Optical polaron formation in quantum systems with permanent dipoles

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 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.