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@ARTICLE{Shen:610715,
author = {Shen, Zhou and Paulraj, Lourdu Xavier and Bean, Richard and
Bielecki, Johan and Bergemann, Martin and Daurer, Benedikt
and Ekeberg, Tomas and Estillore, Armando D. and Fangohr,
Hans and Giewekemeyer, Klaus and Karnevskiy, Mikhail and
Kirian, Richard and Kirkwood, Henry and Kim, Yoonhee and
Koliyadu, Jayanath and Lange, Holger and Letrun, Romain and
Lübke, Jannik and Mall, Abhishek and Michelat, Thomas and
Morgan, Andrew J. and Roth, Nils and Samanta, Amit K. and
Sato, Tokushi and Sikorski, Marcin and Schulz, Florian and
Vagovic, Patrik and Wollweber, Tamme and Worbs, Lena and
Maia, Filipe and Horke, Daniel Alfred and Küpper, Jochen
and Mancuso, Adrian and Chapman, Henry N. and Ayyer, Kartik
and Loh, Duane},
title = {{R}esolving {N}onequilibrium {S}hape {V}ariations among
{M}illions of {G}old {N}anoparticles},
journal = {ACS nano},
volume = {18},
number = {24},
issn = {1936-0851},
address = {Washington, DC},
publisher = {Soc.},
reportid = {PUBDB-2024-04692, arXiv:2401.04896},
pages = {15576-15589},
year = {2024},
abstract = {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.},
cin = {CFEL-I / FS-CFEL-CMI / UNI/CUI / UNI/EXP},
ddc = {540},
cid = {I:(DE-H253)CFEL-I-20161114 /
I:(DE-H253)FS-CFEL-CMI-20220405 /
$I:(DE-H253)UNI_CUI-20121230$ /
$I:(DE-H253)UNI_EXP-20120731$},
pnm = {631 - Matter – Dynamics, Mechanisms and Control
(POF4-631) / DFG project 390715994 - EXC 2056: CUI: Advanced
Imaging of Matter (390715994) / DFG project 194651731 - EXC
1074: Hamburger Zentrum für ultraschnelle Beobachtung
(CUI): Struktur, Dynamik und Kontrolle von Materie auf
atomarer Skala (194651731) / AXSIS - Frontiers in Attosecond
X-ray Science: Imaging and Spectroscopy (609920)},
pid = {G:(DE-HGF)POF4-631 / G:(GEPRIS)390715994 /
G:(GEPRIS)194651731 / G:(EU-Grant)609920},
experiment = {EXP:(DE-H253)XFEL-SPB-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:38810115},
eprint = {2401.04896},
howpublished = {arXiv:2401.04896},
archivePrefix = {arXiv},
SLACcitation = {$\%\%CITATION$ = $arXiv:2401.04896;\%\%$},
UT = {WOS:001235248800001},
doi = {10.1021/acsnano.4c00378},
url = {https://bib-pubdb1.desy.de/record/610715},
}