Quantifying Charge Carrier Recombination Losses in MAPbI₃/C60 and MAPbI₃/Spiro-OMeTAD with and without Bias Illumination

To increase the open-circuit voltage in perovskite-based solar cells, recombination processes at the interface with transport layers (TLs) should be identified and reduced. We investigated the charge carrier dynamics in bilayers of methylammonium lead iodide (MAPbI3) with C60 or Spiro-OMeTAD using time-resolved microwave conductance (TRMC) measurements with and without bias illumination (BI). By modeling the results, we quantified recombination losses in bare MAPbI3 and extraction into the TLs. Only under BI did we find that the density of deep traps increases in bare MAPbI3, substantially enhancing trap-mediated losses. This reversible process is prevented in a bilayer with C60 but not with Spiro-OMeTAD. While under BI extraction rates reduce significantly in both bilayers, only in MAPbI3/Spiro-OMeTAD does interfacial recombination also increases, substantially reducing the quasi Fermi level splitting. This work demonstrates the impact of BI on charge dynamics and shows that adjusting the Fermi level of TLs is imperative to reduce interfacial recombination losses.