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Improving efficiency in RGB phosphorescent and white organic light emitting diodes via donor-spiro-boron acceptor host materials 通过供体-螺硼受体主材料提高 RGB 磷光和白色有机发光二极管的效率
IF 2.7 4区 工程技术 Q3 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-28 DOI: 10.1016/j.orgel.2024.107086
Aziz Khan , Xing Chen , Man-Keung Fung , Zhiming Wang

The universal host material with boron acceptor core structure is exceptionally sparse to be designed for red, green, and blue in efficient phosphorescent organic light emitting diodes (PhOLEDs) accompanying white OLEDs, possessing indistinguishable device feature. Herein, two boron acceptors spiro-host materials namely 1'-(4-(dimesitylboranyl)phenyl)-10-phenyl-10H-spiro[acridine-9,9′-fluorene] (TPA-PBM) and 1-(4-(dimesitylboranyl)phenyl)-3′,6′-dimethylspiro[fluorene-9,8′-indolo[3,2,1-de]acridine] (2MeCz-PBM) were designed and synthesized. The designed rigid donor strategy exhibited good device performance among the reported boron donor-spiro-acceptor (D-spiro-A) skeleton for organic light emitting diodes (OLEDs). In particular, we fabricate RGB three-color phosphorescent OLEDs based on TPA-PBM and 2MeCz-PBM. The red devices exhibit a maximum external quantum efficiency (EQE) of nearly 28 % (26.8 % for TPA-PBM and 27.5 % for 2MeCz-PBM), with an electroluminescence spectrum at 608 nm. The green/blue devices obtain maximum EQEs of 21.2 %/15.3 % and 21.8 % 17.3 %, for TPA-PBM and 2MeCz-PBM, respectively. Furthermore, green devices display an extremely low efficiency roll-off with decreasing 1 % and 3 % at luminance of 5000 cd m−2. Additionally, the two-color white OLED using 2MeCz-PBM exhibits EQEmax and PEmax are 24.5 % and 62.9 lm W−1 respectively, the EQE remain 23.8 % at commercial lighting brightness of 1000 cd m−2. The WOLED also shows a stable white spectrum with CIE varying range of (0.41, 0.47) to (0.39, 0.46) at 100 cd m−2 to 15000 cd m−2. All obtained results confirmed that our targeted molecules have advantage of carrier balance and efficient charge recombination, which might replace many other commercial host materials.

在高效磷光有机发光二极管(PhOLED)和白光有机发光二极管(OLED)中,具有硼受体核心结构的通用宿主材料异常稀少,无法设计出适用于红、绿、蓝三种颜色的宿主材料,也无法实现无差别的器件特性。在此,两种硼受体螺基材料,即 1'-(4-(二甲基二硼烷基)苯基)-10-苯基-10H-螺[吖啶-9、9′-芴](TPA-PBM)和 1-(4-(二甲基二硼烷基)苯基)-3′,6′-二甲基螺[芴-9,8′-吲哚并[3,2,1-de]吖啶](2MeCz-PBM)。在已报道的用于有机发光二极管(OLED)的硼供体-螺受体(D-spiro-A)骨架中,所设计的刚性供体策略表现出良好的器件性能。特别是,我们基于 TPA-PBM 和 2MeCz-PBM 制备了 RGB 三色磷光 OLED。红色器件的最大外部量子效率(EQE)接近 28%(TPA-PBM 为 26.8%,2MeCz-PBM 为 27.5%),电致发光光谱为 608 纳米。对于 TPA-PBM 和 2MeCz-PBM 而言,绿色/蓝色器件的最大 EQE 分别为 21.2 %/15.3 % 和 21.8 % 17.3 %。此外,在亮度为 5000 cd m-2 时,绿色器件显示出极低的效率衰减,分别为 1 % 和 3 %。此外,使用 2MeCz-PBM 的双色白色有机发光二极管的 EQEmax 和 PEmax 分别为 24.5 % 和 62.9 lm W-1,在商业照明亮度为 1000 cd m-2 时,EQE 仍为 23.8 %。WOLED 也显示出稳定的白光谱,在 100 cd m-2 到 15000 cd m-2 的 CIE 变化范围为 (0.41, 0.47) 到 (0.39, 0.46)。所有结果都证实,我们的目标分子具有载流子平衡和高效电荷重组的优势,可以取代许多其他商业宿主材料。
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引用次数: 0
Manipulating the photophysical properties of multi-donor molecules for fast reverse intersystem crossing in solution-processed OLED devices 操纵多供体分子的光物理性质,在溶液加工的有机发光二极管器件中实现快速反向系统间交叉
IF 2.7 4区 工程技术 Q3 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-25 DOI: 10.1016/j.orgel.2024.107085
Hengwei Tian , Xuming Zhuang , Zhi-Ping Yan , Hai Bi , Zhiqiang Li , Yue Wang , Yanping Huo

The slow reverse intersystem crossing (RISC) rate in thermally activated delayed fluorescence (TADF) emitters result in extended exciton lifetime and pronounced efficiency loss at high luminance level. To address this limitation, we have developed and characterized a series of novel compounds featuring triazine cores substituted with tert-butyl carbazole moieties at various positions and quantities. The objective here is to fine-tune the charge transfer properties, thereby enhancing the efficiency of the RISC process. Our studies reveal that through-space charge transfer is more effective than long-range through-bond charge transfer in minimizing the singlet-triplet energy gap and accelerating RISC. The optimized compound, 4tCzTrz, exhibits an exceptionally fast RISC rate of 1.02 × 107 s−1 and a high photoluminescence quantum yield of up to 100 %. Solution-processed organic light-emitting diodes (OLEDs) incorporating this molecule have achieved outstanding maximum external quantum efficiencies of around 20 %, whether used as an emitter directly or as a sensitizer to boost overall emission efficiency.

热激活延迟荧光(TADF)发射器的反向系统间交叉(RISC)速率较慢,导致激子寿命延长,在高亮度下效率明显下降。为了解决这一局限性,我们开发并鉴定了一系列新型化合物,其特点是三嗪核心在不同位置和数量上被叔丁基咔唑取代。我们的目标是对电荷转移特性进行微调,从而提高 RISC 过程的效率。我们的研究表明,在最小化单重-三重能隙和加速 RISC 过程方面,空间电荷转移比长程通键电荷转移更有效。优化后的化合物 4tCzTrz 的 RISC 速率高达 1.02 × 107 s-1,光量子产率高达 100%。含有这种分子的溶液加工有机发光二极管(OLED),无论是直接用作发射器,还是用作敏化剂以提高整体发射效率,都取得了出色的最大外部量子效率,约为 20%。
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引用次数: 0
Spirobifluorene-appended multi-resonance thermally activated delayed fluorescence emitter for efficient narrowband blue OLEDs with suppressed ACQ effect 用于抑制 ACQ 效应的高效窄带蓝色 OLED 的螺二芴添加型多共振热激活延迟荧光发射器
IF 3.2 4区 工程技术 Q1 Physics and Astronomy Pub Date : 2024-06-11 DOI: 10.1016/j.orgel.2024.107084
Jia-Chen Li , Zhang-Li Cheng , Jie Li , Hui Wang , Feng Huang , Ying-Chun Cheng , Hao Wu , Xin Xiong , Jia Yu , Hua-Yue Wu , Jie-Yu Zhou , Kai Wang , Xiao-Hong Zhang , Jun Ye

Multi-resonance (MR) thermally activated delayed fluorescence (TADF) materials with planar rigidity show great potential as emitters in organic light-emitting diodes (OLEDs) due to their high photoluminescence quantum yields and narrowband emission. However, their strong intermolecular interaction trends usually result in redshifted and broadened emission spectra as well as low device efficiencies due to the aggregation-caused quenching (ACQ) effect. In this paper, a bulky spirobifluorene unit was appended onto an asymmetric carbazole/diphenylamine-embedded MR skeleton to relieve such trends, thus affording a new MR-TADF blue emitter, BNSF-1. Introducing spirobifluorene significantly relieves the intermolecular interaction trends of MR backbones without affecting their original photophysical properties. The corresponding sensitizer-free OLED devices based on BNSF-1 exhibit narrowband sky-blue electroluminescence peaking at 475 nm with a full width at half-maximum of 25 nm, as well as a maximum external quantum efficiency of 25.9 %. More importantly, BNSF-1 exhibited negligible spectral broadening and ACQ trends as the doping ratio increased. Our work provides a feasible method for constructing doping concentration-insensitive MR-TADF emitters.

具有平面刚性的多共振(MR)热激活延迟荧光(TADF)材料由于具有高光致发光量子产率和窄带发射特性,在有机发光二极管(OLED)中作为发光体显示出巨大的潜力。然而,由于聚集淬灭(ACQ)效应,它们强烈的分子间相互作用趋势通常会导致发射光谱的红移和拓宽,以及较低的器件效率。本文在不对称咔唑/二苯胺嵌入式 MR 骨架上附加了一个大螺二芴单元,以缓解这种趋势,从而获得了一种新型 MR-TADF 蓝色发射体 BNSF-1。螺二芴的引入大大缓解了 MR 骨架的分子间相互作用趋势,而不会影响其原有的光物理特性。基于 BNSF-1 的相应无敏化剂 OLED 器件在 475 nm 处显示出峰值为 25 nm 的窄带天蓝色电致发光,最大外部量子效率为 25.9%。更重要的是,随着掺杂率的增加,BNSF-1 的光谱展宽和 ACQ 趋势均可忽略不计。我们的工作为构建对掺杂浓度不敏感的 MR-TADF 发射器提供了一种可行的方法。
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引用次数: 0
Photophysics and thermally activated delayed fluorescence (TADF) of fullerene C70 and C70 methano and pseudodihydro monoadducts: A comparative study 富勒烯 C70 和 C70 甲烷和假二氢单加合物的光物理和热激活延迟荧光 (TADF):比较研究
IF 3.2 4区 工程技术 Q1 Physics and Astronomy Pub Date : 2024-06-06 DOI: 10.1016/j.orgel.2024.107083
Tiago Palmeira , Célia Santos , Mario N. Berberan-Santos

A comparative study of the photophysical properties of pristine C70 and two C70 derivatives, including their thermally activated delayed fluorescence (TADF) is reported. It is observed that the addition of a substituent group to the C70 cage-like structure changes both the radiative and the nonradiative rate constants, the change being more pronounced for the nonradiative processes (S1→S0 internal conversion and S1→T1 and T1→S0 intersystem crossings). A new method of TADF analysis (global analysis of time-resolved and steady-state data) is presented and applied. Both derivatives are found to display a less efficient TADF when compared with C70.

报告对原始 C70 和两种 C70 衍生物的光物理特性进行了比较研究,包括它们的热激活延迟荧光(TADF)。研究发现,在 C70 笼状结构中添加取代基团会改变辐射和非辐射速率常数,而非辐射过程(S1→S0 内部转换和 S1→T1 及 T1→S0 系统间交叉)的变化更为明显。提出并应用了一种新的 TADF 分析方法(时间分辨和稳态数据的全局分析)。结果发现,与 C70 相比,这两种衍生物的 TADF 效率较低。
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引用次数: 0
Enhanced synaptic behavior of neuromorphic device based on organic electrochemical transistors by adding Aminosilane 通过添加氨基硅烷增强基于有机电化学晶体管的神经形态器件的突触行为
IF 3.2 4区 工程技术 Q1 Physics and Astronomy Pub Date : 2024-05-27 DOI: 10.1016/j.orgel.2024.107076
Dae-Hee Kim , Jiyoul Lee , Yonghee Kim , Hocheon Yoo , Eun Kwang Lee

Herein, we propose a strategy to enhance the synaptic behavior of neuromorphic devices based on organic electrochemical transistors (OECT) by introducing (3-aminopropyl)triethoxysilane (APT) into the conjugated polymer film channel. Various film analyses utilizing optical and atomic force microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy revealed that the addition of APT to the poly (3-hexylthiophene) (P3HT) film facilitated the formation of highly crystalline P3HT aggregation, thereby suppressing film degradation induced by repetitive ion injection and ejection under gate bias. Furthermore, electrical characterization of the OECT devices incorporating P3HT channels demonstrated an expanded hysteresis region and improved memory characteristics upon APT addition, which contains functional groups with high electron density, favorably influencing synaptic plasticity features such as short-term plasticity (STP), long-term plasticity (LTP), short-term memory (STM), and long-term memory (LTM). Consequently, it led to the fortification and resilience of synaptic behavior in OECTs, positioning them as a promising candidate for neuromorphic devices.

在此,我们提出了一种策略,通过在共轭聚合物薄膜通道中引入(3-氨基丙基)三乙氧基硅烷(APT)来增强基于有机电化学晶体管(OECT)的神经形态器件的突触行为。利用光学和原子力显微镜、X 射线衍射和 X 射线光电子能谱进行的各种薄膜分析表明,在聚(3-己基噻吩)(P3HT)薄膜中添加 APT 有助于形成高度结晶的 P3HT 聚集,从而抑制了在栅极偏压下重复离子注入和射出引起的薄膜降解。此外,对含有 P3HT 通道的 OECT 器件进行的电学表征表明,添加 APT 后,磁滞区域扩大,记忆特性得到改善。APT 含有高电子密度的官能团,对突触可塑性特征(如短期可塑性(STP)、长期可塑性(LTP)、短期记忆(STM)和长期记忆(LTM))产生有利影响。因此,OECTs 的突触行为得到了强化和恢复,使其成为神经形态设备的理想候选材料。
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引用次数: 0
Improving efficiency and flexibility of non-halogenated solvent-processed dual-layer organic solar cells through solvent vapor annealing 通过溶剂气相退火提高无卤溶剂加工双层有机太阳能电池的效率和灵活性
IF 3.2 4区 工程技术 Q1 Physics and Astronomy Pub Date : 2024-05-27 DOI: 10.1016/j.orgel.2024.107075
Lin Zhang , Jun Zhang , Yumeng Ma , Xueliang Guo , Hui Huang , Zhaozhao Bi , Yilin Wang , Yong Zhang , Chen Xie , Wenchen Luo , Xiaotian Hu , Wei Ma , Yongbo Yuan

Dual-layer organic solar cells (OSCs), fabricated through sequential-casting with separately dissolved donor and acceptor materials, offer simplified solution preparation and morphology control. However, the poor solubility of organic materials in non-halogenated solvents often results in undesirable vertical component distribution and insufficient donor/acceptor interfaces in non-halogenated solvent-processed dual-layer OSCs, adversely affecting photovoltaic performance and flexibility. In this study, we applied a solvent vapor annealing (SVA) method using CS2 solvent in o-xylene solvent-processed dual-layer OSCs. The SVA method effectively adjusted the vertical component distribution of the active layer and increased the donor/acceptor interfaces, leading to an improved power conversion efficiency (PCE) of 17.24 %. Additionally, SVA films exhibited superior tensile properties, with a crack onset strain of 5.07 %, surpassing that of the as-cast films (4.32 %), attributed to the stronger interaction between the donor and acceptor layers with more donor/acceptor interfaces. Consequently, large-area (1 cm2) flexible devices achieved a significant efficiency of 14.20 % and maintained excellent mechanical flexibility, with 80 % of the initial efficiency retained after 1000 bending cycles. This work presents an effective approach for fabricating high-performance non-halogenated solvent-processed flexible dual-layer OSCs.

双层有机太阳能电池(OSC)是通过分别溶解供体和受体材料的顺序浇铸法制造的,可简化溶液制备和形态控制。然而,有机材料在非卤化溶剂中的溶解性较差,往往导致非卤化溶剂处理的双层有机太阳能电池中不理想的垂直成分分布和供体/受体界面不足,从而对光伏性能和灵活性产生不利影响。在这项研究中,我们在邻二甲苯溶剂处理的双层 OSC 中采用了 CS2 溶剂蒸汽退火(SVA)方法。SVA 方法有效地调整了活性层的垂直成分分布,增加了供体/受体界面,使功率转换效率 (PCE) 提高到 17.24%。此外,SVA 薄膜还具有优异的拉伸性能,其裂纹起始应变为 5.07%,超过了原铸薄膜(4.32%),这归功于供体层和受体层之间更强的相互作用以及更多的供体/受体界面。因此,大面积(1 平方厘米)柔性器件的效率显著提高到 14.20%,并保持了极佳的机械柔韧性,1000 次弯曲循环后仍能保持 80% 的初始效率。这项研究提出了一种制造高性能非卤化溶剂加工柔性双层 OSC 的有效方法。
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引用次数: 0
Acceptor-σ-donor-σ-acceptor host material for red phosphorescent and thermally activated delayed fluorescent OLEDs 用于红色磷光和热激活延迟荧光 OLED 的受体-σ-供体-σ-受体主材料
IF 3.2 4区 工程技术 Q1 Physics and Astronomy Pub Date : 2024-05-23 DOI: 10.1016/j.orgel.2024.107072
Meng-Tian Li , Zhi-Hao Qu , Ruihong Liu , Yue-Jian Yang , Peng Zuo , Liang-Sheng Liao , Zuo-Quan Jiang

A novel bipolar host molecule di-spiro [fluorene-9,5′-quinolino [3,2,1-de] acridine-9′,9″-fluorene]-2,2″,7,7″-tetracarbonitrile (QACN) featuring an Acceptor-σ-Donor-σ-Acceptor structure was developed. Systematic investigations into its photophysical, electrochemical, and thermal properties unveiled exceptional thermal stability, a three-dimensional spatial configuration, and bipolar carrier transport capability. Employing QACN as the host material in red phosphorescent and thermally activated delayed fluorescent (TADF) organic light-emitting diodes (OLEDs) yielded a maximum external quantum efficiency of 25.3 % and 16.5 %, respectively. Compared with the commercial material TPBi (EQE = 12.0 %, λEL = 668 nm) and mCP (EQE = 14.5 %, λEL = 652 nm), the TADF OLEDs based on QACN achieved a higher EQE and a large red-shift emission (EQE = 16.5 %, λEL = 694 nm). These findings underscore the potential of QACN as an effective host material for red phosphorescent and TADF emitters and provide a new auxiliary finesse for realizing deep red and near-infrared (NIR) OLEDs.

一种新型双极宿主分子二螺[芴-9,5′-喹啉并[3,2,1-de]吖啶-9′,9″-芴]-2,2″,7,7″-四碳腈(QACN)被开发出来,它具有受体-σ-供体-σ-受体结构。对其光物理性质、电化学性质和热性质的系统研究揭示了其卓越的热稳定性、三维空间构型和双极载流子传输能力。在红色磷光和热激活延迟荧光(TADF)有机发光二极管(OLED)中使用 QACN 作为宿主材料,其最大外部量子效率分别达到 25.3% 和 16.5%。与商用材料 TPBi(EQE = 12.0 %,λEL = 668 nm)和 mCP(EQE = 14.5 %,λEL = 652 nm)相比,基于 QACN 的 TADF 有机发光二极管实现了更高的 EQE 和更大的红移发射(EQE = 16.5 %,λEL = 694 nm)。这些发现强调了 QACN 作为红色磷光体和 TADF 发射器的有效宿主材料的潜力,并为实现深红色和近红外 (NIR) 有机发光二极管提供了一种新的辅助材料。
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引用次数: 0
Efficient electron injection layer for thermal stability of top emission phosphorescent organic light emitting diodes 高效电子注入层提高顶部发射型磷光有机发光二极管的热稳定性
IF 3.2 4区 工程技术 Q1 Physics and Astronomy Pub Date : 2024-05-17 DOI: 10.1016/j.orgel.2024.107061
Thi Na Le , Ramachandran Elumalai , Seung Ju Ok , Yeonhwa Lee , Seung Yong Song , Min Chul Suh

Thermal stability holds significant importance in both high-resolution and large-area organic light-emitting diodes (OLEDs) due to its potential impacts on pixel shrinkage, thereby adversely affecting visual quality and long-term device functionality. The thermal instability could be from the thermal diffusion of metal ions or small molecules occurring at the interface between the electron injection layer (EIL) and the cathode material, influenced by differing surface properties and binding strength. In this study, we meticulously engineered magnesium fluoride (MgF2) as EIL to mitigate the aforementioned challenges. Important physical properties associated with the EIL/cathode interaction were systematically analyzed. Employing Ag:Yb (2.5:1) as the cathode, we achieved notable enhancements in current efficiency and a reduced turn-on voltage for a green device operating under optical microcavity conditions. Thermal degradation test conducted over 240 h on fabricated devices revealed that employing MgF2 as the EIL markedly enhanced thermal stability compared to devices utilizing Yb as the EIL reference. The robust EIL/cathode system observed herein is attributed to the high binding energy between the EIL and cathode materials utilized in this study.

热稳定性对高分辨率和大面积有机发光二极管(OLED)具有重要意义,因为它可能会影响像素收缩,从而对视觉质量和设备的长期功能产生不利影响。热不稳定性可能是由于金属离子或小分子在电子注入层(EIL)和阴极材料之间的界面上发生热扩散,并受到不同表面特性和结合强度的影响。在本研究中,我们精心设计了氟化镁(MgF2)作为电子注入层,以减轻上述挑战。我们对与 EIL/阴极相互作用相关的重要物理特性进行了系统分析。采用银:镱(2.5:1)作为阴极,我们显著提高了电流效率,并降低了在光学微腔条件下运行的绿色器件的开启电压。对制造的器件进行的 240 小时热降解测试表明,与使用镱作为 EIL 参考的器件相比,使用 MgF2 作为 EIL 明显提高了热稳定性。本研究中观察到的 EIL/阴极系统的稳健性归功于 EIL 与阴极材料之间的高结合能。
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引用次数: 0
Tracking deep-level defects in degrading perovskite solar cells with a multifactorial approach 采用多因素方法跟踪退化的 Perovskite 太阳能电池中的深层缺陷
IF 3.2 4区 工程技术 Q1 Physics and Astronomy Pub Date : 2024-05-16 DOI: 10.1016/j.orgel.2024.107074
Carlos Biaou , Matthew Mcphail , Kazutaka Eriguchi , Vivek Subramanian , Oscar Dubon

In this work, we provide a mechanistic understanding of the degradation of perovskite solar cells in operation by focusing on methylammonium lead triiodide (CH3NH3PbI3 or MAPbI3) and tracking the evolution of electronic defects via photo-induced current transient spectroscopy (PICTS). Moreover, we also record the degradation of its photovaltaic characteristics over time under various electric load and temperature conditions. Using PICTS, we found that bands of trap states, initially highly localized deep within the band gap of the perovskite, widened over the exposure period. This effect was exacerbated with increasing temperature. Further, using the design of experiment methodology for this multifactorial study, we found that two interaction factors (temperature× load & temperature× time) were significant in the degradation of the perovskite cells, validating the importance of our holistic approach. Through these observations, we establish a mechanistic link between deep-level traps and photovoltaic characteristics.

在这项研究中,我们以三碘化甲铵铅(CH3NH3PbI3 或 MAPbI3)为研究对象,通过光诱导电流瞬态光谱(PICTS)跟踪电子缺陷的演变,从机理上了解了过氧化物太阳能电池在运行过程中的降解情况。此外,我们还记录了在各种电负载和温度条件下,其光变色特性随时间的衰减情况。通过 PICTS,我们发现陷阱态带最初高度集中在过氧化物带隙的深处,但随着暴露时间的延长,陷阱态带逐渐扩大。这种效应随着温度的升高而加剧。此外,在这项多因素研究中,我们采用了实验设计方法,发现两个交互因素(温度×负载&;温度×时间)对包晶电池的降解有显著影响,从而验证了我们的整体方法的重要性。通过这些观察,我们建立了深层陷阱与光伏特性之间的机理联系。
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引用次数: 0
Theoretical insights into long-range coupling of electron-hole pairs in TCTA–PO-T2T exciplex 关于 TCTA-PO-T2T 复合物中电子-空穴对长程耦合的理论见解
IF 3.2 4区 工程技术 Q1 Physics and Astronomy Pub Date : 2024-05-11 DOI: 10.1016/j.orgel.2024.107073
Yichao Jin, Zhaoyue Lü, Xiao Wang, Zongkai Tang, Haichuan Mu

This work reports theoretical investigations concerning long-range coupling of electron-hole pairs in spatially separated exciplex (SSE) systems via Density Functional Theory and Time-Dependent Density Functional Theory. Based on TCTA−PO-T2T parent exciplex, where 4,4′,4″-Tris(carbazol-9-yl)triphenylamine (TCTA) serves as donor (D) and 2,4,6-Tris[3-(diphenylphosphinyl)phenyl]-1,3,5-triazine (PO-T2T) as acceptor (A), SSEs are constructed by intentionally tuning the D−A distance. The calculation results demonstrate that all SSEs, even if the D−A distance is over 14 Å, exhibit the clear and strong charge transfer character in terms of DCT, qCT, and t indexes. As the D−A distance increases, the energy gap of SSEs is increased, resulting in the blueshift of emission spectra. Calculation and experiment results show a good consistency, indicating that our model could well describe SSEs. Meanwhile, the reduced energy gap between CT and 3LE and more degenerate states could boost reverse intersystem crossing via vibronic coupling and hyperfine coupling, eventually improving the electroluminescent performance of SSEs. Our study suggests that manipulation of relative energy alignment via controlling D−A distance not only promotes the properties of exciplexes, but also offers guidance for designing thermally activated delayed fluorescence emitters through-space charge transfer.

本研究报告通过密度泛函理论和时变密度泛函理论,对空间分离赋形剂(SSE)体系中电子-空穴对的长程耦合进行了理论研究。以 4,4′,4″-三(咔唑-9-基)三苯胺(TCTA)为供体(D)、2,4,6-三[3-(二苯基膦酰基)苯基]-1,3,5-三嗪(PO-T2T)为受体(A)的 TCTA-PO-T2T 母复合物为基础,通过有意调节 D-A 间距构建了 SSE。计算结果表明,即使 D-A 间距超过 14 Å,所有 SSE 在 DCT、qCT 和 t 指数方面都表现出明显而强烈的电荷转移特性。随着 D-A 间距的增大,SSE 的能隙也随之增大,从而导致发射光谱的蓝移。计算和实验结果显示出良好的一致性,表明我们的模型可以很好地描述 SSE。同时,CT 和 3LE 之间能隙的减小以及更多的退化态可以通过振子耦合和超频耦合促进反向系统间交叉,最终改善 SSE 的电致发光性能。我们的研究表明,通过控制 D-A 间距来操纵相对能量排列不仅能促进赋形剂的特性,还能为通过空间电荷转移设计热激活延迟荧光发射器提供指导。
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引用次数: 0
期刊
Organic Electronics
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