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

作　　者：Shanshan Gao Menghua Cui Ruiru Li Ling Liang Ying Liu Liming Xie 

机构地区：[1]CAS Key Laboratory of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China [2]Academy for Advanced Interdisciplinary Studies, Peking University, Beijing 100871, China [3]University of Chinese Academy of Science, Beijing 100049, China

出　　处：《Science Bulletin》2017年第1期9-15,共7页科学通报（英文版）

基　　金：supported by ‘‘Strategic Priority Research Program” of Chinese Academy of Sciences (XDA09040300);Beijing Science and Technology Project (Z151100003915077);Beijing Nova Programme (Z151100000315081);Beijing Talents Fund (2015000021223ZK17)

摘　　要：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 conven- tional FCS method has limitations in extracting autocorrelations for different species and cross correla- tions between different species. Recently developed fluorescence lifetime correlation spectroscopy （FLCS） based on time-tagged time-resolved （TITR） 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 TITR 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 bv the micro arrival times of photon pairs at each delay time.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.

关 键 词：Fluorescence lifetime Fluorescence correlation spectroscopy Cross correlation 

分 类 号：O657.3[理学—分析化学]