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This paper proposes a method
to simulate nonadiabatic dynamics initiated by thermal light, including solar
radiation, in the frame of mixed quantum-classical (MQC) methods, like surface
hopping. The method is based on the Chenu-Brumer approach, which treats the
thermal radiation as an ensemble of coherent pulses. It is composed of three
steps, 1) sampling initial conditions from a broad blackbody spectrum, 2) dynamics
propagation using conventional methods, and 3) ensemble averaging considering
the field and realization time of the pulses. The application of MQC dynamics with
pulse ensemble (MQC-PE) to a model system of nucleic acid photophysics showed the
emergence of a steady excited-state population. In another test case, modeling
retinal photophysics, MQC-PE predicted that although the photoisomerization
occurs within 200 fs, it may take tens of microseconds of continuous solar
irradiation to photoactivate a single retinal. Such emergent long timescales
may impact our understanding of biological and technological phenomena
occurring under solar radiation.
Version 5: Fix typos and minor changes in style and orthography.
Version 4: Fix typos and minor changes in style and orthography. New funding source added.
Version 3: Table 1 added.
Version 2: New notes added to SI.