Nanoscale Inhomogeneity and Epitaxial Strain Control Metallicity in Single Crystalline Thin Films of High Entropy Oxide

Abstract Understanding the electronic transport properties of thin films of high‐entropy oxide (HEO), having multiple elements at the same crystallographic site, is crucial for their potential electronic applications. However, very little is known about the metallic phase of HEOs even in bulk form. This work delves into the interplay between global and local structural distortion and electronic properties of single crystalline thin films of (La 0.2 Pr 0.2 Nd 0.2 Sm 0.2 Eu 0.2 )NiO 3 , which exhibit metal‐insulator transition under tensile strain. Employing electron microscopy and elemental resolved electron energy loss spectroscopy, we provide direct evidence of nanoscale chemical inhomogeneities at the rare‐earth site, leading to a broad distribution of Ni–O–Ni bond angles. However, the octahedral rotation pattern remains the same throughout. The metallic phase consists of insulating patches with more distorted Ni–O–Ni bond angles, responsible for higher resistance exponents with increased compositional complexity. Moreover, a rare, fully metallic state of HEO thin film is achieved under compressive strain. We further demonstrate a direct correlation between the suppression of the insulating behavior and increased electronic hopping. Our findings provide a foundation for exploring Mott‐Anderson electron localization physics in the high‐entropy regime.