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: Contribution to journalArticle

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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

Thermal conductivity
Inelastic neutron scattering
Molecular dynamics
Earth (planet)
Experiments
cupric sulfide
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: Contribution to journalArticle

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