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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:
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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: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: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
Publisher's Version of Record
DOI: 10.1126/science.aaw1773

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Cited by: 16 works
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    Works referencing / citing this record:

    Fragile-to-Strong Crossover in Supercooled Liquid Ag-In-Sb-Te Studied by Ultrafast Calorimetry
    journal, July 2015

    • Orava, Jiri; Hewak, Daniel W.; Greer, A. Lindsay
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    • DOI: 10.1002/adfm.201501607

    Characteristic Ordering in Liquid Phase-Change Materials
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    • Steimer, Christoph; Coulet, Vanessa; Welnic, Wojciech
    • Advanced Materials, Vol. 20, Issue 23
    • DOI: 10.1002/adma.200700016

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    journal, October 2018

    • Wuttig, Matthias; Deringer, Volker L.; Gonze, Xavier
    • Advanced Materials, Vol. 30, Issue 51
    • DOI: 10.1002/adma.201803777

    A Quantum‐Mechanical Map for Bonding and Properties in Solids
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    • Raty, Jean‐Yves; Schumacher, Mathias; Golub, Pavlo
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    • DOI: 10.1007/s003390101087

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    • DOI: 10.1021/cg500347g

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    • DOI: 10.1038/35053024

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    • DOI: 10.1038/35087524

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    Measurement of crystal growth velocity in a melt-quenched phase-change material
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    • Salinga, Martin; Carria, Egidio; Kaldenbach, Andreas
    • Nature Communications, Vol. 4, Issue 1
    • DOI: 10.1038/ncomms3371

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    • Raty, Jean Yves; Zhang, Wei; Luckas, Jennifer
    • Nature Communications, Vol. 6, Issue 1
    • DOI: 10.1038/ncomms8467

    Phase-change materials for rewriteable data storage
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    • Wuttig, Matthias; Yamada, Noboru
    • Nature Materials, Vol. 6, Issue 11
    • DOI: 10.1038/nmat2009

    Resonant bonding in crystalline phase-change materials
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    • Nature Materials, Vol. 7, Issue 8
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    • Nature Materials, Vol. 10, Issue 2
    • DOI: 10.1038/nmat2931

    Characterization of supercooled liquid Ge2Sb2Te5 and its crystallization by ultrafast-heating calorimetry
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    • Orava, J.; Greer, A. L.; Gholipour, B.
    • Nature Materials, Vol. 11, Issue 4
    • DOI: 10.1038/nmat3275

    Time-domain separation of optical properties from structural transitions in resonantly bonded materials
    journal, July 2015

    • Waldecker, Lutz; Miller, Timothy A.; Rudé, Miquel
    • Nature Materials, Vol. 14, Issue 10
    • DOI: 10.1038/nmat4359

    Liquid–liquid critical point in supercooled silicon
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    • Vasisht, Vishwas V.; Saw, Shibu; Sastry, Srikanth
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    • DOI: 10.1038/nphys1993

    How fragility makes phase-change data storage robust: insights from ab initio simulations
    journal, October 2014

    • Zhang, Wei; Ronneberger, Ider; Zalden, Peter
    • Scientific Reports, Vol. 4, Issue 1
    • DOI: 10.1038/srep06529

    Structural, electronic and kinetic properties of the phase-change material Ge2Sb2Te5 in the liquid state
    journal, June 2016

    • Schumacher, Mathias; Weber, Hans; Jóvári, Pál
    • Scientific Reports, Vol. 6, Issue 1
    • DOI: 10.1038/srep27434

    Dynamics of ultrafast reversible phase transitions in GeSb films triggered by picosecond laser pulses
    journal, November 1999

    • Siegel, J.; Afonso, C. N.; Solis, J.
    • Applied Physics Letters, Vol. 75, Issue 20
    • DOI: 10.1063/1.125244

    Mechanical stresses upon crystallization in phase change materials
    journal, November 2001

    • Pedersen, T. P. Leervad; Kalb, J.; Njoroge, W. K.
    • Applied Physics Letters, Vol. 79, Issue 22
    • DOI: 10.1063/1.1415419

    Calorimetric measurements of phase transformations in thin films of amorphous Te alloys used for optical data storage
    journal, March 2003

    • Kalb, J.; Spaepen, F.; Wuttig, M.
    • Journal of Applied Physics, Vol. 93, Issue 5
    • DOI: 10.1063/1.1540227

    Supercooled and Glassy Water
    journal, June 2003

    • Debenedetti, Pablo G.; Stanley, H. Eugene
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    • DOI: 10.1063/1.1595053

    Atomic force microscopy measurements of crystal nucleation and growth rates in thin films of amorphous Te alloys
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