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Interferometric coherent Raman spectroscopy: Resonant and non‐resonant contributions
Author(s) -
Schaertel S. A.,
Albrecht A. C.
Publication year - 1994
Publication title -
journal of raman spectroscopy
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.748
H-Index - 110
eISSN - 1097-4555
pISSN - 0377-0486
DOI - 10.1002/jrs.1250250716
Subject(s) - raman spectroscopy , interferometry , coherent anti stokes raman spectroscopy , hyperpolarizability , spectroscopy , chemistry , resonance (particle physics) , optics , physics , nuclear magnetic resonance , raman scattering , analytical chemistry (journal) , atomic physics , nonlinear system , quantum mechanics , nonlinear optical , chromatography
Abstract The theory of the recently discovered interferometric coherent Raman spectroscopy (ICRS) is extended to explicitly include terms resulting from non‐resonant contributions to the overall non‐linear susceptibility. The derived expression is applicable to both interferometric coherent anti‐Stokes Raman spectroscopy (ICARS) and interferometric coherent Stokes Raman spectroscopy (ICSRS) and can be applied to both neat solutions and binary mixtures. It is shown that the total description of ICRS must include a resonant term, a non‐resonant term and a resonant‐non‐resonant cross‐term, each of which exhibits analytically unique behavior in time‐domain ICRS experiments. From the complete expression one can extract relative strengths of the resonant and non‐resonant molecular hyperpolarizabilities. Resonant hyperpolarizabilities thus obtained may be used to determine absolute Raman cross‐sections, without making absolute measurements. Conversely, for a sample for which the absolute Raman cross‐section is independently known, one can determine the value of the non‐resonant hyperpolarizability.