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Title: Ultrafast Three-Dimensional X-ray Imaging of Deformation Modes in ZnO Nanocrystals

Imaging the dynamical response of materials following ultrafast excitation can reveal energy transduction mechanisms and their dissipation pathways, as well as material stability under conditions far from equilibrium. Such dynamical behaviour is challenging to characterize, especially operando at nanoscopic spatiotemporal scales. In this letter, we use x-ray coherent diffractive imaging to show that ultrafast laser excitation of a ZnO nanocrystal induces a rich set of deformation dynamics including characteristic ‘hard’ or inhomogeneous and ‘soft’ or homogeneous modes at different time scales, corresponding respectively to the propagation of acoustic phonons and resonant oscillation of the crystal. By integrating the 3D nanocrystal structure obtained from the ultrafast x-ray measurements with a continuum thermo-electro-mechanical finite element model, we elucidate the deformation mechanisms following laser excitation, in particular, a torsional mode that generates a 50% greater electric potential gradient than that resulting from the flexural mode. Furthermore, understanding of the time-dependence of these mechanisms on ultrafast scales has significant implications for development of new materials for nanoscale power generation.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [1] ; ORCiD logo [1] ;  [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. ESRF - The European Synchrotron, Grenoble (France)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 2; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; integrated imaging; power generation; ultrafast X-ray; ZnO; nanocrystal
OSTI Identifier:
1376886

Cherukara, Mathew J., Sasikumar, Kiran, Cha, Wonsuk, Narayanan, Badri, Leake, Steven J., Dufresne, Eric M., Peterka, Tom, McNulty, Ian, Wen, Haidan, Sankaranarayanan, Subramanian K. R. S., and Harder, Ross J.. Ultrafast Three-Dimensional X-ray Imaging of Deformation Modes in ZnO Nanocrystals. United States: N. p., Web. doi:10.1021/acs.nanolett.6b04652.
Cherukara, Mathew J., Sasikumar, Kiran, Cha, Wonsuk, Narayanan, Badri, Leake, Steven J., Dufresne, Eric M., Peterka, Tom, McNulty, Ian, Wen, Haidan, Sankaranarayanan, Subramanian K. R. S., & Harder, Ross J.. Ultrafast Three-Dimensional X-ray Imaging of Deformation Modes in ZnO Nanocrystals. United States. doi:10.1021/acs.nanolett.6b04652.
Cherukara, Mathew J., Sasikumar, Kiran, Cha, Wonsuk, Narayanan, Badri, Leake, Steven J., Dufresne, Eric M., Peterka, Tom, McNulty, Ian, Wen, Haidan, Sankaranarayanan, Subramanian K. R. S., and Harder, Ross J.. 2016. "Ultrafast Three-Dimensional X-ray Imaging of Deformation Modes in ZnO Nanocrystals". United States. doi:10.1021/acs.nanolett.6b04652. https://www.osti.gov/servlets/purl/1376886.
@article{osti_1376886,
title = {Ultrafast Three-Dimensional X-ray Imaging of Deformation Modes in ZnO Nanocrystals},
author = {Cherukara, Mathew J. and Sasikumar, Kiran and Cha, Wonsuk and Narayanan, Badri and Leake, Steven J. and Dufresne, Eric M. and Peterka, Tom and McNulty, Ian and Wen, Haidan and Sankaranarayanan, Subramanian K. R. S. and Harder, Ross J.},
abstractNote = {Imaging the dynamical response of materials following ultrafast excitation can reveal energy transduction mechanisms and their dissipation pathways, as well as material stability under conditions far from equilibrium. Such dynamical behaviour is challenging to characterize, especially operando at nanoscopic spatiotemporal scales. In this letter, we use x-ray coherent diffractive imaging to show that ultrafast laser excitation of a ZnO nanocrystal induces a rich set of deformation dynamics including characteristic ‘hard’ or inhomogeneous and ‘soft’ or homogeneous modes at different time scales, corresponding respectively to the propagation of acoustic phonons and resonant oscillation of the crystal. By integrating the 3D nanocrystal structure obtained from the ultrafast x-ray measurements with a continuum thermo-electro-mechanical finite element model, we elucidate the deformation mechanisms following laser excitation, in particular, a torsional mode that generates a 50% greater electric potential gradient than that resulting from the flexural mode. Furthermore, understanding of the time-dependence of these mechanisms on ultrafast scales has significant implications for development of new materials for nanoscale power generation.},
doi = {10.1021/acs.nanolett.6b04652},
journal = {Nano Letters},
number = 2,
volume = 17,
place = {United States},
year = {2016},
month = {12}
}