We have used a theoretical insight regarding the relationship between the symmetric and asymmetric stretch chiral SFG responses of water to devise a new strategy for fitting chiral SFG spectra and extracting frequency distributions. We have shown that the characteristic "up-down" or "down-up" line shape of the O-H stretch response of chiral water superstructures is due to the incomplete cancellation of opposite-phase symmetric and asymmetric stretch components. We previously showed that O-H/N-H coupling is critical to the modeling of the N-H stretch component of the SFG spectra of LK7b and LE7b. Thus, future investigations will need to incorporate the effects of intermolecular coupling. Although we consider only intramolecular coupling as a first approximation in this study, we have shown that the theory derived within this approximation introduces a new strategy for analyzing the experimental and computational spectra. This strategy allows for spectral interpretation to extract molecular information. The application of our theoretical model for analyzing previous experimental data has captured the isotopic shifts of water O-H stretches and revealed physical pictures of a correlation between protein stability and hydrogen-bonding interactions of water in the first hydration shell. It is possible that similar insights can be developed for other types of vibrational spectroscopy or other molecular systems, enabling more insightful analysis of experimental spectra and a better understanding of computational results.