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具有优异电输运性能的热电薄膜是发展高效面内散热技术的关键材料, 但是过低的电输运性能是制约其应用的重要难题. 热电磁耦合新效应是近年来发展的一种优化综合热电性能的新方法. 为了探索热电磁耦合新效应对热电薄膜电输运性能的影响机制, 本研究发展了一种球磨分散-丝网印刷-热压固化一体化成型的方法, 成功制备了一系列Fe纳米粒子作为第二相的xFe/BST/环氧树脂热电磁薄膜, 并重点研究了其热电磁耦合作用及其对电热输运性能的影响规律. 研究发现, xFe/Bi0.5Sb1.5Te3 (BST)/环氧树脂热电磁薄膜中存在正、负磁阻共存的现象; BST(000l)择优取向因子与正磁阻(MR+)之间呈正比例关系并增加热电磁薄膜的电导率; 源于强铁磁性Fe纳米粒子局部磁矩的自旋相关散射的负磁阻(MR–)会增加Seebeck系数. 因此, 室温附近Fe/BST/环氧树脂热电磁薄膜的功率因子高达2.87 mW/(K2·m), 与BST/环氧树脂热电薄膜相比, 提高了78%. 这些结果表明, 热电磁薄膜中正、负磁阻的共存不仅可解耦热电材料中电导率与Seebeck系数之间的耦合关系, 还可以为磁纳米粒子诱导优异热电转换性能提供新的物理机制.
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关键词:
- p型Bi2Te3基热电磁薄膜 /
- 磁各向异性 /
- 磁阻 /
- 自旋相关散射
Thermoelectric (TE) films with excellent electrical transport property are key materials for developing efficient in-plane heat dissipation technology, but their low electrical transport property is a challenge that restricts their application. Recently, a new thermo-electro-magnetic coupling effect has been proposed to significantly improve the comprehensive TE performance. In order to explore the influence of the above effects on the electric transport property of TE films, we develop an integrated preparation method through ball milling dispersion, screen-printing and hot-pressing curing, obtaining a series of xFe/Bi0.5Sb1.5Te3 (BST)/epoxy TE films in which Fe nanoparticles serve as the second phase, resulting in the thermo-electro-magnetic coupling effect , and also we study their influence on the electrothermal transport performance. The results are shown below. The positive and negative magnetoresistance are co-existent in xFe/BST/epoxy thermoelectromagnetic films; the preferred orientation factor of BST (000l) is positively proportional to the positive magnetoresistance (MR+), resulting in an increase of the conductivity; the spin-dependent scattering of negative magnetoresistance (MR–) derived from the local magnetic moment of strong ferromagnetic Fe nanoparticles increases the Seebeck coefficient. Hence, the power factor of Fe/BST/epoxy thermoelectromagnetic film near room temperature reaches 2.87 mW⋅K–2⋅m–1, which is 78% higher than that of BST/epoxy thermoelectric film. These results indicate that the coexistence of positive and negative magnetoresistance in thermoelectromagnetic films can not only relieve the coupling relationship between conductivity and Seebeck coefficient in TE materials, but also provide a new physical mechanism for the excellent TE conversion performance induced by magnetic nanoparticles.-
Keywords:
- p-type Bi2Te3 based thermoelectromagnetic films /
- magnetic anisotropy /
- magnetoresistance /
- spin dependent scattering
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图 1 xFe/BST/环氧树脂热电磁薄膜物相组成 (a) xFe/BST/环氧树脂热电磁薄膜的XRD谱; (b) 2θ为27.8°—28.6°的放大XRD谱
Fig. 1. Phase constituents of xFe/BST/epoxy thermoelectromagnetic films: (a) XRD patterns of xFe/BST/epoxy thermoelectromagnetic films; (b) the enlarged XRD patterns in the 2θ range of 27.8°–28.6°.
图 2 xFe/BST/环氧树脂热电磁薄膜的HRTEM微观结构 (a) Fe02的HAADF-STEM像; (b)—(f) Bi, Te, Sb, Fe和O的面分布
Fig. 2. Microstructures of xFe/BST/epoxy thermoelectromagnetic films from HRTEM: (a) HAADF-STEM image of Fe02; (b)–(f) corresponding elemental mappings of Bi, Te, Sb, Fe, and O.
图 3 xFe/BST/环氧树脂热电磁薄膜电输运性能 (a)电导率和Seebeck系数; (b) 功率因子
Fig. 3. Electrical transport properties of the xFe/BST/epoxy thermoelectromagnetic films: (a) Electrical conductivity and Seebeck coefficient; (b) power factor.
图 4 xFe/BST/环氧树脂热电磁薄膜的磁各向异性 (a) 测量装置; (b) Fe00, (c) Fe01, (d) Fe02, (e) Fe03和(f) Fe04在300 K时⊥H和∥H的M-H曲线. 图(b)—(f)中右下插图是零场(H = 0)附近的M-H曲线, 所有xFe/BST/环氧树脂热电磁薄膜的M-H曲线已经进行了扣除BST/环氧树脂热电薄膜背底的数据处理
Fig. 4. Magnetic anisotropy of xFe/BST/epoxy thermoelectromagnetic films: (a) Measuring setup; M-H curves of (b) Fe00, (c) Fe01, (d) Fe02, (e) Fe03, and (f) Fe04⊥H (and ∥H) at 300 K. The lower-right insets in panels (b)–(f) show the M-H curves near zero field (H = 0), the M-H curves of xFe/BST/epoxy thermoelectromagnetic films were processed by BST/epoxy films background subtraction.
图 5 xFe/BST/环氧树脂热电磁薄膜磁阻特征 (a), (b) 1.0—2.5 T范围内, 50 K时Fe00和Fe02的MR随磁场H与面外方向夹角θ的变化曲线; (c), (d) 0—2.5 T范围内, 50—300 K时Fe00和Fe02的测量MR(MRm)随磁场的变化曲线; (e) 50 K时Fe00和xFe/BST/环氧薄膜热电磁薄膜(Fe0x, x = 1, 2, 3, 4)的MRm随磁场的变化曲线. MR-($ {\text{MR}}_{{\text{Fe0}}x}^{\text{m}} - {\text{MR}}_{{\text{Fe0}}x}^{+}$)和两种MR–的拟合曲线分别显示在图(e)的下半部分, 并用虚线和颜色标注
Fig. 5. Magnetoresistance characteristic of xFe/BST/epoxy thermoelectromagnetic films: (a), (b) The MR dependence of the included angle θ between the magnetic field H and the out-plane direction of (a) Fe00 and (b) Fe02 in the range of 1.0–2.5 T at 50 K; (c), (d) the magnetic field dependences of measured MR (MRm) of (c) Fe00 and (d) Fe02 at 50–300 K in the range of 0–2.5 T; (e) the magnetic field dependences of MRm of Fe00 and xFe/BST/epoxy flexible films (Fe0x, x = 1, 2, 3, 4) at 50 K. The MR- ($ {\text{MR}}_{{\text{Fe0}}x}^{\text{m}} - {\text{MR}}_{{\text{Fe0}}x}^{+} $) and fitting curves of two kinds of MR– are shown in the lower half of panel (e) with the color remarks and the dotted lines, respectively.
图 6 无MR–的BST/环氧树脂热电薄膜的物相组成分析 (a) #0Fe00, #1Fe00, #2Fe00, #3Fe00和#4Fe00的XRD图案, 对应的压力为0, 4, 8, 12和16 MPa; (b) 在27.6°—28.5°范围内XRD谱放大图; (c) 取向因子F随烧结压力的变化曲线
Fig. 6. Phase constituents and preferential orientation of BST/epoxy thermoelectricity films ignoring MR–: (a) XRD patterns of #0Fe00, #1Fe00, #2Fe00, #3Fe00, and #4Fe00 corresponding the pressure being 0, 4, 8, 12, and 16 MPa; (b) the enlarged XRD patterns in the 2θ range of 27.6°–28.5°; (c) the pressure dependence of the F of (000l) preferential orientation of BST.
图 7 BST/环氧树脂热电薄膜的$ {\text{MR}}_{{\text{\# }}x}^{+} $随(000l)择优取向度的变化曲线 (a) 50 K时, 不同F的BST/环氧树脂热电薄膜的测量$ {\text{MR}}_{{\text{\# }}x}^ + $随磁场的变化曲线; (b) 50 K时, 不同F的BST/环氧树脂热电薄膜的Δ$ {\text{MR}}_{{\text{\# }}x}^ + $随ΔF#x的变化曲线, 在H = 0.5—2.5 T下, 拟合方程为$ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} = {K_0}{{\Delta }}F_\# ^y{H^2} $, 其中(K0, y)分别是0.5 T为(30.67, 2.075), 1.0 T为(24.92, 2.049), 1.5 T为(19.79, 2.006), 2.0 T为(16.54, 1.983)和2.5 T为(13.79, 1.937); (c)拟合方程为$ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} = {K_0}{{\Delta }}F_\# ^2{H^2} $, 其中K0是常数
Fig. 7. The $ {\text{MR}}_{{\text{\# }}x}^{+} $ dependences of the (000l) preferential orientation F#x of BST in BST/epoxy thermoelectricity films: (a) The variation of $ {\text{MR}}_{{\text{\# }}x}^ + $ with the magnetic field at 50 K in the range of 0–2.5 T; (b) the fitting correlation between ΔF# and $ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} $ at H = 0.25–2.5 T, which is expressed as $ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} = {K_0}{{\Delta }}F_\# ^y{H^2} $, where (K0, y) is (34.29, 2.129) for 0.5 T, (24.46, 2.021) for 1.0 T, (14.27, 1.902) for 1.5 T, (19.480, 2.063) for 2.0 T, and (16.12, 2.013) for 2.50 T; (c) $ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} = {K_0}{{\Delta }}F_\# ^2{H^2} $, where K0 is constant.
表 1 xFe/BST/环氧树脂热电磁薄膜的F, ΔF, MRm, MR–和MR+值
Table 1. Values of F, ΔF, MRm, MR–, and MR+ of xFe/BST/epoxy thermoelectromagnetic films.
No. F ΔF 0.5 T 1.0 T 1.5 T 2.0 T 2.5 T MRm MR+ MR– MRm MR+ MR– MRm MR+ MR– MRm MR+ MR– MRm MR+ MR– Fe00 0.26 0.00 0.85 0.85 0.00 2.36 2.36 0.00 4.87 4.87 0.00 7.70 7.70 0.00 11.51 11.51 0.00 Fe01 0.31 0.05 0.30 0.86 –0.57 1.07 2.42 –1.34 2.29 4.98 –2.69 3.86 7.87 –4.01 5.70 11.75 –6.05 Fe02 0.41 0.15 0.44 1.00 –0.56 1.41 2.87 –1.50 2.84 5.86 –3.02 4.66 9.24 –4.57 6.78 13.67 –6.90 Fe03 0.38 0.12 0.73 0.94 –0.21 1.96 2.69 –0.73 3.61 5.50 –1.90 5.63 8.68 –3.06 7.93 12.89 –4.96 Fe04 0.36 0.10 0.80 0.92 –0.11 2.08 2.59 –0.51 4.30 5.31 –1.01 7.19 8.38 –1.19 10.47 12.47 –2.00 
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表 2 不同样品300 K时⊥H方向的实测磁性能参数
Table 2. Magnetic properties of the ⊥H of the different samples at 300 K.
Samples x Ms/(emu·g–1) Hk/Oe Keff/(105 erg·g–1) ΔE/(104 erg·g–1) Hc/Oe Mr/(emu·g–1) Fe01 0.1% 107.76 9703.48 5.23 5.94 123.65 5.42 Fe02 0.2% 122.17 14456.38 8.83 8.98 93.37 4.84 Fe03 0.3% 95.80 10700.42 5.13 7.31 78.80 1.09 Fe04 0.4% 95.12 10144.43 4.82 6.23 117.48 4.14
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表 3 BST/环氧树脂热电薄膜的F#, ΔF#, $ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} $和K0的值
Table 3. Values of F#, ΔF#, $ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} $, and K0 of BST/epoxy thermoelectricity films.
Sample F# ΔF# 0.5 T 1.0 T 1.5 T 2.0 T 2.5 T $ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} $ K0 $ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} $ K0 $ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} $ K0 $ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} $ K0 $ {{\Delta {\mathrm{MR}}}}_{\text{\# }}^{+} $ K0 #0Fe00 0.26 0.00 0.00 26.99 0.00 22.91 0.00 19.59 0.00 17.04 0.00 15.35 #1Fe00 0.34 0.08 0.04 26.99 0.11 22.91 0.31 19.59 0.44 17.04 0.63 15.35 #2Fe00 0.37 0.11 0.07 26.99 0.28 22.91 0.49 19.59 0.88 17.04 1.21 15.35 #3Fe00 0.42 0.16 0.18 26.99 0.60 22.91 1.15 19.59 1.69 17.04 2.48 15.35 #4Fe00 0.46 0.20 0.28 26.99 0.95 22.91 1.83 19.59 2.85 17.04 3.96 15.35
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表 4 xFe/BST/环氧树脂热电磁薄膜在不同H中的K1, K2, K3, $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{S}}{\mathrm{D}}}^{-} $和$ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{W}}{\mathrm{L}}}^{-} $值
Table 4. Values of K1, K2, K3, $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{S}}{\mathrm{D}}}^{-} $, and $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{W}}{\mathrm{L}}}^{-} $ of xFe/BST/epoxy thermoelectromagnetic films in different H
No. K1 K2 K3 0.5 T 1.0 T 1.5 T 2.0 T 2.5 T $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{S}}{\mathrm{D}}}^{-} $ $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{W}}{\mathrm{L}}}^{-} $ $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{S}}{\mathrm{D}}}^{-} $ $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{W}}{\mathrm{L}}}^{-} $ $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{S}}{\mathrm{D}}}^{-} $ $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{W}}{\mathrm{L}}}^{-} $ $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{S}}{\mathrm{D}}}^{-} $ $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{W}}{\mathrm{L}}}^{-} $ $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{S}}{\mathrm{D}}}^{-} $ $ {{\mathrm{M}}{\mathrm{R}}}_{{\mathrm{W}}{\mathrm{L}}}^{-} $ Fe00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 Fe01 56.30 0.12 0.52 –0.20 –0.37 –0.82 –0.52 –2.06 –0.64 –3.27 –0.74 –5.23 –0.82 Fe02 36.77 0.17 0.45 –0.24 –0.32 –1.02 –0.47 –2.47 –0.55 –3.94 –0.64 –6.18 –0.71 Fe03 19.10 0.20 0.23 –0.05 –0.16 –0.50 –0.23 –1.61 –0.28 –2.73 –0.33 –4.60 –0.36 Fe04 6.38 0.22 0.17 –0.00 –0.12 –0.34 –0.17 –0.81 –0.21 –0.95 –0.24 –1.73 –0.27
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[1] Wang L M, Zhang Z M, Liu Y C, Wang B R, Fang L, Qiu J J, Zhang K, Wang S R 2018 Nat. Commun. 9 3817
Google Scholar
[2] Yang Q Y, Yang S Q, Qiu P F, Peng L M, Wei T R, Zhang Z, Shi X, Chen L D 2022 Science 377 854
Google Scholar
[3] He S Y, Li Y B, Liu L, Jiang Y, Feng J J, Zhu W, Zhang J Y, Dong Z R, Deng Y, Luo J, Zhang W Q, Chen G 2020 Sci. Adv. 6 eaaz8423
Google Scholar
[4] Hinterleitner B, Knapp I, Poneder M, Shi Y, Müller H, Eguchi G, Eisenmenger-Sittner C, Stöger-Pollach M, Kakefuda Y, Kawamoto N, Guo Q, Baba T, Mori T, Ullah S, Chen X Q, Bauer E 2019 Nature 576 85
Google Scholar
[5] Qin B C, Wang D Y, Liu X X, Qin Y X, Dong J F, Luo J F, Li J W, Liu W, Tan G J, Tang X F, Li J F, He J Q, Zhao L D 2021 Science 373 556
Google Scholar
[6] Jiang B B, Wang W, Liu S X, Wang Y, Wang C F, Chen Y N, Xie L, Huang M Y, He J Q 2022 Science 377 208
Google Scholar
[7] Chang C, Wu M H, He D Q, Pei Y L, Wu C F, Wu X F, Yu H L, Zhu F Y, Wang K D, Chen Y, Huang L, Li J F, He J Q, Zhao L D 2018 Science 360 778
Google Scholar
[8] Zhao W Y, Liu Z Y, Sun Z G, Zhang Q J, Wei P, Mu X, Zhou H Y, Li C C, Ma S F, He D Q, Ji P X, Zhu W T, Nie X L, Su X L, Tang X F, Shen B G, Dong X L, Yang J H, Liu Y, Shi J 2017 Nature 549 247
Google Scholar
[9] Zhao W Y, Liu Z Y, Wei P, Zhang Q J, Zhu W T, Su X L, Tang X F, Yang J H, Liu Y, Shi J, Chao Y M, Lin S Q, Pei Y Z 2017 Nat. Nanotechnol. 12 55
Google Scholar
[10] Ma S F, Li C C, Wei P, Zhu W T, Nie X L, Sang X H, Zhang Q J, Zhao W Y 2020 J. Mater. Chem. A 8 4816
Google Scholar
[11] Ma S F, Li C C, Cui W J, Sang X H, Wei P, Zhu W T, Nie X L, Sun F H, Zhao W Y, Zhang Q J 2021 Sci. China Mater. 64 2835
Google Scholar
[12] Li C C, Ma S F, Wei P, Zhu W T, Nie X L, Sang X H, Sun Z, Zhang Q J, Zhao W Y 2020 Energy Environ. Sci. 13 535
Google Scholar
[13] Li C C, Ma S F, Cui W J, Sang X H, Wei P, Zhu W T, Nie X L, Zhao W Y, Zhang Q J 2021 Mater. Today Phys. 19 100409
Google Scholar
[14] Xing L, Cui W, Sang X H, Hu F, Wei P, Zhu W T, Nie X L, Zhang Q J, Zhao W Y 2021 J. Materiomics. 7 998
Google Scholar
[15] Li C C, Zhao W Y, Zhang Q J 2022 Sci. Bull. 67 891
Google Scholar
[16] Zhao Y, Nie X L, Sun C L, Chen Y F, Ke S Q, Li C, Zhu W T, Sang X H, Zhao W Y, Zhang Q J 2021 ACS Appl. Mater. Interfaces 13 58746
Google Scholar
[17] Chen Y F, Nie X L, Sun C L, Ke S Q, Xu W J, Zhao Y, Zhu W T, Zhao W Y, Zhang Q J 2022 Adv. Funct. Mater. 32 2111373
Google Scholar
[18] Boona S R, Vandaele K, Boona I N, McComb D W, Heremans J P 2016 Nat. Commun. 7 13714
Google Scholar
[19] Uchida K I 2022 Nat. Mater. 21 136
Google Scholar
[20] Sakai A, Minami S, Koretsune T, Chen T T, Higo T, Wang Y, Nomoto T, Hirayama M, Miwa S, Nishio-Hamane D, Ishii F, Arita R, Nakatsuji S 2020 Nature 581 53
Google Scholar
[21] Pan Y, Le C, He B, Watzman S J, Yao M, Gooth J, Heremans J P, Sun Y, Felser C 2022 Nat. Mater. 21 203
Google Scholar
[22] Chen T T, Minami S, Sakai A, Wang Y, Feng Z, Nomoto T, Hirayama M, Ishii R, Koretsune T, Arita R, Nakatsuji S 2022 Sci. Adv. 8 eabk1480
Google Scholar
[23] Lotgering F K 1959 J. Inorg. Nucl. Chem. 9 113
Google Scholar
[24] Zhao L, Deng H, Korzhovska I, Chen Z, Konczykowski M, Hruban A, Oganesyan V, Krusinelbaum L 2014 Nat. Mater. 13 580
Google Scholar
[25] Pippard A B 1989 Magnetoresistance in Metals (New York: Cambridge University Press) pp23–24
[26] Mu X, Zhou H Y, He D Q, Zhao W Y, Wei P, Zhu W T, Nie X L, Liu H J, Zhang Q J 2017 Nano Energy 33 55
Google Scholar
[27] Khosla R P, Fischer J R 1970 Phys. Rev. B 2 4084
Google Scholar
[28] Kawabata A 1980 Solid State Commun. 34 431
Google Scholar
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