Abstract

We introduce a spectroscopic method for measuring the frequency-dependent second-order response using ultrabroadband strongly chirped laser pulses. The dispersion suppresses nonlinear frequency mixing, hence the second-order response of a material can be unambiguously retrieved. We demonstrate this method by measuring the frequency-dependent second-harmonic (SH) response of the metals gold, aluminium, silver, and copper in the wavelength range of about 900–1150 nm and compare the results to classical SH spectroscopy. The SH spectra indicate that interband transitions in the metals influence the overall nonlinear optical response.

© 2014 Optical Society of America

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