Metal halide perovskites of the general formula ABX3—where A is a monovalent cation such as caesium, methylammonium or formamidinium; B is divalent lead, tin or germanium; and X is a halide anion—have shown great potential as light harvesters for thin-film photovoltaics1–5. Among a large number of compositions investigated, the cubic α-phase of formamidinium lead triiodide (FAPbI3) has emerged as the most promising semiconductor for highly efficient and stable perovskite solar cells6–9, and maximizing the performance of this material in such devices is of vital importance for the perovskite research community. Here we introduce an anion engineering concept that uses the pseudo-halide anion formate (HCOO−) to suppress anion-vacancy defects that are present at grain boundaries and at the surface of the perovskite films and to augment the crystallinity of the films. The resulting solar cell devices attain a power conversion efficiency of 25.6 per cent (certified 25.2 per cent), have long-term operational stability (450 hours) and show intense electroluminescence with external quantum efficiencies of more than 10 per cent. Our findings provide a direct route to eliminate the most abundant and deleterious lattice defects present in metal halide perovskites, providing a facile access to solution-processable films with improved optoelectronic performance. Incorporation of the pseudo-halide anion formate during the fabrication of α-FAPbI3 perovskite films eliminates deleterious iodide vacancies, yielding solar cell devices with a certified power conversion efficiency of 25.21 per cent and long-term operational stability.

/pdf/pseudo-halide-anion-engineering-for-a-fapbi3-perovskite-4k3k8u9skp.pdf

Pseudo-halide anion engineering for α-FAPbI3 perovskite solar cells.

Passivating surface and bulk defects of perovskite films has been proven to be an effective way to minimize nonradiative recombination losses in perovskite solar cells (PVSCs). The lattice interference and perturbation of atomic periodicity at the perovskite surfaces often significantly affect the material properties and device efficiencies. By tailoring the terminal groups on the perovskite surface and modifying the surface chemical environment, the defects can be reduced to enhance the photovoltaic performance and stability of derived PVSCs. Here, we report a rationally designed bifunctional molecule, piperazinium iodide (PI), containing both R2NH and R2NH2+ groups on the same six-membered ring, behaving both as an electron donor and an electron acceptor to react with different surface-terminating ends on perovskite films. The resulting perovskite films after defect passivation show released surface residual stress, suppressed nonradiative recombination loss, and more n-type characteristics for sufficient energy transfer. Consequently, charge recombination is significantly suppressed to result in a high open-circuit voltage (VOC) of 1.17 V and a reduced VOC loss of 0.33 V. A very high power conversion efficiency (PCE) of 23.37% (with 22.75% certified) could be achieved, which is the highest value reported for inverted PVSCs. Our work reveals a very effective way of using rationally designed bifunctional molecules to simultaneously enhance the device performance and stability.

Regulating Surface Termination for Efficient Inverted Perovskite Solar Cells with Greater Than 23% Efficiency

Multifunctional Enhancement for Highly Stable and Efficient Perovskite Solar Cells

Iodine-terminated self-assembled monolayer (I-SAM) was used in perovskite solar cells (PSCs) to achieve a 50% increase of adhesion toughness at the interface between the electron transport layer (ETL) and the halide perovskite thin film to enhance mechanical reliability. Treatment with I-SAM also increased the power conversion efficiency from 20.2% to 21.4%, reduced hysteresis, and improved operational stability with a projected T80 (time to 80% initial efficiency retained) increasing from ~700 hours to 4000 hours under 1-sun illumination and with continuous maximum power point tracking. Operational stability-tested PSC without SAMs revealed extensive irreversible morphological degradation at the ETL/perovskite interface, including voids formation and delamination, whereas PSCs with I-SAM exhibited minimal damage accumulation. This difference was attributed to a combination of a decrease in hydroxyl groups at the interface and the higher interfacial toughness.

https://science.sciencemag.org/content/sci/372/6542/618.full.pdf

Interfacial toughening with self-assembled monolayers enhances perovskite solar cell reliability

Perovskite solar cells (PSCs) emerging as a promising photovoltaic technology with high efficiency and low manufacturing cost have attracted the attention from all over the world. Both the efficiency and stability of PSCs have increased steadily in recent years, and the research on reducing lead leakage and developing eco-friendly lead-free perovskites pushes forward the commercialization of PSCs step by step. This review summarizes the main progress of PSCs in 2020 and 2021 from the aspects of efficiency, stability, perovskite-based tandem devices, and lead-free PSCs. Moreover, a brief discussion on the development of PSC modules and its challenges toward practical application is provided.

/pdf/the-main-progress-of-perovskite-solar-cells-in-2020-2021-7uupnnsvyw.pdf

The Main Progress of Perovskite Solar Cells in 2020-2021.

The upscaling of perovskite solar cells to module scale and long-term stability have been recognized as the most important challenges for the commercialization of this emerging photovoltaic technology. In a perovskite solar module, each interface within the device contributes to the efficiency and stability of the module. Here, we employed a holistic interface stabilization strategy by modifying all the relevant layers and interfaces, namely the perovskite layer, charge transporting layers and device encapsulation, to improve the efficiency and stability of perovskite solar modules. The treatments were selected for their compatibility with low-temperature scalable processing and the module scribing steps. Our unencapsulated perovskite solar modules achieved a reverse-scan efficiency of 16.6% for a designated area of 22.4 cm2. The encapsulated perovskite solar modules, which show efficiencies similar to the unencapsulated one, retained approximately 86% of the initial performance after continuous operation for 2,000 h under AM1.5G light illumination, which translates into a T90 lifetime (the time over which the device efficiency reduces to 90% of its initial value) of 1,570 h and an estimated T80 lifetime (the time over which the device efficiency reduces to 80% of its initial value) of 2,680 h. The upscaling of layer treatments and processing that afford high efficiency and stability in small-area perovskite solar cells remains challenging. Liu et al. show how the efficiency and stability of perovskite modules can be improved using an integrated approach to interface and layer engineering.

A holistic approach to interface stabilization for efficient perovskite solar modules with over 2,000-hour operational stability

https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.201903696

Highly Efficient Perovskite Solar Cells Enabled by Multiple Ligand Passivation

A series of challenging issues such as field-driven spectral drift for the CsPbClxBr3–x system and mixed phases in quasi-two-dimensional structures still exist when devising blue-emitting perovskites. In this Letter, the CsPbBr3 quantum-dot (QD) system is proposed to overcome these challenges. However, to date, the CsPbBr3 QD films with tunable colors from green to blue still cannot be achieved using existing methods. Herein, a simple one-step spin-coating route incorporated with efficient ligand passivation is developed to realize this goal. The size restriction of CsPbBr3 QDs is enabled by a diammonium ligand, propane-1,3-diammonium bromide (PDAB). A mixed-ligand system of phenethylammonium bromide (PEAB) with PDAB is further explored to enhance their optical performance. The CsPbBr3 QDs experience a second growth process upon controlled air exposure, which is utilized to realize their size control and emission wavelength tunability. The CsPbBr3 QD-based devices exhibit no spectral drift in electrolumin...

/pdf/engineering-green-to-blue-emitting-cspbbr3-quantum-dot-films-4pgb49v7u7.pdf

Engineering Green-to-Blue Emitting CsPbBr3 Quantum-Dot Films with Efficient Ligand Passivation

All-inorganic α-CsPbBrxI3-x perovskites featuring nano-sized crystallites show great potential for pure-red light-emitting diode (LED) applications. Currently, the CsPbBrxI3–x LEDs based on nano-sized α-CsPbBrxI3-x crystallites have been fabricated mainly via the classical colloidal route including a tedious procedure of nanocrystal synthesis, purification, ligand or anion exchange, film casting, etc. With the usually adopted conventional LED device structure, only high turn-on voltages (> 2.7) have been achieved for CsPbBrxI3-x LEDs. Moreover, this mix-halide system may suffer from severe spectra-shift under bias. In this report, CsPbBrxI3-x thin films featuring nano-sized crystallites are prepared by incorporating multiple ammonium ligands in a one-step spin-coating route. The multiple ammonium ligands constrain the growth of CsPbBrxI3-x nanograins. Such CsPbBrxI3-x thin films benefit from quantum confinement. The corresponding CsPbBrxI3-x LEDs, adopting a conventional LED structure of indium-doped tin oxide (ITO)/poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)/CsPbBrxI3-x/[6, 6]-phenyl C61 butyric acid methyl ester (PCBM)/bathocuproine (BCP)/Al, emit pure-red color at Commission Internationale de l’eclairage (CIE) coordinates of (0.709, 0.290), (0.711, 0.289), etc., which represent the highest color-purity for reported pure-red perovskite LEDs and meet the Rec. 2020 requirement at CIE (0.708, 0.292) very well. The CsPbBrxI3-x LED shows a low turn-on voltage of 1.6 V, maximum external quantum efficiency of 8.94%, high luminance of 2,859 cdm−2, and good color stability under bias.

CsPbBrxI3-x thin films with multiple ammonium ligands for low turn-on pure-red perovskite light-emitting diodes

Control of forward and inverse reactions between perovskites and precursor materials is key to attaining high-quality perovskite materials. Many techniques focus on synthesizing nanostructured CsPb...

/pdf/inverse-growth-of-large-grain-size-and-stable-inorganic-4bjz87cty6.pdf

Maowei Jiang

Papers

A holistic approach to interface stabilization for efficient perovskite solar modules with over 2,000-hour operational stability

Highly Efficient Perovskite Solar Cells Enabled by Multiple Ligand Passivation

Engineering Green-to-Blue Emitting CsPbBr3 Quantum-Dot Films with Efficient Ligand Passivation

CsPbBrxI3-x thin films with multiple ammonium ligands for low turn-on pure-red perovskite light-emitting diodes

Inverse Growth of Large-Grain-Size and Stable Inorganic Perovskite Micronanowire Photodetectors.