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Calculation of Photon-Count Number Distributions via Master Equations

机译:通过主方程计算光子数分布

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摘要

Fitting of photon-count number histograms is a way of analysis of fluorescence intensity fluctuations, a successor to fluorescence correlation spectroscopy. First versions of the theory for calculating photon-count number distributions have assumed constant emission intensity by a molecule during a counting time interval. For a long time a question has remained unanswered: to what extent is this assumption violated in experiments? Here we present a theory of photon-count number distributions that takes account of intensity fluctuations during a counting time interval. Theoretical count-number distributions are calculated via a numerical solution of Master equations (ME), which is a set of differential equations describing diffusion, singlet-triplet transitions, and photon emission. Detector afterpulsing and dead-time corrections are also included. The ME-theory is tested by fitting a series of photon-count number histograms corresponding to different lengths of the counting time interval. Compared to the first version of fluorescence intensity multiple distribution analysis theory introduced in 2000, the fit quality is significantly improved. It is discussed how a theory of photon-count number distributions, which assumes constant emission intensity during a counting time interval, may also yield a good fit quality. We argue that the spatial brightness distribution used in calculations of the fit curve is not the true spatial brightness distribution. Instead, a number of dynamic processes, which cause fluorescence intensity fluctuations, are indirectly taken into account via the profile adjustment parameters.
机译:拟合光子数直方图是分析荧光强度波动的一种方法,它是荧光相关光谱法的后续技术。用于计算光子数分布的理论的第一个版本假定分子在计数时间间隔内具有恒定的发射强度。长期以来,一个问题一直没有得到答案:在何种程度上违反了这一假设?在这里,我们提出了一种光子计数分布的理论,该理论考虑了在计数时间间隔内的强度波动。理论计数数分布是通过Master方程(ME)的数值解计算的,该方程是一组描述扩散,单重态-三重态跃迁和光子发射的微分方程。还包括检测器后脉冲和停滞时间校正。通过拟合一系列与计数时间间隔的不同长度相对应的光子计数直方图来测试ME理论。与2000年引入的第一版荧光强度多重分布分析理论相比,拟合质量得到了显着提高。讨论了在计数时间间隔内假设发射强度恒定的光子计数分布理论,如何也能产生良好的拟合质量。我们认为,在拟合曲线的计算中使用的空间亮度分布不是真正的空间亮度分布。取而代之的是,通过轮廓调整参数间接地考虑引起荧光强度波动的许多动态过程。

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