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Random terpolymerization is an effective approach to achieving highly efficient and outdoor-stable terpolymer photovoltaics. However, the working principle behind this remains unclear. Herein, we report spectroscopic, morphological, and computational results and conclude the previous work on terpolymer research to unveil their structure–property relations and elucidate key rules for high-efficiency and outdoor-stable terpolymer photovoltaics. More specifically, introducing a strong electron-deficient or electron-rich third moiety is suggested to enable broadened absorption with minimized non-radiative voltage losses. Besides, the third component should manipulate the D/A miscibility towards a thermodynamically more stable morphology. However, the content of the third component should be small to maintain molecular orientation and exciton diffusion length in conjunction with optimized phase-separation and crystallinity, in turn reducing bimolecular carrier recombination. Obeying these rules, terpolymer solar cells based on the parent donors D18 and PM6 with enhanced power conversion efficiency (PCE) and excellent outdoor stability are demonstrated. Our findings provide a rationale for explaining and achieving high-performance and outdoor-stable terpolymer photovoltaics, paving the path to commercialization.

Accelerating the shift towards renewable materials and sustainable processes for printed organic electronic devices is crucial for a green circular economy. Currently, the fabrication of organic devices with competitive performances is linked to toxic petrochemical-based solvents with considerable carbon emissions. Here we show that terpene solvents obtained from renewable feedstocks can replace non-renewable environmentally hazardous solvent counterparts in the production of highly efficient organic photovoltaics (OPVs) light-emitting diodes (OLEDs) and field-effect transistors (OFETs) with on-par performances. Using a Hansen solubility ink formulation framework, we identify various terpene solvent systems and investigate effective film formation and drying mechanisms required for optimal charge transport. This approach is universal for state-of-the-art materials in OPVs, OLEDs and OFETs. We created an interactive library for green solvent selections and made it publicly available through the OMEGALab website. As potential carbon-negative solvents, terpenes open a unique and universal approach towards efficient, large-area and stable organic electronic devices.

The open-circuit voltage (V

The Urbach energy is an expression of the static and dynamic disorder in a semiconductor and is directly accessible via optical characterization techniques. The strength of this metric is that it elegantly captures the optoelectronic performance potential of a semiconductor in a single number. For solar cells, the Urbach energy is found to be predictive of a material's minimal open-circuit-voltage deficit. Performance calculations considering the Urbach energy give more realistic power conversion efficiency limits than from classical Shockley-Queisser considerations. The Urbach energy is often also found to correlate well with the Stokes shift and (inversely) with the carrier mobility of a semiconductor. Here, we discuss key features, underlying physics, measurement techniques, and implications for device fabrication, underlining the utility of this metric.

Recent achievements in amorphous/crystalline silicon heterojunction (SHJ) solar cells and perovskite/SHJ tandem solar cells place hydrogenated amorphous silicon (a-Si:H) at the forefront of photovoltaics. Due to the extremely low effective doping efficiency of trivalent boron in amorphous tetravalent silicon, light harvesting of aforementioned devices is limited by their fill factors (FFs), a direct metric of the charge carrier transport. It is challenging but crucial to develop highly conductive doped a-Si:H with minimal FF losses. Here we report that light soaking can efficiently boost the dark conductance of boron-doped a-Si:H thin films. Light induces diffusion and hopping of weakly bound hydrogen atoms, which activates boron doping. The effect is reversible and the dark conductivity decreases over time when the solar cell is no longer illuminated. By implementing this effect to SHJ solar cells, we achieved a certified total-area power conversion efficiency of 25.18% with a FF of 85.42% on a 244.63 cm2 wafer.

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.

Organic semiconductor photocatalysts for the production of solar fuels are attractive as they can be synthetically tuned to absorb visible light while simultaneously retaining suitable energy levels to drive a range of processes. However, a greater understanding of the photophysics that determines the function of organic semiconductor heterojunction nanoparticles is needed to optimize performance. Here, we show that such materials can intrinsically generate remarkably long-lived reactive charges, enabling them to efficiently drive sacrificial hydrogen evolution. Our optimized hetereojunction photocatalysts comprise the conjugated polymer PM6 matched with Y6 or PCBM electron acceptors, and achieve external quantum efficiencies of 1.0% to 5.0% at 400 to 900 nm and 8.7% to 2.6% at 400 to 700 nm, respectively. Employing transient and operando spectroscopies, we find that the heterojunction structure in these nanoparticles greatly enhances the generation of long-lived charges (millisecond to second timescale) even in the absence of electron/hole scavengers or Pt. Such long-lived reactive charges open potential applications in water-splitting Z-schemes and in driving kinetically slow and technologically desirable oxidations.

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.

Utilizing four-dimensional scanning ultrafast electron microscopy (4D-SUEM) is a powerful tool to monitor charge dynamics at material surfaces and interfaces especially for the application in renewable energy field. Herein, we uncover unique physical features for 4D-SUEM upon reducing the acceleration of probed primary electrons to 1 keV, for wide range of materials including various single crystals, thin films and quantum dots upon the presence of oxidized and neat surfaces. Working at 1 keV helps to uncover the migration of photogenerated carriers originating from both sub-surface and bulk layers, under the influence of the carriers scattering and the band-bending phenomena. This approach provides a new avenue for the spatial and temporal access to the surface exclusive dynamics in renewable energy materials to unlock their interfacial behaviors at the nanoscale level.

Advanced functional materials 33(4), 2205557 (2023). doi:10.1002/adfm.202205557, Textured silicon wafers used in silicon solar cell manufacturing offer superior light trapping, which is a critical enabler for high-performance photovoltaics. A similar optical benefit can be obtained in monolithic perovskite/silicon tandem solar cells, enhancing the current output of the silicon bottom cell. Yet, such complex silicon surfaces may affect the structural and optoelectronic properties of the overlying perovskite films. Here, through extensive characterization based on optical and microstructural spectroscopy, it is found that the main effect of such substrate morphology lies in an altering of the photoluminescence response of the perovskite, which is associated with thickness variations of the perovskite, rather than lattice strain or compositional changes. With this understanding, the design of high-performance perovskite/silicon tandems is rationalized, yielding certified power conversion efficiencies of >28%., Published by Wiley-VCH, Weinheim

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.

We thank Rosario Vidal from the Universitat Jaume I (Castello, Spain) for her assistance with the nitrogen drying process. This work is funded by the StartUp funding of the South Dakota School of Mines and Technology. E.A. and S.D.W. thank the King Abdullah University of Science and Technology (KAUST) for the financial support via Office of Sponsored Research (OSR) under award no. KAUST OSR-2018-CARF/CCF-3079, IED OSR-2019-4208, and IED OSR-2020-4208.

Perovskite/silicon tandem solar cells are emerging as a high-efficiency and prospectively cost-effective solar technology with great promise for deployment at the utility scale. However, despite the remarkable performance progress reported lately, assuring sufficient device stability-particularly of the perovskite top cell-remains a challenge on the path to practical impact. In this work, we analyze the outdoor performance of encapsulated bifacial perovskite/silicon tandems, by carrying out field-testing in Saudi Arabia. Over a six month experiment, we find that the open circuit voltage retains its initial value, whereas the fill factor degrades, which is found to have two causes. A first degradation mechanism is linked with ion migration in the perovskite and is largely reversible overnight, though it does induce hysteretic behavior over time. A second, irreversible, mechanism is caused by corrosion of the silver metal top contact with the formation of silver iodide. These findings provide directions for the design of new and more stable perovskite/silicon tandems

Electrochemical lithium (Li) extraction from low-grade salt lake brine, when powered by off-grid renewables, represents a potential approach to meeting the substantially increasing demand for battery-grade Li2CO3. However, this technology has been drastically challenged by the low extraction rate and high production cost, largely due to the lack of research on reactor engineering and system scale-out. Herein, we rationally designed a scalable spiral-microstructured electrochemical reactor (SMER) to accomplish ultrafast and economical Li extraction under harsh brine conditions by virtue of significantly accelerated mass transfer. We showcased that the SMER was stably operated at a Li extraction rate over 5.6 times as much as that of state-of-art devices, and could be up-scaled for commercial production of battery-grade Li2CO3 driven by solar cells. This work lays the ground for sustainable Li extraction from remote low-grade salt lake brine and can be readily applied to more minable Li reserves/resources.

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.

Summary Cost-effective photovoltaics (PVs) require a high energy yield with a long system lifetime. However, both are adversely affected by temperature. Here, we assess the economic impact of thermal effects on PV systems by establishing a temperature-dependent levelized cost of energy (LCOE) model. Using this model, we introduce an equivalent ratio γ (with the unit of absolute efficiency %/K) as a new metric that quantitatively translates the LCOE gain obtained by reducing the module temperature ( T m o d ) to an equivalent absolute power conversion efficiency increase. The substantial value of γ motivates us to investigate the root causes of heating in solar cells and modules, with a focus on crystalline-Si (c-Si) PVs, given its market dominance. To link the heat analysis with T m o d , we establish and validate an opto-electronically coupled thermal model to predict T m o d . This modeling approach enables the quantification of possible ways to mitigate undesired heating effects.

In this work, we present a simple and efficient solution-doping process for preparing high-quality polycrystalline silicon (poly-Si)-based passivating contacts. Commercial phosphorus or boron-doping solutions are spin-coated on crystalline silicon (c-Si) wafers that feature SiO2/poly-Si layers; the doping process is then activated by thermal annealing at high temperatures in a nitrogen atmosphere. With optimized n- and p-type solution doping and thermal annealing, n- and p-type poly-Si passivating contacts featuring simultaneously a low contact recombination parameter (J0c) of 2.4 and 12 fA/cm2 and a low contact resistivity (ρc) of 29 and 20 mΩ·cm2 are achieved, respectively. Taking advantage of the single-sided nature of these solution-doping processes, c-Si solar cells with poly-Si passivating contacts of opposite polarity on the respective wafer surfaces are fabricated using a simple coannealing process, achieving the best power conversion efficiency (PCE) of 18.5% on a planar substrate. Overall, the solution-doping method is demonstrated to be a simple and promising alternative to gas/ion implantation doping for poly-Si passivating-contact manufacturing.

Hole-transporting layers (HTLs) are an essential component in inverted, p-i-n perovskite solar cells (PSCs) where they play a decisive role in extraction and transport of holes, surface passivation, perovskite crystallization, device stability, and cost. Currently, the exploration of efficient, stable, highly transparent and low-cost HTLs is of vital importance for propelling p-i-n PSCs toward commercialization. Compared to their inorganic counterparts, organic HTLs offer multiple advantages such as a tunable bandgap and energy level, easy synthesis and purification, solution processability, and overall low cost. Here, recent progress of organic HTLs, including conductive polymers, small molecules, and self-assembled monolayers, as utilized in inverted PSCs is systematically reviewed and summarized. Their molecular structure, hole-transport properties, energy levels, and relevant device properties and resulting performances are presented and analyzed. A summary of design principles and a future outlook toward highly efficient organic HTLs in inverted PSCs is proposed. This review aims to inspire further innovative development of novel organic HTLs for more efficient, stable, and scalable inverted PSCs.

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.

Three n-type fused lactam semiconducting polymers were synthesized for thermoelectric and transistor applications via a cheap, highly atom-efficient, and nontoxic transition-metal free aldol polycondensation. Energy level analysis of the three polymers demonstrated that reducing the central acene core size from two anthracenes (A-A), to mixed naphthalene-anthracene (A-N), and two naphthalene cores (N-N) resulted in progressively larger electron affinities, thereby suggesting an increasingly more favorable and efficient solution doping process when employing 4-(2,3-dihydro-1,3-dimethyl-1H-benzimidazol-2-yl)-N,N-dimethylbenzenamine (N-DMBI) as the dopant. Meanwhile, organic field effect transistor (OFET) mobility data showed the N-N and A-N polymers to feature the highest charge carrier mobilities, further highlighting the benefits of aryl core contraction to the electronic performance of the materials. Ultimately, the combination of these two factors resulted in N-N, A-N, and A-A to display power factors (PFs) of 3.2 μW m-1 K-2, 1.6 μW m-1 K-2, and 0.3 μW m-1 K-2, respectively, when doped with N-DMBI, whereby the PFs recorded for N-N and A-N are among the highest reported in the literature for n-type polymers. Importantly, the results reported in this study highlight that modulating the size of the central acene ring is a highly effective molecular design strategy to optimize the thermoelectric performance of conjugated polymers, thus also providing new insights into the molecular design guidelines for the next generation of high-performance n-type materials for thermoelectric applications.