Abstract

Optical third-harmonic generation (THG) is dipole allowed. I report a 10(3) signal enhancement of THG that is due to the excitation of a surface plasmon in thin silver films by an attenuated-total-internal-ref lection geometry. Because the THG signal depends on the cube of the incident intensity and the second-harmonic generation depends on the square of the intensity, the THG overtakes the second-harmonic generation at laser intensities beyond 6 x 10(11) W/cm(2).

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