Observing crystal nucleation in four dimensions using atomic electron tomography

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

doi:10.1038/s41586-019-1317-x

Observing crystal nucleation in four dimensions using atomic electron tomography

Journal Article · Wed Jun 26 00:00:00 EDT 2019 · Nature (London)

DOI:https://doi.org/10.1038/s41586-019-1317-x· OSTI ID:1600536

Zhou, Jihan ^[1]; Yang, Yongsoo ^[2]; Yang, Yao ^[3]; Kim, Dennis S. ^[4]; Yuan, Andrew ^[4]; Tian, Xuezeng ^[4]; Ophus, Colin ^[3]; Sun, Fan ^[5]; Schmid, Andreas K. ^[3]; Nathanson, Michael ^[6]; Heinz, Hendrik ^[6]; An, Qi ^[7]; Zeng, Hao ^[5]; Ercius, Peter ^[3]; Miao, Jianwei ^[4]

Univ. of California, Los Angeles, CA (United States). California NanoSystems Inst.; Lawrence Berkeley National Laboratory
Univ. of California, Los Angeles, CA (United States). California NanoSystems Inst.; Korea Advanced Inst. of Science and Technology, Daejeon (South Korea)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Los Angeles, CA (United States). California NanoSystems Inst.
State Univ. of New York (SUNY), Buffalo, NY (United States); Univ. at Buffalo, NY (United States)
Univ. of Colorado, Boulder, CO (United States)
Univ. of Nevada, Reno, NV (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Los Angeles, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-05CH11231; SC0010378

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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