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高压下非铅双钙钛矿Cs2TeCl6的结构和光学性质

姚盼盼 王玲瑞 王家祥 郭海中

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高压下非铅双钙钛矿Cs2TeCl6的结构和光学性质

姚盼盼, 王玲瑞, 王家祥, 郭海中

Evolutions of structural and optical properties of lead-free double perovskite Cs2TeCl6 under high pressure

Yao Pan-Pan, Wang Ling-Rui, Wang Jia-Xiang, Guo Hai-Zhong
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  • 无毒环保且稳定的非铅双钙钛矿材料因具有和铅基钙钛矿相似的三维结构, 被认为是铅基钙钛矿材料最有前景的替代品之一. 本文采用溶液法制备了一种新型非铅双钙钛矿材料Cs2TeCl6, 利用金刚石对顶砧高压装置和高压原位同步辐射X射线衍射、紫外-可见吸收光谱技术, 对其在高压下的晶体结构、光学带隙和电子结构演化进行了深入研究. 研究表明, 在实验压力范围(0—50.0 GPa)内Cs2TeCl6晶体结构并未发生改变, 始终保持Fm-3m的结构对称性, 表明该样品具有良好的稳定性; Cs2TeCl6的体积随压力的增加曲线变化比较平滑, 通过三阶Birch-Mumaghan状态方程得到了体弹模量B0 = (18.77 ± 2.88) GPa; Cs2TeCl6为间接带隙半导体, 在0—20.0 GPa范围内其光学带隙随着压力的增大逐渐减小, 这与高压下八面体[TeCl6]2–的收缩相关. 完全卸压后, Cs2TeCl6恢复到加压前的初始状态. 研究结果为深入理解此类材料的晶体结构和光学性质提供科学依据, 并为调控其晶格结构、光学带隙及电子结构提供思路.
    In recent years, organic-inorganic hybrid perovskite materials have been widely used in solar cells, photodetectors, and light-emitting diodes due to their advantages such as high light absorption coefficient, good carrier mobility, and long carrier diffusion length. However, the high toxicity of lead and poor stability still restrict the application and promotion of such materials. The lead-free double perovskite material derived from the concept of “heterovalent substitution”, while maintaining the high symmetrical structure of perovskite, avoids using the toxic lead elements, which has the advantages of environmental friendly, stable structure, and suitable band gap. At present, the limited research on lead-free double perovskite materials still leaves a big room to researchers, and such a limited research seriously restricts the development and promotion of such materials. Therefore, the relationship between the structure and performance of lead-free double perovskite materials needs further exploring in order to provide theoretical basis for the practical application of such materials. Here in this work, the lead-free double perovskite material Cs2TeCl6 is prepared by the solution method. The crystal structure and optical properties of the lead-free double perovskite Cs2TeCl6 under high pressure are investigated by using diamond anvil cell combined with in-situ high-pressure angle-dispersive X-ray diffraction and ultraviolet-visible absorption technology. The results show that the crystal structure of Cs2TeCl6 is not changed within the experimental pressure range of 0-50.0 GPa, and the structural symmetry of Fm-3m is still maintained, indicating the sample has good stability. The lattice constant and volume of Cs2TeCl6 gradually decrease within the pressure range of 0-50.0 GPa. The volume and pressure of Cs2TeCl6 are fitted using the third-order Birch-Mumaghan equation of state, the bulk elastic modulus is obtained to be B0 = (18.77 ± 2.88) GPa. The smaller bulk elastic modulus indicates that the lead-free double perovskite material Cs2TeCl6 has higher compressibility. The optical band gap of Cs2TeCl6 is 2.68(3) eV at 1 atm and its optical band gap gradually decreases with the increase of pressure, which is related to the shrinkage of octahedral [TeCl6]2– under high pressure. The calculation results show that the Cs2TeCl6 possesses an indirect band gap, the valence band maximum is mainly composed of Cl 3p orbits, and the conduction band minimum is mainly composed of Te 5p and Cl 3p orbits. After the pressure is completely relieved, Cs2TeCl6 returns to the initial state. The above conclusions further deepen the understanding of the crystal structure and optical properties of lead-free double perovskite Cs2TeCl6, and provide a theoretical basis for designing and optimizing the lead-free double perovskite materials.
      通信作者: 王玲瑞, wanglr@zzu.edu.cn ; 郭海中, hguo@zzu.edu.cn
    • 基金项目: 国家自然科学基金(批准号: 11904322)、中国科学院创新交叉团队(批准号: JCTD-2019-01)和河南省高校科技创新团队(批准号: 20IRTSTHN014)资助的课题
      Corresponding author: Wang Ling-Rui, wanglr@zzu.edu.cn ; Guo Hai-Zhong, hguo@zzu.edu.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant No. 11904322), the Interdisciplinary Innovation Team of the Chinese Academy of Sciences, China (Grant No. JCTD-2019-01), and the Science and Technology Innovation Team in Colleges and Universities of Henan Province, China (Grant No. 20IRTSTHN014)
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  • 图 1  不同压力下Cs2TeCl6的同步辐射XRD光谱

    Fig. 1.  Angle-dispersive XRD patterns of Cs2TeCl6 at various pressures.

    图 2  不同压力下Cs2TeCl6的精修结果

    Fig. 2.  Rietveld refinements of Cs2TeCl6 at different pressures.

    图 3  Cs2TeCl6的(a)晶格常数、(b) Te—Cl键长和(c)体积随压力的变化曲线

    Fig. 3.  High-pressure evolution of (a) the lattice parameters, (b) Te—Cl bond length and (c) volume of Cs2TeCl6.

    图 4  (a), (b) 不同压力下Cs2TeCl6的吸收光谱; (c) Cs2TeCl6的带隙随压力的变化

    Fig. 4.  (a), (b) Optical absorption spectra of Cs2TeCl6 at various pressures; (c) pressure dependence of band gap.

    图 5  Cs2TeCl6在不同压力下理论计算的能带结构和态密度

    Fig. 5.  Calculated band structures and density of states (DOS) of Cs2TeCl6 at various pressures.

  • [1]

    Dursun I, Shen C, Parida M R, Pan J, Sarmah S P, Priante D, Alyami N, Liu J, Saidaminov M I, Alias M S, Abdelhady A L, Ng T K, Mohammed O F, Ooi B S, Bakr O M 2016 ACS Photonics 3 1150Google Scholar

    [2]

    Chen J, Zhao X, Kim S G, Park N G 2019 Adv. Mater. 31 e1902902Google Scholar

    [3]

    Liu M, Johnston M B, Snaith H J 2013 Nature 501 395Google Scholar

    [4]

    Xu Y, Chen Q, Zhang C, Wang R, Wu H, Zhang X, Xing G, Yu W W, Wang X, Zhang Y, Xiao M 2016 J. Am. Chem. Soc. 138 3761Google Scholar

    [5]

    Wang J, Zhang C, Liu H, McLaughlin R, Zhai Y, Vardeny S R, Liu X, McGill S, Semenov D, Guo H, Tsuchikawa R, Deshpande V V, Sun D, Vardeny Z V 2019 Nat. Commun. 10 129Google Scholar

    [6]

    Tan Z K, Moghaddam R S, Lai M L, Docampo P, Higler R, Deschler F, Price M, Sadhanala A, Pazos L M, Credgington D, Hanusch F, Bein T, Snaith H J, Friend R H 2014 Nat. Nanotechnol. 9 687Google Scholar

    [7]

    Li Y, Shi Z F, Li X J, Shan C X 2019 Chin. Phys. B 28 017803Google Scholar

    [8]

    Kojima A, Teshima K, Shirai Y, Miyasaka T 2009 J. Am. Chem. Soc. 131 6050Google Scholar

    [9]

    Best Research-Cell Efficiency Chart https://www.nrel.gov/pv/cell-efficiency.html [2020-06-26]

    [10]

    Wang Z, Shi Z, Li T, Chen Y, Huang W 2017 Angew. Chem. Int. Ed. 56 1190Google Scholar

    [11]

    Zhang Q, Hao F, Li J, Zhou Y, Wei Y, Lin H 2018 Sci. Technol. Adv. Mater. 19 425Google Scholar

    [12]

    Abate A 2017 Joule 1 659Google Scholar

    [13]

    Qin X, Zhao Z, Wang Y, Wu J, Jiang Q, You J 2017 J. Semicond. 38 011002Google Scholar

    [14]

    Zhang Y Y, Chen S Y, Xu P, Xiang H J, Gong X G, Walsh A, Wei S H 2018 Chin. Phys. Lett. 35 036104Google Scholar

    [15]

    Zhao X G, Yang D, Ren J C, Sun Y, Xiao Z, Zhang L 2018 Joule 2 1662Google Scholar

    [16]

    Zhao X G, Yang J H, Fu Y, Yang D, Xu Q, Yu L, Wei S H, Zhang L 2017 J. Am. Chem. Soc. 139 2630Google Scholar

    [17]

    Ju M G, Chen M, Zhou Y, Garces H F, Dai J, Ma L, Padture N P, Zeng X C 2018 ACS Energy Lett. 3 297Google Scholar

    [18]

    Chen M, Ju M G, Carl A D, Zong Y, Grimm R L, Gu J, Zeng X C, Zhou Y, Padture N P 2018 Joule 2 558Google Scholar

    [19]

    Greul E, Petrus M L, Binek A, Docampo P, Bein T 2017 J. Mater. Chem. A 5 19972Google Scholar

    [20]

    程金光 2017 物理学报 66 037401Google Scholar

    Cheng J G 2017 Acta Phys. Sin. 66 037401Google Scholar

    [21]

    董家君, 姚明光, 刘世杰, 刘冰冰 2017 物理学报 66 039101Google Scholar

    Dong J J, Yao M G, Liu S J, Liu B B, 2017 Acta Phys. Sin. 66 039101Google Scholar

    [22]

    段德芳, 马艳斌, 邵子霁, 谢慧, 黄晓丽, 刘冰冰, 崔田 2017 物理学报 66 036102Google Scholar

    Duan D F, Ma Y B, Shao Z J, Xie H, Huang X L, Liu B B, Cui T 2017 Acta Phys. Sin. 66 036102Google Scholar

    [23]

    时旭含, 李海燕, 姚震, 刘冰冰 2020 物理学报 69 067101Google Scholar

    Shi X H, Li H Y, Yao Z, Liu B B 2020 Acta Phys. Sin. 69 067101Google Scholar

    [24]

    王春杰, 王月, 高春晓 2020 物理学报 69 147202Google Scholar

    Wang C J, Wang Y, Gao C X 2020 Acta Phys. Sin. 69 147202Google Scholar

    [25]

    Wang L, Wang K, Zou B 2016 J. Phys. Chem. Lett. 7 2556Google Scholar

    [26]

    Xiao G, Cao Y, Qi G, Wang L, Liu C, Ma Z, Yang X, Sui Y, Zheng W, Zou B 2017 J. Am. Chem. Soc. 139 10087Google Scholar

    [27]

    Zhang L, Zeng Q, Wang K 2017 J. Phys. Chem. Lett. 8 3752Google Scholar

    [28]

    Zhang L, Liu C, Wang L, Liu C, Wang K, Zou B 2018 Angew. Chem. Int. Ed. 57 11213Google Scholar

    [29]

    郭宏伟, 刘然, 王玲瑞, 崔金星, 宋波, 王凯, 刘冰冰, 邹勃 2017 物理学报 66 030701Google Scholar

    Guo H W, Liu R, Wang L R, Cui J X, Song B, Wang K, Liu B B, Zou B 2017 Acta Phys. Sin. 66 030701Google Scholar

    [30]

    Li Q, Wang Y, Pan W, Yang W, Zou B, Tang J, Quan Z 2017 Angew. Chem. Int. Ed. 56 15969Google Scholar

    [31]

    Wang L, Yao P, Wang F, Li S, Chen Y, Xia T, Guo E, Wang K, Zou B, Guo H 2020 Adv. Sci. 7 1902900Google Scholar

    [32]

    Maughan A E, Ganose A M, Bordelon M M, Miller E M, Scanlon D O, Neilson J R 2016 J. Am. Chem. Soc. 138 8453Google Scholar

    [33]

    Birch F 1978 J. Geophys. Res. 83 1257Google Scholar

    [34]

    Lee Y, Mitzi D B, Barnes P W, Vogt T 2003 Phys. Rev. B 68 020103Google Scholar

    [35]

    Lü X, Wang Y, Stoumpos C C, Hu Q, Guo X, Chen H, Yang L, Smith J S, Yang W, Zhao Y, Xu H, Kanatzidis M G, Jia Q 2016 Adv. Mater. 28 8663Google Scholar

    [36]

    Tauc J, Grigorovici R, Vancu A 1966 Phys. Status Solidi 15 627Google Scholar

    [37]

    Sa R, Wei Y, Zha W, Liu D 2020 Chem. Phys. Lett. 754 137538Google Scholar

    [38]

    Wang L, Ou T, Wang K, Xiao G, Gao C, Zou B 2017 Appl. Phys. Lett. 111 233901Google Scholar

    [39]

    Kong L, Liu G, Gong J, Hu Q, Schaller R D, Dera P, Zhang D, Liu Z, Yang W, Zhu K, Tang Y, Wang C, Wei S H, Xu T, Mao H K 2016 Proc. Natl. Acad. Sci. 113 8910Google Scholar

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出版历程
  • 收稿日期:  2020-06-26
  • 修回日期:  2020-07-10
  • 上网日期:  2020-11-02
  • 刊出日期:  2020-11-05

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