Probing the Key Roles of Back-Interface in Performance of Carbon-Based Hole-Transport-Layer Free Perovskite Solar Cells

Abstract

Carbon electrodes have gained widespread attention as a sustainable, stable, and low-cost alternative to metal electrodes in perovskite solar cells (PSCs). However, the power conversion efficiency (PCE) of the carbon electrode-based PSCs (C-PSCs) without the hole-transport-layer (HTL) lags far behind their metal-electrode-based counterparts (M-PSCs), and the key factors causing this PCE downgrading have not been comprehensively elucidated. Herein, we study the photovoltaic performance of various HTL-free C-PSCs employing four typical absorbers, namely MAPbI3 (MA=CH3NH3), FAPbI3 (FA= CH(NH2)2), one-step processed FA0.85MA0.15PbI3 (FA/MA-OS), and two-step processed FA1-xMAxPbI3 (FA/MA-TS). Unexpectedly, we found that the PCE of C-PSCs is MAPbI3>FAPbI3>FA/MA-TS>FA/MA-OS, quite different than that of devices with Ag-electrode (FAPbI3> FA/MA-TS>FA/MA-OS>MAPbI3). The in-depth studies reveal that the remarkable differences in surface roughness, surface potential (SP) distribution, and local built-in potential (Vbi) of four absorber films directly affect both the physical and electrical contacts between perovskite and carbon electrode, which finally determine the efficiency of C-PSCs. Among them, the MAPbI3 films possess the smallest roughness and minimum SP gaps between the grain boundaries (GBs) and the grain interiors (GIs), which enable compact contact at perovskite/carbon interface and higher Vbi within the C-PSCs for fast charge transfer, significantly suppressed nonradiative recombination, and thus the highest PCE (15.42%). Based on these findings, we provide some promising approaches for the development of high-efficiency C-PSCs, especially for the ones employing FA-based perovskite absorbers which have performed excellently in M-PSCs.