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Journal Articles Proceedings of the National Academy of Sciences of the United States of America Year : 2021

Crystallization kinetics of atomic crystals revealed by a single-shot and single-particle X-ray diffraction experiment

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Akinobu Niozu
Liviu Neagu
Carlo Callegari
  • Function : Author
Michele Di Fraia
  • Function : Author
Giorgio Rossi
Davide Emilio Galli
  • Function : Author
Tommaso Pincelli
  • Function : Author
Alessandro Colombo
Shigeki Owada
Kensuke Tono
Takashi Kameshima
  • Function : Author
Yasumasa Joti
  • Function : Author
Tetsuo Katayama
  • Function : Author
Tadashi Togashi
  • Function : Author
Makina Yabashi
Kazuhiro Matsuda
Christoph Bostedt
  • Function : Author
Kiyoshi Ueda
Kiyonobu Nagaya
  • Function : Author

Abstract

Crystallization is a fundamental natural phenomenon and the ubiquitous physical process in materials science for the design of new materials. So far, experimental observations of the structural dynamics in crystallization have been mostly restricted to slow dynamics. We present here an exclusive way to explore the dynamics of crystallization in highly controlled conditions (i.e., in the absence of impurities acting as seeds of the crystallites) as it occurs in vacuum. We have measured the early formation stage of solid Xe nanoparticles nucleated in an expanding supercooled Xe jet by means of an X-ray diffraction experiment with 10-fs X-ray free-electron laser (XFEL) pulses. We found that the structure of Xe nanoparticles is not pure face-centered cubic (fcc), the expected stable phase, but a mixture of fcc and randomly stacked hexagonal close-packed (rhcp) structures. Furthermore, we identified the instantaneous coexistence of the comparably sized fcc and rhcp domains in single Xe nanoparticles. The observations are explained by the scenario of structural aging, in which the nanoparticles initially crystallize in the highly stacking-disordered rhcp phase and the structure later forms the stable fcc phase. The results are reminiscent of analogous observations in hard-sphere systems, indicating the universal role of the stacking-disordered phase in nucleation.

Dates and versions

cea-03495868 , version 1 (20-12-2021)

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Cite

Akinobu Niozu, Yoshiaki Kumagai, Toshiyuki Nishiyama Hiraki, Hironobu Fukuzawa, Koji Motomura, et al.. Crystallization kinetics of atomic crystals revealed by a single-shot and single-particle X-ray diffraction experiment. Proceedings of the National Academy of Sciences of the United States of America, 2021, 118 (51), pp.e2111747118. ⟨10.1073/pnas.2111747118⟩. ⟨cea-03495868⟩
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