Snaith group

Abstract:

Lead halide perovskite nanocrystals are currently under intense investigation as components of solution-processed light-emitting devices (LEDs). We demonstrate LEDs based on Ag doped-passivated CsPbI₃ perovskite nanocrystals with external quantum efficiency of 11.2% and an improved stability. Ag and trilayer MoO₃/Au/MoO₃ structure were used as cathode and anode, respectively, which reduce the electron injection barrier and ensure the high transparency and low resistance of the anode. Silver ions diffuse into perovskite film from the Ag electrode, as confirmed by the elemental mapping, the presence of Ag 3d peaks in the X-ray photoelectron spectrum, and the peak shift in the X-ray diffraction patterns of CsPbI₃. In addition to doping, silver ions play the beneficial role of passivating surface defect states of CsPbI₃ nanocrystals, which results in increased photoluminescence quantum yield, elongated emission lifetime, and improved stability of perovskite films.

Abstract:

The highest power conversion efficiencies (PCEs) reported for perovskite solar cells (PSCs) with inverted planar structures are still inferior to those of PSCs with regular structures, mainly because of lower open-circuit voltages (Voc). Here we report a strategy to reduce nonradiative recombination for the inverted devices, based on a simple solution-processed secondary growth technique. This approach produces a wider bandgap top layer and a more n-type perovskite film, which mitigates nonradiative recombination, leading to an increase in Voc by up to 100 millivolts. We achieved a high Voc of 1.21 volts without sacrificing photocurrent, corresponding to a voltage deficit of 0.41 volts at a bandgap of 1.62 electron volts. This improvement led to a stabilized power output approaching 21% at the maximum power point.

Abstract:

Room-temperature films of black-phase caesium lead iodide (CsPbI3) are widely thought to be trapped in a cubic perovskite polymorph. Here, we challenge this assumption. We present structural refinement of room temperature black-phase CsPbI3 in an orthorhombic polymorph. We demonstrate that this polymorph is adopted by both powders and thin-films of black-phase CsPbI3, fabricated either by high- or low-temperature processes. We perform electronic band structure calculations for the orthorhombic polymorph and find agreement with experimental data and close similarities with orthorhombic methylammonium lead iodide. We investigate the structural transitions and thermodynamic stability of the various polymorphs of CsPbI3, and show that the orthorhombic polymorph is the most stable among its other perovskite polymorphs, but it remains less stable than the yellow non-perovskite polymorph.