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Theoretical analysis reveals excitation density impacts collective dynamics in molecular systems.
Theoretical descriptions of collective light–matter dynamics often rely on the mean-field (MF) or single-excitation (SE) approximation, yet the parameter regimes where they apply are rarely clearly delineated. Here we show that representative limiting regimes are characterized by two independent parameters: the number of molecules ( N ) and the excitation number ( N exc ). In the Tavis–Cummings model, when N ≫ 1 and the excitation density ( N exc / N ) goes to 0, the MF and SE descriptions agree and yield linear collective dynamics, showing harmonic Rabi oscillations. At finite excitation density ( N exc / N ∼ O ( 1 ) ), the large- N limit remains accurately described by MF dynamics but becomes nonlinear in N exc / N, manifested by a Duffing equation for the cavity amplitude with anharmonic Rabi frequency. We further use cluster expansion to examine finite- N correlations beyond MF. When local vibronic interactions are included, the same linear collective limit is reached by both approximations, with SE reaching it through polaron decoupling and MF through linearization. This two-parameter regime map clarifies the limits in which different theoretical descriptions provide valid descriptions of collective light–matter dynamics.
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Ying et al. (2026) studied this question.
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