2009/02/23 by Adrián A. Budini, Adrian A. Budini · 1 citation
Computer Science · Engineering · Physics and Astronomy · #Molecular Junctions and Nanostructures #Quantum Information and Cryptography #Spectroscopy and Quantum Chemical Studies #cond-mat.other #physics.optics #quant-ph
paper · pdf · doi:10.1103/physreva.79.043804
published as Phys. Rev. A 79, 043804 (2009) · 18 pages, 6 figures
arxiv created 2009/02/23 · openalex publication_date 2009/04/03 · arxiv updated 2009/12/01 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
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 nanoenvironment. 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, such as 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 one 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.