Synthesis of (111) oriented films of rare-earth pyrochlore titanates with sub-unit cell precision

Frustrated rare-earth pyrochlore titanates have been introduced as promising candidates to realize quantum spin ice (QSI) with a 2-in-2-out magnetic ordering as its ground state. The realization of this class of materials in the thin-film form, especially as heterostructures, has been predicted to result in the unusual magnetic states stemming from the interfacial magnetism combined with the oriented Kagome-triangular frustrated lattice. Here, we report the successful layer-by-layer growth of high-quality thin films of the frustrated quantum pyrochlores, R₂Ti₂O₇ (R = Er, Yb, and Tb), along the (111) direction. We confirmed their high crystallinity and proper chemical composition, discovered a robust mode of growth, and observed a pressure-sensitive growth for Tb₂Ti₂O₇. The availability of large area (111)-oriented QSI structures with planar geometry offers a new complementary to the bulk platform.