Reversible disorder-order transitions in atomic crystal nucleation

Author:

Jeon Sungho1ORCID,Heo Taeyeong1ORCID,Hwang Sang-Yeon2ORCID,Ciston Jim3ORCID,Bustillo Karen C.3ORCID,Reed Bryan W.4ORCID,Ham Jimin1ORCID,Kang Sungsu56,Kim Sungin56ORCID,Lim Joowon1ORCID,Lim Kitaek1ORCID,Kim Ji Soo56,Kang Min-Ho56ORCID,Bloom Ruth S.4ORCID,Hong Sukjoon1ORCID,Kim Kwanpyo78ORCID,Zettl Alex91011ORCID,Kim Woo Youn2ORCID,Ercius Peter3ORCID,Park Jungwon56ORCID,Lee Won Chul1ORCID

Affiliation:

1. Department of Mechanical Engineering, BK21 FOUR ERICA-ACE Center, Hanyang University, Ansan, Gyeonggi 15588, Republic of Korea.

2. Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea.

3. National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA 94720, USA.

4. Integrated Dynamic Electron Solutions, Inc., Pleasanton, CA 94588, USA.

5. School of Chemical and Biological Engineering and Institute of Chemical Processes, Seoul National University, Seoul 08826, Republic of Korea.

6. Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea.

7. Department of Physics, Yonsei University, Seoul 03722, Republic of Korea.

8. Center for Nanomedicine, IBS, Seoul 03722, Republic of Korea.

9. Department of Physics, University of California, Berkeley, CA 94720, USA.

10. Materials Sciences Division, LBNL, Berkeley, CA 94720, USA.

11. Kavli Energy NanoSciences Institute, Berkeley, CA 94720, USA.

Abstract

Watching early stage nucleation In classic nucleation theory, a metastable disordered dense liquid or amorphous solid cluster spontaneously and irreversibly transforms into a crystalline nucleus. Jeon et al. observed the formation of gold crystals on a graphene substrate through the reduction of a precursor using an electron beam. Rather than the classic view, they instead observed a nucleation pathway that involves dynamic and reversible fluctuations of developing nuclei between disordered and crystalline states. The lifetime in the disordered state decreases with increasing cluster size, and at sufficiently small sizes, the binding energy per atom is large enough relative to the energy required to induce melting that the heat imparted upon binding is enough to drive partial collapse of an ordered cluster into the disordered state. Science , this issue p. 498

Funder

National Science Foundation

U.S. Department of Energy

National Research Foundation of Korea

Samsung Science and Technology Foundation

Institutes for Basic Science

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

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