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Abstract Strong coupling between polarization (P) and strain (ɛ) in ferroelectric complex oxides offers unique opportunities to dramatically tune their properties. Here colossal strain tuning of ferroelectricity in epitaxial KNbO3thin films grown by sub‐oxide molecular beam epitaxy is demonstrated. While bulk KNbO3exhibits three ferroelectric transitions and a Curie temperature (Tc) of ≈676 K, phase‐field modeling predicts that a biaxial strain of as little as −0.6% pushes itsTc> 975 K, its decomposition temperature in air, and for −1.4% strain, toTc> 1325 K, its melting point. Furthermore, a strain of −1.5% can stabilize a single phase throughout the entire temperature range of its stability. A combination of temperature‐dependent second harmonic generation measurements, synchrotron‐based X‐ray reciprocal space mapping, ferroelectric measurements, and transmission electron microscopy reveal a single tetragonal phase from 10 K to 975 K, an enhancement of ≈46% in the tetragonal phase remanent polarization (Pr), and a ≈200% enhancement in its optical second harmonic generation coefficients over bulk values. These properties in a lead‐free system, but with properties comparable or superior to lead‐based systems, make it an attractive candidate for applications ranging from high‐temperature ferroelectric memory to cryogenic temperature quantum computing.
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This content will become publicly available on February 11, 2026
Strain Effects in SrHfO 3 Films Grown by Hybrid Molecular Beam Epitaxy
Perovskite oxide heterostructures host a large number of interesting phenomena such as ferroelectricity, which are often driven by octahedral distortions in the crystal that may induce polarization. SrHfO3 (SHO) is a perovskite oxide with a pseudocubic lattice parameter of 4.08 Å that previous density functional theory (DFT) calculations suggest can be stabilized in a ferroelectric P4mm phase when stabilized with sufficient compressive strain. Additionally, it is insulating and possesses a large band gap and a high dielectric constant, making it an ideal candidate for oxide electronic devices. To test the viability of epitaxial strain as a driver of ferroic phase transitions, SHO films were grown by hybrid molecular beam epitaxy (hMBE) with a tetrakis(ethylmethylamino)hafnium(IV) source on GdScO3 and TbScO3 substrates. Strained SHO phases were characterized using X-ray diffraction, X-ray absorption spectroscopy, and scanning transmission electron microscopy to determine the space group of the strained films, with the results compared to those of DFT-optimized models of phase stability versus strain. Contrary to past reports, we find that compressively strained SrHfO3 undergoes octahedral tilt distortions without associated ferroelectric polarization and most likely takes on the I4/mcm phase with the a0a0c– tilt pattern.
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- PAR ID:
- 10575059
- Publisher / Repository:
- American Chemical Society
- Date Published:
- Journal Name:
- ACS Applied Electronic Materials
- Volume:
- 7
- Issue:
- 3
- ISSN:
- 2637-6113
- Page Range / eLocation ID:
- 983 to 996
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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