• ultrafast nonlinear optics;
  • coherent anti-Stokes Raman scattering;
  • nonlinear microscopy;
  • pulse shaping;
  • evolutionary algorithms


The identification of large molecules in complex environments requires probing of multiple vibrational resonances rather than a single resonance. Phase-shaping the excitation pulses allows the coherent mixing of several resonances so that the presence of molecules can be inferred directly from the integrated output pulse energy. This avoids the need for the collection of spectra or multiple measurements. This article describes a particular implementation for coherent anti-Stokes Raman scattering microscopy that uses a broadband pump and probe field in combination with a narrowband Stokes field. We numerically study the possibilities of optimizing selectivity, specificity, and sensitivity by precalculating pulse shapes using an evolutionary algorithm. Copyright © 2011 John Wiley & Sons, Ltd.