Hybridized Local And Charge-transfer Research Articles

Efficient Deep-Blue Fluorescent OLEDs Based on a D-π-A Emitter Profiting From Intramolecular Hydrogen Bonds and a Hybridized Excited State.

High performance deep-blue emitters with a Commission International de l'Eclairage (CIE) coordinate of CIEy≤0.08 are highly desired in ultrahigh-definition displays. Herein, we designed and synthesized an efficient D-π-A deep-blue emitter, 2-(6-([1,1' : 3',1''-terphenyl]-5'-yl)pyridin-3-yl)-1-phenyl-1H-phenanthro[9,10-d] imidazole (mPTPH), using the synergistic effect of intramolecular hydrogen bond (H-bond) and hybridized excited state. Single-crystal structure analysis confirmed that there exist intra- and intermolecular H-bond interactions which could inhibit the structure vibration and increase photoluminescence efficiency. The photophysical and theoretical results show that mPTPH exhibited hybridized local and charge-transfer (HLCT) feature with strong deep-blue emission. Ultimately, the non-doped device based on mPTPH exhibited high maximum luminance of 20610 cd m-2. The doped device achieved high maximum external quantum efficiency of 5.4 % and small efficiency roll-off with deep-blue emission peak of 413 nm and CIE coordinate of (0.16, 0.08).

High‐Efficiency Deep‐Blue Solution‐Processed Organic Light‐Emitting Diodes Using Carbazole Dendrons Modified Hybridized Local and Charge‐Transfer Emitters

In the pursuit of efficient and cost‐effective organic light‐emitting diodes (OLEDs), the development of solution‐processed hybridized local and charge transfer (HLCT) emitters presents a promising approach. HLCT materials uniquely integrate the advantages of both singlet and triplet excitons, surpassing the traditional spin statistical limit of 25% while offering high photoluminescence efficiency and balanced charge transport properties. Herein, we report the synthesis and characterization of two new deep blue, solution‐processable HLCT fluorophores, G1FTPI and G2FTPI. These compounds incorporate fluorenyl carbazole dendron units into the HLCT luminogenic triphenylamine‐phenanthroimidazole (TPI) molecule. Their HLCT and photoluminescence (PL) properties were experimentally and theoretically investigated using solvation effects and density functional theory (DFT) calculations. The molecules exhibit deep blue emission with a high solid‐state fluorescence quantum yield, good solution‐processed film‐forming quality, and high hole mobility values of 2.18 – 2.61 × 10‐6 cm2 V‐1s‐1. Both compounds were successfully employed as non‐doped emissive layers in solution‐processed OLEDs, demonstrating excellent electroluminescent (EL) performance. Notably, the G2FTPI‐based device emitted a deep blue light at 432 nm with CIE coordinates of (0.158, 0.098) and achieved a a maximum current efficiency (CEmax) of 3.13 cd A‐1 and a maximum external quantum efficiency (EQEmax) of 5.30%.

Efficient Triplet Harvesting via Hot Exciton Utilization in Solution Processed OLEDs Employing Tetraphenyl Buta‐1,3‐Diene Based AIE Emitters

AbstractHigh photoluminescence quantum yield (PLQY) especially in solid‐state together with harvesting radiative triplet excitons are essential to achieve efficient organic light‐emitting diodes (OLEDs). Herein, the aggregation induced emission (AIE) active tetraphenyl buta‐1,3‐diene (TPB) moiety has been employed and tactfully modified to obtain orthogonally oriented donor‐acceptor (D‐A‐π‐A‐D) type derivatives (namely, TPB‐CHO‐TPA and TPB‐CN‐TPA) which possess additionally the hybridized local and charge transfer (HLCT) type excited‐state. Moreover, computational studies have revealed the possibility of triplet harvesting through hot exciton mechanism in these designed emitters. These key features along with excellent solubility in most of the organic solvents have encouraged to utilize these as light emitting materials for solution processed non‐doped and doped OLED devices. The optimal OLED device using TPB‐CHO‐TPA exhibits yellow light emission (ELmax = 572 nm and CIEx,y = 0.48, 0.51) having maximum external quantum efficiency (EQEmax) of 7.6% with power and current efficiency of 6.1 lm W−1 and 8.9 cd A−1 where the calculated exciton utilization efficiency (EUE) approaches to 97%, indicating efficient triplet harvesting in electroluminescence process. This work signifies a novel design strategy for AIE‐based HLCT type emitters having efficient hot exciton utilization which can pave the way for future development of TPB based highly efficient OLED devices.

Rational Molecular Design of Phenanthroimidazole-Based Fluorescent Materials toward High-Efficiency Deep-Blue OLEDs by Molecular Isomer Engineering.

Organic light-emitting diodes (OLEDs) have been extensively investigated in full-color displays and energy-saving lighting owing to their unique advantages. However, deep-blue OLEDs based on nondoped emitting layers with a satisfactory external quantum efficiency (EQE) are still rare for applications. In this work, six hot exciton materials, PPIM-12F, PPIM-22F, PPIM-13F, PPIM-23F, PPIM-1CN, and PPIM-2CN, are designed and synthesized via an isomer engineering design strategy and their photophysical properties and OLED performance are systematically investigated. These emitters all possess wide band gaps (3.53-3.69 eV), hybrid local and charge transfer (HLCT) characteristics, and good thermal stabilities. The C2 series compounds, PPIM-22F, PPIM-23F, and PPIM-2CN, all show redder emission peaks than the N1 series counterparts of PPIM-12F, PPIM-13F, and PPIM-1CN. In addition, the LUMO energy levels decrease consecutively in the sequence of PPIM-22F < PPIM-23F < PPIM-2CN and are all lower than their respective N1 series position isomers of PPIM-12F, PPIM-13F, and PPIM-1CN. The CV measurements indicate that such a design strategy renders the fine-tuning of LUMO energy levels, and the incorporation of electron acceptors at the extended C2 position of the PI unit is a better choice to improve the electron injection ability. Theoretical simulations indicate that they may harvest the triplet exciton through an upper-level reverse intersystem crossing process, which decreases the gathering of triplet excitons and allows the OLEDs to be fabricated by nondoping technology. Among them, PPIM-22F with a difluorobenzene substituent at the C2 position manifests the best performance in OLEDs, which exhibits the maximum EQE of 7.87% and Commission Internationale de ĺEclairage (CIE) coordinates of (0.16, 0.10). This work demonstrates an effective strategy for considerable improvement in device performance by a subtle change in the molecular structure through isomer engineering.

Hybrid Local and Charge Transfer Emitters Utilizing Hyperconjugation Effect Towards Solution-Processed Ultra-Deep-Blue OLEDs with External Quantum Efficiency Approaching 12.

Hybrid local and charge transfer (HLCT) excited state materials, which possess weak donor-acceptor (D-A) pure organic structures, deserve one of the most promising efficient and stable blue emitters. Through high-lying reverse intersystem crossing (hRISC) process, 75% triplet excitons generated by electrical excitation could be harvested and utilized in organic light-emitting diodes (OLEDs). However, there are still significant challenges to achieve high-efficiency ultra-deep-blue HLCT emitters with low Commission Internationale de l'Eclairage (CIE) 1931 chromaticity coordinate y values. Here, a series of novel blue HLCT emitters based on spiro[1,8-diazafluorene-9,2'-imidazole] structure were designed and synthesized by fine-tuning the spiro[fluorene-9,2'-imidazole] core structure in our previous work through heteroatom substitution and hyperconjugation effect. The target emitters were endowed with excellent photophysical and electrochemical merits, thermal stability and solution processibility. The solution-processed OLED device based on 4',5'-bis(4-(9H-carbazol-9-yl)phenyl)spiro[1,8-diazafluorene-9,2'-imidazole] (NFIP-CZ) achieved efficient ultra-deep-blue emission (CIEx,y = 0.1581, 0.0422) with the maximum external quantum efficiency (EQEmax), maximum current efficiency (CEmax) and maximum power efficiency (PEmax) of 11.94%, 4.07 cd·A-1 and 2.56 lm·W-1. The record EQE is a breakthrough in both solution-processed and vacuum vapor deposition ultra-deep-blue HLCT-OLEDs currently.

High‐Lying Triplet Excitons Utilization of Silole Derivatives Enables their Efficiency Breakthrough in OLEDs

AbstractSiloles are routinely studied in the application of organic light‐emitting diodes (OLEDs) due to their high performances of solid‐state fluorescence property and carrier mobility. The structures of siloles used in electroluminescence device reported so far can only utilize singlet excitons, limiting the device efficiency and commercialization. Seeking to build appliable molecular structures to achieve triplet excitons utilization in silole‐core emitters, two derivatives are designed, Silole‐1DPA‐TRZ and Silole‐1Cz‐TRZ, in which electron acceptor of triazine (TRZ) together with electron donors of diphenylamine (DPA) and carbazole (Cz) modified at 1‐position of silole unit form silole‐D‐A structures. This special molecular design, for the first time, enables triplet excitons harvest via high‐lying reverse intersystem crossing (hRISC) process in silole derivatives with hybridized local and charge‐transfer (HLCT) characteristics. Experimental and theoretical studies show that relative to a stronger charge transfer state of Silole‐1Cz‐TRZ, a more equal local excitation/charge transfer distribution in the HLCT state of Silole‐1DPA‐TRZ is realized, making its application in silole‐based OLED with an efficiency breakthrough of ≈9.1% maximum external quantum efficiency (EQEmax).

Deep-blue electroluminescence with orthogonal donor-acceptor structure: The role of charge-transfer excited state component in hybrid local and charge-transfer (HLCT) excited state

In this work, three orthogonally bonded phenanthroimidazole based donor-acceptor (D-A) structured blue-emissive materials N-SBPMCN, N-ABPMCN and N-TBPMCN with different donor moieties are designed synthesized. Theoretical combined experimental researches proved that the involving of weak donor (spiro-fluorene and anthracene) and strong donor triphenylamine can form different locally-emissive (LE) dominated hybrid local and charge-transfer (HLCT) excited state, which can contribute to their high photoluminescent quantum yield (PLQY), satisfied electroluminescence performance and blue purity. Specifically, N-TBPMCN with strong donor triphenylamine that possesses more CT excited state components demonstrates the best electroluminescence performance and blue purity among the three materials, revealing that the molecular design of orthogonal D-A structure is of great potential in blue-emissive functional materials. Additionally, we also discovered that intermolecular CT state can also contribute to high exciton utilization.

Revelation of room temperature liquid crystallinity and yellow-orange electroluminescence (EQE>7%) in a columnar self-assembled N-annulated perylene bisimide

The synthesis of highly fluorescent compounds is a critical necessity to facilitate cost-effective and metal-independent production of organic light-emitting diodes (OLEDs). This investigation introduces a readily soluble, electron-deficient N-annulated perylene bisimide (PBI-NST) equipped with a swallow tail, exhibiting room temperature columnar oblique mesophase with a low clearing point and high photoluminescence quantum yield, positioning it as a promising candidate for efficient OLEDs. Leveraging the luminescent properties of PBI-NST, a series of OLED devices were fabricated with PBI-NST as the sole emitter and at various concentrations in CBP host material. Impressively, doped devices employing the compound at 0.5 wt% emitter within the host material CBP displayed an exceptional external quantum efficiency (EQE) of 7.2 %, accompanied by a luminance of 2689 cd/m2. Further, a voltage dependent emission tuning was also noticed. The notable increase in EQE is mainly attributed to the contributions of hybrid local and charge transfer (HLCT) and triplet–triplet annihilation (TTA) process. The substantial enhancement in EQE marks a significant advancement in the application of multifunctional columnar self-assembled materials for OLED development.

Hybrid Local and Charge-Transfer Material with Ultralong Room Temperature Phosphorescence for Efficient Organic Afterglow Light-Emitting Diodes.

Organic ultralong room temperature phosphorescence (OURTP) materials capable of combining various emission behaviors for diversified optoelectronic properties and applications have recently gained a vigorous development, but it remains a forbidden challenge in designing OURTP molecules with hybrid local and charge-transfer (HLCT) feature, possibly due to the elevated difficulties in simultaneously meeting the stringent requirements of both HLCT and OURTP emitters. Here, through introducing multiple heteroatoms into one-dimensional fused ring of coumarin with moderate charge transfer perturbation in donor-π-acceptor architecture, we demonstrate a HLCT-featured OURTP molecule showing both promoted fluorescence with a quantum yield of 77% in solution and long-lived OURTP with a lifetime of 251 ms in conventional host material used in electroluminescent device. Thus, efficient OURTP organic light-emitting diodes (OLEDs) were fabricated, exhibiting bright electroluminescence with an exciton utilization efficiency of 85% and yellow OURTP lasting over 2 s for afterglow. Impressively, the HLCT OURTP-OLEDs can be further optimized to reach an unprecedented total external quantum efficiency (EQE) of ~12% and OURTP EQE up to 3.11%, representing the highest performance among the reported OURTP-OLEDs. These impressive results highlight the significance to fuse HLCT and OURTP together in enriching OURTP materials and improving the afterglow OLED performances.

Oligocarbazole modified hybridized local and charge transfer emitters for efficient solution-processed deep blue organic light-emitting diodes

Herein, two new blue solution-processable hybridized local and charge transfer (HLCT) fluorophores (pCTPI and mCTPI) were designed and synthesized by incorporating oligocarbazole fragment into the HLCT luminogenic triphenylamine-phenanthroimidazole (TPI) molecule. Their HLCT and photoluminescence properties were experimentally and theoretically probed by the solvation effect and density functional theory calculations. These materials exhibited an intense blue emission (440 nm) with a good solution-processed film-forming quality and decent hole mobility (3.98–4.55 × 10−6 cm2 V−1s−1), resulting in a successful utilization as non-doped emissive layers in simple solution-processed organic light-emitting diodes (OLEDs). The devices showed deep blue emission (430 nm) with excellent electroluminescence (EL) performance and narrow EL emission as compared to the TPI-based device. Notably, pCTPI-based solution-processed OLED achieved a luminance of 4938 cd m−2 and an external quantum efficiency of 6.35 %.

An efficient “hot exciton” fluorophore based on a dicyanophenanthrene-triphenylamine hybrid

The study presents the design, synthesis, and characterization of DCNP-2TPA, a novel “hot exciton” fluorophore featuring a donor-acceptor structure combining dicyanophenanthrene and triphenylamine. Through a comprehensive analysis including structural examination, theoretical modeling, and optical assessments, the suitability of DCNP-2TPA for integration into organic light-emitting diodes (OLEDs) is evaluated. Comparative to existing dicyanophenanthrene-based emitters, DCNP-2TPA demonstrates significantly enhanced luminescence efficiency, by virtue of the incorporation of two triphenylamine moieties with moderate electron-donating strength. Furthermore, DCNP-2TPA exhibits aggregation-induced emission (AIE) properties and showcases hybridized local and charge-transfer (HLCT) excited states, offering an efficient "hot exciton" channel for triplet harvesting. Employing DCNP-2TPA as the emissive core, OLED devices achieve a noteworthy external quantum efficiency of 8.42 %, highlighting the promise of DCNP-2TPA as an efficient candidate for OLED applications.

Efficient and ultra-high luminance orange-red organic light emitting diode (OLED) based on triphenylamine-benzothiadiazole-phenoxazine hybrid molecule with hybrid local and charge-transfer (HLCT) characteristic

Due to the energy gap law, red emission needs relatively narrow energy gap, thus the nonradiative transition rate (knr) grows exponentially and eventually impacts the materials fluorescent efficiency. Here, an orange-red emission donor-acceptor-π-donor (D-A-π-D’) material N, N-diphenyl-4-(7-(4-(10-phenyl-10 H-phenoxazin-3-yl) phenyl) benzo [c] (Huang et al., 2019; Park et al., 2008; Caspar et al., 1982) [1,2,5] thiadiazol-4-yl) aniline (TBphPP) was designed and synthesized. Introducing a benzene π-bridge between the strong donor 10-phenyl-10H-phenoxazin (PPOX) and acceptor 2,1,3-benzothiadiazole (BTZ) not only is able to stretch the molecular conjugation so as to increase the proportion of LE state in hybrid local and charge-transfer (HLCT) state but also increase the overlap area of the electron cloud to improve luminous efficiency. As a result, the non-doped organic light-emitting diode (OLED) of TBphPP exhibited high luminance of 17,886 cd m−2 and relatively high exciton utilization efficiency (EUE) of 44 % with a standard red electroluminescent peak at 620 nm. Importantly, the optimized doped device based on TBphPP achieved high performance that the maximum external quantum efficiency (EQEmax) was up to 9.86 % with a higher EUE of 66.2 % and the efficiency roll-off (ηroll-off) at 100,000 cd m−2 was only 3.55 %. Simultaneously, it has reached ultra-high luminescence of 180,583 cd m−2, high current efficiency of 29.02 cd A−1 and power efficiency of 16.47 l m W−1. To our knowledge, the TBphPP device with such ultra-high luminance and high efficiency is one of the best performance orange-red materials based on HLCT characteristic.

Rational Design of Coumarin-Based Hybridized Local and Charge-Transfer Blue Emitters for Solution-Processed Organic Light-Emitting Diodes.

Hybridized local and charge-transfer (HLCT) with the utilization of both singlet and triplet excitons through the "hot excitons" channel have great application potential in highly efficient blue organic light-emitting diodes (OLEDs). The proportion of charge-transfer (CT) and locally excited (LE) components in the relevant singlet and triplet states makes a big difference for the high-lying reverse intersystem crossing process. Herein, three novel donor (D)-acceptor (A) type HLCT materials, 7-([1,1'-biphenyl]-4-yl(9,9-dimethyl-9H-fluoren-2-yl)amino)-3-phenyl-1H-isochromen-1-one (pPh-7P), 7-([1,1'-biphenyl]-4-yl(9,9-dimethyl-9H-fluoren-2-yl)amino)-3-methyl-1H-isochromen-1-one (pPh-7M), and 6-([1,1'-biphenyl]-4-yl(9,9-dimethyl-9H-fluoren-2-yl)amino)-3-methyl-1H-isochromen-1-one (pPh-6M), were rationally designed and synthesized with diphenylamine derivative as donor and oxygen heterocyclic coumarin moiety as acceptors. The proportions of CT and LE components were fine controlled by changing the connection site of diphenylamine derivative at C6/C7-position and the substituent at C3-position of coumarin moiety. The HLCT characteristics of pPh-7P, pPh-7M, and pPh-6M were systematically demonstrated through photophysical properties and density functional theory calculations. The solution-processed doped OLEDs based on pPh-6M exhibited deep-blue electroluminescence with the maximum emission wavelength of 446 nm, maximum luminance of 8755 cd m-2, maximum current efficiency of 5.83 cd A-1, and maximum external quantum efficiency of 6.54 %. The results reveal that pPh-6M with dominant 1LE and 3CT components has better OLED performance.

Achieving Record External Quantum Efficiency of 11.5 % in Solution-Processable Deep-Blue Organic Light-Emitting Diodes Utilizing Hot Exciton Mechanism.

High performance solution-processable deep-blue emitters with a Commission International de l'Eclairage (CIE) coordinate of CIEy≤0.08 are highly desired in ultrahigh-definition display. Although, deep-blue materials with hybridized local and charge-transfer (HLCT) excited-state feature are promising candidates, their rigidity and planar molecular structures limit their application in solution-processing technique. Herein, four novel deep-blue solution-processable HLCT emitters were first proposed by attaching rigid imide aliphatic rings as functional units onto the HLCT emitting core. The functional units not only improve solubility, enhance thermal properties and morphological stability of the emitting core, but also promote photoluminescence efficiency, balance charge carrier transport, and inhibit aggregation-caused quenching effect due to the weak electron-withdrawing property as well as steric hindrance. The corresponding solution-processable organic light-emitting diodes (OLEDs) substantiate an unprecedented maximum external quantum efficiency (EQEmax) of 11.5 % with an emission peak at 456 nm and excellent colour purity (full width at half maximum=56 nm and CIEy=0.09). These efficiencies represent the state-of-the-art device performance among the solution-processable blue OLEDs based on the "hot exciton" mechanism. This simple strategy opens up a new avenue for designing highly efficient solution-processable deep-blue organic luminescent materials.

Achieving Record External Quantum Efficiency of 11.5 % in Solution‐Processable Deep‐Blue Organic Light‐Emitting Diodes Utilizing Hot Exciton Mechanism

AbstractHigh performance solution‐processable deep‐blue emitters with a Commission International de l′Eclairage (CIE) coordinate of CIEy≤0.08 are highly desired in ultrahigh‐definition display. Although, deep‐blue materials with hybridized local and charge‐transfer (HLCT) excited‐state feature are promising candidates, their rigidity and planar molecular structures limit their application in solution‐processing technique. Herein, four novel deep‐blue solution‐processable HLCT emitters were first proposed by attaching rigid imide aliphatic rings as functional units onto the HLCT emitting core. The functional units not only improve solubility, enhance thermal properties and morphological stability of the emitting core, but also promote photoluminescence efficiency, balance charge carrier transport, and inhibit aggregation‐caused quenching effect due to the weak electron‐withdrawing property as well as steric hindrance. The corresponding solution‐processable organic light‐emitting diodes (OLEDs) substantiate an unprecedented maximum external quantum efficiency (EQEmax) of 11.5 % with an emission peak at 456 nm and excellent colour purity (full width at half maximum=56 nm and CIEy=0.09). These efficiencies represent the state‐of‐the‐art device performance among the solution‐processable blue OLEDs based on the “hot exciton” mechanism. This simple strategy opens up a new avenue for designing highly efficient solution‐processable deep‐blue organic luminescent materials.

Enhancing Fast RISC in Hot‐Exciton Thermally Activated Delayed Fluorescence Emitter Through Fused Ring Modification: A Theoretical Insights

AbstractRecent progress has shown promising advancements in enhancing the Reverse intersystem crossing (RISC) process between high‐energy triplet states (Tn, n ≥ 1) and radiative singlet states (Sm) through the utilization of the classic D‐A‐D' strategy. In this study, 12 molecules employing phenyl carbazole and a peripheral phenanthroimidazole as the donors and fused cores as acceptors are theoretically designed. Additionally, electron‐withdrawing groups such as fluorine and cyano, as well as electron‐donating group like methoxy, are incorporated into anthracene, napthaoxadiazole, and napthothiadiazole derivatives, acting as fused core components. Theoretical analyses reveal that among the molecules examined, eight adhere to the three golden principle rules, demonstrating a large energy gap between S1‐T1, the minimal ΔES1‐T2, and large T2‐T1. Additionally, these molecules exhibit significant Spin‐orbit coupling (SOC) and maintain a strong Hybridized local and charge transfer (HLCT) character, facilitating the fast hRISC from T2 to S1. The auxiliary inclusion of heteroatoms, such as oxygen and sulfur, on the anthracene core, aligns with the prerequisite strategy, ultimately reinforcing the SOC. Furthermore, replacing the methoxy group on the Nz bridge significantly enhances the SOC, resulting in a substantial increase in the hRISC rate (10 +08 s−1). Overall, the findings substantially elevate the photophysical attributes of the designed molecules through the utilization of the hRISC channel.

New Phenanthro[9,10-d]oxazole-Based Fluorophores with Hybridized Local and Charge-Transfer Characteristics for Highly Efficient Blue Non-Doped OLEDs with Negligible Efficiency Roll-Off.

It is vital to develop highly efficient non-doped blue organic light-emitting diodes (OLEDs) with high color purity and low-efficiency roll-off for applications in display and lighting. Herein, two blue D-A fluorophores TPA-PO and TPA-DPO are designed and synthesized, in which phenanthro[9,10-d]oxazole (PO) acts as the acceptor and triphenylamine as the donor. TPA-PO and TPA-DPO display good thermal stability and efficient luminescence efficiency in neat film. Results based on photophysical property and theoretical calculation demonstrate that TPA-PO and TPA-DPO possess the hybridized local and charge-transfer (HLCT) feature, which can utilize the triplet exciton to achieve highly efficient electroluminance (EL). The non-doped OLEDs with TPA-PO/TPA-DPO as pure emissive layer show the uniform EL emission peak at 468 nm, corresponding to CIE coordinates of (0.168, 0.187) and (0.167, 0.167), respectively. The TPA-DPO-based non-doped OLEDs provide the maximum external quantum efficiency (EQE) of 7.99 % and high exciton utility efficiency of 48.4 %~72.6 %. Moreover, the TPA-DPO-based device exhibits low-efficiency roll-off, still maintaining the EQE of 6.03 % at the high luminance of 5000 cd m-2. Those findings state clearly that PO is a promising building block of blue fluorophore with a potential HLCT feature to be applied in non-doped OLEDs.

Deep red/near-infrared electro-fluorescence material with nearly 10% external quantum efficiency based on hybridized local and charge-transfer

Although the hot exciton mechanism with hybridized local and charge-transfer (HLCT) characteristics is a promising molecular design strategy, there are few organic deep red (DR) and near-infrared (NIR) HLCT-type emitters with high external quantum efficiency (EQE). Herein, this work reports three DR/NIR emitters with high EQE, TNZ-3PPOXP, TPANZPOXP, and 2PPOXNZ. These emitters show DR/NIR emission in the neat film, 664 nm for TNZ-3PPOXP, 718 nm for TPANZPOXP, and 724 nm for 2PPOXNZ. Interestingly, the emitters all possess hybridized local and charge-transfer (HLCT) characteristics and potential hot exciton channels. The corresponding non-doped OLED achieve high exciton utilization efficiency (EUE) and NIR emission, 55.6 %@694 nm for TNZ-3PPOXP, 82.8 %@736 nm for TPANZPOXP, and 42.3 %@756 nm for 2PPOXNZ. More importantly, with these emitters as the guest, PO-01 as the phosphorescent sensitizer, and CBP as the host, the sensitization device achieved nearly 10 % EQE, 9.55 %@662 nm for TNZ-3PPOXP, 4.20 %@699 nm for TPANZPOXP, and 4.49 %@702 nm for 2PPOXNZ. To our knowledge, this is one of the highest device efficiencies based on HLCT as the guest.

A Breakthrough in Color‐Tunable All‐Fluorescent White OLEDs through the Cooperation Between a New Blue HLCT Fluorophore and a Long‐Wavelength TADF Emitter

AbstractIt is a vitally important and challenging task to achieve high efficiency and wide color‐tunable white organic light emitting diodes (CT‐WOLEDs) meeting the needs of various decoration and lighting applications. Here, a high‐performance single‐cell all‐fluorescent CT‐WOLED with a single‐doped single‐emissive‐layer structure has been developed employing a multi‐functional hybrid local and charge transfer (HLCT) fluorophore 2‐(4‐(9H‐carbazol‐9‐yl)−2′,5′‐difluoro‐[1,1′:4′,1′'‐terphenyl]−4‐yl)−1‐phenyl‐1H‐phenanthro[9,10‐d]imidazole (PICZ2F) as a deep‐blue emitter as well as an effective host for a yellow thermally activated delayed fluorescence emitter. The record‐breaking power efficiency of 89.50 lm W‒1 and correlated color temperature (CCT) span from 3749 to 18 279 K are achieved simultaneously, which is not only one of the state‐of‐the‐art CT‐WOLEDs reported so far, but also comparable to the best values from all‐fluorescent white devices with a single‐emissive‐layer. Moreover, by using PICZ2F as an emitter, an external quantum efficiency (EQE) of 7.10% with the Commission Internationale de lEclairage (CIE) coordinates of (0.155, 0.068) is achieved in the doped device, and a low‐efficiency roll‐off even at a high luminance of 15 000 cd m−2 (EQE15000: 5.80%) is achieved in the non‐doped device. Overall, the findings provide a promising strategy to develop simple but efficient CT‐WOLEDs.

Construction of Weakly Hybridized Excited State Using Donor‐π‐Acceptor Structure and Applications: From Highly Efficient Pure‐Blue Electro‐Fluorescence to Visible‐Light Polymerization

AbstractHerein this work, a novel donor‐π‐acceptor (D‐π‐A) pure‐blue hybrid local and charge‐transfer (HLCT) fluorescent material TDFBO and its functionalization as organic light emitting diode (OLED) emitter and photoinitiator (PI) in photopolymerization is reported. The weak‐hybridization property involved by the fluorene π‐bridge can simultaneously give satisfied photo‐luminescent quantum yield (PLQY) and make efficient “hot‐exciton” channel achievable. Moreover, the D‐π‐A structure can also promote an exceeding electron mobility as high as 3.57×10−4 cm2 V−1 s−1. Finally, it is noted that the TDFBO‐doped OLED can be regarded as the best one among the pure‐blue emissive OLEDs, which exhibits a high maximum external quantum efficiency of 11.1%, while the rolling‐off only stands on a low level, as 6% at 100 cd m−2. Additionally, a relatively high final conversion of C = C double bond in a representative acrylate monomer is also attained by photoinitiation of TDFBO under 405 nm LED, where the photopolymerization has been applied to 3D printing.