Two-Dimensional Correlation Spectroscopy (2D-COS) for Analysis of Spatially Resolved Vibrational Spectra.

The last two decades have seen tremendous progress in the application of two-dimensional correlation spectroscopy (2D-COS) as a versatile analysis method for data series obtained using a large variety of different spectroscopic modalities, including infrared (IR) and Raman spectroscopy. The analysis technique is applicable to a series of spectra recorded under the influence of an external sample perturbation. Two-dimensional COS analysis is not only helpful to decipher correlations, which may exist between distinct spectral features, but can also be utilized to obtain the sequence of individual spectral changes. The focus of this review article is on the application of 2D-COS for analyzing spatially resolved data with special emphasis on hyperspectral imaging (HSI) study. In this review, we briefly introduce the fundamentals of the generalized 2D-COS analysis approach, discuss specific points of 2D-COS application to spatially resolved spectra and demonstrate essential aspects of data pre-processing for 2D-COS analysis of spatially resolved spectra. Based on illustrative examples, we show that 2D-COS is useful for spectral band assignment in HSI applications and demonstrate its utility for detecting subtle correlations between spectra features, or between features from different imaging modalities in the case of heterospectral (multimodal) HSI. Furthermore, a short overview on existing 2D-COS software tools is provided. It is hoped that this article represents not only a useful guideline for 2D-COS analyses of spatially resolved hyperspectral data but supports also further dissemination of the 2D-COS analysis method as a whole.