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arXiv 0902.4019quant-phcond-mat.otherphysics.optics
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单分子光谱学的开放量子系统方法

Open quantum system approach to single-molecule spectroscopy

Adrian A. Budini

备注：
18 pages, 6 figures
发表信息：
Phys. Rev. A 79, 043804 (2009)
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摘要：

本文采用开放量子系统方法，对基于连续激光激发的单分子光谱学实验进行了表征。荧光团系统的演变遵循有效的哈密顿微观动力学，其中其特征参数，即，它的电偶极子，跃迁频率和拉比频率，以及量子化的背景电磁场和它们的相互作用，被定义在一个扩展的希尔伯特空间与当地纳米环境的不同配置状态。在追踪出电磁场和构型状态之后，根据Lindblad速率方程写出荧光团密度矩阵。与散射激光场，如光谱，强度-强度相关性，光子计数统计，相关的观测值，从量子电动力学计算得到的有效微观动力学的基础上。与随机模型相比，这种方法允许以统一的方式描述散射激光场的完整量子性质以及环境波动的经典性质。通过分析光谱扩散、寿命波动和光辅助过程等不同过程，我们举例说明了本方法的强大功能。

英文摘要：

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.

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