Abstract
Spectral line shapes obtained with four-wave mixing Raman spectroscopy and stimulated Raman spectroscopy are investigated experimentally and theoretically. While both techniques are commonly used as high-resolution spectroscopies, the systematic differences in their spectra have not been well explored. Using an experimental setup capable of simultaneous measurement of coherent Stokes Raman spectroscopy and inverse Raman spectroscopy spectra, we are able to perform a direct comparison between both classes of Raman spectroscopies and to reveal even minor differences in the resulting spectra. After deriving the effect of Doppler broadening in these spectroscopies and taking the influence of neighboring lines into account, we are able to explain the observed differences in the Q-branch vibrational spectra of nitrogen. Possible systematic errors in different high-resolution Raman spectroscopies are discussed.
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