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    Dynamical Heterogeneity in the Supercooled Liquid State of the Phase Change Material GeTe
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    † Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1-5 CH-8093 Zurich, Switzerland
    ⊥ Faculty of Informatics, Università della Svizzera Italiana, Via G. Buffi 13, CH-6900 Lugano, Switzerland
    ‡ Department of Civil, Environmental and Geomatic Engineering, ETH Zurich, CH-8903 Zurich, Switzerland
    Lehrstuhl für Theoretische Chemie, Ruhr-Universität Bochum, Universitätsstrasse 150, D-44780 Bochum, Germany, and
    § Dipartimento di Scienza dei Materiali, Università di Milano-Bicocca, Via R. Cozzi 53, I-20125 Milano, Italy
    *(G.C.S.) E-mail: [email protected]
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    The Journal of Physical Chemistry B

    Cite this: J. Phys. Chem. B 2014, 118, 47, 13621–13628
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    https://doi.org/10.1021/jp507361f
    Published October 30, 2014
    Copyright © 2014 American Chemical Society
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    Abstract

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    A contending technology for nonvolatile memories of the next generation is based on a remarkable property of chalcogenide alloys known as phase change materials, namely their ability to undergo a fast and reversible transition between the amorphous and crystalline phases upon heating. The fast crystallization has been ascribed to the persistence of a high atomic mobility in the supercooled liquid phase, down to temperatures close to the glass transition. In this work we unravel the atomistic, structural origin of this feature in the supercooled liquid state of GeTe, a prototypical phase change compound, by means of molecular dynamic simulations. To this end, we employed an interatomic potential based on a neural network framework, which allows simulating thousands of atoms for tens of ns by keeping an accuracy close to that of the underlying first-principles framework. Our findings demonstrate that the high atomic mobility is related to the presence of clusters of slow and fast moving atoms. The latter contain a large fraction of chains of homopolar Ge–Ge bonds, which at low temperatures have a tendency to move by discontinuous cage-jump rearrangements. This structural fingerprint of dynamical heterogeneity provides an explanation of the breakdown of the Stokes–Einstein relation in GeTe, which is the ultimate origin of the fast crystallization of phase change materials exploited in the devices.

    Copyright © 2014 American Chemical Society

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    Results of dynamical heterogeneity in the supercooled liquid state of the phase change material GeTe. This material is available free of charge via the Internet at http://pubs.acs.org.

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    The Journal of Physical Chemistry B

    Cite this: J. Phys. Chem. B 2014, 118, 47, 13621–13628
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jp507361f
    Published October 30, 2014
    Copyright © 2014 American Chemical Society
    Request reuse permissions

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