Pulse-sequenced coherent anti-Stokes Raman scattering spectroscopy: a method for suppression of the nonresonant background

Abstract

A new technique for suppressing the nonresonant contribution to the coherent anti-Stokes Raman scattering (CARS) signal is presented. This involves two-laser three-beam CARS generation using picosecond pulses in which one of the pump beams is delayed with respect to the two others. A reduction of 2 orders of magnitude is obtained for the 656-cm⁻¹ vibrational line of CS₂ in a 10% mixture of CS₂ in toluene. This reduction is limited by the ratio of the energy in our pulse laser to that in its trailing background, which is about 100:1. Use of alternative laser systems would reduce the background by about 10¹²:1.

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