# 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

 Title: 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 Author: Aggarwal, R. L.; Farrar, L. W.; Parkhill, J; Aspuru-Guzik, Alan; Polla, D. L. Note: Order does not necessarily reflect citation order of authors. Citation: Aggarwal, R. L., L. W. Farrar, J. Parkhill, Alan Aspuru-Guzik, and D. L. Polla. 2012. “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.” Journal of Raman Spectroscopy 43 (7) (July): 911–916. doi:10.1002/jrs.3102. http://dx.doi.org/10.1002/jrs.3102. Access Status: Full text of the requested work is not available in DASH at this time (“dark deposit”). For more information on dark deposits, see our FAQ. Full Text & Related Files: aspuru-guzik-measurement.pdf (305.6Kb; PDF) Abstract: The components of the third-order nonlinear optical susceptibility $$\chi^{(3)}$$ for the $$1002-cm^{–1}$$ 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 $$2.8 ± 0.3 × 10^{–12}$$, $$2.0 ± 0.2 × 10^{–12}$$, and $$0.8 ± 0.1 × 10^{–12} cm g^{–1} s^2$$ were measured for the xxxx, xxyy, and xyyx components of $$|3\chi^{(3)}|$$, respectively. We have calculated these quantities using a microscopic model, reproducing the same qualitative trend. The Raman cross-section $$\sigma_{RS}$$ for the $$1002-cm^{–1}$$ mode of neat benzenethiol has been determined to be $$3.1 ± 0.6 × 10^{–29} cm^2$$ 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) $$\Gamma$$ was determined to be $$2.4 ± 0.3 cm^{–1}$$ using normal Stokes Raman scattering. The measured values of $$\sigma_{RS}$$ and $$\Gamma$$ yield a value of $$2.1 ± 0.4 × 10^{–12} cm g^{–1} s^2$$ for the resonant component of $$3χ^{(3)}$$. A value of $$1.9 ± 0.9 × 10^{–12} cm g^{–1} s^2$$ has been deduced for the nonresonant component of $$3\chi^{(3)}$$. Published Version: doi:10.1002/jrs.3102 Citable link to this page: http://nrs.harvard.edu/urn-3:HUL.InstRepos:12697344 Downloads of this work: