skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Real-time atomistic observation of structural phase transformations in individual hafnia nanorods

Abstract

High-temperature phases of hafnium dioxide have exceptionally high dielectric constants and large bandgaps, but quenching them to room temperature remains a challenge. Scaling the bulk form to nanocrystals, while successful in stabilizing the tetragonal phase of isomorphous ZrO 2, has produced nanorods with a twinned version of the room temperature monoclinic phase in HfO 2. Here we use in situ heating in a scanning transmission electron microscope to observe the transformation of an HfO 2 nanorod from monoclinic to tetragonal, with a transformation temperature suppressed by over 1000°C from bulk. When the nanorod is annealed, we observe with atomic-scale resolution the transformation from twinned-monoclinic to tetragonal, starting at a twin boundary and propagating via coherent transformation dislocation; the nanorod is reduced to hafnium on cooling. Unlike the bulk displacive transition, nanoscale size-confinement enables us to manipulate the transformation mechanism, and we observe discrete nucleation events and sigmoidal nucleation and growth kinetics.

Authors:
 [1];  [2];  [3];  [4];  [4];  [3];  [5]
  1. Univ. of Kentucky, Lexington, KY (United States). Dept. of Chemistry
  2. Univ. at Buffalo, NY (United States). Dept. of Chemistry
  3. Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry. Dept. of Materials Science and Engineering
  4. Texas A & M Univ., College Station, TX (United States). Dept. of Materials Science and Engineering
  5. Univ. of Kentucky, Lexington, KY (United States). Dept. of Chemistry; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Aeronautic and Space Administration (NASA); National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR)
Contributing Org.:
Univ. at Buffalo, NY (United States)
OSTI Identifier:
1376500
Grant/Contract Number:
AC05-00OR22725; NNX10AL96H; DMR-1504702; DMR-1455154; CMMI-1534534; FA9550-16-1-0180
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; nanoparticles; structural properties; transmission electron microscopy

Citation Formats

Hudak, Bethany M., Depner, Sean W., Waetzig, Gregory R., Talapatra, Anjana, Arroyave, Raymundo, Banerjee, Sarbajit, and Guiton, Beth S.. Real-time atomistic observation of structural phase transformations in individual hafnia nanorods. United States: N. p., 2017. Web. doi:10.1038/ncomms15316.
Hudak, Bethany M., Depner, Sean W., Waetzig, Gregory R., Talapatra, Anjana, Arroyave, Raymundo, Banerjee, Sarbajit, & Guiton, Beth S.. Real-time atomistic observation of structural phase transformations in individual hafnia nanorods. United States. doi:10.1038/ncomms15316.
Hudak, Bethany M., Depner, Sean W., Waetzig, Gregory R., Talapatra, Anjana, Arroyave, Raymundo, Banerjee, Sarbajit, and Guiton, Beth S.. Fri . "Real-time atomistic observation of structural phase transformations in individual hafnia nanorods". United States. doi:10.1038/ncomms15316. https://www.osti.gov/servlets/purl/1376500.
@article{osti_1376500,
title = {Real-time atomistic observation of structural phase transformations in individual hafnia nanorods},
author = {Hudak, Bethany M. and Depner, Sean W. and Waetzig, Gregory R. and Talapatra, Anjana and Arroyave, Raymundo and Banerjee, Sarbajit and Guiton, Beth S.},
abstractNote = {High-temperature phases of hafnium dioxide have exceptionally high dielectric constants and large bandgaps, but quenching them to room temperature remains a challenge. Scaling the bulk form to nanocrystals, while successful in stabilizing the tetragonal phase of isomorphous ZrO2, has produced nanorods with a twinned version of the room temperature monoclinic phase in HfO2. Here we use in situ heating in a scanning transmission electron microscope to observe the transformation of an HfO2 nanorod from monoclinic to tetragonal, with a transformation temperature suppressed by over 1000°C from bulk. When the nanorod is annealed, we observe with atomic-scale resolution the transformation from twinned-monoclinic to tetragonal, starting at a twin boundary and propagating via coherent transformation dislocation; the nanorod is reduced to hafnium on cooling. Unlike the bulk displacive transition, nanoscale size-confinement enables us to manipulate the transformation mechanism, and we observe discrete nucleation events and sigmoidal nucleation and growth kinetics.},
doi = {10.1038/ncomms15316},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {Fri May 12 00:00:00 EDT 2017},
month = {Fri May 12 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 4works
Citation information provided by
Web of Science

Save / Share: