Rational Design of Solution-Processed Ti–Fe–O Ternary Oxides for Efficient Planar CH₃NH₃PbI₃ Perovskite Solar Cells with Suppressed Hysteresis

Electron-extraction layer (EEL) plays a critical role in determining the charge extraction and the power conversion efficiencies of the organometal-halide perovskite solar cells (PSCs). In this work, Ti–Fe–O ternary oxides were first developed to work as an efficient EEL in planar PSC. Compared with the widely used TiO<i>_x</i> and the pure FeO<i>_x</i>, the ternary composites show superior properties in multiple aspects including the excellent stability of the precursor solution, good coverage on the substrates, outstanding electrical properties, and suitable energy levels. By varying the Fe content from 0 to 100% in the Ti–Fe–O composites, the conductivity of the resultant compact layer was markedly improved, confirmed by consistent results from the conductive atomic force microscopy and the linear sweep voltammetry measurements. Meanwhile, the compositional engineering tunes the energy level alignment of the Ti–Fe–O EEL/CH₃NH₃PbI₃ interface to a region that is favorable for obtaining excellent charge-extraction property. The combinational advantages of the Ti–Fe–O composites significantly improved the photovoltaic performance of the as-prepared solar cells. An increase of over 20% in the short-circuit current (<i>J</i>_SC) density has been achieved due to a modified EEL conductivity and energy alignment with the perovskite layer. The reduction in the surface recombination and enhancement of the charge collection efficiency also result in about 15% increase in the fill factor. Notably, the device also showed remarkably alleviated hysteresis behavior, revealing a prominently inhibited surface recombination

High Efficiency Inverted Planar Perovskite Solar Cells with Solution-Processed NiO_<i>x</i> Hole Contact

NiO_<i>x</i> is a promising hole-transporting material for perovskite solar cells due to its high hole mobility, good stability, and easy processability. In this work, we employed a simple solution-processed NiO_<i>x</i> film as the hole-transporting layer in perovskite solar cells. When the thickness of the perovskite layer increased from 270 to 380 nm, the light absorption and photogenerated carrier density were enhanced and the transporting distance of electron and hole would also increase at the same time, resulting in a large charge transfer resistance and a long hole-extracted process in the device, characterized by the UV–vis, photoluminescence, and electrochemical impedance spectroscopy spectra. Combining both of these factors, an optimal thickness of 334.2 nm was prepared with the perovskite precursor concentration of 1.35 M. Moreover, the optimal device fabrication conditions were further achieved by optimizing the thickness of NiO_<i>x</i> hole-transporting layer and PCBM electron selective layer. As a result, the best power conversion efficiency of 15.71% was obtained with a <i>J</i>_sc of 20.51 mA·cm^–2, a <i>V</i>_oc of 988 mV, and a FF of 77.51% with almost no hysteresis. A stable efficiency of 15.10% was caught at the maximum power point. This work provides a promising route to achieve higher efficiency perovskite solar cells based on NiO or other inorganic hole-transporting materials

Tunable Crystallization and Nucleation of Planar CH₃NH₃PbI₃ through Solvent-Modified Interdiffusion

A smooth and compact light absorption perovskite layer is a highly desirable prerequisite for efficient planar perovskite solar cells. However, the rapid reaction between CH₃NH₃I methylammonium iodide (MAI) and PbI₂ often leads to an inconsistent CH₃NH₃PbI₃ crystal nucleation and growth rate along the film depth during the two-step sequential deposition process. Herein, a facile solvent additive strategy is reported to retard the crystallization kinetics of perovskite formation and accelerate the MAI diffusion across the PbI₂ layer. It was found that the ultrasmooth perovskite thin film with narrow crystallite size variation can be achieved by introducing favorable solvent additives into the MAI solution. The effects of dimethylformamide, dimethyl sulfoxide, γ-butyrolactone, chlorobenzene, and diethyl ether additives on the morphological properties and cross-sectional crystallite size distribution were investigated using atomic force microscopy, X-ray diffraction, and scanning electron microscopy. Furthermore, the light absorption and band structure of the as-prepared CH₃NH₃PbI₃ films were investigated and correlated with the photovoltaic performance of the equivalent solar cell devices. Details of perovskite nucleation and crystal growth processes are presented, which opens new avenues for the fabrication of more efficient planar solar cell devices with these ultrasmooth perovskite layers