Tailored PEDOT:PSS hole transport layer for higher performance in perovskite solar cells: Enhancement of electrical and optical properties with improved morphology

Precise control over the charge carrier dynamics throughout the device can result in outstanding performance of perovskite solar cells (PSCs). Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) is the most actively studied hole transport material in p-i-n structured PSCs. However, charge transport in the PEDOT:PSS is limited and inefficient because of its low conductivity with the presence of the weak ionic conductor PSS. In addition, morphology of the underlying PEDOT:PSS layer in PSCs plays a crucial role in determining the optoelectronic quality of the active perovskite absorber layer. This work is focused on realization of a non-wetting conductive surface of hole transport layer suitable for the growth of larger perovskite crystalline domains. This is accomplished by employing a facile solvent-engineered (ethylene glycol and methanol) approach resulting in removal of the predominant PSS in PEDOT:PSS. The consequence of acquiring larger perovskite crystalline domains was observed in the charge carrier dynamics studies, with the achievement of higher charge carrier lifetime, lower charge transport time and lower transfer impedance in the solvent-engineered PEDOT:PSS-based PSCs. Use of this solvent-engineered treatment for the fabrication of MAPbI₃ PSCs greatly increased the device stability witnessing a power conversion efficiency of 18.18%, which corresponds to ∼37% improvement compared to the untreated PEDOT:PSS based devices.