Exploratory studies have been conducted to probe competitive H-atom abstraction and SET- promoted, silyl-transfer reactions of excited states of silylalkyl ketones and (silylalkyl) phthalimides. Photochemical investigations with the (silylalkyl) phthalimides have demonstrated that typical γ-H atom abstraction reactions occur upon irradiation in less polar and less silophilic solvents. In contrast, irradiation of these substances in polar-protic- ...