Quantitative deconvolution of autocorrelations and cross correlations from two-dimensional lifetime decay maps in fluorescence lifetime correlation spectroscopy

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• 作者：Shanshan Gao^a ; ¹ ; Menghua Cui^a ; ^b ; ^c ; ¹ ; Ruiru Li^a ; ^c ; Ling Liang^a ; Ying Liu^a ; ^{liuy1@nanoctr.cn} ; Liming Xie^a ; ^{xielm@nanoctr.cn}
• 关键词：Fluorescence lifetime ; Fluorescence correlation spectroscopy ; Cross correlation
• 刊名：Science Bulletin
• 出版年：2017
• 出版时间：15 January 2017
• 年：2017
• 卷：62
• 期：1
• 页码：9-15
• 全文大小：2453 K
• 卷排序：62

文摘

Fluorescence correlation spectroscopy (FCS) is a widely used method for measuring molecular diffusion and chemical kinetics. However, when a mixture of fluorescent species is taken into account, the conventional FCS method has limitations in extracting autocorrelations for different species and cross correlations between different species. Recently developed fluorescence lifetime correlation spectroscopy (FLCS) based on time-tagged time-resolved (TTTR) photon recording, which can record the global and micro arrival time for each individual photon, has been used to discriminate different species according to fluorescence lifetime. Here, based on two-dimensional lifetime decay maps constructed from TTTR photon stream, we have developed a quantitative lifetime-deconvolution FCS model (LDFCS) to extract precise chemical rates for chemical conversions in multi-species systems. The key point of LDFCS model is separation of different species according to the global distribution of fluorescence lifetime and then deconvolution of autocorrelations and cross-correlations from the two-dimensional lifetime decay maps constructed by the micro arrival times of photon pairs at each delay time.