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Title: Imaging transient melting of a nanocrystal using an X-ray laser

Abstract

Significance Despite phase transitions, such as melting, being ubiquitous in nature, understanding what occurs at the nanoscale (such as in nanocrystals) has so far remained challenging. With ensemble studies of nanocrystals it is often difficult to discriminate between intrinsic size-dependent properties and effects due to sample size and shape dispersity. Here, using an X-ray free electron laser we image the reversible melting of an individual nanocrystal induced by an ultrashort laser. It is revealed that the melting occurs transiently, repeatably, and inhomogeneously. This is consistent with a core-shell model where the exterior is melted and a solid core remains. These findings reveal, unambiguously, that core-shell melting occurs, which has important implications for understanding nanoscale phenomena.

Authors:
 [1];  [2];  [2];  [3];  [3];  [3];  [3];  [3];  [3];  [4];  [5];  [6];  [7];  [8];  [9]
  1. London Centre for Nanotechnology, University College London, London WC1E 6BT, United Kingdom,, Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA 94025,, Center for Free-Electron Laser Science, Deutsches Elektronensynchrotron, 22607 Hamburg, Germany,
  2. London Centre for Nanotechnology, University College London, London WC1E 6BT, United Kingdom,
  3. Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025,
  4. Australian Research Council Centre of Excellence for Advanced Molecular Imaging, La Trobe University, Bundoora, VIC 3086, Australia,
  5. Advanced Photon Source, Argonne National Laboratory, Argonne, IL 60439,
  6. Department of Engineering Science, University of Oxford, Oxford OX1 3PJ, United Kingdom,, Research Complex at Harwell, Didcot, Oxfordshire OX11 0DE, United Kingdom,
  7. Department of Physics, Clarendon Laboratory, University of Oxford, Oxford OX1 3PU, United Kingdom
  8. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA 94025,
  9. London Centre for Nanotechnology, University College London, London WC1E 6BT, United Kingdom,, Research Complex at Harwell, Didcot, Oxfordshire OX11 0DE, United Kingdom,
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1235108
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 112 Journal Issue: 24; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English

Citation Formats

Clark, Jesse N., Beitra, Loren, Xiong, Gang, Fritz, David M., Lemke, Henrik T., Zhu, Diling, Chollet, Matthieu, Williams, Garth J., Messerschmidt, Marc M., Abbey, Brian, Harder, Ross J., Korsunsky, Alexander M., Wark, Justin S., Reis, David A., and Robinson, Ian K. Imaging transient melting of a nanocrystal using an X-ray laser. United States: N. p., 2015. Web. doi:10.1073/pnas.1417678112.
Clark, Jesse N., Beitra, Loren, Xiong, Gang, Fritz, David M., Lemke, Henrik T., Zhu, Diling, Chollet, Matthieu, Williams, Garth J., Messerschmidt, Marc M., Abbey, Brian, Harder, Ross J., Korsunsky, Alexander M., Wark, Justin S., Reis, David A., & Robinson, Ian K. Imaging transient melting of a nanocrystal using an X-ray laser. United States. https://doi.org/10.1073/pnas.1417678112
Clark, Jesse N., Beitra, Loren, Xiong, Gang, Fritz, David M., Lemke, Henrik T., Zhu, Diling, Chollet, Matthieu, Williams, Garth J., Messerschmidt, Marc M., Abbey, Brian, Harder, Ross J., Korsunsky, Alexander M., Wark, Justin S., Reis, David A., and Robinson, Ian K. Tue . "Imaging transient melting of a nanocrystal using an X-ray laser". United States. https://doi.org/10.1073/pnas.1417678112.
@article{osti_1235108,
title = {Imaging transient melting of a nanocrystal using an X-ray laser},
author = {Clark, Jesse N. and Beitra, Loren and Xiong, Gang and Fritz, David M. and Lemke, Henrik T. and Zhu, Diling and Chollet, Matthieu and Williams, Garth J. and Messerschmidt, Marc M. and Abbey, Brian and Harder, Ross J. and Korsunsky, Alexander M. and Wark, Justin S. and Reis, David A. and Robinson, Ian K.},
abstractNote = {Significance Despite phase transitions, such as melting, being ubiquitous in nature, understanding what occurs at the nanoscale (such as in nanocrystals) has so far remained challenging. With ensemble studies of nanocrystals it is often difficult to discriminate between intrinsic size-dependent properties and effects due to sample size and shape dispersity. Here, using an X-ray free electron laser we image the reversible melting of an individual nanocrystal induced by an ultrashort laser. It is revealed that the melting occurs transiently, repeatably, and inhomogeneously. This is consistent with a core-shell model where the exterior is melted and a solid core remains. These findings reveal, unambiguously, that core-shell melting occurs, which has important implications for understanding nanoscale phenomena.},
doi = {10.1073/pnas.1417678112},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 24,
volume = 112,
place = {United States},
year = {Tue Jun 16 00:00:00 EDT 2015},
month = {Tue Jun 16 00:00:00 EDT 2015}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1073/pnas.1417678112

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Works referenced in this record:

Time-Resolved X-ray Diffraction Investigation of the Modified Phonon Dispersion in InSb Nanowires
journal, January 2014

  • Jurgilaitis, A.; Enquist, H.; Andreasson, B. P.
  • Nano Letters, Vol. 14, Issue 2
  • DOI: 10.1021/nl403596b

Single mimivirus particles intercepted and imaged with an X-ray laser
journal, February 2011

  • Seibert, M. Marvin; Ekeberg, Tomas; Maia, Filipe R. N. C.
  • Nature, Vol. 470, Issue 7332
  • DOI: 10.1038/nature09748

X-ray line broadening from filed aluminium and wolfram
journal, January 1953


Ultrafast laser-induced premelting and structural transformation of gold nanorod
journal, February 2013

  • Gan, Yong; Jiang, Shan
  • Journal of Applied Physics, Vol. 113, Issue 7
  • DOI: 10.1063/1.4792659

Phase retrieval from the magnitude of the Fourier transforms of nonperiodic objects
journal, January 1998

  • Miao, J.; Sayre, D.; Chapman, H. N.
  • Journal of the Optical Society of America A, Vol. 15, Issue 6
  • DOI: 10.1364/JOSAA.15.001662

Softening of the Symmetric Breathing Mode in Gold Particles by Laser-Induced Heating
journal, July 2003

  • Hartland, Gregory V.; Hu, Min; Sader, John E.
  • The Journal of Physical Chemistry B, Vol. 107, Issue 30
  • DOI: 10.1021/jp0276092

Extending the methodology of X-ray crystallography to allow imaging of micrometre-sized non-crystalline specimens
journal, July 1999

  • Miao, Jianwei; Charalambous, Pambos; Kirz, Janos
  • Nature, Vol. 400, Issue 6742
  • DOI: 10.1038/22498

First lasing and operation of an ångstrom-wavelength free-electron laser
journal, August 2010


Laser-induced heating and melting of gold nanoparticles studied by time-resolved x-ray scattering
journal, November 2004


Nanoscale thermal transport. II. 2003–2012
journal, March 2014

  • Cahill, David G.; Braun, Paul V.; Chen, Gang
  • Applied Physics Reviews, Vol. 1, Issue 1
  • DOI: 10.1063/1.4832615

Fourier-transform inelastic X-ray scattering from time- and momentum-dependent phonon–phonon correlations
journal, October 2013

  • Trigo, M.; Fuchs, M.; Chen, J.
  • Nature Physics, Vol. 9, Issue 12
  • DOI: 10.1038/nphys2788

Ultrafast laser melting of Au nanoparticles: atomistic simulations
journal, May 2011

  • Wang, Ningyu; Rokhlin, S. I.; Farson, D. F.
  • Journal of Nanoparticle Research, Vol. 13, Issue 10
  • DOI: 10.1007/s11051-011-0402-3

Phase retrieval algorithms: a comparison
journal, January 1982


High-resolution ab initio three-dimensional x-ray diffraction microscopy
journal, January 2006

  • Chapman, Henry N.; Barty, Anton; Marchesini, Stefano
  • Journal of the Optical Society of America A, Vol. 23, Issue 5
  • DOI: 10.1364/JOSAA.23.001179

Noninvasive laser-induced photoacoustic tomography for structural and functional in vivo imaging of the brain
journal, June 2003

  • Wang, Xueding; Pang, Yongjiang; Ku, Geng
  • Nature Biotechnology, Vol. 21, Issue 7
  • DOI: 10.1038/nbt839

Nonhomogeneous surface premelting of Au nanoparticles
journal, September 2008


The CSPAD megapixel x-ray camera at LCLS
conference, October 2012

  • Hart, Philip; Boutet, Sébastien; Carini, Gabriella
  • SPIE Optical Engineering + Applications, SPIE Proceedings
  • DOI: 10.1117/12.930924

Three-dimensional mapping of a deformation field inside a nanocrystal
journal, July 2006

  • Pfeifer, Mark A.; Williams, Garth J.; Vartanyants, Ivan A.
  • Nature, Vol. 442, Issue 7098
  • DOI: 10.1038/nature04867

Atomic Resolution Imaging of a Carbon Nanotube from Diffraction Intensities
journal, May 2003


Dynamics of Size-Selected Gold Nanoparticles Studied by Ultrafast Electron Nanocrystallography
journal, May 2007

  • Ruan, Chong-Yu; Murooka, Yoshie; Raman, Ramani K.
  • Nano Letters, Vol. 7, Issue 5
  • DOI: 10.1021/nl070269h

A Surface Phase Transition of Supported Gold Nanoparticles
journal, April 2007

  • Plech, Anton; Cerna, Roland; Kotaidis, Vassilios
  • Nano Letters, Vol. 7, Issue 4
  • DOI: 10.1021/nl070187t

Ultrafast Three-Dimensional Imaging of Lattice Dynamics in Individual Gold Nanocrystals
journal, May 2013


Thermal Conductivity Reduction and Thermoelectric Figure of Merit Increase by Embedding Nanoparticles in Crystalline Semiconductors
journal, February 2006


Near-Infrared Resonant Nanoshells for Combined Optical Imaging and Photothermal Cancer Therapy
journal, July 2007

  • Gobin, André M.; Lee, Min Ho; Halas, Naomi J.
  • Nano Letters, Vol. 7, Issue 7, p. 1929-1934
  • DOI: 10.1021/nl070610y

Surface generation and detection of phonons by picosecond light pulses
journal, September 1986


The Effect of Cold‐Work Distortion on X‐Ray Patterns
journal, June 1950

  • Warren, B. E.; Averbach, B. L.
  • Journal of Applied Physics, Vol. 21, Issue 6
  • DOI: 10.1063/1.1699713

Melting of Pb nanocrystals
journal, June 1998