Prof Henry Snaith FRS

Abstract:

Light-emitting diodes (LEDs) made from metal halide perovskites have demonstrated external electroluminescent quantum efficiencies (EQEEL) in excess of 20%. However, their poor operational stability, resulting in lifetimes of only tens to hundreds of hours, needs to be dramatically improved prior to commercial use. There is little consensus in the community upon which factors limit the stability of these devices. Here, we investigate the role played by ammonium cations on the operational stability. We vary the amount of phenylethylammonium bromide, a widely used alkylammonium salt, that we add to a precursor solution of CsPbBr3 and track changes in stability and EQEEL. We find that while phenylethylammonium bromide is beneficial in achieving high efficiency, it is highly detrimental to operational stability. We investigate material properties and electronic characteristics before and after degradation and find that both a reduction in the radiative efficiency of the emitter and significant changes in current–voltage characteristics explain the orders of magnitude drop in the EQEEL, which we attribute to increased ionic mobility. Our results suggest that engineering new contacts and further investigation into materials with lower ionic mobility should yield much improved stability of perovskite LEDs.

Abstract:

Current designs for all-perovskite multi-junction solar cells require mixed-metal Pb-Sn compositions to achieve narrower band gaps than are possible with their neat Pb counterparts. The lower band gap range achievable with mixed-metal Pb-Sn perovskites also encompasses the 1.3 to 1.4 eV range that is theoretically ideal for maximising the efficiency of single-junction devices. Here we examine the optoelectronic quality and photovoltaic performance of the ((HC(NH2)2)0.83Cs0.17)(Pb1-ySny)I3 family of perovskite materials across the full range of achievable band gaps by substituting between 0.001% and 70% of the Pb content with Sn. We reveal that a compositional range of "defectiveness"exists when Sn comprises between 0.5% and 20% of the metal content, but that the optoelectronic quality is restored for Sn content between 30-50%. When only 1% of Pb content is replaced by Sn, we find that photoconductivity, photoluminescence lifetime, and photoluminescence quantum efficiency are reduced by at least an order of magnitude, which reveals that a small concentration of Sn incorporation produces trap sites that promote non-radiative recombination in the material and limit photovoltaic performance. While these observations suggest that band gaps between 1.35 and 1.5 eV are unlikely to be useful for optoelectronic applications without countermeasures to improve material quality, highly efficient narrower band gap absorber materials are possible at or below 1.33 eV. Through optimising single-junction photovoltaic devices with Sn compositions of 30% and 50%, we respectively demonstrate a 17.6% efficient solar cell with an ideal single-junction band gap of 1.33 eV and an 18.1% efficient low band gap device suitable for the bottom absorber in all-perovskite multi-junction cells.

Abstract:

An amendment to this paper has been published and can be accessed via a link at the top of the paper.