Open quantum system approach to single-molecule spectroscopy

Abstract

In this paper, single-molecule spectroscopy experiments based on continuous laser excitation are characterized through an open quantum system approach. The evolution of the fluorophore system follows from an effective Hamiltonian microscopic dynamic where its characteristic parameters, i.e., its electric dipole, transition frequency, and Rabi frequency, as well as the quantization of the background electromagnetic field and their mutual interaction, are defined in an extended Hilbert space associated to the different configurational states of the local nano-environment. After tracing out the electromagnetic field and the configurational states, the fluorophore density matrix is written in terms of a Lindblad rate equation. Observables associated to the scattered laser field, like optical spectrum, intensity-intensity correlation, and photon-counting statistics, are obtained from a quantum-electrodynamic calculation also based on the effective microscopic dynamic. In contrast with stochastic models, this approach allows to describe in a unified way both the full quantum nature of the scattered laser field as well as the classical nature of the environment fluctuations. By analyzing different processes such as spectral diffusion, lifetime fluctuations, and light assisted processes, we exemplify the power of the present approach.

18 pages, 6 figures

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• Thermodynamics of quantum jump trajectories in systems driven by classical fluctuations
• Superthermal photon bunching in terms of simple probability distributions
• Post-Markovian quantum master equations from classical environment fluctuations
• Quantum-jumps and photon-statistic in fluorescent systems coupled to classically fluctuating reservoirs
• Non-Markovian quantum jumps from measurements in bipartite Markovian dynamics
• Jump-diffusion unravelling of a non Markovian generalized Lindblad master equation
• Smoothed quantum-classical states in time-irreversible hybrid dynamics
• Stochastic wave-function unravelling of the generalized Lindblad equation
• Entropic relations for retrodicted quantum measurements
• Quantum-classical hybrid dynamics: coupling mechanisms and diffusive approximation
• Bipartite entanglement induced by classically-constrained quantum dissipative dynamics