Minimizing Interfacial Energy Loss and Volatilization of Formamidinium via Polymer-Assisted D-A supramolecular Self-Assembly Interface for Inverted Perovskite Solar Cells with 25.78% Efficiency.

2D perovskite passivation strategies effectively reduce defect-assisted carrier nonradiative recombination losses on the perovskite surface. Nonetheless, severe energy losses are causing by carrier thermalization, interfacial nonradiative recombination, and conduction band offset still persist at heterojunction perovskite/PCBM interfaces, which limits further performance enhancement of inverted heterojunction PSCs. Here, 5,10,15,20-tetrakis(pentafluorophenyl)porphyrin (5FTPP) is introduced between 3D/2D perovskite heterojunction and PCBM. Compared to tetraphenylporphyrin without electron-withdrawing fluoro-substituents, 5FTPP can self-assemble with PCBM at interface into donor-acceptor (D-A) complex with stronger supramolecular interaction and lower energy transfer losses. This rapid energy transfer from donor (5FTPP) to acceptor (PCBM) within femtosecond scale is demonstrated to enlarge hot carrier extraction rates and ranges, reducing thermalization losses. Furthermore, the incorporation of polystyrene derivative (PD) reinforces D-A interaction by inhibiting self-π-π stacking of 5FTPP, while fine-tuning conduction band offset and suppressing interfacial nonradiative recombination via Schottky barrier, dipole, and n-doping. Notably, the multidentate anchoring of PD-5FTPP with FA+, Pb2+, and I- mitigates the adverse effects of FA+ volatilization during thermal stress. Ultimately, devices with PD-5FTPP achieve a power conversion efficiency of 25.78% (certified: 25.36%), maintaining over 90% of initial efficiency after 1000 h of continuous illumination at the maximum power point (65 °C) under ISOS-L-2 protocol.

Sequentially Processed Bulk-Heterojunction-Buried Structure for Efficient Organic Solar Cells with 500 nm Thickness.

Large-area printing fabrication is a distinctive feature of organic solar cells (OSCs). However, the advance of upscalable fabrication is challenged by the thickness of organic active layers considering the importance of both exciton dissociation and charge collection. In this work, a bulk-heterojunction-buried (buried-BHJ) structure is introduced by sequential deposition to realize efficient exciton dissociation and charge collection, thereby contributing to efficient OSCs with 500 nm thick active layers. The buried-BHJ distributes donor and acceptor phases in the vertical direction as charge transport channels, while numerous BHJ interfaces are buried in each phase to facilitate exciton dissociation simultaneously. It is found that buried-BHJ configurations possess efficient exciton dissociation and rapid charge transport, resulting in reduced recombination losses. In comparison with traditional structures, the buried-BHJ structure displays a decent tolerance to film thickness. In particular, a power conversion efficiency of 16.0% is achieved with active layers at a thickness of 500 nm. To the best of the authors' knowledge, this represents the champion efficiency of thick film OSCs.

Synergetic Regulation of Interface Defects and Carriers Dynamics for High-Performance Lead-Free Perovskite Solar Cells.

Severe nonradiative recombination and open-circuit voltage loss triggered by high-density interface defects greatly restrict the continuous improvement of Sn-based perovskite solar cells (Sn-PVSCs). Herein, a novel amphoteric semiconductor, O-pivaloylhydroxylammonium trifluoromethanesulfonate (PHAAT), is developed to manage interface defects and carrier dynamics of Sn-PVSCs. The amphiphilic ionic modulators containing multiple Lewis-base functional groups can synergistically passivate anionic and cationic defects while coordinating with uncoordinated Sn2+ to compensate for surface charge and alleviate the Sn2+ oxidation. Especially, the sulfonate anions raise the energy barrier of surface oxidation, relieve lattice distortion, and inhibit nonradiative recombination by passivating Sn-related and I-related deep-level defects. Furthermore, the strong coupling between PHAAT and Sn perovskite induces the transition of the surface electronic state from p-type to n-type, thus creating an extra back-surface field to accelerate electron extraction. Consequently, the PHAAT-treated device exhibits a champion efficiency of 13.94% with negligible hysteresis. The device without any encapsulation maintains 94.7% of its initial PCE after 2000 h of storage and 91.6% of its initial PCE after 1000 h of continuous illumination. This work provides a reliable strategy to passivate interface defects and construct p-n homojunction to realize efficient and stable Sn-based perovskite photovoltaic devices.

Different Morphology Dependence for Efficient Indoor Organic Photovoltaics: The Role of the Leakage Current and Recombination Losses.

Efficient indoor organic photovoltaics (OPVs) have attracted strong attention for their application in indoor electronic devices. However, the route to optimal photoactive film morphology toward high-performance indoor devices has remained obscure. The leakage current dominated by morphology exerts distinguishing influence on the performance under different illuminations. We have demonstrated that morphology reoptimization plays an important role in indoor OPVs, and their optimal structural features are different from what we laid out for outdoor devices. For indoor OPVs, in order to facilitate low leakage current, it is essential to enhance the crystallinity, phase separation, and domain purity, as well as keeping small surface roughness of the active layer. Furthermore, considering the reduced bimolecular recombination at low light intensity, we have shown that PM6:M36-based indoor devices can work effectively with a large ratio of the donor and acceptor. Our work correlating structure-performance relation and the route to optimal morphology outlines the control over device leakage current and recombination losses boosting the progress of efficient indoor OPVs.

A Narrow-Bandgap n-Type Polymer with an Acceptor-Acceptor Backbone Enabling Efficient All-Polymer Solar Cells.

Narrow-bandgap polymer semiconductors are essential for advancing the development of organic solar cells. Here, a new narrow-bandgap polymer acceptor L14, featuring an acceptor-acceptor (A-A) type backbone, is synthesized by copolymerizing a dibrominated fused-ring electron acceptor (FREA) with distannylated bithiophene imide. Combining the advantages of both the FREA and the A-A polymer, L14 not only shows a narrow bandgap and high absorption coefficient, but also low-lying frontier molecular orbital (FMO) levels. Such FMO levels yield improved electron transfer character, but unexpectedly, without sacrificing open-circuit voltage (Voc ), which is attributed to a small nonradiative recombination loss (Eloss,nr ) of 0.22 eV. Benefiting from the improved photocurrent along with the high fill factor and Voc , an excellent efficiency of 14.3% is achieved, which is among the highest values for all-polymer solar cells (all-PSCs). The results demonstrate the superiority of narrow-bandgap A-A type polymers for improving all-PSC performance and pave a way toward developing high-performance polymer acceptors for all-PSCs.

Improving Efficiency and Stability in Quasi-2D Perovskite Light-Emitting Diodes by a Multifunctional LiF Interlayer.

Owing to the enlarged exciton binding energy and the ability to confine charge carriers compared to their three-dimensional (3D) counterparts, research on quasi-two-dimensional (quasi-2D) perovskite materials and the correlative application in light-emitting diodes (LEDs) has attracted considerable attention. However, high density of defects, exciton emission trapping, and unbalanced charge injection are still the main intractable obstacles to their further development and practical application. Herein, we report an efficient multifunctional interlayer, lithium fluoride (LiF), to boost the performance of green-emitting quasi-2D perovskite LEDs (PeLEDs) by simultaneously overcoming the aforementioned issues. The introduced LiF interlayer not only eliminates the defects at perovskite grain boundaries and the surface by reinforcing the chemical bonds with uncoordinated lead ions but also restrains the emission of perovskite from quenching triggered by the electron transport layer and reduces excess electron injections to effectively balance carriers in the device. As a result, the resulting green quasi-2D PeLED shows a maximum external quantum efficiency of 16.35%, which is the best value obtained for quasi-2D perovskite-based LEDs reported so far, with simultaneous improvement in the operating lifetime of the device.

Gradient Engineered Light Absorption Layer for Enhanced Carrier Separation Efficiency in Perovskite Solar Cells.

Carrier transport behavior in the perovskite light absorption layer significantly impacts the performance of perovskite solar cells (PSCs). In this work, reduced carrier recombination losses were achieved by the design of a band structure in perovskite materials. An ultrathin (PbI2/PbBr2)n film with a gradient thickness ratio was deposited as the lead halide precursor layer by a thermal evaporation method, and PSCs with a gradient band structure in the perovskite absorption layer were fabricated by a two-step method in ambient atmosphere. For comparison, PSCs with homogeneous perovskite materials of MAPbI3 and MAPbIxBr3 - x were fabricated as well. It is found that the gradient type-II band structure greatly reduces the carrier lifetime and enhances the carrier separation efficiency. As a result, the PSCs with a gradient band structure exhibit an average power conversion efficiency of 17.5%, which is 1-2% higher than that of traditional PSCs. This work provides a novel method for developing high-efficiency PSCs.

VHEE beam dosimetry at CERN Linear Electron Accelerator for Research under ultra-high dose rate conditions.

The aim of this work is the dosimetric characterization of a plane parallel ionization chamber under defined beam setups at the CERN Linear Electron Accelerator for Research (CLEAR). A laser driven electron beam with energy of 200 MeV at two different field sizes of approximately 3.5 mm FWHM and approximately 7 mm FWHM were used at different pulse structures. Thereby the dose-per-pulse range varied between approximately 0.2 and 12 Gy per pulse. This range represents approximately conventional dose rate range beam conditions up to ultra-high dose rate (UHDR) beam conditions. The experiment was based on a water phantom which was integrated into the horizontal beamline and radiochromic films and an Advanced Markus ionization chamber was positioned in the water phantom. In addition, the experimental setup were modelled in the Monte Carlo simulation environment FLUKA. In a first step the radiochromic film measurements were used to verify the beamline setup. Depth dose distributions and dose profiles measured by radiochromic film were compared with Monte Carlo simulations to verify the experimental conditions. Second, the radiochromic films were used for reference dosimetry to characterize the ionization chamber. In particular, polarity effects and the ion collection efficiency of the ionization chamber were investigated for both field sizes and the complete dose rate range. As a result of the study, significant polarity effects and recombination loss of the ionization chamber were shown and characterized. However, the work shows that the behavior of the ionization chamber at the laser driven beam line at the CLEAR facility is comparable to classical high dose-per-pulse electron beams. This allows the use of ionization chambers on the CLEAR system and thus enables active dose measurement during the experiment. Compared to passive dose measurement with film, this is an important step forward in the experimental equipment of the facility.