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Time-resolved atomic-resolution Brownian tomography of single nanocrystals reveals size-dependent dynamics

Journal Article · · Science Advances
 [1];  [2];  [1];  [1];  [3];  [4];  [5];  [5];  [6];  [7];  [8];  [1]
  1. National Cancer Institute, Frederick, MD (United States)
  2. National Cancer Institute, Frederick, MD (United States); University of Maryland, College Park, MD (United States)
  3. University of Chicago, IL (United States)
  4. Cornell University, Ithaca, NY (United States)
  5. Institute for Basic Science (IBS), Seoul (Korea, Republic of); Seoul National University (Korea, Republic of)
  6. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  7. University of Maryland, College Park, MD (United States)
  8. Institute for Basic Science (IBS), Seoul (Korea, Republic of); Seoul National University (Korea, Republic of); Seoul National University, Gyeonggi-do (Korea, Republic of)

Atomic-resolution structure identification of nanocrystals by graphene liquid cell electron microscopy (GLC-EM) has revealed that small, solubilized platinum nanocrystals consist of an ordered crystalline core surrounded by mobile surface atoms, which dissociate during oxidative etching, resulting in distinct temporal structural states. Requirements imposed by the 3D reconstruction algorithm limit the number of structural states that can be resolved. We introduce a regularized 3D reconstruction algorithm that exploits the redundancy inherent in the experimental data, allowing us to improve the time resolution. Our developments provide a comprehensive molecular picture at unprecedented spatial and temporal resolution of the nonlinear, linear, and fluctuating dynamic phenomena that single nanocrystals undergo during the GLC-EM experiment. We determined atomic structures of 66 temporal structural states, extracted from 15 time trajectories of individual nanocrystals. Large (478 to 698 atoms) and small (<300 atoms) nanocrystals show etching that preserves a stable core, whereas mid-sized (351 to 571 atoms) nanocrystals present dynamics that change the coordination of the core.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
2587750
Journal Information:
Science Advances, Journal Name: Science Advances Journal Issue: 32 Vol. 11; ISSN 2375-2548
Publisher:
American Association for the Advancement of Science (AAAS)Copyright Statement
Country of Publication:
United States
Language:
English

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