Abstract

AbstractExtending previous second‐harmonic generation (SHG) single‐wavelength studies [1] of Si nanocrystals (NCs) embedded in fused silica, we implement spectroscopic cross‐polarized two‐beam SHG (XP2‐SHG) by employing an optical parametric amplifier as a source of widely tunable (1.6 ≤ Eph ≤ 2.4 eV) femtosecond pulses.Subsequent isolation of the SH signal produced by the NCs yields the oscillator strength and phase of their nonlinear response. We obtain a broad resonance between bulk Si E1 and E2 critical points. Possible explanations for the spectroscopic result are discussed. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

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