Proceedings of nanoGe Fall Meeting 2018 (NFM18)
DOI: https://doi.org/10.29363/nanoge.nfm.2018.218
Publication date: 6th July 2018
In less than 10 years, hybrid organic-inorganic perovskites have emerged as a new generation of absorber materials for high-efficiency and low-cost solar cells [1], [2]. More recently, fully inorganic perovskite quantum dots (QD) also led to promising efficiencies [3], [4] and then become a serious alternative to hybrid organic-inorganic perovskites. Currently, the record efficiency for QD solar cells is obtained with CsPbI3. High resolution in-situ synchrotron XRD measurements have been performed on CsPbI3 as a function of the temperature and revealed a highly anisotropic variation of the lattice parameters. Moreover, CsPbI3 can be temporarily maintained in a perovskite-like structure down to room temperature, stabilizing a metastable perovskite polytype (black-phase) crucial for photovoltaic applications. Structural, vibrational and electronic properties of the three experimentally observed black phases are further scrutinized using theoretical approaches [5], [6]. A symmetry-based tight-binding model, calibrated with self-consistent GW calculations including spin-orbit coupling, affords further insight into their electronic properties. A Rashba effect is thus predicted for both cubic and tetragonal phases when using the symmetry breaking structures obtained through frozen phonon calculations.
The ab initio simulations have been performed on HPC resources of CINES under the allocation 2017-[x2017096724] made by GENCI (Grand Equipement National de Calcul Intensif).
[1] A. Kojima, et al., Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells. J.
Am. Chem. Soc. 2009, 131, 6050−6051.
[2] Best research-cell efficiencies; https://www.nrel.gov/pv/assets/images/efficiency-chart.png (accessed Nov 7, 2017).
[3] H. Bian et al., Graded Bandgap CsPbI2+xBr1-x Perovskite Solar Cells with a Stabilized Efficiency of 14.4%, Joule (2018), https://doi.org/10.1016/j.joule.2018.04.012
[4] E. M. Sanehira, et al., Enhanced Mobility CsPbI3 Quantum Dot Arrays for Record-efficiency, High-voltage Photovoltaic Cells. Sci. Adv. 2017, 3, eaao4204.
[5] A. Marronnier et al., Structural Instabilities Related to Highly Anharmonic Phonons in Halide Perovskites. . J. Phys. Chem. Lett. 2017, 8, 2659−2665
[6] A. Marronnier et al., Anharmonicity and Disorder in the Black Phases of Cesium Lead Iodide Used for Stable Inorganic Perovskite Solar Cells. ACS Nano 2018, 12, 3477−3486