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Updated: Oct 22, 2025

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
Real-Time Exciton Dynamics with Time-Dependent Density-Functional Theory
Jiuyu Sun1,2, Cheng-Wei Lee3, Alina Kononov4
1Department of Physics and Astronomy, University of Missouri, Columbia, Missouri 65211, USA.
Abstract:
Linear-response time-dependent density-functional theory (TDDFT) can describe excitonic features in the optical spectra of insulators and semiconductors, using exchange-correlation (xc) kernels behaving as -1/k^{2} to leading order. We show how excitons can be modeled in real-time TDDFT, using an xc vector potential constructed from approximate, long-range corrected xc kernels. We demonstrate, for various materials, that this real-time approach is consistent with frequency-dependent linear response, gives access to femtosecond exciton dynamics following short-pulse excitations, and can be extended with some caution into the nonlinear regime.
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