Related papers: Permutationally symmetric molecular aggregates

Permutationally symmetric molecular aggregates

URL: http://arxiv.org/abs/2604.12395v1
Date: Tue, 14 Apr 2026 07:32:00 GMT
Title: Permutationally symmetric molecular aggregates
Abstract summary: Linear optical spectra of molecular aggregates are often approximated by classical optics methods.<n>We show that a $1/N$ expansion corrects the classical optics limit with finite $N$ corrections to the linear response of the aggregate.<n>Our findings clarify how quantum optical features that go beyond classical optics can already be present in simple arrays of quantum emitters.
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License: http://creativecommons.org/licenses/by/4.0/
Abstract: Linear optical spectra of molecular aggregates are often approximated by classical optics methods such as the discrete-dipole approximation (DDA), coherent exciton scattering (CES), and coherent potential approximation (CPA), where the only quantum-mechanical input to the calculation is the linear susceptibility of the monomers. However, the limits of validity of these classical optics methods remain opaque. Here, starting from a quantum mechanical Hamiltonian for the aggregate, we identify a limit where DDA/CPA/CES is exact: all-to-all coupled permutationally symmetric aggregates of $N \to \infty$ monomers. The permutational symmetry of this molecular version of the Lipkin-Meshkov-Glick model, which is closely related to that of the molecular polariton problem of many identical molecules coupled to a single-cavity mode, allows us to borrow recent techniques developed for the latter. In particular, we identify a $1/N$ expansion that corrects the classical optics limit with finite $N$ corrections to the linear response of the aggregate. These corrections feature as Raman-like transitions of a single monomer. We illustrate these findings with calculations on the very physically-relevant setup of a homodimer. Our findings clarify how quantum optical features that go beyond classical optics can already be present in simple arrays of quantum emitters such as molecular aggregates.

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