Metastable polar orthorhombic local structure of hydrothermally grown HfO2 nanocrystals
Cell Reports Physical Science(2024)
摘要
Metastable polymorphs of periodic solids manifest atomic connectivities that represent local minima in free energy landscapes. Upon scaling to nanometer-sized dimensions, surface and stress energy can modify phase stabilities, providing a means of accessing metastable polymorphs that exhibit distinctive function. The recent discovery of the non-centrosymmetric orthorhombic phase of HfO2 in strained and doped thin films has generated considerable excitement, given that it may enable scalable ferroelectric devices for energy-efficient computing. In this work, we prepare HfO2 nanocrystals ca. 6 nm in diameter using a hydrothermal process. Total scattering and extended X-ray absorption fine-structure analyses are used to probe the local structure of the prepared nanocrystals. The measurements indicate that hydrothermally prepared HfO2 nanocrystals adopt a kinetically trapped orthorhombic local structure. The results demonstrate the rich landscape of crystal structures accessible for binary transition-metal oxides and the sensitivity of ultra-small nanocrystals to surface stresses and polarization.
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关键词
polar orthorhombic structure,ferroelectricity,nanocrystal,hafnium oxide,pair distribution function,extended X-ray absorption fine structure
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