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 polarised Fock states of light. We derive a master
equation for these systems by employing an optical polaron transformation that
captures the photon mode polarisation 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 optimise 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.
- Optical polaron formation in quantum systems with permanent dipoles
- Adam BurgessMarian FlorescuDominic Michael Rouse
- DS-2017-079, Leverhulme Trust (United Kingdom, London)EP/M008576/1, Engineering and Physical Sciences Research Council (United Kingdom, Swindon) - EPSRCEP/M027791/1, Engineering and Physical Sciences Research Council (United Kingdom, Swindon) - EPSRCEP/T517896/1, Engineering and Physical Sciences Research Council (United Kingdom, Swindon) - EPSRC
- We would like to thank the Tempo Collaboration for use of the open-source code Oqupy [53]. In particular, we thank Gerald Fux for extremely insightful conversations on the use of Oqupy. D.M.R. also thanks Ahsan Nazir and Owen Diba for helpful discussions. 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, and the EPSRC (United Kingdom) Strategic Equipment Grant No. EP/L02263X/1 (EP/M008576/1) and EPSRC (United Kingdom) Grant EP/M027791/1 awards to M.F. D.M.R. is supported by EPSRC (United Kingdom) Grant EP/T517896/1.
- 99783836302346
- School of Maths and Physics
- English
- Preprint