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Title: Deciphering chemical order/disorder and material properties at the single-atom level

Perfect crystals are rare in nature. Real materials often contain crystal defects and chemical order/disorder such as grain boundaries, dislocations, interfaces, surface reconstructions and point defects. Such disruption in periodicity strongly affects material properties and functionality. Despite rapid development of quantitative material characterization methods, correlating three-dimensional (3D) atomic arrangements of chemical order/disorder and crystal defects with material properties remains a challenge. On a parallel front, quantum mechanics calculations such as density functional theory (DFT) have progressed from the modelling of ideal bulk systems to modelling ‘real’ materials with dopants, dislocations, grain boundaries and interfaces; but these calculations rely heavily on average atomic models extracted from crystallography. To improve the predictive power of first-principles calculations, there is a pressing need to use atomic coordinates of real systems beyond average crystallographic measurements. Here we determine the 3D coordinates of 6,569 iron and 16,627 platinum atoms in an iron-platinum nanoparticle, and correlate chemical order/disorder and crystal defects with material properties at the single-atom level. We identify rich structural variety with unprecedented 3D detail including atomic composition, grain boundaries, anti-phase boundaries, anti-site point defects and swap defects. We show that the experimentally measured coordinates and chemical species with 22 picometre precision can be usedmore » as direct input for DFT calculations of material properties such as atomic spin and orbital magnetic moments and local magnetocrystalline anisotropy. The work presented here combines 3D atomic structure determination of crystal defects with DFT calculations, which is expected to advance our understanding of structure–property relationships at the fundamental level.« less
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [1] ;  [1] ;  [1] ;  [5] ;  [6] ;  [1] ;  [7] ;  [8] ;  [9] ;  [5] ;  [4] ;  [1]
  1. Univ. of California, Los Angeles, CA (United States). Dept. of Physics and Astronomy and California NanoSystems Inst.
  2. Univ. of California, Los Angeles, CA (United States). Dept. of Physics and Astronomy and California NanoSystems Inst.; National Sun Yat-sen Univ., Kaohslung (Taiwan). Dept. of Physics
  3. Univ. of California, Los Angeles, CA (United States). Dept. of Physics and Astronomy and California NanoSystems Inst.; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Center for Electron Microscopy
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Center for Electron Microscopy
  5. State Univ. of New York (SUNY), Buffalo, NY (United States). Dept. of Physics
  6. Univ. of Birmingham (United Kingdom). Schol of Physics and Astronomy and Nanoscale Physics Research Lab.
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). national Center for Computational Sciences
  8. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Computer Science and Mathematics Division and Center for Nanophase Materials Sciences
  9. Univ. of Nebraska, Omaha, NE (United States). Dept. of Physics
Publication Date:
Grant/Contract Number:
AC05-00OR22725; SC0010378; DMR-1548924; DMR-1437263; DARPA-BAA-12-63; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 542; Journal Issue: 7639; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); Defense Advanced Research Projects Agency (DARPA)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 74 ATOMIC AND MOLECULAR PHYSICS; imaging techniques; magnetic materials; magnetic properties and materials; structural properties
OSTI Identifier:
1342669
Alternate Identifier(s):
OSTI ID: 1436148