Stabilizing metastable tetragonal HfO2 using a non-hydrolytic solution-phase route: ligand exchange as a means of controlling particle size

Chemical Science
Gregory R WaetzigSarbajit Banerjee

Abstract

There has been intense interest in stabilizing the tetragonal phase of HfO2 since it is predicted to outperform the thermodynamically stable lower-symmetry monoclinic phase for almost every application where HfO2 has found use by dint of its higher dielectric constant, bandgap, and hardness. However, the monoclinic phase is much more thermodynamically stable and the tetragonal phase of HfO2 is generally accessible only at temperatures above 1720 °C. Classical models comparing the competing influences of bulk free energy and specific surface energy predict that the tetragonal phase of HfO2 ought to be stable at ultra-small dimensions below 4 nm; however, these size regimes have been difficult to access in the absence of synthetic methods that yield well-defined and monodisperse nanocrystals with precise control over size. In this work, we have developed a modified non-hydrolytic condensation method to precisely control the size of HfO2 nanocrystals with low concentrations of dopants by suppressing the kinetics of particle growth by cross-condensation with less-reactive precursors. This synthetic method enables us to stabilize tetragonal HfO2 while evaluating ideas for critical size at which surface energy considerations surpass ...Continue Reading

References

Jun 6, 2003·Journal of the American Chemical Society·Jin JooTaeghwan Hyeon
Jul 12, 2011·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Alexandra Navrotsky
Jul 19, 2011·Nature Materials·Rahul MalikG Ceder
Jun 25, 2013·Journal of the American Chemical Society·Mark A LukowskiSong Jin

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Citations

Nov 29, 2016·Physical Chemistry Chemical Physics : PCCP·Qilin GuJohn Wang
May 13, 2017·Nature Communications·Bethany M HudakBeth S Guiton
Apr 1, 2019·Acta Crystallographica Section B, Structural Science, Crystal Engineering and Materials·Scott J McCormack, Waltraud M Kriven

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Methods Mentioned

BETA
X-ray
transmission electron microscopy

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