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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| Dokumentenart | Artikel | ||||||
| Titel eines Journals oder einer Zeitschrift | Journal of Chemical Theory and Computation | ||||||
| Verlag: | American Chemical Society (ACS) | ||||||
|---|---|---|---|---|---|---|---|
| Band: | 21 | ||||||
| Nummer des Zeitschriftenheftes oder des Kapitels: | 19 | ||||||
| Seitenbereich: | S. 9814-9822 | ||||||
| Datum | 25 September 2025 | ||||||
| Institutionen | Physik > 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 |
| ||||||
| Stichwörter / Keywords | optical properties, real-time propagation, Bethe-Salpeter equation, DFT, laser pulse | ||||||
| Dewey-Dezimal-Klassifikation | 500 Naturwissenschaften und Mathematik > 530 Physik 500 Naturwissenschaften und Mathematik > 540 Chemie | ||||||
| Status | Veröffentlicht | ||||||
| Begutachtet | Ja, diese Version wurde begutachtet | ||||||
| An der Universität Regensburg entstanden | Ja | ||||||
| URN der UB Regensburg | urn:nbn:de:bvb:355-epub-779678 | ||||||
| Dokumenten-ID | 77967 |
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