General criterion to discern between coherent and incoherent synthesis of broadband coherent anti-Stokes Raman spectra

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Abstract

Recently, the ordinary qualitative criterion on how to distinguish between coherent and incoherent convolutions of broadband coherent anti-Stokes Raman (CARS) signals generated by degenerate pump lasers has been revised in view of a quantitative analysis. The revision has established that incoherent CARS approach can be justified as unitary limit of the function √πΓ exp[(Γ/σ1)2] erfc(Γ/σ1) /σ1, where Γ and σ1 are respectively the spectral widths of the Raman line and the degenerate pump lasers. The result was, however, limited to nonoverlapping Raman lines. In this work, the extension to a more common situation of closely spaced Raman transitions is considered. For large overlap between adjacent Raman lines, the new analysis suggests significant deviations from the previous result. Weak line mixing is also taken into consideration. Nonetheless, all types of deviations are characterized by a common tendency toward the incoherent limit. Copyright © 2007 John Wiley & Sons, Ltd.
Original languageEnglish
Pages (from-to)1338 - 1344
Number of pages7
JournalJournal of Raman Spectroscopy
Volume38
Issue number10
DOIs
Publication statusPublished - Oct 2007

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All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Spectroscopy

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