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

Abstract

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 homogeneousmore » 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.« less

Authors:
 [1];  [2];  [3];  [1];  [1];  [1];  [3];  [4];  [3];  [5];  [5];  [6];  [4];  [3];  [1]
  1. Univ. of California, Los Angeles, CA (United States). California NanoSystems Inst.
  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. State Univ. of New York (SUNY), Buffalo, NY (United States); Univ. at Buffalo, NY (United States)
  5. Univ. of Colorado, Boulder, CO (United States)
  6. Univ. of Nevada, Reno, NV (United States)
Publication Date:
Research Org.:
Univ. of California, Los Angeles, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1600536
Grant/Contract Number:  
[AC02-05CH11231]
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
[Journal Name: Nature (London); Journal Volume: 570; Journal Issue: 7762; Related Information: See atomic structures deposited in the Materials Databank (https://www.materialsdatabank.org/)Other raw data and code:http://www.physics.ucla.edu/research/imaging/nucleation/index.html]; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Zhou, Jihan, Yang, Yongsoo, Yang, Yao, Kim, Dennis S., Yuan, Andrew, Tian, Xuezeng, Ophus, Colin, Sun, Fan, Schmid, Andreas K., Nathanson, Michael, Heinz, Hendrik, An, Qi, Zeng, Hao, Ercius, Peter, and Miao, Jianwei. Observing crystal nucleation in four dimensions using atomic electron tomography. United States: N. p., 2019. Web. doi:10.1038/s41586-019-1317-x.
Zhou, Jihan, Yang, Yongsoo, Yang, Yao, Kim, Dennis S., Yuan, Andrew, Tian, Xuezeng, Ophus, Colin, Sun, Fan, Schmid, Andreas K., Nathanson, Michael, Heinz, Hendrik, An, Qi, Zeng, Hao, Ercius, Peter, & Miao, Jianwei. Observing crystal nucleation in four dimensions using atomic electron tomography. United States. doi:10.1038/s41586-019-1317-x.
Zhou, Jihan, Yang, Yongsoo, Yang, Yao, Kim, Dennis S., Yuan, Andrew, Tian, Xuezeng, Ophus, Colin, Sun, Fan, Schmid, Andreas K., Nathanson, Michael, Heinz, Hendrik, An, Qi, Zeng, Hao, Ercius, Peter, and Miao, Jianwei. Wed . "Observing crystal nucleation in four dimensions using atomic electron tomography". United States. doi:10.1038/s41586-019-1317-x.
@article{osti_1600536,
title = {Observing crystal nucleation in four dimensions using atomic electron tomography},
author = {Zhou, Jihan and Yang, Yongsoo and Yang, Yao and Kim, Dennis S. and Yuan, Andrew and Tian, Xuezeng and Ophus, Colin and Sun, Fan and Schmid, Andreas K. and Nathanson, Michael and Heinz, Hendrik and An, Qi and Zeng, Hao and Ercius, Peter and Miao, Jianwei},
abstractNote = {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.},
doi = {10.1038/s41586-019-1317-x},
journal = {Nature (London)},
number = [7762],
volume = [570],
place = {United States},
year = {2019},
month = {6}
}

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Works referenced in this record:

Prediction of absolute crystal-nucleation rate in hard-sphere colloids
journal, February 2001

  • Auer, Stefan; Frenkel, Daan
  • Nature, Vol. 409, Issue 6823
  • DOI: 10.1038/35059035

Three-dimensional coordinates of individual atoms in materials revealed by electron tomography
journal, September 2015

  • Xu, Rui; Chen, Chien-Chun; Wu, Li
  • Nature Materials, Vol. 14, Issue 11
  • DOI: 10.1038/nmat4426

Accurate determination of crystal structures based on averaged local bond order parameters
journal, September 2008

  • Lechner, Wolfgang; Dellago, Christoph
  • The Journal of Chemical Physics, Vol. 129, Issue 11
  • DOI: 10.1063/1.2977970

FePt Nanoparticles as an Fe Reservoir for Controlled Fe Release and Tumor Inhibition
journal, October 2009

  • Xu, Chenjie; Yuan, Zhenglong; Kohler, Nathan
  • Journal of the American Chemical Society, Vol. 131, Issue 42
  • DOI: 10.1021/ja905938a

Electron tomography at 2.4-ångström resolution
journal, March 2012

  • Scott, M. C.; Chen, Chien-Chun; Mecklenburg, Matthew
  • Nature, Vol. 483, Issue 7390
  • DOI: 10.1038/nature10934

GENFIRE: A generalized Fourier iterative reconstruction algorithm for high-resolution 3D imaging
journal, September 2017


Real-Space Imaging of Nucleation and Growth in Colloidal Crystallization
journal, April 2001


Bond-orientational order in liquids and glasses
journal, July 1983

  • Steinhardt, Paul J.; Nelson, David R.; Ronchetti, Marco
  • Physical Review B, Vol. 28, Issue 2
  • DOI: 10.1103/PhysRevB.28.784

Nucleation
journal, December 2010

  • Vekilov, Peter G.
  • Crystal Growth & Design, Vol. 10, Issue 12
  • DOI: 10.1021/cg1011633

Theoretical study of antiphase boundaries in fcc alloys
journal, August 1990


Self-propagation of pathogenic protein aggregates in neurodegenerative diseases
journal, September 2013


Building two-dimensional materials one row at a time: Avoiding the nucleation barrier
journal, December 2018


Quasi-planar nucleus structure in apoferritin crystallization
journal, August 2000

  • Yau, S. -T.; Vekilov, Peter G.
  • Nature, Vol. 406, Issue 6795
  • DOI: 10.1038/35020035

In situ TEM imaging of CaCO3 nucleation reveals coexistence of direct and indirect pathways
journal, September 2014


Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995


Image Denoising by Sparse 3-D Transform-Domain Collaborative Filtering
journal, August 2007

  • Dabov, Kostadin; Foi, Alessandro; Katkovnik, Vladimir
  • IEEE Transactions on Image Processing, Vol. 16, Issue 8
  • DOI: 10.1109/TIP.2007.901238

Volume, Shape, and Roundness of Quartz Particles
journal, April 1935

  • Wadell, Hakon
  • The Journal of Geology, Vol. 43, Issue 3
  • DOI: 10.1086/624298

Numerical prediction of absolute crystallization rates in hard-sphere colloids
journal, February 2004

  • Auer, S.; Frenkel, D.
  • The Journal of Chemical Physics, Vol. 120, Issue 6
  • DOI: 10.1063/1.1638740

Insights into phase transition kinetics from colloid science
journal, April 2002

  • Anderson, Valerie J.; Lekkerkerker, Henk N. W.
  • Nature, Vol. 416, Issue 6883
  • DOI: 10.1038/416811a

Stable Prenucleation Calcium Carbonate Clusters
journal, December 2008


Misfit-energy-increasing dislocations in vapor-deposited CoFe/NiFe multilayers
journal, April 2004


The microscopic pathway to crystallization in supercooled liquids
journal, July 2012

  • Russo, John; Tanaka, Hajime
  • Scientific Reports, Vol. 2, Issue 1
  • DOI: 10.1038/srep00505

Deciphering chemical order/disorder and material properties at the single-atom level
journal, February 2017

  • Yang, Yongsoo; Chen, Chien-Chun; Scott, M. C.
  • Nature, Vol. 542, Issue 7639
  • DOI: 10.1038/nature21042

Heterogeneous nucleation and shape transformation of multicomponent metallic nanostructures
journal, November 2014

  • Kwon, Soon Gu; Krylova, Galyna; Phillips, Patrick J.
  • Nature Materials, Vol. 14, Issue 2
  • DOI: 10.1038/nmat4115

Three-dimensional imaging of dislocations in a nanoparticle at atomic resolution
journal, March 2013

  • Chen, Chien-Chun; Zhu, Chun; White, Edward R.
  • Nature, Vol. 496, Issue 7443
  • DOI: 10.1038/nature12009

Precise particle tracking against a complicated background: polynomial fitting with Gaussian weight
journal, September 2007


Formation of bimetallic clusters in superfluid helium nanodroplets analysed by atomic resolution electron tomography
journal, October 2015

  • Haberfehlner, Georg; Thaler, Philipp; Knez, Daniel
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9779

Atomic electron tomography: 3D structures without crystals
journal, September 2016


Three-Dimensional Elemental Mapping at the Atomic Scale in Bimetallic Nanocrystals
journal, August 2013

  • Goris, Bart; De Backer, Annick; Van Aert, Sandra
  • Nano Letters, Vol. 13, Issue 9
  • DOI: 10.1021/nl401945b

Origin of the Failure of Classical Nucleation Theory: Incorrect Description of the Smallest Clusters
journal, April 2007


The Initial Stages of Template-Controlled CaCO3 Formation Revealed by Cryo-TEM
journal, March 2009

  • Pouget, E. M.; Bomans, P. H. H.; Goos, J. A. C. M.
  • Science, Vol. 323, Issue 5920, p. 1455-1458
  • DOI: 10.1126/science.1169434

Observing classical nucleation theory at work by monitoring phase transitions with molecular precision
journal, December 2014

  • Sleutel, Mike; Lutsko, Jim; Van Driessche, Alexander E. S.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6598

Accurate Simulation of Surfaces and Interfaces of Face-Centered Cubic Metals Using 12−6 and 9−6 Lennard-Jones Potentials
journal, October 2008

  • Heinz, Hendrik; Vaia, R. A.; Farmer, B. L.
  • The Journal of Physical Chemistry C, Vol. 112, Issue 44
  • DOI: 10.1021/jp801931d

Molecular nucleation mechanisms and control strategies for crystal polymorph selection
journal, April 2018

  • Van Driessche, Alexander E. S.; Van Gerven, Nani; Bomans, Paul H. H.
  • Nature, Vol. 556, Issue 7699
  • DOI: 10.1038/nature25971

Enhancement of Protein Crystal Nucleation by Critical Density Fluctuations
journal, September 1997


Structure and bonding at the atomic scale by scanning transmission electron microscopy
journal, April 2009


Melting of icosahedral gold nanoclusters from molecular dynamics simulations
journal, June 2005

  • Wang, Yanting; Teitel, S.; Dellago, Christoph
  • The Journal of Chemical Physics, Vol. 122, Issue 21
  • DOI: 10.1063/1.1917756