Measurement Of The Third-Order Nonlinear Optical Susceptibility Chi((3)) For The 1002-Cm(-1) Mode Of Benzenethiol Using Coherent Anti-Stokes Raman Scattering With Continuous-Wave Diode Lasers

The components of the third-order nonlinear optical susceptibility ?(3) for the 1002-cm1 mode of neat benzenethiol have been measured using coherent anti-Stokes Raman scattering with continuous-wave diode pump and Stokes lasers at 785.0 and 852.0?nm, respectively. Values of 2.8?+/-?0.3?x?1012, 2.0?+/-?0.2?x?1012, and 0.8?+/-?0.1?x?1012?cm center dot g1 center dot s2 were measured for the xxxx, xxyy, and xyyx components of |3?(3)|, respectively. We have calculated these quantities using a microscopic model, reproducing the same qualitative trend. The Raman cross-section sRS for the 1002-cm1 mode of neat benzenethiol has been determined to be 3.1?+/-?0.6?x?1029?cm2 per molecule. The polarization of the anti-Stokes Raman scattering was found to be parallel to that of the pump laser, which implies negligible depolarization. The Raman linewidth (full-width at half-maximum) G was determined to be 2.4?+/-?0.3?cm1 using normal Stokes Raman scattering. The measured values of sRS and G yield a value of 2.1?+/-?0.4?x?1012?cm center dot g1 center dot s2 for the resonant component of 3?(3). A value of 1.9?+/-?0.9?x?1012?cm center dot g1 center dot s2 has been deduced for the nonresonant component of 3?(3). Copyright (c) 2011 John Wiley & Sons, Ltd.