Phys. Rev. Lett. 90, 213902 (2003) [4 pages]Femtosecond Phase-and-Polarization Control for Background-Free Coherent Anti-Stokes Raman SpectroscopyReceived 2 December 2002; published 30 May 2003 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. © 2003 The American Physical Society URL:
http://link.aps.org/doi/10.1103/PhysRevLett.90.213902
DOI:
10.1103/PhysRevLett.90.213902
PACS:
42.65.Dr, 32.80.Qk, 78.47.+p
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