Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.211
Publication date: 23rd September 2021
Inverted p-i-n perovskite solar cells (PSCs) are pivotal for fabricating perovskite-based tandem photovoltaics with the highest performance. However, severe non-radiative recombination at the perovskite/electron transport layer and at the grain boundaries (GBs) still limits their open-circuit voltage (VOC) and fill factor (FF) as compared to their n-i-p counterparts. We introduce a novel dual passivation approach using phenethylammonium chloride (PEACl) to simultaneuosly passivate the GBs and the perovskite/C60 interface by using PEACl:PbCl2 as the additive and PEACl for surface treatment, respectively. [1] Employing the self-assembled monolayer [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz) as hole-transporting layer and a methylammonium-free Cs0.18FA0.82PbI3 perovskite absorber (bandgap ~1.57 eV), we achieve a substantially enhanced charge carrier lifetime and quasi-Fermi level splitting (~63 mV enhancement) compared to reference devices. By analyzing X-ray diffraction, cathodoluminescence, scanning electron microscopy, X-ray/ultraviolet photoelectron spectroscopy and Kelvin probe force microscopy measurements, we attribute the positive effects to the formation of a thin heterogeneous 2D Ruddlesden Popper (PEA)2(Cs1−xFAx)n−1Pbn(I1−yCly)3n+1 phase with n ~1-2 at the GBs and film surface. This leads to efficient chemical passivation of GB and surface defects as well as additional electronic passivation at the perovskite/C60 interface due to hole-blocking. Our dual passivation strategy results in one of the highest reported PCEs for p-i-n PSCs of 22.7% with a remarkable VOC and FF of 1.162 V and 83.2%, respectively. In addition, the dual passivated PSCs exhibit a strongly enhanced activation energy for ion migration together with an enhanced stability under light illumnation and prolonged heat treatment.