Temperature-dependent interatomic force constants and phonon coherent resonance contribution in quaternary non-centrosymmetric chalcogenides BaAg2SnSe4

Abstract

Phonon heat transfer by thermoelectric modules undoubtedly plays a pivotal role for the future waste heat recovery and utilization. BaAg2SnSe4, a prototypical glasslike compound among quaternary non-centrosymmetric chalcogenides, demonstrates remarkable thermoelectric performance due to its exceptionally low lattice thermal conductivity (κL). Even with a comprehensive grasp of the underlying cause behind ultra-low κL and the subsequent heightened thermoelectric conversion efficiency, the temperature-dependent lattice dynamics and glass-like attributes governing κL continue to pose unresolved questions. In this study, we investigate the phonon thermal transport properties of quaternary BaAg2SnSe4 by incorporating the influence of phonon coherent resonance, thereby departing from the conventional Peierls's framework. Based on the temperature dependence of the interatomic force constants and coherences’ contribution to total lattice thermal conductivity (κL(C)), we intriguingly observe that the particle-like driven lattice thermal conductivity (κL(P)) and κL(C) have the quite significant and dominant role for describing ultralow phonon transport behaviors in the middle-high-temperature regions. Specially, enhanced phonon anharmonicity coupled with excited coherent phonons due to increasing temperature yields two close values, with 700 K values of 0.16 and 0.13 W/mK predicted for BaAg2SnSe4, respectively, accelerating its application in thermoelectric field. Furthermore, we also find that the off-diagonal terms of heat flux operators in κL exist distinction for different phonons, with zero contribution modes exhibiting temperature-independent phonon coherence effect. Temperature response of the force constants tensors and coherent resonance proposed in our work can be employed as a powerful tool, which would substantially be expected to inspire a broad revisiting phonon transport study in various device applications, including advanced thermal barrier coatings and superior thermoelectrics.