Enhanced Nonlinear-Optical Interactions in Nanostructured Semiconductors V. Yu. Timoshenko, L. A. Golovan, S. V. Zabotnov, V. A. Melnikov, A. Zheltikov, and P. K. Kashkarov Moscow State M.V. Lomonosov University, Faculty of Physics, 119992 Moscow, Russia Phone/Fax: +7(095)9391566, E-mail: vtim@vega.phys.msu.su Novel artificial photonic and nonlinear optical media can be formed by nanostructuring bulk semiconductors. We report on linear and non-linear optical properties of electrochemically prepared porous Si (PSi) and porous GaP. These materials are composed from nanocrystals and nanopores whose dimensions can be tuned from several nanometers to several micrometers by using different preparation conditions, e.g. substrate doping level, etching duration and current density. PSi layers formed from low symmetry c-Si wafers are found to exhibit optical properties of uniaxial birefringent crystals operating in visible and infrared spectral range. Both the birefringence and dichroism are explained by the form anisotropy of Si nanocrystals assembling PSi layers. The optical axis direction and birefringence value depend on the crystallographic orientation of Si substrate and PSi preparation conditions. The inplane birefringence of (110) PSi layers can be strong enough to compensate for the normal dispersion of material in the visible and middle IR ranges. This remarkable fact allows phase-matched nonlinear optical wave interactions in the birefringent PSi to be achieved. Additionally, an increase of the nonlinear optical susceptibility and modifications of its anisotropy parameter are possible for the birefringent PSi because of the local electric fields in ensembles of anisotropically shaped Si nanocrystals. An enhancement of the effective nonlinear optical susceptibilities is possible in macroporous GaP because of the light localization phenomenon.