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The irreversibly bound interfacial layer deposited by the y-aminopropysilanetriol adhesion promoter onto a crystalline silicon substrate, which remains even after profuse washing, was found by XPS to have resulted from the fragmentation and rearrangement of the original y-aminopropylsilanetriol molecule. A mechanism is proposed, involving the homolytic scission of the terminal N-C bond. One of the subsequent reactions is believed to involve hydrogen loss by abstraction and the formation of a terminal vinyl group. which bonds to the substrate. Support for this mechanism is found in IR spectroscopy of this layer.KEY WORDS amine-terminated silane ester adhesion promoter; irreversibly bound surface layer; surface analysis; infrared spectroscopy; homolytic bond scission; fragmentation and rearrangement.