RESUMEN

Ultrathin (∼10 nm) insulating polymer films are commonly employed as an interfacial modification layer (IML) to improve charge balance and suppress interfacial exciton quenching in quantum dot light-emitting diodes (QLEDs). However, because the thickness is smaller than the energy transfer distance, interfacial exciton quenching is only partially suppressed, leading to the degrading of device performance. In this work, a thick (35 nm) inorganic CdS film is developed to serve as the IML of CdSe quantum-dot-based QLED. Benefiting from relatively low electron mobility and well-matched energy level, the CdS IML can effectively improve charge balance. In addition, because the thickness is larger than the energy transfer distance, interfacial exciton quenching can be completely blocked. As a result, the QLEDs with CdS IML exhibit a maximum EQE of 21.2% and a peak current efficiency of 24.2 cd A-1, which are about 1.32- and 1.4-fold higher than 16.1% and 17.3 cd A-1 of the devices without CdS IML, respectively. Our work offers an efficient method to completely block interfacial exciton quenching, which may open a new avenue for developing higher-performance QLEDs.

RESUMEN

Despite its benefits for facilitating device fabrication, utilization of a polymeric hole transport layer (HTL) in inverted quantum dots (QDs) light-emitting devices (IQLEDs) often leads to poor device performance. In this work, we find that the poor performance arises primarily from electron leakage, inefficient charge injection, and significant exciton quenching at the HTL interface in the inverted architecture and not due to solvent damage effects as is widely believed. We also find that using a layer of wider band gap QDs as an interlayer (IL) in between the HTL and the main QDs' emission material layer (EML) can facilitate hole injection, suppress electron leakage, and reduce exciton quenching, effectively mitigating the poor interface effects and resulting in high electroluminescence performance. Using an IL in IQLEDs with a solution-processed poly(9,9-dioctylfluorene-alt-N-(4-sec-butylphenyl)-diphenylamine) (TFB), HTL improves the efficiency by 2.85× (from 3 to 8.56%) and prolongs the lifetime by 9.4× (from 1266 to 11,950 h at 100 cd/m2), which, to the best of our knowledge, is the longest lifetime for an R-IQLED with a solution-coated HTL. Measurements on single-carrier devices reveal that while electron injection becomes easier as the band gap of the QDs decreases, hole injection surprisingly becomes more difficult, indicating that EMLs of QLEDs are more electron-rich in the case of red devices and more hole-rich in the case of blue devices. Ultraviolet photoelectron spectroscopy measurements verify that blue QDs have a shallower valence band energy than their red counterparts, corroborating these conclusions. The findings in this work, therefore, provide not only a simple approach for achieving high performance in IQLEDs with solution-coated HTLs but also novel insights into charge injection and its dependence on QDs' band gap as well as into different HTL interface properties of the inverted versus upright architecture.

RESUMEN

Triose phosphate utilisation (TPU) limits the maximum rate at which plants can photosynthesise. However, TPU is almost never found to be limiting photosynthesis under ambient conditions for plants. This, along with previous results showing adaptability of TPU at low temperature, suggest that TPU capacity is regulated to be just above the photosynthetic rate achievable under the prevailing conditions. A set of experiments were performed to study the adaptability of TPU capacity when plants are acclimated to elevated CO2 concentrations. Plants held at 1500 ppm CO2 were initially TPU limited. After 30 h they no longer exhibited TPU limitations but they did not elevate their TPU capacity. Instead, the maximum rates of carboxylation and electron transport declined. A timecourse of regulatory responses was established. A step increase of CO2 first caused PSI to be oxidised but after 40 s both PSI and PSII had excess electrons as a result of acceptor-side limitations. Electron flow to PSI slowed and the proton motive force increased. Eventually, non-photochemical quenching reduced electron flow sufficiently to balance the TPU limitation. Over several minutes rubisco deactivated contributing to regulation of metabolism to overcome the TPU limitation.

Asunto(s)

RESUMEN

We report high-efficiency and long-lifetime inverted green cadmium-free (InP-based) quantum dot light-emitting diodes (QLEDs) using a stable ZnO/ZnS cascaded electron transport layer (ETL). We have successfully developed a strategy to spin-coat stable ZnS ETLs with a relatively higher conduction band minimum (CBM) and lower electron mobility than that of ZnO, which leads to balanced carrier injection and an improved device lifetime. Analysis shows that by using the ZnO/ZnS cascaded ETL, electron injection is reduced, resulting in an improved charge balance in the QD layer and suppressed exciton quenching, which preserves the emission properties of QDs. Optimized devices with ZnO/ZnS cascaded ETLs show a maximum external quantum efficiency of 10.8% and a maximum current efficiency of 37.5 cd/A; these efficiency values are an almost 2.2-fold improvement compared to those of reference devices without ZnS. The QLED devices also showed a remarkably long lifetime (LT70) of 265 h at an initial luminance of 1000 cd/m2. The predicted half-lifetime (LT50) at 100 cd/m2 is 60,255 h, which, to our knowledge, is currently the longest lifetime yet reported for InP-based green QLEDs.

RESUMEN

Highly efficient, all-solution processed inverted quantum dot light-emitting diodes (QLEDs) are demonstrated by employing 1,3,5-tri(m-pyrid-3-yl-phenyl)benzene (TmPyPB) layer as electron blocking layer. Electron injection from ZnO electron transport layer to quantum dots (QDs) emission layer (EML) can be adjusted by thickness of TmPyPB layer, enabling the balanced charge carriers in QDs EML. With optimal thickness of this TmPyPB adjuster, 59.7% increment in the device current efficiency (from 8.2 to 13.1 cd A-1) and 46.2% improvement in the maximum luminance (from 31916 to 46674 cd m-2) are achieved, compared with those of the control QLED which has double hole transport layer structure. On the other hand, we find luminescence quenching process, which often happens at the interface of ZnO nanoparticles and QDs, is not obvious in our QLEDs, in which the ZnO layer is fabricated in precursor method, and this conclusion is verified through Time Resolution Photoluminescence test. In a word, this strategy provides a direction for optimizing charge carrier balance in all-solution processed inverted QLED.

RESUMEN

Graphene is an optimal material to be employed as an ionic diffusion barrier because of its outstanding impermeability and chemical robustness. Indium tin oxide (ITO) is often used in perovskite light-emitting diodes (PeLEDs), and it can release indium easily upon exposure to the acidic hole-injection layer so that luminescence can be quenched significantly. Here, we exploit the outstanding impermeability of graphene and use it as a chemical barrier to block the etching that can occur in ITO exposed to an acidic hole-injection layer in PeLEDs. This barrier reduced the luminescence quenching that these metallic species can cause, so the photoluminescence lifetime of perovskite film was substantially higher in devices with ITO and graphene layer (87.9 ns) than in devices that had only an ITO anode (22.1 ns). Luminous current efficiency was also higher in PeLEDs with a graphene barrier (16.4 cd/A) than in those without graphene (9.02 cd/A). Our work demonstrates that graphene can be used as a barrier to reduce the degradation of transparent electrodes by chemical etching in optoelectronic devices.

RESUMEN

The phenomenon of positive aging, i.e., efficiency increased with time, is observed in quantum-dot light-emitting diodes (QLEDs). For example, the external quantum efficiency (EQE) of blue QLEDs is significantly improved from 4.93% to 12.97% after storage for 8 d. The origin of such positive aging is thoroughly investigated. The finding indicates that the interfacial reaction between Al cathode and ZnMgO electron transport layer accounts for such improvement. During shelf-aging, the Al slowly reacts with the oxygen from ZnMgO, and consequently, leads to the formation of AlO x and the production of oxygen vacancies in ZnMgO. The AlO x interlayer reduces the electron injection barrier while the oxygen vacancies increase the conductivity of ZnMgO and, as a result, the electron injection is effectively enhanced. Moreover, the AlO x can effectively suppress the quenching of excitons by metal electrode. Due to the enhancement of electron injection and suppression of exciton quenching, the aged blue, green, and red QLEDs exhibit a 2.6-, 1.3-, and 1.25-fold efficiency improvement, respectively. The studies disclose the origin of positive aging and provide a new insight into the exciton quenching mechanisms, which would be useful for further constructing efficient QLED devices.

RESUMEN

Sublimable charged iridium(III) complexes are becoming an attractive family of new phosphors and making their way into vacuum-evaporated-deposited organic light-emitting diodes, while it remains challenging to achieve high device performance. Here, we demonstrate a substantial mitigation of exciton quenching not only by reducing the dopant concentration, but also by controlling the ion distribution in the emissive material layers. We, therefore, achieved green luminescence with high brightness, superior efficiencies, and low driving voltages. Following this strategy, we further developed another six sublimable charged iridium(III) complexes and attained blue-green, yellow, and red-emitting devices with record-high performance. This study represents an important advance in the construction of bright electroluminescence from ionic transition metal complexes and shows their great promise in various optoelectronic applications.

RESUMEN

The effect of postannealing on the device characteristics is systematically investigated. The external quantum efficiency (EQE) of blue quantum-dot light-emitting diodes (QLEDs) is significantly improved from 5.22 to 9.81% after postannealing. Similar results are obtained in green and red QLEDs, whose EQEs are enhanced from 11.47 and 13.60 to 15.57 and 16.59%, respectively. The annealed devices also exhibit a larger current density. The origin of efficiency improvement is thoroughly investigated. Our finding indicates that postannealing promotes the interfacial reaction of Al and ZnMgO and consequently leads to the metallization of the AlZnMgO contact and the formation of the AlO x interlayer. Because of the metallization of AlZnMgO, the contact resistance is effectively reduced, and thus the electron injection is enhanced. On the other hand, the formation of the AlO x interlayer can effectively suppress the quenching of excitons by the metal electrode. Because of the enhancement of electron injection and suppression of exciton quenching, the annealed blue, green, and red QLEDs exhibit a 1.9-, a 1.3-, and a 1.2-fold efficiency improvement, respectively. We envision the results offer a simple yet effective method to enhance the charge injection and the efficiency of QLED devices, which would promote the practical application of QLEDs.

RESUMEN

Quantum-dot light-emitting diodes (QLEDs) may combine superior properties of colloidal quantum dots (QDs) and advantages of solution-based fabrication techniques to realize high-performance, large-area, and low-cost electroluminescence devices. In the state-of-the-art red QLED, an ultrathin insulating layer inserted between the QD layer and the oxide electron-transporting layer (ETL) is crucial for both optimizing charge balance and preserving the QDs' emissive properties. However, this key insulating layer demands very accurate and precise control over thicknesses at sub-10 nm level, causing substantial difficulties for industrial production. Here, it is reported that interfacial exciton quenching and charge balance can be independently controlled and optimized, leading to devices with efficiency and lifetime comparable to those of state-of-the-art devices. Suppressing exciton quenching at the ETL-QD interface, which is identified as being obligatory for high-performance devices, is achieved by adopting Zn0.9 Mg0.1 O nanocrystals, instead of ZnO nanocrystals, as ETLs. Optimizing charge balance is readily addressed by other device engineering approaches, such as controlling the oxide ETL/cathode interface and adjusting the thickness of the oxide ETL. These findings are extended to fabrication of high-efficiency green QLEDs without ultrathin insulating layers. The work may rationalize the design and fabrication of high-performance QLEDs without ultrathin insulating layers, representing a step forward to large-scale production and commercialization.

RESUMEN

The effect of shell thickness on the performance of all-inorganic quantum dot light-emitting diodes (QLEDs) is explored by employing a series of green quantum dots (QDs) (Zn xCd1- xSe/ZnS core/shell QDs with different ZnS shell thicknesses) as the emitters. ZnO nanoparticles and sol-gel NiO are employed as the electron and hole transport materials, respectively. Time-resolved and steady-state photoluminescence results indicate that positive charging processes might occur for the QDs deposited on NiO, which results in emission quenching of QDs and poor device performance. The thick shell outside the core in QDs not only largely suppresses the QD emission quenching but also effectively preserves the excitons in QDs from dissociation of electron-hole pairs when they are subjected to an electric field. The peak efficiency of 4.2 cd/A and maximum luminance of 4205 cd/m2 are achieved for the device based on QDs with the thickest shells (∼4.2 nm). We anticipate that these results will spur progress toward the design and realization of efficient all-inorganic QLEDs as a platform for the QD-based full-colored displays.

RESUMEN

Non-photochemical quenching (NPQ) is the most important photoprotective system in higher plants. NPQ can be divided into several steps according to the timescale of relaxation of chlorophyll fluorescence after reaching a steady state (i.e., the fast phase, qE; middle phase, qZ or qT; and slow phase, qI). The dissipation of excess energy as heat during the xanthophyll cycle, a large component of NPQ, is detectable during the fast to middle phase (sec to min). Although thermal dissipation is primarily investigated using indirect methods such as chlorophyll a fluorescence measurements, such analyses require dark adaptation or the application of a saturating pulse during measurement, making it difficult to continuously monitor this process. Here, we designed an unconventional technique for real-time monitoring of changes in thylakoid lumen pH (as reflected by changes in xanthophyll pigment content) based on the photochemical reflectance index (PRI), which we estimated by measuring light-driven leaf reflectance at 531 nm. We analyzed two Arabidopsis thaliana mutants, npq1 (unable to convert violaxanthin to zeaxanthin due to inhibited violaxanthin de-epoxidase [VDE] activity) and npq4 (lacking PsbS protein), to uncover the regulator of the PRI. The PRI was variable in wild-type and npq4 plants, but not in npq1, indicating that the PRI is related to xanthophyll cycle-dependent thermal energy quenching (qZ) rather than the linear electron transport rate or NPQ. In situ lumen pH substitution using a pH-controlled buffer solution caused a shift in PRI. These results suggest that the PRI reflects only xanthophyll cycle conversion and is therefore a useful parameter for monitoring thylakoid lumen pH (reflecting VDE activity) in vivo.

Asunto(s)

RESUMEN

Inter- and intramolecular charge-transfer processes are combined using an exciplex-forming host and a thermally activated delayed fluorescent dopant, for fabricating efficient fluorescent organic light-emitting diodes along with the reduced efficiency roll-off at high current densities. Extra conversion on the host from triplet exciplexes to singlet exciplexes followed by energy transfer to the dopant reduces population of triplet excitons on dopant molecules, thereby reducing the triplet exciton annihilations at high current densities.

RESUMEN

Highly efficient organic/inorganic hybrid perovskite light-emitting diodes (PeLEDs) based on graphene anode are developed for the first time. Chemically inert graphene avoids quenching of excitons by diffused metal atom species from indium tin oxide. The flexible PeLEDs with graphene anode on plastic substrate show good bending stability; they provide an alternative and reliable flexible electrode for highly efficient flexible PeLEDs.

RESUMEN

A study of hybrid inverted quantum-dot (QD) light-emitting diodes constructed with and without Al2O3 interlayers is presented. The Al2O3 interlayers are deposited at ZnO/QDs or/and QDs/4,4'-bis(carbazol-9-yl)biphenyl interfaces, resulting in large improvement of device performance, including luminance, current efficiency, and device lifetime. Especially, the devices with QD emitters sandwiched by two Al2O3 layers exhibits outstanding performance, the longest operation lifetime, and mediate efficiency. The maximum current efficiency of 15.3 cd/A is obtained, an enhancement factor of 35% in comparison to that (11.3 cd/A) of conventional device without Al2O3 layer. Moreover, device lifetime is also largely enhanced, over 110 000 h for the device containing two Al2O3 interlayers, nearly 40% enhancement relative to that of conventional device that shows a lifetime of only 80 000 h. On the basis of electrical property and photoluminescence spectroscopy studies, we demonstrate that the Al2O3 interlayers play crucial roles in suppressing the leakage current across the device and reducing exciton quenching induced by ZnO.

RESUMEN

Highly efficient, simplified, solution-processed thermally activated delayed-fluorescence organic light-emitting diodes can be realized by using pure-organic thermally activated delayed fluorescence emitters and a multifunctional buffer hole-injection layer, in which high EQE (≈24%) and current efficiency (≈73 cd A(-1) ) are demonstrated. High-efficiency fluorescence red-emitting and blue-emitting devices can also be fabricated in this manner.

RESUMEN

Substrates can significantly affect the electronic properties of organic semiconductors. In this paper, we report the effects of contact-induced doping, arising from charge transfer between a high work function hole extraction layer (HEL) and the organic active layer, on organic photovoltaic device performance. Employing a high work function HEL is found to increase doping in the active layer and decrease photocurrent. Combined experimental and modeling investigations reveal that higher doping increases polaron-exciton quenching and carrier recombination within the field-free region. Consequently, there exists an optimal HEL work function that enables a large built-in field while keeping the active layer doping low. This value is found to be ~0.4 eV larger than the pinning level of the active layer material. These understandings establish a criterion for optimal design of the HEL when adapting a new active layer system and can shed light on optimizing performance in other organic electronic devices.