Exact solution of polaritonic systems with arbitrary light and matter frequency-dependent losses
Exact solution of polaritonic systems with arbitrary light and matter frequency-dependent losses
In this paper, we perform the exact diagonalization of a light–matter strongly coupled system taking into account arbitrary losses via both energy dissipation in the optically active material and photon escape out of the resonator. This allows us to naturally treat the cases of couplings with structured reservoirs, which can strongly impact the polaritonic response via frequency-dependent losses or discrete-to-continuum strong coupling. We discuss the emergent gauge freedom of the resulting theory and provide analytical expressions for all the gauge-invariant observables in both the Power–Zienau–Woolley and the Coulomb representations. In order to exemplify the results, the theory is finally specialized to two specific cases. In the first one, both light and matter resonances are characterized by Lorentzian linewidths, and in the second one, a fixed absorption band is also present. The analytical expressions derived in this paper can be used to predict, fit, and interpret results from polaritonic experiments with arbitrary values of the light–matter coupling and with losses of arbitrary intensity and spectral shape in both the light and matter channels. A Matlab code implementing our results is provided.
Cortese, Erika
3a7d67d1-3321-40b2-91fa-2471dbed7147
De Liberato, Simone
5942e45f-3115-4027-8653-a82667ed8473
28 February 2022
Cortese, Erika
3a7d67d1-3321-40b2-91fa-2471dbed7147
De Liberato, Simone
5942e45f-3115-4027-8653-a82667ed8473
Cortese, Erika and De Liberato, Simone
(2022)
Exact solution of polaritonic systems with arbitrary light and matter frequency-dependent losses.
The Journal of Chemical Physics, 156 (8), [084106].
(doi:10.1063/5.0077950).
Abstract
In this paper, we perform the exact diagonalization of a light–matter strongly coupled system taking into account arbitrary losses via both energy dissipation in the optically active material and photon escape out of the resonator. This allows us to naturally treat the cases of couplings with structured reservoirs, which can strongly impact the polaritonic response via frequency-dependent losses or discrete-to-continuum strong coupling. We discuss the emergent gauge freedom of the resulting theory and provide analytical expressions for all the gauge-invariant observables in both the Power–Zienau–Woolley and the Coulomb representations. In order to exemplify the results, the theory is finally specialized to two specific cases. In the first one, both light and matter resonances are characterized by Lorentzian linewidths, and in the second one, a fixed absorption band is also present. The analytical expressions derived in this paper can be used to predict, fit, and interpret results from polaritonic experiments with arbitrary values of the light–matter coupling and with losses of arbitrary intensity and spectral shape in both the light and matter channels. A Matlab code implementing our results is provided.
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Accepted/In Press date: 31 January 2022
Published date: 28 February 2022
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Funding Information:
S.D.L. is a Royal Society Research Fellow and was partly funded by the Philip Leverhulme Prize of the Leverhulme Trust. The authors acknowledge funding from the RGF\EA\181001 grant from the Royal Society and the Leverhulme Trust under Grant No. RPG-2019-174.
Publisher Copyright:
© 2022 Author(s).
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Local EPrints ID: 472464
URI: http://eprints.soton.ac.uk/id/eprint/472464
ISSN: 0021-9606
PURE UUID: 1ac60943-9fea-496c-ae23-44d362fe4e9a
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Date deposited: 06 Dec 2022 17:34
Last modified: 06 Jun 2024 01:51
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