobj +796 0 obj +<< +/Length 2612 +/N 3 +/Alternate /DeviceRGB +/Filter /FlateDecode + +>> +stream +xwTSϽ7" %z ;HQIP&vDF)VdTG"cE b PQDE݌k 5ޚYg}׺PtX4X\XffGD=HƳ.d,P&s"7C$ +E6<~&S2)212 "įl+ɘ&Y4Pޚ%ᣌ\%g|eTI(L0_&l2E9r9hxgIbטifSb1+MxL 0oE%YmhYh~S=zU&ϞAYl/$ZUm@O ޜl^ ' lsk.+7oʿ9V;?#I3eE妧KD d9i,UQ h +A1vjpԁzN6p\W p G@ +K0ށiABZyCAP8C@&*CP=#t] 4}a ٰ;GDxJ>,_“@FXDBX$!k"EHqaYbVabJ0՘cVL6f3bձX'?v 6-V``[a;p~\2n5׌ &x*sb|! +ߏƿ' Zk! $l$T4QOt"y\b)AI&NI$R$)TIj"]&=&!:dGrY@^O$ _%?P(&OJEBN9J@y@yCR nXZOD}J}/G3ɭk{%Oחw_.'_!JQ@SVF=IEbbbb5Q%O@%!BӥyҸM:e0G7ӓ e%e[(R0`3R46i^)*n*|"fLUo՝mO0j&jajj.ϧwϝ_4갺zj=U45nɚ4ǴhZ ZZ^0Tf%9->ݫ=cXgN].[7A\SwBOK/X/_Q>QG[ `Aaac#*Z;8cq>[&IIMST`ϴ kh&45ǢYYF֠9<|y+ =X_,,S-,Y)YXmĚk]c}džjcΦ浭-v};]N"&1=xtv(}'{'IߝY) Σ -rqr.d._xpUەZM׍vm=+KGǔ ^WWbj>:>>>v}/avO8 +FV> 2 u/_$\BCv< 5 ]s.,4&yUx~xw-bEDCĻHGKwFGEGME{EEKX,YFZ ={$vrK +.3\rϮ_Yq*©L_wד+]eD]cIIIOAu_䩔)3ѩiB%a+]3='/40CiU@ёL(sYfLH$%Y jgGeQn~5f5wugv5k֮\۹Nw]m mHFˍenQQ`hBBQ-[lllfjۗ"^bO%ܒY}WwvwXbY^Ю]WVa[q`id2JjGէ{׿m>PkAma꺿g_DHGGu;776ƱqoC{P38!9 ҝˁ^r۽Ug9];}}_~imp㭎}]/}.{^=}^?z8hc' +O*?f`ϳgC/Oϩ+FFGGόzˌㅿ)ѫ~wgbk?Jި9mdwi獵ޫ?cǑOO?w| x&mf +endstream + +endobj +797 0 obj +<< +/Length 2612 +/N 3 +/Alternate /DeviceRGB +/Filter /FlateDecode + +>> +stream +xwTSϽ7" %z ;HQIP&vDF)VdTG"cE b PQDE݌k 5ޚYg}׺PtX4X\XffGD=HƳ.d,P&s"7C$ +E6<~&S2)212 "įl+ɘ&Y4Pޚ%ᣌ\%g|eTI(L0_&l2E9r9hxgIbטifSb1+MxL 0oE%YmhYh~S=zU&ϞAYl/$ZUm@O ޜl^ ' lsk.+7oʿ9V;?#I3eE妧KD d9i,UQ h +A1vjpԁzN6p\W p G@ +K0ށiABZyCAP8C@&*CP=#t] 4}a ٰ;GDxJ>,_“@FXDBX$!k"EHqaYbVabJ0՘cVL6f3bձX'?v 6-V``[a;p~\2n5׌ &x*sb|! +ߏƿ' Zk! $l$T4QOt"y\b)AI&NI$R$)TIj"]&=&!:dGrY@^O$ _%?P(&OJEBN9J@y@yCR nXZOD}J}/G3ɭk{%Oחw_.'_!JQ@SVF=IEbbbb5Q%O@%!BӥyҸM:e0G7ӓ e%e[(R0`3R46i^)*n*|"fLUo՝mO0j&jajj.ϧwϝ_4갺zj=U45nɚ4ǴhZ ZZ^0Tf%9->ݫ=cXgN].[7A\SwBOK/X/_Q>QG[ `Aaac#*Z;8cq>[&IIMST`ϴ kh&45ǢYYF֠9<|y+ =X_,,S-,Y)YXmĚk]c}džjcΦ浭-v};]N"&1=xtv(}'{'IߝY) Σ -rqr.d._xpUەZM׍vm=+KGǔ ^WWbj>:>>>v}/avO8 +FV> 2 u/_$\BCv< 5 ]s.,4&yUx~xw-bEDCĻHGKwFGEGME{EEKX,YFZ ={$vrK +.3\rϮ_Yq*©L_wד+]eD]cIIIOAu_䩔)3ѩiB%a+]3='/40CiU@ёL(sYfLH$%Y jgGeQn~5f5wugv5k֮\۹Nw]m mHFˍenQQ`hBBQ-[lllfjۗ"^bO%ܒY}WwvwXbY^Ю]WVa[q`id2JjGէ{׿m>PkAma꺿g_DHGGu;776ƱqoC{P38!9 ҝˁ^r۽Ug9];}}_~imp㭎}]/}.{^=}^?z8hc' +O*?f`ϳgC/Oϩ+FFGGόzˌㅿ)ѫ~wgbk?Jި9mdwi獵ޫ?cǑOO?w| x&mf +endstream + +endobj +798 0 obj +<< +/Length 2612 +/N 3 +/Alternate /DeviceRGB +/Filter /FlateDecode + +>> +stream +xwTSϽ7" %z ;HQIP&vDF)VdTG"cE b PQDE݌k 5ޚYg}׺PtX4X\XffGD=HƳ.d,P&s"7C$ +E6<~&S2)212 "įl+ɘ&Y4Pޚ%ᣌ\%g|eTI(L0_&l2E9r9hxgIbטifSb1+MxL 0oE%YmhYh~S=zU&ϞAYl/$ZUm@O ޜl^ ' lsk.+7oʿ9V;?#I3eE妧KD d9i,UQ h +A1vjpԁzN6p\W p G@ 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