Modeling the Raman spectrum of graphitic material in rock samples with fluorescence backgrounds: accuracy of fitting and uncertainty estimation.

Abstract

We propose a robust technique called Savitzky-Golay second-derivative (SGSD) fitting for modeling the in situ Raman spectrum of graphitic materials in rock samples such as carbonaceous chondrite meteorites. In contrast to non-derivative techniques, with assumed locally linear or nth-order polynomial fluorescence backgrounds, SGSD produces consistently good fits of spectra with variable background fluorescence of any slowly varying form, without fitting or subtracting the background. In combination with a Monte Carlo technique, SGSD calculates Raman parameters (such as peak width and intensity) with robust uncertainties. To explain why SGSD fitting is more accurate, we compare how different background subtraction techniques model the background fluorescence with the wide and overlapping peaks present in a real Raman spectrum of carbonaceous material. Then, the utility of SGSD is demonstrated with a set of real and simulated data compared to commonly used linear background techniques. Researchers may find the SGSD technique useful if their spectra contain intense background interference with unknown functional form or wide overlapping peaks, and when the uncertainty of the spectral data is not well understood.