Marek, Stepan and 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). pp. 9814-9822. ISSN 1549-9618, 1549-9626
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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.
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | BASIS-SETS; ELECTRONIC EXCITATIONS; GREENS-FUNCTION; EXCHANGE; GW; SPECTRA; HOLE; |
| Subjects: | 500 Science > 530 Physics 500 Science > 540 Chemistry & allied sciences |
| Divisions: | Physics > Institute of Theroretical Physics Regensburg Center for UltrafastNanoscopy (RUN) |
| Depositing User: | Dr. Gernot Deinzer |
| Date Deposited: | 07 May 2026 07:34 |
| Last Modified: | 07 May 2026 07:35 |
| URI: | https://pred.uni-regensburg.de/id/eprint/65777 |
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