Minimizing Interfacial Recombination in 1.8 eV Triple-Halide Perovskites for 27.5% Efficient All-Perovskite Tandems.

All-perovskite tandem solar cells show great potential to enable the highest performance at reasonable costs for a viable market entry in the near future. In particular, wide-bandgap (WBG) perovskites with higher open-circuit voltage (VOC ) are essential to further improve the tandem solar cells' performance. Here, a new 1.8 eV bandgap triple-halide perovskite composition in conjunction with a piperazinium iodide (PI) surface treatment is developed. With structural analysis, it is found that the PI modifies the surface through a reduction of excess lead iodide in the perovskite and additionally penetrates the bulk. Constant light-induced magneto-transport measurements are applied to separately resolve charge carrier properties of electrons and holes. These measurements reveal a reduced deep trap state density, and improved steady-state carrier lifetime (factor 2.6) and diffusion lengths (factor 1.6). As a result, WBG PSCs achieve 1.36 V VOC , reaching 90% of the radiative limit. Combined with a 1.26 eV narrow bandgap (NBG) perovskite with a rubidium iodide additive, this enables a tandem cell with a certified scan efficiency of 27.5%.

Impact of dynamic co-evaporation schemes on the growth of methylammonium lead iodide absorbers for inverted solar cells.

A variety of different synthesis methods for the fabrication of solar cell absorbers based on the lead halide perovskite methylammonium lead iodide (MAPbI3, MAPI) have been successfully developed in the past. In this work, we elaborate upon vacuum-based dual source co-evaporation as an industrially attractive processing technology. We present non-stationary processing schemes and concentrate on details of co-evaporation schemes where we intentionally delay the start/end points of one of the two evaporated components (MAI and PbI2). Previously, it was found for solar cells based on a regular n-i-p structure, that the pre-evaporation of PbI[Formula: see text] is highly beneficial for absorber growth and solar cell performance. Here, we apply similar non-stationary processing schemes with pre/post-deposition sequences for the growth of MAPI absorbers in an inverted p-i-n solar cell architecture. Solar cell parameters as well as details of the absorber growth are compared for a set of different evaporation schemes. Contrary to our preliminary assumptions, we find the pre-evaporation of PbI2 to be detrimental in the inverted configuration, indicating that the beneficial effect of the seed layers originates from interface properties related to improved charge carrier transport and extraction across this interface rather than being related to an improved absorber growth. This is further evidenced by a performance improvement of inverted solar cell devices with pre-evaporated MAI and post-deposited PbI2 layers. Finally, we provide two hypothetical electronic models that might cause the observed effects.