RESUMEN
In organic light-emitting diodes, positive and negative charge carriers mostly migrate at different rates. This could result in excitons formed in the EML often migrating to the vicinity of the hole transport layer and the electron transport layer. To address this, it is important to design high-quality multi-resonance hosts that can balance the migration rate of carriers. Here, we report two newly developed multi-resonance hosts, m-ICzPBI and o-ICzPBI. The hosts contain an indolo[3,2,1-jk]carbazole (ICz) motif, which functionalized as either a donor or an acceptor unit. The hosts exhibit extremely high molecular rigidity and thermal stability. Devices A and B were constructed using FIrpic as a phosphorescent emitter with m-ICzPBI or o-ICzPBI as a host. Device A achieved high maximum values of EQE, PE and CE of 13.4%, 24.8 lm W-1 and 31.6 cd A-1, respectively, and low efficiency roll-off at 5000 cd m-2 of 8.6%, 10.6 lm W-1 and 20.3 cd A-1, respectively.
Asunto(s)
Carbazoles , Radiación , Humanos , Transporte de Electrón , Donantes de Tejidos , VibraciónRESUMEN
Two tetradentate Pt(II) complexes with peripheral bulky-group hindrances [Pt(pzpyOczpy-B1) and Pt(pzpyOczpy-B2)] were synthesized and fully investigated for their structural and blue phosphorescent properties. Both X-ray crystallography and computational simulation revealed that bulky substituents incorporated into the C-pyrazolyl and C-pyridinyl positions lie out of the cyclometallated plane, thus alleviating the intramolecular distortions as well as reducing the intermolecular interaction in the solid state. In dichloromethane, their emission peaks at 460 nm with a narrow full width at half-maximum (FWHM) of less than 50 nm, and the photoluminescent quantum yields are over 95% with short decay lifetimes (<5 µs). Solution-processed blue devices are fabricated based on the two complexes. Device A based on Pt(pzpyOczpy-B1) shows excellent electroluminescent performances with the maximum current efficiency, power efficiency, and external quantum efficiency of 47.0 cd/A, 24.6 lm/W, and 22.9%, respectively. The understanding on inert peripheral hindrances provides an effective approach to designing Pt(II) complexes for high-quality blue phosphorescent emitters.
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The secondary kinetic isotope effects (KIEs) of red phosphorescent Ir(III) complexes and the corresponding devices have been investigated. The selective deuterated red emitters show negligible influence on the luminescent spectra, but have positive effects on the quantum efficiencies and stabilities in the devices. As secondary KIEs predicted, the photolysis coinciding with the electrolysis of the deuterated complexes in the devices, measured via decreasing of luminescent intensity, are reduced in rate. An about 33% increase of the device working lifetime could be readily obtained with the strategy of selective deuteration on the emitter complexes. The findings demonstrate the importance of the isotopic effect on the performance improvement of organic light emitting devices and will also trigger the study on organic optoelectronic materials via isotopic tools.
RESUMEN
Described herein is a stable complex, Pt(mpzpyOczpy-mesi), embodying efficient, narrow blue emission. The highly twisted structure of the complex improves the stability and efficiency of photo- and electroluminescence by reducing the intermolecular interactions. The complex in solution shows high photoluminescence efficiency (>95%) and radiative decay rate (Kr = 2.9 × 105 s-1) with a narrow emission spectrum. The bottom-emitting phosphorescent device, BE1, exhibits durable deep blue emission with CIE coordinates of (0.145, 0.166) and 5.2 h of LT50 at an initial luminance of 685 cd/m2. Top-emitting devices, TE1 and TE2, achieve ultrapure blue color with CIEx,y values of (0.141, 0.068) and (0.140, 0.071), respectively. TE4 shows high brightness of 3405 cd m-2 at 50 mA m-2, EQE of 10.2% at 1000 cd/m2, and almost negligible color deviation around (0.135, 0.096) at viewing angles of 0°-60°.
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Poly(3,4ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) has been intensively studied for its thermoelectric applications. Structural modulation to improve crystalline ordering, chain conformation and film morphology is a promising way to decouple the trade-off between conductivity and Seebeck coefficient and thus improve the thermoelectric power factor. Post treatment with ionic liquid ([CoCl2 â 6H2 O]:[ChCl]) bearing cobalt-containing anions resulted in a remarkable enhancement of the power factor to 76.8â µW m-1 K-2 . This IL combines the influence of a high-boiling polar organic solvent and diffusing ions. A high σ mainly resulted from the efficient removal of PSS chains, ordering of the structure and delocalization of bipoloran-dominant transport after conformational change. The increase in S was not due to dedoping of PEDOT chains, but rather the sharp feature of the density of states at the Fermi level induced by ion-exchange with unconventional anions.
RESUMEN
Blue phosphorescent tetradentate pyridyl-carbolinyl Pt(II) complexes, Pt(ppzOclpy-Me), Pt(ppzOclpy-iPr), and Pt(ppzOclpy-mesi), were purposefully synthesized and investigated with their photophysical and luminescent properties. The complexes, incorporating with carbolinyl moieties, have twisted planar structure. X-ray crystallography revealed that the intraligand N···H-C hydrogen bond reversely turned the twisty pyridyl moiety back into the chelating plane. Computational analyses confirmed that the metal-to-ligand charge-transfer transition character appears in the singlet manifolds. However, the ligand-centered transitions rule in their triplet states, which accounts for the phosphorescent emission. The Pt(II) complexes emit blue light with peak wavelengths (λmax) of 461-481 nm and moderate photoluminescent quantum yields (Φ = 34-46% in dichloromethane and Φ = 44-52% in films). The electroluminescent devices were fabricated by solution processes, giving blue emissions peaking at around 470 nm.
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In this report, a solution-processable cohost system incorporating N,N'-di(naphtalene-1-yl)-N,N'-diphenylbenzidine (NPB) and Csp3-annulated phenylquinoline derivatives, including spiro[indeno[1,2-b]quinoline-11,8'-indolo[3,2,1-de]acridine] (IAIQ), 10-phenyl-10H-spiro[acridine-9,11'-indeno[1,2-b]quinoline] (PAIQ) and 3,3'-(11H-indeno[1,2-b]quinoline-11,11-diyl)bis(N-phenyl-N-(m-tolyl)aniline) (m-TPA-DPIQ), is developed for highly efficient saturated red phosphorescent organic light emitting diodes (OLEDs). IAIQ, PAIQ, and m-TPA-DPIQ, designed with the increase of molecular flexibility, are systematically investigated. Solution-processable devices based on the efficient phosphorescent emitter bis[2-(3,5-dimethylphenyl)isoquinolinato](2,8-dimethyl-4,6-nonanedionato)Iridium [Ir(mpiq)2divm] are successfully fabricated, and give electroluminescent peaks at 634-636 nm with Commission Internationale de L'Eclairage coordinates of (0.70, 0.30). Under optimized conditions, the devices incorporating IAIQ, PAIQ, and m-TPA-DPIQ exhibit high external quantum efficiency with the maximum value at 25.1%, 23.4%, and 23.3%, respectively, and all exceeding 18% at the luminance of 1000 cd/m2. In application, the supersaturated red devices with excellent performance could facilitate the development of wet-made displays. The newly developed Csp3-annulated host materials with their excitonic properties also showoff the tactic to construct cohost system for high-quality phosphorescent OLEDs.
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Despite the widespread use of naphthamide atropisomers in biologically active compounds and asymmetric catalysis, few catalytic methods have succeeded in the enantioselective synthesis of these compounds. Herein, a chiral Brønsted acid (CBA) catalysis strategy was developed for readily scalable dynamic kinetic resolution of challenging ortho-formyl naphthamides with pyrrolylanilines. The chiral axis of the atropisomeric amide and a stereogenic center were simultaneously established for a new family of potential biologically active pyrrolopyrazine compounds with high enantio- and diastereoselectivities (up to >20 : 1 d.r. and 98 : 2 e.r.). Epimerization experiments of its derivatives reveal that the N-substitution of the nearby stereogenic center could affect the configurational stability of the axially chiral aromatic amides. These results might be useful for the construction of other kinds of novel axially chiral molecules with a low rotational barrier.
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Three Pt(II) complexes, Pt(czpyOczpy), Pt(czpyOczpy-Me), and Pt(czpyOczpy-OMe), are designed to elucidate the inherent relationship between electronically excited-state and photo- and electroluminescent properties. These complexes showed a blue-shifted phosphorescence with a narrowing spectral profile, which are interrelated with the variation of T1 states from the 3MLCT, hybridized 3(MLCT/LC) to 3LC transition. This change is ascribed to the destabilization of LUMO energy levels on the pyridinyl site, leading to more electron distribution on the carbazolide unit in T1. Moreover, the solution-processed device of Pt(czpyOczpy-OMe), featuring a 3LC transition, shows the best color purity of blue light. Compared to the device of Pt(czpyOczpy) with 3MLCT character, the device of Pt(czpyOczpy-Me) with hybridized 3(MLCT/LC) exhibits improved color purity and external quantum efficiency (10.2%) at a luminance of 1000 cd/m2. Therefore, this work gives a mechanistic interpretation of the phosphorescent properties of tetradentate Pt(II) complexes derived from the manageable lowest triplet excited states.
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Ag2CO3-catalyzed hydrogen isotope exchange of five-membered heteroarenes is disclosed. The reaction can be conducted in the open air, at ambient temperature, and with D2O as deuterium source. Moreover, this protocol showed orthogonal site selectivity to existing technology, thereby greatly expanding the scope of substrates for HIE reaction. The mechanistic study indicated that the carbonate group plays a crucial role to achieve high levels of deuterium incorporation by lowering the activation energy of H/D exchange process.
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A practical and readily scalable reaction sequence was developed for the straightforward synthesis of a new family of larger π-conjugated naphthopyrans by a Brønsted acid-catalyzed aromatic annulation of alkoxyallenes with inert naphthols. The cascade pathway involves allylation/cyclization/debenzyloxylation/isomerization/dehydration. The new class of solid state diphenylmethylene substituted naphthopyrans are fluorescent emissive and proved to have aggregation-induced emission (AIE) behavior.
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Ag-mediated trifluoromethylthiolation of inert Csp3-H bond with CF3SOCl is described. Widely available reagents and operational simplicity make this protocol attractive.
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The structural and photophysical properties of tetradentate Pt(ppzOppz), Pt(ppzOpopy), Pt(ppzOczpy), and Pt(czpyOczpy) have been experimentally and theoretically explored. Single-crystal diffraction measurements provided accurate structural information. Electrochemical and photophysical characterizations revealed internal electronic energy levels in ground and excited states. (Time-dependent) Density functional theory calculation revealed electron distributions in transition processes of S0 â S1 and S1 â T1 â S0. Electronic transition study indicated that Pt(ppzOppz) demonstrated mixed MLCT/LC states and Pt(czpyOczpy) showed MLCT-dominated states in S1 and T1. Both Pt(ppzOpopy) and Pt(ppzOczpy) presented strong delocalized spin transition (DST) during intersystem crossing. Upon frame modification of Pt(ppzOczpy), we found that their S1 and T1 can be independently manipulated. These blue emitters showed a tunable and narrow emission band (the narrowest fwhm was 19 nm) with luminescence efficiency as high as 86%. The findings of the DST transition mode in the neutral Pt(II) complexes provide guidance for rational design of novel phosphorescent materials.
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The distal and proximal bond of difluoro(methylene)cyclopropanes (F2MCPs) could be cleaved, respectively, under different conditions to give the corresponding ring-opening products. The reaction mechanisms are discussed.