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 to . At laser intensities below , 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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