Preparation and thermoelectric properties of layered Bi1–xSbxSe nanocrystalline films

Xu Jing; He Zi-Min; Yang Wen-Long; Wu Rong; Lai Xiao-Fang; Jian Ji-Kang

doi:10.7498/aps.71.20220834

Abstract

BiSe is found to be a promising near-room-temperature thermoelectric material with higher performance than traditional Bi₂Se₃ due to its ultra-low intrinsic lattice thermal conductivity. In this work, N-type BiSe nanocrystalline thin films with (00l) preferred orientation are first prepared via vacuum thermal evaporation method, and Bi_1–xSb_xSe nanocrystalline films with different doping concentrations are obtained by Sb co-evaporation. The phases, morphologies, chemical compositions and valences, lattical vibrations, and electrical properties of these films are characterized. It is found that the Sb dopant successfully enters into the crystal lattice and replaces the Bi site of Bi₂Se₃ quintuple layers and Bi₂ bilayers without selectivity, and the difference of gold properties between Sb atom and Bi atoms leads the carrier concentration to sharply decrease and the Seebeck coefficient in doped BiSe to increase. Meanwhile,the sizes of nanocrystals in the films decrease and the denser layered structure is formed due to the Sb doping, which is conducive to the carrier transport in the samples, and the in-plane carrier mobility of the films effectively increases from 13.6 cm²·V^–1·s^–1 (BiSe) to 19.3 cm²·V^–1·s^–1 (Bi_0.65Sb_0.35Se). The maximum room-temperature power factor of 2.18 μW·cm^–1·K^–2 is obtained in Bi_0.76Sb_0.24Se, which is higher than that in undoped BiSe. The results of this work indicate that the BiSe-based thin films have potential applications in room temperature thermoelectric thin film devices.

Keywords:

Authors and contacts

1.
School of Physics and Optoelectronic Engineering, Guangdong University of Technology, Guangzhou 510006, China
2.
School of Physical Science and Technology, Xinjiang University, Xinjiang 830046, China

Corresponding author: Jian Ji-Kang, jianjikang@126.com

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 52072078, 51702058).

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References

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图 1 Bi_1–xSb_xSe纳米晶薄膜(x = 0, 0.15, 0.24, 0.35)的物相表征　(a) XRD图谱; (b)图(a)中(005)峰的放大图谱; (c) 晶格常数随Sb掺杂浓度的变化

Figure 1. (a) XRD patterns of Bi_1–xSb_xSe films (x = 0, 0.15, 0.24, 0.35); (b) enlarged pattern of (005) peak in (a); (c) the lattice constant varies with the concentrations of Sb .

DownLoad: Full-Size Img PowerPoint

图 2 Bi_1–xSb_xSe纳米薄膜(x = 0, 0.15, 0.24, 0.35)表面和截面的SEM图像　(a) BiSe; (b) Bi_0.85Sb_0.15Se; (c) Bi_0.76Sb_0.24Se; (d) Bi_0.65Sb_0.35Se

Figure 2. SEM images of surface and cross section of Bi_1–xSb_xSe films (a) BiSe; (b) Bi_0.85Sb_0.15Se; (c) Bi_0.76Sb_0.24Se; (d) Bi_0.65Sb_0.35Se.

DownLoad: Full-Size Img PowerPoint

图 3 Bi_0.65Sb_0.35Se薄膜的mapping图像　(a) 表面; (b) 截面

Figure 3. Mapping images of (a) surface and (b) cross section of Bi_0.65Sb_0.35Se thin film.

DownLoad: Full-Size Img PowerPoint

图 4 Bi_1–xSb_xSe薄膜(x = 0, 0.15, 0.24, 0.35)在激发波长为532 nm下的散射拉曼图谱

Figure 4. Raman scattering spectra of Bi_1–xSb_xSe films (x = 0, 0.15, 0.24, 0.35) with an excitation laser wavelength of 532 nm.

DownLoad: Full-Size Img PowerPoint

图 5 Bi_0.65Sb_0.35Se薄膜样品的XPS谱　(a) 总谱; (b) Bi 4f; (c) Sb 3d; (d) Se 3d

Figure 5. XPS spectrum of Bi_0.65Sb_0.35Se films: (a) Total spectrum; (b) Bi 4f; (c) Sb 3d; (d) Se 3d.

DownLoad: Full-Size Img PowerPoint

图 6 Bi_1–xSb_xSe纳米晶薄膜(x = 0, 0.15, 0.24, 0.35)在不同温度下的　(a) 载流子浓度; (b) 迁移率; (c) 面内电导率; (d) 塞贝克系数; (e) 功率因子

Figure 6. Temperature dependence of (a) carrier concentrations, (b) electron mobilities, (c) the in-plane conductivities, (d) Seebeck coefficients and (e) power factors for Bi_1–xSb_xSe (x = 0, 0.15, 0.24, 0.35) samples.

DownLoad: Full-Size Img PowerPoint

表 1 Bi_1–xSb_xSe纳米薄膜的实验条件

Table 1. Experimental conditions of Bi_1–xSb_xSe thin films.

样品	(Bi+Bi₂Se₃)蒸发源温度/℃	Sb蒸发源温度/℃	源与衬底的距离/cm	衬底温度/ ℃	蒸镀时间/ min
BiSe	500	—	10	475	10
Bi_0.85Sb_0.15Se	500	300	10	475	10
Bi_0.76Sb_0.24Se	500	350	10	475	10
Bi_0.65Sb_0.35Se	500	375	10	475	10

DownLoad: CSV

表 2 Bi_1–xSb_xSe薄膜的元素原子比

Table 2. Atomic ratio of Bi_1–xSb_xSe thin films.

样品	Bi/%	Sb/%	Se/%
BiSe	49.97	—	50.03
Bi_0.85Sb_0.15Se	42.37	7.53	50.10
Bi_0.76Sb_0.24Se	38.01	11.91	50.08
Bi_0.65Sb_0.35Se	32.49	17.45	50.05

DownLoad: CSV

表 3 Bi_1–xSb_xSe (x = 0, 0.15, 0.24, 0.35)薄膜的拉曼振动峰(cm^–1)

Table 3. Raman vibration peaks (cm^–1) of Bi_1–xSb_xSe (x = 0, 0.15, 0.24, 0.35) films.

	BiSe	Bi_0.85Sb_0.15Se	Bi_0.76Sb_0.24Se	Bi_0.65Sb_0.35Se
$ \rm A^1_{1g} $	68.1	70.5	70.9	71.4
E_g	93.7	95.4	95.9	96.7
$ \rm E^2_g $	120.6	121.4	122.1	122.9
$\rm A^2_{1g}$	155.4	157.9	160.5	161.5

DownLoad: CSV

表 4 Bi_1–xSb_xSe(x = 0, 0.15, 0.24, 0.35)薄膜在室温下的霍尔效应测试结果

Table 4. The electrical transport properties of Bi_1–xSb_xSe (x = 0, 0.15, 0.24, 0.35) thin films at room temperature.

薄膜样品	载流子浓度 n/(10²⁰ cm^–3)	载流子迁移率 μ/(cm²·V^–1·s^–1)	电导率 σ/(S·cm^–1)
BiSe	2.5	13.6	544.2
Bi_0.85Sb_0.15Se	1.9	16.7	502.3
Bi_0.76Sb_0.24Se	1.6	18.4	468.8
Bi_0.65Sb_0.35Se	1.3	19.3	416.8

DownLoad: CSV

[1]	Zhou M, Al-Furjan M S H, Zou J, Liu W 2018 Renew. Sust. Energ. Rev. 82 3582 Google Scholar
[2]	Kraemer D, Jie Q, McEnaney K, Cao F, Liu W, Weinstein L A, Loomis J, Ren Z, Chen G 2016 Nat. Energy 1 16153 Google Scholar
[3]	Hasan M N, Wahid H, Nayan N, Mohamed Ali M S 2020 Int. J. Energy Res. 44 6170 Google Scholar
[4]	Chen A, Madan D, Wright P K, Evans J W 2011 J. Micromech. Microeng. 21 104006 Google Scholar
[5]	Orr B, Akbarzadeh A, Mochizuki M, Singh R 2016 Appl. Therm. Eng. 101 490 Google Scholar
[6]	Lee K H, Kim S W 2017 J. Korean Ceram. Soc. 54 75 Google Scholar
[7]	Samanta M, Pal K, Pal P, Waghmare U V, Biswas K 2018 J. Am. Chem. Soc. 140 5866 Google Scholar
[8]	Lind H, Lidin S, Häussermann U 2005 Phys. Rev. B. 72 184101 Google Scholar
[9]	Ju Z, Hou Y, Bernard A, Taufour V, Yu D, Kauzlarich S M 2019 CS Appl. Electron. 1 1917
[10]	Samanta M, Biswas K 2020 Chem. Mater. 32 8819 Google Scholar
[11]	Zhang J, Huang G 2014 Solid State Commun. 197 34 Google Scholar
[12]	Valla T, Ji H, Schoop L, Weber A, Pan Z-H, Sadowski J, Vescovo E, Fedorov A, Caruso A, Gibson Q 2012 Phys. Rev. B. 86 241101 Google Scholar
[13]	Ouyang Y, Zhang Z W, Li D F, Chen J, Zhang G 2019 Ann. Phys. (Berlin) 531 1800437 Google Scholar
[14]	Qiu B, Ruan X L 2009 Phys. Rev. B 80 165203 Google Scholar
[15]	He J, Hu X X, Li D F, Chen J 2022 Nano Res. 15 3804 Google Scholar
[16]	Shen X C, Zhang X, Zhang B, Wang G Y, He J, Zhou X Y 2020 Rare Metals 39 1374 Google Scholar
[17]	He Z M, Lan K L, Chen S Y, Dong Y Z, Lai X F, Liu F S, Jian J K 2022 J. Alloys Compd. 901 163652 Google Scholar
[18]	Shi X L, Zou J, Chen Z G 2020 Chem. Rev. 120 7399 Google Scholar
[19]	魏江涛, 杨亮亮, 秦源浩, 宋培帅, 张明亮, 杨富华, 王晓东 2021 物理学报 70 047301 Google Scholar Wei J T, Yang L L, Qin Y H, Song P S, Zhang M L, Yang F H, Wang X D 2021 Acta Phys. Sin. 70 047301 Google Scholar
[20]	Venkatasubramanian R, Siivola E, Colpitts T, O'Quinn B 2001 Nature 413 597 Google Scholar
[21]	Li J F, Liu W S, Zhao L D, Zhou M 2010 NPG Asia Mater. 2 152 Google Scholar
[22]	Wu H, Carrete J, Zhang Z, Qu Y, Shen X, Wang Z, Zhao L-D, He J 2014 NPG Asia Mater. 6 e108 Google Scholar
[23]	Dun C, Hewitt C A, Huang H, Xu J, Zhou C, Huang W, Cui Y, Zhou W, Jiang Q, Carroll D L 2015 Nano Energy 18 306 Google Scholar
[24]	陈赟斐, 魏锋, 王赫, 赵未昀, 邓元 2021 物理学报 70 207303 Google Scholar Chen Y F, Wei F, Wang H, Zhao W Y, Deng Y 2021 Acta Phys. Sin. 70 207303 Google Scholar
[25]	Adam A M, El-Khouly A, Diab A K 2021 J. Alloys Compd. 851 156887 Google Scholar
[26]	Lu M P, Liao C N, Huang J Y, Hsu H C 2015 Inorg. Chem. 54 7438 Google Scholar
[27]	Kim K, Kim G, Kim S I, Lee K H, Lee W 2019 J. Alloys Compd. 772 593 Google Scholar
[28]	Chen C L, Wang H, Chen Y Y, Day T, Snyder G J 2014 J. Mater. Chem. A. 2 11171 Google Scholar
[29]	Han M K, Hoang K, Kong H, Pcionek R, Uher C, Paraskevopoulos K M, Mahanti S D, Kanatzidis M G 2008 Chem. Mater. 20 3512 Google Scholar
[30]	Ibrahim E M M, Hakeem A M A, Adam A M M, Shokr E K 2015 Phys. Scr. 90 045802 Google Scholar
[31]	Bando H, Koizumi K, Oikawa Y, Daikohara K, Kulbachinskii V A, Ozaki H 2000 J. Phys. Condens. Matter 12 5607 Google Scholar
[32]	Jia F, Liu Y Y, Zhang Y F, Shu X, Chen L, Wu L M 2020 J. Am. Chem. Soc. 142 12536 Google Scholar
[33]	Liu X, Chen J, Luo M, Leng M, Xia Z, Zhou Y, Qin S, Xue D J, Lv L, Huang H, Niu D, Tang J 2014 ACS Appl. Mater. Interfaces 6 10687 Google Scholar
[34]	Zhang C, Yin H, Han M, Dai Z, Pang H, Zheng Y, Lan Y Q, Bao J, Zhu J 2014 ACS Nano 8 3761 Google Scholar
[35]	Heremans J P, Jovovic V, Toberer E S, Saramat A, Kurosaki K, Charoenphakdee A, Yamanaka S, Snyder G J 2008 Science 321 554 Google Scholar
[36]	Jia B, Liu S, Li G, Liu S, Zhou Y, Wang Q 2019 Thin Solid Films 672 133 Google Scholar

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