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arXiv · 2601.03863

Two-Mode Floquet Fewest Switches Surface Hopping for Nonadiabatic Dynamics Driven by Two-Frequency Laser Fields

Jiayue Han·Vahid Mosallanejad·Ruihao Bi·Wenjie Dou
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Abstract

Two-frequency (two-color) laser fields provide a powerful and flexible means for steering molecular dynamics. However, quantitatively reliable and scalable theoretical tools for simulating laser-driven nonadiabatic processes under such fields remain limited. Here, we develop a two-mode Floquet fewest switches surface hopping (two-mode F-FSSH) approach for two-frequency driving within a mixed quantum-classical framework. We validate the algorithm on three driven one-dimensional two-state models: a Rabi model and two avoided-crossing scattering models. The electronic and nuclear dynamics are benchmarked against numerically exact results from split-operator calculations, showing good agreement across a broad range of field parameters and initial conditions. These results establish two-mode F-FSSH as a practical framework for simulating and designing two-frequency control protocols and motivate extensions to more realistic experimental settings.

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Jiayue Han, Vahid Mosallanejad, Ruihao Bi, Wenjie Dou. 2026-01-07. Two-Mode Floquet Fewest Switches Surface Hopping for Nonadiabatic Dynamics Driven by Two-Frequency Laser Fields. https://arxiv.org/abs/2601.03863

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