Recently,PbSnSe_(2)alloy was found to exhibit a large hysteresis effect on transport properties,demonstrating its significant potential for thermoelectric applications.Using ab initio approaches,we studied the carrier...Recently,PbSnSe_(2)alloy was found to exhibit a large hysteresis effect on transport properties,demonstrating its significant potential for thermoelectric applications.Using ab initio approaches,we studied the carrier transport properties of PbSnSe_(2)crystal,which is a special case of the alloy with the shortest-range order.A peak power factor of 134.2μW cm^(-1)K^(-2)was found along the crossplane direction in the n-type PbSnSe_(2)at a doping concentration of 7×10^(20)cm^(-3)at 700 K.This high power factor originates from delocalized p electrons between intra-plane Pb-Se pairs and between cross-plane Sn-Se pairs that can build up transport channels for conducting electrons,leading to a high electrical conductivity of 5.9×10^(5)S m^(-1).Introducing Pb atoms into Pnma phase SnSe can decrease the phonon group velocities and enhance the phonon-phonon scatterings,leading to a low thermal conductivity of 0.53 W m^(-1)K^(-1)at 700 K along the cross-plane direction.The calculated peak ZT of~3 along the cross-plane direction at an n-type doping concentration of around 5×10^(19)cm^(-3),which represents a theoretical upper limit for an idealized PbSnSe_(2)crystal.This work interprets the origins of three-dimensional charge and two-dimensional phonon transport behavior in PbSnSe_(2)and demonstrates that such crystals are promising high-performance thermoelectric semiconductors.展开更多
基金National Key Research and Development Program of China,Grant/Award Number:2022YFB3803900National Natural Science Foundation of China,Grant/Award Number:52076089。
文摘Recently,PbSnSe_(2)alloy was found to exhibit a large hysteresis effect on transport properties,demonstrating its significant potential for thermoelectric applications.Using ab initio approaches,we studied the carrier transport properties of PbSnSe_(2)crystal,which is a special case of the alloy with the shortest-range order.A peak power factor of 134.2μW cm^(-1)K^(-2)was found along the crossplane direction in the n-type PbSnSe_(2)at a doping concentration of 7×10^(20)cm^(-3)at 700 K.This high power factor originates from delocalized p electrons between intra-plane Pb-Se pairs and between cross-plane Sn-Se pairs that can build up transport channels for conducting electrons,leading to a high electrical conductivity of 5.9×10^(5)S m^(-1).Introducing Pb atoms into Pnma phase SnSe can decrease the phonon group velocities and enhance the phonon-phonon scatterings,leading to a low thermal conductivity of 0.53 W m^(-1)K^(-1)at 700 K along the cross-plane direction.The calculated peak ZT of~3 along the cross-plane direction at an n-type doping concentration of around 5×10^(19)cm^(-3),which represents a theoretical upper limit for an idealized PbSnSe_(2)crystal.This work interprets the origins of three-dimensional charge and two-dimensional phonon transport behavior in PbSnSe_(2)and demonstrates that such crystals are promising high-performance thermoelectric semiconductors.
