Interferometric differentiation between resonant coherent anti-Stokes Raman scattering and nonresonant four-wave-mixing processes

A major impediment to the use of coherent anti-Stokes Raman scattering (CARS) to identify biological molecules is that the illumination levels required to produce a measurable signal often also produce significant nonresonant background from the medium, especially from water. We present a method of nonlinear interferometry to differentiate between which components of the anti-Stokes signal are resonant and nonresonant. The technique takes advantage of the persistence of intermediate states involved in the resonant process. This method is applicable to most existing pulsed CARS illumination methods and provides for identification of resonant CARS. We demonstrate the method by examining the signals produced by acetone, which exhibits resonance, and water, which does not. © 2004 American Institute of Physics. [DOI: 10.1063/1.1829162]