Construction of New Theoretical Modeling to Understand and Control Single Quantum Dot Intermittent Blinking

为了阐明间歇性闪烁动力学的机制，我们开发了一系列新的数据驱动的时间序列分析和建模技术，直接从单分子（SM）量子点（QD）荧光实验中提取潜在的动力学方案。这些包括变化点分析的发展和应用，使我们能够正确地提取开和关强度驻留时间统计数据，以及一种新的动力学方案（KS）构建方法的发展，该方法揭示了从时间序列中捕获完整统计信息的最无偏KS。所开发的方法不仅在SM QD实验中证明了它们的高可靠性和适用性，而且在SM酶转换实验和SM f1_atp酶旋转评估等其他SM测量中也证明了它们的高可靠性和适用性。

To elucidate the mechanisms of intermittent blinking kinetics, we developed a series of novel data-driven time series analysis and modeling techniques to extract the underlying kinetic scheme directly from single molecule (SM) quantum dot (QD) fluorescence experiments. These include the development and application of the change-point analysis that allows us to correctly extract the on and off intensity dwell-time statistics, and the development of a novel kinetic scheme (KS) construction methodology which unveils the most unbiased KS capturing the full statistical information from time series. The developed methods have demonstrated their high reliability and applicability not only in SM QD experiments, but also in a wide range of other SM measurements, such as in the SM enzymatic turnover experiments and the SM F1_ATPase rotation assessments.