Year: 2024
Type: article
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.
Source: ACS Nano
Authors: 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
Institutions: National University of Singapore, Center for Free-Electron Laser Science, Max Planck Institute for the Structure and Dynamics of Matter, Universität Hamburg, Deutsches Elektronen-Synchrotron DESY, Hamburg Centre for Ultrafast Imaging, European X-Ray Free-Electron Laser, Diamond Light Source, Uppsala University, Arizona State University, University of Potsdam, The University of Melbourne, Lawrence Berkeley National Laboratory, National Energy Research Scientific Computing Center, Radboud University Nijmegen, La Trobe University
Language: English
Subfield: Radiation
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $4,500
Funders: National Science Foundation, Joachim Herz Stiftung, Human Frontier Science Program, National University of Singapore, Ministry of Education - Singapore, Deutsche Forschungsgemeinschaft, Directorate for Biological Sciences, BioXFEL Science and Technology Center, Faculty of Science, National University of Singapore, Deutsches Elektronen-Synchrotron
OpenAlex ID: W4399141237