Chemically‐Disordered Transparent Conductive Perovskites With High Crystalline Fidelity

Kinetically arrested, chemically disordered perovskite thin films exhibit exquisite crystalline fidelity, broad IR–UV transparency, and low resistivity, despite incorporating five mismatched 3d–5d cations, including Cr and W. This study unites electronic correlation, cation diversity, valence complexity, and disorder—enabling new transparent conductors and paving the way toward novel quantum and spintronic applications. Abstract 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. This work demonstrates 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 thin and thick epitaxial layers. This combination produces an optical transparency window that surpasses that of the constituent end‐members in the UV and IR, while maintaining relatively low electrical resistivity. This work addresses 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 and their interactions – though unavailable to them – thus offering performance advances in optical, high‐frequency, spintronic, and quantum devices. Kinetically arrested, chemically disordered perovskite thin films exhibit exquisite crystalline fidelity, broad IR–UV transparency, and low resistivity, despite incorporating five mismatched 3d–5d cations, including Cr and W. This study unites electronic correlation, cation diversity, valence complexity, and disorder—enabling new transparent conductors and paving the way toward novel quantum and spintronic applications. Abstract 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. This work demonstrates this new learning in epitaxial Sr x (Ti,Cr,Nb,Mo,W)O 3 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 thin and thick epitaxial layers. This combination produces an optical transparency window that surpasses that of the constituent end-members in the UV and IR, while maintaining relatively low electrical resistivity. This work addresses 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 and their interactions – though unavailable to them – thus offering performance advances in optical, high-frequency, spintronic, and quantum devices. Advanced Science, Volume 12, Issue 42, November 13, 2025.