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Although power conversion efficiency (PCE) of solar cells (SCs) continues to improve, they are still far from practical application because of their complex synthesis process, high cost and inferior operational stability. Carbon quantum dots with high material stability and remarkable photoluminescence are successfully used in light-emitting diodes. A good light emitter should also be an efficient SC according to the photon balance in Shockley-Quieisser formulation, in which all excitons are ultimately separated. However, the finite quantum-sized sp2 domain leads to tight exciton bonding, and highly delocalized electron clouds in irregular molecular stacks form disordered charge transfer, resulting in severe energy loss. Herein, an axially growing carbon quantum ribbon (AG-CQR) with a wide optical absorption range of 440-850 nm is reported. Structural and computational studies reveal that AG-CQRs (aspect ratio ≈2:1) with carbonyl groups at both ends regulate energy level and efficiently separate excitons. The stacking-controlled two-dimensional AG-CQR film further directionally transfers electrons and holes, particularly in AB stacking mode. Using this film as active layer alone, the SCs yield a maximum PCE of 1.22%, impressive long-term operational stability of 380 h, and repeatability. This study opens the door for the development of new-generation carbon-nanomaterial-based SCs for practical applications.
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With the rapid development of non-fullerene acceptors (NFAs), the power conversion efficiency (PCE) of organic solar cells (OSCs) is increasing. According to their different chemical structures, NFAs can initially be divided into two categories: small molecule acceptors (SMAs) and polymerized small molecule acceptors (PSMAs). Due to the strong absorption capacity and controllable energy levels, the PCE of devices based on SMAs has approached 20%. Compared with SMAs, PSMAs have advantages in stability and flexibility, and the PCE of PSMA-based devices has exceeded 18%. However, the higher synthesis cost and lower batch repeatability hinder its further development. Recently, the concept of giant molecule acceptors (GMAs) has been proposed. These materials have a clear molecular structure and are considered novel acceptor materials that combine the advantages of SMAs and PSMAs. Currently, the PCE of devices based on GMAs has exceeded 19%. In this review, we will introduce the latest developments in SMAs, PSMAs, and GMAs. Then, the advantages of GMAs and the relationship between their structure and performance will be analyzed. In the end, perspectives on the opportunities and challenges of these materials are provided, which could inspire further development of NFAs for advanced OSCs.
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Integrated electrochromic devices powered by photovoltaic cells have evoked a lot of interest due to their promising commercial prospects. However, their application has been restricted by the voltage adaption between the self-powered voltage and the color-changing threshold voltage (Vt). Herein, a strategy of bidirectional voltage regulating is proposed to develop a novel stand-alone integrated photovoltachromic device (I-PVCD), which integrates perovskite/organic tandem solar cells (P/O-TSCs) to drive color-changing process of conjugated poly(3-hexylthiophene) (P3HT) films. To lower the driving-voltage of electrochromic layer, C60 is introduced to decrease the onset oxidation potential of P3HT film, and thus leading to a reduced Vt of 0.70 V benefiting from the enhanced highest occupied molecular orbital level and decreased charge transfer resistance from 67.46 to 49.89 Ω. Simultaneously, PBDB-T is utilized as the hole transport layer in the interconnecting layer of CsPbI2Br/PTB7-Th:IEICO-4F P/O-TSC to improve its open-circuit voltage (Voc) to 1.85 V. Under their synergetic merits, a I-PVCD with a wider self-adaptive voltage range is achieved. This device can undergo fast and reversible chromic transition from beautiful magenta to transparent only under the solar radiation, and demonstrates a coloration efficiency of 351.90 cm2 C-1 and a switching time of 2 s besides its excellent operating reliability.
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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.
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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.
RESUMEN
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.
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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.
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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.
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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 0.1â cm2 and 1â cm2 active area, respectively. The obtained high efficiency of 38.24 % under 1000â lux illumination suggests its potential in indoor photovoltaics for powering the Internet of Things, etc.
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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.
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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.
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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.
RESUMEN
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 âCâO, âNH, and âOâ 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 âCâO and âOâ groups in VM can immobilize the uncoordinated Pb2+ to manage the positively charged defect and the formation of NâH···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.
RESUMEN
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.
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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.
RESUMEN
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 0.07â cm2 â 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 000â cd m-2 . This study represents a significant advance that CQDs-based electroluminescent device can be utilized for potential display and lighting applications.
RESUMEN
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 9450/4236â cd m-2 , high current efficiency of 1.57/2.34â cd A-1 and low turn-on voltage of 3.1/3.6â 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.
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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.
RESUMEN
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.