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Title: Polymorphism in magic-sized Au144(SR)60 clusters

Abstract

Ultra-small, magic-sized metal nanoclusters represent an important new class of materials with properties between molecules and particles. However, their small size challenges the conventional methods for structure characterization. We present the structure of ultra-stable Au144(SR)60 magic-sized nanoclusters obtained from atomic pair distribution function analysis of X-ray powder diffraction data. Our study reveals structural polymorphism in these archetypal nanoclusters. Additionally, in order to confirm the theoretically predicted icosahedral-cored cluster, we also find samples with a truncated decahedral core structure, with some samples exhibiting a coexistence of both cluster structures. Although the clusters are monodisperse in size, structural diversity is apparent. Finally, the discovery of polymorphism may open up a new dimension in nanoscale engineering.

Authors:
 [1]; ORCiD logo [2];  [3];  [3];  [4];  [3]; ORCiD logo [5]
  1. Columbia Univ., New York, NY (United States). Dept. of Applied Physics and Applied Mathematics
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
  3. Colorado State Univ., Fort Collins, CO (United States). Dept. of Chemistry
  4. European Synchrotron Radiation Facility (ESRF), Grenoble (France)
  5. Columbia Univ., New York, NY (United States). Dept. of Applied Physics and Applied Mathematics; Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1336145
Report Number(s):
BNL-112624-2016-JA
Journal ID: ISSN 2041-1723; R&D Project: PO011; KC0201060
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal Issue: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Jensen, Kirsten M. O., Juhas, Pavol, Tofanelli, Marcus A., Heinecke, Christine L., Vaughan, Gavin, Ackerson, Christopher J., and Billinge, Simon J. L.. Polymorphism in magic-sized Au144(SR)60 clusters. United States: N. p., 2016. Web. doi:10.1038/ncomms11859.
Jensen, Kirsten M. O., Juhas, Pavol, Tofanelli, Marcus A., Heinecke, Christine L., Vaughan, Gavin, Ackerson, Christopher J., & Billinge, Simon J. L.. Polymorphism in magic-sized Au144(SR)60 clusters. United States. https://doi.org/10.1038/ncomms11859
Jensen, Kirsten M. O., Juhas, Pavol, Tofanelli, Marcus A., Heinecke, Christine L., Vaughan, Gavin, Ackerson, Christopher J., and Billinge, Simon J. L.. Tue . "Polymorphism in magic-sized Au144(SR)60 clusters". United States. https://doi.org/10.1038/ncomms11859. https://www.osti.gov/servlets/purl/1336145.
@article{osti_1336145,
title = {Polymorphism in magic-sized Au144(SR)60 clusters},
author = {Jensen, Kirsten M. O. and Juhas, Pavol and Tofanelli, Marcus A. and Heinecke, Christine L. and Vaughan, Gavin and Ackerson, Christopher J. and Billinge, Simon J. L.},
abstractNote = {Ultra-small, magic-sized metal nanoclusters represent an important new class of materials with properties between molecules and particles. However, their small size challenges the conventional methods for structure characterization. We present the structure of ultra-stable Au144(SR)60 magic-sized nanoclusters obtained from atomic pair distribution function analysis of X-ray powder diffraction data. Our study reveals structural polymorphism in these archetypal nanoclusters. Additionally, in order to confirm the theoretically predicted icosahedral-cored cluster, we also find samples with a truncated decahedral core structure, with some samples exhibiting a coexistence of both cluster structures. Although the clusters are monodisperse in size, structural diversity is apparent. Finally, the discovery of polymorphism may open up a new dimension in nanoscale engineering.},
doi = {10.1038/ncomms11859},
journal = {Nature Communications},
number = 7,
volume = 7,
place = {United States},
year = {Tue Jun 14 00:00:00 EDT 2016},
month = {Tue Jun 14 00:00:00 EDT 2016}
}

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Cited by: 115 works
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Reverse Monte Carlo modeling for local structures of noble metal nanoparticles using high-energy XRD and EXAFS
journal, January 2019

  • Harada, Masafumi; Ikegami, Risa; Kumara, Loku Singgappulige Rosantha
  • RSC Advances, Vol. 9, Issue 51
  • DOI: 10.1039/c9ra06519a

Phase transformations and capacity fade mechanism in Li x Sn nanoparticle electrodes revealed by operando 7 Li NMR
journal, January 2019

  • Lorie Lopez, Jose L.; Grandinetti, Philip J.; Co, Anne C.
  • Journal of Materials Chemistry A, Vol. 7, Issue 17
  • DOI: 10.1039/c9ta03345a

Structure analysis of supported disordered molybdenum oxides using pair distribution function analysis and automated cluster modelling
journal, February 2020

  • Lindahl Christiansen, Troels; Kjær, Emil T. S.; Kovyakh, Anton
  • Journal of Applied Crystallography, Vol. 53, Issue 1
  • DOI: 10.1107/s1600576719016832

Unraveling the long-pursued Au 144 structure by x-ray crystallography
journal, October 2018


Ab initio molecular dynamics studies of Au38(SR)24 isomers under heating
journal, March 2019

  • Juarez-Mosqueda, Rosalba; Malola, Sami; Häkkinen, Hannu
  • The European Physical Journal D, Vol. 73, Issue 3
  • DOI: 10.1140/epjd/e2019-90441-5

When Crystals Go Nano - The Role of Advanced X-ray Total Scattering Methods in Nanotechnology: When Crystals Go Nano - The Role of Advanced X-ray Total Scattering Methods in Nanotechnology
journal, August 2018

  • Bertolotti, Federica; Moscheni, Daniele; Guagliardi, Antonietta
  • European Journal of Inorganic Chemistry, Vol. 2018, Issue 34
  • DOI: 10.1002/ejic.201800534

Spatially Localized Synthesis and Structural Characterization of Platinum Nanocrystals Obtained Using UV Light
journal, August 2018

  • Quinson, Jonathan; Kacenauskaite, Laura; Christiansen, Troels L.
  • ACS Omega, Vol. 3, Issue 8
  • DOI: 10.1021/acsomega.8b01613

Thermally-induced reversible structural isomerization in colloidal semiconductor CdS magic-size clusters
journal, June 2018


Unraveling the long-pursued Au 144 structure by x-ray crystallography
journal, October 2018


Structure of Manganese Oxide Nanoparticles Extracted via Pair Distribution Functions
journal, March 2020