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过渡金属配合物TADF发光材料研究进展
特邀报告 | 更新时间：2023-02-16
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过渡金属配合物TADF发光材料研究进展 增强出版
- Advances in Thermally Activated Delayed Fluorescence of Transition Metal Complexes
- 发光学报 2023年 44卷 第1期 (2023)
- 作者机构：深圳大学 材料科学与工程学院， 深圳市新型信息显示与存储材料重点实验室,广东,深圳,518055
- 作者简介：
- 基金信息：国家自然科学基金(21801170);广东省基础与应用基础研究委员会面上项目(2021A1515010175)
- DOI：10.37188/CJL.20220308 中图分类号： O482.31
纸质出版日期：2023-01-05，
收稿日期：2022-08-26，
修回日期：2022-09-19，
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引用本文
张靖羚,李凯,杨楚罗.过渡金属配合物TADF发光材料研究进展[J].发光学报,2023,44(01):12-25.
ZHANG Jingling,LI Kai,YANG Chuluo.Advances in Thermally Activated Delayed Fluorescence of Transition Metal Complexes[J].Chinese Journal of Luminescence,2023,44(01):12-25.
张靖羚,李凯,杨楚罗.过渡金属配合物TADF发光材料研究进展[J].发光学报,2023,44(01):12-25. DOI： 10.37188/CJL.20220308.
ZHANG Jingling,LI Kai,YANG Chuluo.Advances in Thermally Activated Delayed Fluorescence of Transition Metal Complexes[J].Chinese Journal of Luminescence,2023,44(01):12-25. DOI： 10.37188/CJL.20220308.
过渡金属配合物TADF发光材料研究进展 增强出版
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"data": "高效率利用三重态激子发光是制备高性能有机发光二极管（OLED）的关键。除磷光过渡金属配合物外，具有热活化延迟荧光（TADF）特性的过渡金属配合物能够将三重态激子上转换为单重态激子，进而通过单重态激子辐射发光，为开发金属配合物发光材料提供了新的途径。然而，过去十年来OLED发光材料的研究主要聚焦在纯有机TADF体系上，过渡金属配合物TADF材料的研究投入相对偏少。但是，已有研究表明金属配合物能够利用金属的重原子效应促进反向系间窜越（RISC）过程，提升TADF发光效率并缩短TADF寿命，有利于制备高效率、低滚降的OLED。本文根据金属中心不同的d电子构型分类筛选了TADF金属配合物研究领域中代表性的材料体系，对其激发态属性、光物理和器件性能进行了概括和讨论。通过对不同类型的TADF金属配合物发光性能的归纳和比较，揭示了金属中心和配体结构对配合物发光性质的影响规律，对进一步开发高性能的金属配合物TADF材料，尤其是基于廉价金属元素的TADF配合物具有重要的指导意义。"
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"data": "Efficient harvesting of triplet excitons is crucial to the development of high-performance organic light-emitting diodes（OLEDs）. Other than phosphorescence， the thermally activated delayed fluorescence（TADF） mechanism enables the upconversion of triplet excitons to singlet ones "
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"data": " reverse intersystem crossing（RISC）， followed by fluorescent radiation from the spin-allowed singlet excited states， providing another pathway to transition metal complexes for utilizing triplet excitons. However， the past decade has witnessed a blooming research interest in the purely organic TADF materials while the TADF metal complexes has only received much less attentions. Whereas， it has been shown that the presence of metal atom can boost the RISC rate through its heavy atom effect， leading to improved TADF emissions with high efficiencies and short lifetimes. Therefore， TADF metal complexes hold advantageous for the fabrication of high-performance OLEDs in terms of high-efficiency and small efficiency roll-off. This article summarizes the advances in TADF metal complexes by focusing on the excited state nature related to different electronic configurations， the photophysical and electroluminescence performance of representative TADF metal complexes. The structure-property relationship has been discussed which is conceived to provide useful guidelines for further design of TADF metal complexes， particularly those based on inexpensive metal elements."
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"data": [
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"name": "text",
"data": "自二十世纪八十年代末邓青云博士在以8-羟基喹啉铝（Alq"
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"data": "）薄膜为发光层的三明治构型器件中观测到有机电致发光以来"
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"data": "]"
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]
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"name": "text",
"data": "，有机发光二极管（Organic light-emitting diode, OLED）的研究受到了广泛的关注。与液晶显示（Liquid crystal display，LCD）技术相比，OLED显示具有诸多优势，例如结构简单、色纯度高、能耗低以及响应速度快等。而可弯折等柔性特点则能够拓宽OLED在汽车智能座舱、医疗影像、照明等领域的应用，并且有望使OLED显示在增强现实（AR）和虚拟现实（VR）应用方面大放异彩。因此，开发高效、色纯度更好、成本更低的OLED材料成为近三十多年来材料科学领域的研究焦点之一。"
}
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"data": [
{
"name": "text",
"data": "在电场的作用下，电子与空穴复合产生25%的单重态激子和75%的三重态激子。传统的有机荧光OLED仅能利用单重态激子发光，最高实现25%的内量子效率（IQE）和5%左右的外量子效率（EQE）"
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"data": "2"
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{
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"data": "。1998年，Baldo等利用铂（Pt）的重原子效应诱导产生强自旋轨道耦合（SOC）效应，促进单重态激子通过系间窜越（ISC）生成三重态激子，首次实现了磷光电致发光，器件的内量子效率（IQE）达到了100%"
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"data": {
"text": "3",
"type": "bibr",
"rid": "R3",
"data": [
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"data": "3"
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]
},
{
"name": "text",
"data": "。与此同时，Ma等采用锇（Ⅱ）配合物Os（CN）"
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"data": "也获得了三重态发光的OLED"
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"data": [
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"type": "bibr",
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{
"name": "text",
"data": "，自此开启了基于过渡金属配合物的第二代磷光OLED的研究。需要指出的是，第三过渡系金属（如铱、铂）由于显著的SOC常数，在磷光OLED材料研究领域获得了巨大的关注。尤其是，目前已商业化的红光和绿光OLED材料均采用铱（Ir）配合物。然而，贵金属材料的稀缺性一直以来被认为是限制磷光OLED广泛应用的一个瓶颈。因此，开发新型发光材料具有重要的意义。由日本科学家Adachi教授引领的纯有机热活化延迟荧光（Thermally activated delayed fluorescence，TADF）材料的研究在过去10年里受到了该领域科学家的极大关注"
},
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"data": [
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"data": "["
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"type": "bibr",
"rid": "R5",
"data": [
{
"name": "text",
"data": "5"
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}
},
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"data": "]"
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]
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{
"name": "text",
"data": "。其机理是，三重态激子通过反向系间窜越（RISC）过程上转换为单重态激子，随后经单重态发射延迟荧光，从而可以实现理论上100%的IQE。目前，基于纯有机TADF发光分子的OLED外量子效率已经和高效率磷光铱（Ⅲ）和铂（Ⅱ）配合物分子相当。然而，由于不存在重原子且RISC是自旋禁阻的过程，纯有机TADF分子的RISC速率通常较慢，其延迟荧光寿命相对较长，导致严重的效率滚降，且不利于器件的运行稳定性"
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"data": "。"
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"data": [
{
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"data": "关于配合物TADF现象的报道可以追溯到40年前"
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"data": [
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"data": "["
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"data": [
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"type": "bibr",
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"text": "7-8",
"type": "bibr"
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},
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},
{
"name": "text",
"data": "。McMillin研究组发现当温度从室温降至4 K时，铜（Ⅰ）配合物的发光颜色从绿色红移至黄色，发光寿命从30 μs延长至250 μs，具有典型的E型延迟荧光特征（即TADF）。2010年，Deaton等"
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},
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]
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"data": "报道了具有高效率TADF特性的双核铜（Ⅰ）配合物，并基于该配合物制造了绿光OLED器件，EQE高达16.1%，领先于当时已报道的铜配合物OLEDs。与此同时，Yersin等开始了铸币金属配合物TADF的深入研究"
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]
},
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"name": "text",
"data": "。特别需要指出的是，与纯有机TADF材料相比，通过合适的分子设计能够利用金属的重原子效应促进快速的RISC过程，从而缩短配合物分子的延迟荧光寿命"
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"data": "。"
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"data": [
{
"name": "text",
"data": "近年来，对金属配合物TADF发光材料的研究主要集中于d"
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"data": "铸币金属以及少量d"
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"data": "金属配合物"
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"data": {
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"type": "bibr",
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"data": [
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"type": "bibr"
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"name": "text",
"data": "。与磷光铱、铂配合物相比，金属配合物TADF材料所采用的金属元素在地壳中丰度更高，具有成本优势。通过合理的配体选择与分子结构设计调控配合物的激发态性质，得到高效率、短激发态寿命、色纯度高、光色可调的金属配合物TADF材料，对拓展其在OLED及其他智能光电功能材料等领域的应用具有重要意义。"
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"data": "本文选择近年来报道的代表性的d"
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"data": "电子构型的TADF过渡金属配合物"
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"data": {
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"type": "bibr",
"rid": "R20",
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"data": "20"
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}
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"R22",
"R23",
"R24",
"R25",
"R26",
"R27",
"R28",
"R29",
"R30",
"R31",
"R32",
"R33",
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},
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"data": "，对其激发态属性与光物理性质进行总结与讨论（具体数据见"
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"data": {
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"data": "），尝试揭示不同配合物的金属中心和配体结构与光物理性质之间的关系，希望为设计具有高效TADF性质的过渡金属配合物提供有指导意义的研究思路。"
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"data": "文献中相关配合物的光物理数据以及OLED数据"
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"data": "根据金属中心和配体的电子结构不同，过渡金属配合物具有丰富多样的激发态属性，所涉及的前线轨道主要有金属的d轨道、配体的π（或者主要为p轨道）和π"
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"data": "。2010年，Deaton等合成了一种通过P^N^P型配体桥联的双核铜（Ⅰ）分子（"
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"data": "）。作者采用该配合物制备的OLED展示出了高达16%的最大EQE，并且效率滚降小，是铜配合物OLED研究领域的一个重要突破。与此同时，Yersin研究组通过分子设计构建LLCT激发态，也开发了一类电中性的TADF铜（Ⅰ）配合物（如"
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}
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{
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}
]
},
{
"name": "text",
"data": "。上述工作的一个重要意义是明确地揭示了激发态的电荷转移特性使铜（Ⅰ）配合物激发态单重态-三重态能级差（Δ"
},
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{
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"data": "）减小，有利于促进RISC过程，实现高效率的TADF发射。这为解决磷光铜配合物长期以来所面临的辐射跃迁速率慢和发射寿命长的难题提供了一个极其可行的思路。领域内研究人员后续开发了一系列高效的TADF铜（Ⅰ）和银（Ⅰ）配合物（如"
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}
},
{
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"data": "。需要指出的是，传统四面体构型的铜（Ⅰ）配合物常伴随激发态的Jahn-Teller结构扭转形变，可能会影响配合物的发光效率。因此，配体中通常需要引入大位阻基团来抑制分子的激发态畸变。"
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},
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"data": "/ 4，4'-环己基二［N，N-二（4-甲基苯基）苯胺］（TAPC）真空蒸镀薄膜的激发与发射光谱"
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"data": "报道了一类基于直线型二配位结构的卡宾-金属-酰胺（CMA）类金（Ⅰ）配合物（"
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"text": "图4",
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},
{
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"data": "），延迟荧光寿命短至0.35 μs。其中，具有强给电子特性的咔唑作为电子给体，具有π-吸电子特性的环（烷基）（氨基）卡宾（CAAC）作为电子受体，使得配合物激发态具有显著的LLCT属性，是获得高效率TADF的关键（"
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{
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},
{
"name": "text",
"data": "）。与此同时，作者提出配合物的给、受体在基态下几乎处于共平面的构型，有利于保持配体-配体间的电荷转移跃迁的振子强度，确保配合物分子S"
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"data": "态具有大的辐射跃迁速率。作者采用该类型配合物获得了最大EQE超过25%的OLED。"
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"data": "配合物分子的HOMO、LUMO分布"
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"data": "［"
},
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"data": {
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}
]
},
{
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"data": "。"
}
]
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"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.4"
}
],
"title": [
{
"name": "text",
"data": "（a）Chemical structure of "
},
{
"name": "bold",
"data": [
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"data": "Au⁃1"
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]
},
{
"name": "text",
"data": ". （b）Calculated HOMO and LUMO for "
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"data": "2019年，Hamze等基于上述设计思路开发了一类高效率的TADF铜（Ⅰ）配合物（如"
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"data": "），其PLQY接近100%，但在蓝光OLED中仅获得了约9%的EQE"
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"text": "23",
"type": "bibr",
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]
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"data": "。同年，该团队报道的卡宾-铜-咔唑绿光配合物（"
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]
},
{
"name": "text",
"data": "，"
},
{
"name": "xref",
"data": {
"text": "图5",
"type": "fig",
"rid": "F5",
"data": [
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]
}
},
{
"name": "text",
"data": "）在薄膜中的PLQY和发光寿命分别为90%和1 μs，在OLED器件中展示出近20%的最大EQE "
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"data": "["
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"type": "bibr",
"rid": "R24",
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},
{
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"data": "]"
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]
},
{
"name": "text",
"data": "。该分子设计策略同样适用于银（Ⅰ）配合物"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
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"name": "xref",
"data": {
"text": "25",
"type": "bibr",
"rid": "R25",
"data": [
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"name": "text",
"data": "25"
}
]
}
},
{
"name": "text",
"data": ","
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"data": {
"text": "45",
"type": "bibr",
"rid": "R45",
"data": [
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"data": "45"
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]
}
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{
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]
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{
"name": "text",
"data": "。尤其是，Hamze等发现银（Ⅰ）配合物（"
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"data": "Ag⁃2"
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},
{
"name": "text",
"data": ", "
},
{
"name": "xref",
"data": {
"text": "图5",
"type": "fig",
"rid": "F5",
"data": [
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"name": "text",
"data": "图5"
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}
},
{
"name": "text",
"data": "）与金（Ⅰ）和铜（Ⅰ）配合物相比具有更短的TADF发射寿命，通过结构分析和理论研究揭示了其快速的RISC源自于HOMO和LUMO更远的空间分离"
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"data": "["
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"data": {
"text": "25",
"type": "bibr",
"rid": "R25",
"data": [
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"data": "25"
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]
},
{
"name": "text",
"data": "。除咔唑外，Romanov "
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"data": [
{
"name": "text",
"data": "["
},
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"name": "xref",
"data": {
"text": "26",
"type": "bibr",
"rid": "R26",
"data": [
{
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"data": "26"
}
]
}
},
{
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"data": "]"
}
]
},
{
"name": "text",
"data": " 和Ying "
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "27",
"type": "bibr",
"rid": "R27",
"data": [
{
"name": "text",
"data": "27"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "等采用其他酰胺类配体也开发了发光性质优异的CMA型配合物（如"
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"data": [
{
"name": "text",
"data": "Au⁃2"
}
]
},
{
"name": "text",
"data": "和"
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"data": [
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"data": "Cu⁃6"
}
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},
{
"name": "text",
"data": "，"
},
{
"name": "xref",
"data": {
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"type": "fig",
"rid": "F5",
"data": [
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"name": "text",
"data": "图5"
}
]
}
},
{
"name": "text",
"data": "）。关于该类型配合物的一系列研究表明保持HOMO和LUMO空间分离的同时，调控激发态前线轨道中金属成分的合理占比对于实现高效率TADF是分子设计的关键。采用具有电子给体和受体特性的配体分别与金属配位构建金属微扰的LLCT激发态，是设计TADF金属配合物的一个有效的思路。特别需要指出的是，过多的金属轨道占比会增强SOC效应，且MLCT激发态因为HOMO和LUMO的空间分离程度小，而不利于TADF发射。"
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"data": "近期，Yang等采用吡嗪稠环的卡宾配体开发了一系列高效率的TADF金（Ⅰ）配合物（如"
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"data": "。尤其需要指出的，通过在咔唑配体上引入位阻基团，作者从实验上明确地证实了该类型配合物具有扭曲的基态构型，且同样能够获得优异的TADF性能。空间位阻的存在能够进一步减小Δ"
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]
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"data": "，促进RISC，以此来平衡S"
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"data": "1"
}
]
},
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"data": [
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"data": "0"
}
]
},
{
"name": "text",
"data": "跃迁振子强度，并同时抑制非辐射跃迁。这一研究结果为解决CMA类型配合物的TADF激发态机理争议提供了充分的实验依据，并在理论计算上得到了有力的支持。Tang等采用同类型的卡宾配体开发了一系列稳定性显著提升的TADF铜（Ⅰ）配合物分子（"
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]
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"data": "，所制备的OLED的最大EQE超过20%，初始亮度1 000 cd·m"
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]
},
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"data": "下的运行寿命（LT"
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"data": "90"
}
]
},
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"data": "）超过1 300 h，是该领域的一个重大突破。通过理论计算，作者指出卡宾配体的缺电子特性能够与金属中心形成反馈π键，有助于增强配位作用，提升配合物的稳定性。同时，卡宾配体的大位阻对于金属中心起到屏蔽作用，也有利于分子稳定性。需要指出的是，文献中虽然关于铜（Ⅰ）配合物OLED的研究已有大量报道，但是有关其器件运行稳定性的数据罕有提及，是开发廉价金属配合物发光材料的一个严峻的挑战。该工作有力地证明了铜（Ⅰ）配合物同样可以获得优异的器件稳定性，为该领域人员继续探索提供了强大的信心。"
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"data": "（a）CMA型配合物结构示意图；（b）扭曲型CMAs结构示意图；（c）"
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"data": "（a）Sketches of reported carbene"
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"data": "除了采用酰胺类配体，Li等采用含胺取代基的芳基配体同样实现了基于LLCT激发态的直线型TADF金（Ⅰ）配合物"
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"data": "运行寿命估算超过77 000 h。直线型二配位金（Ⅰ）配合物，尤其是基于金-金作用的双核或者聚集体系，具有丰富的光物理性质，在无机光物理、发光材料和光化学领域均受到了科学家的广泛关注。然而，单核金（Ⅰ）配合物在光电器件方面的应用却远远滞后于同属于第三过渡系的铱（Ⅲ）和铂（Ⅱ）配合物。其中一个关键原因是二配位构型的金（Ⅰ）配合物由于螯合效应弱，在稳定性方面存在劣势。该研究工作在共价配位键的基础上引入非共价次级配位作用，为开发稳定的金（Ⅰ）配合物发光体系提供了一个崭新的思路，并能够拓展应用于其他金属元素。"
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"data": "除LLCT激发态外，采用具有给-受体性质的配体能够获得ILCT激发态的d"
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"data": "铸币金属配合物，并实现高效的TADF发光。2016年，Liang等在N^N配体上引入吖啶基团作为强电子给体，合成了铜（Ⅰ）配合物"
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"text": "图9",
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]
}
},
{
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]
},
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"data": "。2020年，该研究组基于相同的思路同样获得了高效率的TADF银（Ⅰ）配合物（"
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"data": "Ag⁃3"
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"text": "图9",
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"data": "），然而并未报道其OLED性能"
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"data": "分子结构式。"
}
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"label": [
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}
],
"title": [
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"data": "Chemical structures of "
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"data": "近期，Teng等详细报道了一类具有ILCT激发态的TADF银（Ⅰ）配合物（如"
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"type": "fig",
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},
{
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"data": "）的设计、合成、光物理和器件性能研究"
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"data": "["
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}
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{
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]
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"data": "。根据理论计算，N^N配体虽然具有最低的ILCT单重态激发态，但是其Δ"
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"data": "E"
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]
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]
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"data": "大于0.4 eV，不具有TADF特性。与Ag（Ⅰ）配位后，尽管配合物分子的最低激发态仍然主要是基于亚胺配体的ILCT态，但是变温寿命的测试结果证实"
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"data": "缩小至0.16 eV。通过溶液法制备的该银（Ⅰ）配合物的OLED器件获得了最大EQE约为8.76%的器件，是当时文献报道中为数不多的OLED性能数据。"
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"data": "分子结构式；（b）室温下10% "
},
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"data": [
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"data": "Ag⁃4"
}
]
},
{
"name": "text",
"data": "/二［2-（（氧代）二苯基膦基）苯基］醚（DPEPO）掺杂膜瞬态PL衰减曲线；（c）"
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"data": "Ag⁃4"
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]
},
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"data": "配合物器件外量子效率与亮度关系"
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},
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"text": "34",
"type": "bibr",
"rid": "R34",
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"data": "。"
}
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"label": [
{
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"data": "Fig.10"
}
],
"title": [
{
"name": "text",
"data": "（a）Chemical structure of "
},
{
"name": "bold",
"data": [
{
"name": "text",
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}
]
},
{
"name": "text",
"data": ". （b）Transient PL decay curve of "
},
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{
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"data": "Ag⁃4"
}
]
},
{
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"data": " doped into a bis［2-［（oxo）diphenylphosphino］phenyl］（DPEPO） film（10%） at 298 K. （c）Temperature dependence of the decay time for a powder of "
},
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"data": [
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"data": "Ag⁃4"
}
]
},
{
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"data": ". （d）Plots of external quantum efficiency "
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}
]
},
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"data": " luminance of "
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"data": "综上，通过采用具有合适电子结构的配体开发一价铸币金属配合物的TADF分子具有合成简便以及激发态属性可调性强的优点。尤其是，由于金属中心的满d电子构型，该类配合物不存在非辐射的dd激发态。这一特性所带来的一个有利的结果是只要充分抑制分子激发态的结构畸变，就能够获得高效率的TADF发射。另一方面，这一特性极大地减小了分子设计对配体选择的限制。因此，过去十年来涌现了一系列基于铸币金属的TADF分子的文献报道。然而，与其他电子构型的金属配合物（如基于环金属配体的铱（Ⅲ）、铂（Ⅱ）配合物等）相比，正一价铸币金属配合物的稳定性有待提高。虽然具有高PLQY和高EQE的器件已经有广泛的报道，但运行稳定性优异的器件尚未实现，是该领域亟待解决的一个难题。"
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"data": "一价铸币金属配合物的TADF性能得到了广泛研究，而具有TADF特性的平面四配位构型的d"
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"data": "配合物却罕有报道。2015年，Zhu等发现四齿钯（Ⅱ）配合物（"
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"data": "Pd⁃1"
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]
},
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"data": {
"text": "图11",
"type": "fig",
"rid": "F11",
"data": [
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"data": "图11"
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}
},
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"data": "）在室温下表现出TADF和磷光的双重发射特征"
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"data": "["
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"data": "。在溶液中，配合物"
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}
]
},
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"data": "的PLQY达到了77%，绿光掺杂器件的最大EQE达到了21%。然而，如"
},
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"text": "图 11",
"type": "fig",
"rid": "F11",
"data": [
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"data": "图 11"
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"data": "所示，室温下"
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"data": "的光致发光以磷光为主，TADF发射占比小。另一方面，处于热力学平衡的S"
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"data": "1"
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]
},
{
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"data": "和T"
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"data": "1"
}
]
},
{
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"data": "态的发光寿命达到了140 μs，明显长于绝大多数的铸币金属配合物TADF分子。长激发态寿命表明从T"
},
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"data": "1"
}
]
},
{
"name": "text",
"data": "态到S"
},
{
"name": "sub",
"data": [
{
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"data": "1"
}
]
},
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"name": "text",
"data": "态反向系间窜越的过程缓慢，这与T"
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]
},
{
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"data": "态的失活以磷光发射为主相符。同样的现象在Zach等报道的钯（Ⅱ）（"
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"data": "Pd⁃2"
}
]
},
{
"name": "text",
"data": "）和铂（Ⅱ）的卟啉配合物中也有所体现"
},
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"name": "sup",
"data": [
{
"name": "text",
"data": "["
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"data": {
"text": "36",
"type": "bibr",
"rid": "R36",
"data": [
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"data": "36"
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]
}
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"data": "]"
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]
},
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"data": "。究其原因，所述配合物分子设计中均采用了传统的π-共轭配体，激发态具有显著的局域特性，因此Δ"
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}
]
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]
},
{
"name": "text",
"data": "较大，不利于RISC过程。这一推断可以从发射光谱的精细结构得到佐证。"
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"data": "（a）"
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"title": [
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]
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"data": "。在甲基环己烷溶液中，配合物"
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]
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"data": "的PLQY高达83%。变温光谱和瞬态光谱测试证实室温下"
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"data": "仅为66 meV，故而将其延迟荧光寿命缩短至2.1 μs（"
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"data": "）。由于其良好的溶解性，由溶液法制备的"
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"data": "的红光OLED器件最大EQE达到了7.4%，且在高亮度下随电流密度的增大其效率滚降较低。"
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"data": "（a）"
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]
},
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"data": "分子结构式；（b）室温下"
},
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"data": [
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"data": "Pt⁃1"
}
]
},
{
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"data": "在不同溶剂中的吸收与光致发光光谱；（c）"
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]
},
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"data": "的变温光致发光寿命"
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"data": [
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"data": "［"
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},
{
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"data": "。"
}
]
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"label": [
{
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"data": "Fig.12"
}
],
"title": [
{
"name": "text",
"data": "（a）Chemical structure of "
},
{
"name": "bold",
"data": [
{
"name": "text",
"data": "Pt⁃1"
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]
},
{
"name": "text",
"data": ". （b）Absorption and photoluminescence spectra of "
},
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"data": [
{
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"data": "Pt⁃1"
}
]
},
{
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"data": " in various solvents at room temperature. （c）Temperature dependent lifetime of "
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}
]
},
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"data": "［"
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"data": "对于金（Ⅲ）配合物，由于金（Ⅲ）离子的d"
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"data": "1"
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]
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"data": "态辐射跃迁速率小；另一方面，金原子的dσ"
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"data": "能级较低，容易引起其T"
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"data": "1"
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]
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{
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"data": "态快速的非辐射跃迁。这两种因素共同导致了大部分金（Ⅲ）配合物的磷光发光效率低。2017年，To等采用含强给电子基团的芳基配体合成了一类具有LLCT激发态的TADF金（Ⅲ）配合物（如"
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"data": "Au‐6"
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},
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"data": "，"
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"data": {
"text": "图13",
"type": "fig",
"rid": "F13",
"data": [
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"data": "["
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]
}
},
{
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]
},
{
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"data": "。这些配合物分子在溶液和薄膜中的发光量子产率分别达到了79%和84%。更重要的是，"
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]
},
{
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"data": "的发光寿命缩短到了1 μs以下，具备了作为优异的OLED发光材料的潜力。通过溶液法所制备的OLEDs器件最高EQE达到了23.8%。基于相同的思路，该研究组选用炔类配体获得了稳定性更好的TADF金（Ⅲ）配合物（"
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"data": "Au‐7"
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"text": "图13",
"type": "fig",
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"data": "图13"
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},
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"data": "["
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"data": {
"text": "39",
"type": "bibr",
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}
},
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"data": "]"
}
]
},
{
"name": "text",
"data": "。通过真空蒸镀法制备的OLED器件最大亮度达到70 300 cd·m"
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"data": "-2"
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"data": "，最大EQE达到了23.4%。"
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"data": "（a）"
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"data": [
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"data": "Au⁃6、Au⁃7、Au⁃8、Au⁃9"
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},
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"data": "分子结构式；（b）基于"
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"data": "Au⁃8"
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]
},
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"name": "text",
"data": "分子OLED器件发射光谱（左）及配合物器件外量子效率与亮度关系（右）"
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]
}
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"data": "］"
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]
},
{
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"data": "。"
}
]
},
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"label": [
{
"name": "text",
"data": "Fig.13"
}
],
"title": [
{
"name": "text",
"data": "（a）Chemical structures of "
},
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"name": "bold",
"data": [
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"data": "Au⁃6"
}
]
},
{
"name": "text",
"data": "， "
},
{
"name": "bold",
"data": [
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"data": "Au⁃7"
}
]
},
{
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"data": "， "
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},
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"data": " and "
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]
},
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"data": ". （b）Normalized EL spectra of OLEDs based on "
},
{
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"data": "Au⁃8"
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]
},
{
"name": "text",
"data": "（left） and EQE-luminance characteristics of OLEDs based on "
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]
},
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"data": "（right）"
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"data": "［"
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"data": "2020年，为了结合四齿d"
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"name": "text",
"data": "8"
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]
},
{
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"data": "配合物的稳定性优势，该研究组设计了一类给体-受体型的负三价四齿配体，并用于合成了TADF 金（Ⅲ）配合物（如"
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"data": "Au-8"
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"rid": "F13",
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"data": "图 13"
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"data": {
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"data": "。这些金（Ⅲ）配合物在溶液中的PLQY高达94%，在聚甲基丙烯酸甲酯（PMMA）薄膜中PLQY也达到了89%。通过真空蒸镀法制备的OLEDs最大EQE高达25.03%。在1 000 cd·m"
},
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"data": "-2"
}
]
},
{
"name": "text",
"data": "的亮度下，EQE仍然维持在22.01%，效率滚降小。尤其是，在100 cd·m"
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"data": [
{
"name": "text",
"data": "-2"
}
]
},
{
"name": "text",
"data": "的初始亮度下运行寿命（LT"
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"data": "95"
}
]
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{
"name": "text",
"data": "）达到5 280 h。以上器件性能代表了文献报道中的金（Ⅲ） 配合物OLEDs的最高水平。最近，Wong等通过在咔唑给体上修饰给电子／吸电子基团，设计合成了一系列具有LLCT/ILCT激发态的金（Ⅲ）配合物，通过激发态属性的调控，实现了在薄膜中的高效率TADF发射。其中，"
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{
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"data": "的PLQY率达到了79%（"
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"type": "fig",
"rid": "F13",
"data": [
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"data": "图13"
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}
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{
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"data": "），在 1 000 cd·m"
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"data": "-2"
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]
},
{
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"data": "的亮度下器件效率滚降低于1%，并且器件的稳定性得到了较好的提升"
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]
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"data": [
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"data": "需要指出的是，尽管上述研究已经表明钯（Ⅱ）和铂（Ⅱ）配合物同样可以发射TADF，但是采用π-共轭配体对于获得TADF具有很大的不确定性。因为局域激发态（如ππ"
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]
},
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"data": "）的Δ"
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"data": "通常比较大，不利于TADF。分子的前线轨道分布对于Δ"
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]
},
{
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"data": "具有决定性影响，比如近年来流行的多重共振体系"
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"data": [
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"data": "["
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"data": {
"text": "47",
"type": "bibr",
"rid": "R47",
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"data": "47"
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]
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}
]
},
{
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"data": "和上述双核铂（Ⅱ）配合物都具有小的Δ"
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]
},
{
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"data": "ST"
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]
},
{
"name": "text",
"data": "，但是其在配合物分子中难以精准调控。这也解释了文献报道中TADF钯（Ⅱ）和铂（Ⅱ）配合物数量少的原因。相比之下，金（Ⅲ）配合物采用LLCT和ILCT激发态的思路更具可行性，容易通过合理的分子设计实现。然而，对于铂（Ⅱ）配合物，即便采用与金（Ⅲ）配合物类似的配体结构，其SOC效应往往也更突出，更容易发射磷光。这一因素对于钯（Ⅱ）配合物影响比较小，因此，研究人员采用该策略有望获得TADF钯（Ⅱ）配合物。总之，我们认为对于设计TADF金属配合物而言，除了构建电荷转移激发态（LLCT或ILCT），精准地调控金属原子的参与程度是一个关键因素。未来，对于不同的金属中心建立像纯有机TADF材料一样具有普适性的分子设计策略具有重要意义。"
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"data": "在第三过渡系金属元素中，由于地壳中的钨元素储量丰富，其配合物分子的发光研究也因此备受关注"
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]
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{
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"data": "。Chan等通过在salen配体外围修饰具有给电子性能的胺基取代基，合成了一类顺式结构的钨（Ⅵ）配合物分子（如"
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"text": "图 14",
"type": "fig",
"rid": "F14",
"data": [
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"data": "图 14"
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}
},
{
"name": "text",
"data": "），在空气中具有良好的稳定性"
},
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]
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"data": "。配合物"
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"data": "W⁃1"
}
]
},
{
"name": "text",
"data": "在PMMA薄膜中的PLQY达到84%，激发态寿命为1 μs。光谱探测证实了该配合物的TADF发光机理。理论计算表明该体系配合物具有ILCT激发态。需要指出的是，连接外围二芳基胺与salen配体的间二甲基苯对于减小分子的Δ"
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},
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]
},
{
"name": "text",
"data": "是必要的，其位阻效应能够使HOMO和LUMO有效地分离。作者利用"
},
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"data": "W⁃1"
}
]
},
{
"name": "text",
"data": "作为发光分子，首次实现了基于钨（Ⅵ）配合物的高性能OLED，其最大EQE和最大亮度分别达到15.8%和16 890 cd·m"
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]
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"data": "分子结构式；（b）基于"
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"data": "W⁃1"
}
]
},
{
"name": "text",
"data": "分子的OLED器件发射光谱（左）及器件外量子效率与亮度关系（右）"
},
{
"name": "sup",
"data": [
{
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"data": "［"
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"label": [
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"data": [
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"data": "Zr⁃1"
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]
},
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"data": ". （b）Normalized EL spectra of OLEDs based on "
},
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"data": "W⁃1"
}
]
},
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"data": "（left） and EQE-luminance characteristics of OLEDs based on "
},
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]
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"data": " ［"
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"data": {
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"rid": "R42",
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]
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{
"name": "text",
"data": "过渡金属配合物由于全空的d轨道，存在低能级的LMCT激发态。由于激发过程中金属中心的广泛参与，该类型配合物具有丰富的光化学反应活性"
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"data": "["
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"data": "。Zhang等在锆（Ⅳ）配合物分子（"
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"data": "Zr⁃1"
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]
},
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"text": "图14",
"type": "fig",
"rid": "F14",
"data": [
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"data": "）中发现了TADF现象"
},
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"data": "["
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"data": {
"text": "43",
"type": "bibr",
"rid": "R43",
"data": [
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"data": "43"
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]
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},
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]
},
{
"name": "text",
"data": "。然而，所述配合物具有长达350 μs的激发态寿命，且发光效率低，不适于制备高性能OLED。需要注意的是，虽然激发态前线轨道含有金属d轨道成分，但如此长的延迟荧光寿命表明除金属原子外的其他因素亟待优化调控。前线轨道的空间分离不充分是潜在的原因之一。结合理论计算进行分子结构设计，进一步缩短分子的发光寿命，是获得高效率、短寿命TADF锆（Ⅳ）配合物的必要前提。考虑到地壳中锆元素的储量丰富，开发基于锆配合物的光电材料具有重要价值。"
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"data": [
{
"name": "text",
"data": "本文总结了TADF过渡金属配合物的研究进展，根据金属中心d轨道电子构型和激发态属性的不同对配合物分子进行了分类，对代表性的d"
},
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"data": [
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"name": "text",
"data": "10"
}
]
},
{
"name": "text",
"data": "铸币金属配合物、平面构型的d"
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"data": [
{
"name": "text",
"data": "8"
}
]
},
{
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"data": "金属配合物、d"
},
{
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"data": [
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"data": "0"
}
]
},
{
"name": "text",
"data": "钨（Ⅵ）和锆（Ⅳ）配合物的光物理性质及其OLED性能进行了总结、对比和讨论。已有研究表明，通过合理的配体设计调控分子的激发态，同时借助金属中心对于激发态的调控作用，能够促进过渡金属配合物的RISC过程，使得原来衰减较慢的三重态激发态转换为单重态激发态，进而辐射高效率的TADF。因此，与纯有机TADF材料相比，金属配合物TADF材料的延迟荧光寿命通常较短，凸显了金属原子的显著调控作用。"
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"data": [
{
"name": "text",
"data": "目前，具有TADF性质的过渡金属配合物主要集中在d"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "10"
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]
},
{
"name": "text",
"data": "铸币金属元素上。其简单、高效的配位反应条件、简易可调的LLCT激发态属性、以及能够避免dd激发态猝灭发光的结构特点使得该类金属配合物获得了广泛的关注。研究人员通过对激发态的精准调控，在基于多齿配体的d"
},
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"data": [
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"data": "8"
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]
},
{
"name": "text",
"data": "金属配合物方面也获得了非常优异的光物理和器件性能。然而，其发光颜色的调控目前比较有局限性。尤其是相关的文献报道数量少，激发态的调控难度大，尚未建立可行性强的分子设计思路。具有d"
},
{
"name": "sup",
"data": [
{
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"data": "0"
}
]
},
{
"name": "text",
"data": "电子构型的金属配合物面临同样的研究现状。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "相比于开发高效率的磷光分子，TADF机制为开发基于非贵金属元素的发光配合物提供了一种可行的思路。已报道的研究工作表明除了铂、金、钯等稀缺元素外，基于铜、银、和钨的配合物同样能够获得高效率、短延迟寿命的TADF，以及高效率的OLEDs。因此，TADF过渡金属配合物值得研究人员进一步深入探索，在发光贵金属配合物的研究基础上取得突破。"
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"data": [
{
"name": "text",
"data": "本文专家审稿意见及作者回复内容的下载地址："
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"data": {
"text": [
{
"name": "text",
"data": "http://cjl.lightpublishing.cn/thesisDetails#10.37188/"
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"data": [
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"data": "CJL.20220308."
}
]
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{
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"data": "张靖羚,李凯,杨楚罗.过渡金属配合物TADF发光材料研究进展[J].发光学报,2023,44(01):12-25."
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"text": "张靖羚,李凯,杨楚罗.过渡金属配合物TADF发光材料研究进展[J].发光学报,2023,44(01):12-25."
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"text": "ZHANG Jingling,LI Kai,YANG Chuluo.Advances in Thermally Activated Delayed Fluorescence of Transition Metal Complexes[J].Chinese Journal of Luminescence,2023,44(01):12-25."
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"text": [
{
"name": "text",
"data": "国家自然科学基金（21801170）； 广东省基础与应用基础研究委员会面上项目（2021A1515010175）"
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"data": "Supported by National Natural Science Foundation of China（21801170）； Guangdong Basic and Applied Basic Research Foundation（2021A1515010175）"
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"history": {
"received": "2022-08-26",
"revised": "2022-09-19",
"ppub": "2023-01-05",
"opub": "2023-02-16"
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"journalTitle": "发光学报",
"issue": "1",
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}
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