Abstract

The toxicity and bioavailability of lead (Pb) in halide perovskites motivates the search of Pb-free perovskite-inspired materials (PIMs), which would replicate the great optoelectronic properties of the traditional Pb-based counterparts. Among them, pnictohalides employing antimony or bismuth are especially attractive due to their low toxicity and inherent air stability. Their wide bandgaps (⁓2 eV) can broaden the application scenario beyond single-junction solar cells, being specifically suitable for e.g., silicon-perovskite tandems, indoor photovoltaics (IPVs), and photocatalysis.Despite outstanding indoor power conversion efficiencies up to 60% have been theoretically predicted for PIM-based IPVs, this research is still in a very early stage. In this talk, I will highlight some of our key findings on two-dimensional Sb- and/or Bi- based two-dimensional pnictohalides for sustainable indoor light harvesting. The considerable presence of both intrinsic and surface defects in wide-bandgap PIMs is mostly responsible for the modest indoor power conversion efficiency (PCE(i)) reported so far up to ⁓5% at 1000 lux white LED illumination. I will discuss the effective defect mitigation strategies relying on compositional engineering that we proposed to significantly improve the PCE(i) up to nearly 10% (9.53%). Our extensive characterizations at both material and device level evidence the successful suppression of trap-assisted and interfacial charge recombination as the result of a reduced defect density within the PIM domains and/or at their surface.The importance of our findings for the energy research community (within and beyond halide perovskite) lies in promoting future compositional design effort to reduce the defects in the next-generation wide-bandgap absorbers for eco-friendly energy generation and consumption.

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