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Time-resolved Brownian tomography of single nanocrystals in liquid during oxidative etching

Journal Article · · Nature Communications
 [1];  [2];  [3];  [4];  [2];  [5];  [5];  [5];  [2];  [2];  [2];  [2];  [2];  [6];  [2];  [4];  [7];  [8];  [5];  [2]
  1. Univ. of Chicago, IL (United States); Seoul National Univ. (Korea, Republic of); Institute for Basic Science (IBS), Seoul (Korea, Republic of)
  2. Seoul National Univ. (Korea, Republic of); Institute for Basic Science (IBS), Seoul (Korea, Republic of)
  3. Cornell Univ., Ithaca, NY (United States); Seoul National Univ. (Korea, Republic of); Institute for Basic Science (IBS), Seoul (Korea, Republic of)
  4. Yonsei Univ., Seoul (Korea, Republic of)
  5. National Cancer Institute, Frederick, MD (United States)
  6. Soongsil University, Seoul (Korea, Republic of)
  7. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
  8. Hanyang Univ., Ansan (Korea, Republic of)

Colloidal nanocrystals inherently undergo structural changes during chemical reactions. The robust structure-property relationships, originating from their nanoscale dimensions, underscore the significance of comprehending the dynamic structural behavior of nanocrystals in reactive chemical media. Moreover, the complexity and heterogeneity inherent in their atomic structures require tracking of structural transitions in individual nanocrystals at three-dimensional (3D) atomic resolution. In this study, we introduce the method of time-resolved Brownian tomography to investigate the temporal evolution of the 3D atomic structures of individual nanocrystals in solution. The methodology is applied to examine the atomic-level structural transformations of Pt nanocrystals during oxidative etching. The time-resolved 3D atomic maps reveal the structural evolution of dissolving Pt nanocrystals, transitioning from a crystalline to a disordered structure. Our study demonstrates the emergence of a phase at the nanometer length scale that has received less attention in bulk thermodynamics.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
2528035
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 16; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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