Structural control for high performance Bi2Te3–xSex thermoelectric thin films

Chen Yun-Fei; Wei Feng; Wang He; Zhao Wei-Yun; Deng Yuan

doi:10.7498/aps.70.20211090

Abstract

Bi₂Te₃-based alloys have been long regarded as the materials chosen for room temperature thermoelectric (TE) applications. With superior TE performances, Bi₂Te₃-based bulk materials have been commercially used to fabricate TE devices already. However, bulk materials are less suitable for the requirements for applications of flexible or thin film TE devices, and therefore the thin film materials with advanced TE properties are highly demanded. Comparing with bulk materials and P-type Bi₂Te₃-based thin films, the TE properties of N-type Bi₂Te₃-based thin films have been relatively poor so far and need further improving for practical applications. In this study, a series of N-type Bi₂Te_3–_xSe_x thin films is prepared via magnetron sputtering method, and their structures can be precisely controlled by adjusting the sputtering conditions. Preferential layered growth of the Bi₂Te_3–_xSe_x thin films along the (00l) direction is achieved by adjusting the substrate temperature and working pressure. Superior electrical conductivity over 10⁵ S/m is achieved by virtue of high in-plane mobility. combining the advanced Seebeck coefficient of Bi₂Te₃-based material with superior electrical conductivity of highly oriented Bi₂Te_3–_xSe_x thin film, a high power factor (PF) of the optimal Bi₂Te_3–_xSe_x thin film can be enhanced to 42.5 μW/(cm·K²) at room temperature, which is comparable to that of P-type Bi₂Te₃-based thin film and bulk material.

Keywords:

Authors and contacts

1.
Hangzhou Innovation Institute, Beihang University, Hangzhou 310052, China
2.
Research Institute for Frontier Science, Beihang University, Beijing 100083, China

Corresponding author: Zhao Wei-Yun, zhaowyhz@buaa.edu.cn ; Deng Yuan, dengyuan@buaa.edu.cn

Funds: Project supported by the National Key Research and Development Program of China (Grant No. 2018YFA0702100).

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References

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[21]	Duan X, Jiang Y 2011 Thin Solid Films 519 3007 Google Scholar
[22]	Bourgault D, Garampon C Giroud, Caillault N, Carbone L, Aymami J A 2008 Thin Solid Films 516 8579 Google Scholar
[23]	Bottnrt H, Chen G, Venkatasubramanian R 2006 MRS Bulletin 31 211 Google Scholar
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图 1 各Bi₂Te_3–xSe_x薄膜试样表面及断面形貌　(a) BTS1; (b) BTS2; (c) BTS3; (d) BTS4; (e) BTS5; (f) BTS6

Figure 1. Surface and cross-section morphology of Bi₂Te_3–xSe_x thin films: (a) BTS1; (b) BTS2; (c) BTS3; (d) BTS4; (e) BTS5; (f) BTS6.

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图 2 各Bi₂Te_3–xSe_x薄膜试样XRD图谱

Figure 2. XRD patterns of Bi₂Te_3–xSe_x thin films.

DownLoad: Full-Size Img PowerPoint

图 3 Bi₂Te_3–xSe_x薄膜层状生长过程示意图　(a) 表面形貌; (b) 断面形貌

Figure 3. Schematic diagram showing the growing process of Bi₂Te_3–xSe_x thin film with 2-D layered structure in (a) top view and (b) cross sectional view.

DownLoad: Full-Size Img PowerPoint

图 4 各薄膜试样热电参数　(a) Seebeck系数; (b)电导率; (c)功率因子

Figure 4. Thermoelectric properties of all the samples: (a) Seebeck coefficient; (b) electrical conductivity; (c) power factor.

DownLoad: Full-Size Img PowerPoint

表 1 不同试样的制备参数

Table 1. Sputtering parameters of all the samples.

试样 Bi₂Te_3–xSe_x
直流靶功
率/W Te射频靶
功率/W 气压/Pa 温度/℃ 时间/h

BTS1 12 25 3 350 2
BTS2 12 25 1 450 2
BTS3 12 25 2 450 2
BTS4 12 25 3 450 2
BTS5 12 25 3 450 1
BTS6 12 25 3 450 3

DownLoad: CSV

表 2 霍尔效应测试

Table 2. Hall measurements of all the samples.

试样载流子浓度/(10¹⁹ cm^–3) 载流子迁移率/(cm²·V^–1·s^–1) 电导率
/(10⁴ S·m^–1)

BTS1 11.7 17.1 3.2
BTS2 12.7 30.6 6.2
BTS3 10.0 59.8 9.6
BTS4 8.3 84.2 11.2
BTS5 7.2 45.2 5.2
BTS6 9.1 63.9 9.3

DownLoad: CSV

表 3 元素原子比

Table 3. Atomic ratio by EDS measurements.

试样 Bi/% Te/% Se/%

BTS1 36.5 60.2 3.3
BTS2 41.7 53.6 4.7
BTS3 41.6 53.9 4.5
BTS4 41.3 54.3 4.4
BTS5 41.4 54.8 3.8
BTS6 41.8 53.5 4.7

DownLoad: CSV

map

[1]	Li P, Cai L, Zhai P, Tang X, Zhang Q, Niino M 2010 J. Electron. Mater. 39 1522 Google Scholar
[2]	Suter C, Jovanovic Z R, Steinfeld A 2012 Appl. Energ. 99 379 Google Scholar
[3]	Yu Y, Zhu W, Wang Y, Zhu P, Peng K, Deng Y 2020Appl. Energ. 275 115404
[4]	ChenY, Tan X, Peng S, Xin C, Delahoy A E, Chin K K, Zhang C 2018 J. Electron. Mater. 47 1201 Google Scholar
[5]	Zhou X, Zou J, Chen Z 2020 Chem. Rev. 120 7399 Google Scholar
[6]	Qin H, Liu Y, Zhang Z, Wang Y, Cao J, Cai W, Zhang Q, Sui J 2018 Mater. Today. Phys. 6 31 Google Scholar
[7]	Wei H, Tang J, Xi D 2020 J. Alloy. Compd. 817 153284 Google Scholar
[8]	Liu W, Zhang Q, Lan Y, Chen S, Yan X, Zhang Q, Wang H, Wang D, Chen G, Ren Z 2011 Adv. Energy. Mater. 1 577 Google Scholar
[9]	Wei H, Tang J, Wang H, Xu D 2020 J. Mater. Chem. A 8 24524 Google Scholar
[10]	Zhu W, Deng Y, Cao L 2017 Nano Energy 34 463 Google Scholar
[11]	Vineis C J, Shakouri A, Majumdar A, Kanatzidis M G 2010 Adv. Mater. 22 3970 Google Scholar
[12]	Zhang Z, Wang Y, Deng Y, Xu Y 2011 Solid. State. Commun. 151 1520 Google Scholar
[13]	Takashiri M, Tanaka S, Miyazaki K 2010 Thin Solid Films 519 619 Google Scholar
[14]	Parashchuk T, Kostyuk O, Nykyruy L, Dashevsky Z 2020 Mater. Chem. Phys. 253 123427 Google Scholar
[15]	Bassi A Li, Bailini A, Casari C S, Donati F, Mantegazza A, Passoni M, Russo V, Bottani C E 2009 J. Appl. Phys. 105 123407
[16]	Peranio N, Winkler M, Aabdin Z, Konig J, Bottner H, Eibl O 2012 Phys. Status Solidi A 209 289 Google Scholar
[17]	Zhu W, Deng Y, Wang Y, Luo B, Cao L 2014 Thin Solid Films 556 270 Google Scholar
[18]	Mu X, Zhou H, He D, Zhao W, Wei P, Zhu W, Nie X, Liu H, Zhang Q 2017 Nano Energy 33 55 Google Scholar
[19]	Deng Y, Zhang Z, Wang Y, Xu Y 2012 J. Nanopart Res. 14 775 Google Scholar
[20]	Duan X, Jiang Y 2010 Appl. Surf. Sci. 256 7365 Google Scholar
[21]	Duan X, Jiang Y 2011 Thin Solid Films 519 3007 Google Scholar
[22]	Bourgault D, Garampon C Giroud, Caillault N, Carbone L, Aymami J A 2008 Thin Solid Films 516 8579 Google Scholar
[23]	Bottnrt H, Chen G, Venkatasubramanian R 2006 MRS Bulletin 31 211 Google Scholar
[24]	Lewis B, Campell D S 1967J. Vac. Sci. Technol. 4 209
[25]	Zhang Z, Lagally M 1997 Science 276 377 Google Scholar

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Structural control for high performance Bi₂Te_3–xSe_x thermoelectric thin films