The spectra of the isotropic and anisotropic contributions to second-harmonic generation from modified Si(001) surfaces are separated using polarization selection and rotational anisotropy. A bulk anisotropic resonance is observed at a two-photon energy of The isotropic surface contributions for native oxide Si and thermal oxide Si show peaks at and respectively. Interference between these contributions and the bulk signal can shift the apparent resonance position if they are not separated. The surface produces a noninterfering contribution that is comparable to the interfering contribution for H-terminated Si but negligible for oxidized silicon.
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