Many-electron dynamics in laser-driven molecules: wavefunction theory vs. density functional theory.

Physical Chemistry Chemical Physics : PCCP
Florian BedurkePeter Saalfrank

Abstract

With recent experimental advances in laser-driven electron dynamics in polyatomic molecules, the need arises for their reliable theoretical modelling. Among efficient, yet fairly accurate methods for many-electron dynamics are Time-Dependent Configuration Interaction Singles (TD-CIS) (a Wave Function Theory (WFT) method), and Real-Time Time-Dependent Density Functional Theory (RT-TD-DFT), respectively. Here we compare TD-CIS combined with extended Atomic Orbital (AO) bases, TD-CIS/AO, with RT-TD-DFT in a grid representation of the Kohn-Sham orbitals, RT-TD-DFT/Grid. Possible ionization losses are treated by complex absorbing potentials in energy space (for TD-CIS/AO) or real space (for RT-TD-DFT), respectively. The comparison is made for two test cases: (i) state-to-state transitions using resonant lasers (π-pulses), i.e., bound electron motion, and (ii) large-amplitude electron motion leading to High Harmonic Generation (HHG). Test systems are a H2 molecule and cis- and trans-1,2-dichlorethene, C2H2Cl2, (DCE). From time-dependent electronic energies, dipole moments and from HHG spectra, the following observations are made: first, for bound state-to-state transitions enforced by π-pulses, TD-CIS nicely accounts for the expected...Continue Reading

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Citations

Nov 4, 2021·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Emanuele Coccia, Eleonora Luppi

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Software Mentioned

RT
DFT
Octopus
WFT
AO
CIS
Grid
TD

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