Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV16)
Publication date: 28th March 2016
The organic-inorganic halide perovskite CH3NH3PbI3 (MAPI) has demonstrated long minority carrier lifetimes and diffusion lengths. Here we present a model which shows that this slow recombination originates from a spin-split indirect-gap. The nature of the band edge is due to large internal electric fields acting on spin-orbit-coupled band extrema, shifting conduction band minima, making the fundamental band gap slightly indirect. A first-principles description of photoluminescence within the Quasiparticle Self-Consistent GW (QSGW) approximation is developed to investigate this phenomena. The rate of recombination and lifetimes are also predicted as a function of temperature and light intensity using this model. We find that the radiative recombination rate related to operating condition of solar cells is reduced by a factor of 350 compared to more conventional direct gap semiconductors. The numerical prediction for minority-carrier lifetime agrees well with reported measurements on single-crystal MAPI. We also demonstrate the existence of indirect gap in the case of disordered orientation of molecules and that the band edge fluctuates in time. This study explains why hybrid halide perovskites can make efficient solar cells.
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