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1.
ACS Appl Mater Interfaces ; 10(21): 18113-18122, 2018 May 30.
Artigo em Inglês | MEDLINE | ID: mdl-29733188

RESUMO

Although organic electroluminescent materials have long promised the prospect of making organic light emitting devices (OLEDs) via low-cost solution-coating techniques, the electroluminescence stability of devices made by such techniques continues to be rather limited making them unsuitable for commercialization. The root causes of the lower stability of OLEDs made by solution-coating versus the more conventional vacuum-deposition remain unknown. In this work, we investigate and compare between solution-coated and vacuum-deposited materials under prolonged excitation, using the archetypical host material 4,4'-bis( N-carbazolyl)-1,1'-biphenyl as a model OLED material. Results show that solution-coated films are more susceptible to degradation by excitons in comparison to their vacuum-deposited counterparts, resulting in a faster decrease in their luminescent quantum yield. The degradation rate also depends on the choice of solvent that was used in the solution-coating process. Results also show that the decrease in quantum yield is caused by exciton-induced chemical decomposition in the material as well as some possible molecular reorganization or aggregation, both of which are induced by excitons and proceed more quickly in case of solution-coated films. The faster degradation in the solution-coated films appears to originate primarily from their different morphological makeup and not due to chemical impurities. The findings uncover what appears to be one of the fundamental root causes of the lower stability of solution-coated OLEDs in general.

2.
Adv Sci (Weinh) ; 5(2): 1700608, 2018 02.
Artigo em Inglês | MEDLINE | ID: mdl-29610726

RESUMO

A new concept of host, electroplex host, is developed for high efficiency and long lifetime phosphorescent organic light-emitting diodes by mixing two host materials generating an electroplex under an electric field. A carbazole-type host and a triazine-type host are selected as the host materials to form the electroplex host. The electroplex host is found to induce light emission through an energy transfer process rather than charge trapping, and universally improves the lifetime of red, yellow, green, and blue phosphorescent organic light-emitting diodes by more than four times. Furthermore, the electroplex host shows much longer lifetime than a common exciplex host. This is the first demonstration of using the electroplex as the host of high efficiency and long lifetime phosphorescent organic light-emitting diodes.

3.
J Am Chem Soc ; 140(20): 6260-6270, 2018 05 23.
Artigo em Inglês | MEDLINE | ID: mdl-29688006

RESUMO

The pyren-1'-yl-functionalized dithiadiazolyl (DTDA) radical, C16H9CNSSN (1), is monomeric in solution and exhibits fluorescence in the deep-blue region of the visible spectrum (440 nm) upon excitation at 241 nm. The salt [1][GaCl4] exhibits similar emission, reflecting the largely spectator nature of the radical in the fluorescence process, although the presence of the radical leads to a modest quenching of emission (ΦF = 98% for 1+ and 50% for 1) through enhancement of non-radiative decay processes. Time-dependent density functional theory studies on 1 coupled with the similar emission profiles of both 1+ and 1 are consistent with the initial excitation being of predominantly pyrene π-π* character. Spectroscopic studies indicate stabilization of the excited state in polar media, with the fluorescence lifetime for 1 (τ = 5 ns) indicative of a short-lived excited state. Comparative studies between the energies of the frontier orbitals of pyren-1'-yl nitronyl nitroxide (2, which is not fluorescent) and 1 reveal that the energy mismatch and poor spatial overlap between the DTDA radical SOMO and the pyrene π manifold in 1 efficiently inhibit the non-radiative electron-electron exchange relaxation pathway previously described for 2. Solid-state films of both 1 and [1][GaCl4] exhibit broad emission bands at 509 and 545 nm, respectively. Incorporation of 1 within a host matrix for OLED fabrication revealed electroluminescence, with CIE coordinates of (0.205, 0.280) corresponding to a sky-blue emission. The brightness of the device reached 1934 cd/m2 at an applied voltage of 16 V. The crystal structure of 1 reveals a distorted π-stacked motif with almost regular distances between the pyrene rings but alternating long-short contacts between DTDA radicals. Solid state measurements on a thin film of 1 reveal emission occurs at shorter wavelengths (375 nm) whereas conductivity measurements on a single crystal of 1 show a photoconducting response at longer wavelength excitation (455 nm).

4.
ACS Appl Mater Interfaces ; 9(46): 40564-40572, 2017 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-29094922

RESUMO

We investigate and compare between organic light-emitting devices (OLEDs) fabricated by solution-coating versus vacuum-deposition. Electroluminescence, photoluminescence, and chromatographic measurements on typical OLED host materials reveal significant electromer formation in layers fabricated by solution-processing, pointing to stronger intermolecular interactions in these systems. Delayed electroluminescence measurements reveal that solution-processed layers also have increased charge traps. The findings provide insights on the morphological differences between solution-processed and vacuum-deposited materials and shed light on the root causes behind the lower electroluminescence stability of solution-processed OLEDs.

5.
ACS Appl Mater Interfaces ; 9(16): 14145-14152, 2017 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-28361540

RESUMO

We investigate the origins of the long-wavelength bands that appear in the emission spectra of carbazole-based host materials and play a role in the electroluminescence (EL) spectral changes of phosphorescent organic light emitting devices (PhOLEDs) with electrical aging. 4,4'-Bis(carbazol-9-yl)biphenyl (CBP) is used as a model carbazole host material and is studied using photoluminescence, EL, and atomic force microscopy measurements under various stress scenarios in both single and bilayer devices and in combination with various electron transport layer (ETL) materials. Results show that exciton-induced morphological aggregation of CBP is behind the appearance of those long-wavelength bands and that complexation between the aggregated CBP molecules and ETL molecules plays a role in this phenomenon. Comparisons between the effects of exciton and thermal stress suggest that exciton-induced aggregation may be limited to short-range molecular ordering or pairing (e.g., dimer or trimer species formation) versus longer-range ordering (crystallization) in the case of thermal stress. The findings provide new insights into exciton-induced degradation in wide band gap host materials and its role in limiting the stability of PhOLEDs.

6.
Angew Chem Int Ed Engl ; 54(17): 5201-4, 2015 Apr 20.
Artigo em Inglês | MEDLINE | ID: mdl-25727757

RESUMO

Dual emitting cores for thermally activated delayed fluorescent (TADF) emitters were developed. Relative to the corresponding TADF emitter with a single emitting core the TADF emitter with a dual emitting core, 3,3',5,5'-tetra(carbazol-9-yl)-[1,1'-biphenyl]-2,2',6,6'-tetracarbonitrile, showed enhanced light absorption accompanied by a high photoluminescence quantum yield. The quantum and power efficiencies of the TADF devices were enhanced by the dual emitting cores.

7.
Sci Rep ; 5: 7859, 2015 Jan 19.
Artigo em Inglês | MEDLINE | ID: mdl-25598436

RESUMO

A hybrid white organic light-emitting diode (WOLED) with an external quantum efficiency above 20% was developed using a new blue thermally activated delayed fluorescent material, 4,6-di(9H-carbazol-9-yl)isophthalonitrile (DCzIPN), both as a blue emitter and a host for a yellow phosphorescent emitter. DCzIPN showed high quantum efficiency of 16.4% as a blue emitter and 24.9% as a host for a yellow phosphorescent emitter. The hybrid WOLEDs with the DCzIPN host based yellow emitting layer sandwiched between DCzIPN emitter based blue emitting layers exhibited high external quantum efficiency of 22.9% with a warm white color coordinate of (0.39, 0.43) and quantum efficiency of 21.0% with a cool white color coordinate of (0.31, 0.33) by managing the thickness of the yellow emitting layer.

8.
Adv Mater ; 26(38): 6642-6, 2014 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-25179914

RESUMO

High quantum efficiency above 18% in a solution-processed thermally activated delayed-fluorescence device is achieved by modifying a common delayed-fluorescence emitter with a tert-butyl substituent.

9.
Adv Mater ; 26(24): 4050-5, 2014 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-24706501

RESUMO

High quantum efficiency close to 25% and long lifetime in green thermally activated delayed fluorescent and phosphorescent organic light emitting diodes are achieved using universal 3',5'-di(carbazol-9-yl)-[1,1'-biphenyl]-3,5-dicarbonitrile host material.

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