journal article·2024-06-18Open access

Resolving Nonequilibrium Shape Variations among Millions of Gold Nanoparticles

Zhou Shen, Paul Lourdu Xavier, Richard Bean, Johan Bielecki, Martin Bergemann, Benedikt J. Daurer, Tomas Ekeberg, Armando D. Estillore, Hans Fangohr, Klaus Giewekemeyer, Mikhail Karnevskiy, Richard A. Kirian, Henry Kirkwood, Yoonhee Kim, Jayanath C. P. Koliyadu, Holger Lange, Romain Letrun, Jannik Lübke, Abhishek Mall, Thomas Michelat, Andrew J. Morgan, Nils Roth, Amit K. Samanta, Tokushi Sato, Marcin Sikorski, Florian Schulz, Patrik Vagovic, Tamme Wollweber, Lena Worbs, Filipe Maia, Daniel Alfred Horke, Jochen Küpper, Adrian P. Mancuso, Henry N. Chapman, Kartik Ayyer, N. Duane Loh

ACS Nano· Volume 18· Issue 24

Abstract

High Resolution Image Download MS PowerPoint Slide Nanoparticles, exhibiting functionally relevant structural heterogeneity, are at the forefront of cutting-edge research. Now, high-throughput single-particle imaging (SPI) with X-ray free-electron lasers (XFELs) creates opportunities for recovering the shape distributions of millions of particles that exhibit functionally relevant structural heterogeneity. To realize this potential, three challenges have to be overcome: (1) simultaneous parametrization of structural variability in real and reciprocal spaces; (2) efficiently inferring the latent parameters of each SPI measurement; (3) scaling up comparisons between 10 5 structural models and 10 6 XFEL-SPI measurements. Here, we describe how we overcame these three challenges to resolve the nonequilibrium shape distributions within millions of gold nanoparticles imaged at the European XFEL. These shape distributions allowed us to quantify the degree of asymmetry in these particles, discover a relatively stable “shape envelope” among nanoparticles, discern finite-size effects related to shape-controlling surfactants, and extrapolate nanoparticles’ shapes to their idealized thermodynamic limit. Ultimately, these demonstrations show that XFEL SPI can help transform nanoparticle shape characterization from anecdotally interesting to statistically meaningful.
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Research context

OpenAlex topics: Gold and Silver Nanoparticles Synthesis and Applications · nanoparticles nucleation surface interactions · Nanocluster Synthesis and Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Physics, National University of Singapore, 117551 Singapore

Max Planck Institute for the Structure and Dynamics of Matter, 22761 Hamburg, Germany

Center for Free-Electron Laser Science, 22761, Hamburg, Germany

The Hamburg Center for Ultrafast Imaging, Universität Hamburg, 22761 Hamburg, Germany

Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany

European XFEL, 22869 Schenefeld, Germany

Center for BioImaging Sciences, National University of Singapore, 117557 Singapore

Diamond Light Source, Harwell Campus, Didcot OX11 0DE, U.K.

Department of Cell and Molecular Biology, Uppsala University, 75124 Uppsala, Sweden

Department of Physics, Arizona State University, Tempe, Arizona 85287, United States

Institute of Physics and Astronomy, Universität Potsdam, Karl-Liebknecht-Str. 24, 14476 Potsdam, Germany

Department of Physics, Universität Hamburg, 22761 Hamburg, Germany

University of Melbourne, Physics, Melbourne, VIC 3010, Australia

Institute of Nanostructure and Solid State Physics, University of Hamburg, 22761 Hamburg, Germany

NERSC, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Radboud University Institute for Molecules and Materials, 6525 AJ Nijmegen, The Netherlands

Department of Chemistry, Universität Hamburg, 20146 Hamburg, Germany

Department of Chemistry and Physics, La Trobe Institute for Molecular Science, La Trobe University, Melbourne, VIC 3086, Australia

Funding

Ministry of Education - Singapore · BioXFEL Science and Technology Center · Joachim Herz Stiftung · Faculty of Science, National University of Singapore · Human Frontier Science Program · National University of Singapore · National Science Foundation

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