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This paper focuses on the determination of the speciation in calcium-silicate glasses from Raman spectra and describes in detail the statistical method to determine quantitatively the speciation from collected spectra. We developed a novel statistical method employing optimization technique to determine the number of active species and partial spectral contributions for overlapped spectra. This method allows deconvoluting overlapping spectra from spectral data such as UV-vis, Raman, X-ray, photoelectron spectroscopy (XPS), or other. We treat spectral methods that have absolute and relative information. By viewing the data as noisy or uncertain, we put all steps to deconvolute spectral data on a unified statistical approach, which allows to model spectral data with more realism. The suggested method enables us to calculate from overlapping spectra directly the individual contributions of each active component (species) present in the system without making any assumptions on the shape or peak positions of the components in individual spectra.

Quantitative Raman spectroscopy: Challenges, shortfalls, and solutions—Application to calcium silicate glasses