AbstractIntegrating epitaxial BaTiO3 (BTO) with Si is essential for leveraging its ferroelectric, piezoelectric, and nonlinear optical properties in microelectronics. Recently, heterogeneous integration approaches that involve growth of BTO on ideal substrates followed by transfer to a desired substrate show promise of achieving excellent device‐quality films. However, beyond simple demonstrations of the existence of ferroelectricity, robust devices with high endurance are not yet demonstrated on Si using the latter approach. Here, using a novel two‐step approach to synthesize epitaxial BTO using pulsed laser deposition on water‐soluble Sr3Al2O6 (on SrTiO3 substrates), successful integration of high‐quality BTO capacitors on Si is demonstrated, with remanent polarisation Pr = 7 µC cm−2, coercive field Ec = 150 kV cm−1, ferroelectric and electromechanical endurance of > 106 cycles. The study further addresses the challenge of cracking and disintegration of thicker films by first transferring a large area (5 mm x 5 mm) of the templated layer of BTO (≈30 nm thick) on the desired substrate, followed by the growth of high‐quality BTO on this substrate, as revealed by high‐resolution X‐ray diffraction (HRXRD) and high‐resolution scanning transmission electron microscopy (HRSTEM) measurements. These templated Si substrates offer a versatile platform for integrating any epitaxial complex oxides with diverse functionalities onto any inorganic substrate.
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