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Highly-efficient solar cells containing lead halide perovskites are expected to revolutionize sustainable energy production in the coming years. Combining these next-generation solar panels with agriculture, can optimize land-use, but brings new risks in case of leakage into the soil. Perovskites are generally assumed to be toxic because of the lead (Pb), but experimental evidence to support this prediction is scarce. We used Arabidopsis thaliana to test the toxicity of the lead-based perovskite MAPbI3 (MA = CH3NH3) and several of its precursors in plants. Our results show that MAPbI3 severely hampers plant growth at concentrations above 5 microM. Surprisingly, we find that the precursors MAI is equally toxic, while lead-based precursors without iodide are only toxic above 500 microM. These observations reveal that perovskite toxicity at low concentrations is caused by iodide ions specifically, and contrast the widespread idea that lead is the most harmful component. We calculate that iodide toxicity thresholds are likely to reach in the soil upon perovskite leakage, but much less so for lead toxicity thresholds. Hence, this work stresses the importance to further understand and predict harmful effects of iodide-containing perovskites in the environment.
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Over the last few years of the heyday of hybrid halide perovskites, so many metal cations additives have been tested to improve their optoelectronic properties that it is already difficult to find an element that has not yet been tried. In general, the variety of these approaches is united under the name doping, however, there is currently no clear understanding of the mechanisms of the influence of the metal ion additives on the properties of the lead halide perovskite materials. For many ions there is even no consensus on the most fundamental questions: what lattice position does a given ion occupy and is it incorporated in the structure at all? Here, we derived a system of effective radii of different metal ions in the iodine environment for the set of iodide compounds and reveal their crystal chemical role in the APbI3 perovskites. We analysed the possible lattice positions for 40 most common monovalent, divalent, and trivalent metals to reveal whether they could successfully enter into the perovskite structures. We show that, at most, three parameters - effective size, electronegativity and the softness of metal ions are the main ones for crystal chemical analysis of the possibility of metal doping of hybrid halide perovskites. Our results provide a useful theoretical guidance to rationalize and improve current doping strategies of hybrid halide perovskites with metal ions.
The long carrier lifetime and defect tolerance in metal halide perovskites (MHPs) are major contributors to the superb performance of MHP optoelectronic devices. Large polarons were reported to be responsible for the long carrier lifetime. Yet microscopic mechanisms of the large polaron formation including the so-called phonon melting, are still under debate. Here, time-of-flight (TOF) inelastic neutron scattering (INS) experiments and first-principles density-functional theory (DFT) calculations were employed to investigate the lattice vibrations (or phonon dynamics) in methylammonium lead iodide ($rm{MAPbI_3}$), a prototypical example of MHPs. Our findings are that optical phonons lose temporal coherence gradually with increasing temperature which vanishes at the orthorhombic-to-tetragonal structural phase transition. Surprisingly, however, we found that the spatial coherence is still retained throughout the decoherence process. We argue that the temporally decoherent and spatially coherent vibrations contribute to the formation of large polarons in this metal halide perovskite.
Hybrid organic-inorganic halide perovskites have shown remarkable optoelectronic properties (1-3), believed to originate from correlated motion of charge carriers and the polar lattice forming large polarons (4-7). Few experimental techniques are capable of probing these correlations directly, requiring simultaneous sub-meV energy and femtosecond temporal resolution after absorption of a photon (8). Here we use transient multi-THz spectroscopy, sensitive to the internal motions of charges within the polaron, to temporally and energetically resolve the coherent coupling of charges to longitudinal optical phonons in single crystal CH3NH3PbI3 (MAPI). We observe room temperature quantum beats arising from the coherent displacement of charge from the coupled phonon cloud. Our measurements provide unambiguous evidence of the existence of polarons in MAPI.
Halide perovskites excel in the pursuit of highly efficient thin film photovoltaics, with power conversion efficiencies reaching 25.5% in single junction and 29.5% in tandem halide perovskite/silicon solar cell configurations. Operational stability of perovskite solar cells remains a barrier to their commercialisation, yet a fundamental understanding of degradation processes, including the specific sites at which failure mechanisms occur, is lacking. Recently, we reported that performance-limiting deep sub-bandgap states appear in nanoscale clusters at particular grain boundaries in state-of-the-art $Cs_{0.05}FA_{0.78}MA_{0.17}Pb(I_{0.83}Br_{0.17})_{3}$ (MA=methylammonium, FA=formamidinium) perovskite films. Here, we combine multimodal microscopy to show that these very nanoscale defect clusters, which go otherwise undetected with bulk measurements, are sites at which degradation seeds. We use photoemission electron microscopy to visualise trap clusters and observe that these specific sites grow in defect density over time under illumination, leading to local reductions in performance parameters. Scanning electron diffraction measurements reveal concomitant structural changes at phase impurities associated with trap clusters, with rapid conversion to metallic lead through iodine depletion, eventually resulting in pinhole formation. By contrast, illumination in the presence of oxygen reduces defect densities and reverses performance degradation at these local clusters, where phase impurities instead convert to amorphous and electronically benign lead oxide. Our work shows that the trapping of charge carriers at sites associated with phase impurities, itself reducing performance, catalyses redox reactions that compromise device longevity. Importantly, we reveal that both performance losses and intrinsic degradation can be mitigated by eliminating these defective clusters.
Many optoelectronic properties have been reported for lead halide perovskite polycrystalline films. However, ambiguities in the evaluation of these properties remain, especially for long-range lateral charge transport, where ionic conduction can complicate interpretation of data. Here we demonstrate a new technique to measure the long-range charge carrier mobility in such materials. We combine quasi-steady-state photo-conductivity measurements (electrical probe) with photo-induced transmission and reflection measurements (optical probe) to simultaneously evaluate the conductivity and charge carrier density. With this knowledge we determine the lateral mobility to be ~ 2 cm2/Vs for CH3NH3PbI3 (MAPbI3) polycrystalline perovskite films prepared from the acetonitrile/methylamine solvent system. Furthermore, we present significant differences in long-range charge carrier mobilities, from 2.2 to 0.2 cm2/Vs, between films of contemporary perovskite compositions prepared via different fabrication processes, including solution and vapour phase deposition techniques. Arguably, our work provides the first accurate evaluation of the long-range lateral charge carrier mobility in lead halide perovskite films, with charge carrier density in the range typically achieved under photovoltaic operation.
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