Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy

Phys Rev Lett. 2003 May 30;90(21):213902. doi: 10.1103/PhysRevLett.90.213902. Epub 2003 May 30.


Phase-and-polarization coherent control is applied to control the nonlinear response of a quantum system. We use it to obtain high-resolution background-free single-pulse coherent anti-Stokes Raman spectra. The ability to control both the spectral phase and the spectral polarization enables measurement of a specific off-diagonal susceptibility tensor element while exploiting the different spectral response of the resonant Raman signal and the nonresonant background to achieve maximal background suppression.