Bel Golan, Zheng Yujun, Brown Frank L H
Department of Chemistry and Biochemistry, University of California, Santa Barbara, California 93106-9510, USA.
J Phys Chem B. 2006 Sep 28;110(38):19066-82. doi: 10.1021/jp062345v.
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.
我们将用于计算单分子光子发射统计量的生成函数技术（郑宇；布朗，F.L.H.《物理评论快报》2003年，90卷，238305页）扩展到由多能级量子动力学支配的系统。这为研究纯随机和混合量子 - 随机模型范围之外的现象开辟了可能性。特别地，当前方法允许计算经光谱分辨且受量子相干影响的光子统计量。几个模型计算说明了该技术的通用性，并突出了量子力学模型与相关随机近似出现时的定量和定性差异。计算表明，与通常的宽带检测方案相比，将光子统计量作为光子频率的函数进行研究有可能揭示更多关于系统动力学的信息。
