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Fabrication And Characterization Of Photonic Crystal Slow Light Waveguides And Cavities
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Published on: November 30, 2012

Communications: Ab initio second-order nonlinear optics in solids.

Eleonora Luppi1, Hannes Hübener, Valérie Véniard

  • 1Laboratoire des Solides Irradiés, Ecole Polytechnique, CNRS-CEA/DSM, European Theoretical Spectroscopy Facility (ETSF), F-91128 Palaiseau, France. eleonora.luppi@polytechnique.edu

The Journal of Chemical Physics
|July 2, 2010
PubMed
Summary
This summary is machine-generated.

We developed a new theory using time-dependent density-functional theory to calculate second-order nonlinear optical properties. Including excitonic effects is crucial for accurately predicting second-harmonic generation spectra in semiconductors like GaAs.

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Area of Science:

  • Condensed matter physics
  • Materials science
  • Computational physics

Background:

  • Accurate theoretical prediction of nonlinear optical properties is essential for materials design.
  • Existing methods often struggle to incorporate many-body effects like local fields and excitons.

Purpose of the Study:

  • To develop a first-principles theory for calculating the macroscopic second-order susceptibility (χ(2)).
  • To investigate the role of many-body effects, specifically crystal local fields and excitons, in second-harmonic generation (SHG).

Main Methods:

  • Utilizing time-dependent density-functional theory (TDDFT).
  • Incorporating many-body effects including crystal local fields and excitons.
  • Applying the theory to calculate SHG spectroscopy.

Main Results:

  • The developed theory successfully computes SHG spectra.
  • Calculations for the cubic semiconductor GaAs show excellent agreement with experimental data.
  • Crystal local fields alone were insufficient; excitonic effects were necessary for accurate predictions.

Conclusions:

  • The first-principles TDDFT approach, including excitonic effects, provides accurate predictions of SHG spectra.
  • This method offers a robust tool for studying nonlinear optical properties in materials.
  • Excitonic effects play a critical role in determining the SHG response of semiconductors.