OLED电子传输材料研究进展 增强出版

{ "defaultlang": "zh", "titlegroup": { "articletitle": [ { "lang": "zh", "data": [ { "name": "text", "data": "OLED电子传输材料研究进展" } ] }, { "lang": "en", "data": [ { "name": "text", "data": "Recent Advances on Electronic Transport Materials in OLEDs" } ] } ] }, "contribgroup": { "author": [ { "name": [ { "lang": "zh", "surname": "唐", "givenname": "振宇", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "TANG", "givenname": "Zhenyu", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [ "first-author" ], "bio": [ { "lang": "zh", "text": [ "唐振宇（1994-），男，辽宁大连人，博士研究生，2019年于上海大学获得硕士学位，主要从事OLED材料和器件方向的研究。 E-mail： tangzhenyu@stu.pku.edu.cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941508&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941518&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941513&type=", "width": "24.89202881", "height": "29.88732910", "fontsize": "" } ], "data": [ [ { "name": "text", "data": "唐振宇" }, { "name": "text", "data": "（1994-），男，辽宁大连人，博士研究生，2019年于上海大学获得硕士学位，主要从事OLED材料和器件方向的研究。 E-mail： " }, { "name": "text", "data": "tangzhenyu@stu.pku.edu.cn" } ] ] } ], "email": "tangzhenyu@stu.pku.edu.cn", "deceased": false }, { "name": [ { "lang": "zh", "surname": "郭", "givenname": "浩清", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "GUO", "givenname": "Haoqing", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [], "deceased": false }, { "name": [ { "lang": "zh", "surname": "肖", "givenname": "静", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "XIAO", "givenname": "Jing", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff2", "text": "2" } ], "role": [ "corresp" ], "corresp": [ { "rid": "cor1", "lang": "en", "text": "E-mail： xiaojingzx@163.com", "data": [ { "name": "text", "data": "E-mail： xiaojingzx@163.com" } ] } ], "bio": [ { "lang": "zh", "text": [ "肖静（1979-），女，山东泰安人，博士，教授，2007年于北京交通大学获得博士学位，主要从事有机电子材料和器件方向的研究。 E-mail: xiaojingzx@163.com" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941524&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941533&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941530&type=", "width": "24.89202881", "height": "29.88732147", "fontsize": "" } ], "data": [ [ { "name": "text", "data": "肖静" }, { "name": "text", "data": "（1979-），女，山东泰安人，博士，教授，2007年于北京交通大学获得博士学位，主要从事有机电子材料和器件方向的研究。 E-mail: " }, { "name": "text", "data": "xiaojingzx@163.com" } ] ] } ], "email": "xiaojingzx@163.com", "deceased": false }, { "name": [ { "lang": "zh", "surname": "陈", "givenname": "志坚", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "CHEN", "givenname": "Zhijian", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [], "deceased": false }, { "name": [ { "lang": "zh", "surname": "肖", "givenname": "立新", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "XIAO", "givenname": "Lixin", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [ "corresp" ], "corresp": [ { "rid": "cor2", "lang": "en", "text": "lxxiao@pku.edu.cn", "data": [ { "name": "text", "data": "lxxiao@pku.edu.cn" } ] } ], "bio": [ { "lang": "zh", "text": [ "肖立新(1966-)，男，湖南衡阳人，博士，教授，博士生导师，2000年于东京大学获得博士学位，主要从事OLED材料和器件以及太阳能电池方向的研究。 E-mail: lxxiao@pku.edu.cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941539&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941545&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941543&type=", "width": "24.89202499", "height": "29.88732910", "fontsize": "" } ], "data": [ [ { "name": "text", "data": "肖立新" }, { "name": "text", "data": "(1966-)，男，湖南衡阳人，博士，教授，博士生导师，2000年于东京大学获得博士学位，主要从事OLED材料和器件以及太阳能电池方向的研究。 E-mail: " }, { "name": "text", "data": "lxxiao@pku.edu.cn" } ] ] } ], "email": "lxxiao@pku.edu.cn", "deceased": false } ], "aff": [ { "id": "aff1", "intro": [ { "lang": "zh", "label": "1", "text": "北京大学 物理学院， 人工微结构和介观物理国家重点实验室， 北京　100871", "data": [ { "name": "text", "data": "北京大学 物理学院， 人工微结构和介观物理国家重点实验室， 北京　100871" } ] }, { "lang": "en", "label": "1", "text": "State Key Laboratory for Artificial Microstructures and Mesoscopic Physics， Department of Physics， Peking University， Beijing 100871， China", "data": [ { "name": "text", "data": "State Key Laboratory for Artificial Microstructures and Mesoscopic Physics， Department of Physics， Peking University， Beijing 100871， China" } ] } ] }, { "id": "aff2", "intro": [ { "lang": "zh", "label": "2", "text": "泰山学院 物理与电子工程学院， 山东 泰安　271000", "data": [ { "name": "text", "data": "泰山学院 物理与电子工程学院， 山东 泰安　271000" } ] }, { "lang": "en", "label": "2", "text": "College of Physics and Electronic Engineering， Taishan University， Taian， 271000， China", "data": [ { "name": "text", "data": "College of Physics and Electronic Engineering， Taishan University， Taian， 271000， China" } ] } ] } ] }, "abstracts": [ { "lang": "zh", "data": [ { "name": "p", "data": [ { "name": "text", "data": "有机电致发光（OLED）是目前最有竞争力的显示技术，市场占有量逐年攀升。高效、稳定的OLED，特别是深蓝光器件，性能仍需提升，其关键问题是高性能的电子传输材料的研发。这是由于有机分子难以获得较高电子迁移率，器件中的复合区域通常靠近电子传输层一侧，这就要求电子传输材料需要具有较高三线态能级来限域激子，尤其是高能量的蓝光激子。而高三线态（弱共轭）和高迁移率（强共轭）一直是有机分子设计中难以调和的矛盾，此外更宽的带隙也会导致较差的热稳定性，这些难题始终限制着OLED电子传输材料的发展。本文分类介绍了高性能的电子传输材料所需要具备的几点特性，包括热稳定性、光化学稳定性、电子迁移率、前线轨道能级和三重态能级等，并且综述了21世纪以来OLED小分子电子传输材料的重要研究进展，以期对未来开发理想的电子传输材料提供参考。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "Organic light emitting diodes （OLED） technology is considered to be the next generation of display technology， and has gradually occupied the mainstream of the market， but the performance of OLED is still largely limited by electron transport materials， especially in high-performance deep blue light devices. Because it is difficult for organic molecules to obtain high electron mobility， and the recombination zone in the device is usually close to the interface of the electron transport layer， which requires the electron transport material to have a high triplet energy level to confine the exciton， especially the blue light exciton with high energy. However， high triplet states （poor conjugation） and high mobility （strong conjugation） have always been difficult to reconcile in the design of organic molecules， and a wider band gap will also lead to poorer thermal stability. These problems have been affecting the development of OLED electronic transport materials. In this paper， several elements of high performance electronic transport materials are introduced， including thermal stability， photochemical stability， electron mobility， the frontier orbital and the triplet energy level and so on. And the important research progresses of the micromolecular electron transport materials in 21st century are summarized， in order to provide the reference for the development of the ideal electronic transfer materials in the future." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "有机电致发光" } ], [ { "name": "text", "data": "电子传输材料" } ], [ { "name": "text", "data": "稳定性" } ], [ { "name": "text", "data": "电子迁移率" } ], [ { "name": "text", "data": "三重态能级" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "organic light-emitting diodes" } ], [ { "name": "text", "data": "electronic transport materials" } ], [ { "name": "text", "data": "stability" } ], [ { "name": "text", "data": "electron mobility" } ], [ { "name": "text", "data": "triplet energy" } ] ] } ], "highlights": [], "body": [ { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "1　引　　言" } ], "level": "1", "id": "s1" } }, { "name": "p", "data": [ { "name": "text", "data": "进入21世纪以来，随着电视机、计算机以及智能手机和互联网的普及发展，人们每天能接收到成千上万的来自世界各地的信息，而这其中有70%是通过视觉获得的。因此，显示技术成为信息时代人与世界之间的桥梁。自1897年德国物理学家Braun发明第一台阴极射线显示管以来，显示技术不断地被改进和发展。在过去的十几年中，液晶显示（LCD）成为主流显示技术。近年来，有机发光二极管（OLED） 由于具备发光柔和、响应速度快、色彩度饱满、视角广等优点逐渐被业界认为是最理想的显示技术，特别是在柔性显示方面的应用更是具有无法替代的优势。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "OLED里程碑式的工作是1987年柯达公司的邓青云教授报道的以芳香二胺作为空穴传输材料（HTM）、8-羟基喹啉铝（Alq" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "）作为电子传输（ETM）和发光材料（EM）制备的双层无定形薄膜型OLED器件，其最大外量子效率（EQE）达到1%，最高亮度达到1 000 cd·m" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "，OLED器件由此具备了进入实用化阶段的可能" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "1", "type": "bibr", "rid": "R1", "data": [ { "name": "text", "data": "1" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。此后，OLED迎来了飞速发展，本世纪初开始市场化，目前已经成为主流显示之一，并独占柔性显示市场。OLED的工作原理与LED类似，通过电极注入的空穴和电子经过传输层进入发光材料，在库仑力作用下空穴和电子结合产生激子，激子辐射跃迁回到基态从而发出光子" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "2", "type": "bibr", "rid": "R2", "data": [ { "name": "text", "data": "2" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。但是，由于构成有机发光材料的共轭分子之间的相互作用是范德华力，作用力较弱，所以激子结合能较大，发光过程主要是激子行为。根据自旋态，激子分为三线态激子（75%）和单线态激子（25%）。三线态激子为跃迁禁阻，难以辐射跃迁发出光子，这就限制了OLED器件的效率。为了利用全部的激子，马於光和Forrest等于1997年先后提出了磷光OLED材料，利用重金属原子来增强自旋-轨道耦合作用，打破三线态的自旋禁阻，实现磷光的室温发光，突破了此前荧光OLED内量子效率（IQE）25%的理论极限" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "3", "type": "bibr", "rid": "R3", "data": [ { "name": "text", "data": "3" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "4", "type": "bibr", "rid": "R4", "data": [ { "name": "text", "data": "4" } ] } } ], "rid": [ "R3", "R4" ], "text": "3-4", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。此外，近年来研究较多的热活化延迟荧光（TADF）材料也能够实现100%的激子利用率。TADF材料由Adachi等最早用于OLED器件，其原理是通过合理调控分子结构，使得三线态与单线态能级差足够小，使三线态激子在热作用下可以反系间窜跃至单线态从而辐射跃迁产生延迟荧光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "5", "type": "bibr", "rid": "R5", "data": [ { "name": "text", "data": "5" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "6", "type": "bibr", "rid": "R6", "data": [ { "name": "text", "data": "6" } ] } } ], "rid": [ "R5", "R6" ], "text": "5-6", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "即使是OLED已经在市面上大规模应用的今日，还面临着许多问题尚未彻底解决，深蓝光OLED器件仍有效率低下、工作寿命短等瓶颈。这是由于深蓝光发光所需的宽带隙有机材料具有性质不稳定、器件中激子难以限域等问题" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "7", "type": "bibr", "rid": "R7", "data": [ { "name": "text", "data": "7" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，高效率长寿命的深蓝光OLED的实现甚至被喻为有机电子学领域的“圣杯”" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "8", "type": "bibr", "rid": "R8", "data": [ { "name": "text", "data": "8" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。有机分子的导电性由两个方面决定：一、分子内载流子传输源于共轭π键，p-p电子云重叠形成成键轨道（π对应HOMO能级）和反成键轨道（π" }, { "name": "sup", "data": [ { "name": "text", "data": "*" } ] }, { "name": "text", "data": "对应LUMO能级），成键轨道具有更好的离域性，所以这有利于空穴在HOMO能级上的传输；二、分子间的传输主要通过跳跃式模型，它依赖于相邻分子前线分子轨道电子云的重叠，因为成键轨道离域性好，所以电子云更好地重叠，这也有利于有机材料的空穴传输。所以有机材料难以获得较高的电子迁移率，因此对于高性能有机电子传输材料的开发一直是领域中很多研究者们的研究目标。不论是为了未来服务于深蓝光OLED器件，抑或是进一步推动有机电子学的前沿研究，或是将有机半导体材料应用于更广泛的电子器件当中，有机电子传输材料的相关研究均有至关重要的意义。因此，本文从实现高性能电子传输材料所需的特性出发，总结了近年来有机小分子电子传输材料的重要研究进展，以期对未来的相关研究提供参考。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2　电子传输材料的要素" } ], "level": "1", "id": "s2" } }, { "name": "p", "data": [ { "name": "text", "data": "本文主要关注应用于高效OLED器件的高性能有机电子传输材料，因此从影响OLED器件性能的角度入手，介绍高性能电子传输材料的稳定性、电子迁移率、能级等重要特性。" } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.1　稳定性" } ], "level": "2", "id": "s2a" } }, { "name": "p", "data": [ { "name": "text", "data": "电子传输材料的稳定性对面向应用的OLED器件寿命来说至关重要，其稳定性可大致分为热（物理）稳定性和化学稳定性两种。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "由于OLED器件在生产时需经过包括光刻、蒸镀、封装等多道工序，不可避免地需要承受高温处理的影响，而且器件在工作时也会产生大量焦耳热。以往的研究表明，高温环境会对OLED器件产生致命的破坏。其不仅体现在高温会使得热稳定性差的有机薄膜由无定形薄膜开始结晶化从而导致器件衰减" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "9", "type": "bibr", "rid": "R9", "data": [ { "name": "text", "data": "9" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "；温度升高也会使得OLED器件发光区域产生不均匀的局部电流，导致发光不均匀" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "；高温环境也会产生热应力并在降温后使得薄膜形成褶皱，使OLED的效率和工作寿命大幅衰减" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "11", "type": "bibr", "rid": "R11", "data": [ { "name": "text", "data": "11" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，甚至导致器件短路从而产生不发光的“黑点”" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "12", "type": "bibr", "rid": "R12", "data": [ { "name": "text", "data": "12" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。有机材料的热稳定性可以通过玻璃化转变温度（" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "）来衡量，目前，研究者们普遍通过合理设计分子结构（例如提升分子量或采用刚性分子结构）来获得具有更高" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "的有机材料。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "和无机材料相比，有机分子具有较低的电子迁移率，电子传输材料的老化直接影响OLED器件的老化。因此，电子传输材料对于热稳定性的要求极高，大多常见的有机分子的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "通常在几十摄氏度至150 ℃左右；而针对实际应用的长寿命高稳定性OLED器件，理想的电子传输材料至少达到150 ℃以上的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "除了热稳定性以外，对于有机电子传输材料来说化学稳定性也是重要的考量。大多数OLED器件在工作中由于电子传输性能会低于空穴传输性能，使得其激子复合区域接近于电子传输层（如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "所示）。早期就有研究表明，一旦空穴泄露到电子传输层中产生ETM的阳离子，器件会发生严重老化" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。后来的研究发现，有机分子激发态下的能量如果大于分子其中某个C—" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "text", "data": "化学键的键解离能（BDE），有可能产生C—" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "text", "data": "化学键断裂导致分子降解" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "14", "type": "bibr", "rid": "R14", "data": [ { "name": "text", "data": "14" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，这一点也可经激光解吸-飞行时间质谱（LDI-TOF-MS）实验证实" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "15", "type": "bibr", "rid": "R15", "data": [ { "name": "text", "data": "15" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "常见的OLED器件中激子复合区域" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.1" } ], "title": [ { "name": "text", "data": "Recombination zone for excitons in OLED" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941549&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941556&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941552&type=", "width": "34.45935059", "height": "51.56200409", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "为了防止电子传输层被空穴入侵而导致的老化，通常会设计出最高占据分子轨道（HOMO）能级较深的ETM分子，通过拉大与发光层HOMO能级的能级差来阻止空穴泄露至电子传输层。为了提升分子的化学稳定性，则可以通过合理的分子设计手段，使得分子中最弱C—" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "text", "data": "单键的BDE（也称BDEf）尽量大于其分子的单线态（S" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "）和三线态能量（" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "），从而使得ETM分子避免降解老化" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "16", "type": "bibr", "rid": "R16", "data": [ { "name": "text", "data": "16" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.2　电子迁移率" } ], "level": "2", "id": "s2b" } }, { "name": "p", "data": [ { "name": "text", "data": "高效的OLED器件需要平衡的空穴和电子注入，而有机分子中电子的迁移率往往低于空穴迁移率，这是由有机材料导电性质决定的，见上文的分析。因此，为了获得高效且稳定的OLED器件，研究者们一直在致力于提高有机电子传输材料的迁移率。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "目前常见的有机小分子空穴传输材料的迁移率一般为10" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "~10" }, { "name": "sup", "data": [ { "name": "text", "data": "-4" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "·V" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "·s" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "，而有机小分子电子传输材料的电子迁移率大多数仅有10" }, { "name": "sup", "data": [ { "name": "text", "data": "-4" } ] }, { "name": "text", "data": "~10" }, { "name": "sup", "data": [ { "name": "text", "data": "-6" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "·V" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "·s" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "。从分子设计的角度，研究者们通常采用引入吡啶（Pyridine）、嘧啶（Pyrimidine）、三嗪（Triazine）等含氮六元杂环，以及磷氧化物（Phosphine oxide）、喹啉（Quinoline）、三唑（Triazole）等吸电子基团（分子式如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "所示）来提升有机分子的电子迁移率。这是由于吸电子类基团大多具有拉低分子LUMO能级的能力，有利于与高功函的电极匹配，实现材料n型导电能力的增强；并且引入氢键等分子间相互作用，提升电子传输能力。此外，设计平面型的分子结构也有助于电子云的重叠从而通过提升电荷传输性来提升电子迁移率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "17", "type": "bibr", "rid": "R17", "data": [ { "name": "text", "data": "17" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "几种常见的吸电子基团" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.2" } ], "title": [ { "name": "text", "data": "Several common electron accepting groups" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941560&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941568&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941565&type=", "width": "75.22137451", "height": "37.74426270", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "除了通过分子设计来直接提升有机小分子的电子迁移率，研究者们还尝试采用n型掺杂的策略来提升有机电子传输材料的迁移率和稳定性，即将具有较小电离能的电子给体（n型掺杂剂，如活泼金属等）掺杂于具有较大电子亲和能的有机电子传输层中，这可以使得电子自发地从给体转移到电子传输层分子中。这种n型掺杂策略不仅可以填充电子传输材料膜层中的陷阱，减少载流子的捕获而提升电子迁移率，还可以调控最低占据分子轨道（LUMO）能级来提升电子的注入性能。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "电子传输层n型掺杂剂种类很多，早期有直接采用活泼金属如Li、Cs和Mg等单质作为电子传输层和Al电极层间的n型掺杂剂" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "18", "type": "bibr", "rid": "R18", "data": [ { "name": "text", "data": "18" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } } ], "rid": [ "R18", "R19", "R20" ], "text": "18-20", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，但是这些金属有可能扩散至发光层中导致激子猝灭，限制了器件的效率和稳定。也有采用金属氧化物作为n型掺杂剂，例如采用MnO与Alq" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "掺杂可以提升Alq" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "的迁移率和电子注入能力，且可同时改善有机材料的空气稳定性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "21", "type": "bibr", "rid": "R21", "data": [ { "name": "text", "data": "21" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。8-羟基喹啉-锂（Liq）是目前被广泛使用的电子传输层n型掺杂剂，得益于其独特的与Al电极相互作用的机制，基于Liq作为电子传输层掺杂剂的OLED器件普遍具有优异且稳定的性能" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "22", "type": "bibr", "rid": "R22", "data": [ { "name": "text", "data": "22" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "24", "type": "bibr", "rid": "R24", "data": [ { "name": "text", "data": "24" } ] } } ], "rid": [ "R22", "R23", "R24" ], "text": "22-24", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。此外，近年来也有研究者采用金属与有机分子配位的n型掺杂策略，这种金属配位活化的策略具有空气稳定、无副产物等优势，具有优异的性能，未来有望替代传统的碱金属或碱金属盐等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "25", "type": "bibr", "rid": "R25", "data": [ { "name": "text", "data": "25" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "有机半导体材料的迁移率测试方式大多采用飞行时间法（TOF）或空间电荷限制电流法（SCLC）。其中TOF法测试相对较为准确直接，而SCLC法更便捷，容易在实验室实现。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.3　能级" } ], "level": "2", "id": "s2c" } }, { "name": "p", "data": [ { "name": "text", "data": "除了稳定性和电子迁移率以外，合适的电子传输材料LUMO、HOMO以及三线态能级也是实现高性能OLED的重要前提。为了降低电子注入到发光层的势垒，实现低驱动电压以及优良的发光性能，电子传输层必须具有合适的LUMO能级。高性能的有机电子传输材料的LUMO能级大多处于-2.5~-3.5 eV，这是因为常用的电极如LiF/Al的界面功函约为3.4 eV，电子传输层LUMO能级与电极功函数的势垒越小则越容易注入电子。前文提到的电子传输层n型掺杂策略的一个主要优势就是可以减小电子传输层、电子注入层和电极层之间的势垒，大幅提升电子注入性能。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "早期人们曾认为电子传输材料的电子迁移率是限制OLED效率的主要因素，但是后续有研究人员发现，如果电子传输材料具有足够深的HOMO能级，即使具有较低的迁移率，依然能够实现高效的OLED器件" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "26", "type": "bibr", "rid": "R26", "data": [ { "name": "text", "data": "26" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，这是由于深HOMO能级能够阻止空穴进入电子传输层，不仅减少了非辐射跃迁导致的激子猝灭，也减少了电子传输层的老化。因此设计具有较深HOMO能级的电子传输材料也是重要的研究目标。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "不论是已经走向应用的磷光材料还是未来具有巨大应用潜力的TADF类材料，在OLED器件中对发光层激子的限域需求是类似的。如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（a）所示为磷光和TADF发光原理，由于电流注入下生成的单线态与三线态激子的比例为1∶3，只有将占比达到75%的三线态激子全部利用才能实现100%的内量子效率；而基于磷光和TADF机制的发光材料往往需要具有较高的三线态能级，尤其是蓝色或深蓝色发光材料通常具有高达2.6~3.0 eV的三线态能级。因此理想的OLED器件需要两侧传输层都具有高三线态能级以实现类似“量子阱”的结构来达成对发光层中三线态的限域，如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（b）所示。而如前文所述，通常OLED中电子迁移率低于空穴迁移率，导致器件中的激子复合区域靠近电子传输层一侧，这就对电子传输层的三线态阻挡能力提出了较高的要求" }, { "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": "。" } ] }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "（a） 磷光发光和TADF发光机理；（b）空穴传输/发光层/电子传输层的理想三线态能级。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.3" } ], "title": [ { "name": "text", "data": "（a）Phosphorescence and TADF luminescence mechanism. （b）Ideal triplet state levels in the HTM/EML/ETM." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941572&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941581&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941578&type=", "width": "120.70251465", "height": "50.95886230", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "然而，若想在有机分子中实现高的三线态能级，往往需要通过减弱共轭的方式实现。虽然弱共轭体系会带来带隙和三线态能级的提高，但也会大幅降低材料的迁移率，甚至分子的稳定性也会降低。因此一直以来，实现电子传输材料高迁移率和高三线态的平衡是一项巨大的挑战，吸引了许多研究者为之付出努力" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "总而言之，理想的有机小分子电子传输材料需要具备诸多要素（特性），主要为：通过较高的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "和键解离能获得良好的热及化学稳定性；需具备高电子迁移率以使器件中空穴-电子注入平衡获得优秀的器件性能；需具备合适的LUMO（-2.5～-3.5 eV）能级获得优异的电子注入；需具备足够深的HOMO（-6.0～-7.0 eV）能级来阻挡空穴；需具备较高的三线态能级（2.8～3.5 eV）以限域发光层中的三线态激子。目前，能够同时兼顾以上几点的分子少之又少，不论是学术还是产业领域仍都在努力探索性能更佳的有机小分子电子传输材料。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3　有机小分子电子传输材料研究进展" } ], "level": "1", "id": "s3" } }, { "name": "p", "data": [ { "name": "text", "data": "开发高效的ETM对提高OLED器件的效率和稳定性至关重要，本节将介绍一些经典的和近年来报道的电子传输材料。Alq" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "、TPBi、Bphen和BCP等是使用较多的传统电子传输材料。Alq" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "是最早报道的用于OLED的有机材料，其" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "高达172 ℃，并且得益于其具有两个同相异构体阻止结晶化，具有良好的稳定性，在过去很长一段时间里被认为是最好的电子传输材料。但是，Alq" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "的HOMO能级仅有-5.8 eV，与常用的主体材料HOMO能级接近，不能够阻挡空穴" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "29", "type": "bibr", "rid": "R29", "data": [ { "name": "text", "data": "29" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。基于苯并咪唑的TPBi是在各种光电器件研究中被广泛使用的一种电子传输材料，其LUMO能级为-2.7 eV，HOMO能级为-6.2 eV，" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "能级为2.65 eV，TOF法测得迁移率约为1×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-5" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "·V" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "·s" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "，具有不错的电子注入和空穴阻挡能力、尚可的电子迁移率和优秀的稳定性，但是其短板在于不够高的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "能级限制了其在蓝色磷光或TADF-OLED中的应用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "30", "type": "bibr", "rid": "R30", "data": [ { "name": "text", "data": "30" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "31", "type": "bibr", "rid": "R31", "data": [ { "name": "text", "data": "31" } ] } } ], "rid": [ "R30", "R31" ], "text": "30-31", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Bphen也是常用的电子传输材料，邻菲罗啉基团为其带来了优秀的电子迁移率，比TPBi要高一个数量级，并且HOMO能级为-6.4 eV，能够有效阻挡空穴；但Bphen自身的稳定性较差，容易导致器件老化，寿命缩短" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。BCP则是结构与Bphen类似的分子，苯环上多出了两个甲基使得BCP的HOMO和LUMO能级均被拉低，更有利于阻挡空穴；但是甲基也使得BCP的电子迁移率大幅降低，使BCP的应用受到了限制" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "在OLED电子传输材料研究领域，来自日本的Kido课题组做出了很多贡献，他们曾报道了一系列性能优异的电子传输材料。2008—2009年，Kido课题组报道了经典的基于苯基吡啶的系列分子。TmPyPB、TpPyPB、Tm2PyPB和Tm4PyPB是四个结构相似的以三苯基苯为核心的分子，其区别只在于苯基吡啶以及苯环上N的取代位置不同。TmPyPB和TpPyPB的HOMO能级很接近，为 -6.7 eV左右，而LUMO能级分别为-2.74 eV和-3.04 eV。TmPyPB得益于间位连接的苯环和N原子，限制了分子内共轭，获得了高达2.75 eV的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "能级，电子迁移率约为1×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "·V" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "·s" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "；TpPyPB的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "仅有2.57 eV，但是拥有更加出色的电子迁移率，SCLC测试高达7.9×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "·V" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "·s" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "，这已经是与空穴传输材料迁移率接近的水平" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "34", "type": "bibr", "rid": "R34", "data": [ { "name": "text", "data": "34" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Tm2PyPB和Tm4PyPB与TmPyPB的区别仅在于苯基吡啶上的N原子取代位置分别为邻位和对位，由于其核心骨架结构一样，三者的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "能级均为2.75 eV左右，并且迁移率也比较接近，但是它们的LUMO和HOMO能级则以N原子邻位、间位、对位的顺序逐渐变深。最后通过OLED器件发现，TmPyPB因具有较高的迁移率获得了最高的EQE，而Tm4PyPB得益于优秀的LUMO（-2.94 eV）和HOMO（-6.68 eV）能级在蓝色磷光器件中获得了最低的驱动电压" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "35", "type": "bibr", "rid": "R35", "data": [ { "name": "text", "data": "35" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。此外，Kido课题组还通过增加吡啶数量或修改核心基团调控电子传输材料的功能性，例如BmPyPB和3TPYMB" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "36", "type": "bibr", "rid": "R36", "data": [ { "name": "text", "data": "36" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，其中3TPYMB由于B元素的引入打断了共轭，使得其" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "能级高达3.0 eV" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。上述分子的结构如" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "所示。" } ] }, { "name": "fig", "data": { "id": "F4", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图4" } ], "title": [ { "name": "text", "data": "一些经典电子传输材料和基于苯基吡啶的电子传输材料" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.4" } ], "title": [ { "name": "text", "data": "Some classical ETMs and phenylpyridine based ETMs" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941585&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941594&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39941590&type=", "width": "137.49871826", "height": "58.58067322", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "2007年，Tanaka等报道了基于嘧啶骨架的分子B3PYMPM，" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "能级位于2.76 eV，具有不错的热稳定性；同时LUMO能级为-3.2 eV，有利于电子注入，TOF法电子迁移率约为1×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-5" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "·V" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "·s" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "，在绿色磷光OLED中表现出了优秀的性能" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。随后Sasabe等继续采用嘧啶骨架陆续开发了B4PyPPM和B4PyMPM，B4PyPPM与B4PYMPM相比上方的苯环换成甲基，虽然其迁移率降低至10" }, { "name": "sup", "data": [ { "name": "text", "data": "-6" } ] }, { "name": "text", "data": "量级，但是LUMO能级被拉深至-3.4 eV，电子注入性能获得提升" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "39", "type": "bibr", "rid": "R39", "data": [ { "name": "text", "data": "39" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。而B4PyMPM则是将B3PyMPM中吡啶间位N的位置改到对位，其" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "能级为2.80 eV，而由于独特的分子间氢键相互作用，其电子迁移率也上升到了1×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-4" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "·V" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "·s" }, { "name": "sup", "data": [ { "name": "text", "data": "-1 [" }, { "name": "xref", "data": { "text": "40", "type": "bibr", "rid": "R40", "data": [ { "name": "text", "data": "40" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。该分子在后续研究中也展现了优异的性能，以器件结构为ITO/HATCN/TAPC/17%Ir（ppy）" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "-doped BCzTPA/50%Ir（ppy）" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "-doped CBP/B" }, { "name": "sub", "data": [ { "name": "text", "data": "4" } ] }, { "name": "text", "data": "PyPPM/Liq/Al，调控激子复合区域，绿光OLED开启电压甚至低至1.97 V" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "41", "type": "bibr", "rid": "R41", "data": [ { "name": "text", "data": "41" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "作者课题组一直以来也致力于基于吡啶的电子传输材料的开发，最早曾于2007年就报道了高热稳定性的吡唑并菲啰啉的ETM，其性能优于Alq" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "42", "type": "bibr", "rid": "R42", "data": [ { "name": "text", "data": "42" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。2009年，报道了基于四苯基硅核心外接吡啶的分子DPPS，由于Si元素减弱共轭，DPPS展现出较宽的HOMO-LUMO带隙和高达2.7 eV的三线态能级。虽然其电子迁移率较低，但是依赖其优异的空穴阻挡性能，依然在蓝色磷光OLED中实现了高效率和低启亮电压，这也使人们从此更加关注空穴阻挡能力的重要性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "43", "type": "bibr", "rid": "R43", "data": [ { "name": "text", "data": "43" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。由于DPPS中心的Si硅原子会导致较差的热稳定性，作者课题组于2011年采用苯环替代Si原子，得到超扭曲结构的ETM材料TemPPB，大的空间位阻抑制了电子的离域，使得该分子获得了高达3.2 eV的三线态能级；并且热稳定性也获得提升，在蓝色磷光器件中获得了高达24.5%的EQE" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "44", "type": "bibr", "rid": "R44", "data": [ { "name": "text", "data": "44" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。2012年报道了基于芴为核心、两侧外接三联吡啶的分子DTPF，两种基团的结合使该分子不仅具有优秀的电子传输性能，还能获得深蓝光的发光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "45", "type": "bibr", "rid": "R45", "data": [ { "name": "text", "data": "45" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。此后，作者课题组进一步利用高稳定性螺芴和电子注入传输性能优异的三联吡啶基团开发了一系列D-A-D型高性能电子传输材料，于2018年先后报道了22-TPSF和27-TPSF两个分子，得益于刚性扭转的螺芴核心带来优秀的稳定性，它们的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "均在190 ℃以上；并且与22-TPSF相比，由于27-TPSF独特的错位平行分子堆叠方式引入了更强的分子间氢键作用，获得了优秀的注入和传输性能，在绿色磷光器件中实现了EQE高达28.2%，以及 1 000 cd·m" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "下长达6 800 h的半衰寿命" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "17", "type": "bibr", "rid": "R17", "data": [ { "name": "text", "data": "17" } ] } }, { "name": "text", "data": ", " }, { "name": "xref", "data": { "text": "46", "type": "bibr", "rid": "R46", "data": [ { "name": "text", "data": "46" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。基于27-TPSF，于2019年报道了三联吡啶上外部N原子间位取代的27-mTPSF，使分子间氢键相互作用进一步增强，与27-TPSF相比获得了更强的电子注入和传输性能" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "47", "type": "bibr", "rid": "R47", "data": [ { "name": "text", "data": "47" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。进一步地，作者课题组也报道了基于对位取代的二吡啶苯环螺芴衍生物4-4PySF，发现与间位相比，对位吡啶能够进一步提升分子间相互作用，获得更好的热稳定性以及电子迁移率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "48", "type": "bibr", "rid": "R48", "data": [ { "name": "text", "data": "48" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。此外，利用大的空间位阻和增加吸电子基团数目可以提升分子的稳定性和电子传输能力，基于该思想设计的具有刚性十字交叉结构的4oTPSF展现出超过200 ℃的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "，并且其器件工作稳定性也获得了提升" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "49", "type": "bibr", "rid": "R49", "data": [ { "name": "text", "data": "49" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "以蒽为核心的分子由于共轭效应较强，容易获得较高的电子迁移率，但是通常" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "能量很低。清华大学段炼课题组曾报道了两种补偿方案，其一是通过平衡空穴迁移率防止激子在电子传输层一侧聚集导致被ETM三线态猝灭。他们基于该策略设计了高迁移率电子传输材料DPPyA" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "50", "type": "bibr", "rid": "R50", "data": [ { "name": "text", "data": "50" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，TOF法测试其电子迁移率高达1.5×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "·V" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "·s" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "，通过采用迁移率略低的空穴传输层，实现了优良的器件性能，采用ITO/HATCN/NPB/TCTA∶15% Ir（mppy）" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "/DIC-TRZ∶15%Ir（mppy）" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "/DPPyA/LiF/Al结构，以不到3 V的电压亮度就达到了10 000 cd·m" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "。其二是通过“空间屏蔽”作用，在蒽两侧接入具有高" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "的侧链基团，以增大发光层的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "激子与蒽核心的距离，避免较低的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "猝灭发光层中的激子；同时空间位阻基团也提升了分子的热稳定性，" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "达到了185 ℃。该策略设计的分子BPBiPA虽然" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "能量仅有1.82 eV，但也在绿色磷光器件中展现了优异的性能" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "51", "type": "bibr", "rid": "R51", "data": [ { "name": "text", "data": "51" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "为了实现高" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "与高电子迁移率之间的平衡，增强分子间和分子内的电子偶联作用是一个有效的策略。基于此，张其胜等于2022年报道了一系列基于螺芴双硫杂蒽（9,9′-spirobithioxanthene）骨架的分子，它们均具有宽带隙和大于2.7 eV的三线态能级，并且也拥有与大共轭类分子相当的电子迁移率。其中性能最佳的T3PySS在SCLC法中迁移率达到了2.1×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-4" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "·V" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "·s" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "，且在器件中也具有很好的工作稳定性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "除上述分子之外，还有很多采用其他吸电子基团的设计，例如咪唑、三嗪和磷氧键基团等。苯并咪唑具有较高的三线态能级，也是研究较早的一种吸电子基团（如TPBi），与TPBi相比，在中心苯环上接入氰基可以进一步拉低LUMO能级，提升其电子注入能力，以此设计的iTPBI-CN获得了热稳定性和器件性能的提升" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "52", "type": "bibr", "rid": "R52", "data": [ { "name": "text", "data": "52" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。磷氧化合物具有较强的吸电子特性，特别是其具有不扩展核心结构的共轭，可以保持核心结构的高三重态能量。TSPO1是基于四苯基硅烷和二苯基氧化亚膦的高三重态能ETM，其高达3.36 eV的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "和6.8 eV的HOMO阻挡了三重态激子猝灭和空穴泄漏。将TSPO1作为激子阻挡层应用于深蓝磷光OLED中，获得了25.1%的高外量子效率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "53", "type": "bibr", "rid": "R53", "data": [ { "name": "text", "data": "53" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。采用三嗪基团和磷氧键设计的PO-T2T具有较高的" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "和电子迁移率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "54", "type": "bibr", "rid": "R54", "data": [ { "name": "text", "data": "54" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，但其LUMO能级过深而容易产生激基复合物" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "55", "type": "bibr", "rid": "R55", "data": [ { "name": "text", "data": "55" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，并且大多的磷氧化合物的稳定性都较差，可能与磷氧双键的不稳定性有关。上述涉及的分子式见" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "，本文所涉及分子的能级图见" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "，所涉及分子的性能参数总结于" }, { "name": "xref", "data": { "text": "表1", "type": "table", "rid": "T1", "data": [ { "name": "text", "data": "表1" } ] } }, { "name": "text", "data": "中。" } ] }, { "name": "fig", "data": { "id": "F5", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图5" } ], "title": [ { "name": "text", "data": 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