Issue 43, 2015

Laser-induced electron localization in H2+: mixed quantum-classical dynamics based on the exact time-dependent potential energy surface

Abstract

We study the exact nuclear time-dependent potential energy surface (TDPES) for laser-induced electron localization with a view to eventually developing a mixed quantum-classical dynamics method for strong-field processes. The TDPES is defined within the framework of the exact factorization [A. Abedi, N. T. Maitra, and E. K. U. Gross, Phys. Rev. Lett., 2010, 105, 123002] and contains the exact effect of the couplings to the electronic subsystem and to any external fields within a scalar potential. We compare its features with those of the quasistatic potential energy surfaces (QSPES) often used to analyse strong-field processes. We show that the gauge-independent component of the TDPES has a mean-field-like character very close to the density-weighted average of the QSPESs. Oscillations in this component are smoothened out by the gauge-dependent component, and both components are needed to yield the correct force on the nuclei. Once the localization begins to set in, the gradient of the exact TDPES tracks one QSPES and then switches to the other, similar to the description provided by surface-hopping between QSPESs. We show that evolving an ensemble of classical nuclear trajectories on the exact TDPES accurately reproduces the exact dynamics. This study suggests that the mixed quantum-classical dynamics scheme based on evolving multiple classical nuclear trajectories on the exact TDPES will be a novel and useful method to simulate strong field processes.

Graphical abstract: Laser-induced electron localization in H2+: mixed quantum-classical dynamics based on the exact time-dependent potential energy surface

Article information

Article type
Paper
Submitted
12 Jun 2015
Accepted
24 Sep 2015
First published
25 Sep 2015

Phys. Chem. Chem. Phys., 2015,17, 29271-29280

Author version available

Laser-induced electron localization in H2+: mixed quantum-classical dynamics based on the exact time-dependent potential energy surface

Y. Suzuki, A. Abedi, N. T. Maitra and E. K. U. Gross, Phys. Chem. Chem. Phys., 2015, 17, 29271 DOI: 10.1039/C5CP03418C

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