Single-Beam and Enhanced Two-Beam Second-Harmonic Generation from Silicon Nanocrystals by Use of Spatially Inhomogeneous Femtosecond Pulses

Details Single-Beam and Enhanced Two-Beam Second-Harmonic Generation from Silicon Nanocrystals by Use of Spatially Inhomogeneous Femtosecond Pulses Single-Beam and Enhanced Two-Beam Second-Harmonic Generation from Silicon Nanocrystals by Use of Spatially Inhomogeneous Femtosecond Pulses

Jan 2005

adsabs.harvard.edu/cgi-bin/nph-data_query?bibcode=2005phrvl..94d7401f&link_type=abstract

Physical Review Letters, vol. 94, Issue 4, id. 047401

Physics

26

Nanocrystals And Nanoparticles, Frequency Conversion, Harmonic Generation, Including Higher-Order Harmonic Generation, Semiconductors, Optical Properties Of Surfaces

Scientific paper

Optical second-harmonic generation (SHG) is used as a noninvasive probe of the interfaces of Si nanocrystals (NCs) embedded uniformly in an SiO2 matrix. Measurements of the generated SH mode verify that the second-harmonic polarization has a nonlocal dipole form proportional to (E→·∇)E→ that depends on inhomogeneities in the incident field E→, as proposed in recent models based on a locally noncentrosymmetric dipolar response averaged over the spherical NC interfaces. A two-beam SHG geometry is found to enhance this polarization greatly compared to single-beam SHG, yielding strong signals useful for scanning, spectroscopy, and real-time monitoring. This configuration provides a general strategy for enhancing the second-order nonlinear response of centrosymmetric samples, as demonstrated here for both Si nanocomposites and their glass substrates.

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