Phase-shaping strategies for coherent anti-Stokes Raman scattering

The identification of largemolecules in complex environments requires probing of multiple vibrational resonances rather than a single resonance. Phase-shaping the excitation pulses allows the coherentmixing 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 ormultiplemeasurements. This article describes a particular implementation for coherent anti-StokesRaman 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.