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Updated: May 28, 2025

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
CUT-E as a 1/N expansion for multiscale molecular polariton dynamics
Juan B Pérez-Sánchez1, Arghadip Koner1, Sricharan Raghavan-Chitra1
1Department of Chemistry, University of California San Diego, La Jolla, California 92093, USA.
Abstract:
Molecular polaritons arise when the collective coupling between an ensemble of N molecules and an optical mode exceeds individual photon and molecular linewidths. The complexity of their description stems from their multiscale nature, where the local dynamics of each molecule can, in principle, be influenced by the collective behavior of the entire ensemble. To address this, we previously introduced a formalism called collective dynamics using truncated equations (CUT-E). CUT-E approaches the problem in two stages. First, it exploits permutational symmetries to obtain a substantial simplification of the problem. However, this is often insufficient for parameter regimes relevant to most experiments. Second, it takes the exact solution of the problem in the N → ∞ limit as a reference and derives systematic finite-N corrections. Here, we provide a novel derivation of CUT-E based on recently developed bosonization techniques. We lay down its connections with 1/N expansions that are ubiquitous in other fields of physics and present previously unexplored key aspects of this formalism, including various types of approximations and extensions to high-excitation manifolds.
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