RbPbI3 Seed Embedding in PbI2 Substrate Tailors the Facet Orientation and Crystallization Kinetics of Perovskites.

High power conversion efficiencies (PCEs) in perovskite solar cells (PSCs) have always been awe-inspiring, but perovskite films scalability is an exacting precondition for PSCs commercial deployment, generally unachievable through the antisolvent technique. On the contrary, in the two-step sequential method, the perovskite's uncontrolled crystallization and unnecessary PbI2 residue impede the device's performance. These two issues motivated to empower the PbI2 substrate with orthorhombic RbPbI3 crystal seeds, which act as grown nuclei and develop orientated perovskites lattice stacks, improving the perovskite films morphologically and reducing the PbI2 content in eventual perovskite films. Thence, achieving a PCE of 24.17% with suppressed voltage losses and an impressive life span of 1140 h in the open air.

A Functional Biological Molecule Restores the PbI2 Residue-Induced Defects in Two-Step Fabricated Perovskites.

Coating the perovskite layer via a two-step method is an adaptable solution for industries compared to the anti-solvent process. But what about the impact of unreacted PbI2? Usually, it is generated during perovskite conversion in a two-step method and considered beneficial within the grain boundaries, while also being accused of enhancing the interface defects and nonradiative recombination. Several additives are mixed in PbI2 precursors for the purpose of improving the perovskite crystallinity and hindering the Pb2+ defects. Herein, in lieu of adding additives to the PbI2, the effects of the PbI2 residue via the electron transport layer/perovskite interface modification are explored. Consequently, by introducing artemisinin decorated with hydrophobic alkyl units and a ketone group, it reduces the residual PbI2 and improves the perovskites' crystallinity by coordinating with Pb2+. In addition, artemisinin-deposited perovskite enhances both the stability and efficiency of perovskite solar cells by suppressing nonradiative recombination.

Enhanced optoelectronic quality of perovskite films with excess CH3NH3I for high-efficiency solar cells in ambient air.

Solution-processed polycrystalline perovskite films contribute critically to the high photovoltaic performance of perovskite-based solar cells (PSCs). The inevitable electronic trap states at grain boundaries and intrinsic defects such as metallic lead (Pb0) and halide vacancies in perovskite films cause serious carrier recombination loss. Furthermore, the film can easily decompose into PbI2 in a moist atmosphere. Here, we introduce a simple strategy, through a small increase in methylammonium iodide (CH3NH3I, MAI), molar proportion (5%), for perovskite fabrication in ambient air with ∼50% relative humidity. Analysis of the morphology and crystallography demonstrates that excess MAI significantly promotes grain growth without decomposition. X-ray photoemission spectroscopy shows that no metallic Pb0 exists in the perovskite film and the I/Pb ratio is improved. A time-resolved photoluminescence measurement indicates efficient suppression of non-radiative recombination in the perovskite layer. As a result, the device yields improved power conversion efficiency from 14.06% to 18.26% with reduced hysteresis and higher stability under AM1.5G illumination (100 mW cm-2). This work strongly provides a feasible and low-cost way to develop highly efficient PSCs in ambient air.

A Novel Upside-Down Thermal Annealing Method Toward High-Quality Active Layers Enables Organic Solar Cells with Efficiency Approaching 20.

The emerging non-fullerene acceptors with low voltage losses have pushed the power conversion efficiency of organic solar cells (OSCs) to ≈20% with auxiliary morphology optimization. Thermal annealing (TA), as the most widely adopted post-treatment method, has been playing an essential role in realizing the potential of various material systems. However, the procedure of TA, i.e., the way that TA is performed, is almost identical among thousands of OSC papers since ≈30 years ago other than changes in temperature and annealing time. Herein, a reverse thermal annealing (RTA) technique is developed, which can enhance the dielectric constant of active layer film, thereby producing a smaller Coulomb capture radius (14.93 nm), meanwhile, forming a moderate nano-scale phase aggregation and a more favorable face-on molecular stacking orientation. Thus, this method can reduce the decline in open circuit voltage of the conventional TA method by achieving decreased radiative (0.334 eV) and non-radiative (0.215 eV) recombination loss. The power conversion efficiency of the RTA PM6:L8-BO-X device increases to 19.91% (certified 19.42%) compared to the TA device (18.98%). It is shown that this method exhibits a superb universality in 4 other material systems, revealing its dramatic potential to be employed in a wide range of OSCs.

Acidic "Water-in-Salt" Electrolyte Enables a High-Energy Symmetric Supercapacitor Based on Titanium Carbide MXene.

Titanium carbide MXene, Ti3C2Tx, exhibits ultrahigh capacitance in acidic electrolytes at negative potentials yet poor stability at positive potentials, resulting in low-energy densities for Ti3C2Tx-based symmetric supercapacitors. Utilizing "water-in-salt" electrolytes has successfully expanded the stable operation potential window of MXenes. However, this advancement comes at the cost of sacrificing their high capacitance in acidic electrolytes. In this work, we report an acidic "water-in-salt" (AWIS) electrolyte composed of sulfuric acid and saturated lithium halide, which effectively doubled the energy density of the Ti3C2Tx-based symmetric supercapacitor compared to those with bare acidic electrolytes. Specifically, the AWIS electrolyte successfully expanded the voltage window of the symmetric device to 1.1 V. A high specific capacitance of 112.34 F g-1 (at 10 mV s-1) was obtained due to the presence of proton redox. As a result, the symmetric device achieved a high-energy density of 19.1 Wh kg-1 and a high capacitance retention of 96.3% after 10,000 cycles. This work demonstrates the importance of designing stable and redox-active electrolytes for high-energy MXene-based symmetric supercapacitors.

Synergic Surface Modifications of PbS Quantum Dots by Sodium Acetate in Solid-State Ligand Exchange toward Short-Wave Infrared Photodetectors.

PbS quantum dots (QDs) are promising for short-wave infrared (SWIR) photodetection and imaging. Solid-state ligand exchange (SSLE) is a low-fabrication-threshold QD solid fabrication method. However, QD treatment by SSLE remains challenging in seeking refined surface passivation to achieve the desired device performance. This work investigates using NaAc in the ligand exchange process to enhance the film morphology and electronic coupling configuration of QD solids. By implementing various film and photodetector device characterization studies, we confirm that adding NaAc with a prominent adding ratio of 20 wt % NaAc with tetrabutylammonium iodide (TBAI) in the SSLE leads to an improved film morphology, reduced surface roughness, and decreased trap states in the QD solid films. Moreover, compared to the devices without NaAc treatment, those fabricated with NaAc-treated QD solids exhibit an enhanced performance, including lower dark current density (<100 nA/cm2), faster response speed, higher responsivity, detectivity, and external quantum efficiency (EQE reaching 25%). The discoveries can be insightful in developing efficient, low-cost, and low-fabrication-threshold QD SWIR detection and imager applications.

Composition engineering of perovskite absorber assisted efficient textured monolithic perovskite/silicon heterojunction tandem solar cells.

A two-terminal (2T) perovskite/silicon heterojunction tandem solar cell (PVSK/SHJ) is considered one of the most promising candidates for next-generation photovoltaics with the possibility of achieving a power conversion efficiency (PCE) exceeding 30% at low production cost. However, the current mismatch and voltage loss have seriously decreased the performance of 2T PVSK/SHJ tandem solar cells. Here, we report the composition engineering for perovskite top cells to prepare a high performance 2T tandem cell by tuning CsBr co-evaporating rates and increasing concentrations of FAI/FABr solutions. We show that the variation in composition for the perovskite absorber effectively optimized the band gap and diminished the defects of the top cell. Our investigations reveal that the current mismatch of sub-cells was carefully tuned by introducing CsBr at varied co-evaporating rates and the voltage loss was decreased by increasing concentrations of FAI/FABr solutions. Thus, we achieved a PCE of 23.22% in two-terminal monolithic tandems with an area of 1.2 cm2 by tuning the composition of the perovskite absorber.

MXene-Modulated Electrode/SnO2 Interface Boosting Charge Transport in Perovskite Solar Cells.

Interface engineering is imperative to boost the extraction capability in perovskite solar cells (PSCs). We propose a promising approach to enhance the electron mobility and charge transfer ability of tin oxide (SnO2) electron transport layer (ETL) by introducing a two-dimensional carbide (MXene) with strong interface interaction. The MXene-modified SnO2 ETL also offers a preferable growth platform for perovskite films with reduced trap density. Through a spatially resolved imaging technique, profoundly reduced non-radiative recombination and charge transport losses in PSCs based on MXene-modified SnO2 are also observed. As a result, the PSC achieves an enhanced efficiency of 20.65% with ultralow saturated current density and negligible hysteresis. We provide an in-depth mechanistic understanding of MXene interface engineering, offering an alternative approach to obtain efficient PSCs.

Beneficial effects of potassium iodide incorporation on grain boundaries and interfaces of perovskite solar cells.

Grain boundaries and interfacial impurities are the main factors that limit the further development of polycrystalline perovskite solar cells because their existence severely deteriorates the device performance. In order to optimize the efficiency of perovskite solar cells, it is essential to eliminate these defects. In the present work, potassium iodide (KI) is incorporated into the perovskite absorber. KI incorporation improves the crystallinity of the perovskite, increases the grain size, and decreases the contact potential distribution at the grain boundary, which are verified by X-ray diffraction, scanning electronic microscopy and Kelvin probe force microscopy. Besides, the activation energy of the recombination, estimated from the temperature dependent current-voltage of perovskite solar cells, is larger than the bandgap calculated from the temperature coefficient. These suggest that KI incorporation effectively passivates the grain boundaries and interfacial defects. As a result, charge trapping in the absorber as well as the bimolecular and trap-assisted recombination of the device are significantly suppressed. Consequently, the open circuit voltage and fill factor of the incorporated devices are greatly improved, enabling an optimized power conversion efficiency of 19.5%, in comparison with that of 17.3% for the control one. Our work provides an effective strategy of defect passivation in perovskite solar cells by KI incorporation and clarifies the mechanism of the performance optimization of KI incorporated devices.

Self-Organized Fullerene Interfacial Layer for Efficient and Low-Temperature Processed Planar Perovskite Solar Cells with High UV-Light Stability.

In this Communication, a self-organization method of [6,6]-phenyl-C61-butyric acid 2-((2-(dimethylamino)-ethyl) (methyl)amino)ethyl ester (PCBDAN) interlayer in between 6,6-phenyl C61-butyric acid methyl ester (PCBM) and indium tin oxide (ITO) has been proposed to improve the performance of N-I-P perovskite solar cells (PSCs). The introduction of self-organized PCBDAN interlayer can effectively reduce the work function of ITO and therefore eliminate the interface barrier between electron transport layer and electrode. It is beneficial for enhancing the charge extraction and decreasing the recombination loss at the interface. By employing this strategy, a highest power conversion efficiency of 18.1% has been obtained with almost free hysteresis. Furthermore, the N-I-P PSCs have excellent stability under UV-light soaking, which can maintain 85% of its original highest value after 240 h accelerated UV aging. This self-organization method for the formation of interlayer can not only simplify the fabrication process of low-cost PSCs, but also be compatible with the roll-to-roll device processing on flexible substrates.

Hysteresis-free perovskite solar cells made of potassium-doped organometal halide perovskite.

Potassium-doped organometal halide perovskite solar cells (PSCs) of more than 20% power conversion efficiency (PCE) without I-V hysteresis were constructed. The crystal lattice of the organometal halide perovskite was expanded with increasing of the potassium ratio, where both absorption and photoluminescence spectra shifted to the longer wavelength, suggesting that the optical band gap decreased. In the case of the perovskite with the 5% K+, the conduction band minimum (CBM) became similar to the CBM level of the TiO2-Li. In this situation, the electron transfer barrier at the interface between TiO2-Li and the perovskite was minimised. In fact, the transient current rise at the maximum power voltages of PSCs with 5% K+ was faster than that without K+. It is concluded that stagnation-less carrier transportation could minimise the I-V hysteresis of PSCs.

Ambient Engineering for High-Performance Organic-Inorganic Perovskite Hybrid Solar Cells.

Considering the evaporation of solvents during fabrication of perovskite films, the organic ambience will present a significant influence on the morphologies and properties of perovskite films. To clarify this issue, various ambiences of N,N-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), and chlorobenzene (CBZ) are introduced during fabrication of perovskite films by two-step sequential deposition method. The results reveal that an ambient CBZ atmosphere is favorable to control the nucleation and growth of CH3NH3PbI3 grains while the others present a negative effect. The statistical results show that the average efficiencies of perovskite solar cells processed in an ambient CBZ atmosphere can be significantly improved by a relatively average value of 35%, compared with those processed under air. The efficiency of the best perovskite solar cells can be improved from 10.65% to 14.55% by introducing this ambience engineering technology. The CH3NH3PbI3 film with large-size grains produced in an ambient CBZ atmosphere can effectively reduce the density of grain boundaries, and then the recombination centers for photoinduced carriers. Therefore, a higher short-circuit current density is achieved, which makes main contribution to the improvement in efficiency. These results provide vital progress toward understanding the role of ambience in the realization of highly efficient perovskite solar cells.

Fulleropyrrolidinium Iodide As an Efficient Electron Transport Layer for Air-Stable Planar Perovskite Solar Cells.

Organic-inorganic halide perovskite solar cells have attracted great attention in recent years. But there are still a lot of unresolved issues related to the perovskite solar cells such as the phenomenon of anomalous hysteresis characteristics and long-term stability of the devices. Here, we developed a simple three-layered efficient perovskite device by replacing the commonly employed PCBM electrical transport layer with an ultrathin fulleropyrrolidinium iodide (C60-bis) in an inverted p-i-n architecture. The devices with an ultrathin C60-bis electronic transport layer yield an average power conversion efficiency of 13.5% and a maximum efficiency of 15.15%. Steady-state photoluminescence (PL) and time-resolved photoluminescence (TRPL) measurements show that the high performance is attributed to the efficient blocking of holes and high extraction efficiency of electrons by C60-bis, due to a favorable energy level alignment between the CH3NH3PbI3 and the Ag electrodes. The hysteresis effect and stability of our perovskite solar cells with C60-bis become better under indoor humidity conditions.