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In this work, an efficient and robust hole transport layer (HTL) based on blended poly((9,9-dioctylfluorenyl-2,7-diyl)-alt-(9-(2-ethylhexyl)-carbazole-3,6-diyl)) (PF8Cz) and crosslinkable 3,3'-(9,9-dimethyl-9H-fluorene-2,7-diyl)bis(9-(4-vinylphenyl)-9H-carbazole) (FLCZ-V) is introduced for high-performance and stable blue quantum dot-based light-emitting diodes (QLEDs), wherein FLCZ-V can in situ-crosslink to a continuous network polymer after thermal treatment and the linear polymer PF8CZ becomes intertwined and imprisoned. As a result, the blended HTL shows a high hole mobility (1.27 × 10-4 cm2 V-1 s-1) and gradient HOMO levels (-5.4 eV of PF8CZ and -5.7 eV of FLCZ-V) that can facilitate hole injecting so as to ameliorate the charge balance and, at the same time, achieve better electron-blocking capability that can effectively attenuate HTL decomposition. Meanwhile, the crosslinked blended HTL showed excellent solvent resistance and a high surface energy of 40.34 mN/m, which is favorable to enhance wettability for the deposition of a follow-up layer and attain better interfacial contact. Based on the blended HTL, blue QLEDs were fabricated by both spin-coating and inkjet printing. For the spin-coated blue QLED, a remarkable enhancement of external quantum efficiency (EQE) of 15.5% was achieved. Also, the EQE of the inkjet-printed blue QLED reached 9.2%, which is thus far the best result for the inkjet-printed blue QLED.
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The operating lifetime of quantum-dot light-emitting diodes (QLED) is a bottleneck for commercial display applications. To enhance the operational stability of QLEDs, we developed a robust solution-processed highly conductive hole-transport-layer (HTL) structure, which enables a thick HTL structure to mitigate the electric field. An alternating doping strategy, which involves multiple alternating stacks of N4,N4'-di(naphthalen-1-yl)-N4,N4'-bis(4-vinylphenyl)biphenyl-4,4'-diamine and phosphomolybdic acid layers, could provide significantly improved conductivity; more specifically, the 90 nm-thick alternatingly doped HTL exhibited higher conductivity than the 45 nm-thick undoped HTL. Therefore, when applied to a QLED, the increase in the thickness of the alternatingly doped HTL increased device reliability. As a result, the lifetime of the QLED with a thick, alternatingly doped HTL was 48-fold higher than that of the QLED with a thin undoped HTL. This alternating doping strategy provides a new paradigm for increasing the stability of solution-based optoelectronic devices in addition to QLEDs.
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BiVO4-based photoanode is one of the most promising photoanodes for photoelectrocatalytic water splitting. However, the serious problem of interface charge recombination limits its further development. Here, a Mo:BiVO4/NiOx/CPF-TCzB/NiCoBi photoanode is constructed with double hole transport layer and an energy level gradient to achieve an effective photo-generated holes extraction and accumulation at the surface electrocatalyst. The conjugated polycarbazole framework CPF-TCzB is used as hole transport layer to eliminate the charge recombination center between Mo:BiVO4 and NiCoBi electrocatalyst and realize the extraction and storage of photo-generated hole; NiOx nanoparticles are further inserted between Mo:BiVO4 and CPF-TCzB to form a gradient energy level, eliminating the energy level barrier and optimizing band alignment. As a result, Mo:BiVO4/NiOx/CPF-TCzB/NiCoBi achieves a much higher photocurrent densities of 3.14 mA cm-2 than that of Mo:BiVO4 (0.42 mA cm-2) at 0.6 V versus RHE. This work provides an specific way to adjust the band structure of BiVO4-based photoanodes and realize efficient hole extraction and storage for PEC water splitting.
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In colloidal quantum dot light-emitting diodes (QD-LEDs), replacing organic hole transport layers (HTLs) with their inorganic counterparts is expected to yield distinct advantages due to their inherent material robustness. However, despite the promising characteristics of all-inorganic QD-LEDs, some challenges persist in achieving stable operation; for example, the electron overflow toward the inorganic HTL and charge accumulation within working devices return a temporal inconsistency in device characteristics. To address these challenges, we propose an operational approach that employs an alternating-current (AC) in all-inorganic QD-LEDs. We carry out comprehensive studies on the optoelectrical characteristics of all-inorganic QD-LEDs under direct-current (DC) or AC operation and demonstrate that AC operation can facilitate efficient charge carrier recombination within the QD emissive layer, leading to improved device efficiency and temporally invariant optoelectronic characteristics. Leveraging the intrinsic material robustness of inorganic charge transport layers (CTLs), our current study suggests a promising pathway toward enhancing the performance and stability of QD-LEDs, particularly for futuristic display applications.
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Considering the increasing demand for high-resolution light-emitting diodes (LEDs), it is important that direct fine patterning technologies for LEDs be developed, especially for quantum-dot LEDs (QLEDs). Traditionally, the patterning of QLEDs relies on resin-based photolithography techniques, requiring multiple steps and causing performance deterioration. Nondestructive direct patterning may provide an easy and stepwise method to achieve fine-pixelated units in QLEDs. In this study, two isomeric tridentate cross-linkers (X8/X9) are presented and can be blended into the hole transport layer (HTL) and the emissive layer (EML) of QLEDs. Because of their photosensitivity, the in situ cross-linking process can be efficiently triggered by ultraviolet irradiation, affording high solvent resistance and nondestructive direct patterning of the layers. Red QLEDs using the cross-linked HTL demonstrate an impressive external quantum efficiency of up to 22.45%. Through lithographic patterning enabled by X9, line patterns of HTL and EML films exhibit widths as narrow as 2 and 4 µm, respectively. Leveraging the patterned HTL and EML, we show the successful fabrication of pixelated QLED devices with an area size of 3 × 3 mm2, alongside the successful production of dual-color pixelated QLED devices. These findings showcase the promising potential of direct patterning facilitated by engineered cross-linkers for the cost-effective fabrication of pixelated QLED displays.
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Light-induced phase segregation, particularly when incorporating bromine to widen the bandgap, presents significant challenges to the stability and commercialization of perovskite solar cells. This study explores the influence of hole transport layers, specifically poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine (PTAA) and [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz), on the dynamics of phase segregation. Through detailed characterization of the buried interface, we demonstrate that Me-4PACz enhances perovskite photostability, surpassing the performance of PTAA. Nanoscale analyses using in situ Kelvin probe force microscopy and quantitative nanomechanical mapping techniques elucidate defect distribution at the buried interface during phase segregation, highlighting the critical role of substrate wettability in perovskite growth and interface integrity. The integration of these characterization techniques provides a thorough understanding of the impact of the buried bottom interface on perovskite growth and phase segregation.
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Quantum-dot light-emitting diodes (QLEDs), a kind of promising optoelectronic device, demonstrate potential superiority in next-generation display technology. Thermal cross-linked hole transport materials (HTMs) have been employed in solution-processed QLEDs due to their excellent thermal stability and solvent resistance, whereas the unbalanced charge injection and high cross-linking temperature of cross-linked HTMs can inhibit the efficiency of QLEDs and limit their application. Herein, a low-temperature cross-linked HTM of 4,4'-bis(3-(((4-vinylbenzyl)oxy)methyl)-9H-carbazol-9-yl)-1,1'-biphenyl (DV-CBP) with a flexible styrene side chain is introduced, which reduces the cross-linking temperature to 150 °C and enhances the hole mobility up to 1.01 × 10-3 cm2 V-1 s-1. More importantly, the maximum external quantum efficiency of 21.35% is successfully obtained on the basis of the DV-CBP as a cross-linked hole transport layer (HTL) for blue QLEDs. The low-temperature cross-linked high-mobility HTL using flexible side chains could be an excellent alternative for future HTL development.
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Perovskite solar cells (PSCs) have gained much attention in recent years because of their improved energy conversion efficiency, simple fabrication process, low processing temperature, flexibility, light weight, and low cost of constituent materials when compared with their counterpart silicon based solar cells. Besides, stability and toxicity of PSCs and low power conversion efficiency have been an obstacle towards commercialization of PSCs which has attracted intense research attention. In this research paper, a Glass/Cu2O/CH3NH3SnI3/ZnO/Al inverted device structure which is made of cheap inorganic materials, n-type transparent conducting oxide (TCO)-free, stable, photoexcited toxic-free perovskite have been carefully designed, simulated and optimized using a one-dimensional solar cell capacitance simulator (SCAPS-1D) software. The effects of layers' thickness, perovskite's doping concentration and back contact electrodes have been investigated, and the optimized structure produced an open circuit voltage (Voc) of 1.0867 V, short circuit current density (JSC) of 33.4942 mA/cm2, fill factor (FF) of 82.88% and power conversion efficiency (PCE) of 30.17%. This paper presents a model that is first of its kind where the highest PCE performance and eco-friendly n-type TCO-free inverted CH3NH3SnI3 based perovskite solar cell is achieved using all-inorganic transport materials.
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At present, heavy-metal-free quantum dot light-emitting diodes (QLEDs) have shown great potential as a research hotspot in the field of optoelectronic devices. This article reviews the research on heavy-metal-free quantum dot (QD) materials and light-emitting diode (LED) devices. In the first section, we discussed the hazards of heavy-metal-containing quantum dots (QDs), such as environmental pollution and human health risks. Next, the main representatives of heavy-metal-free QDs were introduced, such as InP, ZnE (E=S, Se and Te), CuInS2, Ag2S, and so on. In the next section, we discussed the synthesis methods of heavy-metal-free QDs, including the hot injection (HI) method, the heat up (HU) method, the cation exchange (CE) method, the successful ionic layer adsorption and reaction (SILAR) method, and so on. Finally, important progress in the development of heavy-metal-free QLEDs was summarized in three aspects (QD emitter layer, hole transport layer, and electron transport layer).
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Conventional hole transport layer (HTL) Spiro-OMeTAD requires the addition of hygroscopic dopants due to its low conductivity and hole mobility, resulting in a high preparation cost and poor device stability. Cuprous thiocyanate (CuSCN) is a cost-effective alternative with a suitable energy structure and high hole mobility. However, CuSCN-based perovskite solar cells (PSCs) are affected by environmental factors, and the solvents of an HTL can potentially corrode the perovskite layer. In this study, a Co3O4/CuSCN/Co3O4 sandwich structure was proposed as an HTL for inorganic Cs2PbI2Cl2/CsPbI2.5Br0.5 PSCs to address these issues. The Co3O4 layers can serve as buffer and encapsulation layers, protecting the perovskite layer from solvent-induced corrosion and enhancing hole mobility at the interface. Based on this sandwich structure, the photovoltaic performances of the Cs2PbI2Cl2/CsPbI2.5Br0.5 PSCs are significantly improved, with the power conversion efficiency (PCE) increasing from 9.87% (without Co3O4) to 11.06%. Furthermore, the thermal stability of the devices is also significantly enhanced, retaining 80% of its initial PCE after 40 h of continuous aging at 60 °C. These results indicate that the Co3O4/CuSCN/Co3O4 sandwich structure can effectively mitigate the corrosion of the perovskite layer by solvents of an HTL and significantly improves the photovoltaic performance and thermal stability of devices.
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Perovskite solar cell (PSC) is a promising photovoltaic technology that achieves over 26% power conversion efficiency (PCE). However, the high materials costs, complicated fabrication process, as well as poor long-term stability, are stumbling blocks for the commercialization of the PSCs in normal structures. The hole transport layer (HTL)-free carbon-based PSCs (C-PSCs) are expected to overcome these challenges. However, C-PSCs have suffered from relatively low PCE due to severe energy loss at the perovskite/carbon interface. Herein, the study proposes to boost the hole extraction capability of carbon electrode by incorporating functional manganese (II III) oxide (Mn3O4). It is found that the work function (WF) of the carbon electrode can be finely tuned with different amounts of Mn3O4 addition, thus the interfacial charge transfer efficiency can be maximized. Besides, the mechanical properties of carbon electrode can also be strengthened. Finally, a PCE of 19.03% is achieved. Moreover, the device retains 90% of its initial PCE after 2000 h of storage. This study offers a feasible strategy for fabricating efficient paintable HTL-free C-PSCs.
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The performance of blue quantum dot light-emitting diodes (QLEDs) is limited by unbalanced charge injection, resulting from insufficient holes caused by low mobility or significant energy barriers. Here, we introduce an angular-shaped heteroarene based on cyclopentane[b]thiopyran (C8-SS) to modify the hole transport layer poly-N-vinylcarbazole (PVK), in blue QLEDs. C8-SS exhibits high hole mobility and conductivity due to the π···π and S···π interactions. Introducing C8-SS to PVK significantly enhanced hole mobility, increasing it by 2 orders of magnitude from 2.44 × 10-6 to 1.73 × 10-4 cm2 V-1 s-1. Benefiting from high mobility and conductivity, PVK:C8-SS-based QLEDs exhibit a low turn-on voltage (Von) of 3.2 V. More importantly, the optimized QLEDs achieve a high peak power efficiency (PE) of 7.13 lm/W, which is 2.65 times that of the control QLEDs. The as-proposed interface engineering provides a novel and effective strategy for achieving high-performance blue QLEDs in low-energy consumption lighting applications.
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Perovskite solar cells (PSCs) offer impressive performance and flexibility, thanks to their simple, low-temperature deposition methods. Their band gap tunability allows for a wide range of applications, transitioning from opaque to transparent devices. This study introduces the first flexible, bifacial PSCs using the FAPbBr3 perovskite. We investigated the impact of optimizing electron and hole transport layers on the cells' bifaciality, transparency, and stability. PSCs achieved a maximum power conversion efficiency (PCE) of 6.8 and 18.7% under 1 sun and indoor light conditions (1200 lx), respectively, showing up to 98% bifaciality factor and an average visible transmittance (AVT) of 55%. Additionally, a P1-P2-P3 laser ablation scheme has been developed on the flexible poly(ethylene terephthalate) (PET) substrate for perovskite solar modules showing a PCE of 4.8% and high geometrical fill factor (97.8%). These findings highlight the potential of flexible, bifacial PSCs for diverse applications such as building-integrated photovoltaics (BIPV), agrivoltaics, automotive technology, wearable sensors, and Internet of things (IoT).
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Carbon electrode-based perovskite solar cells (c-PSCs) without a hole transport layer (HTL) have obtained a significant interest owing to their cost-effective, stable, and simplified structure. However, their application is limited by low efficiency and the prevalence of high-temperature processed electron transport layer (ETL), e.g. TiO2, which also has poor optoelectronic properties, including low conductivity and mobility. In this study, a series of organic materials, namely PCBM ((Park et al., 2023; Park et al., 2023) [6,6]-phenyl-C61-butyric acid methyl ester, C72H14O2), Alq3 (Al(C9H6NO)3), BCP (2,9-Dimethyl-4,7-diphenyl-1,10-phenanthroline, C26H20N2), C60, ICBA (indene-C60 bisadduct, C78H16) and PEIE (poly (ethylenimine) ethoxylated, (C37H24O6N2)n) have been numerically analyzed in SCAPS-1D solar simulator to explore alternative potential ETL materials for HTL-free c-PSCs. The presented device has FTO/ETL/CH3NH3PbI3/carbon structure, and its performance is optimized based on significant design parameters. The highest achieved PCEs for PCBM, Alq3, BCP, C60, ICBA, and PEIE-based devices are 22.85%, 19.08%, 20.99%, 25.51%, 23.91%, and 22.53%, respectively. These PCEs are obtained for optimum absorber thickness for each case, with an acceptor concentration of 1.0 × 1017 cm-3 and defect density of 2.5 × 1013 cm-3. The C60-based cell has been found to outperform with device parameters as Voc of 1.29 V, Jsc of 23.76 mA/cm2, and FF of 82.67%. As the design lacks stability when only organic materials are employed, each of the presented devices have been analyzed by applying BiI3, LiF, and ZnO as protective layers with the performances not compromised. We believe that our obtained results will be of great interest in developing stable and efficient HTL-free c-PSCs.
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Developing an insoluble cross-linkable hole transport layer (HTL) plays an important role for solution-processed quantum dots light-emitting diodes (QLEDs) to fabricate a multilayer device with separated quantum dots layers and HTLs. In this work, a facile photothermal synergic cross-linking strategy is simultaneous annealing and UV irradiation to form the high-quality cross-linked film as the HTL without any photoinitiator, which efficiently reduces the cross-linking temperature to the low temperature of 130 °C and enhances the hole mobility of the 3-vinyl-9-{4-[4-(3-vinylcarbazol-9-yl)phenyl]phenyl}carbazole (CBP-V) thin films. The obtained high-quality cross-linked CBP-V films exhibited smooth morphology, excellent solvent resistance, and high mobility. Moreover, the high-performance red, green, and blue (RGB) QLEDs are successfully fabricated by using the photothermal synergic cross-linked HTLs, which achieved the maximum external quantum efficiency of 25.69, 24.42, and 16.51%, respectively. This work presents a strategy of using the photothermal synergic cross-linked HTLs for fabrication of high-performance QLEDs and advancing their related device applications.
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Tracking the dynamics of ultrafast hole injection into copper thiocyanate (CuSCN) at the interface can be experimentally challenging. These challenges include restrictions in accessing the ultraviolet spectral range through transient electronic spectroscopy, where the absorption spectrum of CuSCN is located. Time-resolved vibrational spectroscopy solves this problem by tracking marker modes at specific frequencies and allowing direct access to dynamical information at the molecular level at donor-acceptor interfaces in real time. This study uses photoabsorber PM6 (poly[(2,6-(4,8-bis(5-(2-ethylhexyl-3-fluoro)thiophen-2-yl)-benzo[1,2-b:4,5-b']dithiophene))-alt-(5,5-(1',3'-di-2-thienyl-5',7'-bis(2-ethylhexyl)-benzo[1',2'-c:4',5'-c']dithiophene-4,8-dione))]) as a model system to explore and decipher the hole transfer dynamics of CuSCN using femtosecond (fs) mid-infrared (IR) spectroscopy. The time-resolved results indicate that excited PM6 exhibits a sharp vibrational mode at 1599 cm-1 attributed to the carbonyl group, matching the predicted frequency position obtained from time-dependent density functional theory (DFT) calculations. The fs mid-IR spectroscopy demonstrates a fast formation (<168 fs) and blue spectral shift of the CN stretching vibration from 2118 cm-1 for CuSCN alone to 2180 cm-1 for PM6/CuSCN, confirming the hole transfer from PM6 to CuSCN. The short interfacial distance and high frontier orbital delocalization obtained from the interfacial DFT models support a coherent and ultrafast regime for hole transfer. These results provide direct evidence for hole injection at the interface of CuSCN for the first time using femtosecond mid-IR spectroscopy and serve as a new investigative approach for interfacial chemistry and solar cell communities.
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Nowadays, the extensively used lead sulfide (PbS) quantum dot (QD) hole transport layer (HTL) relies on layer-by-layer method to replace long chain oleic acid (OA) ligands with short 1,2-ethanedithiol (EDT) ligands for preparation. However, the inevitable significant volume shrinkage caused by this traditional method will result in undesired cracks and disordered QD arrangement in the film, along with adverse increased defect density and inhomogeneous energy landscape. To solve the problem, a novel method for EDT passivated PbS QD (PbS-EDT) HTL preparation using small-sized benzoic acid (BA) as intermediate ligands is proposed in this work. BA is substituted for OA ligands in solution followed by ligand exchange with EDT layer by layer. With the new method, smoother PbS-EDT films with more ordered and closer QD packing are gained. It is demonstrated stronger coupling between QDs and reduced defects in the QD HTL owing to the intermediate BA ligand exchange. As a result, the suppressed nonradiative recombination and enhanced carrier mobility are achieved, contributing to ≈20% growth in short circuit current density (Jsc) and a 23.4% higher power conversion efficiency (PCE) of 13.2%. This work provides a general framework for layer-by-layer QD film manufacturing optimization.
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Two-dimensional (2D) materials have attracted attention due to their excellent optoelectronic properties, but their applications are limited by their defects and vacancies. Surface modification is an effective method to restore their performance. Here, ZrSe2 is modified with conductive polymer p-toluenesulfonic acid (PTSA). It is found that PTSA can obtain electrons of ZrSe2 through the combination of -SO3H and ZrSe2, thus forming interfacial dipoles, which improve the work function of ZrSe2. In addition, -OH in PTSA can effectively fill the Se vacancy in ZrSe2 to form P-type doping, thereby improving its conductivity. ZrSe2 modified by the PTSA material is first used as a hole transport layer (HTL) in organic solar cells (OSCs). The efficiency of OSCs based on the PBDB-T:ITIC and PM6:L8-BO binary active layer with ZrSe2:PTSA as the novel HTL reaches 10.66 and 18.14%, which are obviously higher than the efficiency of OSCs with pure ZrSe2 as the HTL (8.48 and 15.64%). More interestingly, the stability of the device with ZrSe2:PTSA as HTL is significantly better than that of PEDOT:PSS. This study shows that the modification of the organic material can effectively improve the photoelectric performance of ZrSe2 and explores the physical mechanism of the interaction between the organic modifier and 2D materials.
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The doped organic hole transport layer (HTL) is crucial for achieving high-efficiency perovskite solar cells (PSCs). However, the traditional doping strategy undergoes a time-consuming and environment-dependent oxidation process, which hinders the technology upgrades and commercialization of PSCs. Here, we reported a new strategy by introducing a cascade reaction in traditional doped Spiro-OMeTAD, which can simultaneously achieve rapid oxidation and overcome the erosion of perovskite by 4-tert-butylpyridine (tBP) in organic HTL. The ideal dopant iodobenzene diacetate was utilized as the initiator that can react with Spiro to generate Spiroâ + radicals quickly and efficiently without the participation of ambient air, with the byproduct of iodobenzene (DB). Then, the DB can coordinate with tBP through a halogen bond to form a tBP-DB complex, minimizing the sustained erosion from tBP to perovskite. Based on the above cascade reaction, the resulting Spiro-based PSCs have a champion PCE of 25.76 % (certificated of 25.38 %). This new oxidation process of HTL is less environment-dependent and produces PSCs with higher reproducibility. Moreover, the PTAA-based PSCs obtain a PCE of 23.76 %, demonstrating the excellent applicability of this doping strategy on organic HTL.
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Nickel oxide (NiOX) is an ideal inorganic hole transport material for the fabrication of inverted perovskite solar cells owing to its excellent optical and semiconductor properties. Currently, the main research on developing the performance of NiOX-based perovskite solar cells focuses on improving the conductivity of NiOX thin films and preventing the redox reactions between metal cations (Ni3+ on the surface of NiOX) and organic cations (FA+ or MA+ in the perovskite precursors) at the NiOX/perovskite interface. In this study, a new type of interface defects in NiOX-based CsPbI2Br solar cells is reported. That is the Pb2+ from CsPbI2Br perovskites can diffuse into the lattice of NiOX surface as the annealing temperature of perovskites changes. The diffusion of Pb2+ increases the ratio of Ni3+/Ni2+ on the surface of NiOX, leading to an increase in the density of trap state at the interface between NiOX and perovskites, which eventually results in a serious decline in the photovoltaic performance of solar cells.