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The paper demonstrates that emitter-emitter interactions in quantum emitter arrays allow nonlinear optical susceptibilities of individual emitters to manifest in the array's linear response, even without cavities or permutational symmetry. They show that Raman features of individual monomers appear as vibrational sidebands in the collective resonances of coupled heterodimers and linear chains. By tuning Raman-type anharmonicities, the authors achieve systematic control of spectral features, revealing a quantum optical effect beyond mean-field approximations.
Quantum emitter arrays can exhibit nonlinear optical behavior in their linear spectra, opening new avenues for controlling light-matter interactions at the nanoscale.
Classical optical frameworks such as the discrete dipole approximation (DDA) assume that the linear spectrum of coupled quantum emitters can be computed solely from the linear susceptibilities of individual constituents. However, recent polariton studies show that cavity linear response can encode nonlinear optical susceptibilities. Here, we demonstrate that this phenomenon is more general: emitter-emitter interactions allow nonlinearities of individual emitters to emerge in the linear response of arrays, without cavities or permutational symmetry. To illustrate this phenomenon, we show linear spectra for coupled heterodimers and linear chains, and demonstrate that Raman features of individual monomers show up as vibrational sidebands of collective resonances. Moreover, tuning Raman-type anharmonicities enables systematic control of spectral features, establishing a genuine quantum optical effect in molecular aggregates and quantum emitter arrays, which goes beyond mean-field descriptions in light-matter interactions.
