Extracting accurate light–matter couplings from disordered polaritons

Author:

Schwennicke Kai1,Giebink Noel C.2ORCID,Yuen-Zhou Joel1ORCID

Affiliation:

1. Department of Chemistry and Biochemistry , 8784 University of California San Diego , La Jolla , CA 92093 , USA

2. Department of Electrical Engineering and Computer Science, and Physics , 1259 University of Michigan , Ann Arbor , MI 48109 , USA

Abstract

Abstract The vacuum Rabi splitting (VRS) in molecular polaritons stands as a fundamental measure of collective light–matter coupling. Despite its significance, the impact of molecular disorder on VRS is not fully understood yet. This study delves into the complexities of VRS amidst various distributions and degrees of disorder. Our analysis provides precise analytical expressions for linear absorption, transmission, and reflection spectra, along with a “sum” rule, offering a straightforward protocol for extracting accurate collective light–matter coupling values from experimental data. Importantly, our study cautions against directly translating large VRS to the onset of ultrastrong coupling regime. Furthermore, for rectangular disorder, we witness the emergence of narrow side bands alongside a broad central peak, indicating an extended coherence lifetime even in the presence of substantial disorder. These findings not only enhance our understanding of VRS in disordered molecular systems but also open avenues for achieving prolonged coherence lifetimes between the cavity and molecules via the interplay of collective coupling and disorder.

Funder

Air Force Office of Scientific Research

Publisher

Walter de Gruyter GmbH

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