42 lines
2.4 KiB
TeX
42 lines
2.4 KiB
TeX
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\documentclass[10pt]{letter}
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\usepackage{UPS_letterhead,xcolor,mhchem,mathpazo,ragged2e}
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\newcommand{\alert}[1]{\textcolor{red}{#1}}
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\definecolor{darkgreen}{HTML}{009900}
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\begin{document}
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\begin{letter}%
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{To the Editors of the Journal of Chemical Physics}
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\opening{Dear Editors,}
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\justifying
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Please find enclosed our manuscript entitled \textit{``Dynamical Kernels for Optical Excitations''}, which we would like you to consider as a Regular Article in the \textit{Journal of Chemical Physics}.
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This contribution fits nicely in the section \textit{``Theoretical Methods and Algorithms''}.
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This contribution has never been submitted in total nor in parts to any other journal, and has been seen and approved by all authors.
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In the present manuscript, we discuss, in a pedagogical way, the physics of dynamical (i.e., frequency-dependent) kernels for the computation of optical excitations within linear response theory.
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In particular, we consider three dynamical kernels, namely i) an a priori built kernel inspired by the dressed TD-DFT kernel of Maitra and coworkers, ii) the dynamical kernel stemming from the BSE formalism derived originally by Strinati, and iii) the second-order BSE kernel derived first by the group of Weitao Yang.
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The principal take-home message of the present paper is that dynamical kernels have much more to give that one would think.
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In more scientific terms, dynamical kernels can provide, thanks to their frequency-dependent nature, additional excitations that can be associated to higher-order excitations (such as the infamous double excitations).
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However, they sometimes give too much, and generate spurious excitations, i.e., excitation which does not corresponds to any physical excited state.
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Using a simple two-model system, prototypical examples of valence, charge-transfer, and Rydberg excitations are studied.
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From these, we have observed that, overall, the dynamical correction usually improves the static excitation energies, and that, if one has no interest in double excitations, a perturbative treatment is an excellent alternative to a non-linear resolution of the dynamical equations.
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We expect this work to be of interest to a wide audience within the chemistry and physics communities.
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We suggest Paola Gori-Giorgi, Neepa Maitra, Valerio Olevano, Patrick Rinke, Weitao Yang, Michael Rohlfing, and Lucia Reining as potential referees.
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We look forward to hearing from you soon.
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\closing{Sincerely, the authors.}
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\end{letter}
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\end{document}
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