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Fast and robust two-dimensional inverse Laplace transformation of single-molecule fluorescence lifetime data

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Title
Fast and robust two-dimensional inverse Laplace transformation of single-molecule fluorescence lifetime data
Author(s)
Saurabh Talele; John T. King
Publication Date
2021-10-19
Journal
Biophysical Journal, v.120, no.20, pp.4590 - 4599
Publisher
Biophysical Society
Abstract
© 2021 Biophysical Society.Fluorescence spectroscopy at the single-molecule scale has been indispensable for studying conformational dynamics and rare states of biological macromolecules. Single-molecule two-dimensional (2D) fluorescence lifetime correlation spectroscopy is an emerging technique that holds promise for the study of protein and nucleic acid dynamics, as the technique is 1) capable of resolving conformational dynamics using a single chromophore, 2) resolves forward and reverse transitions independently, and 3) has a dynamic window ranging from microseconds to seconds. However, the calculation of a 2D fluorescence relaxation spectrum requires an inverse Laplace transform (ILT), which is an ill-conditioned inversion that must be estimated numerically through a regularized minimization. Current methods for performing ILTs of fluorescence relaxation can be computationally inefficient, sensitive to noise corruption, and difficult to implement. Here, we adopt an approach developed for NMR spectroscopy (T1-T2 relaxometry) to perform one-dimensional (1D) and 2D-ILTs on single-molecule fluorescence spectroscopy data using singular-valued decomposition and Tikhonov regularization. This approach provides fast, robust, and easy to implement Laplace inversions of single-molecule fluorescence data. We compare this approach to the widely used maximal entropy method.
URI
https://pr.ibs.re.kr/handle/8788114/10737
DOI
10.1016/j.bpj.2021.08.031
ISSN
0006-3495
Appears in Collections:
Center for Soft and Living Matter(첨단연성물질 연구단) > 1. Journal Papers (저널논문)
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