From cb946fb56f8531cb75456726d0c12f7a445f6298 Mon Sep 17 00:00:00 2001 From: Pierre-Francois Loos Date: Mon, 7 Sep 2020 15:44:58 +0200 Subject: [PATCH] fig1 --- Manuscript/QUEST_WIREs.tex | 44 +++++++++++++++++----------------- Manuscript/fig1/fig1.pdf | Bin 0 -> 35600 bytes Manuscript/fig1/fig1.tex | 47 +++++++++++++++++++++++++++++++++++++ 3 files changed, 69 insertions(+), 22 deletions(-) create mode 100644 Manuscript/fig1/fig1.pdf create mode 100644 Manuscript/fig1/fig1.tex diff --git a/Manuscript/QUEST_WIREs.tex b/Manuscript/QUEST_WIREs.tex index 934edee..4d5de0e 100644 --- a/Manuscript/QUEST_WIREs.tex +++ b/Manuscript/QUEST_WIREs.tex @@ -126,7 +126,7 @@ In the same vein, we have also produced chemically-accurate theoretical 0-0 ener We refer the interested reader to Ref.~\cite{Loos_2019b} where we review the generic benchmark studies devoted to adiabatic and 0-0 energies performed in the last two decades. The QUEST dataset has the particularity to be based in a large proportion on selected configuration interaction (SCI) reference excitation energies as well as high-order CC methods such as CCSDT and CCSDTQ \cite{Oliphant_1991,Kucharski_1992}. -Recently, SCI methods have been a force to reckon with for the computation of highly-accurate energies in small- and medium-sized molecules as they yield near-FCI quality energies for only a fraction of the computational cost of a genuine FCI calculation \cite{Holmes_2017,Chien_2018,Loos_2018a,Li_2018,Loos_2019,Loos_2020b,Loos_2020c,Loos_2020a,Li_2020,Eriksen_2020,Loos_2020e,Yao_2020}. +Recently, SCI methods have been a force to reckon with for the computation of highly-accurate energies in small- and medium-sized molecules as they yield near full configuration interaction (FCI) quality energies for only a fraction of the computational cost of a genuine FCI calculation \cite{Holmes_2017,Chien_2018,Loos_2018a,Li_2018,Loos_2019,Loos_2020b,Loos_2020c,Loos_2020a,Li_2020,Eriksen_2020,Loos_2020e,Yao_2020}. Due to the fairly natural idea underlying SCI methods, the SCI family is composed by numerous members \cite{Bender_1969,Whitten_1969,Huron_1973,Abrams_2005,Bunge_2006,Bytautas_2009,Giner_2013,Caffarel_2014,Giner_2015,Garniron_2017b,Caffarel_2016a,Caffarel_2016b,Holmes_2016,Sharma_2017,Holmes_2017,Chien_2018,Scemama_2018,Scemama_2018b,Garniron_2018,Evangelista_2014,Schriber_2016,Schriber_2017,Liu_2016,Per_2017,Ohtsuka_2017,Zimmerman_2017,Li_2018,Ohtsuka_2017,Coe_2018,Loos_2019}. Their fundamental philosophy consists, roughly speaking, in retaining only the most energetically relevant determinants of the FCI space following a given criterion to avoid the exponential increase of the size of the CI expansion. Originally developed in the late 1960's by Bender and Davidson \cite{Bender_1969} as well as Whitten and Hackmeyer, \cite{Whitten_1969} new efficient SCI algorithms have resurfaced recently. @@ -158,14 +158,14 @@ Finally, we draw our conclusions in Sec.~\ref{sec:ccl} where we discuss, in part The molecules included in the QUEST dataset have been systematically optimized at the CC3/aug-cc-pVTZ level of theory, except for a very few cases. As shown in Refs.~\cite{Hattig_2005c,Budzak_2017}, CC3 provides extremely accurate ground- and excited-state geometries. These optimizations have been performed using DALTON 2017 \cite{dalton} and CFOUR 2.1, \cite{cfour} applying default parameters. -For the open-shell derivatives, the geometries are optimized at the UCCSD(T)/aug-cc-pVTZ level using the GAUSSIAN16 program \cite{Gaussian16} and applying the ``tight'' convergence threshold. -For the present review article, we have gathered all the geometries in the {\SupInf}. -\footnote{These geometries can be found at...} +For the open-shell derivatives \cite{Loos_2020c}, the geometries are optimized at the UCCSD(T)/aug-cc-pVTZ level using the GAUSSIAN16 program \cite{Gaussian16} and applying the ``tight'' convergence threshold. +%For the present review article, we have gathered all the geometries in the {\SupInf}. +%\footnote{These geometries can be found at...} %======================= \subsection{Basis sets} %======================= -For the entire set, we rely on one Pople basis set [6-31+G(d)], the augmented family of Dunning basis sets aug-cc-pVXZ (where X $=$ D, T, Q, and 5), and sometimes its doubly- and triply-augmented variants, d-aug-cc-pVXZ and t-aug-cc-pVXZ respectively. +For the entire set, we rely on the 6-31+G(d) Pople basis set, the augmented family of Dunning basis sets aug-cc-pVXZ (where X $=$ D, T, Q, and 5), and sometimes its doubly- and triply-augmented variants, d-aug-cc-pVXZ and t-aug-cc-pVXZ respectively. Doubly- and triply-augmented basis sets are usually employed for Rydberg states where it is not uncommon to observe a strong basis set dependence due to the very diffuse nature of these excited states. %================================== @@ -221,11 +221,11 @@ For the STEOM-CCSD calculations, it was checked that the active character percen When comparisons between various codes/implementations were possible, we could not detect variations in the transition energies larger than $0.01$ eV. For radicals, we applied both the U (unrestricted) and RO (restricted open-shell) versions of CCSD and CC3 as implemented in the PSI4 code \cite{Psi4} to perform our benchmarks. -State-averaged (SA) CASSCF and CASPT2 \cite{Roos,Andersson_1990} have been performed with MOLPRO (RS2 contraction level). \cite{molpro} -Concerning the NEVPT2 calculations, the partially-contracted (PC) and strongly-contracted (SC) variants have been systematically tested. \cite{Angeli_2001a, Angeli_2001b, Angeli_2002} +State-averaged (SA) CASSCF and CASPT2 \cite{Roos,Andersson_1990} have been performed with MOLPRO (RS2 contraction level) \cite{molpro}. +Concerning the NEVPT2 calculations, the partially-contracted (PC) and strongly-contracted (SC) variants have been tested \cite{Angeli_2001a,Angeli_2001b,Angeli_2002}. From a strict theoretical point of view, we point out that PC-NEVPT2 is supposed to be more accurate than SC-NEVPT2 given that it has a larger number of perturbers and greater flexibility. -When there is a strong mixing between states with same spin and spatial symmetries, we have also performed calculations with multi-state (MS) CASPT2 (MS-MR formalism), \cite{Finley_1998} and its extended variant (XMS-CASPT2). \cite{Shiozaki_2011} -Unless otherwise stated, all CASPT2 calculations have been performed with level shift and IPEA parameters set to the standard values of $0.3$ and $0.25$ a.u., respectively. +In the case of double excitations \cite{Loos_2019}, we have also performed calculations with multi-state (MS) CASPT2 (MS-MR formalism), \cite{Finley_1998} and its extended variant (XMS-CASPT2) \cite{Shiozaki_2011}, when there is a strong mixing between states with same spin and spatial symmetries. +The CASPT2 calculations have been performed with level shift and IPEA parameters set to the standard values of $0.3$ and $0.25$ a.u., respectively, unless otherwise stated. Large active spaces carefully chosen and tailored for the desired transitions have been selected. The definition of the active space considered for each system as well as the number of states in the state-averaged calculation is provided in their corresponding publication. @@ -243,7 +243,15 @@ The definition of the active space considered for each system as well as the num %======================= \subsection{Overview} %======================= -The QUEST database gathers more than \alert{470} highly-accurate excitation energies of various natures (valence, Rydberg, $n \ra \pis$, $\pi \ra \pis$, singlet, triplet, doublet, and double excitations) for molecules ranging from diatomics to ... +The QUEST database gathers more than \alert{470} highly-accurate excitation energies of various natures (valence, Rydberg, $n \ra \pis$, $\pi \ra \pis$, singlet, triplet, doublet, and double excitations) for molecules ranging from diatomics to molecules as large as naphthalene. +Each of the five subsets making up the QUEST dataset is detailed below. + +%%% FIGURE 1 %%% +\begin{figure}[bt] + \centering + \includegraphics[width=0.5\linewidth]{fig1/fig1} + \caption{Composition of each of the five subsets making up the present QUEST dataset of highly-accurate vertical excitation energies.} +\end{figure} %======================= \subsection{QUEST\#1} @@ -270,7 +278,7 @@ Nevertheless, these two methods were found to be more accurate for transition wi %======================= \subsection{QUEST\#3} %======================= -The QUEST\#3 benchmark set \cite{Loos_2020b} is, by far, our largest set, and consists of highly accurate vertical transition energies obtained for 27 molecules encompassing 4, 5, and 6 non-hydrogen atoms (acetone, acrolein, benzene, butadiene, cyanoacetylene, cyanoformaldehyde, cyanogen, cyclopentadiene, cyclopropenone, cyclopropenethione, diacetylene, furan, glyoxal, imidazole, isobutene, methylenecyclopropene, propynal, pyrazine, pyridazine, pyridine, pyrimidine, pyrrole, tetrazine, thioacetone, thiophene, thiopropynal, and triazine) for a total of 238 vertical transition energies and 90 oscillator strengths with a reasonably good balance between singlet, triplet, valence, and Rydberg excited states. +The QUEST\#3 benchmark set \cite{Loos_2020b} is, by far, our largest set, and consists of highly accurate vertical transition energies and oscillator strengths obtained for 27 molecules encompassing 4, 5, and 6 non-hydrogen atoms (acetone, acrolein, benzene, butadiene, cyanoacetylene, cyanoformaldehyde, cyanogen, cyclopentadiene, cyclopropenone, cyclopropenethione, diacetylene, furan, glyoxal, imidazole, isobutene, methylenecyclopropene, propynal, pyrazine, pyridazine, pyridine, pyrimidine, pyrrole, tetrazine, thioacetone, thiophene, thiopropynal, and triazine) for a total of 238 vertical transition energies and 90 oscillator strengths with a reasonably good balance between singlet, triplet, valence, and Rydberg excited states. For these 238 transitions, we have estimated that 224 are chemically accurate for the considered geometry. To define the TBEs of the QUEST\#3 set, we employed CC methods up to the highest technically possible order (CC3, CCSDT, and CCSDTQ), and, when affordable SCI calculations with very large reference spaces (up to hundred million determinants in certain cases), as well as the most reliable multiconfigurational method, NEVPT2, for double excitations. Most of our TBEs are based on CCSDTQ (4 non-hydrogen atoms) or CCSDT (5 and 6 non-hydrogen atoms) excitation energies. @@ -295,10 +303,9 @@ Likewise, the excitation energies obtained with CCSD are much less satisfying fo \subsection{QUEST\#5} %======================= -QUEST\#5 are additional accurate excitation energies that we have produced for the present article (aza-naphthalene, benzoquinone, cyclopentadienone, cyclopentadienethione, hexatriene, maleimide, naphthalene, nitroxyl, streptocyanine-C3, streptocyanine-C5, and thioacrolein). -The additional set is composed of small molecules as well as larger molecules. +The QUEST\#5 subset is composed by additional accurate excitation energies that we have produced for the present article. +This new set gathers small molecules as well as larger molecules (aza-naphthalene, benzoquinone, cyclopentadienone, cyclopentadienethione, hexatriene, maleimide, naphthalene, nitroxyl, streptocyanine-C3, streptocyanine-C5, and thioacrolein). QUEST\#5 does also provide additional FCI/6-31+G* estimates for the five- and six-membered rings considered in QUEST\#3. -\alert{add-on to other sets.} %-------------------------------------- \subsubsection{Toward larger molecules} @@ -484,13 +491,6 @@ Triazine & $^1A_1''(n \ra \pis)$ & 4.85 & 4.84 & 4.769(132) \\ %%%%%%%%%%%%%%%%%%%%%%%%%%%%% - -\begin{figure}[bt] - \centering - \includegraphics[width=0.5\linewidth]{example-image-rectangle} - \caption{This is the caption.} -\end{figure} - %%%%%%%%%%%%%%%%%%%%%%%%%%%%% \section{Benchmarks} \label{sec:bench} @@ -596,6 +596,6 @@ He is the author of more than 500 scientific papers. He has been ERC grantee (20 \newpage -\graphicalabstract{example-image-1x1}{Please check the journal's author guildines for whether a graphical abstract, key points, new findings, or other items are required for display in the Table of Contents.} +\graphicalabstract{fig1/fig1}{Composition of each of the five subsets making up the present QUEST dataset of highly-accurate vertical excitation energies.} \end{document} diff --git a/Manuscript/fig1/fig1.pdf b/Manuscript/fig1/fig1.pdf new file mode 100644 index 0000000000000000000000000000000000000000..6a15c36ab29f60a52ff23ac4d5bc1196daf1f976 GIT binary patch literal 35600 zcma&tQYNv&-tTZFkwWZFbpR=2Nz9+jh-66SF5`VxN3@wDJe!eUjIr zP!gA9U}5BdrI=kDT7~5%W+rwpwua^Bhh>s8v$t@yBxYgd<{|!n4lI+Tm949pGcl8- zt&yvlxS5HAsTr)GAgqh4vzd_{tjGFQ#)Lf{7kb!>7c3|Qtfxp=xVt?8Ib@@1acvU4 z+OOs%8J2Un^~bXh7jCvgX|{$+M!i868bnX-PocbM`Zb2+OLIyCOPF2?GD&q96AZGN zP|m^S@HHa%CVNe`Ka`3ld%d}I!(GSTE zOha2(XymURAA7IskZh$3TSa8xjyQM^CE#hb+V!WmyO8LkPE$-K41n{nIQ(Q{q~b$q 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(4*0.587785, 4*0.809017) {QUEST\#1 \\ \tiny small-sized molecules \\ \tiny \bf \red{JCTC 14 (2018) 4360}}; + \node [QUEST2, align=center] (Q2) at (4*0.951057, -4*0.309017) {QUEST\#2 \\ \tiny double excitations \\ \tiny \bf \red{JCTC 15 (2019) 1939}}; + \node [QUEST3, align=center] (Q3) at (4*0, -4*1.00000) {QUEST\#3 \\ \tiny medium-sized molecules \\ \tiny \bf \red{JCTC 16 (2020) 1711} }; + \node [QUEST4, align=center] (Q4) at (-4*0.951057,-4*0.309017) {QUEST\#4 \\ \tiny exotic molecules \& radicals \\ \tiny \bf \red{JCTC 16 (2020) 3720}}; + \node [QUEST5, align=center] (Q5) at (-4*0.587785, 4*0.809017) {QUEST\#5 \\ \tiny larger molecules \\ \tiny \bf \red{This study}}; + \path + (Q1) edge [->,color=black] node [above,sloped,black] {} (Q) + (Q2) edge [->,color=black] node [above,sloped,black] {} (Q) + (Q3) edge [->,color=black] node [above,sloped,black] {} (Q) + (Q4) edge [->,color=black] node [above,sloped,black] {} (Q) + (Q5) edge [->,color=black] node [above,sloped,black] {} (Q) + ; + \end{scope} +\end{tikzpicture} + +\end{document}