The Structure of Liquid and Amorphous Hafnia
Understanding the atomic structure of amorphous solids is important in predicting and tuning their macroscopic behavior. Here, we use a combination of high-energy X-ray diffraction, neutron diffraction, and molecular dynamics simulations to benchmark the atomic interactions in the high temperature s...
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doaj-35abdd9510db458a9e226b72af63c3f72020-11-24T21:15:23ZengMDPI AGMaterials1996-19442017-11-011011129010.3390/ma10111290ma10111290The Structure of Liquid and Amorphous HafniaLeighanne C. Gallington0Yasaman Ghadar1Lawrie B. Skinner2J. K. Richard Weber3Sergey V. Ushakov4Alexandra Navrotsky5Alvaro Vazquez-Mayagoitia6Joerg C. Neuefeind7Marius Stan8John J. Low9Chris J. Benmore10X-ray Science Division, Argonne National Laboratory, Argonne, IL 60439, USAArgonne Leadership Computing Facility, Argonne National Laboratory, Argonne, IL 60439, USAX-ray Science Division, Argonne National Laboratory, Argonne, IL 60439, USAX-ray Science Division, Argonne National Laboratory, Argonne, IL 60439, USAPeter A. Rock Thermochemistry Laboratory and NEAT ORU, University of California at Davis, Davis, CA 95616, USAPeter A. Rock Thermochemistry Laboratory and NEAT ORU, University of California at Davis, Davis, CA 95616, USAArgonne Leadership Computing Facility, Argonne National Laboratory, Argonne, IL 60439, USAChemical and Engineering Materials Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830, USAGlobal Security Sciences, Argonne National Laboratory, Argonne, IL 60439, USAComputing, Environment and Life Sciences, Argonne National Laboratory, Argonne, IL 60439, USAX-ray Science Division, Argonne National Laboratory, Argonne, IL 60439, USAUnderstanding the atomic structure of amorphous solids is important in predicting and tuning their macroscopic behavior. Here, we use a combination of high-energy X-ray diffraction, neutron diffraction, and molecular dynamics simulations to benchmark the atomic interactions in the high temperature stable liquid and low-density amorphous solid states of hafnia. The diffraction results reveal an average Hf–O coordination number of ~7 exists in both the liquid and amorphous nanoparticle forms studied. The measured pair distribution functions are compared to those generated from several simulation models in the literature. We have also performed ab initio and classical molecular dynamics simulations that show density has a strong effect on the polyhedral connectivity. The liquid shows a broad distribution of Hf–Hf interactions, while the formation of low-density amorphous nanoclusters can reproduce the sharp split peak in the Hf–Hf partial pair distribution function observed in experiment. The agglomeration of amorphous nanoparticles condensed from the gas phase is associated with the formation of both edge-sharing and corner-sharing HfO6,7 polyhedra resembling that observed in the monoclinic phase.https://www.mdpi.com/1996-1944/10/11/1290X-ray diffractionneutron diffractionmolecular dynamicsliquid structureamorphous materialsnanoparticleshafnium oxide |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
Leighanne C. Gallington Yasaman Ghadar Lawrie B. Skinner J. K. Richard Weber Sergey V. Ushakov Alexandra Navrotsky Alvaro Vazquez-Mayagoitia Joerg C. Neuefeind Marius Stan John J. Low Chris J. Benmore |
spellingShingle |
Leighanne C. Gallington Yasaman Ghadar Lawrie B. Skinner J. K. Richard Weber Sergey V. Ushakov Alexandra Navrotsky Alvaro Vazquez-Mayagoitia Joerg C. Neuefeind Marius Stan John J. Low Chris J. Benmore The Structure of Liquid and Amorphous Hafnia Materials X-ray diffraction neutron diffraction molecular dynamics liquid structure amorphous materials nanoparticles hafnium oxide |
author_facet |
Leighanne C. Gallington Yasaman Ghadar Lawrie B. Skinner J. K. Richard Weber Sergey V. Ushakov Alexandra Navrotsky Alvaro Vazquez-Mayagoitia Joerg C. Neuefeind Marius Stan John J. Low Chris J. Benmore |
author_sort |
Leighanne C. Gallington |
title |
The Structure of Liquid and Amorphous Hafnia |
title_short |
The Structure of Liquid and Amorphous Hafnia |
title_full |
The Structure of Liquid and Amorphous Hafnia |
title_fullStr |
The Structure of Liquid and Amorphous Hafnia |
title_full_unstemmed |
The Structure of Liquid and Amorphous Hafnia |
title_sort |
structure of liquid and amorphous hafnia |
publisher |
MDPI AG |
series |
Materials |
issn |
1996-1944 |
publishDate |
2017-11-01 |
description |
Understanding the atomic structure of amorphous solids is important in predicting and tuning their macroscopic behavior. Here, we use a combination of high-energy X-ray diffraction, neutron diffraction, and molecular dynamics simulations to benchmark the atomic interactions in the high temperature stable liquid and low-density amorphous solid states of hafnia. The diffraction results reveal an average Hf–O coordination number of ~7 exists in both the liquid and amorphous nanoparticle forms studied. The measured pair distribution functions are compared to those generated from several simulation models in the literature. We have also performed ab initio and classical molecular dynamics simulations that show density has a strong effect on the polyhedral connectivity. The liquid shows a broad distribution of Hf–Hf interactions, while the formation of low-density amorphous nanoclusters can reproduce the sharp split peak in the Hf–Hf partial pair distribution function observed in experiment. The agglomeration of amorphous nanoparticles condensed from the gas phase is associated with the formation of both edge-sharing and corner-sharing HfO6,7 polyhedra resembling that observed in the monoclinic phase. |
topic |
X-ray diffraction neutron diffraction molecular dynamics liquid structure amorphous materials nanoparticles hafnium oxide |
url |
https://www.mdpi.com/1996-1944/10/11/1290 |
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