Fast Real-Time Time-Dependent Density Functional Theory Calculations with the Parallel Transport Gauge

Jia, Weile; An, Dong; Wang, Lin -Wang; Lin, Lin

doi:10.1021/acs.jctc.8b00580

Title: Fast Real-Time Time-Dependent Density Functional Theory Calculations with the Parallel Transport Gauge

Journal Article · Tue Oct 23 00:00:00 EDT 2018 · Journal of Chemical Theory and Computation

DOI:https://doi.org/10.1021/acs.jctc.8b00580· OSTI ID:1543629

^[1]; An, Dong ^[1]; Wang, Lin -Wang ^[2];

^[3]

Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Real-time time-dependent density functional theory (RT-TDDFT) is known to be hindered by the very small time step (attosecond or smaller) needed in the numerical simulation, because of the fast oscillation of electron wave functions, which significantly limits its range of applicability for the study of ultrafast dynamics. In this paper, we demonstrate that such oscillation can be considerably reduced by optimizing the gauge choice using the parallel transport formalism. RT-TDDFT calculations can thus be significantly accelerated using a combination of the parallel transport gauge and implicit integrators, and the resulting scheme can be used to accelerate any electronic structure software that uses a Schrödinger representation. Here, using absorption spectrum, ultrashort laser pulse, and Ehrenfest dynamics calculations for example, we show that the new method can utilize a time step that is on the order of 10–100 attoseconds using a planewave basis set. Thanks to the significant increase of the size of the time step, we also demonstrate that the new method is more than 10 times faster, in terms of the wall clock time, when compared to the standard explicit fourth-order Runge–Kutta time integrator for silicon systems ranging from 32 to 1024 atoms.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR)

Grant/Contract Number:: AC02-05CH11231; SC0017867

OSTI ID:: 1543629

Journal Information:: Journal of Chemical Theory and Computation, Vol. 14, Issue 11; ISSN 1549-9618

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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Cited By (2)

Propagation of maximally localized Wannier functions in real-time TDDFT Yost, Dillon C.; Yao, Yi; Kanai, Yosuke The Journal of Chemical Physics, Vol. 150, Issue 19 https://doi.org/10.1063/1.5095631	journal	May 2019
Propagation of maximally localized Wannier functions in real-time TDDFT Yost, Dillon C.; Yao, Yi; Kanai, Yosuke arXiv https://doi.org/10.48550/arxiv.1903.05081	text	January 2019