Interface Reactive Sputtering of Transparent Electrode for High-Performance Monolithic and Stacked Perovskite Tandem Solar Cells.

Sputtered indium tin oxide (ITO) fulfills the requirements of top transparent electrodes (TTEs) in semitransparent perovskite solar cells (PSCs) and stacked tandem solar cells (TSCs), as well as of the recombination layers in monolithic TSCs. However, the high-energy ITO particles will cause damage to the devices. Herein, the interface reactive sputtering strategy is proposed to construct cost-effective TTEs with high transmittance and excellent carrier transporting ability. Polyethylenimine (PEI) is chosen as the interface reactant that can react with sputtered ITO nanoparticles, so that, coordination compounds can be formed during the deposition process, facilitating the carrier transport at the interface of C60/PEI/ITO. Besides, the impact force of energetic ITO particles is greatly alleviated, and the intactness of the underlying C60 layer and perovskite layer is guaranteed. Thus, the prepared semitransparent subcells achieve a significantly enhanced power conversion efficiency (PCE) of 19.17%, surpassing those based on C60/ITO (11.64%). Moreover, the PEI-based devices demonstrate excellent storage stability, which maintains 98% of their original PCEs after 2000 h. On the strength of the interface reactive sputtering ITO electrode, a stacked all-perovskite TSC with a PCE of 26.89% and a monolithic perovskite-organic TSC with a PCE of 24.33% are successfully fabricated.

Onion-like multicolor thermally activated delayed fluorescent carbon quantum dots for efficient electroluminescent light-emitting diodes.

Carbon quantum dots are emerging as promising nanomaterials for next-generation displays. The elaborate structural design is crucial for achieving thermally activated delayed fluorescence, particularly for improving external quantum efficiency of electroluminescent light-emitting diodes. Here, we report the synthesis of onion-like multicolor thermally activated delayed fluorescence carbon quantum dots with quantum yields of 42.3-61.0%. Structural, spectroscopic characterization and computational studies reveal that onion-like structures assembled from monomer carbon quantum dots of different sizes account for the decreased singlet-triplet energy gap, thereby achieving efficient multicolor thermally activated delayed fluorescence. The devices exhibit maximum luminances of 3785-7550 cd m-2 and maximum external quantum efficiency of 6.0-9.9%. Importantly, owing to the weak van der Waals interactions and adequate solution processability, flexible devices with a maximum luminance of 2554 cd m-2 are realized. These findings facilitate the development of high-performance carbon quantum dots-based electroluminescent light-emitting diodes that are promising for practical applications.

One-Step Extrusion Preparation for Low-Cost Multicolored Carbon Dot Fluorescent Films.

Carbon dots (CDs), an emerging class of environmentally friendly luminescent materials, have been extensively applied in full-color display of light-emitting diodes (LEDs). However, the synthesis of CDs usually requires high pressure, and the conventional preparation of CD-based LED films involves intricate manufacturing techniques. The resulting security risk and high cost restrict the further application of CD-based LEDs. Here, we present a cost-effective method to obtain CD-based LED films via in situ extrusion in a twin-screw extruder. By fine-tuning the extrusion temperature, we created blue-emitting LEDs. The resulting fluorescent films exhibited remarkable stability, retaining 94% fluorescence intensity after 180 days of storage. We also prepared yellow, pure white, and cool white LEDs with malleable shapes, validating the versatility of the in situ extrusion method. More importantly, the manufacturing cost for CD-based films amounts to only about 0.8 RMB/g, which is substantially lower than that of the reported preparation methods. This work offers a cost-effective, safe, and massive approach to preparing photoluminescent LEDs, paving the way for the development of more sustainable and efficient CD-based LEDs.

Research Advances of Nonfused Ring Acceptors for Organic Solar Cells.

The last few decades have witnessed the rapid development of organic solar cells (OSCs). High power conversion efficiencies (PCEs) of over 19% have been successfully achieved due to the emergence of fused-ring acceptors (FRAs). However, the high complexity and low yield for the material synthesis result in high production costs of FRAs, limiting the further commercial application of OSCs. In contrast, nonfused ring acceptors (NFRAs) with the merits of facile synthesis, high yield, and preferable stability can promote the development of low-cost OSCs. Currently, the PCEs of NFRAs-based OSCs have exceeded 17%, which is expected to reach efficiency comparable to that of the FRAs-based OSCs. This review describes the advantages of the recent advances in NFRAs, which emphasizes exploring how the chemical structures of NFRAs influence molecular conformation, aggregation, and packing modes. In addition, the further development of NFRA materials is prospected from molecular design, morphological control, and stability perspectives.

Bright Blue Emission Lead-Free Halides with Narrow Bandwidth Enabled by Oversaturated Europium Doping.

Eu2+-based lead-free metal halide nanocrystals (LFMH NCs), including CsEuCl3 NCs and CsX:Eu2+ NCs (X = Cl or Br), exhibit highly efficient narrow-band blue photoluminescence, making them competitive candidates for next-generation lighting and displays. However, the growing mechanism of the aforementioned NCs lacks in-depth study, which hinders the development of Eu2+-based nanomaterials. Herein, we demonstrate the colloidal synthesis of CsBr:Eu2+ NCs based on an air-stable europium source. The NCs show deep blue photoluminescence centered at 444 nm, with a maximum photoluminescence quantum yield (PLQY) reaching 53.4% and a fwhm of 30 nm. We further reveal the mechanism that determines CsBr host growth and Eu2+ doping in CsBr:Eu2+ nanocrystals, especially dopant trapping and self-purification, that determine the PLQY level. Pure white, warm white, and cold white LEDs are fabricated based on CsBr:Eu2+ NCs, red and green phosphors, and their performance suits the needs of high-quality lighting.

Facile Hydrogen-Bonding Assisted Crystallization Modulation for Large-area High-quality CsPbI2 Br Films and Efficient Solar Cells.

The thermally stable inorganic cesium-based perovskites promise efficient and stable photovoltaics. Unfortunately, the strong ionic bonds lead to uncontrollable rapid crystallization, making it difficult in fabricating large-area black-phase film for photovoltaics. Herein, we developed a facile hydrogen-bonding assisted strategy for modulating the crystallization of CsPbI2 Br to achieve uniform large-area phase-pure films with much-reduced defects. The simple addition of methylamine acetate in precursors not only promotes the formation of intermediate phase via hydrogen bonding to circumvent the direct crystallization of CsPbI2 Br from ionic precursors but also widens the film processing window, thus enabling to fabricate large-area high-quality phase-pure CsPbI2 Br film under benign conditions. Combining with stable dopant-free poly(3-hexylthiophene), the CsPbI2 Br solar cells achieve the record-high efficiencies of 18.14 % and 16.46 % for 0.1 cm2 and 1 cm2 active area, respectively. The obtained high efficiency of 38.24 % under 1000 lux illumination suggests its potential in indoor photovoltaics for powering the Internet of Things, etc.

Transparent Recombination Electrode with Dual-Functional Transport and Protective Layer for Efficient and Stable Monolithic Perovskite/Organic Tandem Solar Cells.

Rational selection and design of recombination electrodes (RCEs) are crucial to enhancing the power conversion efficiency (PCE) and stability of monolithic tandem solar cells (TSCs). Sputtered indium tin oxide (ITO) with high conductivity and excellent transmittance is introduced as RCE in perovskite/organic TSCs. To prevent high-energy ITO particles destroy the underlying material during sputtering, dual-functional transport and protective layer (C1) is employed. The styryl group in C1 can be thermally crosslinked to serve as a sputtering protective layer. Meanwhile, the conjugated phenanthroline skeleton in C1 shows high electron mobility and hole blocking capability to promote the electron transport process at the interfaces and effectively reduce charge accumulation. Monolithic perovskite/organic TSC with high PCE of 24.07% and excellent stability is demonstrated by stacking a 1.77 eV bandgap perovskite layer and a 1.35 eV bandgap organic active layer. This strategy provides new insights for overcoming the fundamental efficiency limits of single-junction devices and promotes the further development of TSC devices.

Interface Modification Using Li-Doped Hollow Titania Nanospheres for High-Performance Planar Perovskite Solar Cells.

Titania nanospheres have been utilized as building blocks of electron transporting layers (ETLs) for mesoscopic perovskite solar cells (PSCs). Nevertheless, the power conversion efficiencies (PCEs) reported so far for the mesoscopic PSCs containing titania nanospheres are generally lower than those of the state-of-the-art planar PSCs. Here, we have prepared Li-doped hollow titania nanospheres (Li-HTS) through a "cation-exchange" approach and used them for the first time to modify the SnO2 ETL/perovskite interfaces of planar PSCs. The Li-HTS-modified PSC delivered a PCE of 23.28% with a fill factor (FF) of over 80%, which is significantly higher than the PCE of the control device (20.51%). This is the best PCE achieved for PSCs containing titania nanospheres. Moreover, interfacial modification using Li-HTS greatly improves the stability of the PSCs. This work demonstrates the potential of interface modification using inorganic nanostructures for enhancing the efficiency and stability of planar PSCs.

Thermodynamic Phase Transition of Three-Dimensional Solid Additives Guiding Molecular Assembly for Efficient Organic Solar Cells.

Fine-tuning the thermodynamic self-assembly of molecules via volatile solid additives has emerged to be an effective way to construct high-performance organic solar cells. Here, three-dimensional structured solid molecules have been designed and applied to facilitate the formation of organized molecular assembly in the active layer. By means of systematic theory analyses and film-morphology characterizations based on four solid candidates, we preselected the optimal one, 4-fluoro-N,N-diphenylaniline (FPA), which possesses good volatility and strong charge polarization. The three-dimensional solids can induce molecular packing in active layers via strong intermolecular interactions and subsequently provide sufficient space for the self-reassembly of active layers during the thermodynamic transition process. Benefitting from the optimized morphology with improved charge transport and reduced energy disorder in the FPA-processed devices, high efficiencies of over 19 % were achieved. The strategy of three-dimensional additives inducing ordered self-assembly structure represents a practical approach for rational morphology control in highly efficient devices, contributing to deeper insights into the structural design of efficient volatile solid additives.

Managing Interfacial Charged Defects with Multiple Active Sited Macrocyclic Valinomycin for Efficient and Stable Inverted Perovskite Solar Cells.

The unavoidably positively and negatively charged defects at the interface between perovskite and electron transport layer (ETL) often lead to severe surface recombination and unfavorable energy level alignment in inverted perovskite solar cells (PerSCs). Inserting interlayers at this interface is an effective approach to eliminate charged defects. Herein, the macrocyclic molecule valinomycin (VM) with multiple active sites of ─C═O, ─NH, and ─O─ is employed as an interlayer at the perovskite/ETL contact to simultaneously eliminate positively and negatively charged defects. Combined with a series of theoretical calculations and experimental analyzes, it is demonstrated that the ─C═O and ─O─ groups in VM can immobilize the uncoordinated Pb2+ to manage the positively charged defect and the formation of N─H···I hydrogen bonding can recompense the formamidine vacancies to eliminate the negatively charged defect. In addition, the VM interlayer induces a favorable downshift band bending at the perovskite/ETL interface, facilitating charge separation and boosting charge transfer. Thanks to the reduced charged defects and favorable energy level alignment, the fabricated inverted PerSC delivers an outstanding power conversion efficiency of 24.06% with excellent long-term ambient and thermal stability. This work demonstrates that managing charged defects via multiple functional groups and simultaneously regulating energy level alignment is a reliable strategy to boost the performance of PerSCs.

Hexachlorotriphosphazene-assisted buried interface passivation for stable and efficient wide-bandgap perovskite solar cells.

Large open-circuit voltage (Voc) loss is the main issue limiting the efficiency improvement in wide bandgap perovskite solar cells (PerSCs). Herein, a facile buried interface treatment by hexachlorotriphosphazene is developed to suppress the Voc loss. The PerSCs include a [Cs0.22FA0.78Pb(I0.85Br0.15)3]0.97(MAPbCl3)0.03 (1.67 eV) absorber and deliver an efficiency of 21.47% and a Voc of 1.21 V (Voc loss of 0.46 V). More importantly, the unencapsulated PerSCs maintain 90% of the initial efficiency after aging 500 h in N2.

Color-stable blue light-emitting diodes with defect management by sulfonate.

Utilizing bromine-based quasi-two-dimensional (quasi-2D) perovskite is a feasible strategy to achieve efficient and stable blue perovskite light-emitting diodes (PeLEDs). However, dimension discretization is prone to emerge due to the irregular phase distribution and massive defects in the perovskite system. Here, we introduce alkali-salt to modulate the phase distribution for reducing the n = 1 phase and propose a novel Lewis base to serve as a passivating agent to decrease defects. This revealed that the external quantum efficiency (EQE) dramatically improves due to the suppression of severe non-radiative recombination losses. Consequently, efficient blue PeLEDs were obtained with a peak EQE of 3.82% located at 487 nm.

Triphenylamine-Derived Solid-State Emissive Carbon Dots for Multicolor High-Efficiency Electroluminescent Light-Emitting Diodes.

Two kinds of triphenylamine-derived solid-state emissive carbon dots (CDs) with orange and yellow color are facilely synthesized through solvothermal treatment, taking advantage of the nonplanar structure and good carrier mobility of triphenylamine unit. Theoretical calculations show that the triphenylamine structure could greatly inhibit the direct π-π stacking of aromatic skeletons and enhance the fluorescence properties of CDs in aggregation state. By adopting the CDs as single emissive layer, high-performance orange-color and green-color electroluminescent light-emitting diodes (LEDs) are successfully fabricated, with maximum brightness of 9450/4236 cd m-2 , high current efficiency of 1.57/2.34 cd A-1 and low turn-on voltage of 3.1/3.6 eV are respectively achieved. Significantly, white-color LED device is further prepared. This work provides a universal platform for the construction of novel solid-state emissive CDs with significant applications in photoelectric device.

Intense Circularly Polarized Fluorescence and Room-Temperature Phosphorescence in Carbon Dots/Chiral Helical Polymer Composite Films.

Chiral carbon dots (C-dots) with a circularly polarized fluorescence (CPF) property have attracted tremendous attention due to their significant applications in chiral optoelectronics and theranostics. However, constructing circularly polarized room-temperature phosphorescent (CPRTP) C-dots remains a great challenge. Herein, a strategy is established to achieve efficient CPF and CPRTP emissions in C-dots/chiral helical polymer bilayer composite film. Taking advantage of the chiral filter effect of chiral helical polymer, intense CPF and CPRTP emissions with large dissymmetric factors up to 1.4 × 10-1 and 1.2 × 10-2 are respectively obtained, even though there is only a simple interface contact between the C-dots layer and the chiral helical polymer layer. More importantly, white-color CPF emission and multiple information display and encryption are further realized based on the prepared chiral luminescent composite films.

Carbon Quantum Dots with Near-Unity Quantum Yield Bandgap Emission for Electroluminescent Light-Emitting Diodes.

Carbon quantum dots (CQDs) feature bright and tunable photoluminescence, solution processability, and low toxicity, showing great potential in optoelectronics. However, the large-scale synthesis of CQDs with near-unity photoluminescence quantum yield (PLQY) has not been achieved so far. In this study, we perform radical-assisted synthesis of hexagon-shaped CQDs (H-CQDs) delivering near-unity PLQY (96 %). Experimental and theoretical analyses revealed that the large vertically oriented transition dipole moment of H-CQDs originating from high symmetry results in nearly 100 % PLQY. The H-CQDs also exhibited a high electron mobility of up to 0.07 cm2  V-1 s-1 . These properties enable the H-CQD-based light-emitting diodes with a high external quantum efficiency of 4.6 % and a record maximum brightness of over 11 000 cd m-2 . This study represents a significant advance that CQDs-based electroluminescent device can be utilized for potential display and lighting applications.

Gram-Scale Room-Temperature Synthesis of Solid-State Fluorescent Carbon Nanodots for Bright Electroluminescent Light Emitting Diodes.

The reaction conditions of high temperature and high pressure will introduce structural defects, high energy consumption, and security risks, severely hindering the industrial application of organic carbon nanodots (CDs). Moreover, the aggregation caused quenching effect also fundamentally limits the CDs based electroluminescent light emitting diodes (LEDs). Herein, for the first time, a rapid one-step room temperature synthetic strategy is introduced to prepare highly emissive solid-state-fluorescent CDs (RT-CDs). A strong oxidizing agent, potassium periodate (KIO4 ), is adopted as a catalyst to facilitate the cyclization of o-phenylenediamine and 4-dimethylamino phenol in aqueous solution at room temperature for only 5 min. The resultant organic molecule, 2-(dimethylamino) phenazine, will self-assemble kinetically to generate supramolecular-structure CDs during crystallization. The elaborately arranged supramolecular structure (J aggregates) endows CDs with intense solid-state-fluorescence. Density functional theory (DFT) calculation shows that the excited state of RT-CDs exhibits charge transfer characteristic owing to the unique donor-Π-acceptor structure. A high-performance monochrome RT-CDs based electroluminescent LEDs (2967 cd m-2 and 1.38 cd A-1 ) were fabricated via systematic optimizations of device engineering. This work provides a concrete and feasible avenue for the rapid and massive preparation of CDs, advancing the commercialization of CDs based optoelectronic devices.

Self-Aggregated Light-Trapping Nanodots for Highly Efficient Organic Solar Cells.

The typical thickness of the photoactive layer in organic solar cells (OSCs) is around 100 nm, which limits the absorption efficiency of the incident light and the power conversion efficiency (PCE) of OSCs. Therefore, light-trapping schemes to reduce the optical losses in the thin photoactive layers are critically important for efficient OSCs. Herein, light-trapping and electron-collection dual-functional small organic molecules, N,N,N',N'-tetraphenyloxalamide (TPEA) and N,N,N',N'-tetraphenylmalonamide (TPMA), are designed and synthesized by a one-step acylation reaction. Driven by strong intermolecular force, TPEA and TPMA tend to self-aggregate into hemispherical light-trapping nanodots on the photoactive layer, resulting in enhanced light harvesting. Meanwhile, TPEA and TPMA demonstrate high electron mobility and excellent electron-collection ability.  Compared with the device without cathode buffer layer (CBL, PCE = 14.09%), PM6:BTP-eC9 based OSCs with TPEA and TPMA light-trapping CBLs demonstrate greatly enhanced PCE of 16.21% and 17.85%, respectively. Furthermore, a record PCE of 19.02% can be achieved for PM6:BTP-eC9:PC71 BM based ternary OSC with TPMA light-trapping CBL. Moreover, TPMA exhibits a low synthesis cost of only 0.61 $ g-1 with high yield. These findings could open a window for the rational design of multifunctional CBLs for efficient and stable OSCs.

Bismuth Complex Controlled Morphology Evolution and CuSCN-Induced Transport Improvement Enable Efficient BiI3 Solar Cells.

Bismuth triiodide (BiI3) is a particularly promising absorber material for inorganic thin-film solar cells due to its merits of nontoxicity and low cost. However, one key factor that limits the efficiency of BiI3 solar cells is the film morphology, which is strongly correlated with the trap states of the BiI3 film. Herein, we report a coordination engineering strategy by using Lewis base dimethyl sulfoxide (DMSO) to induce the formation of a stable BiI3(DMSO)2 complex for controlling the morphology of BiI3 films. Density functional theory calculations further provide a theoretical framework for understanding the interaction of the BiI3(DMSO)2 complex with BiI3. The obtained BiI3(DMSO)2 complex could assist the fabrication of highly uniform and pinhole-free films with preferred crystallographic orientation. This high-quality film enables reduced trap densities, a suppressed charge recombination, and improved carrier mobility. In addition, the use of copper(I) thiocyanate (CuSCN) as a hole transport layer improves the charge transport, enabling the realization of solar cells with a record power conversion efficiency of 1.80% and a champion fill factor of 51.5%. Our work deepens the insights into controlling the morphology of BiI3 thin films through the coordination engineering strategy and paves the way toward further improving the photovoltaic performances of BiI3 solar cells.

Efficient Perovskite Indoor Photovoltaics with Open-Circuit Voltage of 1.15 V via Collaborative Optimization of CsPbI2 Br Layer and Hole Transport Layer.

All-inorganic CsPbI2 Br perovskite has attracted great attention due to the stable crystal structure and moisture resistance, and its 1.91 eV bandgap is close to the optimal bandgap of indoor artificial light sources, making it be the best candidate for the indoor photovoltaics (IPVs) to power a wide range of internet of things related electronic devices. Herein, we report on the preparation of CsPbI2 Br with α-phase and the improvement of its phase stability by adding lead acetate in the CsPbI2 Br precursor. A series of dopant-free conjugated polymers (P3HT, PBDB-T, and PM6) with different highest occupied molecular orbital energy levels are introduced as hole transport layers for building IPV devices. The PM6 based devices having better energy alignment with perovskite demonstrate best indoor photovoltaic performance, giving a remarkable open-circuit voltage of 1.15 V and high fill factor of 81.86% under 1000 lux (330 µW cm-2 ) light-emitting diode illumination, and finally realizing a decent power conversion efficiency of 33.68%. Our findings suggest that collaboratively optimize the CsPbI2 Br layer and hole transport layer is an effective approach to realize high performance IPVs.