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Marek, Štěpán ; Wilhelm, Jan

Linear and Nonlinear Optical Properties of Molecules from Real-Time Propagation Based on the Bethe–Salpeter Equation

Marek, Štěpán und Wilhelm, Jan (2025) Linear and Nonlinear Optical Properties of Molecules from Real-Time Propagation Based on the Bethe–Salpeter Equation. Journal of Chemical Theory and Computation 21 (19), S. 9814-9822.

Veröffentlichungsdatum dieses Volltextes: 15 Okt 2025 13:23
Artikel
DOI zum Zitieren dieses Dokuments: 10.5283/epub.77967


Zusammenfassung

We present a real-time propagation method for computing linear and nonlinear optical properties of molecules based on the Bethe–Salpeter equation. The method follows the time evolution of the one-particle density matrix under an external electric field. We include electron–electron interaction effects through a self-energy model based on the screened exchange approximation. Quasiparticle energies ...

We present a real-time propagation method for computing linear and nonlinear optical properties of molecules based on the Bethe–Salpeter equation. The method follows the time evolution of the one-particle density matrix under an external electric field. We include electron–electron interaction effects through a self-energy model based on the screened exchange approximation. Quasiparticle energies are taken from a prior GW calculation to construct the effective single-particle Hamiltonian, and we represent all operators and wave functions in an atom-centered Gaussian basis. We benchmark the accuracy of the real-time propagation against the standard linear-response Bethe–Salpeter equation by using a set of organic molecules. We find very good agreement when computing linear-response isotropic polarizability spectra from both approaches with a mean absolute deviation of 30 meV in peak positions. Beyond linear response, we simulate second harmonic generation and optical rectification in a noncentrosymmetric molecule. We foresee broad applicability of real-time propagation based on the Bethe–Salpeter equation for the study of linear and nonlinear optical properties of molecules, as the method has a computational cost similar to that of time-dependent density functional theory with hybrid functionals.



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Details

DokumentenartArtikel
Titel eines Journals oder einer ZeitschriftJournal of Chemical Theory and Computation
Verlag:American Chemical Society (ACS)
Band:21
Nummer des Zeitschriftenheftes oder des Kapitels:19
Seitenbereich:S. 9814-9822
Datum25 September 2025
InstitutionenPhysik > Institut für Theoretische Physik
Regensburg Center for Ultrafast Nanoscopy (RUN)
Projekte
Gefördert von: Deutsche Forschungsgemeinschaft (DFG) (503985532)
Gefördert von: Deutsche Forschungsgemeinschaft (DFG) (314695032)
Gefördert von: Deutsche Forschungsgemeinschaft (DFG) (5394206)
Gefördert von: Deutsche Forschungsgemeinschaft (DFG) (Nicht ausgewählt)
Identifikationsnummer
WertTyp
10.1021/acs.jctc.5c01246DOI
arXiv:2507.21279arXiv-ID
Stichwörter / Keywordsoptical properties, real-time propagation, Bethe-Salpeter equation, DFT, laser pulse
Dewey-Dezimal-Klassifikation500 Naturwissenschaften und Mathematik > 530 Physik
500 Naturwissenschaften und Mathematik > 540 Chemie
StatusVeröffentlicht
BegutachtetJa, diese Version wurde begutachtet
An der Universität Regensburg entstandenJa
URN der UB Regensburgurn:nbn:de:bvb:355-epub-779678
Dokumenten-ID77967

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