CUT-E as a 1/<i>N</i> expansion for multiscale molecular polariton dynamics

J Juan B. Pérez-Sánchez (Department of Chemistry, University of California San Diego , La Jolla, California 92093,) A Arghadip Koner (Department of Chemistry and Biochemistry) S Sricharan Raghavan-Chitra (Department of Chemistry, University of California San Diego , La Jolla, California 92093,) J Joel Yuen-Zhou (Department of Chemistry and Biochemistry)

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.

Article Details

Volume / Issue Vol. 162, Issue 6
Published February 14, 2025
ISSN 0021-9606
Publisher American Institute of Physics

Journal Info

The Journal of Chemical Physics

American Institute of Physics

ISSN: 0021-9606 Physical Sciences

Authors (4)

J

Juan B. Pérez-Sánchez

Department of Chemistry, University of California San Diego , La Jolla, California 92093,

A

Arghadip Koner

Department of Chemistry and Biochemistry

S

Sricharan Raghavan-Chitra

Department of Chemistry, University of California San Diego , La Jolla, California 92093,

J

Joel Yuen-Zhou

Department of Chemistry and Biochemistry