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Report No.

Enhanced covalency and nanostructured-phonon scattering lead to high thermoelectric performance in $$n$$-type PbS

Rathore, E.*; Juneja, R.*; Sarkar, D.*; Roychowdhury, S.*; Kofu, Maiko   ; Nakajima, Kenji  ; Singh, A. K.*; Biswas, K.*

We demonstrate a high thermoelectric figure of merit (zT) of 1.45 at 900 K for Ge doped (4-10 mol%) $$n$$-type PbS, which is the one of the highest values among all $$n$$-type PbS-based thermoelectric materials. This high performance is achieved by simultaneous (a) enhancement of covalency in chemical bonding which increases the electrical conductivity, and (b) reduction of lattice thermal conductivity to an ultra-low value of 0.56 W m$$^{-1}$$K$$^{-1}$$ at 900 K by the introduction of nanometer-sized (5-10 nm) precipitates of Pb$$_{2}$$GeS$$_{4}$$ in PbS matrix which strongly scatter the heat-carrying phonons. The presence of low-lying transverse acoustic (TA) and longitudinal acoustic (LA) phonon modes at 48.24 cm$$^{-1}$$ and 91.83 cm$$^{-1}$$, respectively are experimentally revealed from inelastic neutron scattering (INS) experiments. The softening of low-frequency modes at a higher temperature and ultra-short phonon lifetime (1-4.5 ps) further explain the ultra-low thermal conductivity.



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Category:Chemistry, Physical



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