title: In Situ 3D Imaging of Catalysis Induced Strain in Gold Nanoparticles.
abstract: Multielectron transfer processes are crucially important in energy and biological science but require favorable catalysts to achieve fast kinetics. Nanostructuring catalysts can dramatically improve their properties, which can be difficult to understand due to strain- and size-dependent thermodynamics, the influence of defects, and substrate-dependent activities. Here, we report three-dimensional (3D) imaging of single gold nanoparticles during catalysis of ascorbic acid decomposition using Bragg coherent diffractive imaging (BCDI). Local strains were measured in single nanoparticles and modeled using reactive molecular dynamics (RMD) simulations and finite element analysis (FEA) simulations. RMD reveals the pathway for local strain generation in the gold lattice: chemisorption of hydroxyl ions. FEA reveals that the RMD results are transferable to the nanocrystal sizes studied in the experiment. Our study probes the strain-activity connection and opens a powerful avenue for theoretical and experimental studies of nanocrystal catalysis.
authors.affiliation: Department of Physics, University of California-San Diego , La Jolla, California 92093-0319, United States.|Materials Science Division, Argonne National Laboratory , Argonne, Illinois 60439, United States.
authors.forename: Andrew
authors.initials: A
authors.lastname: Ulvestad
authors.affiliation: Center for Nanoscale Materials, Argonne National Laboratory , Argonne, Illinois 60439, United States.
authors.forename: Kiran
authors.initials: K
authors.lastname: Sasikumar
authors.affiliation: Department of Physics, University of California-San Diego , La Jolla, California 92093-0319, United States.|Advanced Photon Source, Argonne National Laboratory , Argonne, Illinois 60439, United States.
authors.forename: Jong Woo
authors.initials: JW
authors.lastname: Kim
authors.affiliation: Advanced Photon Source, Argonne National Laboratory , Argonne, Illinois 60439, United States.
authors.forename: Ross
authors.initials: R
authors.lastname: Harder
authors.affiliation: Advanced Photon Source, Argonne National Laboratory , Argonne, Illinois 60439, United States.
authors.forename: Evan
authors.initials: E
authors.lastname: Maxey
authors.affiliation: Stanford PULSE Institute, SLAC National Accelerator Laboratory Menlo Park, California 94025, United States.|Center for Free-Electron Laser Science (CFEL), Deutsches Elektronensynchrotron (DESY) , Notkestrasse 85, 22607 Hamburg, Germany.
authors.forename: Jesse N
authors.initials: JN
authors.lastname: Clark
authors.affiliation: Center for Nanoscale Materials, Argonne National Laboratory , Argonne, Illinois 60439, United States.
authors.forename: Badri
authors.initials: B
authors.lastname: Narayanan
authors.affiliation: Center for Nanoscale Materials, Argonne National Laboratory , Argonne, Illinois 60439, United States.
authors.forename: Sanket A
authors.initials: SA
authors.lastname: Deshmukh
authors.affiliation: Mathematics and Computer Science Division, Argonne National Laboratory , Argonne, Illinois 60439, United States.
authors.forename: Nicola
authors.initials: N
authors.lastname: Ferrier
authors.affiliation: School of Chemistry & Bio21 Institute, University of Melbourne , Parkville, Victoria 3010, Australia.
authors.forename: Paul
authors.initials: P
authors.lastname: Mulvaney
authors.affiliation: Center for Nanoscale Materials, Argonne National Laboratory , Argonne, Illinois 60439, United States.
authors.forename: Subramanian K R S
authors.initials: SK
authors.lastname: Sankaranarayanan
authors.affiliation: Department of Physics, University of California-San Diego , La Jolla, California 92093-0319, United States.
authors.forename: Oleg G
authors.initials: OG
authors.lastname: Shpyrko