Enhanced 3-D asynchronous correlation data preprocessing method for Raman spectroscopy of Chinese handmade paper

Abstract

We have developed a novel 3D asynchronous correlation method (3D-ACM) designed for the classification and identification of Chinese handmade paper samples using Raman spectra and machine learning. The 3D-ACM approach involves two rounds of tensor product and Hilbert transform operations. In the tensor product process, the outer product of the spectral data from different samples within the same category is computed, establishing inner connections among all samples within that category. The Hilbert transform introduces a 90-degree phase shift, resulting in a true three-dimensional spectral data structure. This expansion significantly increases the number of equivalent frequency points and samples within each category. This enhancement substantially boosts spectral resolution and reveals more hidden information within the spectral data. To maximize the potential of 3D-ACM, we employed six machine learning models: principal component analysis (PCA) with linear regression (LR), support vector machine (SVM) with LR, k-Nearest Neighbors (KNN), random forest (RF), and convolutional neural network (CNN). When applied to the 3D-ACM data preprocessing method, R-squared values of PLS-LR, KNN, RF and CNN supervised models, approached or equaled 1. This indicates exceptional performance comparable to unsupervised models like PCA. 3D-ACM stands as a versatile mathematical technique not confined to spectral data. It also eliminates the necessity for additional experimental setups or external control conditions, distinct from traditional two-dimensional correlation spectroscopy. Moreover, it preserves the original experimental data, setting it apart from conventional data preprocessing methods. This positions 3D-ACM as a promising tool for future material classification and identification in conjunction with machine learning.