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Controllable interfacial strain can manipulate the physical properties of epitaxial films and help understand the physical nature of the correlation between the properties and the atomic microstructures. By using a proper design of vicinal single-crystal substrate, the interface strain in epitaxial thin films can be well controlled by adjusting the miscut angle via a surface-step-terrace matching growth mode. Here, we demonstrate that LaAlO 3  (LAO) substrates with various miscut angles of 1.0°, 2.75°, and 5.0° were used to tune the dielectric properties of epitaxial CaCu 3 Ti 4 O 12  (CCTO) thin films. A model of coexistent compressive and tensile strained domains is proposed to understand the epitaxial nature. Our findings on the self-tuning of the compressive and tensile strained domain ratio along the interface depending on the miscut angle and the stress relaxation mechanism under this growth mode will open a new avenue to achieve CCTO films with high dielectric constant and low dielectric loss, which is critical for the design and integration of advanced heterostructures for high performance capacitance device applications.

Surface step terrace tuned microstructures and dielectric properties of highly epitaxial CaCu3Ti4O12 thin films on vicinal LaAlO3 substrates