RESUMO
Rationally tuning the emission position and narrowing the full width at half-maximum (FWHM) of an emitter is of great importance for many applications. By synergistically improving rigidity, strengthening the resonant strength, inhibiting molecular bending and rocking, and destabilizing the HOMO energy level, a deep-blue emitter (CZ2CO) with a peak wavelength of 440â nm and an ultranarrow spectral FWHM of 16â nm (0.10â eV) was developed via intramolecular cyclization in a carbonyl/N resonant core (QAO). The dominant υ0-0 transition character of CZ2CO gives a Commission Internationale de I'Éclairage coordinates (CIE) of (0.144, 0.042), nicely complying with the BT.2020 standard. Moreover, a hyper-fluorescent device based on CZ2CO shows a high maximum external quantum efficiency (EQEmax ) of 25.6 % and maintains an EQE of 22.4 % at a practical brightness of 1000â cd m-2 .
RESUMO
The development of photoinduced luminescent radicals with dynamic emission color is still challenging. Herein we report a novel molecular radical system (TBIQ) that shows photo-controllable luminescence, leading to a wide range of ratiometric color changes via light excitation. The conjugated skeleton of TBIQ is decorated with steric-demanding tertiary butyl groups that enable appropriate intermolecular interaction to make dynamic intermolecular coupling possible for controllable behaviors. We reveal that the helicenic pseudo-planar conformation of TBIQ experiences a planarization process after light excitation, leading to more compactly stacked supermolecules and thus generating radicals via intermolecular charge transfer. The photo-controllable luminescent radical system is employed for a high-level information encryption application. This study may offer unique insight into molecular dynamic motion for optical manufacturing and broaden the scope of smart-responsive materials for advanced applications.
RESUMO
Upon fusing the pyrazinyl pyrazole entity in giving pyrazolo[3,4-f]quinoxaline chelate, the corresponding Os(II) based NIR emitter exhibited "invisible" and efficient electroluminescence with a peak maximum at 811â nm. A maximum external quantum efficiency of 0.97 % and a suppressed efficiency roll-off till a current density of 300â mA cm-2 was also exhibited.
RESUMO
Four blue-emissive iridium(III) complexes bearing a 3,3'-(1,3-phenylene)bis[1-isopropyl-6-(trifluoromethyl)-3H-imidazo[4,5-b]pyridin-2-ylidene]-based pincer chelate, which are derived from PXn·H3(PF6)2, where n = 1-4, and a cyclometalating chelate given from 9-[6-[5-(trifluoromethyl)-2λ2-pyrazol-3-yl]pyridin-2-yl]-9H-carbazole [(PzpyCz)H2], were successfully synthesized and employed as both an emissive dopant and a sensitizer in the fabrication of organic light-emitting diode (OLED) devices. These functional chelates around a IrIII atom occupied two mutually orthogonal coordination arrangements and adopted the so-called bis-tridentate architectures. Theoretical studies confirmed the dominance of the electronic transition by the pincer chelates, while the dianionic PzpyCz chelate was only acting as a spectator group. Phosphorescent OLED devices with [Ir(PX3)(PzpyCz)] (B3) as the dopant gave a maximum external quantum efficiency (EQE) of 21.93% and CIExy of (0.144, 0.157) and was subjected to only â¼10% of roll-off in efficiency at a high current density of 1000 cd m-2. Blue-emissive narrow-band hyperphosphorescence was also obtained using B3 as an assistant sensitizer and ν-DABNA as a terminal emitter, giving both an improved EQE of 26.17% and CIExy of (0.116, 0.144), confirming efficient Förster resonance energy transfer in this hyperdevice.
RESUMO
Three multi-dentate coordinated chelates LnH2 (n = 1, 2, and 3), comprising a linked 1-(pyridin-2-yl)ethylbenzene and one pyrazolyl pyridine unit and showing either tridentate or tetradentate coordination modes, are successfully designed and synthesized. Dinuclear Ir(III) complexes [Ir(κ4-Ln)(µ-Cl)]2 bearing tetradentate coordinated κ4-Ln chelate (2a, n = 1; 2b, n = 2; 2c, n = 3) were next obtained en route from the respective intermediate [Ir(κ3-LnH)Cl(µ-Cl)]2 bearing the tridentate coordinated κ3-LnH chelate (1a, n = 1; 1b, n = 2; 1c, n = 3). Next, mononuclear Ir(III) complexes Ir(κ4-Ln)(thd) (3a, n = 1; 3b, n = 2; 3c, n = 3) with the tetradentate chelate were obtained upon treatment of 2 with 2,2,6,6-tetramethyl-3,5-heptanedione (thd)H in the presence of K2CO3. Concurrently, methylation of 2c in the presence of MeI and nBu4NCl afforded tridentate Ir(κ3-L3HMe)Cl3 (4) and, next, can be converted to tetradentate Ir(κ4-L3Me)Cl2 (5) by further cyclometalation and HCl elimination in refluxing diethylene glycol monoethyl ether solution. The Ir(III) complexes 3a, 4, and 5 were unambiguously identified using spectroscopic methods, together with single-crystal X-ray structural analyses on Ir(III) derivatives 3a, 4, and 5. Their photophysical and ,electrochemical properties and device fabrication properties were also investigated and compared with results from theoretical studies.
RESUMO
In this work, we report a series of bis-tridentate Ir(III) metal complexes, comprising a dianionic pyrazole-pyridine-phenyl tridentate chelate and a monoanionic chelate bearing a peripheral carbene and carboline coordination fragment that is linked to the central phenyl group. All these Ir(III) complexes were synthesized with an efficient one-pot and two-step method, and their emission hue was fine-tuned by variation of the substituent at the central coordination entity (i.e., pyridinyl and phenyl group) of each of the tridentate chelates. Their photophysical and electrochemical properties, thermal stabilities and electroluminescence performances are examined and discussed comprehensively. The doped devices based on [Ir(cbF)(phyz1)] (Cb1) and [Ir(cbB)(phyz1)] (Cb4) give a maximum external quantum efficiency (current efficiency) of 16.6% (55.2 cd/A) and 13.9% (43.8 cd/A), respectively. The relatively high electroluminescence efficiencies indicate that bis-tridentate Ir(III) complexes are promising candidates for OLED applications.
RESUMO
A new ternary acceptor (A)-donor (D)-acceptor (A) asymmetrically twisted deep-blue emitting molecule, PPI-2BI, was synthesized by attaching two electrophilic benzimidazole (BI) units to the C2 and N1 positions of a phenanthroimidazole (PI) donor unit. Profiting from the enhanced D-A electronic coupling, the electron injecting and transporting abilities of the new triangle-shaped A-D-A molecule are considerably improved and the molecule shows high photoluminescence (PL) and electroluminescence (EL) efficiencies. By using PPI-2BI as a non-doped emitting layer (EML), the resulting organic light-emitting device exhibits emission with color coordinates of (0.158, 0.124) and a maximum external quantum efficiency (EQE), current efficiency (CE), and power efficiency (PE) of 4.63 %, 4.98â cd A-1 , and 4.82â lm W-1 , respectively. Additionally, a simple bilayer device using PPI-2BI as both the EML and the electron-transporting layer (ETL) also shows an EQE of 3.81 % with little changes to the color purity. Remarkably, a PPI-2BI-based doped device emits efficient near-ultraviolet EL with color coordinates of (0.154, 0.047) and an EQE of 4.12 %, which is comparable to that of the best reported near-UV emitting devices.
RESUMO
Donor-acceptor (D-A) molecular architecture has been shown to be an effective strategy for obtaining high-performance electroluminescent materials. In this work, two D-A molecules, Ph-BPA-BPI and Py-BPA-BPI, have been synthesized by attaching highly fluorescent phenanthrene or pyrene groups to the C6- and C9-positions of a locally excited-state emitting phenylamine-phenanthroimidazole moiety. Equipped with good physical and hybridized local and charge-transfer properties, both molecules show high performances as blue emitters in nondoped organic light-emitting devices (OLEDs). An OLED using Ph-BPA-BPI as the emitting layer exhibits deep-blue emission with CIE coordinates of (0.15, 0.08), and a maximum external quantum efficiency (EQE), current efficiency (CE), and power efficiency (PE) of 4.56 %, 3.60â cd A(-1) , and 3.66â lm W(-1) , respectively. On the other hand, a Py-BPA-BPI-based, sky-blue OLED delivers the best results among nondoped OLEDs with CIEy values of < 0.3 reported so far, for which a very low turn-on voltage of 2.15â V, CIE coordinates of (0.17, 0.29), and maximum CE, PE, and EQE values of 10.9â cd A(-1) , 10.5â lm W(-1) , and 5.64 %, were achieved, respectively. More importantly, both devices show little or even no efficiency roll-off and high singlet exciton-utilizing efficiencies of 36.2 % for Ph-BPA-BPI and 39.2 % for Py-BPA-BPI.
RESUMO
Solar-driven CO2 reduction to yield high-value chemicals presents an appealing avenue for combating climate change, yet achieving selective production of specific products remains a significant challenge. We showcase two osmium complexes, przpOs, and trzpOs, as CO2 reduction catalysts for selective CO2-to-methane conversion. Kinetically, the przpOs and trzpOs exhibit high CO2 reduction catalytic rate constants of 0.544 and 6.41 s-1, respectively. Under AM1.5 G irradiation, the optimal Si/TiO2/trzpOs have CH4 as the main product and >90% Faradaic efficiency, reaching -14.11 mA cm-2 photocurrent density at 0.0 VRHE. Density functional theory calculations reveal that the N atoms on the bipyrazole and triazole ligands effectively stabilize the CO2-adduct intermediates, which tend to be further hydrogenated to produce CH4, leading to their ultrahigh CO2-to-CH4 selectivity. These results are comparable to cutting-edge Si-based photocathodes for CO2 reduction, revealing a vast research potential in employing molecular catalysts for the photoelectrochemical conversion of CO2 to methane.
RESUMO
Deep-blue multi-resonance (MR) emitters with stable and narrow full-width-at-half-maximum (FWHM) are of great importance for widening the color gamut of organic light-emitting diodes (OLEDs). However, most planar MR emitters are vulnerable to intermolecular interactions from both the host and guest, causing spectral broadening and exciton quenching in thin films. Their emission in the solid state is environmentally sensitive, and the color purity is often inferior to that in solutions. Herein, a molecular design strategy is presented that simultaneously narrows the FWHM and suppresses intermolecular interactions by combining intramolecular locking and peripheral shielding within a carbonyl/nitrogen-based MR core. Intramolecularly locking carbonyl/nitrogen-based bears narrower emission of 2,10-dimethyl-12,12-diphenyl-4H-benzo[9,1]quinolizino[3,4,5,6,7-defg]acridine-4,8(12H)-dione in solution and further with peripheral-shielding groups, deep-blue emitter (12,12-diphenyl-2,10-bis(9-phenyl-9H-fluoren-9-yl)-4H-benzo[9,1]quinolizino[3,4,5,6,7-defg]acridine-4,8(12H)-dione, DPQAO-F) exhibits ultra-pure emission with narrow FWHM (c.a., 24 nm) with minimal variations (∆FWHM ≤ 3 nm) from solution to thin films over a wide doping range. An OLED based on DPQAO-F presents a maximum external quantum efficiency (EQEmax) of 19.9% and color index of (0.134, 0.118). Furthermore, the hyper-device of DPQAO-F exhibits a record-high EQEmax of 32.7% in the deep-blue region, representing the first example of carbonyl/nitrogen-based OLED that can concurrently achieve narrow bandwidth in the deep-blue region and a high electroluminescent efficiency surpassing 30%.
RESUMO
Simultaneously realizing improved carrier mobility and good photoluminescence (PL) efficiency in red thermally activated delayed-fluorescence (TADF) emitters remains challenging but important. Herein, two isomeric orange-red TADF emitters, oPDM and pPDM, with the same basic donor-acceptor backbone but a pyrimidine (Pm) attachment at different positions are designed and synthesized. The two emitters show similarly good PL properties, including narrow singlet-triplet energy offsets (0.11 and 0.15 eV) and high photoluminescence quantum yields (ca. 100 and 88%) in doped films. An orange-red organic light-emitting diode (OLED) employing oPDM as an emitter achieves an almost twice as high maximum external quantum efficiency (28.2%) compared with that of a pPDM-based OLED. More balanced carrier-transporting properties are responsible for their contrasting device performances, and the position effect of the Pm substituent leads to significantly distinct molecular packing behaviors in the aggregate states and different carrier mobilities.
RESUMO
To achieve high-efficiency deep-blue electroluminescence satisfying Rec.2020 standard blue gamut, two thermally activated delayed fluorescent (TADF) emitters are developed: 5-(2,12-di-tert-butyl-5,9-dioxa-13b-boranaphtho[3,2,1-de]anthracen-7-yl)-10,10-diphenyl-5,10-dihydrodibenzo[b,e][1,4]azasiline (TDBA-PAS) and 10-(2,12-di-tert-butyl-5,9-dioxa-13b-boranaphtho[3,2,1-de]anthracen-7-yl)-9,9-diphenyl-9,10-dihydroacridine (TDBA-DPAC). Inheriting from their parented organoboron multi-resonance core, both emitters show very promising deep-blue emissions with relatively narrow full width at half-maximum (FWHM, ≈50 nm in solution), high photoluminescence quantum yield (up to 92.3%), and short emission lifetime (≤2.49 µs) with fast reverse intersystem crossing (>106 s-1 ) in doped films. More importantly, replacing the spiro-centered sp3 C atom (TDBA-DPAC) with the larger-radius sp3 Si atom (TDBA-PAS), enhanced conformational heterogeneities in bulky-group-shielded TADF molecules are observed in solution, doped film, and device. Consequently, OLEDs based on TDBA-PAS retain high maximum external quantum efficiencies ≈20% with suppressed efficiency roll-off and color index close to Rec.2020 blue gamut over a wide doping range of 10-50 wt%. This study highlights a new strategy to restrain spectral broadening and redshifting and efficiency roll-off in the design of deep-blue TADF emitters.
RESUMO
Enhancing the reverse intersystem crossing (RISC) process of thermally activated delayed fluorescent (TADF) emitters is an effective approach to realize efficient organic light-emitting diodes (OLEDs) with low efficiency roll-off. In this work, we designed two novel TADF emitters, SAT-DAC and SATX-DAC, via a spiro architecture. Efficient maximum external quantum efficiencies (EQEs) of 22.6 and 20.9% with reduced efficiency roll-off (EQEs of 17.9 and 17.0% at 1000 cd m-2) were achieved via a "two-RISC-channel" strategy. X-ray diffraction shows close donor (D)/acceptor (A) spacing and suitable D/A orientation in crystals of the two emitters favoring both intra- and intermolecular through-space charge transfer (TSCT) processes. Transient photoluminescence decay measurements show that both emitters have two RISC channels leading to kISCT exceeding 106 s-1. These results suggest that the "two-RISC-channel" design can be a novel approach for enhancing performance of TADF emitters, in particular at high excitation densities.
RESUMO
Parasitic diseases have been widely epidemic in China with a long history. Great endeavours made in past 70 years led to significant decrease in morbidity and mortablity caused by several major parasitic diseases, while challenges existed to eliminate parasitic diseases. Surveillance-response system has play a crucial role in identifying public health problems, ascertaining the distribution and epidemic dynamics, discovering outbreaks and epidemic anomalies, evaluating the effects of on-site intervention activities and identifying risk factors. In this article, we reviewed the progress of the surveillance system for parasitic diseases, analysed the role of NIPD in the construction and application of surveillance-response system of parasitic diseases through elaborating the surveillance activities and typical surveillance-response events led by NIPD. Suggestion and comments for improve the surveillance-response system were put forward for further control or elimination of parasitic diseases.
Assuntos
Academias e Institutos , Monitoramento Epidemiológico , Programas Governamentais , Programas Nacionais de Saúde , Doenças Parasitárias , Animais , China/epidemiologia , Humanos , Doenças Parasitárias/epidemiologia , Doenças Parasitárias/prevenção & controleRESUMO
Phosphorescence/fluorescence hybrid white organic light-emitting diodes (OLEDs) are highly appealing for solid-state lighting. One major challenge is how to fully utilize the electrically generated excitons for light output. Herein, an efficient strategy to realize full exciton radiation is successfully revealed by a judicious molecular design and suitable device engineering. A blue host emitter TP-PPI is designed and synthesized, exhibiting a near 100% photoluminescence quantum yield and a high triplet energy level, enabling high-performance blue fluorescence and sensitization of a yellow phosphorescent dopant. Full exciton radiation in hybrid white OLEDs is demonstrated with a single emitting layer formed by doping a yellow phosphor (PO-01) into TP-PPI. Near 100% exciton utilization and state-of-the-art external quantum efficiency of 27.5% are achieved with the high-efficiency blue-emitting host and an electron-trap engineered device architecture.
RESUMO
Sky-blue and blue-emitting, carbazolyl functionalized, bis-tridentate Ir(III) phosphors Cz-1-Cz-3 with bright emission and short radiative lifetime are successfully synthesized in a one-pot manner. They exhibit very high photostability against UV-vis irradiation in degassed toluene, versus both green and true-blue-emitting reference compounds, i.e., fac-[Ir(ppy)3] and mer-[Ir(pmp)3]. Organic light-emitting diodes (OLEDs) based on Cz-2 exhibit maximum external quantum efficiency (EQE) of 21.6%, EQE of 15.1% at 100 cd m-2, and with CIE x,y coordinates of (0.17, 0.25). This study provides a conceptual solution to the exceedingly stable and efficient blue phosphor. It is promising that long lifespan blue OLED based on these emitters can be attained with further engineering of devices suitable for commercial application.
RESUMO
A novel host material featuring a spiro-annulated benzimidazole configuration is exploited for blue phosphorescent organic light-emitting devices (PhOLEDs). The new material exhibits a high triplet energy (3.07 eV) and a bipolar characteristic and is effective as the host for FIrpic-, FIr6- and FK306-based blue PhOLEDs with high performances.
RESUMO
Two novel D-σ-A host materials 11,11-bis(9-phenyl-9H-carbazol-3-yl)-11H-benzo[4,5]imidazo[1,2-a]indole (BII-BCz) and 4,4'-(11H-benzo[4,5]imidazo[1,2-a]indole-11,11-diyl)bis(N,N-diphenylaniline) (BII-TPA) are synthesized by using the sp3 carbon attached to a newly designed 11H-benzo[4,5]imidazo[1,2-a]indole building block to link two electron-donating groups. The resulting materials feature high triplet energy levels, good thermal properties and suitable photophysical properties as universal hosts for full-color phosphorescent organic light-emitting diodes (OLEDs). Both BII-BCz and BII-TPA reveal excellent performances in blue, green, yellow, orange and red phosphorescent OLEDs with the same device structure. The employment of the new D-σ-A materials as single hosts in white OLEDs with a simple device structure allows us to achieve state-of-the-art performances. A single-emissive-layer white device based on BII-BCz demonstrates the highest performance with an external quantum efficiency up to 28.2% at 1000 cd m-2. Furthermore, this device displays extremely stable emission spectra, with a ΔCIE of only (0.009, 0.005) from 1000 to 10 000 cd m-2.
RESUMO
Organic materials containing arylamines have been widely used as hole-transporting materials as well as emitters in organic light-emitting devices (OLEDs). However, it has been pointed out that the C-N bonds in these arylamines can easily suffer from degradation in excited states, especially in deep-blue OLEDs. In this work, phenanthro[9,10-d]imidazole (PI) is proposed as a potential donor with higher stability than those of arylamines. Using PI as the donor, a donor-acceptor type deep-blue fluorophore 1-phenyl-2-(4â³-(1-phenyl-1H-benzo[d]imidazol-2-yl)-[1,1':4',1â³-terphenyl]-4-yl)-1H-phenanthro[9,10-d]imidazole (BITPI) is designed and synthesized. Results from UV-aging test on neat films of BITPI and other three arylamine compounds demonstrate that PI is indeed a more stable donor comparing to common arylamines. An OLED using BITPI as an emitter exhibits good device performances (EQE over 7%) with stable deep-blue emission (color index: (0.15, 0.13)) and longer operation lifetime than the similarly structured device using arylamine-based emitter. Single-organic layer device based on BITPI also shows superior performances, which are comparable to the best results from the arylamine-based donor-acceptor emitters, suggesting that PI is a stable donor with good hole transport/injection capability.