Spectral fitting has been a standard approach for extracting molecular information from vibrational spectra, including those obtained by chirality-sensitive vibrational sum frequency generation spectroscopy (chiral SFG). In recent years, chiral SFG has emerged as a powerful technique for studying the macromolecular hydration shell. Few experimental techniques are able to probe water in biological hydration shells selectively. As a surface-selective technique, chiral SFG is able to resolve chirality at interfaces. Our group has shown that this technique is selective to the first hydration shell around a b-sheet protein. In general, data analysis of vibrational studies is performed by fitting vibrational spectra.