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Control over the concurrent occurrence of structural (monoclinic to tetragonal) and electrical (insulator to the conductor) transitions presents a formidable challenge for VO₂-based thin film devices. Speed, lifetime, and reliability of these devices can be significantly improved by utilizing solely electrical transition while eliminating structural transition. We design a novel strain-stabilized isostructural VO₂epitaxial thin-film system where the electrical transition occurs without any observable structural transition. The thin-film heterostructures with a completely relaxed NiO buffer layer have been synthesized allowing complete control over strains in VO₂films. The strain trapping in VO₂thin films occurs below a critical thickness by arresting the formation of misfit dislocations. We discover the structural pinning of the monoclinic phase in (10 ± 1 nm) epitaxial VO₂films due to bandgap changes throughout the whole temperature regime as the insulator-to-metal transition occurs. Using density functional theory, we calculate that the strain in monoclinic structure reduces the difference between long and short V-V bond-lengths (Δ_V−V) in monoclinic structures which leads to a systematic decrease in the electronic bandgap of VO₂. This decrease in bandgap is additionally attributed to ferromagnetic ordering in the monoclinic phase to facilitate a Mott insulator without going through the structural transition.

This work provides the details of a simple and reliable method with less damage to prepare electron transparent samples for in situ studies in scanning/transmission electron microscopy. In this study, we use epitaxial VO₂thin films grown on c‐Al₂O₃by pulsed laser deposition, which have a monoclinic–rutile transition at ~68°C. We employ an approach combining conventional mechanical wedge‐polishing and Focused Ion beam to prepare the electron transparent samples of epitaxial VO₂thin films. The samples are first mechanically wedge‐polished and ion‐milled to be electron transparent. Subsequently, the thin region of VO₂films are separated from the rest of the polished sample using a focused ion beam and transferred to the in situ electron microscopy test stage. As a critical step, carbon nanotubes are used as connectors to the manipulator needle for a soft transfer process. This is done to avoid shattering of the brittle substrate film on the in situ sample support stage during the transfer process. We finally present the atomically resolved structural transition in VO₂films using this technique. This approach significantly increases the success rate of high‐quality sample preparation with less damage for in situ studies of thin films and reduces the cost and instrumental/user errors associated with other techniques.

The present work highlights a novel, simple, reliable approach with reduced damage to make electron transparent samples for atomic‐scale insights of temperature‐dependent transitions in epitaxial thin film heterostructures using in situ TEM studies.