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

被引:2
作者
Talele, Saurabh [1 ,2 ]
King, John T. [1 ]
机构
[1] Inst Basic Sci, Ctr Soft & Living Matter, Ulsan, South Korea
[2] Ulsan Natl Inst Sci & Technol, Dept Biomed Engn, Ulsan, South Korea
关键词
RESONANCE ENERGY-TRANSFER; 1ST KIND; DYNAMICS; RECONSTRUCTION; SPECTROSCOPY;
D O I
10.1016/j.bpj.2021.08.031
中图分类号
Q6 [生物物理学];
学科分类号
071011 ;
摘要
Fluorescence spectroscopy at the single-molecule scale has been indispensable for studying conformational dy-namics 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 fluores-cence relaxation spectrum requires an inverse Laplace transform (ILT), which is an ill-conditioned inversion that must be esti-mated 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 spec-troscopy 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.
引用
收藏
页码:4590 / 4599
页数:10
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