Snaith group

Abstract:

Metal halide perovskite nanocrystal (PNC) light-emitting devices (LEDs) are promising in the future ultra-high-definition display applications due to their tunable bandgap and high color purity. Balanced carrier injection is indispensable for realizing highly efficient LEDs. Herein, cobalt (Co) was doped into ZnO to modulate the electron mobility of a pristine electron transport layer (ETL) and to inhibit exciton quenching at the ZnO/EML interface due to the passivation of oxygen vacancies and the reduction of electron concentration resulting from the trapping of electrons by the Co²⁺-induced deep impurity level. Also, the bandgap was widened due to the size confinement effect. All of those were beneficial to achieve a balanced charge injection during the operating process. Consequently, the maximum luminance increased from 867 cd m^-2 for ZnO LEDs to 1858 cd m^-2 for Co-doped ZnO LEDs, and there was a 70% increase of external quantum efficiency (EQE). By further inserting a polyethylenimine (PEI) layer in the Co-doped ZnO LEDs, the EQE reached 13.0%.

Abstract:

Mixed lead–tin (Pb–Sn) halide perovskites with optimum band gaps near 1.3 eV are promising candidates for next-generation solar cells. However, the performance of solar cells fabricated with Pb–Sn perovskites is restricted by the facile oxidation of Sn(II) to Sn(IV), which induces self-doping. Maltol, a naturally occurring flavor enhancer and strong metal binding agent, was found to effectively suppress Sn(IV) formation and passivate defects in mixed Pb–Sn perovskite films. When used in combination with Sn(IV) scavenging, the maltol surface treatment led to high-quality perovskite films which showed enhanced photoluminescence intensities and charge carrier lifetimes in excess of 7 μs. The scavenging and surface treatments resulted in highly reproducible solar cell devices, with photoconversion efficiencies of up to 21.4% under AM1.5G illumination.

Abstract:

Perovskite photovoltaics advance rapidly, but questions remain regarding point defects: while experiments have detected the presence of electrically active defects no experimentally confirmed microscopic identifications have been reported. Here we identify lead monovacancy (VPb) defects in MAPbI3 (MA = CH3NH3+) using positron annihilation lifetime spectroscopy with the aid of density functional theory. Experiments on thin film and single crystal samples all exhibited dominant positron trapping to lead vacancy defects, and a minimum defect density of ~3 7 1015 cm−3 was determined. There was also evidence of trapping at the vacancy complex (VPbVI)− in a minority of samples, but no trapping to MA-ion vacancies was observed. Our experimental results support the predictions of other first-principles studies that deep level, hole trapping, VPb2−, point defects are one of the most stable defects in MAPbI3. This direct detection and identification of a deep level native defect in a halide perovskite, at technologically relevant concentrations, will enable further investigation of defect driven mechanisms