Publication date: 16th July 2025
Self-assembling monolayers (SAMs) are investigated as an alternative hole-transport layer (HTL) to PEDOT:PSS in tin-lead (Sn-Pb) narrow-bandgap (NBG) perovskites for all-perovskite tandem solar cell (APTSC) application. Here we report on the use of the pseudo-halide precursor additive lead(II)-thiocyanate (Pb(SCN)2) in SAM based NBG perovskite solar cells. Upon increasing the amount of Pb(SCN)2, SAM based layer stacks exhibit progressively reduced non-radiative carrier recombination and superior film morphology. Photoconversion efficiency reaches a maximum of 18.5 % for a concentration of 1 % Pb(SCN)2 and declines drastically for higher concentrations. Time resolved photoluminescence (trPL) and surface photovoltage (trSPV) show that carrier extraction is impeded in Pb(SCN)2-containing layer stacks with Pb(SCN)2 concentrations greater than 1 %, and UV- and X-ray photoelectron spectroscopy reveal the appearance of SAM molecules on the top surface of the perovskite layer. This study highlights that at higher concentrations of Pb(SCN)2, SAM molecules are relocated from the ITO to the perovskite surface and subsequently block electron extraction at the ETL / perovskite interface. Washing the Pb(SCN)2-containing perovskite film with a mixture of isopropyl alcohol (IPA) and toluene (Tol) to potentially remove the relocated SAM on the top surface leads to a recovery of the trPL and trSPV signal.
Achnowledgements go to the technicians of the HySprint laboratories for maintaining excellent working conditions.
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