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Surface and bulk contributions to the second-order nonlinear optical response of a gold film

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Original languageEnglish
Pages (from-to)pp. 233402-1-233402-4
JournalPhysical Review B
Issue number233402
Publication statusPublished - 2009
Publication typeA1 Journal article-refereed


We use two-beam second-harmonic generation to separate the surface (electric dipole origin) and bulk (magnetic dipole and electric quadrupole origin) contributions to the second-order nonlinear optical response of an isotropic gold film. The bulk response is unambiguously observed and explained by momentum damping of electrons in a free-electron model. Although bulk effects could be enhanced by inhomogeneous local fields in metal nanostructures and have been used to model second-harmonic generation from metamaterials [Y. Zeng et al., Phys. Rev. B 79, 235109 (2009)], we find that surface effects dominate the nonlinearity. Our quantitative results for the surface and bulk parameters set the baseline for future descriptions of the second-order response of nanostructured metals.

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