The Structure of Liquid and Amorphous Hafnia

Gallington, Leighanne; Ghadar, Yasaman; Skinner, Lawrie; Weber, J.; Ushakov, Sergey; Navrotsky, Alexandra; Vazquez-Mayagoitia, Alvaro; Neuefeind, Joerg; Stan, Marius; Low, John; Benmore, Chris

doi:10.3390/ma10111290

Title: The Structure of Liquid and Amorphous Hafnia

Journal Article · Fri Nov 10 00:00:00 EST 2017 · Materials

DOI:https://doi.org/10.3390/ma10111290· OSTI ID:1422595

Gallington, Leighanne ^[1]; Ghadar, Yasaman ^[2]; Skinner, Lawrie ^[1]; Weber, J. ^[1]; Ushakov, Sergey ^[3]; Navrotsky, Alexandra ^[3]; Vazquez-Mayagoitia, Alvaro ^[2]; Neuefeind, Joerg ^[4]; Stan, Marius ^[5]; Low, John ^[6]; Benmore, Chris ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
Argonne National Lab. (ANL), Argonne, IL (United States). Argonne Leadership Computing Facility
Univ. of California, Davis, CA (United States). Peter A. Rock Thermochemistry Lab. NEAT ORU
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
Argonne National Lab. (ANL), Argonne, IL (United States). Global Security Sciences
Argonne National Lab. (ANL), Argonne, IL (United States). Computing, Environment and Life Sciences

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 HfO_6,7 polyhedra resembling that observed in the monoclinic phase.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of California, Davis, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); ANL Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; 1506229

OSTI ID:: 1422595

Journal Information:: Materials, Vol. 10, Issue 11; ISSN 1996-1944

Publisher:: MDPICopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 22 works

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