Optical second-harmonic generation from silicon nanocrystals

Michael C. Downer; Peter C. Figliozzi; Yingying Jiang; Liangfeng Sun; Brian Mattern; C. Woody White; Steve P. Withrow

doi:10.1117/12.511483

4 December 2003 Optical second-harmonic generation from silicon nanocrystals

Michael C. Downer, Peter C. Figliozzi, Yingying Jiang, Liangfeng Sun, Brian Mattern, C. Woody White, Steve P. Withrow

Proceedings Volume 5223, Physical Chemistry of Interfaces and Nanomaterials II; (2003) https://doi.org/10.1117/12.511483
Event: Optical Science and Technology, SPIE's 48th Annual Meeting, 2003, San Diego, California, United States

Abstract

Optical second-harmonic generation (SHG)is used as a noninvasive probe of the interfaces of Si nanocrystals (SiNCs)embedded in an SiO₂ matrix. We verify experimentally that the second-harmonic polarization P⁽²⁾ has a quadrupolar form proportional to (E ·∇) E as proposed in recent models based on a locally noncentrosymmetric dipolar polarization averaged over the spherical NC interface. A two-beam sum-frequency geometry is found to enhance this polarization dramatically compared to a single-beam SHG geometry, yielding strong signals useful for scanning, spectroscopy and real time monitoring. Using this two beam geometry, we have produced non-invasive two dimensional SHG maps with few-micron resolution of 1-micron-thick layers of Si-NCs (3 and 5 nm average diameter)produced by ion implanting Si into SiO₂. Samples were scanned over a 5mm x 5mm area with two non-collinear,orthogonally polarized,amplified Ti:S laser pulses (80 fs,810nm,100 μJ,1 kHz repetition rate) while detecting the generated SH signal in transmission. The SHG signal is sensitive to chemical modification of the Si/SiO₂ interface and to local gradients in nanoparticle density.

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Michael C. Downer, Peter C. Figliozzi, Yingying Jiang, Liangfeng Sun, Brian Mattern, C. Woody White, and Steve P. Withrow "Optical second-harmonic generation from silicon nanocrystals", Proc. SPIE 5223, Physical Chemistry of Interfaces and Nanomaterials II, (4 December 2003); https://doi.org/10.1117/12.511483

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KEYWORDS

Second-harmonic generation

Signal detection

Polarization

Glasses

Interfaces

Nanocrystals

Silicon

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