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Pressure-Induced Amorphization in Single-Crystal Ta2O5 Nanowires: A Kinetic Mechanism and Improved Electrical Conductivity

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† High Pressure Science and Engineering Center, University of Nevada, Las Vegas, Nevada 89154, United States
‡ High Pressure Synergetic Consortium, Geophysical Laboratory, Carnegie Institution of Washington, Argonne, Illinois 60439, United States
§ School of Physics, Astronomy, and Computational Sciences, George Mason University, Fairfax, Virginia 22030, United States
∥ CAS Key Laboratory of Materials for Energy Conversion, Shanghai Institute of Ceramics, Chinese Academy of Sciences (CAS), Shanghai 200050, People’s Republic of China
⊥ Electron Microscopy Center, Argonne National Laboratory, Argonne, Illinois 60439, United States
[email protected]
[email protected]
[email protected]
Cite this: J. Am. Chem. Soc. 2013, 135, 37, 13947–13953
Publication Date (Web):August 22, 2013
https://doi.org/10.1021/ja407108u
Copyright © 2013 American Chemical Society
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Abstract

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Pressure-induced amorphization (PIA) in single-crystal Ta2O5 nanowires is observed at 19 GPa, and the obtained amorphous Ta2O5 nanowires show significant improvement in electrical conductivity. The phase transition process is unveiled by monitoring structural evolution with in situ synchrotron X-ray diffraction, pair distribution function, Raman spectroscopy, and transmission electron microscopy. The first principles calculations reveal the phonon modes softening during compression at particular bonds, and the analysis on the electron localization function also shows bond strength weakening at the same positions. On the basis of the experimental and theoretical results, a kinetic PIA mechanism is proposed and demonstrated systematically that amorphization is initiated by the disruption of connectivity between polyhedra (TaO6 octahedra or TaO7 bipyramids) at the particular weak-bonding positions along the a axis in the unit cell. The one-dimensional morphology is well-preserved for the pressure-induced amorphous Ta2O5, and the electrical conductivity is improved by an order of magnitude compared to traditional amorphous forms. Such pressure-induced amorphous nanomaterials with unique properties surpassing those in either crystalline or conventional amorphous phases hold great promise for numerous applications in the future.

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Details of the pair distribution function analysis, four-probe resistance measurement, characterizations of pristine Ta2O5 nanowires, Raman spectra, XRD patterns decompressed from a maximum pressure of 19.2 GPa, TEM images of Ta2O5 nanowires decompressed from 51.8 and 19.2 GPa, FFT patterns from three selected areas of the HRTEM image, phonon mode calculation results, and statistical analysis of bond distances in the orthorhombic Ta2O5 unit cell. This material is available free of charge via the Internet at http://pubs.acs.org.

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