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Defect engineering has brought about a unique level of control for Si-basedsemiconductors, leading to the optimization of various opto-electronicproperties and devices. With regard to perovskite transition metal oxides,oxygen vacancies have been a key ingredient in defect engineering, as they playa central role in determining the crystal field and consequent electronicstructure, leading to important electronic and magnetic phase transitions.Therefore, experimental approaches toward understanding the role of defects incomplex oxides have been largely limited to controlling oxygen vacancies. Inthis study, we report on the selective formation of different types ofelemental vacancies and their individual roles in determining the atomic andelectronic structure of perovskite SrTiO3 (STO) homoepitaxial thin filmsfabricated by pulsed laser epitaxy. Structural and electronic transitions havebeen achieved via selective control of the Sr and oxygen vacancyconcentrations, respectively, indicating a decoupling between the two phasetransitions. In particular, oxygen vacancies were responsible formetal-insulator transitions, but did not influence the Sr vacancy inducedcubic-to-tetragonal structural transition in epitaxial STO thin film. Theindependent control of multiple phase transitions in complex oxides byexploiting selective vacancy engineering opens up an unprecedented opportunitytoward understanding and customizing complex oxide thin films.

Phase transitions via selective elemental vacancy engineering in complex oxide thin films