Over the past few years, lead halide perovskites have emerged as a class of dominant semiconductor materials in the photovoltaic (PV) field with an unprecedented sharp enhancement of power conversion efficiencies (PCEs) up to 22.1%, as well as in other promising optoelectronic applications due to their extraordinary and unique properties. However, the lead toxicity and long-term stability of these lead-based perovskites have raised considerable concerns for their real applications. Exploration of potentially low-toxic metal halide perovskite materials becomes one of the significant pivotal challenges in this century for PV, optoelectronic, and other unexplored applications. In this review, we summarize the recent progress on the development of low-toxic metal halide perovskites with a particular focus on their structures and properties, and discuss their potential applications in PV and optoelectronic devices. Moreover, we suggest current challenges and future research directions with the goal of stimulating further research interest and potential applications

Monolithic all-perovskite tandem photovoltaics promise to combine low-cost and high-efficiency solar energy harvesting with the advantages of all-thin-film technologies. To date, laboratory-scale all-perovskite tandem solar cells have only been fabricated using non-scalable fabrication techniques. In response, this work reports on laser-scribed all-perovskite tandem modules processed exclusively with scalable fabrication methods (blade coating and vacuum deposition), demonstrating power conversion efficiencies up to 19.1% (aperture area, 12.25 cm2; geometric fill factor, 94.7%) and stable power output. Compared to the performance of our spin-coated reference tandem solar cells (efficiency, 23.5%; area, 0.1 cm2), our prototypes demonstrate substantial advances in the technological readiness of all-perovskite tandem photovoltaics. By means of electroluminescence imaging and laser-beam-induced current mapping, we demonstrate the homogeneous current collection in both subcells over the entire module area, which explains low losses (<5%rel) in open-circuit voltage and fill factor for our scalable modules.

Interfacial engineering is the key to high‐performance perovskite solar cells (PSCs). While a wide range of fullerene interlayers are investigated for Pb‐based counterparts with a bandgap of >1.5 eV, the role of fullerene interlayers is barely investigated in Sn‐Pb mixed narrow‐bandgap (NBG) PSCs. In this work, two novel solution‐processed fullerene derivatives are investigated, namely indene‐C60‐propionic acid butyl ester and indene‐C60‐propionic acid hexyl ester (IPH), as the interlayers in NBG PSCs. It is found that the devices with IPH‐interlayer show the highest performance with a remarkable short‐circuit current density of 30.7 mA cm−2 and a low deficit in open‐circuit voltage. The reduction in voltage deficit down to 0.43 V is attributed to reduced non‐radiative recombination that the authors attribute to two aspects: 1) a higher conduction band offset of ≈0.2 eV (>0 eV) that hampers charge‐carrier‐back‐transfer recombination; 2) a decrease in trap density at the perovskite/interlayer/C60 interfaces that results in reduced trap‐assisted recombination. In addition, incorporating the IPH interlayer enhances charge extraction within the devices that results in considerable enhancement in short‐circuit current density. Using a NBG device with an IPH interlayer, a respectable power conversion efficiency of 24.8% is demonstrated in a four‐terminal all‐perovskite tandem solar cell.

Incorporating 2.5% Cs in FA0.8MA0.2Sn0.5Pb0.5I3 improves the photo-stability of the low-bandgap perovskite solar cells. The champion device with power conversion efficiency of 18.9% maintain 92% of its initial efficiency after 120 min MPP tracking.

Heat‐assisted blade‐coating (HABC) technique can be applied for scalable production of perovskite solar cells (PSCs). With the current setups, HABC is not applicable in ambient atmosphere due to the adverse impact of humidity on perovskite films. Here, a modified HABC method is reported to achieve high quality perovskite films under harsh ambient conditions. By using lead acetate trihydrate (PbAc2 · 3H2O) as the lead source, a rapid low‐temperature, short time annealing treatment is discovered. It is found that a small amount of hydrate water in PbAC2 · 3H2O lead source lead to dense and oriented nuclei at the blade‐coating stage. The concomitant MAPbI3 · xH2O on the surface and grain boundaries of perovskite films isolates the moisture in ambient during the annealing process, melts to form a quasi‐liquid nutrition pool for the cultivation of MAPbI3 grain domains via Ostwald ripening. The as‐prepared perovskite films consist of large grain domains of up to 100 μm, which are highly orientated. Based on these films, the conversion efficiency of PSCs reaches 15.8 ± 0.6%, a jump of nearly 40% compared with that of PbAc2‐sourced devices (11.4 ± 1.0%). The robust strategy presented here is a significant contribution towards scalable production of high efficiency PSCs under ambient condition.

Monolithic two-terminal (2T) perovskite/CuInSe 2 (CIS) tandem solar cells (TSCs) combine the promise of an efficient tandem photovoltaic (PV) technology with the simplicity of an all-thin-film device architecture that is compatible with flexible and lightweight PV. In this work, we present the first-ever 2T perovskite/CIS TSC with a power conversion efficiency (PCE) approaching 25% (23.5% certified, area 0.5 cm 2 ). The relatively planar surface profile and narrow band gap (∼1.03 eV) of our CIS bottom cell allow us to exploit the optoelectronic properties and photostability of a low-Br-containing perovskite top cell as revealed by advanced characterization techniques. Current matching was attained by proper tuning of the thickness and bandgap of the perovskite, along with the optimization of an antireflective coating for improved light in-coupling. Our study sets the baseline for fabricating efficient perovskite/CIS TSCs, paving the way for future developments that might push the efficiencies to over 30%.

One of the great challenges of hybrid organic−inorganic perovskite photovoltaics is the material's stability at elevated temperatures. Over the past years, significant progress has been achieved in the field by compositional engineering of perovskite semiconductors, e.g., using multiple-cation perovskites. However, given the large variety of device architectures and nonstandardized measurement protocols, a conclusive comparison of the intrinsic thermal stability of different perovskite compositions is missing. In this work, we systematically investigate the role of cation composition on the thermal stability of perovskite thin films. The cations in focus of this study are methylammonium (MA), formamidinium (FA), cesium, and the most common mixtures thereof. We compare the thermal degradation of these perovskite thin films in terms of decomposition, optical losses, and optoelectronic changes when stressed at 85 °C for a prolonged time. Finally, we demonstrate the effect of thermal stress on perovskite thin films with respect to their performance in solar cells. We show that all investigated perovskite thin films show signs of degradation under thermal stress, though the decomposition is more pronounced in methylammonium-based perovskite thin films, whereas the stoichiometry in methylammonium-free formamidinium lead iodide (FAPbI 3 ) and formamidinium cesium lead iodide (FACsPbI 3 ) thin films is much more stable. We identify compositions of formamidinium and cesium to result in the most stable perovskite compositions with respect to thermal stress, demonstrating remarkable stability with no decline in power conversion efficiency when stressed at 85 °C for 1000 h. Thereby, our study contributes to the ongoing quest of identifying the most stable perovskite compositions for commercial application.

In this study we design and construct high-efficiency, low-cost, highly stable, hole-conductor-free, solid-state perovskite solar cells, with TiO2 as the electron transport layer (ETL) and carbon as the hole collection layer, in ambient air. First, uniform, pinhole-free TiO2 films of various thicknesses were deposited on fluorine-doped tin oxide (FTO) electrodes by atomic layer deposition (ALD) technology. Based on these TiO2 films, a series of hole-conductor-free perovskite solar cells (PSCs) with carbon as the counter electrode were fabricated in ambient air, and the effect of thickness of TiO2 compact film on the device performance was investigated in detail. It was found that the performance of PSCs depends on the thickness of the compact layer due to the difference in surface roughness, transmittance, charge transport resistance, electron-hole recombination rate, and the charge lifetime. The best-performance devices based on optimized TiO2 compact film (by 2000 cycles ALD) can achieve power conversion efficiencies (PCEs) of as high as 7.82%. Furthermore, they can maintain over 96% of their initial PCE after 651 h (about 1 month) storage in ambient air, thus exhibiting excellent long-term stability.