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Cation–Eutectic Transition via Sublattice Melting in CuInP2S6/In4/3P2S6 van der Waals Layered Crystals

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    Cation–Eutectic Transition via Sublattice Melting in CuInP2S6/In4/3P2S6 van der Waals Layered Crystals
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    † †Materials Science and Technology Division and ‡Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, Tennessee 37831, United States
    § X-Ray Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
    ∥ Aerospace Systems Directorate, Air Force Research Laboratory, 1950 Fifth Street, Bldg 18, Wright-Patterson Air Force Base, Ohio 45433, United States
    ⊥ UES Inc., 4401 Dayton-Xenia Road, Beavercreek, Ohio 45432, United States
    # School of Chemical & Biomolecular Engineering, Georgia Institute of Engineering, 311 Ferst Drive NW, Atlanta, Georgia 30332, United States
    *E-mail: [email protected]; [email protected]
    *E-mail: [email protected]
    *E-mail: [email protected]
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    ACS Nano

    Cite this: ACS Nano 2017, 11, 7, 7060–7073
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    https://doi.org/10.1021/acsnano.7b02695
    Published July 7, 2017
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    Abstract

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    Single crystals of the van der Waals layered ferrielectric material CuInP2S6 spontaneously phase separate when synthesized with Cu deficiency. Here we identify a route to form and tune intralayer heterostructures between the corresponding ferrielectric (CuInP2S6) and paraelectric (In4/3P2S6) phases through control of chemical phase separation. We conclusively demonstrate that Cu-deficient Cu1–xIn1+x/3P2S6 forms a single phase at high temperature. We also identify the mechanism by which the phase separation proceeds upon cooling. Above 500 K both Cu+ and In3+ become mobile, while P2S64– anions maintain their structure. We therefore propose that this transition can be understood as eutectic melting on the cation sublattice. Such a model suggests that the transition temperature for the melting process is relatively low because it requires only a partial reorganization of the crystal lattice. As a result, varying the cooling rate through the phase transition controls the lateral extent of chemical domains over several decades in size. At the fastest cooling rate, the dimensional confinement of the ferrielectric CuInP2S6 phase to nanoscale dimensions suppresses ferrielectric ordering due to the intrinsic ferroelectric size effect. Intralayer heterostructures can be formed, destroyed, and re-formed by thermal cycling, thus enabling the possibility of finely tuned ferroic structures that can potentially be optimized for specific device architectures.

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    ACS Nano

    Cite this: ACS Nano 2017, 11, 7, 7060–7073
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.7b02695
    Published July 7, 2017
    Copyright © 2017 American Chemical Society
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