Expanding the Synthesis Space of Complex Oxide Heterostructures: Growth Strategies for Precise Stoichiometry Control during Pulsed Laser Deposition

Advances in complex oxide heterostructures have revealed a wealth of emergent phenomena arising from the delicate interplay of lattice, charge, orbital, and spin degrees of freedom at interfaces. Realizing and controlling these effects, however, demand synthesis approaches that go beyond conventional epitaxy. In this talk, I will discuss strategies that expand the accessible synthesis space for complex oxide interfaces through the use of high-temperature and off-axis growth techniques, coupled with precise stoichiometry control. High-temperature growth enables enhanced adatom mobility and thermodynamic stability, opening access to metastable phases and improved crystalline quality. Off-axis deposition geometries allow for the creation of spatially graded materials libraries, offering a powerful route to explore compositional phase diagrams and optimize growth parameters in a single experiment. These methods are integrated with in situ diagnostics and feedback control to dynamically tune stoichiometry during growth. Together, these approaches provide a framework for deterministic synthesis of oxide heterostructures with tailored functionalities. I will highlight recent examples, focussing on for instance BaTiO₃ and Pb(Zr,Ti)O₃, and discuss their broader implications for designing correlated and quantum oxide materials.