Two-Dimensional Fluctuation Correlation Spectroscopy (2D-FlucCS): A Method to Determine the Origin of Relaxation Rate Dispersion

IF 4.6 Q1 CHEMISTRY, ANALYTICAL ACS Measurement Science Au Pub Date : 2024-02-01 DOI:10.1021/acsmeasuresciau.3c00048
Ruchir Gupta,  and , Sachin Dev Verma*, 
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Abstract

Relaxation rate dispersion, i.e., nonexponential or multicomponent kinetics, is observed in complex systems when measuring relaxation kinetics. Often, the origin of rate dispersion is associated with the heterogeneity in the system. However, both homogeneous (where all molecules experience the same rate but inherently nonexponential) and heterogeneous (where all molecules experience different rates) systems can exhibit rate dispersion. A multidimensional correlation analysis method has been demonstrated to detect and quantify rate dispersion observed in molecular rotation, diffusion, solvation, and reaction kinetics. One-dimensional (1D) autocorrelation function detects rate dispersion and measures its extent. Two-dimensional (2D) autocorrelation function measures the origin of rate dispersion and distinguishes homogeneous from heterogeneous. In a heterogeneous system, implicitly there exist subensembles of molecules experiencing different rates. A three-dimensional (3D) autocorrelation function measures subensemble exchange if present and reveals if the system possesses static or dynamic heterogeneity. This perspective discusses the principles, applications, and potential and also presents a future outlook of two-dimensional fluctuation correlation spectroscopy (2D-FlucCS). The method is applicable to any experiment or simulation where a time series of fluctuation in an observable (emission, scattering, current, etc.) around a mean value can be obtained in steady state (equilibrium or nonequilibrium), provided the system is ergodic.

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二维波动相关光谱(2D-FlucCS):一种确定弛豫率散布起源的方法
在测量弛豫动力学时,会在复杂系统中观察到弛豫速率分散,即非指数或多组分动力学。通常,速率离散的起源与系统中的异质性有关。然而,同质(所有分子的速率相同,但本质上是非指数)和异质(所有分子的速率不同)系统都会出现速率离散现象。已证明一种多维相关分析方法可以检测和量化在分子旋转、扩散、溶解和反应动力学中观察到的速率离散性。一维(1D)自相关函数可检测速率离散并测量其程度。二维(2D)自相关函数测量速率离散的起源,并区分均相和异相。在异质系统中,隐含地存在着经历不同速率的分子子系统。三维(3D)自相关函数可测量是否存在亚集合交换,并揭示系统是否具有静态或动态异质性。本视角讨论了二维波动相关光谱法(2D-FlucCS)的原理、应用和潜力,并对其未来进行了展望。该方法适用于任何实验或模拟,只要系统是遍历的,就能在稳态(平衡或非平衡)下获得观测值(发射、散射、电流等)围绕平均值波动的时间序列。
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来源期刊
ACS Measurement Science Au
ACS Measurement Science Au 化学计量学-
CiteScore
5.20
自引率
0.00%
发文量
0
期刊介绍: ACS Measurement Science Au is an open access journal that publishes experimental computational or theoretical research in all areas of chemical measurement science. Short letters comprehensive articles reviews and perspectives are welcome on topics that report on any phase of analytical operations including sampling measurement and data analysis. This includes:Chemical Reactions and SelectivityChemometrics and Data ProcessingElectrochemistryElemental and Molecular CharacterizationImagingInstrumentationMass SpectrometryMicroscale and Nanoscale systemsOmics (Genomics Proteomics Metabonomics Metabolomics and Bioinformatics)Sensors and Sensing (Biosensors Chemical Sensors Gas Sensors Intracellular Sensors Single-Molecule Sensors Cell Chips Arrays Microfluidic Devices)SeparationsSpectroscopySurface analysisPapers dealing with established methods need to offer a significantly improved original application of the method.
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