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Our ability to design and fabricate electronic devices with reproducibleproperties using complex oxides is critically dependent on our ability tocontrollably synthesize these materials in thin-film form. Structure-propertyrelationships are intimately tied to film and interface composition. Here wereport on the effects of cation stoichiometry in LaCrO3 heteroepitaxial filmsprepared using molecular beam epitaxy. We show that LaCrO3 films growpseudomorphically on SrTiO3(001) over a wide range of La-to-Cr atom ratios.However, the growth mode and structural quality are sensitive to the La-to-Crratio, with La-rich films being of considerably lower structural quality thanCr-rich films. Cation mixing occurs at the interface for all La-to-Cr ratiosinvestigated, and is not quenched by deposition at ambient temperature.Indiffused La atoms occupy Sr sites in the substrate. The presence of defectsin the SrTiO3 substrate is implicated in promoting La indiffusion by comparingthe properties of LaCrO3/SrTiO3 with those of LaCrO3/Si, both prepared atambient temperature. Additionally, pulsed laser deposition is shown to resultin more extensive interfacial mixing than molecular beam epitaxy for depositionat ambient temperature on Si.

Cation nonstoichiometry and its impact on nucleation, structure and defect formation in complex oxide heteroepitaxy : LaCrO3 on SrTiO3(001)