Computational Benchmarking for Ultrafast Electron Dynamics: Wave Function Methods vs Density Functional Theory

Journal of Chemical Theory and Computation
Micael J T OliveiraMatthieu J Verstraete

Abstract

Attosecond electron dynamics in small- and medium-sized molecules, induced by an ultrashort strong optical pulse, is studied computationally for a frozen nuclear geometry. The importance of exchange and correlation effects on the nonequilibrium electron dynamics induced by the interaction of the molecule with the strong optical pulse is analyzed by comparing the solution of the time-dependent Schrödinger equation based on the correlated field-free stationary electronic states computed with the equationof-motion coupled cluster singles and doubles and the complete active space multi-configurational self-consistent field methodologies on one hand, and various functionals in real-time time-dependent density functional theory (TDDFT) on the other. We aim to evaluate the performance of the latter approach, which is very widely used for nonlinear absorption processes and whose computational cost has a more favorable scaling with the system size. We focus on LiH as a toy model for a nontrivial molecule and show that our conclusions carry over to larger molecules, exemplified by ABCU (C10H19N). The molecules are probed with IR and UV pulses whose intensities are not strong enough to significantly ionize the system. By comparing the evo...Continue Reading

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Citations

Aug 1, 2016·The Journal of Chemical Physics·Kai LuoNeepa T Maitra
Apr 3, 2016·The Journal of Chemical Physics·Koji Ando
Oct 13, 2018·Physical Chemistry Chemical Physics : PCCP·Johanna I FuksNeepa T Maitra
Jun 17, 2016·The Journal of Chemical Physics·Neepa T Maitra
Jan 31, 2020·Journal of Chemical Theory and Computation·Adrián Gómez PueyoAlberto Castro

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