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Phonon densities of states (DOS) for the high performing thermoelectricmaterial, AgPbmSbTe2+m (LAST-m, m = 16, 18, and 20), were extracted fromtime-of-flight inelastic neutron scattering measurements. The phonon DOS ofLAST-18 differs remarkably from LAST-16 and LAST-20 by exhibiting a dramaticbroadening of its acoustic modes that increases on heating. This broadeningcoincides with a minimum in the thermal conductivity, a maximum in theelectrical conductivity and Seebeck coefficient, and a related peak inthermoelectric performance. We argue that the anomalous broadening originateswith scattering enhanced by modifications to Te-Ag(Sb) bonds caused by theirresonant electronic states falling near the Fermi energy for m = 18.

Lattice dynamical origin of peak thermoelectric performance in AgPbmSbTe2+m observed by inelastic neutron scattering