Proceedings of Asia-Pacific Conference on Perovskite, Organic Photovoltaics&Optoelectronics (IPEROP25)
Publication date: 17th October 2024
There are concerns about the toxic effects of lead in perovskite solar cell materials on human health and the environment, and there is an urgent need to make the material lead-free. We have previously analyzed the defect structure of Ge-alloyed Sn perovskites, A2SnGeI6 (A=Cs, MA, FA), by first-principles calculations, and have shown that they are defect-resistant materials and are expected to be new lead-free perovskite materials. The aim of this study is to evaluate these Ge-alloyed Sn perovskites by predicting the mobility of carriers, which directly affects the energy conversion efficiency, using first-principles calculations based on the Fröhlich polaron model.
First-principles calculations were performed using the software VASP (Vienna ab initio package) and Quantum Espresso, with PBE and HSE06 as the functional. The mobility of the photogenerated carriers was calculated by the Feynman path integral variational method based on the Fröhlich polaron model, using the Fröhlich coupling constant.
The interaction between electron and hole polarons is expected to be repulsive when the lattice distortion associated with polaron formation is large, and with the experimental observation of Fröhlich polarons for MAPbI3 in 2017, considered a factor that suppresses bimolecular recombination and allows long-range diffusion of carriers. The mobility of CsSnI3 perovskite is obtained as 500-700 cm2/Vs for hole polarons and 70-120 cm2/Vs for electron polarons, which is unbalanced and undesirable from an ambipolar (carrier bidirectional) point of view. However, after Ge alloying (Cs2SnGeI6), the effective masses of electrons and holes are almost the same, and balanced high mobility of 290-440 cm2/Vs is predicted for both electron and hole polarons generated by the interaction with longitudinal optical phonons. The mobility of Ge-alloyed Sn perovskites with A-site as MA and FA will be discussed in the poster.
We acknowledge financial support from NEDO project (“Development of materials for Pb free perovskite tandem solar cells”) on international collaboration.
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