Violation of the Stokes–Einstein relation in Ge2Sb2Te5, GeTe, Ag4In3Sb67Te26, and Ge15Sb85, and its connection to fast crystallization

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  • Shuai Wei
  • Christoph Persch, Institute of Physics (IA), RWTH Aachen University, Tyskland
  • Moritz Stolpe, Heraeus Holding GmbH
  • ,
  • Zach Evenson, Technical University of Munich
  • ,
  • Garrett Coleman, University of Arizona
  • ,
  • Pierre Lucas, University of Arizona
  • ,
  • Matthias Wuttig, Institute of Physics (IA), RWTH Aachen University, JARA-Institute Green IT (PGI-10, FZ-Jülich, Tyskland

Phase-change materials (PCMs) are already commercialized in optical and non-volatile memory devices. Yet, the dynamics of atomic rearrangement processes and their temperature dependence, which govern their ultrafast switching, are still not fully understood. Here we use quasi-elastic neutron scattering to investigate the liquid-state dynamics of four prevailing PCMs Ge2Sb2Te5, GeTe, Ag4In3Sb67Te26(AIST), and Ge15Sb85 above their respective melting points Tm. Self-diffusion coefficients and structural relaxation times on the timescale of picoseconds are extracted from dynamic structure factors. The results indicate an unusual systematic violation of the Stokes-Einstein relation (SER) for each PCM in high-temperature regions above Tm, where the atomic-mobility is high. This is likely related to the formation of locally favored structures in liquid PCMs. Absolute values of diffusivity in the supercooled liquid AIST are derived from crystal-growth velocity, which are almost one order of magnitude higher than that expected from the SER in the technologically relevant temperature range ~20% below Tm. This is relevant to understand the crystallization kinetics of PCMs as crystal growth is controlled by diffusivity. Furthermore, the instantaneous shear modulus is determined ranging from 2 to 3 GPa for liquid PCMs, which permits extracting viscosity from microscopic structural relaxations usually accessible to simulations and scattering techniques.

TidsskriftActa Materialia
Sider (fra-til)491-500
Antal sider10
StatusUdgivet - aug. 2020
Eksternt udgivetJa

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