Direct Visualization of Localized Vibrations at Complex Grain Boundaries

Eric R. Hoglund, De Liang Bao, Andrew O'Hara, Thomas W. Pfeifer, Md Shafkat Bin Hoque, Sara Makarem, James M. Howe, Sokrates T. Pantelides, Patrick E. Hopkins, Jordan A. Hachtel

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20 Scopus citations

Abstract

Grain boundaries (GBs) are a prolific microstructural feature that dominates the functionality of a wide class of materials. The functionality at a GB results from the unique atomic arrangements, different from those in the grain, that have driven extensive experimental and theoretical studies correlating atomic-scale GB structures to macroscopic electronic, infrared optical, and thermal properties. In this work, a SrTiO3 GB is examined using atomic-resolution aberration-corrected scanning transmission electron microscopy and ultrahigh-energy-resolution monochromated electron energy-loss spectroscopy, in conjunction with density functional theory. This combination enables the correlation of the GB structure, nonstoichiometry, and chemical bonding with a redistribution of vibrational states within the GB dislocation cores. The new experimental access to localized GB vibrations provides a direct route to quantifying the impact of individual boundaries on macroscopic properties.

Original languageEnglish
Article number2208920
JournalAdvanced Materials
Volume35
Issue number13
DOIs
StatePublished - Mar 29 2023

Funding

E.R.H. and D.‐L.B. contributed equally to this work. Monochromated EELS research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a DOE Office of Science User Facility using instrumentation within ORNL's Materials Characterization Core provided by UT‐Battelle, LLC, under Contract No. DE‐AC05‐ 00OR22725 with the DOE and sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT‐Battelle, LLC, for the U.S. Department of Energy. Aberration‐corrected drift‐corrected STEM imagining and core‐loss EELS were supported by the Army Research Office, Grant No. W911NF‐21‐1‐0119. Utilization of the Thermo Fisher Scientific Themis‐Z STEM and Helios dual‐beam focus ion beam instruments within UVa's Nanoscale Materials Characterization Facility (NMCF) was fundamental to this work. The authors thank Helge Heinrich for aiding in TEM sample preparation. Theory at Vanderbilt University (D.‐L.B., A.O., and S.T.P.) was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Directorate Grant No. DE‐FG02‐09ER46554 and by the McMinn Endowment at Vanderbilt University. D.‐L.B. was partially supported by the K. C. Wong Education Foundation of the Chinese Academy of Sciences. Calculations were performed at the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE‐AC02‐05CH11231.

Keywords

  • dislocations
  • grain boundaries
  • local atomic vibrations
  • phonons
  • vibrational states

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