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Title: Single-particle mapping of nonequilibrium nanocrystal transformations

Abstract

Chemists have developed mechanistic insight into numerous chemical reactions by thoroughly characterizing nonequilibrium species. Although methods to probe these processes are well established for molecules, analogous techniques for understanding intermediate structures in nanomaterials have been lacking. For this study, we monitor the shape evolution of individual anisotropic gold nanostructures as they are oxidatively etched in a graphene liquid cell with a controlled redox environment. Short-lived, nonequilibrium nanocrystals are observed, structurally analyzed, and rationalized through Monte Carlo simulations. Understanding these reaction trajectories provides important fundamental insight connecting high-energy nanocrystal morphologies to the development of kinetically stabilized surface features and demonstrates the importance of developing tools capable of probing short-lived nanoscale species at the single-particle level.

Authors:
 [1];  [1];  [1];  [2];  [1];  [3];  [4];  [5];  [1];  [4];  [6];  [7];  [1];  [8]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry and Miller Inst. for Basic Research in Science
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  4. Univ. of California, Berkeley, CA (United States). Dept. of Physics
  5. Univ. of California, Berkeley, CA (United States). Biophysics Graduate Group
  6. Univ. of California, Berkeley, CA (United States). Dept. of Physics and Kavli Energy NanoScience Inst.; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  7. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Tel Aviv Univ., Ramat Aviv (Israel). Raymond and Beverly Sackler Center for Computational Molecular and Materials Science
  8. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry, Dept. of Materials Science and Engineering and Kavli Energy NanoScience Inst.; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; King Abdulaziz City for Science and Technology (KACST), Riyadh (Saudi Arabia); Defense Threat Reduction Agency (DTRA); National Science Foundation (NSF); Binational Science Foundation (BSF); Univ. of California, Berkeley, CA (United States); Arnold and Mabel Beckman Foundation
OSTI Identifier:
1347829
Alternate Identifier(s):
OSTI ID: 1436605
Grant/Contract Number:  
AC02-05CH11231; HDTRA1-13-1-0035; CHE-1416161; 2013/604
Resource Type:
Journal Article: Published Article
Journal Name:
Science
Additional Journal Information:
Journal Volume: 354; Journal Issue: 6314; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Ye, Xingchen, Jones, Matthew R., Frechette, Layne B., Chen, Qian, Powers, Alexander S., Ercius, Peter, Dunn, Gabriel, Rotskoff, Grant M., Nguyen, Son C., Adiga, Vivekananda P., Zettl, Alex, Rabani, Eran, Geissler, Phillip L., and Alivisatos, A. Paul. Single-particle mapping of nonequilibrium nanocrystal transformations. United States: N. p., 2016. Web. doi:10.1126/science.aah4434.
Ye, Xingchen, Jones, Matthew R., Frechette, Layne B., Chen, Qian, Powers, Alexander S., Ercius, Peter, Dunn, Gabriel, Rotskoff, Grant M., Nguyen, Son C., Adiga, Vivekananda P., Zettl, Alex, Rabani, Eran, Geissler, Phillip L., & Alivisatos, A. Paul. Single-particle mapping of nonequilibrium nanocrystal transformations. United States. doi:10.1126/science.aah4434.
Ye, Xingchen, Jones, Matthew R., Frechette, Layne B., Chen, Qian, Powers, Alexander S., Ercius, Peter, Dunn, Gabriel, Rotskoff, Grant M., Nguyen, Son C., Adiga, Vivekananda P., Zettl, Alex, Rabani, Eran, Geissler, Phillip L., and Alivisatos, A. Paul. Fri . "Single-particle mapping of nonequilibrium nanocrystal transformations". United States. doi:10.1126/science.aah4434.
@article{osti_1347829,
title = {Single-particle mapping of nonequilibrium nanocrystal transformations},
author = {Ye, Xingchen and Jones, Matthew R. and Frechette, Layne B. and Chen, Qian and Powers, Alexander S. and Ercius, Peter and Dunn, Gabriel and Rotskoff, Grant M. and Nguyen, Son C. and Adiga, Vivekananda P. and Zettl, Alex and Rabani, Eran and Geissler, Phillip L. and Alivisatos, A. Paul},
abstractNote = {Chemists have developed mechanistic insight into numerous chemical reactions by thoroughly characterizing nonequilibrium species. Although methods to probe these processes are well established for molecules, analogous techniques for understanding intermediate structures in nanomaterials have been lacking. For this study, we monitor the shape evolution of individual anisotropic gold nanostructures as they are oxidatively etched in a graphene liquid cell with a controlled redox environment. Short-lived, nonequilibrium nanocrystals are observed, structurally analyzed, and rationalized through Monte Carlo simulations. Understanding these reaction trajectories provides important fundamental insight connecting high-energy nanocrystal morphologies to the development of kinetically stabilized surface features and demonstrates the importance of developing tools capable of probing short-lived nanoscale species at the single-particle level.},
doi = {10.1126/science.aah4434},
journal = {Science},
number = 6314,
volume = 354,
place = {United States},
year = {Fri Nov 18 00:00:00 EST 2016},
month = {Fri Nov 18 00:00:00 EST 2016}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1126/science.aah4434

Citation Metrics:
Cited by: 19 works
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