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Keywords:

  • CARS;
  • supercontinuum impulsive excitation;
  • frequency-resolved optical gating (FROG)

Time-resolved coherent anti-Stokes Raman scattering (CARS) impulsively excited by a supercontinuum (SC) is investigated. We show that it is critical to optimize the temporal overlapping of the constituent solitons of a SC in order to impulsively excite vibrational modes over a broad frequency range. The cross-correlation frequency-resolved optical gating technique is utilized to retrieve the optical response function of molecules under SC impulsive excitation, and background-free CARS with spectral resolution significantly better than the bandwidth of the probe pulses is achieved. Copyright © 2011 John Wiley & Sons, Ltd.