Large crystal local-field effects in second-harmonic generation of a Si/CaF2 interface: An ab initio study

Matteo Bertocchi, Eleonora Luppi, Elena Degoli, Valérie Véniard, and Stefano Ossicini
Phys. Rev. B 86, 035309 – Published 11 July 2012

Abstract

In this work we present the ab initio study of crystal local-field effects in second-harmonic generation spectroscopy for an interface material such as Si/CaF2. Starting from an independent particle picture, we demonstrate the fundamental importance of the polarization effects at the interface discontinuity. The estimation of the magnitude of crystal local-field effects for second-order nonlinear response in Si/CaF2 interface was done by a comparative study with the absorption spectroscopy in the linear response. In both cases, we observe that the microscopic fluctuations due to the inhomogeneities of the system cause a decrease of the intensities of the spectra. However, for second-harmonic generation the decrease is selective and completely inhomogeneous while for absorption it is almost rigid. We also compare our theoretical study with experimental data showing unambiguously that only when crystal local fields are included, it is possible to correctly interpret experimental results.

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  • Received 6 March 2012

DOI:https://doi.org/10.1103/PhysRevB.86.035309

©2012 American Physical Society

Authors & Affiliations

Matteo Bertocchi1,2, Eleonora Luppi3, Elena Degoli4, Valérie Véniard2, and Stefano Ossicini4,5

  • 1Dipartimento di Fisica, Università di Modena e Reggio Emilia, via Campi 213/A, 41125 Modena, Italy
  • 2Laboratoire des Solides Irradiés, Ecole Polytechnique, Route de Saclay, F-91128 Palaiseau and European Theoretical Spectroscopy Facility (ETSF), France
  • 3Department of Chemistry, University of California, Berkeley, California 94702, USA
  • 4Istituto di Nanoscienze-CNR-S3 and Dipartimento di Scienze e Metodi dell’Ingegneria, Università di Modena e Reggio Emilia, Via Amendola 2 Padiglione Morselli, I-42122 Reggio Emilia, Italy
  • 5Centro Interdipartimentale En&Tech, Via Amendola 2 Padiglione Morselli, I-42122 Reggio Emilia, Italy

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Issue

Vol. 86, Iss. 3 — 15 July 2012

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