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Semiclassical electrodynamics is an appealing approach for studyinglight-matter interactions, especially for realistic molecular systems. However,there is no unique semiclassical scheme. On the one hand, intermolecularinteractions can be described instantaneously by static two-body interactionsconnecting different molecules plus a classical transverse E-field; we willcall this Hamiltonian #I. On the other hand, intermolecular interactions canalso be described as effects that are mediated exclusively through a classicalone-body E-field without any quantum effects at all (assuming we ignoreelectronic exchange); we will call this Hamiltonian #II. Moreover, one can alsomix these two Hamiltonians into a third, hybrid Hamiltonian, which preservesquantum electron-electron correlations for lower excitations but describeshigher excitations in a mean-field way. To investigate which semiclassicalscheme is most reliable for practical use, here we study the real-time dynamicsof a pair of identical two-level systems (TLSs) undergoing either resonanceenergy transfer (RET) or collectively driven dynamics. While all approachesperform reasonably well when there is no strong external excitation, we findthat no single approach is perfect for all conditions. Each method has its owndistinct problems: Hamiltonian #I performs best for RET but behaves in acomplicated manner for driven dynamics. Hamiltonian #II is always stable, butobviously fails for RET at short distances. One key finding is that, underexternally driving, a full configuration interaction description of Hamiltonian#I strongly overestimates the long-time electronic energy, highlighting the notobvious fact that, if one plans to merge quantum molecules with classicallight, a full, exact treatment of electron-electron correlations can actuallylead to worse results than a simple mean-field treatment.

physical review. a/physical review, a

Understanding the Nature of Mean-Field Semiclassical Light-Matter  Dynamics: An Investigation of Energy Transfer, Electron-Electron  Correlations, External Driving and Long-Time Detailed Balance