Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
Publication date: 16th December 2024
Metal halide perovskites (MHPs) show great potential in multijunction photovoltaics applications due to their tunable bandgaps through compositional mixing on the halide site. However, wide-bandgap MHPs (>1.7 eV) typically suffer from greater average open-circuit voltage (VOC) losses compared to their narrow-bandgap counterparts (~1.6 eV) owing to energy-level misalignment with charge extraction layers.[1] Herein, we investigate the origin of such losses, focusing on the energy-level misalignment between the valence band maximum and the highest occupied molecular orbital (HOMO) for a commonly employed combination of FA0.83Cs0.17Pb(I1-xBrx)3 with bromide content x ranging from 0 to 1, and poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA).[2] Our research combines time-resolved photoluminescence spectroscopy and numerical modelling to reveal the origin of VOC losses, which stem from the accumulation of holes in the HOMO of hole transport layers, followed by subsequent non-radiative across-interfacial recombination via interfacial defects. By simulating an ideal choice of hole transport material to pair with a mixed-halide MHP whose 1.7 eV bandgap is optimized for silicon/perovskite tandem solar cells, we demonstrate a potential reduction in VOC losses originating from energy-level misalignment. Our findings underscore the pressing need for tailored charge-extraction materials with improved energy-level alignment to enhance the efficiency of solar cells based on wide-bandgap mixed halide MHPs.
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