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

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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

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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.

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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.
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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
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