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AVS Quantum Science

Strong coupling dynamics of driven quantum systems with permanent dipoles

Adam Burgess, Marian Florescu A, Dominic M. Rouse

Published Sep 1, 2023• 6 citations
Publisher

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.

DOI
10.1116/5.0157714

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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.
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.
We investigate the dynamics of polar systems coupled to classical external beams in the ultrastrong coupling regime. The permanent dipole moments (PDMs) sustained by polar systems can couple to the electromagnetic field, giving rise to a variety of processes such as difference frequency and harmonic generation, reflected in the complicated dynamics of the atomic system. Here, we demonstrate that the atomic evolution can be described simply in a dynamic reference frame. We derive a Jaynes-Cummings-like framework with effective parameters describing the frequency shift, coupling strength with the driving field, and a rescaled relaxation rate. The familiar linear scaling of the interaction strength with the field amplitude is replaced with a nonlinear dependence, suggesting potential applications for improving the coherence of quantum system ensembles with permanent dipoles.
We investigate spontaneous radiative processes in a driven polar two-level system whose interaction with the laser field is dominated by broken inversion symmetry rather than by the usual transition dipole coupling. Using a polaron transformation, we derive the dressed eigenstates of the atom-laser system and show that their longitudinal coupling reshapes the spectrum into two displaced harmonic ladders. We then analyze spontaneous transitions induced by a bosonic reservoir, and obtain transition rates that depend on both the laser parameters and the overlap between displaced field states. In the few-photon regime, we identify conditions under which spontaneous emission from the excited state can be strongly suppressed, thereby extending its lifetime, as well as regimes where the ladder structure enables spontaneous absorption from the ground state. In the semiclassical limit of a strong coherent drive, we derive compact analytical expressions for the total transition rates and show that they are governed by Bessel-function weights associated with multiphoton channels. Our results show how broken inversion symmetry qualitatively modifies decay dynamics and radiative cascades, and they establish driven polar quantum systems as a platform for controlling spontaneous light emission beyond the standard inversion-symmetric setting.
We present a new theoretical framework, polarized Fock states (PFSs), to describe the coupled molecule-cavity hybrid system in quantum electrodynamics. Through the quantum light-matter interactions under the dipole Gauge, the molecular permanent dipoles polarize the photon field by displacing the photonic coordinate. Hence, it is convenient to use these shifted Fock states (termed the PFSs) to describe light-matter interactions under the strong coupling regimes. These PFSs are nonorthogonal to each other and are light-matter entangled states. They allow an intuitive understanding of several phenomena that go beyond the prediction of the quantum Rabi model, while also offering numerical convenience to converge the results with much fewer states. With this powerful new theoretical framework, we explain how molecular permanent dipoles lead to the generation of multiple photons from a single electronic excitation (down-conversion), effectively achieving the dynamical Casimir effect through the nuclear vibration instead of cavity mirror oscillations.
We investigate the multiphoton quantum dynamics of a leaking single-mode quantized cavity field coupled with a resonantly driven two-level system possessing permanent dipoles. The frequencies of the interacting subsystems being considered are very different, e.g., the microwave range for the cavity and the optical domain for the frequency of the two-level emitter, respectively. In this way, the emitter couples to the resonator mode only via its diagonal dipole moments. Furthermore, the generalized Rabi frequency resulting from the external coherent driving of the two-level subsystem is also assumed to be different from the resonator's frequency or its multiples. As a consequence, this highly dispersive interaction regime is responsible for the cavity multiphoton quantum dynamics and photon conversion from the optical to microwave range, respectively.
The Rabi Hamiltonian, describing the interaction between a two-level atomic system and a single-cavity mode of the electromagnetic field, is one of the fundamental models in quantum optics. The model becomes exactly solvable by considering an atom without permanent dipole moments, whose excitation energy is quasiresonant with the cavity photon energy, and by neglecting the nonresonant (counter-rotating) terms. In this case, after including the decay of either the atom or the cavity mode to a continuum, one can derive the well-known phenomenology of quasiresonant transitions, including the fluorescence triplets. In this work we consider the most general Rabi model, incorporating the effects of permanent atomic electric dipole moments. Based on a perturbative analysis, we compare the intensities of emission lines induced by rotating terms, counter-rotating terms, and parity-symmetry-breaking terms in order to identify the parameter regimes in which these different contributions play a significant role. The analysis reveals that the emission strength related to the existence of permanent dipoles may surpass the one due to the counter-rotating interaction terms but is usually much weaker than the emission due to the main, resonant coupling. This ratio can be modified in systems with a reduced dimensionality or by engineering the energy spectral density of the continuum.