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Interfacial bond formation during sputter deposition of metal oxide thinfilms onto polycarbonate (PC) is investigated by ab initio molecular dynamicssimulations and X-ray photoelectron spectroscopy (XPS) analysis of PC | Xinterfaces (X = Al$_2$O$_3$, TiO$_2$, TiAlO$_2$). Generally, the predicted bondformation is consistent with the experimental data. For all three interfaces,the majority of bonds identified by XPS are (C-O)-metal bonds, whereas C-metalbonds are the minority. Compared to the PC | Al$_2$O$_3$ interface, the PC |TiO$_2$ and PC | TiAlO$_2$ interfaces exhibit a reduction in the measuredinterfacial bond density by ~ 75 and ~ 65%, respectively. Multiplying thepredicted bond strength with the corresponding experimentally determinedinterfacial bond density shows that Al$_2$O$_3$ exhibits the strongestinterface with PC, while TiO$_2$ and TiAlO$_2$ exhibit ~ 70 and ~ 60% weakerinterfaces, respectively. This can be understood by considering the complexinterplay between the metal oxide composition, the bond strength as well as thepopulation of bonds that are formed across the interface.

Bond formation at polycarbonate | X interfaces (X = Al$_2$O$_3$, TiO$_2$, TiAlO$_2$) studied by theory and experiments