Searching for a route to synthesize in situ epitaxial Pr₂Ir₂O₇ thin films with thermodynamic methods

In situ growth of pyrochlore iridate thin films has been a long-standing challenge due to the low reactivity of Ir at low temperatures and the vaporization of volatile gas species such as IrO₃(g) and IrO₂(g) at high temperatures and high P_O2. To address this challenge, we combine thermodynamic analysis of the Pr-Ir-O₂ system with experimental results from the conventional physical vapor deposition (PVD) technique of co-sputtering. Our results indicate that only high growth temperatures yield films with crystallinity sufficient for utilizing and tailoring the desired topological electronic properties and the in situ synthesis of Pr₂Ir₂O₇ thin films is fettered by the inability to grow with P_O2 on the order of 10 Torr at high temperatures, a limitation inherent to the PVD process. Thus, we suggest techniques capable of supplying high partial pressure of key species during deposition, in particular chemical vapor deposition (CVD), as a route to synthesis of Pr₂Ir₂O₇.