The charge carrier lifetime in organic-inorganic perovskites is one of the most important parameters for modeling and design of solar cells and other types of devices. In this work, we use CH₃NH₃PbI₃ single crystal as a model system to study optical absorption, charge carrier generation, and recombination lifetimes. We show that commonly applied photoluminescence lifetime measurements may dramatically underestimate the intrinsic carrier lifetime in CH₃NH₃PbI₃, which could be due to severe charge recombination at the crystal surface and/or fast electron-hole recombination close to the surface. By using the time-resolved microwave conductivity technique, we investigated the lifetime of free mobile charges inside the crystals. Most importantly, we find that for homogeneous excitation throughout the crystal, the charge carrier lifetime exceeds 15 μs. This means that the diffusion length in CH₃NH₃PbI₃ can be as large as 50 μm if it is no longer limited by the dimensions of the crystallites.

The low photovoltaic efficiency of iron pyrite-based solar cells is often related to the presence of sulfur deficiencies. In this paper surfur-rich iron pyrite nanocrystals (FeS₂ NCs) are synthesized by the hot injection method and deposited using layer by layer deposition. Optical absorption measurements show substantial sub-bandgap absorption, which is attributed to a sulfur-rich, thin surface layer. Microwave photoconductance measurements show very little signal of films with the original long ligands, while an approximately 100-fold higher signal is observed for films treated with FeCl₂ and 1,2-ethanedithiol (EDT) solutions. In mesoporous hybrid systems of FeS₂/SnO₂ both sub-band-gap and above-band-gap photons lead to electron injection from FeS₂ into the SnO₂ conduction band. We explain these findings by proposing that pinning of the Fermi level by the surface layer leads to a downward band bending in the direction of the surface within the FeS₂ NC. Hence, photoexcited electrons will first move toward the shell where they relax into empty surface states. As the holes remain behind in the core of the nanocrystals, this results in a charge-separated state with a long lifetime. Interestingly, these surface electrons are able to migrate in the FeS₂ NP layer by interparticle tunneling and can still decay by injection into SnO₂. Hence, our results indicate that SnO₂ is a suitable electron acceptor for FeS₂. The long-lived charge-separated electrons and holes could be exploited efficiently in photodetectors.