Preparation and thermoelectric properties of Mn3As2-doped Cd3As2 nanostructures

Chen Shang-Feng; Sun Nai-Kun; Zhang Xian-Min; Wang Kai; Li Wu; Han Yan; Wu Li-Jun; Dai Qin

doi:10.7498/aps.71.20220584

Abstract

Cd₃As₂, especially its various nanostructures, has been considered as an excellent candidate for application in novel optoelectronic devices due to its ultrahigh mobility and good air-stability. Recent researches exhibited Cd₃As₂ as a candidate of thermoelectric materials by virtue of its ultralow thermal conductivity in comparison with other semimetals or metals. In this work, at first ( Cd_1–xMn_x)₃As₂ (x = 0, 0.05, 0.1) bulk alloys are prepared by high-pressure sintering to suppress the volatilization of As element, and then several kinds of Mn₃As₂-doped Cd₃As₂ nanostructures are obtained on mica substrates by chemical vapor deposition (CVD), with bamboo-shoot-nanowire structure forming in a high-temperature region and films in a low-temperature region. Effects of Mn₃As₂ doping on the crystalline structure, phase compositions, microstructures and thermoelectric properties of the Cd₃As₂ nanostructures are systematically studied. Energy-dispersive spectrometer (EDS) analysis at various typical positions of the Mn₃As₂-doped Cd₃As₂ nanostructures shows that the Mn content in these nanostructures is in a range of 0.02%–0.18% (atomic percent), which is much lower than the Mn content in ( Cd_1–xMn_x)₃As₂ (x = 0, 0.05, 0.1) parent alloys. The main phases of these nanostructures are all body centered tetragonal α phase with a small amount of primitive tetragonal α′ phase. Doping results in the α″ phase and Mn₂As impurity phase occurring. The Cd₃As₂ film presents a self-assembled cauliflower microstructure. Upon Mn₃As₂ doping, this morphology finally transforms into a vertical-growth seashell structure. In a high temperature region of the mica substrate, a unique bamboo-shoot-nanowire structure is formed, with vertical-growth bamboo shoots connected by nanowires, and at the end of these nanowires grows a white pentagonal flower structure with the highest Mn content of 0.18% (atomic percent) for all the nanostructures. Conductivity of the Cd₃As₂ film and the bamboo-shoot-nanowire structure are ～20 and 320 S/cm, respectively. The remarkable conductivity enhancement can be attributed to higher crystallinity and the formation of nanowire conductive network, which significantly increase carrier concentration and Hall mobility. The Hall mobility values of the nanowire structures range from 2271 to 3048 cm²/(V·s) much higher than the values of 378–450 cm²/(V·s) for the films. The Seebeck coefficient for the bamboo-shoot-nanowire structure is in a range of 59–68 µV/K, which is about 15% higher than those for the films (50–61 µV/K). Although maximal power factor of the bamboo-shoot-nanowire structure is 14 times as high as that of the thin film, reaching 0.144 mW/(m·K²) at room temperature, this value is still one order of magnitude lower than the previously reported value of 1.58 mW/(m·K²) for Cd₃As₂ single crystal.

Keywords:

Authors and contacts

1.
School of Science, Shenyang Ligong University, Shenyang 110159, China
2.
Key Laboratory for Anisotropy and Texture of Materials from Ministry of Education, School of Material Science and Engineering, Northeastern University, Shenyang 110819, China

Corresponding author: Sun Nai-Kun, naikunsun@163.com ; Wu Li-Jun, wulijun20070915@163.com ;

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 52171187) and the Shenyang Ligong University High-level Results-based Development Funding Program, China (Grant No. SYLUXM202107).

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References

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Cited By

图 1 Mn₃As₂掺杂Cd₃As₂纳米结构制备流程示意图

Figure 1. Schematic diagram of preparation process of Mn₃As₂-doped Cd₃As₂ nanostructures.

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图 2 Mn₃As₂掺杂Cd₃As₂薄膜、竹笋纳米线结构的XRD, 以及3种Cd₃As₂晶体结构标准卡片图

Figure 2. XRD patterns of Mn₃As₂-doped Cd₃As₂ films and bamboo-shoot-nanowire structures and standard XRD cards of three Cd₃As₂ crystalline structures.

DownLoad: Full-Size Img PowerPoint

图 3 Mn₃As₂掺杂Cd₃As₂竹笋纳米线结构的拉曼光谱图

Figure 3. Laman spectra of Mn₃As₂-doped bamboo-shoot-nanowire structures.

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图 4 Mn₃As₂掺杂Cd₃As₂薄膜的SEM图(第1和第2列)及EDS分析结果(第3列)　(a)—(c) F0样品 ((a)插图为薄膜横截面图); (d)—(f) F0.05样品; (g)—(i) F0.1样品

Figure 4. SEM images (the first and second column) and EDS analysis results (the third column) of Mn₃As₂-doped Cd₃As₂ films: (a)–(c) F0 sample (the inset of (a) shows the fracture morphology); (d)–(f) F0.05 sample; (g)–(i) F0.1 sample.

DownLoad: Full-Size Img PowerPoint

图 5 Mn₃As₂掺杂Cd₃As₂纳米线的SEM (第1和第2列)及EDS分析结果(第3和第4列)　(a)—(d) N0 样品; (e)—(h) N0.05 样品; (i)—(l) N0.1样品

Figure 5. SEM images (the first and second column) and EDS analysis results (the third and fourth column) of Mn₃As₂-doped Cd₃As₂ nanowires: (a)–(d) N0 sample_; (e)–(h) N0.05 sample; (i)–(l) N0.1 sample.

DownLoad: Full-Size Img PowerPoint

图 6 Cd₃As₂竹笋纳米线结构横截面的SEM图(a)—(c)及EDS元素成分分析结果(d), (e)

Figure 6. SEM images of the fracture cross section (a)–(c) and EDS analysis and compositional distributions (d), (e) of Cd₃As₂ bamboo-shoot-nanowire structure.

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图 7 Cd₃As₂纳米线的微结构表征　(a) TEM图; (b) 元素成分; (c) HRTEM图; (d) 电子衍射花样图

Figure 7. Microstructure characteristics of Cd₃As₂ nanowires: (a) TEM image; (b) elemental compositions; (c) HRTEM image; (d) selected area electron diffraction image.

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图 8 (a)—(c) Mn₃As₂掺杂Cd₃As₂薄膜的电导率 (a)、塞贝克系数(b)、功率因子(c)随温度的变化曲线; (d) Mn₃As₂掺杂Cd₃As₂薄膜的室温载流子浓度和霍尔迁移率

Figure 8. (a)–(c) Temperature dependence of electrical conductivity (a), Seebeck coefficient (b), and power factor (c) of Mn₃As₂-doped Cd₃As₂ films; (d) room-temperature carrier concentration and Hall mobility (d) of Mn₃As₂-doped Cd₃As₂ films.

DownLoad: Full-Size Img PowerPoint

图 9 (a)—(c) Mn₃As₂掺杂Cd₃As₂竹笋纳米线结构的电导率 (a)、塞贝克系数 (b)、功率因子(c)随温度的变化曲线; (d) Mn₃As₂掺杂Cd₃As₂竹笋纳米线结构的室温载流子浓度和霍尔迁移率

Figure 9. (a)–(c) Temperature dependence of electrical conductivity (a), Seebeck coefficient (b), and power factor (c) of Mn₃As₂-doped Cd₃As₂ bamboo-shoot-nanowire structure; (d) room-temperature carrier concentration and Hall mobility of Mn₃As₂-doped Cd₃As₂ bamboo-shoot-nanowire structure.

DownLoad: Full-Size Img PowerPoint

map

[1]	Kaleem U, Meng Y F, Sun Y, et al. 2020 Appl. Phys. Lett. 117 011102 Google Scholar
[2]	Wang H L, Ma J L, Wei Q Q, Zhao J H 2020 J. Semicond. 41 072903 Google Scholar
[3]	Zhang Y X, Nappini S, Sankar R, Bondino F, Gao J F, Politano A 2021 J. Mater. Chem. C 9 1235 Google Scholar
[4]	Liang T, Gibson Q, Ali M N, Liu M H, Cava R J, Ong N P 2015 Nat. Mater. 14 280 Google Scholar
[5]	Cheng P H, Zhang C, Liu Y W, et al. 2016 New J. Phys. 18 083003 Google Scholar
[6]	Park K, Jung M, Kim D, Bayogan J R, Lee J H, An S J, Seo J, Seo J, Ahn J P, Park J 2020 Nano Lett. 20 4939 Google Scholar
[7]	Suslov A V, Davydov A B, Oveshnikov L N, et al. 2019 Phys. Rev. B 99 094512 Google Scholar
[8]	Zhou T, Zhang C, Zhang H S, Xiu F X, Yang Z Q 2016 Inorg. Chem. Front. 3 1637 Google Scholar
[9]	Zhang C, Zhou T, Liang S H, et al. 2016 Chin. Phys. B 25 017202 Google Scholar
[10]	Wang H H, Luo X G, Peng K L, et al. 2019 Adv. Funct. Mater. 29 1902437 Google Scholar
[11]	Pariari A, Khan N, Singha R, Satpati B, Mandal P 2016 Phys. Rev. B 94 165139 Google Scholar
[12]	杨亮亮, 勤源浩, 魏江涛, 宋培帅, 张明亮, 杨富华, 王晓东 2021 70 076802 Google Scholar Yang L L, Qin Y H, Wei J T, Song P S, Zhang M L, Yang F H, Wang X D 2021 Acta Phys. Sin. 70 076802 Google Scholar
[13]	李彩云, 何文科, 王东洋, 张潇, 赵立东 2021 70 208401 Google Scholar Li C Y, He W K, Wang D Y, Zhang X, Zhao L D 2021 Acta Phys. Sin. 70 208401 Google Scholar
[14]	Sun N K, Li W, Pang C, Zhong D H, Li M L 2021 Solid State Commun. 339 114505 Google Scholar
[15]	Liao W W, Yang L, Chen J, et al. 2019 Chem. Eng. J. 371 593 Google Scholar
[16]	Yue Z M, Zhao K P, Chen H Y, Qiu P F, Zhao L D, Shi X 2021 Chin. Phys. Lett. 38 117201 Google Scholar
[17]	胡威威, 孙进昌, 张玗, 龚悦, 范玉婷, 唐新峰, 谭刚健 2022 71 047101 Google Scholar Hu W W, Sun J C, Zhang Y, Guo Y, Fan Y T, Tang X F, Tan G J 2022 Acta Phys. Sin. 71 047101 Google Scholar
[18]	Chen R K, Lee J, Lee W, Li D Y 2019 Chem. Rev. 119 9260 Google Scholar
[19]	Zhu G P, Zhao C W, Wang X W, Wang J 2021 Chin. Phys. Lett. 38 024401 Google Scholar
[20]	Guo J, Zhao X G, Sun N K, Xiao X F, Liu W, Zhang Z D 2021 J. Mater. Sci. Technol. 76 247 Google Scholar
[21]	Celinski Z, Burian A, Rzepa B, Zdanowicz W 1987 Mat. Res. Bull. 22 419 Google Scholar
[22]	Ril A I, Marenkin S F, Volkov V V, Oveshnikov L N, Kozlov V V 2021 J. Alloys Compd. 892 162082
[23]	Oveshnikov L N, Davydov A B, Suslov A V, Ril A I, Marenkin S F, Vasiliev A L, Aronzon B A 2020 Sci. Rep. 10 4601 Google Scholar
[24]	Wei S, Lu J, Yu W C, Zhang H B, Qian Y T 2006 Cryst. Growth Des. 6 849 Google Scholar
[25]	Weszka J 1999 Phys. Stat. Sol. (b) 211 605 Google Scholar
[26]	Davydov A B, Oveshnikov L N, SuSlov A V, Ril A I, Marenkin S F, Aronzon B A 2020 Phys. Solid State 62 419 Google Scholar
[27]	Marenkin S F, Trukhan V M, Fedorchenko I V, TruKhanov S V, Shoukavaya T V 2014 Russ. J. Inorg. Chem. 59 355 Google Scholar
[28]	Li C Z, Zhu R, Ke X X, Zhang J M, Wang L X, Zhang L, Liao Z M, Yu D P 2015 Cryst. Growth Des. 15 3264 Google Scholar
[29]	Rice A D, Park K, Hughes E T, Mukherjee K, Alberi K 2019 Phys. Rev. Mater. 3 121201 Google Scholar
[30]	Li C Z, Wang L X, Liu H W, Wang J, Liao Z M, Yu D P 2015 Nat. Commun. 6 10137 Google Scholar
[31]	Schonherr P, Hesjedal T 2015 Appl. Phys. Lett. 106 013115 Google Scholar
[32]	Hwang Y, Choi J, Dung D D, Shin Y, Cho S 2011 J. Appl. Phys. 109 063914 Google Scholar
[33]	Dai Z J, Manjappa M, Yang Y K, Tan T C W, Qiang B, Han S, Wong L J, Xiu F X, Liu W W, Singh R 2021 Adv. Funct. Mater. 31 2011011 Google Scholar
[34]	Nishihaya S, Uchida M, Nakazawa Y, Akiba K, Kriener M, Kozuka Y, Miyake A, Taguchi Y, Tokunaga M, Kawasaki M 2018 Phys. Rev. B 97 245103 Google Scholar
[35]	Jia Z Z, Li C Z, Li X Q, Shi J R, Liao Z M, Yu D P, Wu X S 2016 Nat. Commun. 7 13013 Google Scholar

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Preparation and thermoelectric properties of Mn₃As₂-doped Cd₃As₂ nanostructures