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Title: Neural network based analysis of multimodal bond distributions using extended x-ray absorption fine structure spectra

Journal Article · · Physical Review. B
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [3]; ORCiD logo [4]
  1. Univ. of Illinois at Urbana-Champaign, IL (United States)
  2. Univ. of Massachusetts, Lowell, MA (United States)
  3. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  4. Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
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Knowledge of the local coordination environment around atomic species in functional materials is critical for understanding their mechanisms of operation. Heterogeneous mixtures of metal complexes are ubiquitous in catalysts, ionic liquids, molten salts, biological enzymes, and geochemical systems, among many others. Extracting information from ensemble-average measurements about the structural and compositional descriptors of each type of coordination complex comprising the mixture is not generally possible, especially when they possess multimodal bond-length distributions. Here, we developed a method that enables the mapping of an x-ray absorption spectrum on the radial distribution function describing the average environment of the metal ions. The supervised neural network based method utilizes an objective training set, for which the choice of the local structural motifs is completely agnostic to the theoretically expected structure and dynamics of the modeled system. The method was validated using first-principles modeling of structural dynamics of nickel complexation in molten salts, and it applies to a large class of heterogeneous systems, including those studied under in situ and operando conditions.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Nuclear Energy (NE), Nuclear Energy University Program (NEUP); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC05-00OR22725; SC0012704; SC0022199; NE0009204
OSTI ID:
2376301
Journal Information:
Physical Review. B, Journal Name: Physical Review. B Journal Issue: 10 Vol. 109; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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