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By combining structural and chemical thin film analysis with detailed plume diagnostics and modeling of the laser plume dynamics, we are able to elucidate the different physical mechanisms determining the stoichiometry of the complex oxides model material SrTiO3 during pulsed laser deposition. Deviations between thin film and target stoichiometry are basically a result of two effects, namely, incongruent ablation and preferential scattering of lighter ablated species during their motion towards the substrate in the O2 background gas. On the one hand, a progressive preferential ablation of the Ti species with increasing laser fluence leads to a regime of Ti-rich thin film growth at larger fluences. On the other hand, in the low laser fluence regime, a more effective scattering of the lighter Ti plume species results in Sr rich films.

Pulsed laser ablation of complex oxides: The role of congruent ablation and preferential scattering for the film stoichiometry