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

Shanshan Gao; Menghua Cui; Ruiru Li; Ling Liang; Ying Liu; Liming Xie

doi:10.1016/j.scib.2016.11.006

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

Sci Bull (Beijing). 2017 Jan 15;62(1):9-15. doi: 10.1016/j.scib.2016.11.006. Epub 2016 Dec 10.

Authors

Shanshan Gao¹, Menghua Cui², Ruiru Li³, Ling Liang¹, Ying Liu⁴, Liming Xie⁵

Affiliations

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 CAS Key Laboratory of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China; Academy for Advanced Interdisciplinary Studies, Peking University, Beijing 100871, China; University of Chinese Academy of Science, Beijing 100049, China.
³ CAS Key Laboratory of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China; University of Chinese Academy of Science, Beijing 100049, China.
⁴ CAS Key Laboratory of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China. Electronic address: liuy1@nanoctr.cn.
⁵ CAS Key Laboratory of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China. Electronic address: xielm@nanoctr.cn.

PMID: 36718073
DOI: 10.1016/j.scib.2016.11.006

Abstract

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.

Keywords: Cross correlation; Fluorescence correlation spectroscopy; Fluorescence lifetime.