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The candidate thermoelectric compounds Mg 3 Sb 2 and Mg 3 Bi 2 show excellent performance near ambient temperature, enabled by an anomalously low lattice thermal conductivity (κ l ) comparable to those of much heavier PbTe or Bi 2 Te 3 Contrary to common mass-trend expectations, replacing Mg with heavier Ca or Yb yields a threefold increase in κ l in CaMg 2 Sb 2 and YbMg 2 Bi 2 Here, we report a comprehensive analysis of phonons in the series A Mg 2  X  2 ( A = Mg, Ca, and Yb; X = Bi and Sb) based on inelastic neutron/x-ray scattering and first-principles simulations and show that the anomalously low κ l of Mg 3  X  2 has inherent phononic origins. We uncover a large phonon softening and flattening of low-energy transverse acoustic phonons in Mg 3  X  2 compared to the ternary analogs and traced to a specific Mg- X bond, which markedly enlarges the scattering phase-space, enabling the threefold tuning in κ l These results provide key insights for manipulating phonon scattering without the traditional reliance on heavy elements.

Soft anharmonic phonons and ultralow thermal conductivity in Mg 3 (Sb, Bi) 2 thermoelectrics

Soft anharmonic phonons and ultralow thermal conductivity in Mg ₃ (Sb, Bi) ₂ thermoelectrics