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arXiv · 1701.02285

Exact single-electron approach to the dynamics of molecules in strong laser fields

Axel Schild·E. K. U. Gross
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Abstract

We present an exact single-electron picture that describes the correlated electron dynamics in strong laser fields. Our approach is based on the factorization of the electronic wavefunction as a product of a marginal and a conditional amplitude. The marginal amplitude, which depends only on one electronic coordinate and yields the exact one-electron density and current density, obeys a time-dependent Schrödinger equation with an effective time-dependent potential. The exact equations are used to derive an approximation that is a step towards a general and feasible ab-initio single-electron approximation for molecules. The derivation also challenges the usual interpretation of the single-active electron approximation. From the study of model systems, we find that the exact and approximate single-electron potentials for processes with negligible two-electron ionization lead to a qualitatively similar dynamics, but that the ionization barrier may be explicitly time-dependent.

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Axel Schild, E. K. U. Gross. 2017-01-09. Exact single-electron approach to the dynamics of molecules in strong laser fields. https://doi.org/10.1103/physrevlett.118.163202

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