Pham Hung Q, Holmes Russell J, Aydil Eray S, Gagliardi Laura
Department of Chemistry, Chemical Theory Center, and Supercomputing Institute, University of Minnesota, 207 Pleasant Street SE, Minneapolis, Minnesota 55455, USA.
Department of Chemical Engineering and Materials Science, University of Minnesota, 421 Washington Ave. SE, Minneapolis, Minnesota 55455, USA.
Nanoscale. 2019 Jun 21;11(23):11173-11182. doi: 10.1039/c9nr01645g. Epub 2019 May 31.
Searching for alternatives to lead-containing metal halide perovskites, we explored the properties of indium-based inorganic double perovskites CsInMX with M = Cu, Ag, Au and X = Cl, Br, I, and of its organic-inorganic hybrid derivative MAInCuCl (MA = CHNH) using computation within Kohn-Sham density functional theory. Among these compounds, CsInCuCl and MAInCuCl were found to be potentially promising candidates for solar cells. Calculations with different functionals provided the direct band gap of CsInCuCl between 1.05 and 1.73 eV. In contrast, MAInCuCl exhibits an indirect band gap between 1.31 and 2.09 eV depending on the choice of exchange-correlation functional. CsInCuCl exhibits a much higher absorption coefficient than that calculated for c-Si and CdTe, common semiconductors for solar cells. Even MAInCuCl is predicted to have a higher absorption coefficient than c-Si and CdTe across the visible spectrum despite the fact that it is an indirect band gap material. The intrinsic charge carrier mobilities for CsInCuCl along the L-Γ path are predicted to be comparable to those for MAPbI. Finally, we carried out calculations of the band edge positions for MAInCuCl and CsInCuCl to offer guidance for solar cell heterojunction design and optimization. We conclude that CsInCuCl and MAInCuCl are promising semiconductors for photovoltaic and optoelectronic applications.
为了寻找含铅金属卤化物钙钛矿的替代物，我们利用Kohn-Sham密度泛函理论中的计算方法，研究了铟基无机双钙钛矿CsInMX（M = Cu、Ag、Au，X = Cl、Br、I）及其有机-无机杂化衍生物MAInCuCl（MA = CHNH）的性质。在这些化合物中，发现CsInCuCl和MAInCuCl是太阳能电池潜在的有前景的候选材料。使用不同泛函进行的计算得出CsInCuCl的直接带隙在1.05至1.73 eV之间。相比之下，MAInCuCl根据交换关联泛函的选择，表现出1.31至2.09 eV之间的间接带隙。CsInCuCl的吸收系数比太阳能电池常用的半导体c-Si和CdTe计算得出的吸收系数高得多。尽管MAInCuCl是间接带隙材料，但预计在整个可见光谱范围内其吸收系数比c-Si和CdTe更高。预测CsInCuCl沿L-Γ路径的本征电荷载流子迁移率与MAPbI的相当。最后，我们对MAInCuCl和CsInCuCl的带边位置进行了计算，为太阳能电池异质结设计和优化提供指导。我们得出结论，CsInCuCl和MAInCuCl是用于光伏和光电子应用的有前景的半导体。
