Layered rare-earth metal oxides,harnessing the dual properties of oxides and two-dimensional layered materials,exhibit remarkable thermal stability and quantum confinement effects.Therefore,this work adopts the first-...Layered rare-earth metal oxides,harnessing the dual properties of oxides and two-dimensional layered materials,exhibit remarkable thermal stability and quantum confinement effects.Therefore,this work adopts the first-principles calculation combined with the Boltzmann transport theory to predict the thermoelectric properties of NdZnSbO compound.The coexistence of weak interlayer van der Waals interactions,robust intralayer ionic bonding,and partial covalent bonding leads to remarkable bonding heterogeneity,which engenders pronounced phonon scattering and imposes constraints on thermal transport along the out-of-plane direction.The weakened chemical bonds induced by the antibonding states,together with the rattling-like behavior of the Zn atom,culminate in the profound anharmonicity in the layered NdZnSbO compound.The weakening bond and heavy element contribute to the softness of phonon modes,which significantly diminishes the phonon group velocity.The redistribution-dominated four-phonon scattering process spans a large optical gap,which effectively reduces the lattice thermal conductivity.The NdZnSbO compound exhibits direct semiconductor characteristic with a bandgap of 0.73 e V by adopting the Heyd-Scuseria-Ernzerhof(HSE06)functional in combination with spin–orbit coupling(SOC)effect.The multi-valley feature of NdZnSbO compound augur favorably for band degeneracy,thus amplifying the power factor.Consequently,an optimal figure-of-merit(ZT)of 3.40 at 900 K is achieved for the n-type NdZnSbO compound.The present study delves deeply insights into the origins for the low thermal conductivity of NdZnSbO compound and proposes an optimization scheme to enhance overall thermoelectric performance.展开更多
By combining neuroevolution potential(NEP)with phonon Boltzmann transport theory,we systematically investigate the thermal transport properties of three two-dimensional(2D)narrow bandgap semiconductors:Ca_(3)N_(2),Ba_...By combining neuroevolution potential(NEP)with phonon Boltzmann transport theory,we systematically investigate the thermal transport properties of three two-dimensional(2D)narrow bandgap semiconductors:Ca_(3)N_(2),Ba_(3)P_(2),and Ba_(3)As_(2).The room-temperature lattice thermal conductivities(κ_(L))of Ca_(3)N_(2),Ba_(3)P_(2),and Ba_(3)As_(2)considering only three-phonon scattering are 6.60 W/m K,11.90 W/m K,and 8.88 W/m K,respectively.When taking into account the higherorder phonon(four-phonon)scattering processes,theκL of these three materials decrease to 6.12 W/m K,9.73 W/m K and6.77 W/m K,respectively.Among these systems,Ba_(3)As_(2)undergoes the most pronounced suppression with a reduction of 23.8%.This is mainly due to the greater scattering phase space which enhances the four-phonon scattering.Meanwhile,it is revealed that unlike the traditional evaluation using the P_(4)/P_(3)ratio as an indicator of the strength of four-phonon interactions,the thermal conductivity of Ba_(3)P_(2)exhibits weaker four-phonon suppression behavior compared to Ba_(3)As_(2),despite hosting a higher P_(4)/P_(3)ratio.That is to say,the strength of four-phonon scattering cannot be evaluated solely by the ratio of P_(4)/P_(3).These results presented in this work shed light on the thermal transport properties of such new 2D semiconductors with narrow bandgaps.展开更多
基金Financial supports from the National Natural Science Foundation of China(21503039)Department of Science and Technology of Liaoning Province(2019MS164)+1 种基金Department of Education of Liaoning Province(LJ2020JCL034)Discipline Innovation Team of Liaoning Technical University(LNTU20TD-16)are greatly acknowledged。
文摘Layered rare-earth metal oxides,harnessing the dual properties of oxides and two-dimensional layered materials,exhibit remarkable thermal stability and quantum confinement effects.Therefore,this work adopts the first-principles calculation combined with the Boltzmann transport theory to predict the thermoelectric properties of NdZnSbO compound.The coexistence of weak interlayer van der Waals interactions,robust intralayer ionic bonding,and partial covalent bonding leads to remarkable bonding heterogeneity,which engenders pronounced phonon scattering and imposes constraints on thermal transport along the out-of-plane direction.The weakened chemical bonds induced by the antibonding states,together with the rattling-like behavior of the Zn atom,culminate in the profound anharmonicity in the layered NdZnSbO compound.The weakening bond and heavy element contribute to the softness of phonon modes,which significantly diminishes the phonon group velocity.The redistribution-dominated four-phonon scattering process spans a large optical gap,which effectively reduces the lattice thermal conductivity.The NdZnSbO compound exhibits direct semiconductor characteristic with a bandgap of 0.73 e V by adopting the Heyd-Scuseria-Ernzerhof(HSE06)functional in combination with spin–orbit coupling(SOC)effect.The multi-valley feature of NdZnSbO compound augur favorably for band degeneracy,thus amplifying the power factor.Consequently,an optimal figure-of-merit(ZT)of 3.40 at 900 K is achieved for the n-type NdZnSbO compound.The present study delves deeply insights into the origins for the low thermal conductivity of NdZnSbO compound and proposes an optimization scheme to enhance overall thermoelectric performance.
基金supported by the National Natural Science Foundation of China(Grant No.52372260)the Science Fund for Distinguished Young Scholars of Hunan Province(Grant Nos.2024JJ2048 and 2021JJ10036)+1 种基金the Science and Technology Innovation Program of Hunan Province(Grant No.2022RC1197)the Scientific Research Fund of Hunan Provincial Education Department(Grant No.22B0512)。
文摘By combining neuroevolution potential(NEP)with phonon Boltzmann transport theory,we systematically investigate the thermal transport properties of three two-dimensional(2D)narrow bandgap semiconductors:Ca_(3)N_(2),Ba_(3)P_(2),and Ba_(3)As_(2).The room-temperature lattice thermal conductivities(κ_(L))of Ca_(3)N_(2),Ba_(3)P_(2),and Ba_(3)As_(2)considering only three-phonon scattering are 6.60 W/m K,11.90 W/m K,and 8.88 W/m K,respectively.When taking into account the higherorder phonon(four-phonon)scattering processes,theκL of these three materials decrease to 6.12 W/m K,9.73 W/m K and6.77 W/m K,respectively.Among these systems,Ba_(3)As_(2)undergoes the most pronounced suppression with a reduction of 23.8%.This is mainly due to the greater scattering phase space which enhances the four-phonon scattering.Meanwhile,it is revealed that unlike the traditional evaluation using the P_(4)/P_(3)ratio as an indicator of the strength of four-phonon interactions,the thermal conductivity of Ba_(3)P_(2)exhibits weaker four-phonon suppression behavior compared to Ba_(3)As_(2),despite hosting a higher P_(4)/P_(3)ratio.That is to say,the strength of four-phonon scattering cannot be evaluated solely by the ratio of P_(4)/P_(3).These results presented in this work shed light on the thermal transport properties of such new 2D semiconductors with narrow bandgaps.
