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1.
Chem Sci ; 15(24): 9112-9119, 2024 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-38903225

RESUMO

The weak spin-orbit coupling (SOC) in metal-free organic molecules poses a challenge in achieving phosphorescence emission. To attain pure phosphorescence in RTP organic emitters, a promising molecular design concept has been proposed. This involves incorporating n → π* transitions and leveraging the heavy atomic effect within the spin-orbit charge transfer-induced intersystem crossing (SOCT-ISC) mechanism of bipolar molecules. Following this design concept, two bipolar metal-free organic molecules (PhSeB and PhSeDB) with donor-acceptor (D-A) and acceptor-donor-acceptor (A-D-A) configurations have been synthesized. When the molecular configuration changes from D-A to A-D-A, PhSeDB exhibits stronger electron coupling and n → π* transitions, which can further enhance the spin-orbit coupling (SOC) together with the heave atom effect from the selenium atom. By the advanced synergism among enhanced n → π* transitions, heavy atom effect and magnified electron coupling to efficiently promote phosphorescence emission, PhSeDB can achieve pure RTP emission in both the solution and doped solid film. Thanks to the higher spin-orbit coupling matrix elements (SOCMEs) for T1 ↔ S0, PhSeDB attains the highest phosphorescence quantum yield (ca. 0.78) among all the RTP organic emitters reported. Consequently, the purely organic phosphorescent light-emitting diodes (POPLEDs) based on PhSeDB achieve the highest external quantum efficiencies of 18.2% and luminance of 3000 cd m-2. These encouraging results underscore the significant potential of this innovative molecular design concept for highly efficient POPLEDs.

2.
Chem Sci ; 15(22): 8506-8513, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38846396

RESUMO

The modulation of emission color is one of the most critical topics in the research field of organic light-emitting diodes (OLEDs). Currently, only two ways are commonly used to tune the emission colors of OLEDs: one is to painstakingly synthesize different emitters with diverse molecular structures, the other is to precisely control the degree of aggregation or doping concentration of one emitter. To develop a simpler and less costly method, herein we demonstrate a new strategy in which the emission colors of OLEDs can be continuously changed with UV light during the device fabrication process. The proof of concept is established by a chromene-based Ir(iii) complex, which shows bright green emission and yellow emission before and after UV irradiation, respectively. Consequently, under different durations of UV irradiation, the resulting Ir(iii) complex is successfully used as the emitter to gradually tune the emission colors of related solution-processed OLEDs from green to yellow. Furthermore, the electroluminescent efficiencies of these devices are unaffected or even increased during this process. Therefore, this work demonstrates a distinctive point of view and approach for modulating the emission colors of OLEDs, which may prove great inspiration for the fabrication of multi-colored OLEDs with only one emitter.

3.
J Am Chem Soc ; 146(1): 39-44, 2024 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-38117532

RESUMO

Herein, we reported the isolation of 2π-aromatic disiladiboretenes (L2Si2B2Ph2) [L = ArC(NtBu)2, Ar = Ph (1), Mes (2)], which have been synthesized from the straightforward reduction of silylene-borane adducts (LSiX → BX2Ph) [X = Cl, Br] with potassium graphite (KC8). X-ray diffraction analysis of 1 and 2 revealed that the Si2B2 units are completely planar, and DFT calculations suggested delocalization of 2π-electrons over the Si2B2 rings. Moreover, their photophysical properties and reactivity toward sulfur were also investigated in detail.

4.
Phys Chem Chem Phys ; 25(37): 25838-25849, 2023 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-37724577

RESUMO

Novel amorphous compounds which could simultaneously use 25% singlet excitons and 75% triplet excitons as the energy source for light amplification enable the reduction of the threshold current density for electrically pumped organic semiconductor laser diodes (OSLDs); however, there is always a trade-off between the high radiative decay rate of the local excited (LE) state that is required for amplified spontaneous emission (ASE) and high exciton utilization benefiting from the charge-transfer (CT) state during electroluminescence (EL). Herein, we have explored a delicate balance to achieve both low ASE threshold and high EL exciton utilization by adopting a carefully tailored hybridized local and charge-transfer (HLCT) molecular design. A series of donor-π-acceptor (D-π-A) molecules (SBz-1, SBz-2 and SBz-3) are synthesized, and the structural change mainly refers to the spatial distance between D and A which could regulate the excited-state character via adjusting the CT length. Notably, the ASE phenomenon with a low threshold (2.97 µJ cm-2) and a high exciton utilization of 57.6% are achieved at the same time for SBz-2 with an appropriate CT length. The results provide guidance for molecular design toward harvesting triplet excitons in organic laser materials.

5.
Angew Chem Int Ed Engl ; 62(41): e202309739, 2023 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-37626014

RESUMO

Highly efficient near-infrared (NIR) emitters have significant applications in medical and optoelectronic fields, but the development stays a great challenge due to the energy gap law. Here, we report two NIR phosphorescent Ir(III) complexes which display emission peaks around 730 nm with a narrow full width at half maximum of only 43 nm. Therefore, pure NIR luminescence can be obtained without having a very long emission wavelength, thus alleviating the restriction of the energy gap law, and obtaining impressively high photoluminescence quantum yield up to 0.70. More importantly, the pure NIR organic light-emitting diode (OLED) fabricated by the solution-processed mothed shows outstanding device performance with the highest external quantum efficiency of 16.43 %, which sets a new record for solution-processed NIR-OLEDs based on different emitters. This work sheds light on the development of Ir(III) complexes with narrowband emissions as highly efficient pure NIR-emitters.

6.
Dalton Trans ; 52(26): 8927-8942, 2023 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-37337994

RESUMO

A series of four-coordinated PtII(C^N)(N-donor ligand)Cl-type complexes have been synthesized through a combination of long-size C^N-type and N-donor ligands. In addition, by varying the coordinating site in the N-donor ligand, a distorted molecular configuration has been constructed in these complexes. Their photophysical features, aggregation-induced phosphorescence emission (AIPE) behaviors, electrochemical properties and electroluminescence (EL) performance have been investigated in detail. It has been found that their AIE behaviors can be enhanced by both employing long-size ligands, especially the N-donor ligand, and adopting a distorted molecular configuration, furnishing a high AIE factor (αAIE) of ca. 13.8. Critically, benefitting from their long-size C^N-type and N-donor ligands, these PtII(C^N)(N-donor ligand)Cl-type complexes can exhibit very sensitive AIE behaviors in a mixture of THF-H2O, indicated by their noticeable emission increase with a low H2O volumetric fraction (fw) of ca. 0.1 in their THF solution. In solution-processed organic light-emitting diodes (OLEDs), they can achieve a luminance of 6743 cd m-2 at 13.5 V, a maximum external quantum efficiency (ηext) of 13.8%, a maximum current efficiency (ηL) of 42.4 cd A-1 and a maximum power efficiency (ηP) of 34.4 lm W-1, respectively. Hence, this research can provide key information for developing phosphorescent complexes with a highly sensitive AIE response and impressive EL ability.

7.
Adv Mater ; 33(44): e2104187, 2021 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-34510560

RESUMO

A fatal weakness in flexible electronics is the mechanical fracture that occurs during repetitive fatigue deformation; thus, controlling the crack development of the conductive layer is of prime importance and has remained a great challenge until now. Herein, this issue is tackled by utilizing an amyloid/polysaccharide molecular composite as an interfacial binder. Sodium alginate (SA) can take part in amyloid-like aggregation of the lysozyme, leading to the facile synthesis of a 2D protein/saccharide hybrid nanofilm over an ultralarge area (e.g., >400 cm2 ). The introduction of SA into amyloid-like aggregates significantly enhances the mechanical strength of the hybrid nanofilm, which, with the help of amyloid-mediated interfacial adhesion, effectively diminishes the microcracks in the hybrid nanofilm coating after repetitive bending or stretching. The microcrack-free hybrid nanofilm then shows high interfacial activity to induce electroless deposition of metal in a Kelvin model on a substrate, which noticeably suppresses the formation of microcracks and consequent conductivity loss during the bending and stretching of the metal-coated flexible substrates. This work underlines the significance of amyloid/polysaccharide nanocomposites in the design of interfacial binders for reliable flexible electronic devices and represents an important contribution to mimicking amyloid and polysaccharide-based adhesive cements created by organisms.


Assuntos
Agregados Proteicos
8.
ACS Appl Mater Interfaces ; 13(30): 36020-36032, 2021 Aug 04.
Artigo em Inglês | MEDLINE | ID: mdl-34283914

RESUMO

The various applications of dinuclear complexes have attracted increasing attention. However, the electroluminescence efficiencies of dinuclear Pt(II) complexes are far from satisfactory. Herein, based on the triphenylamine core, we develop four dinuclear Pt(II) complexes that cover the emission colors from yellow to red with high photoluminescence quantum efficiencies of up to 0.79 in doped films. The solid-state structure of PyDPt is revealed by the single-crystal X-ray diffraction investigation. Besides, solution-processed OLEDs have been fabricated with different electron transport materials. With higher electron mobility and excellent hole-blocking ability, 1,3,5-tri(m-pyridin-3-ylphenyl)benzene (TmPyPB) can help to realize good charge balance in related OLEDs. In addition, angle-dependent PL spectra reveal the preferentially horizontal orientation of these dinuclear Pt(II) complexes in doped CBP films, which benefits the outcoupling efficiencies. Therefore, the yellow OLED based on PyDPt shows unexpected high performance with a peak current efficiency of up to 78.7 cd/A and an external quantum efficiency of up to 22.4%, which is the highest EQE reported for OLEDs based on dinuclear Pt(II) complexes so far. This study demonstrates the great potential of developing dinuclear Pt(II) complexes for achieving excellent electroluminescence efficiencies.

9.
Dalton Trans ; 49(44): 15633-15645, 2020 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-33057516

RESUMO

A series of (C^N)Pt(acac)-type complexes has been successfully synthesized with a benzo[b]furan, benzo[b]thiophene, benzo[b]selenophene, or benzo[b]tellurophene group in the benzoaryl-pyridine ligand. Using X-ray crystallography, the chemical structures of the complexes with benzo[b]selenophene and benzo[b]tellurophene groups have been clearly revealed. The photophysical, electrochemical, and electroluminescent (EL) behaviors of these (C^N)Pt(acac)-type complexes have been fully characterized. Furthermore, both time-dependent functional theory (TD-DFT) and natural transition orbital (NTO) theoretical results have been obtained to gain insight into the absorption and emission features. It has been shown that both the absorption bands with the lowest energy and the phosphorescence emission behaviors are dominated by the benzoaryl-pyridine cyclometalating ligand. Importantly, the effects of the group VIA atoms on the properties of these (C^N)Pt(acac)-type complexes have been revealed. Owing to the rareness of (C^N)Pt(acac)-type complexes with benzo[b]selenophene and benzo[b]tellurophene groups, their EL abilities have been characterized using solution-processed organic light-emitting diodes (OLEDs). The optimized red OLEDs with the complex bearing a benzo[b]selenophene unit show a maximum external quantum efficiency (ηext) of 6.3%, current efficiency (ηL) of 10.5 cd A-1, and power efficiency (ηP) of 9.1 lm W-1, while the EL device with the complex bearing a benzo[b]tellurophene unit can give deep-red emission at ca. 636 nm with ηext of 6.3%, ηL of 6.5 cd A-1, and ηP of 5.8 lm W-1. This research not only provides novel (C^N)Pt(acac)-type complexes, but also furnishes critical information regarding the photophysical and EL behavior of these new complexes.

10.
Inorg Chem ; 59(17): 12362-12374, 2020 Sep 08.
Artigo em Inglês | MEDLINE | ID: mdl-32799532

RESUMO

2-Phenylquinoline (PQ) and four coumarin-based ligand isomers with ease of synthesis have been selected to construct the unsymmetric heteroleptic [Ir(C1∧N)(C2∧N)(acac)]-type complex phosphors for organic light-emitting diodes (OLEDs). Six unsymmetric heteroleptic Ir(III) complexes have been obtained by employing four coumarin-based ligand isomers (L-C5/L-C6/L-C7/L-C8) in the [Ir(PQ)(C∧N)(acac)] structure due to two different coordinating carbon atoms in ligands L-C6 and L-C7 to form C-Ir bond. Through adopting unsymmetric heteroleptic [Ir(C1∧N)(C2∧N)(acac)] structure, these Ir(III) complexes can not only achieve impressive absolute quantum yield Φp (ca. 0.5-1.0), higher than that of complex [Ir(PQ)2(acac)] (ca. 0.4), but also realize a dual modulation of both emission color from orange (AIrC6out, λ = 578 nm) to red (AIrC5, λ = 622 nm) and the character of the lowest triplet excited states (T1), showing both 3MLCT character and 3ILCT (intraligand charge transfer) character in their T1 states. AIrC5, AIrC7out, and AIrC7in show MLCT character from Ir(III) center to ligand L-C5 or L-C7 and ILCT character in ligand L-C5 or L-C7 in their T1 states, while AIrC6out, AIrC6in, and AIrC8 show MLCT character from Ir(III) center to ligand PQ and ILCT character in ligand PQ in their T1 states. Moreover, the color-tuning mechanism and the lowest triplet state characters are investigated in detail. AIrC6in and AIrC8 were selected as emitters to evaluate the electroluminescent (EL) performance due to their high ΦP of nearly up to unity. Optimal orange-emitting device B2 based on AIrC8 can give a maximum external quantum efficiency (ηext) of 23.9%, a maximum current efficiency (ηL) of 70.9 cd A-1, and a maximum power efficiency (ηP) of 60.7 lm W-1. All these impressive results can definitely demonstrate the effectiveness of our simple approach for tuning character of the triplet excited states and achieving high-performance Ir-based phosphors in OLEDs.

11.
Dalton Trans ; 49(15): 4967-4976, 2020 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-32236211

RESUMO

A new 2-phenylpyridine-type (ppy-type) ligand with the dithieno[3,2-b:2',3'-d]phosphole oxide (DTPO) group has been successfully synthesized. Based on this novel ligand, three cyclometalated iridium(iii) complexes (P-Ir-P, P-Ir-T and P-Ir-C) are synthesized with symmetrical and unsymmetrical structures. Photophysical results reveal that these cyclometalated iridium(iii) complexes can show weak near-infrared (NIR) phosphorescence emission with wavelengths of 739 nm for P-Ir-P, 750 nm for P-Ir-T and 746 nm for P-Ir-C. Importantly, transient absorption characterization shows that these cyclometalated iridium(iii) complexes can exhibit strong excited state absorption in the range of ca. 520 to 700 nm, indicating their optical power limiting (OPL) potential in this wavelength range. Open-aperture Z-scan against a 532 nm laser shows their OPL ability in the order of P-Ir-P > P-Ir-C > P-Ir-T. Complex P-Ir-P shows an even better OPL ability than the state-of-the-art OPL material C60, indicating the important potential application of these cyclometalated iridium(iii) complexes as new OPL materials.

12.
Inorg Chem ; 58(21): 14478-14489, 2019 Nov 04.
Artigo em Inglês | MEDLINE | ID: mdl-31618013

RESUMO

A new sublimable dicopper(I) complex bearing 1,2-bis(diphenylphosphino)ethane and 5-trifluoromethyl-3-(2'-pyridyl)pyrazolate ligands has been designed and synthesized, and its crystalline solvated and nonsolvated compounds have also been obtained and investigated. It is shown that only the crystalline solvated compound exhibits reversible and selective luminescence vapochromism, arising from its unique "pyridyl/CH2Cl2/pyridyl" organic sandwich-like stacking arrangement revealed by X-ray crystallography, as supported by time-dependent density functional theory calculations. Additionally, the neutral Cu(I) complex has excellent thermal stability and sublimability, good solid-state luminescence properties, and TADF character, and it is suggested to be a good emitter for vapor-deposited organic light-emitting diodes.

13.
ACS Appl Mater Interfaces ; 11(29): 26152-26164, 2019 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-31265247

RESUMO

Highly efficient deep-red organic light-emitting devices (OLEDs) are indispensable for developing high-performance red-green-blue (RGB) displays and white OLEDs (WOLEDs). However, the shortage of deep-red emitters with high photoluminescence quantum yields (PLQYs) and balanced charge injection/transport abilities has severely restricted the performance of deep-red OLEDs. Herein, we design and synthesize four efficient emitters by combining the isoquinoline group with the thianthrene 5,5,10,10-tetraoxide group. Benefited from the introduction of the thianthrene 5,5,10,10-tetraoxide group, these Ir(III) complexes show improved electron-injection/-transport abilities. By enhancing the contribution of the triplet metal-to-ligand charge transfer (3MLCT) in emissions, the asymmetric configuration endows the related deep-red Ir(III) complexes with high PLQYs of 0.45-0.50 in solutions. More importantly, PLQYs of these Ir(III) complexes in doped host films increase up to 0.91, which is much higher than PLQYs reported for conventional deep-red Ir(III) complexes with impressive electroluminescent performance. As a result, solution-processed OLEDs based on these Ir(III) complexes exhibit deep-red emissions with Commission Internationale de L'Eclairage (CIE x, y) coordinates very close to the National Television System Committee (NTSC)-recommended standard red CIE coordinates of (0.67, 0.33). Furthermore, a deep-red OLED using the asymmetric Ir(III) complex SOIrOPh as the emitter shows outstanding performance with a peak external quantum efficiency (EQE) of 25.8%, which is the highest EQE reported for solution-processed deep-red OLEDs. This work sheds light on the great potential of utilizing the thianthrene 5,5,10,10-tetraoxide group to develop phosphorescent emitters for highly efficient OLEDs.

14.
ACS Appl Mater Interfaces ; 11(30): 27112-27124, 2019 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-31271029

RESUMO

With the 9-phenyl-9-phosphafluorene oxide (PhFlOP) moiety as the acceptor (A) and various donors (D), a series of new organic emitters have been synthesized with a D-A-D configuration. Their photophysical and electrochemical behaviors and electroluminescent (EL) performances have been characterized in detail. The photophysical results have indicated that the PhFlOP-based emitters with acridyl, phenoxazyl, and phenothiazyl as donors show efficient, thermally activated delayed fluorescence (TADF) behavior, especially for the TADF emitter with the phenoxazyl donor possessing an exceptionally high rate constant of reverse intersystem crossing (kRISC) of 6.2 × 105 s-1. It has also been found that their TADF behavior can be greatly affected by the substitution position of the donors. Different from the reported aryl phosphine oxide (APO) acceptors in TADF emitters, the PhFlOP moiety adopts a highly rigid configuration to guarantee a photoluminescent quantum yield as high as 0.80 in the 4,4'-N,N'-dicarbazolebiphenyl film, representing the top-ranking emission ability for the TADF emitters with APO-type acceptors. Benefitting from their advanced TADF performances, the doped organic light-emitting diodes/devices based on these PhFlOP-based TADF emitters can achieve exceptional EL performances with the maximum external quantum efficiency (ηext) of 23.3%, current efficiency (ηL) of 83.7 cd A-1, and power efficiency (ηP) of 59.1 lm W-1. These encouraging EL data show the great potential of the PhFlOP moiety in developing highly efficient TADF emitters.

15.
Inorg Chem ; 58(11): 7393-7408, 2019 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-31094518

RESUMO

Three Ir(C∧N)2(acac)-type and one Ir(C1∧N)(C2∧N)(acac)-type coumarin-based cyclometalated Ir(III) complex isomers (IrC5, IrC7, IrC7-A, and IrC8) have been obtained using three coumarin-based isomers of 2-phenylpyridine (ppy)-type cyclometalating ligands (L-C5, L-C7, and L-C8). Two coordination isomers emerging as principal products (IrC7 and IrC7-A) are obtained in the synthesis of corresponding coumarin-based cyclometalated Ir(III) complexes because of two different coordination sites in ligand L-C7 to form a C-Ir bond. To the best of our knowledge, there are no such isomers reported to date. Interestingly, a broad range of phosphorescent color tuning from green (IrC8, λ = 516 nm) to red (IrC5, λ = 608 nm) has been realized through variation of the pyridyl substitution positions on the fused phenyl ring of the coumarin skeleton. In addition, based on natural transition orbital (NTO) analyses, features of the lowest triplet excited states (T1) from these coumarin-based cyclometalated Ir(III) complex isomers can be tuned easily by these ligand isomers as well. IrC5, IrC7, and IrC7-A show prevailing 3MLCT character associated with their T1 states which emit the phosphorescent signals, while the T1 state of IrC8 exhibits the dominant ligand-centered π-π* transition feature. Importantly, owing to the strong rigidity of the coumarin skeleton, all the coumarin-based cyclometalated Ir(III) complex isomers can show high phosphorescent quantum yields Φp (ca. 0.4-1). Together with the improved electron-injection/electron-transport (EI/ET) ability, all the phosphorescent emitters display impressive electroluminescence (EL) performance. The device based on IrC8 gives the highest EL efficiencies of external quantum efficiency (ηext) 22.7%, current efficiency (ηL) 79.7 cd A-1, and power efficiency (ηP) 58.2 lm W-1, representing the most state-of-the-art EL ability ever achieved by coumarin-based phosphorescent emitters. All these encouraging data definitely suggest the great potential of the coumarin skeleton in both easy tuning of the photophysical properties of ppy-type Ir(III) phosphorescent complexes and developing high-performance phosphorescent emitters.

16.
Adv Sci (Weinh) ; 6(7): 1801930, 2019 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-30989026

RESUMO

Phosphorescent near-infrared (NIR) organic light-emitting devices (OLEDs) have drawn increasing attention for their promising applications in the fields such as photodynamic therapy and night-vision readable displays. Here, three simple phosphorescent Pt(II) complexes are synthesized, and their intermolecular interactions are investigated in crystals and neat films by X-ray single crystal diffraction and grazing-incidence wide-angle X-ray scattering, respectively. The photophysical properties, molecular aggregation (including Pt-Pt interaction), molecular packing orientation, and electron transport ability are all influenced by the strong intermolecular hydrogen bonds. Consequently, the nondoped OLEDs based on tBu-Pt and F-Pt show electroluminescent emissions in NIR region with the highest external quantum efficiencies of 13.9% and 16.7%, respectively.

17.
Adv Sci (Weinh) ; 6(2): 1801432, 2019 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-30693186

RESUMO

Graphene quantum dot (GQD) encapsulated melamine-formaldehyde (MF) polymer microspheres with uniform particle size and tunable high-quality white-light emissions are prepared via a polymer-mediated GQD assembly and encapsulation strategy. In solution, GQDs are first aggregated with MF prepolymer through electrostatic interaction and further encapsulated inside the microspheres formed by polymerization of MF prepolymer under acid catalysis and heating. During this process, the aggregated GQDs are fixed in the MF polymer matrix with their emission extended from blue to full visible range, presenting bright white luminescence under ultraviolet excitation. The prepared white-light-emitting GQD-MF microspheres exhibit uniform morphology with an average particle size of 2.0 ± 0.08 µm and their luminescence properties are effectively regulated by the doping concentration of GQDs in the MF polymer matrix. A series of white-light-emitting GQD-MF microspheres with quantum yields from 0.83 to 0.43, Commission Internationale de L'Eclairage coordinates from (0.28, 0.28) to (0.33, 0.32), and color rendering index from 0.75 to 0.88 are obtained with excellent photostability and thermal stability. By dispersing the GQD-MF microspheres in cross-linked polydimethylsiloxane matrix, flexible film with dual functions of high-quality white-light-emitting and light diffusion is obtained and successfully applied for white light-emitting diode fabrication.

18.
Chem Rec ; 19(8): 1710-1728, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-30637911

RESUMO

Color-tuning for phosphorescent emitters in organic light-emitting diodes (OLEDs) across the entire visible spectrum is prerequisite to fulfil flexible full-color displays and white solid-state lighting. Heteroleptic 2-phenylpyridine-type (ppy-type) Ir(III) and Pt(II) complexes as phosphorescent emitters have been well exploited in the electroluminescence (EL) field due to their outstanding EL performance. Furthermore, the photophysical characters of these heteroleptic Ir(III) and Pt(II) complexes are generally dominated by the nature of cyclometalating ppy-type ligands. Accordingly, either sophisticated modification or judicious combination of different cyclometalating ppy-type ligands will provide a wonderful platform to tune their emission color. In this personal account, we put a special emphasis on our contributions to the novel color-tuning strategies in these heteroleptic ppy-type Ir(III) and Pt(II) complexes. In addition, afforded by our novel color-tuning strategies, ambipolar character or enhanced electron injection/transport (EI/ET) features can be furnished to bring high EL performances.

19.
Inorg Chem ; 57(17): 11027-11043, 2018 Sep 04.
Artigo em Inglês | MEDLINE | ID: mdl-30129751

RESUMO

With the aim of evaluating the potential of selenium-containing groups in developing electroluminescent (EL) materials, a series of asymmetric heteroleptic Ir(III) phosphorescent complexes (Ir-Se0F, Ir-Se1F, Ir-Se2F, and Ir-Se3F) have been synthesized by using 2-selenophenylpyridine and one ppy-type (ppy = 2-phenylpyridine) ligand with a fluorinated selenide group. To the best of our knowledge, these complexes represent unprecedented examples of asymmetric heteroleptic Ir(III) phosphorescent emitters bearing selenium-containing groups. Natural transition orbital (NTO) analysis based on optimized geometries of the first triplet state (T1) have shown that the phosphorescent emissions of these Ir(III) complexes dominantly show 3π-π* features of the 2-selenophenylpyridine ligand with slight metal to ligand charge transfer (MLCT) contribution. In comparison with their symmetric parent complex Ir-Se with two 2-selenophenylpyridine ligands, these asymmetric heteroleptic Ir(III) phosphorescent complexes can show much higher phosphorescent quantum yields (ΦP) of ca. 0.90. Both the hole- and electron-trapping ability of these Ir(III) phosphorescent complexes can be enhanced by selenophene and fluorinated selenide groups to improve their EL efficiencies. The EL abilities of these asymmetric heteroleptic Ir(III) phosphorescent emitters fall in the order Ir-Se3F > Ir-Se2F > Ir-Se1F > Ir-Se0F. The highest EL efficiencies have been achieved by Ir-Se3F in the solution-processed OLEDs with external quantum efficiency (ηext), current efficiency (ηL), and power efficiency (ηP) of 19.9%, 65.6 cd A-1, and 57.3 lm W-1, respectively. These encouraging EL results clearly indicate the great potential of selenium-containing groups in developing high-performance Ir(III) phosphorescent emitters.

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