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Molecular Dynamics Simulations and XAFS (MD-XAFS)

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XAFS Techniques for Catalysts, Nanomaterials, and Surfaces

Abstract

MD-XAFS (Molecular Dynamics X-ray Adsorption Fine Structure) makes the connection between simulation techniques that generate an ensemble of molecular configurations and the direct signal observed from X-ray measurement. Due to the fact that the signal is most sensitive to the structure nearest to a photoelectron source, an understanding of XAFS signal is an exquisite tool for decoding the nearest neighbor coordination and correlated structure of the solvent molecules surrounding the photo-electron source. The XAFS signal can be constructed from an ensemble of scattering paths. Often the signal cannot be decomposed into a few dominant paths with characteristics that can be fitted. MD-XAFS takes advantage of the direct correspondence between the ensemble of molecular configurations and the ensemble of scattering paths, taking into account the complex correlation between them resulting in the observed signal. Due to the fact that significant phenomena are controlled by solvent response and fluctuations, such as diffusion and speciation of species, the establishment of the connection between molecular simulation and experiment has established utility in materials and catalysis systems.

Below we will expand on a variety of approaches that enhance the interpretation of MD-XAFS analysis. We will give examples of its utility in a variety of systems, including 1) the solvation of transition metal ions in water 2) an example of an analysis of a reactive chemistry corresponding to homogeneous catalysis 3) the distribution of reaction centers in a heterogeneous catalysis system as well as 4) fundamental analysis of acid/base equilibrium as a function of concentration. 

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Acknowledgement

This development could not be achieved without the support from our colleagues including John Rehr, Maureen McCarthy, Bruce Palmer, Mali Balasubramanian, Chris Mundy, Marcel Baer, Liem Dang, Shawn Kathmann, Eric Bylaska, Roger Rousseau, Vanda Glezakou. This work was supported by the U.S. Department of Energy (DOE) Office of Science, Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences & Biosciences. Pacific Northwest National Laboratory (PNNL) is operated for the U.S. DOE by Battelle.

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Authors and Affiliations

  1. Physical Sciences Division, Pacific Northwest National Laboratory, 999, Richland, WA, 99354, USA

    Gregory K. Schenter & John L. Fulton

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  1. Gregory K. Schenter
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  2. John L. Fulton
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Correspondence to John L. Fulton .

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Editors and Affiliations

  1. The University of Electro-Communications Innovation Research Center for Fuel Cells, Graduate School of Informatics and Engineering, Tokyo, Japan

    Yasuhiro Iwasawa

  2. Institute for Catalysis, Hokkaido University, Sapporo, Japan

    Kiyotaka Asakura

  3. Research Center for Materials Science, Nagoya University, Nagoya, Japan

    Mizuki Tada

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Schenter, G.K., Fulton, J.L. (2017). Molecular Dynamics Simulations and XAFS (MD-XAFS). In: Iwasawa, Y., Asakura, K., Tada, M. (eds) XAFS Techniques for Catalysts, Nanomaterials, and Surfaces. Springer, Cham. https://doi.org/10.1007/978-3-319-43866-5_18

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