Unveiling the Potential of Ambient Air Annealing for Highly Efficient Inorganic CsPbI3 Perovskite Solar Cells.

Here, we report a detailed surface analysis of dry- and ambient air-annealed CsPbI3 films and their subsequent modified interfaces in perovskite solar cells. We revealed that annealing in ambient air does not adversely affect the optoelectronic properties of the semiconducting film; instead, ambient air-annealed samples undergo a surface modification, causing an enhancement of band bending, as determined by hard X-ray photoelectron spectroscopy measurements. We observe interface charge carrier dynamics changes, improving the charge carrier extraction in CsPbI3 perovskite solar cells. Optical spectroscopic measurements show that trap state density is decreased due to ambient air annealing. As a result, air-annealed CsPbI3-based n-i-p structure devices achieved a 19.8% power conversion efficiency with a 1.23 V open circuit voltage.

Interface Modification for Energy Level Alignment and Charge Extraction in CsPbI3 Perovskite Solar Cells.

In perovskite solar cells (PSCs) energy level alignment and charge extraction at the interfaces are the essential factors directly affecting the device performance. In this work, we present a modified interface between all-inorganic CsPbI3 perovskite and its hole-selective contact (spiro-OMeTAD), realized by the dipole molecule trioctylphosphine oxide (TOPO), to align the energy levels. On a passivated perovskite film, with n-octylammonium iodide (OAI), we created an upward surface band-bending at the interface by TOPO treatment. This improved interface by the dipole molecule induces a better energy level alignment and enhances the charge extraction of holes from the perovskite layer to the hole transport material. Consequently, a Voc of 1.2 V and a high-power conversion efficiency (PCE) of over 19% were achieved for inorganic CsPbI3 perovskite solar cells. Further, to demonstrate the effect of the TOPO dipole molecule, we present a layer-by-layer charge extraction study by a transient surface photovoltage (trSPV) technique accomplished by a charge transport simulation.

Stabilization of Inorganic Perovskite Solar Cells with a 2D Dion-Jacobson Passivating Layer.

Inorganic metal halide perovskites such as CsPbI3 are promising for high-performance, reproducible, and robust solar cells. However, inorganic perovskites are sensitive to humidity, which causes the transformation from the black phase to the yellow δ, non-perovskite phase. Such phase instability has been a significant challenge to long-term operational stability. Here, a surface dimensionality reduction strategy is reported, using 2-(4-aminophenyl)ethylamine cation to construct a Dion-Jacobson 2D phase that covers the surface of the 3D inorganic perovskite structure. The Dion-Jacobson layer mainly grows at the grain boundaries of the perovskite, effectively passivating surface defects and providing favourable interfacial charge transfer. The resulting inorganic perovskite films exhibit excellent humidity resistance when submerged in an aqueous solution (isopropanol:water = 4:1 v/v) and exposed to a 50% humidity air atmosphere. The Dion-Jacobson 2D/3D inorganic perovskite solar cell (PSC) achieves a power conversion efficiency (PCE) of 19.5% with a Voc of 1.197 eV. It retains 83% of its initial PCE after 1260 h of maximum power point tracking under 1.2 sun illumination. The work demonstrates an effective way for stabilizing efficient inorganic perovskite solar cells.

Superacids Based on Pentafluoroorthotellurate Derivatives of Aluminum.

The new Lewis acid Al(OTeF5 )3 and its acetonitrile adduct CH3 CN→Al(OTeF5 )3 were obtained by a simple one-step synthesis in batches of up to 15 g. Al(OTeF5 )3 and the adduct were characterized by vibrational spectroscopy (IR, Raman) and quantum-chemical calculations. Furthermore, five different salts of the new weakly coordinating anion [Al(OTeF5 )4 ]- were prepared in a two-step procedure. [Ph4 P][Al(OTeF5 )4 ], Cs[Al(OTeF5 )4 ], [Ph3 C][Al(OTeF5 )4 ], as well as the protonated benzene derivatives [C9 H13 ][Al(OTeF5 )4 ] and [C6 H7 ][Al(OTeF5 )4 ] were characterized by low-temperature single-crystal X-ray diffraction and NMR spectroscopy. Arenium salts have rarely been characterized in the solid state and were synthesized in this work in a simplified fashion.