Single molecule photon counting statistics for quantum mechanical chromophore dynamics.
Single molecule photon counting statistics for quantum mechanical chromophore dynamics.
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DOI：
10.1021/jp062345v
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发表时间：
2006-04
期刊：
影响因子：
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通讯作者：
G. Bel;Yujun Zheng;F. Brown
中科院分区：
文献类型：
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作者：
G. Bel;Yujun Zheng;F. Brown
我们将用于计算单分子光子发射统计的生成函数技术（Zheng, Y.；Brown, F. L. H. Phys. Rev. Lett. 2003, 90, 238305）扩展到由多级量子动力学控制的系统。这为研究纯随机模型和混合量子随机模型领域之外的现象提供了可能性。特别地，本方法允许计算光谱解析并受量子相干性影响的光子统计数据。几个模型计算说明了该技术的通用性，并强调了量子力学模型和相关随机近似之间出现的定量和定性差异。计算表明，研究光子统计作为光子频率的函数有可能比通常的宽带检测方案揭示更多有关系统动力学的信息。
We extend the generating function technique for calculation of single molecule photon emission statistics (Zheng, Y.; Brown, F. L. H. Phys. Rev. Lett. 2003, 90, 238305) to systems governed by multi-level quantum dynamics. This opens up the possibility to study phenomena that are outside the realm of purely stochastic and mixed quantum-stochastic models. In particular, the present methodology allows for calculation of photon statistics that are spectrally resolved and subject to quantum coherence. Several model calculations illustrate the generality of the technique and highlight quantitative and qualitative differences between quantum mechanical models and related stochastic approximations when they arise. Calculations suggest that studying photon statistics as a function of photon frequency has the potential to reveal more about system dynamics than the usual broadband detection schemes.