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We investigate the polariton-mediated electron transfer reaction in a model system with analytic rate constant theory and direct quantum dynamical simulations. We demonstrate that the photoinduced charge transfer reaction between a bright donor state and dark acceptor state can be significantly enhanced or suppressed by coupling the molecular system to the quantized radiation field inside an optical cavity. This is because the quantum light–matter interaction can influence the effective driving force and electronic couplings between the donor state, which is the hybrid light–matter excitation, and the molecular acceptor state. Under the resonance condition between the photonic and electronic excitations, the effective driving force can be tuned by changing the light–matter coupling strength; for an off-resonant condition, the same effect can be accomplished by changing the molecule–cavity detuning. We further demonstrate that using both the electronic coupling and light–matter coupling helps to extend the effective couplings across the entire system, even for the dark state that carries a zero transition dipole. Theoretically, we find that both the counter-rotating terms and the dipole self-energy in the quantum electrodynamics Hamiltonian are important for obtaining an accurate polariton eigenspectrum as well as the polariton-mediated charge transfer rate constant, especially in the ultrastrong coupling regime.
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Dynamical generation and transfer of nonclassical states in strongly interacting light-matter systems in cavities
Abstract We propose leveraging strong and ultrastrong light-matter coupling to efficiently generate and exchange nonclassical light and quantum matter states. Two initial conditions are considered: (a) a displaced quadrature-squeezed matter state, and (b) a coherent state in a cavity. In both scenarios, polaritons mediate the dynamical generation and transfer of nonclassical states between light and matter. By monitoring the dynamics of both subsystems, we uncover the emergence of cavity-induced beatings in the collective matter oscillations. The beating period depends on the particle density through the vacuum Rabi splitting and peaks sharply under light-matter resonance conditions. For initial condition (a), nonclassicality is efficiently transferred from matter to photons under strong and ultrastrong coupling. However, for initial condition (b), nonclassical photonic states are generated only in the ultrastrong coupling regime due to the counter-rotating terms, highlighting the advantages of ultrastrong coupling. Furthermore, in the ultrastrong coupling regime, distinctive asymmetries relative to cavity detuning emerge in dynamical observables of both light and matter. The nonclassical photons can be extracted through a semi-transparent cavity mirror, while nonclassical matter states can be detected via time-resolved spectroscopy. This work highlights that polariton states may serve as a tool for dynamically generating and transferring nonclassical states, with potential applications in quantum technology.
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- PAR ID:
- 10641681
- Publisher / Repository:
- IOP
- Date Published:
- Journal Name:
- Quantum Science and Technology
- Volume:
- 10
- Issue:
- 2
- ISSN:
- 2058-9565
- Page Range / eLocation ID:
- 025002
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
-
Accepted Manuscript
- Journal Article:
- https://doi.org/10.1088/2058-9565/ada2b8
