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If perovskite solar cells (PSCs) with high power conversion efficiencies (PCEs) are to be commercialized, they must achieve long-term stability, which is usually assessed with accelerated degradation tests. One of the persistent obstacles for PSCs has been successfully passing the damp-heat test (85°C and 85% relative humidity), which is the standard for verifying the stability of commercial photovoltaic (PV) modules. We fabricated damp heat–stable PSCs by tailoring the dimensional fragments of two-dimensional perovskite layers formed at room temperature with oleylammonium iodide molecules; these layers passivate the perovskite surface at the electron-selective contact. The resulting inverted PSCs deliver a 24.3% PCE and retain >95% of their initial value after >1000 hours at damp-heat test conditions, thereby meeting one of the critical industrial stability standards for PV modules.

High-efficiency perovskite-based solar cells comprise sophisticated stacks of materials which, however, often feature different thermal expansion coefficients and are only weakly bonded at their interfaces. This may raise concerns over delamination in such devices, jeopardizing their long-term stability and commercial viability. Here, we investigate the root causes of catastrophic top-contact delamination we observed in state-of-the-art p-i-n perovskite/silicon tandem solar cells. By combining macroscopic and microscopic analyses, we identify the interface between the fullerene electron transport layer and the tin oxide buffer layer at the origin of such delamination. Specifically, we find that the perovskite morphology and its roughness play a significant role in the microscopic adhesion of the top layers, as well as the film processing conditions, particularly the deposition temperature and the sputtering power. Our findings mandate the search for new interfacial linking strategies to enable mechanically strong perovskite-based solar cells, as required for commercialization.

Summary Stacking perovskite solar cells onto crystalline silicon bottom cells in a monolithic tandem configuration enables power-conversion efficiencies (PCEs) well above those of their single-junction counterparts. However, state-of-the-art wide-band-gap perovskite films suffer from phase stability issues. Here, we show how carbazole as an additive to the perovskite precursor solution can not only reduce nonradiative recombination losses but, perhaps more importantly, also can suppress phase segregation under exposure to moisture and light illumination. This enables a stabilized PCE of 28.6% (independently certified at 28.2%) for a monolithic perovskite/silicon tandem solar cell over ∼1 cm2 and 27.1% over 3.8 cm2, built from a textured silicon heterojunction solar cell. The modified tandem devices retain ∼93% of their performance over 43 days in a hot and humid outdoor environment of almost 100% relative humidity over 250 h under continuous 1-sun illumination and about 87% during a 85/85 damp-heat test for 500 h, demonstrating the improved phase stability.

Summary Stable and efficient perovskite/silicon tandem solar cells require defect passivation and suppression of light-induced phase segregation of the wide-band-gap perovskite. Here, we report how molecules containing both electron-rich and electron-poor moieties, such as phenformin hydrochloride (PhenHCl), can satisfy both requirements, independent of the perovskite’s surface chemical composition and its grain boundaries and interfaces. PhenHCl-passivated wide-band-gap (∼1.68 eV) perovskite p-i-n single-junction solar cells deliver an open-circuit voltage (VOC) ∼100 mV higher than control devices, resulting in power conversion efficiencies (PCEs) up to 20.5%. These devices do not show any VOC losses after more than 3,000 h of thermal stress at 85°C in a nitrogen ambient. Moreover, PhenHCl passivation improves the PCE of textured perovskite/silicon tandem solar cells from 25.4% to 27.4%. Our findings provide critical insights for improved passivation of metal halide perovskite surfaces and the fabrication of highly efficient and stable perovskite-based single-junction and tandem solar cells.

The performance of perovskite solar cells with inverted polarity (p-i-n) is still limited by recombination at their electron extraction interface, which also lowers the power conversion efficiency (PCE) of p-i-n perovskite-silicon tandem solar cells. A MgF x interlayer with thickness of ~1 nanometer at the perovskite/C 60 interface favorably adjusts the surface energy of the perovskite layer through thermal evaporation, which facilitates efficient electron extraction and displaces C 60 from the perovskite surface to mitigate nonradiative recombination. These effects enable a champion open-circuit voltage of 1.92 volts, an improved fill factor of 80.7%, and an independently certified stabilized PCE of 29.3% for a monolithic perovskite-silicon tandem solar cell ~1 square centimeter in area. The tandem retained ~95% of its initial performance after damp-heat testing (85°C at 85% relative humidity) for >1000 hours.

In this work, we report perovskite solar cells in the planar p–i–n configuration based on single-step, anti-solvent-free, low-temperature (70 °C) slot-die-coated methylammonium lead tri-iodide (MAP...

Metal halide perovskites have emerged in recent years as promising photovoltaic materials due to their excellent optical and electrical properties, enabling perovskite solar cells (PSCs) with certified power conversion efficiencies (PCEs) greater than 25%. Provided radiative recombination is the dominant recombination mechanism, photon recycling – the process of reabsorption (and re-emission) of photons that result from radiative recombination – can be utilized to further enhance the PCE toward the Shockley–Queisser (S-Q) theoretical limit. Geometrical optics can be exploited for the intentional trapping of such re-emitted photons within the device, to enhance the PCE. However, this scheme reaches its fundamental diffraction limits at the submicron scale. Therefore, introducing photonic nanostructures offer attractive solutions to manipulate and trap light at the nanoscale via light coupling into guided modes, as well as localized surface plasmon and surface plasmon polariton modes. This review focuses on light-trapping schemes for efficient photon recycling in PSCs. First, we summarize the working principles of photon recycling, which is followed by a review of essential requirements to make this process efficient. We then survey photon recycling in state-of-the-art PSCs and propose design strategies to invoke light-trapping to effectively exploit photon recycling in PSCs. Finally, we formulate a future outlook and discuss new research directions in the context of photon recycling.

Highly efficient perovskite solar cells (PSCs) fabricated in the classic n-i-p configuration generally employ triphenylamine-based hole-transport layers (HTLs) such as spiro-OMeTAD, PTAA, and poly-TPD. Controllable doping of such layers has been critical to achieve increased conductivity and high device performance. To this end, LiTFSI/tBP doping and subsequent air exposure is widely utilized. However, this approach often leads to low device stability and reproducibility. Departing from this point, we introduce the Lewis acid tris(pentafluorophenyl)borane (TPFB) as an effective dopant, resulting in a significantly improved conductivity and lowered surface potential for triphenylamine-based HTLs. Here, we specifically investigated spiro-OMeTAD, which is the most widely used HTL for n-i-p devices, and revealed improved power conversion efficiency (PCE) and stability of the PSCs. Further, we demonstrated the applicability of TPFB doping to other triphenylamine-based HTLs. Spectroscopic characterizations reveal that TPFB doping results in significantly improved charge transport and reduced recombination losses. Importantly, the TPFB-doped perovskite devices retained near 85% of the initial PCE after 1000 h of storage in the air, while the conventional LiTFSI-doped device dropped to 75%. Finally, we give insight into utilizing other similar molecular dopants such as fluorine-free triphenylborane and phosphorus-centered tris(pentafluorophenyl)phosphine (TPFP) by density functional theory analysis underscoring the significance of the central boron atom and fluorination in TPFB for the formation of Lewis acid-base adducts.

Crystalline silicon (c-Si) solar cells comprise more than 95% of the photovoltaics (PV) market. At wafer-scale, this technology is gradually reaching its practical power conversion efficiency (PCE) limit. Therefore, new performance-driven and scalable alternatives must be developed to further increase the cost-competitiveness of PV. Stacked PV absorbers with decreasing bandgaps in a tandem configuration utilize more efficiently the solar spectrum, and can thereby overcome the single-junction efficiency limit of conventional solar cells. Specifically, the monolithic, two-terminal tandem solar cell implementation promises a simple, yet high-performance technology with high market-relevance. Metal-halide perovskite absorbers have attracted broad interest in their application as the top cell of such a c-Si based tandem solar cell configuration. Practically, the perovskite and c-Si subcells need to be electronically coupled, where the interfacial structure should guarantee efficient charge recombination of majority carriers (collected from each subcell), without inducing minority-carrier recombination. In this article, we review the mechanism underlying efficient recombination junctions, and discuss available materials systems for perovskite-based tandems, as well as additional requirements such as efficient light coupling into the subcells, processing compatibility, scalability of materials and methods, and stability. We extend our discussion beyond c-Si to thin-film bottom cell technologies such as low-bandgap perovskites and chalcogenides. We conclude with an outlook on considerations for industrialization of such interfacial structures.

Bifacial monolithic perovskite/silicon tandem solar cells exploit albedo—the diffuse reflected light from the environment—to increase their performance above that of monofacial perovskite/silicon tandems. Here we report bifacial tandems with certified power conversion efficiencies >25% under monofacial AM1.5G 1 sun illumination that reach power-generation densities as high as ~26 mW cm–2 under outdoor testing. We investigated the perovskite bandgap required to attain optimized current matching under a variety of realistic illumination and albedo conditions. We then compared the properties of these bifacial tandems exposed to different albedos and provide energy yield calculations for two locations with different environmental conditions. Finally, we present a comparison of outdoor test fields of monofacial and bifacial perovskite/silicon tandems to demonstrate the added value of tandem bifaciality for locations with albedos of practical relevance. Bifacial solar cells can outperform monofacial cells by exploiting sunlight reflected off the ground surface. De Bastiani et al. show that bifacial perovskite/silicon tandem with an optimized bandgap can deliver a power density of 26 mW cm–2 and compare its performance to monofacial cells under outdoor conditions.

Translating the high power conversion efficiencies of single-junction perovskite solar cells in their classic, non-inverted (n-i-p) architecture to efficient monolithic n-i-p perovskite/silicon tandem solar cells with high current densities has been a persistent challenge due to the lack of low-temperature processable, chemically-insoluble contact materials with appropriate polarity and sufficient optical transparency. To address this, we developed sputtered amorphous niobium oxide (a-NbOx) with ligand-bridged C-60 as an efficient electron-selective contact, deposited on the textured-silicon bottom cell. For the sunward, hole-selective contact we implemented a stack of molecularly doped broadband transparent evaporated 2,2 ',7,7 '-tetra(N,N-di-p-tolyl)amino-9,9-spirobifluorene (spiro-TTB) and atomic layer deposited vanadium oxide, which further enhances the device quantum efficiency. Combining these contact materials with two-dimensional perovskite passivation on the micrometer-thick solution-processed perovskite top cell yields 27% efficient monolithic n-i-p perovskite/silicon tandem solar cells, which represents one of the highest power conversion efficiencies reported on pyramidal textured crystalline silicon bottom cells, and the highest with this polarity. The authors would like to thanks to Nini Wei for the TEM images; funding: the research reported in this publication was supported by funding from King Abdullah University of Science and Technology (KAUST) under award no. OSR-CARF/CCF-3079 and award no. IED OSR-2019-4208.

S.Z. and F.H.I. contributed equally to this work. The authors thank the members of the KAUST Solar Center operations team for their technical help and support. This publication is based upon work supported by the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) under award no. KAUST OSR-2018-CARF/CCF-3079, KAUST OSR-CRG RF/1/3383, KAUST OSR-CRG2018-3737, and IED OSR-2019-4208.

Low-cost solar cells based on solution-processed organic inorganic hybrid perovskites with high photovoltage are highly sought after, especially for their use in tandem cells or for driving electrochemical reactions. Towards this end, we herein present a single-step method for the preparation of regular planar heterojunction solar cells based on formamidinium lead tribromide (FAPbBr(3)), which is fabricated through an antisolvent-assisted crystallization process. This results in the formation of improved film quality of the perovskite layer in terms of uniformity, surface coverage, crystallinity,and light absorption. Devices fabricated using such films utilizing 2,2',7,7'-tetrakis-(N,N-p-dimethoxyphenylamino)-9.9'spirobifluorene (spiro-OMeTAD) as the hole-transport layer exhibits an open-circuit voltage (V,) of 1.32 V with a power conversion efficiency (PCE) close to 6%. The de-vice performance is much higher than when using devices based on the conventional one-,step process (i.e., without using an anti solvent), where a Vo, of 1.04 V and a PCE of 1.1 % are obtained. Moreover, the devices,show better reproducibility with very little hysteresis.

Encapsulates are, in general, the passive components of any photovoltaic device that provides the required shielding from the externally stimulated degradation. Here we provide comprehensive physical insight depicting a rather non-trivial active nature, in contrast to the supposedly passive, atomic layer deposition (ALD) grown Al2O3 encapsulate layer on the hybrid perovskite [(FA0.83MA0.17)0.95Cs0.05PbI2.5Br0.5] photovoltaic device having the configuration: glass/FTO/SnO2/perovskite/spiro-OMeTAD/Au/(±) Al2O3. By combining various electrical characterization techniques, our experimental observations indicate that the ALD chemistry produces considerable enhancement of the electronic conductivity of the spiro-OMeTAD hole transport medium (HTM), resulting in electronic modification of the perovskite/HTM interface. Subsequently, the modified interface provides better hole extraction and lesser ionic accumulation at the interface, resulting in a significant lowering of the burn-in decay and nearly unchanged charge transport parameters explicitly under the course of continuous operation. Unlike the unencapsulated device, the modified electronic structure in the Al2O3 coated device is essentially the principal reason for better performance stability. Data presented in this communication suggest that the ionic accumulation at the spiro-OMeTAD/perovskite interface triggers the device degradation in the uncoated devices, which is eventually followed by material degradation, which can be avoided by active encapsulation.

Perovskite solar cells (PSCs) have become a promising photovoltaic (PV) technology, where the evolution of the electron-selective layers (ESLs), an integral part of any PV device, has played a distinctive role to their progress. To date, the mesoporous titanium dioxide (TiO2 )/compact TiO2 stack has been among the most used ESLs in state-of-the-art PSCs. However, this material requires high-temperature sintering and may induce hysteresis under operational conditions, raising concerns about its use toward commercialization. Recently, tin oxide (SnO2 ) has emerged as an attractive alternative ESL, thanks to its wide bandgap, high optical transmission, high carrier mobility, suitable band alignment with perovskites, and decent chemical stability. Additionally, its low-temperature processability enables compatibility with temperature-sensitive substrates, and thus flexible devices and tandem solar cells. Here, the notable developments of SnO2 as a perovskite-relevant ESL are reviewed with emphasis placed on the various fabrication methods and interfacial passivation routes toward champion solar cells with high stability. Further, a techno-economic analysis of SnO2 materials for large-scale deployment, together with a processing-toxicology assessment, is presented. Finally, a perspective on how SnO2 materials can be instrumental in successful large-scale module and perovskite-based tandem solar cell manufacturing is provided.

Despite impressive power conversion efficiencies (PCEs) reported for lab-scale perovskite solar cells (PSCs), obtaining large-area devices with similar performance remains challenging. Fundamentally, this can largely be attributed to a polarity mismatch between the perovskite-precursor solution and the underlying hydrophobic contact materials, resulting in perovskite films of insufficient quality for scaled devices. Specifically, for p-i-n devices, the commonly used DMF/DMSO co-solvent has a significant polarity mismatch with its underlying hole-transporting layer, PTAA. Here, the role of MAPbI3•solvent adduct interaction with the PTAA surface towards the formation of micro- and nano-scale pinholes is elucidated in detail. Replacing DMSO with NMP in the co-solvent system changes the binding energy profoundly, enabling uniform and dense films over large areas. The PCE of DMF/NMP ink-based devices drops slightly with increasing active device area, from 21.5% (0.1 cm2) to 19.8% (6.8 cm2), in comparison with conventional DMF/DMSO ink. This work opens a pathway towards the scalability of solution-processed perovskite optoelectronic devices.

The recent evolution of solution-processed hybrid organic–inorganic perovskite-based photovoltaic devices opens up the commercial avenue for high-throughput roll-to-roll manufacturing technology. To circumvent the thermal limitations that hinder the use of metal oxide charge transport layers on plastic flexible substrates in such technologies, we employed a relatively low-power nitrogen plasma treatment to achieve compact SnO2 thin-film electrodes at near room temperature. The perovskite photovoltaic devices thus fabricated using N2 plasma-treated SnO2 performed on par with thermally annealed SnO2 electrodes and resulted in a power conversion efficiency (PCE) of ca. 20.3% with stabilized power output (SPO) of ca. 19.1% on rigid substrates. Furthermore, the process is extended to realize flexible perovskite solar cells on indium tin oxide (ITO)-coated polyethylene terephthalate (PET) substrates with champion PCE of 18.1% (SPO ca. 17.1%), which retained ca. 90% of its initial performance after 1000 bending cycles. Our investigations reveal that deep ultraviolet irradiation associated with N2 and N2O plasma emission plays a major role in obtaining good quality metal oxide thin films at lower temperatures and offers promise toward facile integration of a wide variety of metal oxides on flexible substrates. NRF (Natl Research Foundation, S’pore) Accepted version

Though perovskite solar cells (PSC) have reached high efficiency comparable to its counterparts, it is still striving towards finding a strong hold in terms of long-term stability. Several approaches have been made to prevent the degradation of PSC. Here, we present low-temperature ALD deposited Al2O3 as an effective encapsulant for PSC. The encapsulated devices improve with PCE reaching up to 19.4% post 300 cycles of Al2O3 deposition. In-situ QCM and FTIR measurements reveal that trimethylaluminum gets trapped inside the spiro-OMeTAD layer and is available for the subsequent dosage of H2O during nucleation regime. Here we unveil the fact that the ALD grown Al2O3 is not only surface limited, but the material penetrates the spiro-OMeTAD and enhances the hole transport property, improving the overall performance of encapsulated cells. Intermittent measurements indicate that encapsulated cells are stable, retaining 84% of its initial efficiency by the end of 300 days. Subsequently we elucidate that the device measurements under continuous illumination and with different bias conditions and atmosphere show that the ALD grown encapsulation prevents ingress of moisture and oxygen into the cells maintaining their stability.

Hybrid perovskite photovoltaic devices heavily rely on the use of organic (rather than inorganic) charge-transport layers on top of a perovskite absorber layer because of difficulties in depositing inorganic materials on top of these fragile absorber layers. However, in comparison to the unstable and expensive organic transport materials, inorganic charge transport layers provide improved charge transport and stability to the device architecture. Here, we report photovoltaic devices using all-inorganic transport layers in a planar p-i-n junction device configuration using formamidinium lead tribromide (FAPbBr(3)) as an absorber. Efficient planar devices are obtained through atomic layer deposition of nickel oxide and sputtered zinc oxide as hole- and electron-transport materials, respectively. Using only inorganic charge-transport layers resulted in planar FAPbBr3 devices with a power conversion efficiency of 6.75 % at an open-circuit voltage of 1.23 V. The transition of planar FAPbBr3 devices making from all-organic towards all inorganic charge-transport layers is studied in detail.

Pseudohalide thiocyanate anion (SCIN-) has been used as a dopant in a methylammonium lead tri-iodide (MAPbI(3)) framework, aiming for its use as an absorber layer for photovoltaic applications. The substitution of SCN- pseudohalide anion, as verified using Fourier transform infrared (FT-IR) spectroscopy, results in a comprehensive effect on the optical properties of the original material. Photoluminescence measurements at room temperature reveal a significant enhancement in the emission quantum yield of MAPbI(3-x)(SCN)(x), as compared to MAPbI(3), suggestive of suppression of nonradiative channels. This increased intensity is attributed to a highly edge specific emission from MAPbI(3-x)(SCN)(x), microcrystals as revealed by photoluminescence microscopy. Fluoresence lifetime imaging measurements further established contrasting carrier recombination dynamics for grain boundaries and the bulk of the doped material. Spatially resolved emission spectroscopy on individual microcrystals of MAPbI(3),(SCN)(x), reveals that the optical bandgap and density of states at various (local) nanodomains are also nonuniform. Surprisingly, several (local) emissive regions within MAPbI(3-x)(SCN)(x), microcrystals are found to be optically unstable under photoirradiation, and display unambiguous temporal intermittency in emission (blinking), which is extremely unusual and intriguing. We find diverse blinking behaviors for the undoped MAPbI, crystals as well, which leads us to speculate that blinking may be a common phenomenon for most hybrid perovskite materials.

Perovskite-based solar cells have attracted much recent research interest with efficiency approaching 20%. While various combinations of material parameters and processing conditions are attempted for improved performance, there is still a lack of understanding in terms of the basic device physics and functional parameters that control the efficiency. Here we show that perovskite-based solar cells have two universal features: an ideality factor close to two and a space-charge-limited current regime. Through detailed numerical modeling, we identify the mechanisms that lead to these universal features. Our model predictions are supported by experimental results on solar cells fabricated at five different laboratories using different materials and processing conditions. Indeed, this work unravels the fundamental operation principle of perovskite-based solar cells, suggests ways to improve the eventual performance, and serves as a benchmark to which experimental results from various laboratories can be compared.

Highly reproducible and reversible thermochromic nature of dihydrated methylammonium lead iodide is found. A wide bandgap variation of the material (similar to 2 eV) is detected between room temperature and 60 degrees C under ambient condition as a result of phase transition caused by moisture absorption and desorption. In situ X-ray diffraction and Fourier transform infrared spectroscopy studies are performed to understand the mechanistic behavior during the phase transition. This thermochromic property is further explored as absorber material in mesostructured solar cells. Temperature-dependent reversible power conversion efficiency greater than 1% under standard test conditions is demonstrated; revealing its potential applicability in building integrated photovoltaics.

Hybrid organic-inorganic semiconducting perovskite photovoltaic cells are usually coupled with organic hole conductors. Here, we report planar, inverse CH3NH3PbI3-xClx-based cells with inorganic hole conductors. Using electrodeposited NiO as hole conductor, we have achieved a power conversion efficiency of 7.3%. The maximum V-oc obtained was 935 mV with an average V-oc value being 785 mV. Preliminary results for similar cells using electrodeposited CuSCN as hole conductor resulted in devices up to 3.8% in efficiency. The ability to obtain promising cells using NiO and CuSCN expands the presently rather limited range of available hole conductors for perovskite cells.

Radio-frequency magnetron sputtering is demonstrated as an effective tool to deposit highly crystalline thin zinc oxide (ZnO) layer directly on perovskite absorber as an electron transport layer (ETL). As an absorber, formamidinium lead tribromide (FAPbBr3) is fabricated through a modified single-step solution process using hydrogen bromide (HBr) as an additive resulting in complete surface coverage and highly crystalline material. A planar p–i–n device architecture with spin-coated poly-(3,4-ethylenedioxythiophene):poly-styrenesulfonic acid (PEDOT:PSS) as hole transport material (HTM) and sputtered ZnO as ETL results in a short circuit current density of 9.5 mA cm−2 and an open circuit potential of 1.19 V. Numerical simulations are performed to validate the underlying loss mechanisms. The use of phenyl C60 butyric acid methyl ester (PCBM) interface layer between FAPbBr3 and sputter-coated ZnO offers shielding from potential plasma-related interface damage. The modified interface results in a better device efficiency of 8.3% with an open circuit potential of 1.35 V. Such devices offer better stability under continuous illumination under ambient conditions in comparison with the conventional organic ETL (PCBM)-based devices.