Single-particle mapping of nonequilibrium nanocrystal transformations

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

doi:10.1126/science.aah4434

Title: Single-particle mapping of nonequilibrium nanocrystal transformations

Journal Article · Fri Nov 18 00:00:00 EST 2016 · Science

DOI:https://doi.org/10.1126/science.aah4434· OSTI ID:1347829

Ye, Xingchen ^[1]; Jones, Matthew R. ^[1]; Frechette, Layne B. ^[1]; Chen, Qian ^[2]; Powers, Alexander S. ^[1]; Ercius, Peter ^[3]; Dunn, Gabriel ^[4]; Rotskoff, Grant M. ^[5]; Nguyen, Son C. ^[1]; Adiga, Vivekananda P. ^[4]; Zettl, Alex ^[6]; Rabani, Eran ^[7]; Geissler, Phillip L. ^[1]; Alivisatos, A. Paul ^[8]

Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
Univ. of California, Berkeley, CA (United States). Dept. of Chemistry and Miller Inst. for Basic Research in Science
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Univ. of California, Berkeley, CA (United States). Dept. of Physics
Univ. of California, Berkeley, CA (United States). Biophysics Graduate Group
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
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
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

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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: 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

Grant/Contract Number:: AC02-05CH11231; HDTRA1-13-1-0035; CHE-1416161; 2013/604

OSTI ID:: 1347829

Alternate ID(s):: OSTI ID: 1436605

Journal Information:: Science, Journal Name: Science Vol. 354 Journal Issue: 6314; ISSN 0036-8075

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 182 works

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