First-principles studies of atomic dynamics in tetrahedrite thermoelectrics

Junchao Li, Mengze Zhu, Douglas L. Abernathy, Xianglin Ke, Donald T. Morelli, Wei Lai

    Research output: Research - peer-reviewArticle

    • 2 Citations

    Abstract

    Cu12Sb4S13-based tetrahedrites are high-performance thermoelectrics that contain earth-abundant and environmentally friendly elements. At present, the mechanistic understanding of their low lattice thermal conductivity (<1 W m-1 K-1 at 300 K) remains limited. This work applies first-principles molecular dynamics simulations, along with inelastic neutron scattering (INS) experiments, to study the incoherent and coherent atomic dynamics in Cu10.5NiZn0.5Sb4S13, in order to deepen our insight into mechanisms of anomalous dynamic behavior and low lattice thermal conductivity in tetrahedrites. Our study of incoherent dynamics reveals the anomalous "phonon softening upon cooling" behavior commonly observed in inelastic neutron scattering data. By examining the dynamic Cu-Sb distances inside the Sb[CuS3]Sb cage, we ascribe softening to the decreased anharmonic "rattling" of Cu in the cage. On the other hand, our study of coherent dynamics reveals that acoustic modes are confined in a small region of dynamic scattering space, which we hypothesize leads to a minimum phonon mean free path. By assuming a Debye model, we obtain a lattice minimum thermal conductivity value consistent with experiments. We believe this study furthers our understanding of the atomic dynamics of tetrahedrite thermoelectrics and will more generally help shed light on the origin of intrinsically low lattice thermal conductivity in these and other structurally similar materials.

    LanguageEnglish (US)
    Article number104811
    JournalAPL Materials
    Volume4
    Issue number10
    DOIs
    StatePublished - Oct 1 2016

    Profile

    cupric sulfide
    Thermal conductivity
    Inelastic neutron scattering
    Experiments
    Molecular dynamics
    Earth (planet)
    Scattering
    Cooling
    Computer simulation

    ASJC Scopus subject areas

    • Materials Science(all)
    • Engineering(all)

    Cite this

    First-principles studies of atomic dynamics in tetrahedrite thermoelectrics. / Li, Junchao; Zhu, Mengze; Abernathy, Douglas L.; Ke, Xianglin; Morelli, Donald T.; Lai, Wei.

    In: APL Materials, Vol. 4, No. 10, 104811, 01.10.2016.

    Research output: Research - peer-reviewArticle

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