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The Bethe-Salpeter Equation Formalism: From Physics to Chemistry

By Xavier Blase, Ivan Duchemin, Denis Jacquemin and Pierre-Francois Loos

Abstract

13 pages, 3 figures, invited Perspective articleInternational audienceThe many-body Green's function Bethe-Salpeter equation (BSE) formalism is steadily asserting itself as a new efficient and accurate tool in the ensemble of computational methods available to chemists in order to predict optical excitations in molecular systems. In particular, the combination of the so-called $GW$ approximation of many-body perturbation theory, giving access to reliable ionization energies and electron affinities, and the BSE formalism, able to model UV/Vis spectra by catching excitonic effects, has shown to provide accurate singlet excitation energies in many chemical scenarios with a typical error of $0.1$--$0.3$ eV. With a similar computational cost as time-dependent density-functional theory (TD-DFT), the BSE formalism is able to provide an accuracy on par with the most accurate global and range-separated hybrid functionals without the unsettling choice of the exchange-correlation functional, resolving further known issues (e.g., charge-transfer excitations) and offering a well-defined path to dynamical kernels. In this \textit{Perspective} article, we provide a historical overview of the BSE formalism, with a particular focus on its condensed-matter roots. We also propose a critical review of its strengths and weaknesses in different chemical situations. Future directions of developments and improvements are also discussed

Topics: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry
Publisher: 'American Chemical Society (ACS)'
Year: 2020
DOI identifier: 10.1021/acs.jpclett.0c01875
OAI identifier: oai:HAL:hal-02873004v1
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