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Multilevel Purcell effect and the impact of vibrational modes in molecular quantum optics

Nation, Charlie; Notararigo, Valentina; Olaya-Castro, Alexandra; (2023) Multilevel Purcell effect and the impact of vibrational modes in molecular quantum optics. Physical Review A , 108 (6) , Article 063712. 10.1103/physreva.108.063712. Green open access

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Abstract

The increased decay rate of a two-level system weakly coupled to an optical cavity, known as the Purcell effect, is a cornerstone of cavity QED. However, the effect of cavity coupling is not well understood if the two-level system is replaced by a multilevel interacting system. Motivated by experiments looking to characterize molecular systems via exploiting a cavity interaction, we study a manifestation of the Purcell effect in a bio-inspired photosynthetic dimer. We focus in particular on how molecular vibrational modes, thought to play an important role in photosynthetic exciton transport, impact the system-cavity behavior in the Purcell regime. We provide a theoretical picture in terms of an effective non-Hermitian Hamiltonian, which extends the simple picture of a Jaynes-Cummings model to the description of a “multilevel” Purcell effect, where different levels have differing Purcell factors, with effective cooperativities mediated by coherent vibrational interactions.

Type: Article
Title: Multilevel Purcell effect and the impact of vibrational modes in molecular quantum optics
Open access status: An open access version is available from UCL Discovery
DOI: 10.1103/physreva.108.063712
Publisher version: http://dx.doi.org/10.1103/physreva.108.063712
Language: English
Additional information: This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third-party material in this article are included in the Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy
URI: https://discovery-pp.ucl.ac.uk/id/eprint/10185024
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