Abstract

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 1011 W/cm2. At laser intensities below 1010 W/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

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