Abstract

The surface-enhanced coherent anti-Stokes Raman scattering (SECARS) from a self-assembled monolayer (SAM) of benzenethiol on a silver-coated surface-enhanced Raman scattering (SERS) substrate has been measured for the 1574 cm<sup>-1</sup> SERS mode. A value of 9.6 ± 1.7×10<sup>-14</sup> W was determined for the resonant component of the SECARS signal using 17.8 mW of 784.9 nm pump laser power and 7.1 mW of 895.5 nm Stokes laser power; the pump and Stokes lasers were polarized parallel to each other but perpendicular to the grooves of the diffraction grating in the spectrometer. The measured value of resonant component of the SECARS signal is in agreement with the calculated value of 9.3×10<sup>-14</sup> W using the measured value of 8.7 ± 0.5 cm<sup>-1</sup> for the SERS linewidth Γ (full width at half-maximum) and the value of 5.7 ± 1.4×10<sup>-7</sup> for the product of the Raman cross section σ<sub>SERS</sub> and the surface concentration <i>N</i><sub>s</sub> of the benzenethiol SAM. The <i>xxxx</i> component of the resonant part of the third-order nonlinear optical susceptibility |3 <inline-graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="i0003-7028-67-2-132-ilm01.tif"/> | for the 1574 cm<sup>-1</sup> SERS mode has been determined to be 4.3 ± 1.1×10<sup>-5</sup> cm<sup>.</sup>g<sup>-1.</sup>s<sup>2</sup>. The SERS enhancement factor for the 1574 cm<sup>-1</sup> mode was determined to be 3.6 ± 0.9×10<sup>7</sup> using the value of 1.8×10<sup>15</sup> molecules/cm<sup>2</sup> for N<sub>s</sub>.

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