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A model system for the photoinduced rearrangement of adsorbates in molecular sieves—composites that hold promise as materials with new electronic and optical properties—is the photoinduced cis–trans isomerization of azobenzene (Az) in the zeolites AIPO4-5, ZSM-5, and silicalite −1. A spectroscopic investigation presented demonstrates that reversible intrazeolite isomerization of Az causes large changes in the optical properties of the composites, e.g., in absorbance and birefringence, making the materials of interest for optical switching.