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Title: Observing crystal nucleation in four dimensions using atomic electron tomography

Journal Article · · Nature (London)
 [1];  [2];  [3];  [4];  [4];  [4];  [3];  [5];  [3];  [6];  [6];  [7];  [5];  [3];  [4]
  1. Univ. of California, Los Angeles, CA (United States). California NanoSystems Inst.; Lawrence Berkeley National Laboratory
  2. Univ. of California, Los Angeles, CA (United States). California NanoSystems Inst.; Korea Advanced Inst. of Science and Technology, Daejeon (South Korea)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Univ. of California, Los Angeles, CA (United States). California NanoSystems Inst.
  5. State Univ. of New York (SUNY), Buffalo, NY (United States); Univ. at Buffalo, NY (United States)
  6. Univ. of Colorado, Boulder, CO (United States)
  7. Univ. of Nevada, Reno, NV (United States)
+ Show Author Affiliations

Nucleation plays a critical role in many physical and biological phenomena that range from crystallization, melting and evaporation to the formation of clouds and the initiation of neurodegenerative diseases. However, nucleation is a challenging process to study in experiments, especially in the early stage when several atoms or molecules start to form a new phase from a parent phase. A number of experimental and computational methods have been used to investigate nucleation processes, but experimental determination of the three-dimensional atomic structure and the dynamics of early stage nuclei has been unachievable. Here we use atomic electron tomography to study early stage nucleation in four dimensions (4D: that is, including time) at atomic resolution. Using FePt nanoparticles as a model system, we find that early stage nuclei are irregularly shaped, each has a core of one to a few atoms with the maximum order parameter, and the order parameter gradient points from the core to the boundary of the nucleus. We capture the structure and dynamics of the same nuclei undergoing growth, fluctuation, dissolution, merging and/or division, which are regulated by the order parameter distribution and its gradient. These experimental observations are corroborated by molecular dynamics simulations of heterogeneous and homogeneous nucleation in liquid–solid phase transitions of Pt. Our experimental and molecular dynamics results differ from classical nucleation theory, indicating that a theory beyond this is needed to describe early stage nucleation at the atomic scale. Looking forward, we anticipate that the reported approach will open the door to the study of many fundamental problems in materials science, nanoscience, condensed matter physics and chemistry, such as phase transition, atomic diffusion, grain boundary dynamics, interface motion, defect dynamics and surface reconstruction with 4D atomic resolution.

Research Organization:
Univ. of California, Los Angeles, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1600536
Alternate ID(s):
OSTI ID: 1831093
Journal Information:
Nature (London), Journal Name: Nature (London) Journal Issue: 7762 Vol. 570; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (9)

The Displacement Field Associated with the Freezing of a Melt and its Role in Determining Crystal Growth Kinetics preprint January 2020
Divining the shape of nascent polymer crystal nuclei journal October 2019
Atomic electron tomography in three and four dimensions journal April 2020
Divining the Shape of Nascent Polymer Crystal Nuclei text January 2019
Enantiomeric Control of Intrinsically Chiral Nanocrystals journal November 2019
Classical nucleation theory predicts the shape of the nucleus in homogeneous solidification journal January 2020
Correlating the three-dimensional atomic defects and electronic properties of two-dimensional transition metal dichalcogenides journal March 2020
Reaction coordinates and rate constants for liquid droplet nucleation: Quantifying the interplay between driving force and memory journal October 2019
The displacement field associated with the freezing of a melt and its role in determining crystal growth kinetics journal February 2020

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