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Title: Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction

The ultrafast laser excitation of matters leads to nonequilibrium states with complex solid-liquid phase-transition dynamics. In this paper, we used electron diffraction at mega–electron volt energies to visualize the ultrafast melting of gold on the atomic scale length. For energy densities approaching the irreversible melting regime, we first observed heterogeneous melting on time scales of 100 to 1000 picoseconds, transitioning to homogeneous melting that occurs catastrophically within 10 to 20 picoseconds at higher energy densities. We showed evidence for the heterogeneous coexistence of solid and liquid. We determined the ion and electron temperature evolution and found superheated conditions. Finally, our results constrain the electron-ion coupling rate, determine the Debye temperature, and reveal the melting sensitivity to nucleation seeds.
Authors:
ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [1] ;  [1] ;  [2] ; ORCiD logo [3] ;  [1] ; ORCiD logo [1] ;  [4] ; ORCiD logo [5] ; ORCiD logo [1] ; ORCiD logo [6] ; ORCiD logo [1] ; ORCiD logo [6] ; ORCiD logo [7] ; ORCiD logo [6] ; ORCiD logo [3] ;  [1] ;  [1] ; ORCiD logo [1]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Univ. of Rostock (Germany). Inst. of Physics
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  4. Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Physics and Astronomy
  5. Univ. of Rostock (Germany). Inst. of Physics
  6. Univ. of Alberta, Edmonton, AB (Canada). Dept. of Electrical and Computer Engineering
  7. Univ. of Duisburg-Essen, Duisburg (Germany). Faculty of Physics. Centre for Nanointegration Duisburg-Essen
Publication Date:
Report Number(s):
LA-UR-18-23801
Journal ID: ISSN 0036-8075
Grant/Contract Number:
AC52-06NA25396; AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 360; Journal Issue: 6396; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Office of Science (SC), Fusion Energy Sciences (FES) (SC-24); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Natural Sciences and Engineering Research Council of Canada (NSERC); German Research Foundation (DFG)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS
OSTI Identifier:
1459842

Mo, M. Z., Chen, Z., Li, R. K., Dunning, M., Witte, B. B. L., Baldwin, J. K., Fletcher, L. B., Kim, J. B., Ng, A., Redmer, R., Reid, A. H., Shekhar, P., Shen, X. Z., Shen, M., Sokolowski-Tinten, K., Tsui, Y. Y., Wang, Y. Q., Zheng, Q., Wang, X. J., and Glenzer, S. H.. Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction. United States: N. p., Web. doi:10.1126/science.aar2058.
Mo, M. Z., Chen, Z., Li, R. K., Dunning, M., Witte, B. B. L., Baldwin, J. K., Fletcher, L. B., Kim, J. B., Ng, A., Redmer, R., Reid, A. H., Shekhar, P., Shen, X. Z., Shen, M., Sokolowski-Tinten, K., Tsui, Y. Y., Wang, Y. Q., Zheng, Q., Wang, X. J., & Glenzer, S. H.. Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction. United States. doi:10.1126/science.aar2058.
Mo, M. Z., Chen, Z., Li, R. K., Dunning, M., Witte, B. B. L., Baldwin, J. K., Fletcher, L. B., Kim, J. B., Ng, A., Redmer, R., Reid, A. H., Shekhar, P., Shen, X. Z., Shen, M., Sokolowski-Tinten, K., Tsui, Y. Y., Wang, Y. Q., Zheng, Q., Wang, X. J., and Glenzer, S. H.. 2018. "Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction". United States. doi:10.1126/science.aar2058.
@article{osti_1459842,
title = {Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction},
author = {Mo, M. Z. and Chen, Z. and Li, R. K. and Dunning, M. and Witte, B. B. L. and Baldwin, J. K. and Fletcher, L. B. and Kim, J. B. and Ng, A. and Redmer, R. and Reid, A. H. and Shekhar, P. and Shen, X. Z. and Shen, M. and Sokolowski-Tinten, K. and Tsui, Y. Y. and Wang, Y. Q. and Zheng, Q. and Wang, X. J. and Glenzer, S. H.},
abstractNote = {The ultrafast laser excitation of matters leads to nonequilibrium states with complex solid-liquid phase-transition dynamics. In this paper, we used electron diffraction at mega–electron volt energies to visualize the ultrafast melting of gold on the atomic scale length. For energy densities approaching the irreversible melting regime, we first observed heterogeneous melting on time scales of 100 to 1000 picoseconds, transitioning to homogeneous melting that occurs catastrophically within 10 to 20 picoseconds at higher energy densities. We showed evidence for the heterogeneous coexistence of solid and liquid. We determined the ion and electron temperature evolution and found superheated conditions. Finally, our results constrain the electron-ion coupling rate, determine the Debye temperature, and reveal the melting sensitivity to nucleation seeds.},
doi = {10.1126/science.aar2058},
journal = {Science},
number = 6396,
volume = 360,
place = {United States},
year = {2018},
month = {6}
}