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Small molecules (typically, 3 to 5 atoms) of both natural and anthropogenic origin widely occur in Earth and planetary atmospheres as well as in planetary and interstellar ices, where they are continuously affected by solar and galactic radiation. The knowledge on the mechanisms of their radiation-induced transformations is of considerable significance for different areas, ranging from ecology and climatic aspects to extraterrestrial prebiotic evolution of matter. The matrix isolation technique was applied for characterization of intermediates resulting from the molecules of atmospheric and astrochemical importance during several decades. However, most of these studies were related to photochemistry and focused on spectroscopic aspects rather than reaction kinetics and mechanisms. This presentation gives an overview of recent model studies on the radiation-induced degradation and reactions of a number of small molecules presenting interest for astrochemistry and atmospheric chemistry (such as H2O, CO2, CH3OH, C2H2, HCN, and simple freons) carried out in our laboratory.