Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
DOI: https://doi.org/10.29363/nanoge.nfm.2022.029
Publication date: 11th July 2022
Electrical doping enables meticulous tuning of the electronic properties in novel hybrid perovskite semiconductors, which is critical for their successful impelmentation as optoelectronic applications. Nevertheless, the use of substitutional/interstitial impurities as dopants remains difficult, mainly due to dopant phase segregation and defect compensation. In contrast, molecular doping stands as a promising pathway to modulate charge carrier density via charge transfer without altering the perovskite crystal structure. However, the underlying processes facilitating molecular doping in perovskites (e.g. host-dopant interactions) remain highly underexplored. In this talk, we will present our recent work on the molecualr doping mechanism of p-type methylammonium tin-lead iodide films by using an n-type molecule, namely 4-(1,3-Dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)phenyl)-N,N-dimethylbenzenamine (n-DMBI-H). By employing a combination of experimental and first principles simulation techniques, we identify preferential dative bonding between amino moieties in n-DMBI-H and Sn atoms in perovskite surfaces as a dominant host-dopant interaction that mediates charge transfer. We will discuss the dopant localization within films and deternime that n-DMBI-H is located at perovskite surfaces and grain boundaries, allowing charge carrier density tuning of nearly one order of magnitude. The talk will conclude with details on the incorporation of n-DMBI-H in p-i-n tin-lead perovskite solar cells, which results in lower charge carrier recombination and higher charge selectivity at perovskite/transport layer interfaces. This work elucidates important insights of perovskite molecular doping that are expected to inspire strategies towards next-generation perovskite optoelectronic devices.
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