Improved thermoelectric performance in PbSe–AgSbSe2 by manipulating the spin-orbit coupling effects

Duan, Sichen; Wang, Hongxiang; Liu, Guoqiang; Wu, Qing-Song; Man, Na; Zhang, Qiang; Tan, Xiaojian; Yin, Yinong; Xiao, Yukun; Hu, Haoyang; Xu, Jingtao; Guo, Kai; Yang, Xinxin; Jiang, Jun

doi:10.1016/j.nanoen.2020.105232

Cited by 26 publications

(37 citation statements)

References 49 publications

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“…[39] However, recent study suggested that the major reason for the increased bandgap in such alloys is the decrease of the lattice constant. [46] As shown in Figure 1a, the increase of bandgap in Pb 1-2x (NaSb) x Se does be accompanied by the decreasing lattice constant. We will show that the two different explanations can lead to different strategies for performance optimization.…”

Section: Resultsmentioning

confidence: 81%

“…Similar approximation was also applied in a previous study on PbSe-AgSbSe 2 , while the calculation results are in good agreement with experimental measurements. [46] As shown in Figure 4a, the pristine PbSe shows a small bandgap of about 0.1 eV, while the compressed PbSe shows a much larger bandgap of ≈0.5 eV. Note that the calculation without spin-orbit coupling produces a metallic phase for PbSe-NaSbSe 2 , as shown in Figure S7, Supporting Information.…”

Section: Resultsmentioning

confidence: 90%

“…The similar relationship between bandgap and lattice constant has been observed in PbSe-AgSbSe 2 . [46] The similar phenomena in the two solid solutions imply that the lattice constant is the key parameter to the band structure modification. For this reason, the band structure of PbSe-NaSbSe 2 solid solution is represented by the one for compressed PbSe.…”

Section: Resultsmentioning

confidence: 94%

“…[44] Recently, the PbSe-based high entropy compounds of Pb 0.99−y Sb 0.012 Sn y Se 1−2x Te x S x were synthesized by B. Jiang et al With the significantly reduced thermal conductivity, the peak ZT of the high-entropy compound reaches 1.8 at 900 K. [45] In the solid solution of PbSe-AgSbSe 2 , a novel strategy of manipulating spin-orbit coupling was reported. [46] Owing to the smaller lattice constant of cubic AgSbSe 2 , the valence and conduction bands of the solid solution would overlap each other at a certain alloying concentration, as the shortening of bond-length enhances the band dispersion. When spin-orbit coupling is taken into account, the band degeneracy at the crossing points is lifted and a bandgap is reopened again.…”

Section: Introductionmentioning

confidence: 99%

“…With the anomalous band structure, the optimized PbSe-AgSbSe 2 solid solution exhibits a much higher Seebeck coefficient than other n-type PbSe-based materials, and an enhanced peak ZT of 1.65 at 850 K was obtained. [46] Considering the similar chemical and crystal structure of AgSbSe 2 and NaSbSe 2 , the enlargement of bandgap in PbSe-NaSbSe 2 would also be due to spin-orbit coupling. If so, PbSe-NaSbSe 2 may require different optimizing conditions from the normal PbSe-based materials.…”

Section: Introductionmentioning

confidence: 99%

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Boosting the Thermoelectric Performance of PbSe from the Band Convergence Driven By Spin‐Orbit Coupling

Cai

Yang

Liu

et al. 2022

Advanced Energy Materials

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the system with weak electron-phonon coupling, the lattice contribution to the thermal conductivity, κ l , can be treated as an independent parameter, since the other transport factors are purely electron dependent. [8][9][10] Some schemes, such as nanostructures and defect engineering, have been implemented to reduce the lattice thermal conductivity by enhancing phonon scattering. [11,12] It is noticeable that the effect of electron-phonon coupling in some systems is significant and complicated. In n-type SnSe, the electron-phonon coupling reduces the carrier mobility by 80%, as the lattice a is slightly enlarged. [13] In p-type silicon, the electronphonon coupling would reduce the lattice thermal conductivity by 45%, when carrier concentration goes above 10 19 cm −3 . [14] On the other hand, the coupling between electronic conductivity and Seebeck coefficient is more intrinsic, as they exhibit the opposite dependence on carrier concentration and electronic effective mass. [15,16] Band engineering was proved to be an effective strategy to optimize the power factor, PF = S 2 σ, by reconstructing the geometry of the band structure near Fermi level. [17][18][19][20][21] P-type PbTe is one of the most representative examples of the band engineering. [21][22][23][24][25] By introducing certain dopants, such as Mg, Mn, Sr, Cd, Eu, the energy distance between the light valence band and the heavy valence band of PbTe can be largely reduced. Such "band convergence" increases the Seebeck coefficient while the electrical conductivity is much less affected. [21,[26][27][28][29][30] The success of band engineering causes PbTe to be one of the most outstanding thermoelectric families. Band convergence in PbSe, however, was found to be difficult to achieve, although it shows a similar two-valley valence band structure to PbTe. [31] The energy difference between the light and heavy bands of PbSe is about 0.5 eV, compared with 0.2 eV for PbTe. [30,[32][33][34] The lower thermoelectric performance of PbSe relative to PbTe was attributed to the intrinsic electronic structure of PbSe. [34] To tune the band structure of p-type PbSe, many different dopants have been examined. [9,23,31,[35][36][37] It was found that some dopants, such as Hg and Sr, show a weak band engineering effect. [36][37][38] With Hg doping, the Seebeck coefficient is largely enhanced at high temperatures, while the enhancement at room-temperature is nearly invisible. This phenomenon reflects PbSe has been expected to be a competitor of the excellent thermoelectric material PbTe, whereas its performance has proved to be limited by its intrinsic electronic structure. In this work, the improved thermoelectric performance of PbSe originating in the novel spin-orbit coupling effect is reported. By alloying with NaSbSe 2 , valence band convergence and bandgap enlargement are achieved in PbSe, resulting in a significantly enlarged Seebeck coefficient. Theoretical calculations indicate that a modified electronic structure by spin-orbit coupling would lead to exotic ther...

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Section: Resultsmentioning

confidence: 81%

Section: Resultsmentioning

confidence: 90%

Section: Resultsmentioning

confidence: 94%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Boosting the Thermoelectric Performance of PbSe from the Band Convergence Driven By Spin‐Orbit Coupling

Cai

Yang

Liu

et al. 2022

Advanced Energy Materials

Self Cite

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Giant Band Convergence and High Thermoelectric Performance in n‐Type PbSe Induced by Spin‐Orbit Coupling

Cai,

Wang,

Zhuang

et al. 2024

Adv Funct Materials

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An ideal thermoelectric material requires the multi‐valley and strong dispersion band structure, for relieving the competition between thermopower and electrical conductivity, whereas the two features barely coexist in natural compounds. Here, the significantly improved thermoelectric performance in n‐type PbSe‐xAgSbS2 with the purposefully renormalized conduction band structure is reported. It is shown that the strong spin‐orbit coupling effect splits the single valley at “L” point into three individuals delicately, as the Dirac point is shifted away from the high symmetry point by the decreasing lattice constant. Compared with the common PbSe‐based compounds, the renormalized system exhibits a range of distinctive properties, such as the 2–3 times larger band gap, 5–10 times lower optimal carrier concentration, and weakly temperature‐dependent Seebeck coefficient. Owing to the achieved giant band convergence and the low thermal conductivity, a high peak zT of 1.75 at 850 K and an outstanding average zT of 1.04 are obtained. Furthermore, the mechanical property and thermal stability of PbSe are considerably improved for the introduced high entropy effect and lattice shrinkage. This study reveals the remarkable impact of spin‐orbit coupling on thermoelectric performance, and suggests that the optimized PbSe material holds great promise for practical applications.

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Realizing Ultrahigh Thermoelectric Performance in n‐Type PbSe Through Lattice Planification and Introducing Liquid‐Like Cu Ions

Pang,

Qin,

Qin

et al. 2024

Adv Funct Materials

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The coupling relationship between electrical and thermal transports makes it rather challenging to enhance thermoelectric performance. Here, electrical and thermal transports are successfully decoupled to realize high performance in n‐type PbSe by utilizing a stepwise strategy. First, the PbSe lattice is plained with extra Pb to compensate for the intrinsic Pb vacancies, which can weaken defect scattering and improve carrier mobility to ≈1230 cm2 V−1 s−1. The room‐temperature power factor triples and reaches ≈32 µW cm−1 K−2, and ZT is significantly enhanced to ≈0.6 in Pb1.006Se. Subsequently, liquid‐like interstitial Cu ions are introduced to inhibit heat conduction without damaging electrical transport. While maintaining a high power factor of ≈25 µW cm−1 K−2, Cu ions strongly suppress phonon transport at high temperature, leading to an ultralow lattice thermal conductivity of ≈0.28 W m−1 K−1 in Pb1.006Cu0.006Se, only 30% of the Cu‐free PbSe. Eventually, a remarkable peak ZT of ≈1.8 at 773 K is achieved along with a high average ZT of ≈1.1 from 300 to 823 K in Pb1.006Cu0.006Se. An outstanding experimental conversion efficiency of ≈7.1% is obtained in the single‐leg device, demonstrating great potential for PbSe as low‐ to mid‐temperature thermoelectrics.

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Improved thermoelectric performance in PbSe–AgSbSe2 by manipulating the spin-orbit coupling effects

Cited by 26 publications

References 49 publications

Boosting the Thermoelectric Performance of PbSe from the Band Convergence Driven By Spin‐Orbit Coupling

Boosting the Thermoelectric Performance of PbSe from the Band Convergence Driven By Spin‐Orbit Coupling

Giant Band Convergence and High Thermoelectric Performance in n‐Type PbSe Induced by Spin‐Orbit Coupling

Realizing Ultrahigh Thermoelectric Performance in n‐Type PbSe Through Lattice Planification and Introducing Liquid‐Like Cu Ions

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