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Anisotropically nanostructured silicon layers exhibit a strong in-plane birefringence. Their optical anisotropy parameters are found to be extremely sensitive to the presence of dielectric substances inside of the pores. Polarization-resolved transmittance measurements provide an extremely sensitive tool to analyze the adsorption of various atoms and molecules in negligible quantities. A variation of the transmitted linearly polarized light intensity up to two orders of magnitude combined with a fast optical response in the range of seconds make these layers a good candidate for sensor applications. © 2001 American Institute of Physics.