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Title: The 3D-architecture of individual free silver nanoparticles captured by X-ray scattering

Abstract

The diversity of nanoparticle shapes generated by condensation from gaseous matter reflects the fundamental competition between thermodynamic equilibration and the persistence of metastable configurations during growth. In the kinetically limited regime, intermediate geometries that are favoured only in early formation stages can be imprinted in the finally observed ensemble of differently structured specimens. Here we demonstrate that single-shot wide-angle scattering of femtosecond soft X-ray free-electron laser pulses allows three-dimensional characterization of the resulting metastable nanoparticle structures. For individual free silver particles, which can be considered frozen in space for the duration of photon exposure, both shape and orientation are uncovered from measured scattering images. We identify regular shapes, including species with fivefold symmetry and surprisingly large aspect ratio up to particle radii of the order of 100 nm. Our approach includes scattering effects beyond Born’s approximation and is remarkably efficient—opening up new routes in ultrafast nanophysics and free-electron laser science

Authors:
 [1];  [1];  [2];  [2];  [2];  [2];  [3];  [4];  [5];  [1];  [1];  [1];  [1];  [2]
  1. Univ. of Rostock, Rostock (Germany)
  2. Technische Univ., Berlin (Germany)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States); Technische Univ., Berlin (Germany)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. FLASH, Hamburg (Germany)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
Contributing Org.:
Linac Coherent Light Source, SLAC National Accelerator Laboratory
OSTI Identifier:
1190465
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Barke, Ingo, Hartmann, Hannes, Rupp, Daniela, Flückiger, Leonie, Sauppe, Mario, Adolph, Marcus, Schorb, Sebastian, Bostedt, Christoph, Treusch, Rolf, Peltz, Christian, Bartling, Stephan, Fennel, Thomas, Meiwes-Broer, Karl-Heinz, and Möller, Thomas. The 3D-architecture of individual free silver nanoparticles captured by X-ray scattering. United States: N. p., 2015. Web. doi:10.1038/ncomms7187.
Barke, Ingo, Hartmann, Hannes, Rupp, Daniela, Flückiger, Leonie, Sauppe, Mario, Adolph, Marcus, Schorb, Sebastian, Bostedt, Christoph, Treusch, Rolf, Peltz, Christian, Bartling, Stephan, Fennel, Thomas, Meiwes-Broer, Karl-Heinz, & Möller, Thomas. The 3D-architecture of individual free silver nanoparticles captured by X-ray scattering. United States. https://doi.org/10.1038/ncomms7187
Barke, Ingo, Hartmann, Hannes, Rupp, Daniela, Flückiger, Leonie, Sauppe, Mario, Adolph, Marcus, Schorb, Sebastian, Bostedt, Christoph, Treusch, Rolf, Peltz, Christian, Bartling, Stephan, Fennel, Thomas, Meiwes-Broer, Karl-Heinz, and Möller, Thomas. Wed . "The 3D-architecture of individual free silver nanoparticles captured by X-ray scattering". United States. https://doi.org/10.1038/ncomms7187. https://www.osti.gov/servlets/purl/1190465.
@article{osti_1190465,
title = {The 3D-architecture of individual free silver nanoparticles captured by X-ray scattering},
author = {Barke, Ingo and Hartmann, Hannes and Rupp, Daniela and Flückiger, Leonie and Sauppe, Mario and Adolph, Marcus and Schorb, Sebastian and Bostedt, Christoph and Treusch, Rolf and Peltz, Christian and Bartling, Stephan and Fennel, Thomas and Meiwes-Broer, Karl-Heinz and Möller, Thomas},
abstractNote = {The diversity of nanoparticle shapes generated by condensation from gaseous matter reflects the fundamental competition between thermodynamic equilibration and the persistence of metastable configurations during growth. In the kinetically limited regime, intermediate geometries that are favoured only in early formation stages can be imprinted in the finally observed ensemble of differently structured specimens. Here we demonstrate that single-shot wide-angle scattering of femtosecond soft X-ray free-electron laser pulses allows three-dimensional characterization of the resulting metastable nanoparticle structures. For individual free silver particles, which can be considered frozen in space for the duration of photon exposure, both shape and orientation are uncovered from measured scattering images. We identify regular shapes, including species with fivefold symmetry and surprisingly large aspect ratio up to particle radii of the order of 100 nm. Our approach includes scattering effects beyond Born’s approximation and is remarkably efficient—opening up new routes in ultrafast nanophysics and free-electron laser science},
doi = {10.1038/ncomms7187},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Wed Feb 04 00:00:00 EST 2015},
month = {Wed Feb 04 00:00:00 EST 2015}
}

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Figures / Tables:

Figure 1 Figure 1 : Schematics of the wide-angle scattering experiment. In Born’s approximation, the far-field scattering intensity reads I(q)∝| ∫ρ(r)eiqrd3r|2, where ρ(r) is the scattering density of the particle centered at r=0. After decomposing r into components parallel (r||) and perpendicular (r) to the projection vector np= kin+ q/2, which ismore » by definition perpendicular to q, the intensity can be recast as I(q)∝| ρ(r)eiqrd2r|2, representing the Fourier transform of the projected density ρ(r) = ∫ρ(r)dr|| on a plane with normal vector np. (a) For small scattering angles, the approximation np||kin is valid, which inhibits access to any structural information along this direction. (b) The variation of np with q for large scattering angles provides access to the 3D properties of the particle. (c) In the experiment, single-shot diffraction patterns of silver particles intersecting the FEL photon beam are captured by the 2D detector.« less

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