Real-Time Exciton Dynamics with Time-Dependent Density-Functional Theory

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/k2 to leading order. We show how excitons can be modeled in real-time TDDFT, using an xc ve...

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Bibliographic Details
Published in:Physical review letters 2021-08, Vol.127 (7), p.1-077401, Article 077401
Main Authors: Sun, Jiuyu, Lee, Cheng-Wei, Kononov, Alina, Schleife, André, Ullrich, Carsten A.
Format: Article
Language:English
Subjects:
Density functional theory
Excitons
Femtosecond pulses
Insulators
Kernels
Real time
Response time
Short pulses
Time dependence
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Summary: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/k2 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.
ISSN:0031-9007
1079-7114
DOI:10.1103/PhysRevLett.127.077401