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Title: Femtosecond x-ray diffraction reveals a liquid–liquid phase transition in phase-change materials

Abstract

In phase-change memory devices, a material is cycled between glassy and crystalline states. The highly temperature-dependent kinetics of its crystallization process enables application in memory technology, but the transition has not been resolved on an atomic scale. Using femtosecond x-ray diffraction and ab initio computer simulations, we determined the time-dependent pair-correlation function of phase-change materials throughout the melt-quenching and crystallization process. We found a liquid–liquid phase transition in the phase-change materials Ag 4 In 3 Sb 67 Te 26 and Ge 15 Sb 85 at 660 and 610 kelvin, respectively. The transition is predominantly caused by the onset of Peierls distortions, the amplitude of which correlates with an increase of the apparent activation energy of diffusivity. This reveals a relationship between atomic structure and kinetics, enabling a systematic optimization of the memory-switching kinetics.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [5];  [6]; ORCiD logo [2];  [7]; ORCiD logo [8];  [8];  [9];  [10]; ORCiD logo [11];  [11];  [12]; ORCiD logo [3]; ORCiD logo [8]; ORCiD logo [13];  [14]; ORCiD logo [10] more »; ORCiD logo [7]; ORCiD logo [3]; ORCiD logo [15]; ORCiD logo [2] « less
  1. Stanford PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Rd., Menlo Park, CA 94025, USA., Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Rd., Menlo Park, CA 94025, USA., European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany.
  2. Faculty of Physics and Center for Nanointegration Duisburg-Essen (CENIDE), University of Duisburg-Essen, Lotharstrasse 1, 47048 Duisburg, Germany.
  3. Institut für Theoretische Festkörperphysik, JARA-FIT and JARA-HPC, RWTH Aachen University, Germany.
  4. Instituto de Optica, CSIC, C/Serrano 121, 28006 Madrid, Spain.
  5. I. Physikalisches Institut and JARA-FIT, RWTH Aachen, Sommerfeldstrasse 14, 52074 Aachen, Germany.
  6. Faculty of Physics and Center for Nanointegration Duisburg-Essen (CENIDE), University of Duisburg-Essen, Lotharstrasse 1, 47048 Duisburg, Germany., Institut für Physik und Astronomie, Universität Potsdam, Karl-Liebknecht-Strasse 24-25, 14476 Potsdam, Germany.
  7. Stanford PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Rd., Menlo Park, CA 94025, USA., Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Rd., Menlo Park, CA 94025, USA.
  8. Department of Physics, Lund University, Professorsgatan 1, 223 62 Lund, Sweden.
  9. Department of Applied Physics, Stanford University, Stanford, CA 94305, USA.
  10. Lawrence Livermore National Laboratory, Livermore, CA 94550, USA.
  11. Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Rd., Menlo Park, CA 94025, USA.
  12. Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Rd., Menlo Park, CA 94025, USA., Paul Scherrer Institute, Forschungsstrasse 111, 5232 Villigen, Switzerland.
  13. Stanford PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Rd., Menlo Park, CA 94025, USA., Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Rd., Menlo Park, CA 94025, USA., Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305, USA.
  14. Institut Laue-Langevin, 71 Avenue des Martyrs, CS 20156, 38042 Grenoble Cedex 9, France.
  15. I. Physikalisches Institut and JARA-FIT, RWTH Aachen, Sommerfeldstrasse 14, 52074 Aachen, Germany., PGI 10 (Green IT), Forschungszentrum Jülich, 52428 Jülich, Germany.
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1527069
Alternate Identifier(s):
OSTI ID: 1532412
Grant/Contract Number:  
AC02-76SF00515; AC52-07NA27344; SFB 616 ”Energy Dissipation at Surfaces”; SFB 1242 “Non-Equilibrium Dynamics of Condensed Matter in the Time Domain”; So408/9-1; SFB 917 ”Nanoswitches”; Ma-5339/2-1; JARA0150 and JARA0183; VR
Resource Type:
Published Article
Journal Name:
Science
Additional Journal Information:
Journal Name: Science Journal Volume: 364 Journal Issue: 6445; Journal ID: ISSN 0036-8075
Publisher:
American Association for the Advancement of Science (AAAS)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Citation Formats

Zalden, Peter, Quirin, Florian, Schumacher, Mathias, Siegel, Jan, Wei, Shuai, Koc, Azize, Nicoul, Matthieu, Trigo, Mariano, Andreasson, Pererik, Enquist, Henrik, Shu, Michael J., Pardini, Tommaso, Chollet, Matthieu, Zhu, Diling, Lemke, Henrik, Ronneberger, Ider, Larsson, Jörgen, Lindenberg, Aaron M., Fischer, Henry E., Hau-Riege, Stefan, Reis, David A., Mazzarello, Riccardo, Wuttig, Matthias, and Sokolowski-Tinten, Klaus. Femtosecond x-ray diffraction reveals a liquid–liquid phase transition in phase-change materials. United States: N. p., 2019. Web. doi:10.1126/science.aaw1773.
Zalden, Peter, Quirin, Florian, Schumacher, Mathias, Siegel, Jan, Wei, Shuai, Koc, Azize, Nicoul, Matthieu, Trigo, Mariano, Andreasson, Pererik, Enquist, Henrik, Shu, Michael J., Pardini, Tommaso, Chollet, Matthieu, Zhu, Diling, Lemke, Henrik, Ronneberger, Ider, Larsson, Jörgen, Lindenberg, Aaron M., Fischer, Henry E., Hau-Riege, Stefan, Reis, David A., Mazzarello, Riccardo, Wuttig, Matthias, & Sokolowski-Tinten, Klaus. Femtosecond x-ray diffraction reveals a liquid–liquid phase transition in phase-change materials. United States. doi:https://doi.org/10.1126/science.aaw1773
Zalden, Peter, Quirin, Florian, Schumacher, Mathias, Siegel, Jan, Wei, Shuai, Koc, Azize, Nicoul, Matthieu, Trigo, Mariano, Andreasson, Pererik, Enquist, Henrik, Shu, Michael J., Pardini, Tommaso, Chollet, Matthieu, Zhu, Diling, Lemke, Henrik, Ronneberger, Ider, Larsson, Jörgen, Lindenberg, Aaron M., Fischer, Henry E., Hau-Riege, Stefan, Reis, David A., Mazzarello, Riccardo, Wuttig, Matthias, and Sokolowski-Tinten, Klaus. Thu . "Femtosecond x-ray diffraction reveals a liquid–liquid phase transition in phase-change materials". United States. doi:https://doi.org/10.1126/science.aaw1773.
@article{osti_1527069,
title = {Femtosecond x-ray diffraction reveals a liquid–liquid phase transition in phase-change materials},
author = {Zalden, Peter and Quirin, Florian and Schumacher, Mathias and Siegel, Jan and Wei, Shuai and Koc, Azize and Nicoul, Matthieu and Trigo, Mariano and Andreasson, Pererik and Enquist, Henrik and Shu, Michael J. and Pardini, Tommaso and Chollet, Matthieu and Zhu, Diling and Lemke, Henrik and Ronneberger, Ider and Larsson, Jörgen and Lindenberg, Aaron M. and Fischer, Henry E. and Hau-Riege, Stefan and Reis, David A. and Mazzarello, Riccardo and Wuttig, Matthias and Sokolowski-Tinten, Klaus},
abstractNote = {In phase-change memory devices, a material is cycled between glassy and crystalline states. The highly temperature-dependent kinetics of its crystallization process enables application in memory technology, but the transition has not been resolved on an atomic scale. Using femtosecond x-ray diffraction and ab initio computer simulations, we determined the time-dependent pair-correlation function of phase-change materials throughout the melt-quenching and crystallization process. We found a liquid–liquid phase transition in the phase-change materials Ag 4 In 3 Sb 67 Te 26 and Ge 15 Sb 85 at 660 and 610 kelvin, respectively. The transition is predominantly caused by the onset of Peierls distortions, the amplitude of which correlates with an increase of the apparent activation energy of diffusivity. This reveals a relationship between atomic structure and kinetics, enabling a systematic optimization of the memory-switching kinetics.},
doi = {10.1126/science.aaw1773},
journal = {Science},
number = 6445,
volume = 364,
place = {United States},
year = {2019},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
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DOI: https://doi.org/10.1126/science.aaw1773

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Cited by: 33 works
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