Bulk dipole contribution to second harmonic generation in diamond lattices

Abstract

It is generally argued that material classes with inversion symmetry do not produce bulk dipole related second harmonic generation (SHG). So, SHG is then either ascribed to surface effects or bulk related electric quadrupole or magnetic dipole effects. Using symmetry and \emph{ab-initio} potentials we show analytically that due to the fact of the decaying harmonic electric field certain diamond crystal orientations, as e.g. Si(111), produce a bulk dipole SHG response. For fcc and bcc lattices with a single atom basis, i.e. for the most important metals, however, SHG can purely arise due to the disturbance induced by the surface. Finally we propose an experiment, exploiting the different dispersion for the fundamental as well as frequency doubled radiation to determine this effect.