This manuscript presents a working model linking chemical disorder and transport properties in correlated-electron perovskites with high-entropy formulations and a framework to actively design them. We demonstrate this new learning in epitaxial Srx(Ti,Cr,Nb,Mo,W)O3 thin films that exhibit exceptional crystalline fidelity despite a diverse chemical formulation where most B-site species are highly misfit with respect to valence and radius. X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy confirm a unique combination of chemical disorder and structural perfection in thick epitaxial layers. This combination produces significant electron correlation, low electrical resistivity, and an optical transparency window that surpasses that of constituent end-members, with a flattened frequency- and temperature-dependent response. We address the computational challenges of modeling such systems and investigate short-range ordering using cluster expansion. These results showcase that unusual d-metal combinations access an expanded property design space that is predictable using end-member characteristics -- though unavailable to them -- thus offering performance advances in optical, spintronic, and quantum devices.
@article{arxiv.2501.09193,
title = {Chemically-Disordered Transparent Conductive Perovskites with High Crystalline Fidelity},
author = {Saeed S. I. Almishal and Pat Kezer and Yasuyuki Iwabuchi and Jacob T. Sivak and Sai Venkata Gayathri Ayyagari and Saugata Sarker and Matthew Furst and Gerald Bejger and Billy Yang and Simon Gelin and Nasim Alem and Ismaila Dabo and Christina M. Rost and Susan B. Sinnott and Vincent Crespi and Venkatraman Gopalan and Roman Engel-Herbert and John T. Heron and Jon-Paul Maria},
journal= {arXiv preprint arXiv:2501.09193},
year = {2025}
}