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1.
Chemistry ; 30(2): e202302943, 2024 Jan 08.
Artículo en Inglés | MEDLINE | ID: mdl-37803935

RESUMEN

Excellent stability is an essential premise for organic diradicals to be used in organic electronic and spintronic devices. We have attached two tris(2,4,6-trichlorophenyl)methyl (TTM) radical building blocks to the two sides of perylene bisimide (PBI) bridges and obtained two regioisomeric diradicals (1,6-TTM-PBI and 1,7-TTM-PBI). Both of the isomers show super stability rather than the monomeric TTM under ambient conditions, due to the increased conjugation and the electron-withdrawing effects of the PBI bridges. The diradicals show distinct and reversible multistep redox processes, and a spectro-electrochemistry investigation revealed the generation of organic mixed-valence (MV) species during reduction processes. The two diradicals have singlet ground states, very small singlet-triplet energy gaps (ΔES-T ) and a pure open-shell character (with diradical character y0 =0.966 for 1,6-TTM-PBI and 0.967 for 1,7-TTM-PBI). This work opens a window to developing very stable diradicals and offers the opportunity of their further application in optical, electronic and magnetic devices.

2.
Angew Chem Int Ed Engl ; : e202407502, 2024 May 09.
Artículo en Inglés | MEDLINE | ID: mdl-38721850

RESUMEN

Currently, much research effort has been devoted to improving the exciton utilization efficiency and narrowing the emission spectra of ultraviolet (UV) fluorophores for organic light-emitting diode (OLED) applications, while almost no attention has been paid to optimizing their light out-coupling efficiency. Here, we developed a linear donor-acceptor-donor (D-A-D) triad, namely CDFDB, which possesses high-lying reverse intersystem crossing (hRISC) property. Thanks to its integrated narrowband UV photoluminescence (PL) (λPL: 397 nm; FWHM: 48 nm), moderate PL quantum yield (ϕPL: 72 %, Tol), good triplet hot exciton (HE) conversion capability, and large horizontal dipole ratio (Θ//: 92 %), the OLEDs based on CDFDB not only can emit UV electroluminescence with relatively good color purity (λEL: 398 nm; CIEx,y: 0.161, 0.040), but also show a record maximum external quantum efficiency (EQEmax) of 12.0 %. This study highlights the important role of horizontal dipole orientation engineering in the molecular design of HE UV-OLED fluorophores.

3.
Phys Chem Chem Phys ; 25(6): 4598-4603, 2023 Feb 08.
Artículo en Inglés | MEDLINE | ID: mdl-36723048

RESUMEN

The stability and degradation mechanism of phosphorescent organic light emitting diodes (OLEDs) has been an unresolved problem in the past decades. Here, we found that electron accumulation at the interface between the electron blocking layer and the emitting layer is one of the reasons for device degradation. By inserting a thin layer with a shallower LUMO level than that of the electron transporting layer between the emitting layer and the electron transporting layer, we successfully reduced the density of electrons at the interface and greatly improved the lifetime of the resulting green phosphorescent OLEDs. The half decay lifetime LT50 at the initial luminance of 1000 cd m-2 reached as high as 399 h, which is 1.7 times longer than that of the compared device without a thin layer.

4.
Phys Chem Chem Phys ; 25(43): 29451-29458, 2023 Nov 08.
Artículo en Inglés | MEDLINE | ID: mdl-37882197

RESUMEN

The lifetime of blue organic light-emitting diodes (OLEDs) has always been a big challenge in practical applications. Blue OLEDs based on triplet-triplet annihilation (TTA) up-conversion materials have potential to achieve long lifetimes due to fusing two triplet excitons to one radiative singlet exciton, but there is a lack of an in-depth understanding of exciton dynamics on degradation mechanisms. In this work, we established a numerical model of exciton dynamics to study the impact factors in the stability of doped blue OLEDs based on TTA up-conversion hosts. By performing transient electroluminescence experiments, the intrinsic parameters related to the TTA up-conversion process of aging devices were determined. By combining the change of excess charge density in the emitting layer (EML) with aging time, it is concluded that the TTA materials are damaged by the excess electrons in the EML during ageing, which is the main degradation mechanism of OLEDs. This work provides a theoretical basis for preparing long-lifetime blue fluorescent OLEDs.

5.
Phys Chem Chem Phys ; 25(39): 26878-26884, 2023 Oct 11.
Artículo en Inglés | MEDLINE | ID: mdl-37782517

RESUMEN

Aggregation-induced delayed fluorescence (AIDF) materials have great potential in non-doped OLEDs due to their high photoluminescence (PL) quantum efficiency in film, high exciton utilization in the aggregated state and negligible efficiency roll-off at high luminance. However, their efficient mechanism in OLEDs is not yet well understood. Here, the exciton dynamics are used to investigate the electroluminescence (EL) mechanism of an AIDF emitter (4-(10H-phenoxazin-10-yl)phenyl)-(9-phenyl-9H-carbazol-3-yl)methanone (CP-BP-PXZ) in detail. It can be seen that the high efficiency and negligible efficiency roll-off in non-doped OLEDs based on CP-BP-PXZ as the emitter are ascribed to the effective reverse intersystem crossing (RISC) from high level triplet T2 to singlet S1 in the aggregated state. Furthermore, CP-BP-PXZ also exhibits excellent properties as a phosphor host due to its good AIDF properties. Thus, high-efficiency red phosphorescent OLEDs with low roll-off efficiency are successfully fabricated based on CP-BP-PXZ as the host. The maximum external quantum efficiency (EQEmax) reaches 23% and is maintained at 21% at a luminance of 1000 cd m-2.

6.
Phys Chem Chem Phys ; 21(48): 26413-26419, 2019 Dec 11.
Artículo en Inglés | MEDLINE | ID: mdl-31774087

RESUMEN

Magnetic field effects in nonmagnetic organic semiconductors (OMFEs) are attracting increasing attention because of the fingerprint characteristics of their line shapes when they are used to analyze the dynamic processes of organic photodiodes. However, the origin and correlation of OMFEs on carriers and excitons are currently still major challenges for researchers. In this study, we strategically designed exciplex-based single-carrier devices to effectively separate carriers and excitons and investigate their OMFEs and relationships. It is found that the obvious positive magneto-conductance (MC) with illumination is not only related to the formation of charge transfer state (CT) excitons, but is also caused by the secondary recombination process between dissociated carriers from the photo-generated excitons and the injected carriers. Moreover, a negative MC appears under dark conditions, reflecting the intrinsic magnetic field effects on carrier transport. The relationships of the OMFEs with the excitons and carriers were further studied by measuring the incident-wavelength dependent photo-induced MC and the magneto-photoluminescence (MPL) of the exciplex films. The two films show similar amplitude-dependent curves, which are contributed by their donor-acceptor absorption properties. Moreover, the strong triplet-polaron annihilation (TPA) processes exhibited in this device afford different amplitude-dependent photo-induced MCs.

7.
Arch Insect Biochem Physiol ; 92(1): 65-84, 2016 May.
Artículo en Inglés | MEDLINE | ID: mdl-27110952

RESUMEN

The ATP-binding cassette (ABC) transporters are important transmembrane proteins encoded by a supergene family. The majority of ABC proteins are primary active transporters that bind and hydrolyze ATP to mediate the efflux of a diverse range of substrates across lipid membranes. In this study, we cloned and characterized a putative multidrug resistance associated protein 1 (MRP1) from Rhopalosiphum padi encoded by ABCC1. Structural analysis showed that this protein has structural features typical of the ABC transporter family. Phylogenetic analysis indicated that the amino acid sequence was highly similar that of the corresponding protein from Acyrthosiphon pisum. Real-time quantitative polymerase chain reaction (PCR) analysis showed that ABCC1 was expressed throughout all R. padi developmental stages, with the highest level of expression in the fourth larval instar. We also examined ABCC1 expression in four different tissue types and found that it was most highly expressed in the midgut. Exposing R. padi to imidacloprid and chlorpyrifos increased ABCC1 expression. Furthermore, ABCC1 expression was higher in the imidacloprid-resistant (IR) and chlorpyrifos-resistant (CR) strains than in an insecticide-susceptible strain (SS) of R. padi. Exposing R. padi to verapamil in combination with insecticides significantly increased the toxicity of the insecticides. The respective synergy factor of CR and IR R. padi strain was 1.33 and 1.26, which was lower than that (2.72 and 1.64, respectively) of the SS. Our results clarify the biological function of ABCC1 in R. padi, particularly its role in insecticide resistance, and suggest novel strategies for pest management that use ABC transporter inhibitors to increase the effectiveness of insecticides.


Asunto(s)
Áfidos/efectos de los fármacos , Áfidos/genética , Bloqueadores de los Canales de Calcio/farmacología , Proteínas de Insectos/genética , Proteínas Asociadas a Resistencia a Múltiples Medicamentos/genética , Secuencia de Aminoácidos , Animales , Áfidos/crecimiento & desarrollo , Áfidos/metabolismo , Cloropirifos/farmacología , Clonación Molecular , ADN Complementario/genética , ADN Complementario/metabolismo , Sinergismo Farmacológico , Imidazoles/farmacología , Proteínas de Insectos/química , Proteínas de Insectos/metabolismo , Insecticidas/farmacología , Larva/efectos de los fármacos , Larva/genética , Larva/crecimiento & desarrollo , Larva/metabolismo , Conformación Molecular , Proteínas Asociadas a Resistencia a Múltiples Medicamentos/química , Proteínas Asociadas a Resistencia a Múltiples Medicamentos/metabolismo , Neonicotinoides , Nitrocompuestos/farmacología , Ninfa/efectos de los fármacos , Ninfa/genética , Ninfa/crecimiento & desarrollo , Ninfa/metabolismo , Filogenia , Alineación de Secuencia , Verapamilo/farmacología
8.
Pestic Biochem Physiol ; 132: 89-95, 2016 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-27521918

RESUMEN

The bird cherry-oat aphid, Rhopalosiphum padi (L.), is one of the most important wheat pests. This aphid damages through direct feeding and by transmitting the Barley yellow dwarf virus (BYDV). Both types of damage significantly reduce the quality and yield of wheat crops globally. Insecticides are the primary method of controlling the bird cherry-oat aphid in China, yet this aphid species has developed resistance to different types of insecticides, especially organophosphates and carbamates. In the last decade, control of R. padi depends primarily on the spray of neonicotinoid insecticides, however, research on the resistance of R. padi to neonicotinoids has been limited. In this study, the full lengths of seven α-subunit (Rpα1, Rpα2, Rpα3, Rpα4, Rpα5, Rpα7-1, and Rpα7-2) and one ß-subunit (Rpß1) genes from R. padi were obtained with RT-PCR and RACE techniques. Sequence analysis showed that these genes had all the characteristics of the nAChR gene family and were highly homologous with the reported nAChR genes from other insects, and alternative splicing was detected in Rpα3 and Rpα5 subunits. Analysis of the cDNA sequence of the extracellular region of the nicotinic acetylcholine receptor ß1 subunit gene from 120 R. padi field samples collected in 11 Provinces revealed 17 single nucleotides polymorphism (SNP) sites, of which seven were amino acid polymorphism sites (V53I, V53G, N54T, A60T, F61L, W79C, and V83I) and two were in the loop D region (W79C and V83I). The current study will facilitate further studies on the molecular mechanisms of targeted resistance of the aphid to neonicotinoid insecticides.


Asunto(s)
Áfidos/genética , Genes de Insecto/genética , Receptores Colinérgicos/genética , Empalme Alternativo/genética , Animales , China , Clonación Molecular , Femenino , Polimorfismo de Nucleótido Simple/genética
9.
Adv Mater ; 35(23): e2212084, 2023 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-36924360

RESUMEN

Nonfullerene-acceptor-based organic solar cells (NFA-OSCs) are now set off to the 20% power conversion efficiency milestone. To achieve this, minimizing all loss channels, including nonradiative photovoltage losses, seems a necessity. Nonradiative recombination, to a great extent, is known to be an inherent material property due to vibrationally induced decay of charge-transfer (CT) states or their back electron transfer to the triplet excitons. Herein, it is shown that the use of a new conjugated nitroxide radical polymer with 2,2,6,6-tetramethyl piperidine-1-oxyl side groups (GDTA) as an additive results in an improvement of the photovoltaic performance of NFA-OSCs based on different active layer materials. Upon the addition of GDTA, the open-circuit voltage (VOC ), fill factor (FF), and short-circuit current density (JSC ) improve simultaneously. This approach is applied to several material systems including state-of-the-art donor/acceptor pairs showing improvement from 15.8% to 17.6% (in the case of PM6:Y6) and from 17.5% to 18.3% (for PM6:BTP-eC9). Then, the possible reasons behind the observed improvements are discussed. The results point toward the suppression of the CT state to triplet excitons loss channel. This work presents a facile, promising, and generic approach to further improve the performance of NFA-OSCs.

10.
BMC Biotechnol ; 12: 39, 2012 Jul 06.
Artículo en Inglés | MEDLINE | ID: mdl-22768962

RESUMEN

BACKGROUND: Widely used restriction-dependent cloning methods are labour-intensive and time-consuming, while several types of ligase-independent cloning approaches have inherent limitations. A rapid and reliable method of cloning native DNA sequences into desired plasmids are highly desired. RESULTS: This paper introduces ABI-REC, a novel strategy combining asymmetric bridge PCR with intramolecular homologous recombination in bacteria for native DNA cloning. ABI-REC was developed to precisely clone inserts into defined location in a directional manner within recipient plasmids. It featured an asymmetric 3-primer PCR performed in a single tube that could robustly amplify a chimeric insert-plasmid DNA sequence with homologous arms at both ends. Intramolecular homologous recombination occurred to the chimera when it was transformed into E.coli and produced the desired recombinant plasmids with high efficiency and fidelity. It is rapid, and does not involve any operational nucleotides. We proved the reliability of ABI-REC using a double-resistance reporter assay, and investigated the effects of homology and insert length upon its efficiency. We found that 15 bp homology was sufficient to initiate recombination, while 25 bp homology had the highest cloning efficiency. Inserts up to 4 kb in size could be cloned by this method. The utility and advantages of ABI-REC were demonstrated through a series of pig myostatin (MSTN) promoter and terminator reporter plasmids, whose transcriptional activity was assessed in mammalian cells. We finally used ABI-REC to construct a pig MSTN promoter-terminator cassette reporter and showed that it could work coordinately to express EGFP. CONCLUSIONS: ABI-REC has the following advantages: (i) rapid and highly efficient; (ii) native DNA cloning without introduction of extra bases; (iii) restriction-free; (iv) easy positioning of directional and site-specific recombination owing to formulated primer design. ABI-REC is a novel approach to DNA engineering and gene functional analysis.


Asunto(s)
ADN/metabolismo , Ingeniería Genética , Reacción en Cadena de la Polimerasa/métodos , Animales , Secuencia de Bases , Clonación Molecular , ADN/química , Cartilla de ADN/metabolismo , Escherichia coli/genética , Escherichia coli/metabolismo , Genes Reporteros , Recombinación Homóloga , Datos de Secuencia Molecular , Miostatina/genética , Plásmidos/genética , Plásmidos/metabolismo , Regiones Promotoras Genéticas , Porcinos
11.
Opt Express ; 20(22): 24411-7, 2012 Oct 22.
Artículo en Inglés | MEDLINE | ID: mdl-23187204

RESUMEN

Highly efficient blue phosphorescent organic light-emitting diodes (PhOLEDs) with a multiple quantum well (MQW) structure were investigated. A peak external quantum efficiency (EQE) of 20.31%, current efficiency of 40.31 cd/A and power efficiency of 30.14 lm/W were achieved in the optimized device with two quantum wells (QWs). The obtained efficiencies are much higher than those of the control devices without QWs. More importantly, the MQW devices exhibit low efficiency roll-off. At a high luminance of 5000 cd/m(2), the EQE still keeps at a high value of 18.86% in the optimized MQW device, and the efficiency roll-off is only 7.14%, which is lower than that of 30.78% in the control device (reduced from 16.05% to 11.11%). Meanwhile, the maximum power efficiency of the optimized MQW device was also exhibited more than 54.80% improvement compared to the control device. The high efficiency and low efficiency roll-off are attributed to the effective confinement of charge carriers and excitons by the state-of-the-art MQWs.

12.
Front Optoelectron ; 15(1): 11, 2022 Apr 20.
Artículo en Inglés | MEDLINE | ID: mdl-36637599

RESUMEN

The transient electroluminescence (EL) technique is widely used to evaluate the carrier mobility in the field of organic light emitting diodes. The traditional analog detection strategy using oscilloscopes is generally limited since the background noise causes an underestimation of the mobility value. In this paper, we utilize time-correlated single-photon counting (TCSPC) to probe the transient EL for mobility calculation. The measurements on tris(8-hydroxyquinoline) aluminum (Alq3) show that the electron mobilities obtained using the TCSPC technique are slightly higher than those obtained from the analog method at all the investigated voltages. Moreover, the TCSPC mobilities demonstrate weaker dependence on the root of electrical field compared to the oscilloscope mobilities. These improvements are attributed to the unique principle of TCSPC, which quantifies the EL intensity by counting the number of single-photon pulses, improving its single-photon sensitivity and eliminating the negative impacts of electrical noise. These advantages make TCSPC a powerful technique in the characterization of time-resolved electroluminescence.

13.
Mater Horiz ; 9(9): 2376-2383, 2022 Aug 30.
Artículo en Inglés | MEDLINE | ID: mdl-35789246

RESUMEN

Aggregation-induced emission (AIE) materials are attractive for the fabrication of high efficiency organic light-emitting diodes (OLEDs) by harnessing "hot excitons" from the high-lying triplet exciton states (Tn, n ≥ 2) and high photoluminescence (PL) quantum efficiency in solid films. However, the electroluminescence (EL) efficiency of most AIE-based OLEDs does not meet our expectation due to some unrevealed exciton loss processes. Herein, we further enhance the efficiency of blue AIE-based OLEDs, and find experimentally and theoretically that the serious exciton loss is caused by the quenching of radiative singlet excitons and long-lived triplet excitons [singlet-triplet annihilation (STA)]. In order to suppress the STA process, 1-(2,5-dimethyl-4-(1-pyrenyl)phenyl)pyrene (DMPPP) with triplet-triplet annihilation up-conversion was doped in two AIE emitters to reduce the triplet excitons on the lowest triplet excited state (T1) of AIE molecules. It can be seen that the external quantum efficiency (EQE) of the resulting blue OLEDs was enhanced to 11.8% with CIE coordinates of (0.15, 0.07) and a negligible efficiency roll-off, realizing the efficiency breakthrough of deep-blue AIE-based OLEDs. This work establishes a physical insight in revealing the exciton loss processes and the fabrication of high-performance AIE-based OLEDs.

14.
Sci Bull (Beijing) ; 66(20): 2090-2098, 2021 Oct 30.
Artículo en Inglés | MEDLINE | ID: mdl-36654267

RESUMEN

Achieving high-efficiency deep blue emitter with CIEy < 0.06 (CIE, Commission Internationale de L'Eclairage) and external quantum efficiency (EQE) >10% has been a long-standing challenge for traditional fluorescent materials in organic light-emitting diodes (OLEDs). Here, we report the rational design and synthesis of two new deep blue luminogens: 4-(10-(4'-(9H-carbazol-9-yl)-2,5-dimethyl-[1,1'-biphenyl]-4-yl)anthracen-9-yl)benzonitrile (2M-ph-pCzAnBzt) and 4-(10-(4-(9H-carbazol-9-yl)-2,5-dimethylphenyl)anthracen-9-yl)benzonitrile (2M-pCzAnBzt). In particular, 2M-ph-pCzAnBzt produces saturated deep blue emissions in a non-doped electroluminescent device with an exceptionally high EQE of 10.44% and CIEx,y (0.151, 0.057). The unprecedented electroluminescent efficiency is attributed to the combined effects of higher-order reversed intersystem crossing and triplet-triplet up-conversion, which are supported by analysis of theoretical calculation, triplet sensitization experiments, as well as nanosecond transient absorption spectroscopy. This research offers a new approach to resolve the shortage of high efficiency deep blue fluorescent emitters.

15.
Adv Mater ; 33(11): e2006953, 2021 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-33565188

RESUMEN

Aggregation-induced emission (AIE) materials are attractive for achieving highly efficient nondoped organic light-emitting diodes (OLEDs) owing to their strong luminescence in the solid state. However, the electroluminescence efficiency of most AIE-based OLEDs remains low owing to the waste of triplet excitons. Here, using theoretical calculations, photophysical dynamics, and magnetoluminescence measurements, the spin conversion process is demonstrated between the high-lying triplet state (Tn ) and the lowest excited singlet state (S1 ) in AIE materials. Moreover, the relative positions of Tn (n < 4) and S1 are shown to have a significant impact on the spin-conversion efficiency, thus influencing the harvesting of triplet excitons and the device efficiency. Finally, by selecting an upconversion material with an appropriate energy level for further utilizing the triplet excitons, a deep-blue fluorescent OLED with CIE coordinates of (0.15, 0.08), a maximum external quantum efficiency of 10.2%, low efficiency roll-off, and a high brightness of 16817 cd m-2 is developed. This is one of the most efficient deep-blue OLEDs based on AIE materials reported so far. These findings also provide new insights into the design of more efficient AIE molecules and corresponding OLEDs by managing high-lying triplet excitons.

16.
Nat Commun ; 12(1): 5889, 2021 Oct 07.
Artículo en Inglés | MEDLINE | ID: mdl-34620849

RESUMEN

Most organic semiconductors have closed-shell electronic structures, however, studies have revealed open-shell character emanating from design paradigms such as narrowing the bandgap and controlling the quinoidal-aromatic resonance of the π-system. A fundamental challenge is understanding and identifying the molecular and electronic basis for the transition from a closed- to open-shell electronic structure and connecting the physicochemical properties with (opto)electronic functionality. Here, we report donor-acceptor organic semiconductors comprised of diketopyrrolopyrrole and naphthobisthiadiazole acceptors and various electron-rich donors commonly utilized in constructing high-performance organic semiconductors. Nuclear magnetic resonance, electron spin resonance, magnetic susceptibility measurements, single-crystal X-ray studies, and computational investigations connect the bandgap, π-extension, structural, and electronic features with the emergence of various degrees of diradical character. This work systematically demonstrates the widespread diradical character in the classical donor-acceptor organic semiconductors and provides distinctive insights into their ground state structure-property relationship.

17.
Chem Sci ; 12(44): 14808-14814, 2021 Nov 17.
Artículo en Inglés | MEDLINE | ID: mdl-34820096

RESUMEN

Manipulating the molecular orbital properties of excited states and the subsequent relaxation processes can greatly alter the emission behaviors of luminophores. Herein we report a vivid example of this, with luminescence conversion from thermally activated delayed fluorescence (TADF) to ultralong room-temperature phosphorescence (URTP) via a facile substituent effect on a rigid benzothiazino phenothiazine tetraoxide (BTPO) core. Pristine BTPO with multiple heteroatoms shows obvious intramolecular charge transfer (ICT) excited states with small exchange energy, featuring TADF. Via delicately functionalizing the BTPO core with peripheral moieties, the excited states of the BTPO derivatives become a hybridized local and charge transfer (HLCT) state in the S1 state and a local excitation (LE) dominated HLCT state in the T1 state, with enlarged energy bandgaps. Upon dispersion in a polymer matrix, the BTPO derivatives exhibit a persistent bright green afterglow with long lifetimes of up to 822 ms and decent quantum yields of up to 11.6%.

18.
ACS Appl Mater Interfaces ; 11(34): 31078-31086, 2019 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-31381286

RESUMEN

Based on exciplexes as hosts, the monochromatic organic light-emitting diodes (OLEDs) have achieved high power and external quantum efficiencies. However, the high-quality white OLEDs (WOLEDs) with high color rendering index (CRI) have the unsatisfactory efficiencies at high luminance, particularly in terms of power efficiency (PE), resulting in high energy consumption. Here, a new design concept using multiple exciplexes as hosts to match different phosphors has been demonstrated to develop high-performance WOLEDs. It can be seen that the resulting WOLEDs work at a low turn-on voltage of 2.3 V and exhibit the large forward-viewing PE and external quantum efficiency (EQE) of 79 lm W-1 and 22.5%, respectively, without light out-coupling techniques. Significantly, the PE and EQE still remain 48.0 lm W-1 and 21.4% at 1000 cd m-2, showing extremely low efficiency roll-off. The CRI is as high as 81. The keys to success are the selection of the different exciplex hosts matched to different phosphors and the reasonable arrangement of emissive layers, which are beneficial to regulate the exciton distribution and reduce the energy losses.

19.
ACS Appl Mater Interfaces ; 11(34): 31139-31146, 2019 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-31368304

RESUMEN

A novel, efficient, deep-blue fluorescent emitter mPAC, with a meta-connected donor-acceptor structure containing phenanthroimidazole (PPI) as the donor and phenylcarbazole-substituted anthracene (An-CzP) as the acceptor, was designed and synthesized. The meta-linkage provided a highly twisted molecular conformation, which efficiently interrupts the intramolecular π-conjugation, resulting in a deep-blue emission. The optimized nondoped device based on mPAC displayed a deep-blue emission with a narrow full width at half-maximum of 56 nm and Commission Internationale de L'Eclairage coordinates of (0.16, 0.09). The maximum external quantum efficiency (EQEmax) is 6.76%, corresponding to a high exciton utilization efficiency (EUE) of 59.3-88.9%. Experimental results and theoretical analysis indicated that the high EUE is mainly ascribed to the reverse intersystem crossing (RISC) from T2 to S1, a "hot exciton" path in which the large T2-T1 energy gap (1.45 eV) and small T2-S1 energy difference (0.18 eV, T2 > S1) hamper the internal crossing from T2 to T1 and facilitate the RISC process. For the hot exciton path, the T2 state can be feasibly arranged to a high energy level, forming a thermal equilibrium with S1, even slightly higher than the deep-blue S1 to realize an exergonic RISC process, which is usually difficult for the thermally activated delayed fluorescence emitters.

20.
ACS Appl Mater Interfaces ; 11(5): 5232-5239, 2019 Feb 06.
Artículo en Inglés | MEDLINE | ID: mdl-30640426

RESUMEN

Praseodymium-doped indium zinc oxide (PrIZO) has been employed as the channel layer of thin-film transistors (TFTs). The TFTs with Pr doping exhibited a remarkable suppression of the light-induced instability. A negligible photo-response and remarkable enhancement in negative gate bias stress under illumination (NBIS) were achieved in the PrIZO-TFTs. Meanwhile, the PrIZO-TFTs showed reasonable characteristics with a high-field-effect mobility of 26.3 cm2/V s, SS value of 0.28 V/decade, and Ion/ Ioff ratio of 108. X-ray photoelectron spectroscopy, microwave photoconductivity decay, and photoluminescence spectra were employed to analyze the effects of the Pr concentrations on the performance of PrIZO-TFTs. We disclosed that acceptor-like trap states induced by Pr ions might lead to the suppression of photo-induced carrier in conduction band, which is a new strategy for improving illumination stability of amorphous oxide semiconductors. Finally, a prototype of fully transparent AMOLED display was successfully fabricated to demonstrate the potential of Pr-doping TFTs applied in transparent devices.

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