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Solid-state dye-sensitized solar cells currently suffer from issues such as inadequate nanopore filling, low conductivity and crystallization of hole-transport materials infiltrated in the mesoscopic TiO 2 scaffolds, leading to low performances. Here we report a record 11% stable solid-state dye-sensitized solar cell under standard air mass 1.5 global using a hole-transport material composed of a blend of [Cu (4,4′,6,6′-tetramethyl-2,2′-bipyridine) 2 ](bis(trifluoromethylsulfonyl)imide) 2 and [Cu (4,4′,6,6′-tetramethyl-2,2′-bipyridine) 2 ](bis(trifluoromethylsulfonyl)imide). The amorphous Cu(II/I) conductors that conduct holes by rapid hopping infiltrated in a 6.5 μm-thick mesoscopic TiO 2 scaffold are crucial for achieving such high efficiency. Using time-resolved laser photolysis, we determine the time constants for electron injection from the photoexcited sensitizers Y123 into the TiO 2 and regeneration of the Y123 by Cu(I) to be 25 ps and 3.2 μs, respectively. Our work will foster the development of low-cost solid-state photovoltaic based on transition metal complexes as hole conductors. Inadequate pore infiltration and low conductivity of hole transporter materials limit the performance of solid-state dye-sensitized solar cells. Using fast charge-exchange Cu(II/I) complexes as part of the hole transporting material, Cao et al . overcome these issues to achieve a record photoconversion efficiency of 11%.

The high conversion efficiency has made metal halide perovskite solar cells a real breakthrough in thin film photovoltaic technology in recent years. Here, we introduce a straightforward strategy to reduce the level of electronic defects present at the interface between the perovskite film and the hole transport layer by treating the perovskite surface with different types of ammonium salts, namely ethylammonium, imidazolium and guanidinium iodide. We use a triple cation perovskite formulation containing primarily formamidinium and small amounts of cesium and methylammonium. We find that this treatment boosts the power conversion efficiency from 20.5% for the control to 22.3%, 22.1%, and 21.0% for the devices treated with ethylammonium, imidazolium and guanidinium iodide, respectively. Best performing devices showed a loss in efficiency of only 5% under full sunlight intensity with maximum power tracking for 550 h. We apply 2D- solid-state NMR to unravel the atomic-level mechanism of this passivation effect. Various approaches have been developed to push higher the efficiency of halide perovskite solar cells. Here Alharbi et al. show that ammonium salts treatment can reduce the defect density at the perovskite surface and understand the passivation mechanism with 2D-solid state NMR.

To develop photosensitizers with high open-circuit photovoltage (V ) is a crucial strategy to enhance the power conversion efficiency (PCE) of co-sensitized solar cells. Here, we show a judiciously tailored organic photosensitizer, coded MS5, featuring the bulky donor N-(2',4'-bis(dodecyloxy)-[1,1'-biphenyl]-4-yl)-2',4'-bis(dodecyloxy)-N-phenyl-[1,1'-biphenyl]-4-amine and the electron acceptor 4-(benzo[c][1,2,5]thiadiazol-4-yl)benzoic acid. Employing MS5 with a copper (II/I) electrolyte enables a dye-sensitized solar cell (DSC) to achieve a strikingly high V of 1.24 V, with the V deficit as low as 130 mV and an ideality factor of merely 1.08. The co-sensitization of MS5 with the wider spectral-response dye XY1b produces a highly efficient and stable DSC with the PCE of 13.5% under standard AM1.5 G, 100 mW cm solar radiation. Remarkably, the co-sensitized solar cell (active area of 2.8 cm ) presents a record PCE of 34.5% under ambient light, rendering it very attractive as an ambient light harvesting energy source for low power electronics.

Lead halide perovskites have recently been used as light absorbers in hybrid organic–inorganic solid-state solar cells, with efficiencies as high as 15% and open-circuit voltages of 1 V. However, a detailed explanation of the mechanisms of operation within this photovoltaic system is still lacking. Here, we investigate the photoinduced charge transfer processes at the surface of the perovskite using time-resolved techniques. Transient laser spectroscopy and microwave photoconductivity measurements were applied to TiO 2 and Al 2 O 3 mesoporous films impregnated with CH 3 NH 3 PbI 3 perovskite and the organic hole-transporting material spiro -OMeTAD. We show that primary charge separation occurs at both junctions, with TiO 2 and the hole-transporting material, simultaneously, with ultrafast electron and hole injection taking place from the photoexcited perovskite over similar timescales. Charge recombination is shown to be significantly slower on TiO 2 than on Al 2 O 3 films. Perovskite solar cells are currently generating great interest in the photovoltaics community, but a detailed understanding of why they are so efficient is lacking. Femtosecond laser spectroscopy and microwave photoconductivity measurements now reveal important insights into the photoinduced charge transfer processes and dynamics of such cells.

Dye-sensitized solar cells (DSCs) have achieved impressive conversion efficiencies for solar energy of over 11% with an electrolyte that contains triiodide/iodide as a redox couple. Although triiodide/iodide redox couples work efficiently in DSCs, they suffer from two major disadvantages: electrolytes that contain triiodide/iodide corrode electrical contacts made of silver (which reduces the options for the scale up of DSCs to module size) and triiodide partially absorbs visible light. Here, we present a new disulfide/thiolate redox couple that has negligible absorption in the visible spectral range, a very attractive feature for flexible DSCs that use transparent conductors as current collectors. Using this novel, iodide-free redox electrolyte in conjunction with a sensitized heterojunction, we achieved an unprecedented efficiency of 6.4% under standard illumination test conditions. This novel redox couple offers a viable pathway to develop efficient DSCs with attractive properties for scale up and practical applications. Although the triiodide/iodide redox couple works efficiently in dye-sensitized solar cells it restricts functionality by absorbing visible light. Now, a disulfide/thiolate redox couple that has negligible absorption in the visible spectral range is presented, which in conjunction with a sensitized heterojunction, displays an efficiency of 6.4% under standard illumination test conditions.

Dye-sensitized solar cells are a promising alternative to traditional inorganic semiconductor-based solar cells. Here we report an open-circuit voltage of over 1,000 mV in mesoscopic dye-sensitized solar cells incorporating a molecularly engineered cobalt complex as redox mediator. Cobalt complexes have negligible absorption in the visible region of the solar spectrum, and their redox properties can be tuned in a controlled fashion by selecting suitable donor/acceptor substituents on the ligand. This approach offers an attractive alternate to the traditional I 3 − /I − redox shuttle used in dye-sensitized solar cells. A cobalt complex using tridendate ligands [Co(bpy-pz) 2 ] 3+/2+ (PF 6 ) 3/2 as redox mediator in combination with a cyclopentadithiophene-bridged donor-acceptor dye (Y123), adsorbed on TiO 2 , yielded a power conversion efficiency of over 10% at 100 mW cm −2 . This result indicates that the molecularly engineered cobalt redox shuttle is a legitimate alternative to the commonly used I 3 − /I − redox shuttle. Dye-sensitized solar cells are a promising alternative to traditional inorganic semiconductor-based solar cells. Yum et al . use a molecularly engineered cobalt complex as a redox mediator to achieve an open-circuit voltage of over 1,000 mV in a mesoscopic dye-sensitized solar cell.

There has been long-standing debate on how free charges are generated in donor:acceptor blends that are used in organic solar cells, and which are generally comprised of a complex phase morphology, where intermixed and neat phases of the donor and acceptor material co-exist. Here we resolve this question, basing our conclusions on Stark effect spectroscopy data obtained in the absence and presence of externally applied electric fields. Reconciling opposing views found in literature, we unambiguously demonstrate that the fate of photogenerated electron–hole pairs—whether they will dissociate to free charges or geminately recombine—is determined at ultrafast times, despite the fact that their actual spatial separation can be much slower. Our insights are important to further develop rational approaches towards material design and processing of organic solar cells, assisting to realize their purported promise as lead-free, third-generation energy technology that can reach efficiencies over 10%. Charge generation and transport are crucial to the performance of organic solar cells, but the mechanism remains controversial. Causa’ et al . show that the phase morphology of polymer:fullerene blends determines the exciton dissociation at femtoseconds, although the spatial separation can occur at picoseconds.

Solar cells that operate efficiently under indoor lighting are of great practical interest as they can serve as electric power sources for portable electronics and devices for wireless sensor networks or the Internet of Things. Here, we demonstrate a dye-sensitized solar cell (DSC) that achieves very high power-conversion efficiencies (PCEs) under ambient light conditions. Our photosystem combines two judiciously designed sensitizers, coded D35 and XY1, with the copper complex Cu( II/I )(tmby) as a redox shuttle (tmby, 4,4′,6,6′-tetramethyl-2,2′-bipyridine), and features a high open-circuit photovoltage of 1.1 V. The DSC achieves an external quantum efficiency for photocurrent generation that exceeds 90% across the whole visible domain from 400 to 650 nm, and achieves power outputs of 15.6 and 88.5 μW cm –2 at 200 and 1,000 lux, respectively, under illumination from a model Osram 930 warm-white fluorescent light tube. This translates into a PCE of 28.9%. A dye-sensitized solar cell that has been designed for efficient operation under indoor lighting could offer a convenient means for powering the Internet of Things.

The stability of hybrid organic–inorganic halide perovskite semiconductors remains a significant obstacle to their application in photovoltaics. To this end, the use of low‐dimensional (LD) perovskites, which incorporate hydrophobic organic moieties, provides an effective strategy to improve their stability, yet often at the expense of their performance. To address this limitation, supramolecular engineering of noncovalent interactions between organic and inorganic components has shown potential by relying on hydrogen bonding and conventional van der Waals interactions. Here, the capacity to access novel LD perovskite structures that uniquely assemble through unorthodox S‐mediated interactions is explored by incorporating benzothiadiazole‐based moieties. The formation of S‐mediated LD structures is demonstrated, including one‐dimensional (1D) and layered two‐dimensional (2D) perovskite phases assembled via chalcogen bonding and S–π interactions. This involved a combination of techniques, such as single crystal and thin film X‐ray diffraction, as well as solid‐state NMR spectroscopy, complemented by molecular dynamics simulations, density functional theory calculations, and optoelectronic characterization, revealing superior conductivities of S‐mediated LD perovskites. The resulting materials are applied in n‐i‐p and p‐i‐n perovskite solar cells, demonstrating enhancements in performance and operational stability that reveal a versatile supramolecular strategy in photovoltaics. A new generation of low‐dimensional hybrid halide perovskite materials assembled via chalcogen bonding and S–π interactions is demonstrated by a combination of techniques, including X‐ray diffraction and solid‐state nuclear magnetic resonance spectroscopy, complemented by molecular dynamics simulations, density functional theory calculations, and optoelectronic characterization, revealing superior conductivities and enhancements in performance and operational stabilities in perovskite solar cells.

One of the most salient features of hybrid lead halide perovskites is the extended lifetime of their photogenerated charge carriers. This property has now been shown experimentally to originate from a slow, thermally activated recombination process.