Linear response of molecular polaritons
- URL: http://arxiv.org/abs/2310.15424v1
- Date: Tue, 24 Oct 2023 00:41:20 GMT
- Title: Linear response of molecular polaritons
- Authors: Joel Yuen-Zhou and Arghadip Koner
- Abstract summary: We show that the collective light-matter strong coupling regime, where $N$ molecular emitters couple to the photon mode of an optical cavity, can be mapped to a quantum impurity model.
We derive simple analytical expressions for linear optical spectra (transmission, reflection, and absorption) where the only molecular input required is the molecular linear susceptibility.
This formalism is applied to a series of illustrative examples showcasing the role of temperature, disorder, vibronic coupling, and optical saturation of the molecular ensemble.
- Score: 0.0
- License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
- Abstract: In this article, we show that the collective light-matter strong coupling
regime, where $N$ molecular emitters couple to the photon mode of an optical
cavity, can be mapped to a quantum impurity model where the photon is the
impurity that is coupled to a bath of anharmonic transitions. In the
thermodynamic limit where $N\gg1$, we argue that the bath can be replaced with
an effective harmonic bath, leading to a dramatic simplification of the problem
into one of coupled harmonic oscillators. We derive simple analytical
expressions for linear optical spectra (transmission, reflection, and
absorption) where the only molecular input required is the molecular linear
susceptibility. This formalism is applied to a series of illustrative examples
showcasing the role of temperature, disorder, vibronic coupling, and optical
saturation of the molecular ensemble, explaining that it is useful even when
describing an important class of nonlinear optical experiments. For
completeness, we provide a comprehensive Appendix that includes a
self-contained derivation of the relevant spectroscopic observables for
arbitrary anharmonic systems (for both large and small $N$) within the
rotating-wave approximation. While some of the presented results herein have
already been reported in the literature, we provide a unified presentation of
the results as well as new interpretations that connect powerful concepts in
open quantum systems and linear response theory with molecular polaritonics.
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