无机材料学报 ›› 2022, Vol. 37 ›› Issue (6): 691-696.DOI: 10.15541/jim20210491
所属专题: 【虚拟专辑】计算材料; 【能源环境】钙钛矿
• 研究快报 • 上一篇
收稿日期:
2021-08-05
修回日期:
2021-08-20
出版日期:
2022-06-20
网络出版日期:
2021-11-01
通讯作者:
孙宜阳, 研究员. E-mail: yysun@mail.sic.ac.cn作者简介:
林啊鸣(1996-), 女, 硕士研究生. E-mail: linaming@student.sic.ac.cn
LIN Aming1,2(), SUN Yiyang1,2(
)
Received:
2021-08-05
Revised:
2021-08-20
Published:
2022-06-20
Online:
2021-11-01
Contact:
SUN Yiyang, professor. E-mail: yysun@mail.sic.ac.cnAbout author:
LIN Aming (1996–), female, Master candidate. E-mail: linaming@student.sic.ac.cn
Supported by:
摘要:
Cs2SnI6是一种稳定且环保的卤化物钙钛矿材料, 在光伏和光电应用方面具有巨大潜力。虽然表面性质对于光电器件的制备至关重要, 但目前尚没有对该材料开展相关的理论研究。利用密度泛函理论计算结合SCAN+rVV10泛函, 本工作研究了Cs2SnI6的(001)、(011)和(111)表面以揭示其热力学稳定性。针对每个表面, 研究考虑了具有不同截断的模型, 包括两个沿(001)方向(分别为CsI2和SnI4终止的表面), 两个沿(011)方向(分别为I4和Cs2SnI2 终止的表面)和三个沿(111)方向(分别为非化学计量比的CsI3、Sn和满足化学计量比的CsI3终止的表面)。由于大多数表面模型是非化学计量比的, 它们的相对稳定性取决于实验制备条件, 因此需要考虑组成元素的化学势。通过确定允许的化学势区域, 研究分析了这些表面的热力学稳定性。结果表明, (001)和 (011)面的表面能会受到化学势的影响, 而满足化学计量比的CsI3终止的(111)表面不受化学势影响, 是Cs2SnI6最稳定的表面。该结果说明, 近期实验普遍观察到的暴露(111)面的晶体是受热力学稳定性驱动形成的。
中图分类号:
林啊鸣, 孙宜阳. Cs2SnI6低指数晶面稳定性的第一性原理计算研究[J]. 无机材料学报, 2022, 37(6): 691-696.
LIN Aming, SUN Yiyang. Stability of Low-index Surfaces of Cs2SnI6 Studied by First-principles Calculations[J]. Journal of Inorganic Materials, 2022, 37(6): 691-696.
Fig. 2 Seven supercell models of Cs2SnI6 surfaces (a) For (001) surface: CsI2-terminated and SnI4-terminated slabs; (b) For (011) surface: I4-terminated and Cs2SnI2-terminated slabs; (c) For (111) surface: non-stoichiometric Sn-terminated, CsI3-terminated and stoichiometric CsI3-terminated slabs
Fig. 3 Calculated total cleavage, relaxation and surface energies of two complementary non-stoichiometric terminations in (001), (011) and (111) orientations, which are compared with the cleavage, relaxation and surface energies of the stoichiometric CsI3-terminated (111) surface
Fig. 4 Illustration of the accessible chemical potential region for Cs2SnI6 Constraints imposed by the formation of competing secondary phases resulting in the allowed region shaded in green
Fig. 5 Stability of low-index surfaces of Cs2SnI6 as a function of chemical potentials (a) Analysis of stability of the two terminations of Cs2SnI6 (001) surface with respect to the allowed region for maintaining equilibrium with the primary phase Cs2SnI6. The orange and blue regions indicate the stable region for CsI2- and SnI4-terminations, respectively; (b) Similar to (a) for the Cs2SnI6 (011) surface. The orange and blue regions are for the I4- and Cs2SnI2-terminations, respectively; (c) Similar to (a) for the Cs2SnI6 (111) surface. The orange and blue regions are for the Sn- and stoichiometric CsI3-terminations, respectively; (d) Surface energies of the seven surface models of Cs2SnI6 as a function of the chemical potentials colorful figures are available on website
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