Polymer passivation layers can improve the open-circuit voltage of perovskite solar cells when inserted at the perovskite–charge transport layer interfaces. Unfortunately, many such layers are poor conductors, leading to a trade-off between passivation quality (voltage) and series resistance (fill factor, FF). Here, we introduce a nanopatterned electron transport layer that overcomes this trade-off by modifying the spatial distribution of the passivation layer to form nanoscale localized charge transport pathways through an otherwise passivated interface, thereby providing both effective passivation and excellent charge extraction. By combining the nanopatterned electron transport layer with a dopant-free hole transport layer, we achieved a certified power conversion efficiency of 21.6% for a 1-square-centimeter cell with FF of 0.839, and demonstrate an encapsulated cell that retains ~91.7% of its initial efficiency after 1000 hours of damp heat exposure.

Rapid development of both efficiency 1 and stability 2 mean that perovskite solar cells are at the forefront of emerging photovoltaic technologies. State-of-the-art cells exhibit voltage losses 3-8 approaching the theoretical minimum and near-unity internal quantum efficiency 9-13 , but conversion efficiencies are limited by the fill-factor (FF < 83%, below the Shockley-Queisser limit of ~90%). This limitation results from non-ideal charge transport between the perovskite absorber and the cell's electrodes 5,8,13-16 . Reducing the electrical series resistance of charge transport layers is therefore crucial for improving efficiency. Here we introduce a reverse-doping process to fabricate nitrogen-doped titanium oxide electron transport layers with outstanding charge transport performance. By incorporating this charge transport material into perovskite solar cells, we demonstrate 1cm 2 cells with FFs >86%, and an average FF ~ 85.3%. We also report a certified steady-state efficiency record of 22.6% for a 1cm 2 cell (23.33% ± 0.58% from reverse current-voltage scan).Nitrogen-doped titanium oxide (titanium oxynitride, TiO x N y ) has been widely investigated for photocatalysis 17,18 , but rarely in perovskite solar cells (PSCs). PSCs incorporating solution-processed TiO x N y have been reported, but device performances have

Swift heavy-ion irradiation of elemental metal nanoparticles (NPs) embedded in amorphous SiO 2 induces a spherical to rodlike shape transformation with the direction of NP elongation aligned to that of the incident ion. Large, once-spherical NPs become progressively more rodlike while small NPs below a critical diameter do not elongate but dissolve in the matrix. We examine this shape transformation for ten metals under a common irradiation condition to achieve mechanistic insight into the transformation process. Subtle differences are apparent including the saturation of the elongated NP width at a minimum sustainable, metal-specific value. Elongated NPs of lesser width are unstable and subject to vaporization. Furthermore, we demonstrate the elongation process is governed by the formation of a molten ion-track in amorphous SiO 2 such that upon saturation the elongated NP width never exceeds the molten ion-track diameter. Ion-solid interactions during swift heavy-ion irradiation (SHII) are dominated by inelastic processes in the form of electron excitation and ionization while, in contrast, the influence of elastic processes such as ballistic displacements is negligible. Macroscopically, amorphous SiO 2 (a-SiO 2 ) undergoes a volume-conserving anisotropic deformation when subjected to SHII such that thin freestanding layers contract and expand, respectively, in directions parallel and perpendicular to that of the incident ion [1]. The viscoelastic model [2,3], based on a transient thermal effect, successfully explains this so-called ion hammering. Microscopically, energy is deposited along the ion path, from incident ion to matrix electrons, and is then dissipated within a narrow cylinder of material surrounding the ion path. The heat flow in both the electron and lattice subsystems is well described as functions of time and radial distance by the inelastic thermal spike (i-TS) model [4,5]. When the temperature of the lattice exceeds that required for melting, the material along the ion path is molten and upon quenching an ion track is formed. Recently, we measured the molten ion-track diameter in a-SiO 2 as a function of electronic stopping power [6]. The ion-track radial density distribution consisted of an under-dense core and over-dense shell (relative to unirradiated material), the formation of which was attributed to a quenched-in pressure wave emanating from the ion-track center [6].Elemental metal nanoparticles (NPs) embedded in a-SiO 2 and subjected to SHII can undergo an intriguing shape transformation where once-spherical NPs become progressively more rodlike with the direction of elongation aligned along that of the incident ion. This phenomenon has been reported for several metals under a wide range of SHII conditions, with Refs. [7][8][9][10][11][12][13][14][15][16][17] citing selected examples. Freestanding metallic NPs irradiated under comparable conditions do not change shape, demonstrating the embedding a-SiO 2 matrix must have a role in the shape transformation process [8,17]. An unambiguous ...

The challenges of making high performance, low temperature processed, p-type transparent conductors (TCs) have been the main bottleneck for the development of flexible transparent 2 electronics. Though a few p-type transparent conducting oxides (TCOs) have shown promising results, they need high processing temperature to achieve the required conductivity which makes them unsuitable for organic and flexible electronic applications. Copper iodide is a wide band gap p-type semiconductor that can be heavily doped at low temperature (<100 o C) to achieve conductivity comparable or higher than many of the well-established p-type TCOs. However, as processed CuI loses its transparency and conductivity with time in an ambient condition which makes them unsuitable for long term applications. Herein, we propose CuI-TiO2 composite thin films as a replacement of pure CuI. We show that the introduction of TiO2 in CuI makes it more stable in ambient condition while also improving its conductivity and transparency. A detailed comparative analysis between CuI and CuI-TiO2 composite thin films have been performed to understand the reasons for improved conductivity, transparency and stability of CuI-TiO2 samples in comparison to pure CuI samples. The enhanced conductivity in CuI-TiO2 stems from the spacecharge layer formation at the CuI/TiO2 interface, while the improved transparency is due to reduced CuI grain growth mobility in the presence of TiO2. The improved stability of CuI-TiO2 in comparison to pure CuI is a result of inhibited recrystallization and grain growth, reduced loss of iodine and limited oxidation of CuI phase in presence of TiO2. For optimized fraction of TiO2, average transparency of ~78% (in 450-800 nm region) and a resistivity of 14 mΩ.cm is achieved, while maintaining a relatively high mobility of ~3.5 cm 2 V-1 s-1 with hole concentration reaching as high as 1.3 x 10 20 cm-3. Most importantly, this work opens up the possibility to design a new range of p-type transparent conducting materials using CuI/insulator composite system such as CuI/SiO2, CuI/Al2O3, CuI/SiNx, etc.

Despite the fact that non-aqueous uranium chemistry is over 60 years old, most polarised-covalent uranium-element multiple bonds involve formal uranium oxidation states IV, V, and VI. The paucity of uranium(III) congeners is because, in common with metal-ligand multiple bonding generally, such linkages involve strongly donating, charge-loaded ligands that bind best to electron-poor metals and inherently promote disproportionation of uranium(III). Here, we report the synthesis of hexauranium-methanediide nanometre-scale rings. Combined experimental and computational studies suggest overall the presence of formal uranium(III) and (IV) ions, though electron delocalisation in this Kramers system cannot be definitively ruled out, and the resulting polarised-covalent U = C bonds are supported by iodide and δ-bonded arene bridges. The arenes provide reservoirs that accommodate charge, thus avoiding inter-electronic repulsion that would destabilise these low oxidation state metal-ligand multiple bonds. Using arenes as electronic buffers could constitute a general synthetic strategy by which to stabilise otherwise inherently unstable metal-ligand linkages.

The ion beam synthesis of Pb nanoparticles (NPs) in silica is studied in terms of a two step thermal annealing process consisting of a low temperature long time aging treatment followed by a high temperature short time one. The samples are investigated by Rutherford backscattering spectrometry and transmission electron microscopy. The results obtained show that highly stable Pb trapping structures are formed during the aging treatment. These structures only dissociate at high temperatures, inhibiting the nucleation of NPs in the metallic phase and causing an atomic redistribution that renders the exclusive formation of a two dimensional, uniform and dense array of Pb NPs at the silica–silicon interface. The results are discussed on the basis of classic thermodynamic concepts.

Developing durable redox materials with fast and stable redox kinetics under high-temperature operating conditions is a key challenge for an efficient industrial-scale production of synthesis gas via two step solar thermochemical redox cycles. Here, we investigate novel electrospun nanostructured La3+-doped strontium manganites, LSM (La x Sr1–x MnO3, x = 0, 0.25, 0.50, and 1), for an efficient CO production with high redox kinetics. The oxidation behavior of these LSM powders was assessed in terms of oxygen recovery and CO yield via thermogravimetric analysis by using air and CO2 as oxidation medium. Strontium manganate (SrMnO3) shows the highest CO yield per cycle of 854.20 μmol g–1 at a rate of ∼400 μmol g–1 min–1 when reduced at 1400 °C and reoxidized at 1000 °C, with high oxygen exchange capacity in terms of oxygen nonstoichiometry of up to 0.29, during CO2 splitting cycles. However, lanthanum manganite (LaMnO3) demonstrated high yield of CO of 329 μmol g–1 with a rate of 110 μmol min–1 g–1 when reduced at 1000 °C and reoxidized at 700 °C, which is 3 times higher than the yield for SrMnO3 at the same conditions. The oxygen recovery in LSM samples was 4–15% higher during oxidation with air than with CO2. Moreover, the improved structural stability of these nanopowders indicates the potential of electrospinning technique for an up-scale synthesis of oxygen carriers. These findings show that a selective LSM system can be utilized for enhanced CO yield with high kinetics and structural stability at reduction temperatures 1000–1400 °C.

We characterize and discuss the impact of hydrogenation on the performance of phosphorus-doped polycrystalline silicon (poly-Si) films for passivating contact solar cells. Combining various characterization techniques including transmission electron microscopy, energy-dispersive X-ray spectroscopy, low-temperature photoluminescence spectroscopy, quasi-steady-state photoconductance, and Fourier-transform infrared spectroscopy, we demonstrate that the hydrogen content inside the doped poly-Si layers can be manipulated to improve the quality of the passivating contact structures. After the hydrogenation process of poly-Si layers fabricated under different conditions, the effective lifetime and the implied open circuit voltage are improved for all investigated samples (up to 4.75 ms and 728 mV on 1 Ω cm n-type Si substrates). Notably, samples with very low initial passivation qualities show a dramatic improvement from 350 μs to 2.7 ms and from 668 to 722 mV.