Strong Lattice Softening Induced by Atomic Mismatch in Meta‐Phase Thermoelectrics

This work demonstrates the validity and universality of atomic mismatch‐induced lattice softening across three metaphase systems: Ag8Sn(S,Te), Cu2(S,Te) and Mg2(Si,Sn). Abstract Conventional strategies for suppressing lattice thermal conductivity κL typically focus on maximizing phonon scattering to reduce phonon mean free path. Such reductions, however, are limited to the interatomic spacing or phonon wavelength. Alternatively, herein, an effective approach is proposed to lower phonon velocity by introducing atoms with significant atomic mismatch into the crystal lattice of three meta‐phases. Specifically, substituting Te for S in Ag8SnS6 and Cu2S, or Sn for Si in Mg2Si considerably increases the atomic mass and weakens the chemical bonding, causing notable reductions in the sound velocity. This reduction further leads to an amorphous‐like, extremely low lattice thermal conductivity κL across the whole temperature range. Consequently, we achieve outstanding thermoelectric performance in these atomic mismatched meta‐phases, with a maximum zT of 1.0 for Ag8SnS4.99Te, 1.1 for Mg2Si0.5Sn0.5, and 2.0 for Cu2S0.5Te0.5. The work demonstrates a new approach to manipulating thermal conductions through lattice softening, providing a promising pathway for designing high‐performance thermoelectric materials. This work demonstrates the validity and universality of atomic mismatch-induced lattice softening across three metaphase systems: Ag 8 Sn(S,Te), Cu 2 (S,Te) and Mg 2 (Si,Sn). Abstract Conventional strategies for suppressing lattice thermal conductivity κ L typically focus on maximizing phonon scattering to reduce phonon mean free path. Such reductions, however, are limited to the interatomic spacing or phonon wavelength. Alternatively, herein, an effective approach is proposed to lower phonon velocity by introducing atoms with significant atomic mismatch into the crystal lattice of three meta-phases. Specifically, substituting Te for S in Ag 8 SnS 6 and Cu 2 S, or Sn for Si in Mg 2 Si considerably increases the atomic mass and weakens the chemical bonding, causing notable reductions in the sound velocity. This reduction further leads to an amorphous-like, extremely low lattice thermal conductivity κ L across the whole temperature range. Consequently, we achieve outstanding thermoelectric performance in these atomic mismatched meta-phases, with a maximum zT of 1.0 for Ag 8 SnS 4.99 Te, 1.1 for Mg 2 Si 0.5 Sn 0.5, and 2.0 for Cu 2 S 0.5 Te 0.5. The work demonstrates a new approach to manipulating thermal conductions through lattice softening, providing a promising pathway for designing high-performance thermoelectric materials. Advanced Science, Volume 12, Issue 48, December 29, 2025.