Semiclassical electrodynamics [with quantum molecules plus classical electromagnetic (EM) fields] is a powerful tool for studying light-matter interactions for realistic nanoscale systems, but there is no one unique semiclassical algorithm; instead, there are many possible methods. In particular, there are many ways to approximate the exact quantum-mechanical cancellation that one finds between the longitudinal EM field and the dipole-dipole interaction operator that leads to causality; this cancellation involves both classical and quantum operators and need not be preserved exactly (but rather only approximately). With this in mind, we have now studied resonance energy transfer (RET) between a pair of two-level systems (TLSs) using a range of different semiclassical methods in three dimensions. Hence, our work suggests that, so far, there is no perfect semiclassical Hamiltonian when propagating light-matter interactions: one must usually sacrifice either causality or short range electron-electron interactions. These conclusions should be very important for future electrodynamics simulations.

Semiclassical energy transfer: What is the right Hamiltonian?

2019 Fall National Meeting

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