Snaith group

Abstract:

Metal halide perovskite based tandem solar cells are promising to achieve power conversion efficiency beyond the theoretical limit of their single-junction counterparts. However, overcoming the significant open-circuit voltage deficit present in wide-bandgap perovskite solar cells remains a major hurdle for realizing efficient and stable perovskite tandem cells. Here, a holistic approach to overcoming challenges in 1.8 eV perovskite solar cells is reported by engineering the perovskite crystallization pathway by means of chloride additives. In conjunction with employing a self-assembled monolayer as the hole-transport layer, an open-circuit voltage of 1.25 V and a power conversion efficiency of 17.0% are achieved. The key role of methylammonium chloride addition is elucidated in facilitating the growth of a chloride-rich intermediate phase that directs crystallization of the desired cubic perovskite phase and induces more effective halide homogenization. The as-formed 1.8 eV perovskite demonstrates suppressed halide segregation and improved optoelectronic properties.

Abstract:

Inside Front Cover
In article number 2300095, Hesjedal and co-workers demonstrate that the substitution of Co2+ ions into the halide perovskite imparts magnetic behavior to the material while maintaining photovoltaic performance. We utilize the Co2+ ions (shown as robots) themselves as probes to sense the local electronic environment of lead in the perovskite, thereby opening the substitution gateway for developing novel functional perovskite materials and devices for future technologies.

Abstract:

Organic dyes with strong absorption in the near-infrared (NIR) region are potentially useful in medical applications, such as tumor imaging and photothermal therapy. In this work, new NIR dyes combining BAr₂ -bridged azafulvene dimer acceptors with diarylaminothienyl donors in a donor-acceptor-donor configuration were synthesized. Surprisingly, it was found that in these molecules the BAr₂ -bridged azafulvene acceptor adopts a 5-membered, rather than 6-membered ring structure. The influence of the aryl substituents on the HOMO and LUMO energy levels of the dye compounds was assessed from electrochemical and optical measurements. Strong electron-withdrawing fluorinated substituents (Ar=C₆ F₅ , 3,5-(CF₃ )₂ C₆ H₃ ) lowered the HOMO energy while preserving the small HOMO-LUMO energy gap, resulting in promising NIR dye molecules that combine strong absorption bands centered around 900 nm with good photostability.

Abstract:

Bandgap tuning is a crucial characteristic of metal-halide perovskites, with benchmark lead-iodide compounds having a bandgap of 1.6 eV. To increase the bandgap up to 2.0 eV, a straightforward strategy is to partially substitute iodide with bromide in so-called mixed-halide lead perovskites. Such compounds are prone, however, to light-induced halide segregation resulting in bandgap instability, which limits their application in tandem solar cells and a variety of optoelectronic devices. Crystallinity improvement and surface passivation strategies can effectively slow down, but not completely stop, such light-induced instability. Here we identify the defects and the intragap electronic states that trigger the material transformation and bandgap shift. Based on such knowledge, we engineer the perovskite band edge energetics by replacing lead with tin and radically deactivate the photoactivity of such defects. This leads to metal halide perovskites with a photostable bandgap over a wide spectral range and associated solar cells with photostable open circuit voltages.