Prof Henry Snaith FRS

Abstract:

We have accurately determined the exciton binding energy and reduced mass of single crystals of methylammonium lead triiodide using magneto-reflectivity at very high magnetic fields. The single crystal has excellent optical properties with a narrow line width of ∼3 meV for the excitonic transitions and a 2s transition that is clearly visible even at zero magnetic field. The exciton binding energy of 16 ± 2 meV in the low-temperature orthorhombic phase is almost identical to the value found in polycrystalline samples, crucially ruling out any possibility that the exciton binding energy depends on the grain size. In the room-temperature tetragonal phase, an upper limit for the exciton binding energy of 12 ± 4 meV is estimated from the evolution of 1s-2s splitting at high magnetic field.

Abstract:

Metal halide perovskites(1) are the subject of intensive research efforts due to the impressive performance achieved in photovoltaic and optoelectronic devices.(2, 3) The attraction toward these materials, hereafter simply perovskites, arises for a multitude of reasons. First, they show optimal primary optoelectronic properties, such as direct band gaps, long carrier diffusion lengths, and low exciton binding energies, resulting in the remarkable power conversion efficiency, over 22%, that these materials already deliver in optimized photovoltaic devices. These properites are accompanied by ease of processing via solution or vapor phase (or a combination of the two) techniques, low cost and abundance of base materials, low temperature of processing leading to versatility in terms of what substrates can be used, and the ability to process multiple layers on top of each other.

Abstract:

The power conversion efficiency of halide perovskite solar cells is heavily dependent on the perovskite layer being sufficiently smooth and pinhole-free. It has been shown that these features can be obtained even when starting out from rough and discontinuous perovskite film by briefly exposing the film to methylamine (MA) vapor. The exact underlying physical mechanisms of this phenomenon are, however, still unclear. By investigating smooth, MA treated films based on very rough and discontinuous reference films of methylammonium triiode (MAPbI₃) and considering their morphology, crystalline features, local conductive properties, and charge carrier lifetime, we unraveled the relation between their characteristic physical qualities and their performance in corresponding solar cells. We discovered that the extensive improvement in photovoltaic performance upon MA treatment is a consequence of the induced morphological enhancement of the perovskite layer together with improved electron injection into TiO₂, which in fact compensates for an otherwise compromised bulk electronic quality simultaneously caused by the MA treatment.