Second-harmonic radiation is generated at a gold surface by use of a laser pulse that is varied in duration from 14 to 29 fs and in intensity from 109 to 1011W/cm2 . At laser intensities below 1010W/cm2 , the second-harmonic signal has the expected quadratic dependence on pump-laser intensity; however, at higher intensities, the dependence is supraquadratic. This difference arises because the leading edge of the laser pulse interacts significantly with the gold electrons to create a nonequilibrium, photoexcited distribution. The second-harmonic generation process occurs before electron–electron or electron–phonon collisions can equilibrate the distribution and therefore serves as a probe of the nonequilibrium distribution.
© 1999 Optical Society of America
K.L. Moore and T.D. Donnelly, "Probing nonequilibrium electron distributions in gold by use of second harmonic generation," Opt. Lett. 24, 990 (1999). doi: 10.1364/OL.24.000990