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1.
Chemistry ; 28(2): e202103543, 2022 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-34730859

RESUMO

A series of [-2, -1, 0] charged-ligand based iridium(III) complexes of [Ir(bph)(bpy)(acac)] (1), [Ir(bph)(2MeO-bpy)(acac)] (2), [Ir(bph)(2CF3 -bpy)(acac)] (3), [Ir(bph)(bpy)(2t Bu-acac)] (4) and [Ir(bph)(bpy)(CF3 -acac)] (5), which using biphenyl as dianionic ligand [-2], acetylacetone (or its derivatives) as monoanionic ligand [-1], and 2,2'-bipyridine (or its derivatives) as neutral ligand [0] were designed and synthesized. The chemical structures were well characterized. All of the ligands have simple chemical structures, thus further making the complexes have excellent thermal stability and are easy to sublimate and purify. Phosphorescent characteristics with short emission lifetime were demonstrated for these emitters. Notably, all of the complexes exhibit remarkable deep red/near infrared emission, which is quite different from the reported [-1, -1, -1] charged-ligand based iridium(III) complexes. The photophysical properties of these complexes are regularly improved by introducing electron-donating or -withdrawing groups into [-1] or [0] charged-ligand. The related organic light-emitting diodes exhibited deep red/near infrared emission with acceptable external quantum efficiency and low turn-on voltage (<2.6 V). This work provides a new idea for the construction of new type phosphorescent iridium(III) emitters with different valence states of [-2, -1, 0] charged ligands, thus offering new opportunities and challenges for their optoelectronic applications.

2.
Mater Horiz ; 9(2): 772-779, 2022 02 07.
Artigo em Inglês | MEDLINE | ID: mdl-34897349

RESUMO

Near-infrared thermally activated delayed fluorescence (NIR-TADF) materials with emission over 700 nm have been insufficiently investigated mainly due to the limited choice of strong donor/acceptor units for molecular construction and the limited electronic coupling between the donors and acceptors. Herein, a novel D-A1-A2-A3 configuration was developed for the design of a NIR-TADF material (TPA-CN-N4-2PY), in which three types of sub-acceptor units (CN: cyano; N4: dipyrido[3,2-a:2',3'-c]phenazine; PY: pyridine) were incorporated into a molecular skeleton to reinforce the electron-accepting strength. The attachment of two pyridine units on TPA-CN-N4 produced TPA-CN-N4-2PY with an extended π-backbone, which shifted the electroluminescence (EL) emission into the NIR region and enhanced the horizontal ratio of emitting dipole orientation (Θ//) simultaneously. TPA-CN-N4-2PY-based OLEDs demonstrated a record-high external quantum efficiency (EQE) of 21.9% with an emission peak at 712 nm and Θ// = 85% at the doping ratio of 9.0 wt%. On the contrary, the parent compound TPA-CN-N4-based OLEDs at the same doping ratio achieved an EQE of 23.4% at 678 nm with Θ// = 75%. This multiple sub-acceptors approach could enrich the design strategy of the NIR-TADF materials, and the large conjugated system could improve the Θ// for achieving efficient emitters.


Assuntos
Eletrônica , Fluorescência
3.
Mater Horiz ; 8(2): 547-555, 2021 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-34821270

RESUMO

By integrating high molecular rigidity and stable chirality, two pairs of D*-A type circularly polarized thermally activated delayed fluorescence (CP-TADF) emitters with an almost absolute quasi-equatorial conformer geometry and excellent photoluminescence quantum efficiencies (PLQYs) are developed, achieving state-of-the-art electroluminescence performance among blue and orange circularly polarized organic light-emitting diodes (CP-OLEDs).

4.
Mater Horiz ; 8(4): 1297-1303, 2021 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-34821922

RESUMO

Rigid electron donors (D) and acceptors (A) have been widely used in recent years for the construction of D-A type thermally activated delayed fluorescence (TADF) materials. However, the chromophore robustness does not always make a positive contribution to the high efficiency of TADF materials. Here, the comparison study of two D-A type red TADF compounds (PT-TPA and PT-Az) demonstrated, for the first time, the positive impact of chromophore flexibility on the efficiency of TADF materials. In PT-Az, the rotation of terminal phenyl groups is restrained by an ethylene linker, leading to its inferior photoluminescence quantum yield (PLQY). In contrast, PT-TPA with free rotation of the phenyl groups showed a low reorganization energy and a large transition dipole moment for the S1→ S0 transition, which resulted in a high fluorescence radiative decay rate. As a result, the optimized devices based on PT-TPA gave a maximum external quantum efficiency (EQE) of 29.7% (632 nm) when doped in a single host and an EQE of 28.8% (648 nm) in an exciplex host. This study provided an insight into the impact of chromophore flexibility on the photophysical properties and device efficiency of TADF materials, and these results may provide valuable guidance for the molecular design of efficient emitters.

5.
Mater Horiz ; 8(8): 2286-2292, 2021 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-34846432

RESUMO

The thermally activated delayed fluorescence (TADF) emitters based on donor-acceptor (D-A) configuration were continuously developed in the past few years, whereas an unsymmetrical TADF emitter with A-D-A' configuration has never been reported. Herein, an A-D-A' type TADF emitter of TRZ-SBA-NAI was firstly developed by simultaneously integrating 2-phenyl-1H-benzo[de]isoquinoline-1,3(2H)-dione and 2,4,6-triphenyl-1,3,5-triazine acceptors into a spirobiacridine donor core. Due to the coexistence of double charge-transfer excited states, TRZ-SBA-NAI displayed dual emission containing a dominant orange-red emission and an anti-Kasha's rule sky-blue emission shoulder in solution. As doped into the host matrix, TRZ-SBA-NAI only exhibited an orange-red emission, together with a high photoluminescence quantum yield of 87%. The linear molecular shape imparted TRZ-SBA-NAI with a high horizontal dipole ratio of 88%. As a result, the TRZ-SBA-NAI based devices achieved a record-high external quantum efficiency of 31.7% with an electroluminescence peak at 593 nm. This finding not only enriches the diversity in TADF molecular design, but also unlocks the huge potential of A-D-A' type TADF emitters for excellent device performance.

6.
Opt Express ; 29(5): 7654-7665, 2021 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-33726262

RESUMO

Sunlight/UV (ultraviolet)-induced degradation is still a critical issue for outdoor applications of organic light-emitting diode (OLED) displays. Therefore, effective UV-blocking structures that can prevent OLED displays from sunlight/UV degradation and still keep the OLED panels' display performance is necessary. In this report, modified distributed Bragg reflector (DBR) structures having UV-absorbing dielectric materials and adjusted layer/pair thicknesses were developed to realize effective UV blocking properties (nearly 0% transmittance below 400 nm), constantly high transmittance like glass in the visible range (∼92%) required for display applications, and sharp transition in transmission between the UV and the visible ranges. Furthermore, under the rigorous IEC 60068-2-5 solar test condition, it was verified that the developed modified, UV-blocking DBR can effectively enhance the OLED panel's resistance against UV/solar-induced degradation, effectively reducing voltage shifts of OLED devices after repeated solar test cycles.

7.
ACS Appl Mater Interfaces ; 13(11): 13478-13486, 2021 Mar 24.
Artigo em Inglês | MEDLINE | ID: mdl-33689279

RESUMO

How to develop efficient red-emitting organometallics of earth-abundant copper(I) is a formidable challenge in the field of organic light-emitting diodes (OLEDs) because Cu(I) complexes have weak spin-orbit coupling and a serious excited-state reorganization effect. Here, a red Cu(I) complex, MAC*-Cu-DPAC, was developed using a rigid 9,9-diphenyl-9,10-dihydroacridine donor ligand in a carbene-metal-amide motif. The Cu(I) complex achieved satisfactory red emission, a high photoluminescence quantum yield of up to 70%, and a sub-microsecond lifetime. Thanks to a linear geometry and the acceptor and donor ligands in a coplanar conformation, the complex exhibited a high horizontal dipole ratio of 77% in the host matrix, first demonstrated for coinage metal(I) complexes. The resulting OLEDs delivered high external quantum efficiencies of 21.1% at a maximum and 20.1% at 1000 nits, together with a red emission peak at ∼630 nm. These values represent the state-of-the-art performance for red-emitting OLEDs based on coinage metal complexes.

8.
Chemistry ; 27(9): 3151-3158, 2021 Feb 10.
Artigo em Inglês | MEDLINE | ID: mdl-33241622

RESUMO

The development of thermally activated delayed fluorescence (TADF) emitters with orange-red emission still lags behind that of their blue, green, and yellow counterparts. Recent research to address this problem mainly focused on developing new acceptor units. There were few donor units designed especially for orange-red emitters. Herein, with benzothiophene fused to a diphenylacridine donor unit, a new donor moiety, namely, 5,5-diphenyl-5,13-dihydrobenzo[4,5]thieno[3,2-c]acridine (BTDPAc), was designed and synthesized. Benefiting from the strong electron-donating ability of the new donor moiety, a new TADF emitter, 2-[4'-(tert-butyl)(1,1'-biphenyl)-4-yl]-6-[5,5-diphenylbenzo[4,5]thieno[3,2-c]acridin-13(5H)-yl]-1H-benzo[de]isoquinoline-1,3(2H)-dione (BTDPAc-PhNAI), shows an orange-red emission with a maximum at 610 nm in dilute toluene solution. Also, with the help of the diphenyl rings of the donor unit, high photoluminescence quantum yields were achieved for BTDPAc-PhNAI over a wide concentration range. Consequently, an orange-red organic light-emitting diode based on BTDPAc-PhNAI achieved a high external quantum efficiency of nearly 20 %, which was comparable to state-of-the-art device performances with similar emission spectra.

9.
Sci Adv ; 6(41)2020 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-33036963

RESUMO

Manipulating orientation of organic emitters remains a formidable challenge in organic light-emitting diodes (OLEDs). Here, expansion of the acceptor plane of thermally activated delayed fluorescence (TADF) emitters was demonstrated to selectively modulate emitting dipole orientation. Two proof-of-the-concept molecules, PXZPyPM and PXZTAZPM, were prepared by introducing a planar 2-phenylpyridine or 2,4,6-triphenyl-1,3,5-triazine substituent into a prototypical molecule (PXZPM) bearing a pyrimidine core and two phenoxazine donors. This design approach suppressed the influence of substituents on electronic structures and associated optoelectronic properties. Accordingly, PXZPyPM and PXZTAZPM preserved almost the same excited states and similar emission characteristics as PXZPM. The expanded acceptor plane of PXZPyPM and PXZTAZPM resulted in a 15 to 18% increase in horizontal ratios of emitting dipole orientation. PXZPyPM supported its green device exhibiting an external quantum efficiency of 33.9% and a power efficiency of 118.9 lumen per watt, competitive with the most efficient green TADF OLEDs reported so far.

10.
J Phys Chem C Nanomater Interfaces ; 123(19): 12400-12410, 2019 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-32952765

RESUMO

Understanding the excited-state dynamics and conformational relaxation in thermally activated delayed fluorescence (TADF) molecules, including conformations that potentially support intramolecular through-space charge transfer, can open new avenues for TADF molecular design as well as elucidate complex photophysical pathways in structurally complex molecules. Emissive molecules comprising a donor (triphenylamine, TPA) and an acceptor (triphenyltriazine, TRZ) bridged by a second donor (9,9-dimethyl-9-10-dihydroacridin, DMAC, or phenoxazine, PXZ) are synthesized and characterized. In solution, the flexibility of the sp3-hybridized carbon atom in DMAC of DMAC-TPA-TRZ, compared to the rigid PXZ, allows significant conformational reorganization, giving rise to multiple charge-transfer excited states. As a result of such a reorganization, the TRZ and TPA moieties become cofacially aligned, driven by a strong dipole-dipole attraction between the TPA and TRZ units, forming a weakly charge-transfer dimer state, in stark contrast to the case of PXZ-TPA-TRZ where the rigid PXZ bridge only supports a single PXZ-TRZ charge transfer (CT) state. The low-energy TPA-TRZ dimer is found to have a high-energy dimer local triplet state, which quenches delayed emission because the resultant singlet CT local triplet energy gap is too large to mediate efficient reverse intersystem crossing. However, organic light-emitting diodes using PXZ-TPA-TRZ as an emitting dopant resulted in external quantum efficiency as high as 22%, more than two times higher than that of DMAC-TPA-TRZ-based device, showing the impact that such intramolecular reorganization and donor-acceptor dimerization have on TADF performance.

11.
Adv Sci (Weinh) ; 5(10): 1800467, 2018 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-30356985

RESUMO

Despite stringent power consumption requirements in many applications, over years organic light-emitting diode (OLED) displays still suffer unsatisfactory energy efficiency due to poor light extraction. Approaches have been reported for OLED light out-coupling, but they in general are not applicable for OLED displays due to difficulties in display image quality and fabrication complexity and compatibility. Thus to date, an effective and feasible light extraction technique that can boost efficiencies and yet keep image quality is still lacking and remains a great challenge. Here, a highly effective and scalable extraction-enhancing OLED display pixel structure is proposed based on embedding the OLED inside a three-dimensional reflective concave structure covered with a patterned high-index filler. It can couple as much internal emission as possible into the filler region and then redirect otherwise confined light for out-coupling. Comprehensive multi-scale optical simulation validates that ultimately high light extraction efficiency approaching ≈80% and excellent viewing characteristics are simultaneously achievable with optimized structures using highly transparent top electrodes. This scheme is scalable and wavelength insensitive, and generally applicable to all red, green, and blue pixels in high-resolution full-color displays. Results of this work are believed to shed light on the development of future generations of advanced OLED displays.

12.
J Biomed Opt ; 23(8): 1-9, 2018 08.
Artigo em Inglês | MEDLINE | ID: mdl-30156065

RESUMO

In optical coherence tomography (OCT) systems, to precisely obtain the scattering properties of samples is an essential issue in diagnostic applications. Especially with a higher density turbid medium, the light interferes among the adjacent scatters. Combining an OCT experiment with the finite-difference time-domain simulation method, the multiple scattering effect is shown to affect the scattering properties of medium depending on the interparticle spacing. The far-field scattering phase function of scatters with various diameters was simulated to further analyze the corresponding anisotropy factors, which can be introduced into the extended Huygens-Fresnel theory to find the scattering coefficient of measured samples.


Assuntos
Simulação por Computador , Espalhamento de Radiação , Tomografia de Coerência Óptica/métodos , Algoritmos , Nanopartículas Metálicas/química , Modelos Químicos , Tamanho da Partícula , Titânio/química
13.
Adv Mater ; 30(5)2018 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-29218854

RESUMO

The combination of rigid acridine donor and 1,8-naphthalimide acceptor has afforded two orange-red emitters of NAI-DMAC and NAI-DPAC with high rigidity in molecular structure and strongly pretwisted charge transfer state. Endowed with high photoluminescence quantum yields (ΦPL ), distinct thermally activated delayed fluorescence (TADF) characteristics, and preferentially horizontal emitting dipole orientations, these emitters afford record-high orange-red TADF organic light-emitting diodes (OLEDs) with external quantum efficiencies of up to 21-29.2%, significantly surpassing all previously reported orange-to-red TADF OLEDs. Notably, the influence of microcavity effect is verified to support the record-high efficiency. This finding relaxes the usually stringent material requirements for effective TADF emitters by comprising smaller radiative transition rates and less than ideal ΦPL s.

14.
Adv Mater ; 29(33)2017 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-28635052

RESUMO

Emissive Ir(III) metal complexes possessing two tridentate chelates (bis-tridentate) are known to be more robust compared to those with three bidentate chelates (tris-bidentate). Here, the deep-blue-emitting, bis-tridentate Ir(III) metal phosphors bearing both the dicarbene pincer ancillary such as 2,6-diimidazolylidene benzene and the 6-pyrazolyl-2-phenoxylpyridine chromophoric chelate are synthesized. A deep-blue organic light-emitting diode from one phosphor exhibits Commission Internationale de l'Eclairage (CIE(x,y) ) coordinates of (0.15, 0.17) with maximum external quantum efficiency (max. EQE) of 20.7% and EQE = 14.6% at the practical brightness of 100 cd m-2 .

15.
ACS Appl Mater Interfaces ; 8(49): 33888-33898, 2016 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-27960361

RESUMO

We report the utilization of both pyrid-2-yl-imidazolylidene and dianionic bipz chelates as constituents in syntheses of a new series of charge-neutral Pt(II) complexes 1-4, among which complex 4 revealed remarkable triboluminescence, i.e., generation of photoemission upon grinding or cracking of the solid sample. The triboluminescence is found to be sensitive to the subtle changes of the associated substituents of pyrid-2-yl-imidazolylidene chelate, as verified by the disappearance of the triboluminescence for complexes 1-3. Alternatively, the well-ordered solid packing of 3, as indicated by the grazing incidence X-ray scattering experiment, serves as an ideal emitter for the fabrication of highly efficient OLEDs, rendering high external quantum efficienciy (25.9%) and luminesce efficiency (90 cd A-1) at the practical brightness of 100 cd m-2. The rather low roll-off in efficiency (24.4%, 85 cd A-1 at high brightness of 1000 cd m-2) is attributed to the short excited-state lifetime of 3 (∼800 ns) in the solid state, which in turn is associated with the MMLCT transition character.

16.
Opt Express ; 24(10): A810-22, 2016 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-27409954

RESUMO

UNLABELLED: We report the characterization and analyses of organic light-emitting devices (OLEDs) using microstructured composite transparent electrodes consisting of the high-index ITO (indium tin oxide) micromesh and the low-index conducting polymer PEDOT: PSS [poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)], that are fabricated by the facile and convenient microsphere lithography and are useful for enhancing light extraction. The rigorous electromagnetic simulation based on the three-dimensional finite-difference time-domain (FDTD) method was conducted to study optical properties and mechanisms in such devices. It provides a different but consistent viewpoint/insight of how this microstructured electrode enhances optical out-coupling of OLEDs, compared to that provided by ray optics simulation in previous works. Both experimental and simulation studies indicate such a microstructured electrode effectively enhances coupling of internal radiation into the substrate, compared to devices with the typical planar ITO electrode. By combining this internal extraction structure and the external extraction scheme (e.g. by attaching extraction lens) to further extract radiation into the substrate, a rather high external quantum efficiency of 46.8% was achieved with green phosphorescent OLEDs, clearly manifesting its high potential.

17.
Adv Mater ; 28(32): 6976-83, 2016 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-27271917

RESUMO

Extremely efficient sky-blue organic electroluminescence with external quantum efficiency of ≈37% is achieved in a conventional planar device structure, using a highly efficient thermally activated delayed fluorescence emitter based on the spiroacridine-triazine hybrid and simultaneously possessing nearly unitary (100%) photoluminescence quantum yield, excellent thermal stability, and strongly horizontally oriented emitting dipoles (with a horizontal dipole ratio of 83%).

18.
Adv Mater ; 28(14): 2795-800, 2016 Apr 13.
Artigo em Inglês | MEDLINE | ID: mdl-26894982

RESUMO

A new class of neutral bis-tridentate Ir(III) metal complexes that show nearly unitary red, green, and blue emissions in solution is prepared and employed for the fabrication of both monochrome and white-emitting organic light-emitting diodes, among which a green device gives external quantum efficiency exceeding 31%.

19.
ACS Nano ; 10(1): 998-1006, 2016 Jan 26.
Artigo em Inglês | MEDLINE | ID: mdl-26730851

RESUMO

Self-assembled aggregates offer great potential for tuning the morphology of organic semiconductors, thereby controlling their size and shape. This is particularly interesting for applications in electroluminescent (EL) devices, but there has been, to date, no reports of a functional EL device in which the size and color of the emissive domains could be controlled using self-assembly. We now report a series of molecules that spontaneously self-organize into small EL domains of sub-micrometer dimensions. By tailoring the emissive chromophores in solution, spherical aggregates that have an average size of 300 nm in diameter and emit any one color, including CIE D65 white, are spontaneously formed in solution. We show that the individual aggregates can be used in EL devices built either using small patterned electrodes or using a sandwich architecture to produce devices emitting in the blue, green, red, and white. Furthermore, sequential deposition of the three primary colors yields an RGB device in which single aggregates of each color are present in close proximity.

20.
Angew Chem Int Ed Engl ; 55(9): 3017-21, 2016 Feb 24.
Artigo em Inglês | MEDLINE | ID: mdl-26822378

RESUMO

The electron positive boron atom usually does not contribute to the frontier orbitals for several lower-lying electronic transitions, and thus is ideal to serve as a hub for the spiro linker of light-emitting molecules, such that the electron donor (HOMO) and acceptor (LUMO) moieties can be spatially separated with orthogonal orientation. On this basis, we prepared a series of novel boron complexes bearing electron deficient pyridyl pyrrolide and electron donating phenylcarbazolyl fragments or triphenylamine. The new boron complexes show strong solvent-polarity dependent charge-transfer emission accompanied by a small, non-negligible normal emission. The slim orbital overlap between HOMO and LUMO and hence the lack of electron correlation lead to a significant reduction of the energy gap between the lowest lying singlet and triplet excited states (ΔET-S ) and thereby the generation of thermally activated delay fluorescence (TADF).

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