Strong coupling dynamics of driven quantum systems with permanent dipoles

Burgess, A., Florescu, M. and Rouse, D. M. (2023) Strong coupling dynamics of driven quantum systems with permanent dipoles. AVS Quantum Science, 5(3), 031402. (doi: 10.1116/5.0157714)

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Abstract

Many optically active systems possess spatially asymmetric electron orbitals. These generate permanent dipole moments, which can be stronger than the corresponding transition dipole moments, significantly affecting the system dynamics and creating polarized Fock states of light. We derive a master equation for these systems with an externally applied driving field by employing an optical polaron transformation that captures the photon mode polarization induced by the permanent dipoles. This provides an intuitive framework to explore their influence on the system dynamics and emission spectrum. We find that permanent dipoles introduce multiple-photon processes and a photon sideband, which causes substantial modifications to single-photon transition dipole processes. In the presence of an external drive, permanent dipoles lead to an additional process that we show can be exploited to control the decoherence and transition rates. We derive the emission spectrum of the system, highlighting experimentally detectable signatures of optical polarons, and measurements that can identify the parameters in the system Hamiltonian, the magnitude of the differences in the permanent dipoles, and the steady-state populations of the system.

Item Type:Articles
Additional Information:The work by A.B. was supported by the Leverhulme Quantum Biology Doctoral Training Centre at the University of Surrey funded by a Leverhulme Trust training centre [grant number DS-2017-079]. The EPSRC Strategic Equipment [grant numbers EP/L02263X/1 (EP/M008576/1)] and EPSRC [grant numbers EP/M027791/1] awards to M.F. D.M.R. was supported by the EPSRC [grant number EP/T517896/1].
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Rouse, Dr Dominic
Creator Roles:
Rouse, D.Conceptualization, Data curation, Formal analysis, Funding acquisition, Investigation, Methodology, Project administration, Resources, Software, Supervision, Validation, Visualization, Writing – original draft, Writing – review and editing
Authors: Burgess, A., Florescu, M., and Rouse, D. M.
College/School:College of Science and Engineering
Journal Name:AVS Quantum Science
Publisher:American Institute of Physics
ISSN:2639-0213
ISSN (Online):2639-0213
Copyright Holders:Copyright: © 2023 The Author(s)
First Published:First published in AVS Quantum Science 5(3): 031402
Publisher Policy:Reproduced under a Creative Commons licence
Data DOI:10.5525/gla.researchdata.1437

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
312561EPSRC DTP 2020/21Christopher PearceEngineering and Physical Sciences Research Council (EPSRC)EP/T517896/1Research and Innovation Services