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Observation of surface frequency doubling in Si(111) mediated by a $$\chi ^4$$ process

Year: 2026
Type: article
Abstract: Nonlinear optical processes such as second-harmonic generation (SHG) provide powerful probes of the structural and electronic properties of semiconductor surfaces and interfaces. While SHG in centrosymmetric materials like silicon has been extensively investigated, higher-order nonlinear contributions remain largely unexplored. Here, we report for the first time the observation of a $$\chi ^4$$ -mediated contribution to SHG from Si(111)– $$SiO_2$$ interfaces, revealed through intensity scaling and azimuthal anisotropy measurements. The frequency-doubled signal exhibits both quadratic and quartic dependence on the incident intensity, with the quartic term displaying a distinct threefold symmetry superimposed on the conventional sixfold SHG pattern. This identifies a previously unreported pathway for nonlinear emission at silicon surfaces. These results were enabled by high-intensity excitation near the laser-induced damage threshold, combined with automated high-sensitivity detection.
Language: English
Open Access status: gold
Estimated APC paid: $2,690
OpenAlex ID: W7225791412
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