Three-color coherent anti-Stokes Raman scattering (CARS) represents non-degenerate four wave mixing that includes both non-resonant and resonant processes, the contributions of which depend upon how the molecular vibrational modes are being excited by the input laser pulses. The scattering signal due to resonant processes builds up progressively. An advanced analytical tool to reveal this deferred resonant signal buildup phenomenon is in need. In this work, we adapt a quantitative analytical tool by introducing one-dimensional and two-dimensional intensity–intensity correlation functions in terms of a new variable (probe pulse delay) and a new perturbation parameter (probe pulse linewidth). In particular, discrete diagonal directional sums are defined here as a tool to reduce both synchronous and asynchronous two-dimensional correlation spectroscopy (2D-COS) maps down to one-dimensional plots while maintaining the valuable analytical information. Detailed analyses using the all-Gaussian coherent Raman scattering closed-form solutions and the representative experimental data for resonant and non-resonant processes are presented and compared. The present work holds a promising potential for industrial application, e.g., by extractive industries to distinguish hydrocarbons (chemically resonant substance) from water (non-resonant contaminant) by utilizing the one- and two-dimensional correlation analyses.

三色相干反斯托克斯拉曼散射 (CARS) 代表非简并四波混合，包括非共振和共振过程，其贡献取决于输入激光脉冲如何激发分子振动模式。由于共振过程产生的散射信号逐渐增加。需要一种高级分析工具来揭示这种延迟共振信号积累现象。在这项工作中，我们通过根据新变量（探针脉冲延迟）和新扰动参数（探针脉冲线宽）引入一维和二维强度-强度相关函数来适应定量分析工具。特别是，离散对角线方向和在这里被定义为一种工具，用于将同步和异步二维相关光谱 (2D-COS) 映射减少到一维图，同时保持有价值的分析信息。使用全高斯相干拉曼散射封闭形式解决方案的详细分析以及共振和非共振过程的代表性实验数据进行了呈现和比较。目前的工作具有工业应用的广阔潜力，例如，通过采掘业利用一维和二维相关分析将碳氢化合物（化学共振物质）与水（非共振污染物）区分开来。使用全高斯相干拉曼散射封闭形式解决方案的详细分析以及共振和非共振过程的代表性实验数据进行了呈现和比较。目前的工作具有工业应用的广阔潜力，例如，通过采掘业利用一维和二维相关分析将碳氢化合物（化学共振物质）与水（非共振污染物）区分开来。使用全高斯相干拉曼散射封闭形式解决方案的详细分析以及共振和非共振过程的代表性实验数据进行了呈现和比较。目前的工作具有工业应用的广阔潜力，例如，通过采掘业利用一维和二维相关分析将碳氢化合物（化学共振物质）与水（非共振污染物）区分开来。