TY - JOUR
T1 - Real-Time Exciton Dynamics with Time-Dependent Density-Functional Theory
AU - Sun, Jiuyu
AU - Lee, Cheng Wei
AU - Kononov, Alina
AU - Schleife, André
AU - Ullrich, Carsten A.
N1 - Funding Information:
J. S. and C. A. U. acknowledge support by NSF Grant No. DMR-1810922, A. K. and A. S. acknowledge support by NSF Grant No. OAC-1740219, and C. W. L. and A. S. acknowledge support from the Office of Naval Research (Grant No. N00014-18-1-2605). This work used the high-performance computing infrastructure provided by Research Computing Support Services at the University of Missouri-Columbia, and the Illinois Campus Cluster, operated by the Illinois Campus Cluster Program (ICCP) in conjunction with the National Center for Supercomputing Applications (NCSA), supported by the University of Illinois at Urbana-Champaign.
Publisher Copyright:
© 2021 American Physical Society.
PY - 2021/8/13
Y1 - 2021/8/13
N2 - 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.
AB - 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.
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U2 - 10.1103/PhysRevLett.127.077401
DO - 10.1103/PhysRevLett.127.077401
M3 - Article
C2 - 34459649
AN - SCOPUS:85113168476
SN - 0031-9007
VL - 127
JO - Physical review letters
JF - Physical review letters
IS - 7
M1 - 077401
ER -