Title: Organic Solar Cell With Efficiency Over 20% and V_OC Exceeding 2.1 V Enabled by Tandem With All-Inorganic Perovskite and Thermal Annealing-Free Process

Abstract: Organic solar cells (OSCs) based on polymer donor and non-fullerene acceptor achieve power conversion efficiency (PCE) more than 19% but their poor absorption below 550 nm restricts the harvesting of high-energy photons. In contrast, wide bandgap all-inorganic perovskites limit the absorption of low-energy photons and cause serious below bandgap loss. Therefore, a 2-terminal (2T) monolithic perovskite/organic tandem solar cell (TSC) incorporating wide bandgap CsPbI₂Br is demonstrated as front cell absorber and organic PM6:Y6 blend as rear cell absorber, to extend the absorption of OSCs into high-energy photon region. The perovskite sub-cell, featuring a sol–gel prepared ZnO/SnO₂ bilayer electron transporting layer, renders a high open-circuit voltage (V_OC). The V_OC is further enhanced by employing thermal annealing (TA)-free process in the fabrication of rear sub-cell, demonstrating a record high V_OC of 2.116 V. The TA-free Ag/PFN-Br interface in organic sub-cell facilitates charge transport and restrains nonradiative recombination. Consequently, a remarkable PCE of 20.6% is achieved in monolithic 2T-TSCs configuration, which is higher than that of both reported single junction and tandem OSCs, demonstrating that tandem with wide bandgap all-inorganic perovskite is a promising strategy to improve the efficiency of OSCs.