Research Progress of Thermally Activated Delayed Fluorescence Materials with Dual-emission Based on Donor-acceptor System Enhanced Publication

{ "defaultlang": "zh", "titlegroup": { "articletitle": [ { "lang": "zh", "data": [ { "name": "text", "data": "基于热活化延迟荧光双发射的有机电子给体-受体型材料研究进展" } ] }, { "lang": "en", "data": [ { "name": "text", "data": "Research Progress of Thermally Activated Delayed Fluorescence Materials with Dual-emission Based on Donor-acceptor System" } ] } ] }, "contribgroup": { "author": [ { "name": [ { "lang": "zh", "surname": "曹", "givenname": "云锋", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "CAO", "givenname": "Yun-feng", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [ "first-author" ], "bio": [ { "lang": "zh", "text": [ "曹云锋(1996-)，男，河北邯郸人，硕士研究生，2018年于河北科技师范学院获得学士学位，主要从事有机/高分子光功能材料的研究。 E-mail: CYF510776@163.com" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211021&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211023&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211026&type=" } ], "data": [ [ { "name": "text", "data": "曹云锋" }, { "name": "text", "data": "(1996-)，男，河北邯郸人，硕士研究生，2018年于河北科技师范学院获得学士学位，主要从事有机/高分子光功能材料的研究。 E-mail: " }, { "name": "text", "data": "CYF510776@163.com" } ] ] } ], "email": "CYF510776@163.com", "deceased": false }, { "name": [ { "lang": "zh", "surname": "李", "givenname": "旭萍", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "LI", "givenname": "Xu-ping", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [], "deceased": false }, { "name": [ { "lang": "zh", "surname": "卢", "givenname": "建军", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "LU", "givenname": "Jian-jun", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [ "corresp" ], "corresp": [ { "rid": "cor1", "lang": "zh", "text": "E-mail: lujianjunktz@tyut.edu.cn", "data": [ { "name": "text", "data": "E-mail: lujianjunktz@tyut.edu.cn" } ] } ], "bio": [ { "lang": "zh", "text": [ "卢建军(1970-)，男，山西太原人，博士，教授，2004年于太原理工大学获得博士学位，主要从事功能高分子材料、有机/高分子光功能材料、高性能纤维、产业用纺织品等方面的应用和研究。 E-mail: lujianjunktz@tyut.edu.cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211029&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211030&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211035&type=" } ], "data": [ [ { "name": "text", "data": "卢建军" }, { "name": "text", "data": "(1970-)，男，山西太原人，博士，教授，2004年于太原理工大学获得博士学位，主要从事功能高分子材料、有机/高分子光功能材料、高性能纤维、产业用纺织品等方面的应用和研究。 E-mail: " }, { "name": "text", "data": "lujianjunktz@tyut.edu.cn" } ] ] } ], "email": "lujianjunktz@tyut.edu.cn", "deceased": false } ], "aff": [ { "id": "aff1", "intro": [ { "lang": "zh", "label": "1", "text": "太原理工大学　省部共建煤基能源清洁高效利用国家重点实验室，山西 　 太原 　 030024", "data": [ { "name": "text", "data": "太原理工大学　省部共建煤基能源清洁高效利用国家重点实验室，山西 　 太原 　 030024" } ] }, { "lang": "en", "label": "1", "text": "State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China", "data": [ { "name": "text", "data": "State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China" } ] } ] } ] }, "abstracts": [ { "lang": "zh", "data": [ { "name": "p", "data": [ { "name": "text", "data": "基于热活化延迟荧光的双发射有机材料，由于具有两种颜色的发光波长，且至少有一种发射的衰减寿命在微秒级以上，因此在白色有机发光二极管、多功能探针与传感、高质量生物成像、防伪等领域具有很大的应用前景。为了合理地设计基于热活化延迟荧光的双发射有机电子给体-受体型材料，最为关键的是研究分子结构与光物理性质之间的构效关系。本文将基于热活化延迟荧光的双发射有机电子给体-受体型分子，根据其发光属性分为三类:热活化延迟荧光-荧光双发射、热活化延迟荧光-磷光双发射和双热活化延迟荧光发射，进一步对其分子设计原则、发光机制和最新进展做出了简要综述，并展望了其发展前景。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "The organic thermally activated delayed fluorescence materials with dual-emission characteristics have possessed great application in fields of white organic light emitting diodes, multifunction probes and sensors, high quality bioimagings, anti-counterfeiting and so on, owing to their different wavelengths and at least one long lifetime more than microseconds. Moreover, it is critical to study the structure-property relationships for designing thermally activated delayed fluorescence moleculars with dual-emission based on donor-acceptor system. In this paper, the thermally activated delayed fluorescence materials with dual-emission based on donor-acceptor system are divided into three categories according to their luminescent properties: thermally activated delayed fluorescence-fluorescence dual emission, thermally activated delayed fluorescence-phosphorescent dual emission and dual thermally activated delayed fluorescence emission. The molecular design principle, luminescence mechanism and the progress are reviewed, noting the remaining challenges and directions for future work." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "热活化延迟荧光" } ], [ { "name": "text", "data": "双发射" } ], [ { "name": "text", "data": "分子设计" } ], [ { "name": "text", "data": "发光机制" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "thermally activated delayed fluorescence" } ], [ { "name": "text", "data": "dual emission" } ], [ { "name": "text", "data": "molecular design" } ], [ { "name": "text", "data": "luminescence mechanism" } ] ] } ], "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": "当用紫外-可见光照射处于基态的分子时，分子的价电子从基态跃迁到激发态，而高能态的激子从激发态辐射到基态失活的过程中存在不同的自旋多重态。从最低激发单重态(S" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": ")辐射的光子称为荧光" }, { "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": "，其发光寿命≤10" }, { "name": "sup", "data": [ { "name": "text", "data": "-8" } ] }, { "name": "text", "data": " s；从最低激发三重态(T" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": ")辐射的光子称为磷光" }, { "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": "，其发光寿命一般大于荧光，且通常情况下磷光寿命在10" }, { "name": "sup", "data": [ { "name": "text", "data": "-6" } ] }, { "name": "text", "data": " s以上。当分子的单重态和三重态之间的能级差(Singlet-triplet energy splitting,Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": ")较小时，在外界热作用下，三重态激子通过反向系间窜越(Reversed intersystem crossing,RISC)过程转变为单重态激子，进而辐射到基态的光子，称为热活化延迟荧光(Thermally activated delayed fluorescence,TADF)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "3", "type": "bibr", "rid": "R3", "data": [ { "name": "text", "data": "3" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。TADF材料由于可以实现100%的内量子效率，且具有较长的发射寿命，在有机发光二极管(Organic light-emitting diodes,OLEDs)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "4", "type": "bibr", "rid": "R4", "data": [ { "name": "text", "data": "4" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "5", "type": "bibr", "rid": "R5", "data": [ { "name": "text", "data": "5" } ] } } ], "rid": [ "R4", "R5" ], "text": "4-5", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、荧光探针" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "6", "type": "bibr", "rid": "R6", "data": [ { "name": "text", "data": "6" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、生物成像" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "7", "type": "bibr", "rid": "R7", "data": [ { "name": "text", "data": "7" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "8", "type": "bibr", "rid": "R8", "data": [ { "name": "text", "data": "8" } ] } } ], "rid": [ "R7", "R8" ], "text": "7-8", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、三线态敏化" }, { "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": "、光催化剂" }, { "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": "等领域得到了广泛应用，是有机发光材料的研究热点之一。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "1961年，Parker和Hatchard" }, { "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": "报道了第一个纯有机TADF分子伊红染料。2011年，Adachi小组" }, { "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": "首次在π-共轭骨架中引入电子给体(Donor, D)和电子受体(Acceptor,A)设计纯有机TADF分子。由于有机电子给体-受体(Donor-Acceptor,D-A)型分子的最高占据轨道(Highest occupied molecular orbital,HOMO)和最低空置轨道(Lowest unoccupied molecular orbital,LUMO)分别位于给体和受体部分，前线轨道之间的重叠区域较小，产生较小的Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": "，从而保证激子进行有效的RISC过程；同时有机D-A分子具有较强的分子间或分子内电荷转移(Charge transfer,CT)特性，因此D-A骨架分子成为高效TADF材料的候选者之一。然而，根据Franck-Condon理论" }, { "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": "，要使化合物的发光效率较高，则HOMO和LUMO在空间上需具有一定重叠，这与TADF分子需具备较小的Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": "值这一条件矛盾。因此，在设计TADF分子时，需考虑合适的D和A单元来构建化合物结构，以同时满足材料对Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": "值和发光效率的要求。目前，有机TADF分子常用的给体单元是含N官能团，例如咔唑、二苯胺、吩噁嗪(Phenoxazine,PXZ)、吩噻嗪(Phenothiazine,PTZ)等及其衍生物；常用的受体单元有:氰基苯、二苯亚砜、苯甲酮、三嗪等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "14", "type": "bibr", "rid": "R14", "data": [ { "name": "text", "data": "14" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "15", "type": "bibr", "rid": "R15", "data": [ { "name": "text", "data": "15" } ] } } ], "rid": [ "R14", "R15" ], "text": "14-15", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "根据Kasha's规则，传统发光分子只能从最低单重态或最低三重态发射光子" }, { "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": "，产生一种波长的发射光。同样地，大多数TADF分子也只表现出单发射，从而限制了其在多色发光和多功能荧光探针中的深入应用。因此，研究人员设计开发了具有双发射特性的TADF单分子，即发光分子具有两种发射波长，发射之一为TADF，另一种发射为普通荧光、磷光或TADF。基于TADF的双发射材料由于具有两种颜色的发光波长且至少有一种发射的衰减寿命在微秒级以上，因此在白色有机发光二极管、比率型荧光探针与化学传感器和高质量生物成像等领域展现出独特的应用优势。本文主要对基于TADF的双发射有机D-A型分子的设计原则、发光机理和应用等方面进行了综述，并展望了其发展前景。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2　基于热活化延迟荧光的双发射" } ], "level": "1", "id": "s2" } }, { "name": "p", "data": [ { "name": "text", "data": "根据有机分子不同的发光属性，我们将基于TADF的双发射有机D-A型分子分为三类(如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "):TADF-荧光双发射、TADF-磷光双发射和双TADF发射。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "基于TADF的双发射" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.1" } ], "title": [ { "name": "text", "data": "TADF-based dual emission" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211039&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211046&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211042&type=" } ] } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.1　TADF -荧光双发射" } ], "level": "2", "id": "s2a" } }, { "name": "p", "data": [ { "name": "text", "data": "基于TADF的双发射中，TADF-荧光双发射是最常见的一种。这主要是因为化合物存在两种形式的最低单重态:第一种形式的最低单重态发射普通荧光；而第二种形式的最低单重态与三线态之间的Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": "值较小，可以实现有效的系间窜越(Intersystem crossing,ISC)和RISC过程，因此发射TADF，如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "所示。" } ] }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "TADF-荧光双发射示意图" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.2" } ], "title": [ { "name": "text", "data": "Schematic diagram of TADF-fluorescence dual emission" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211049&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211055&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211052&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "对于D-A构型的分子来说，给体和受体之间N—C键的自由旋转可能会导致构象异构性。基于PTZ给体的D-A化合物，由于PTZ分子中的C—N键和C—S键的键长不同，具有quasi-axial(A)和quasi-equatorial(E)两种构型。A构型是近平面结构，其电子云密度在整个分子中处于离域状态，单重态和三重态之间的Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": "值较大，表现出普通荧光发射；而E构型的D和A之间有较大扭转角，Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": "值较小，可以有效捕获三线态激子实现RISC过程，表现出TADF发射。因此，当化合物中同时存在A和E构型时，可以实现TADF-荧光双发射。2014年，Adachi小组" }, { "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": "以PTZ为D单元，2,4,6-三苯基-1,3,5-三嗪(TRZ)为A单元，制备了一个D-A结构的TADF分子PTZ-TRZ(化合物1)。由于PTZ的扭曲，PTZ-TRZ存在A和E两种构型，两种构型均表现出来自于分子内的CT发射，其Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": "值分别为1.14 eV和0.18 eV，因此A构型发射荧光，E构型发射TADF，基于该化合物的OLED器件的最大外量子效率(External quantum efficiency,EQE" }, { "name": "sub", "data": [ { "name": "text", "data": "max" } ] }, { "name": "text", "data": ")为10.8%。他们继续将受体TRZ与3个给体PTZ相连制备了TRZ 3(Ph-PTZ)(化合物2)，进一步将其制备成黄绿色OLED器件，外量子效率提高到17.4%" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "18", "type": "bibr", "rid": "R18", "data": [ { "name": "text", "data": "18" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "化合物1~4的结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "17", "type": "bibr", "rid": "R17", "data": [ { "name": "text", "data": "17" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } } ], "rid": [ "R17", "R18", "R19", "R20" ], "text": "17-20", "type": "bibr" } }, { "name": "text", "data": "]" } ] } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.3" } ], "title": [ { "name": "text", "data": "Structure of compound 1-4" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "17", "type": "bibr", "rid": "R17", "data": [ { "name": "text", "data": "17" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } } ], "rid": [ "R17", "R18", "R19", "R20" ], "text": "17-20", "type": "bibr" } }, { "name": "text", "data": "]" } ] } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211057&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211060&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211058&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "白光可以是蓝光和黄光的叠加，因此，双发射材料的发射颜色分别为蓝色和黄色时，具有构建白光OLED器件的潜能。张晓宏等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "19", "type": "bibr", "rid": "R19", "data": [ { "name": "text", "data": "19" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "的研究表明，当D-A分子中含有9,9-二甲基-9,10-二氢吖啶(DMAC)或PXZ等伪平面单元时，分子具有两种构型。当DMAC或PXZ呈平面构型时，D-A分子具有较大扭转角和较小Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": "值，表现出TADF性能；由于DMAC或PXZ的弯曲构型具有较小的空间位阻，因此它们呈弯曲构型时，相应D-A分子的共轭性得到延伸，抑制了TADF性能。他们于2018年报道的两个化合物PTZ-TTR(化合物3)和PTZ-Ph-TTR(化合物4)，均存在两种稳定的构型，近垂直构型发射TADF，而近平面构型发射普通荧光。基于PTZ-TTR的白色OLED器件，其CIE坐标为(0.33,0.33)，基于PTZ-Ph-TTR的白色OLED器件的EQE" }, { "name": "sub", "data": [ { "name": "text", "data": "max" } ] }, { "name": "text", "data": "为16.34%" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "实现TADF-荧光双发射的另一途径是构建三联型D" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "-D" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "-A小分子化合物，通过不同给体与同一受体之间的电荷转移形成两种CT激发态，从而表现出两种发射。周必泰团队" }, { "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": "以三苯胺为第一电子给体D" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "，咔唑为第二电子给体D" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "，二苯并噻吩砜(DBTO2)为A，制备了一种U-型的D" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "-D" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "-A化合物CTPS(化合物5)。CTPS表现出双发射，且两种发射波长均具有激发波长依赖性和溶剂极性依赖性，因此两种发射都来自于CT激发态。低能量的CT(S)态来自于D" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "→A的空间CT，高能量的CT(B)态来自于D" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "→A的化学键CT，且CT(S)激发态发射TADF。这种D-D-A型三联化合物的出现为多色发光打开了新的分子设计思路。" } ] }, { "name": "fig", "data": { "id": "F4", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图4" } ], "title": [ { "name": "text", "data": "化合物5~7的结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "21", "type": "bibr", "rid": "R21", "data": [ { "name": "text", "data": "21" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "23", "type": "bibr", "rid": "R23", "data": [ { "name": "text", "data": "23" } ] } } ], "rid": [ "R21", "R22", "R23" ], "text": "21-23", "type": "bibr" } }, { "name": "text", "data": "]" } ] } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.4" } ], "title": [ { "name": "text", "data": "Structure of compound 5-7" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "21", "type": "bibr", "rid": "R21", "data": [ { "name": "text", "data": "21" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "23", "type": "bibr", "rid": "R23", "data": [ { "name": "text", "data": "23" } ] } } ], "rid": [ "R21", "R22", "R23" ], "text": "21-23", "type": "bibr" } }, { "name": "text", "data": "]" } ] } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211062&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211068&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211065&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "由于在没有重金属元素参与的前提下，TADF材料可以同时捕获单重态和三重态激子，因此，开发基于TADF材料的OLED器件引起了研究者的广泛兴趣。但是，小分子TADF材料用于OLED器件时，存在热稳定性差、相分离等问题，容易引起器件的不稳定性。为了避免上述问题，近几年，很多研究者将目光转移到设计具有良好的热稳定性、可溶液加工及结构易修饰的TADF聚合物材料上。基于此，他们进一步设计具有双发射性能的聚合物用于构建白光OLED器件。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "北京化工大学任忠杰等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "22", "type": "bibr", "rid": "R22", "data": [ { "name": "text", "data": "22" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "首次提出了一种新的策略来设计具有暖白光性质的聚合物，该聚合物不仅具有荧光-TADF双发射性能，且具有聚集增强发射(AEE)的特性。他们设计的聚合物(化合物6)支链中含有不同比例的二苯并噻吩砜-吩噻嗪(PTZ-DBTO2)和二苯并噻吩(DBT)，其中 PTZ-DBTO2发射黄色TADF，而DBT不仅发射蓝色荧光，还可以作为主体材料分散PTZ-DBTO2，从而调节聚合物的发光颜色。当聚合物中DBT与PTZ-DBTO2的比例为82∶18时，聚合物在不同比例的四氢呋喃和水的混合溶液中的发射颜色从绿蓝色到白色或者黄色，聚合物分散在聚甲基丙烯酸甲酯(PMMA)中形成固态薄膜时发射白光。基于该聚合物的暖白光OLED器件的EQE" }, { "name": "sub", "data": [ { "name": "text", "data": "max" } ] }, { "name": "text", "data": "为10.4%,CIE坐标为(0.37,0.38)。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "他们继续以具有TADF性质的PTZ-DBTO2作为橙黄光发射单元、三苯胺衍生物(TPAs)作为主体材料和蓝光发射单元，合成了两种具有TADF-荧光双发射特性的聚合物" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "23", "type": "bibr", "rid": "R23", "data": [ { "name": "text", "data": "23" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ":PTDP-5(化合物7)和PTDP-10。同样地，小分子的发光性质很好地传递到聚合物中，并且，通过增加TPAs的含量，聚合物的发射颜色从PTDP-10的黄色变化为PTDP-5的白色。基于聚合物PTDP-10的OLED器件的EQE" }, { "name": "sub", "data": [ { "name": "text", "data": "max" } ] }, { "name": "text", "data": "为7.1%,CIE为(0.42,0.33)；而基于PTDP-5的OLED器件发射典型的暖白光，EQE" }, { "name": "sub", "data": [ { "name": "text", "data": "max" } ] }, { "name": "text", "data": "为4.8%,CIE坐标为(0.46,0.41)。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "综合以上分析可以看出，对于具有两种不同发光颜色的TADF-荧光双发射材料来说，最重要的用途之一是作为发射层材料构建白色OLED器件。相比于由若干个发光分子组成的体系，这类基于单分子层的双发射材料在用作器件时具有避免相分离、提高稳定性、降低器件构建难度等优势。然而，理想的白光OLED器件的外量子效率应达到100%，因此合理设计蓝/黄双发射单分子材料需要更深入地理解不同的双发射机制。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.2　TADF-磷光双发射" } ], "level": "2", "id": "s2b" } }, { "name": "p", "data": [ { "name": "text", "data": "不同于TADF-荧光双发射，TADF-磷光双发射的衰减寿命都是微秒级以上的长寿命。要实现TADF-磷光双发射，D-A分子需要同时满足两个条件" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "24", "type": "bibr", "rid": "R24", "data": [ { "name": "text", "data": "24" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ":(1)具有足够小的Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": "值，且局域激发三重态(" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "LE)和电荷转移激发三重态(" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "CT)之间具有自旋-振动耦合，以使RISC过程有效进行；(2)具有较大的自旋轨道耦合以产生磷光发射。总的来说，分子的最低三重态发射磷光，同时最低或高能级三重态激子通过RISC转移到S" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "态进行TADF发射，从而实现TADF-磷光双发射，机理如" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "所示。目前，在单分子态能够表现出TADF-磷光双发射的分子主要有以下4种类型。" } ] }, { "name": "fig", "data": { "id": "F5", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图5" } ], "title": [ { "name": "text", "data": "TADF-磷光双发射示意图" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.5" } ], "title": [ { "name": "text", "data": "Schematic diagram of TADF-phosphorescent dual emission" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211071&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211077&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211074&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "第一种，以PTZ的类似物PSeZ(用重原子Se代替PTZ结构中的S)为D单元的D-A化合物。Lee课题组" }, { "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": "以PSeZ为D单元，TRZ为A单元，制备了化合物PSeZTRZ(化合物8)，类似于PTZ具有A和E两种构型，化合物8也具有A和E两种构型。其A构型表现出荧光和磷光的双发射，而E构型表现出TADF-磷光双发射，机理如" }, { "name": "xref", "data": { "text": "图5(a)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(a)" } ] } }, { "name": "text", "data": "所示。这是因为化合物8的" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "LE能量低于" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "CT，因此熄灭了CT态，产生室温磷光。也就是说，当用重原子Se代替S后，同时加强了A和E构型的磷光发射，而对原来A构型的荧光发射和E构型的TADF影响很小。将具有TADF和磷光双发射的E构型化合物分散在3,3-二(咔唑基)联苯(mCBP)中制备薄膜，进一步构建器件，其发射光为黄绿色，外量子效率为17%，这说明引入的重原子并不会降低材料的发光效率。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "基于分子A和E构型导致化合物光物理性质多样性的研究结果，池振国课题组" }, { "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": "开发了一系列具有两种不同给体的不对称软发光物质。他们分别以吩噁嗪和吩噻嗪为给体与二苯砜受体相连构成不对称的给体-受体-给体化合物(化合物9)，相比于O原子取代的吩噁嗪，由较大S原子取代的吩噻嗪分子具有更大的灵活度，在应对刺激时沿N-S轴折叠而使整体分子具有不同的构象，而吩噁嗪保持平面结构。其不同的发色团可以在溶剂、热以及机械等不同的外界刺激下交替发挥作用，即选择性地表达出平面构象的吩噁嗪或折叠构象的吩噻嗪来实现TADF或RTP发射。由于其具有全色发光和动态发射的行为，作者将其用于挥发性有机化合物检测。" } ] }, { "name": "fig", "data": { "id": "F6", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图6" } ], "title": [ { "name": "text", "data": "化合物8~16的结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "25", "type": "bibr", "rid": "R25", "data": [ { "name": "text", "data": "25" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "30", "type": "bibr", "rid": "R30", "data": [ { "name": "text", "data": "30" } ] } } ], "rid": [ "R25", "R26", "R27", "R28", "R29", "R30" ], "text": "25-30", "type": "bibr" } }, { "name": "text", "data": "]" } ] } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.6" } ], "title": [ { "name": "text", "data": "Structure of compound 8-16" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "25", "type": "bibr", "rid": "R25", "data": [ { "name": "text", "data": "25" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "30", "type": "bibr", "rid": "R30", "data": [ { "name": "text", "data": "30" } ] } } ], "rid": [ "R25", "R26", "R27", "R28", "R29", "R30" ], "text": "25-30", "type": "bibr" } }, { "name": "text", "data": "]" } ] } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211081&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211087&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211084&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "第二种，以PTZ-DBTO2为A单元的D-A-D构型的化合物，通过改变D在A单元上的连接位置可以形成“线型”和“角型”区域异构体。Dias和Bryce等" }, { "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": "分别以咔唑和二苯胺衍生物为D单元，PTZ-DBTO2为A单元，合成了一系列D-A-D型化合物。相比于“线型”异构体，A单元呈“角型”被取代时(化合物10和11)，破坏了D-A-D化合物的共轭性，提高了单重态和三重态的能量；同时，减小了三线态之间的能级差，从而促进了化合物的ISC和RISC机制；另外，T" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "和T" }, { "name": "sub", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "text", "data": "之间的非绝热振动耦合使T" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "-T" }, { "name": "sub", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "text", "data": "快速达到平衡，从而激活“角型”异构体的TADF和磷光。因此，通过调节“角型”D-A-D化合物S" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "和T" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "之间以及T" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "和T" }, { "name": "sub", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "text", "data": "之间的能量，可以实现具有两种长寿命的TADF-磷光双发射。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "第三种，以咔唑为D单元、喹啉为A单元形成的D和A之间有特殊扭转角的咔唑-喹啉(CQ)偶联物。Ray小组" }, { "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": "制备了一系列CQ衍生物，发现CQ(化合物12)在室温下表现出TADF-磷光双发射。这是由于平面的咔唑基和喹啉之间有特殊的扭转角，使得高能级的三线态(T" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")和S" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "之间的能级差较小，可以进行有效RISC，从而发射TADF；同时，T" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "态和T" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "态的能量接近，从而使T" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "态发射室温磷光，机理如" }, { "name": "xref", "data": { "text": "图5(b)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(b)" } ] } }, { "name": "text", "data": "所示。当喹啉衍生物苯环上的2和4位被甲基、甲氧基和氰基取代时，增大了S" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "和T" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "之间的能级差，化合物辐射来自于S" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "态的荧光，因此CQ化合物中D单元和A单元特殊的扭转角是其呈现TADF-磷光双发射的主要原因。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "类似地，2019年，陈传峰课题组" }, { "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": "以咔唑为给体、酞酰亚胺为受体设计出一类具有D-N-A结构的化合物(N为酰胺基团上的N原子，化合物13)。其中，给体和受体位于邻位的化合物o-AI-Cz由于具有足够小的Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": "值和强的分子内相互作用而在薄膜和晶态下均呈现TADF和RTP性质，并且在室温下具有长达602 ms的寿命以及超过1 s的有机余辉。将其制成玫瑰花图案后，在紫外灯照射下其呈现蓝色荧光，而移除光源后又呈现绿色的磷光，这使得其可以作为安全油墨应用在有机防伪材料中。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "第四种，以具有磷光发射的分子作为D单元，且其与某一受体偶联后可以发射TADF的D-A-D化合物。2018年，Dias小组" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "30", "type": "bibr", "rid": "R30", "data": [ { "name": "text", "data": "30" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "设计制备了一系列具有TADF-磷光双发射的D-A-D构型的化合物(化合物14)，它们的D单元是二苯基亚胺，其具有长寿命的磷光发射性质" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "31", "type": "bibr", "rid": "R31", "data": [ { "name": "text", "data": "31" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ",A单元喹喔啉经常被用来设计TADF分子。研究发现，尽管Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ST" } ] }, { "name": "text", "data": "值较大，该系列化合物仍具有蓝色的TADF发射和橘黄色的室温磷光。而且，在D和A之间加入一个苯环(化合物15)以及用甲氧基取代二苯基亚胺(化合物16)后，其磷光寿命得到延长，这说明扭曲的二苯基亚胺可能是一个可以抑制非辐射跃迁的D单元。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "从上述分析可以看出， TADF-磷光双发射材料的两种发射光具有不同的衰减寿命，针对这一特征，同时将两种发射的波长和寿命作为检测参数以得到更为丰富的信息，从而应用在防伪、智能传感等领域。但由于同一分子的TADF和磷光往往是竞争关系，且磷光往往需要聚集体或晶体诱导，因此这对材料的形态有一定要求。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.3　双TADF发射" } ], "level": "2", "id": "s2c" } }, { "name": "p", "data": [ { "name": "text", "data": "以上设计具有TADF-荧光或TADF-磷光双发射的有机小分子的策略中，大多依赖于分子存在的异构体，且只有一种异构体表现出TADF-荧光或TADF-磷光双发射。因此，恰当地控制化合物中异构体的比例是调控TADF-荧光和TADF-磷光双发射的关键因素之一；另外，能够表现出双发射的异构化合物的种类有限。因此，基于化合物异构体实现双发射的方法存在一定缺陷和难度。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "鉴于此，中山大学池振国课题组提出设计不对称D-A-D'化合物，利用不同给体向同一受体的电子转移，形成两种独立的CT激发态体系，产生双发射。2015年，他们分别以咔唑和PTZ为给体，二苯砜为受体，制备了不对称D-A-D'化合物SFPC(化合物17)。其母体分子SF2C发射蓝色的TADF，但具有聚集诱导熄灭性质" }, { "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": "；另一个母体分子SF2C发射黄色的TADF，且具有聚集诱导增强效应" }, { "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": "。因此，化合物17在溶液中表现出双TADF发射，但是在聚集态只表现出一个TADF发射峰" }, { "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": "。他们继续选择O2C和O2P作为母体分子，合成了不对称D-A-D'化合物OPC(化合物18)，其在聚集态时表现出蓝色荧光和黄色TADF" }, { "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": "，类似地，化合物SCP(化合物19)在聚集态时也表现出蓝色荧光和黄色TADF" }, { "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": "。这些研究工作为设计白光OLED材料提供了新的思路。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "受到以上分子设计策略的启发，朱亮亮课题组" }, { "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": "以PTZ和吲哚乙酰胺为给体，二苯砜为受体，制备了不对称D-A-D'分子(化合物20)，该分子具有两种独立的CT激发态体系，D-A形成的 CT和D'-A形成的CT'，两种CT激发态体系中的CT" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "与 T" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "和CT'" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "与T'" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "的能级差都很小，因此可以发生有效的RISC过程，产生双TADF发射，具体的机理如" }, { "name": "xref", "data": { "text": "图7", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7" } ] } }, { "name": "text", "data": "所示。另外，化合物20在稀溶液和聚集态中都具有双TADF发射，减少了对氧气的敏感性。同时，两种TADF信号具有互补性，作者进一步将该分子应用于双通道细胞成像，通过两个通道成像信息的叠加，提高了成像信息的完整性，同时将成像失真率降低了30%~40%。该研究拓展了荧光探针在生物成像领域的应用，并为高质量生物成像提供了科学依据。" } ] }, { "name": "fig", "data": { "id": "F7", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图7" } ], "title": [ { "name": "text", "data": "双TADF发射示意图" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.7" } ], "title": [ { "name": "text", "data": "Schematic diagram of dual TADF launch" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211092&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211099&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211096&type=" } ] } }, { "name": "fig", "data": { "id": "F8", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图8" } ], "title": [ { "name": "text", "data": "化合物17~22的结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } } ], "rid": [ "R32", "R33", "R34", "R35", "R36", "R37" ], "text": "32-37", "type": "bibr" } }, { "name": "text", "data": "]" } ] } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.8" } ], "title": [ { "name": "text", "data": "Structure of compound 17-22" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } } ], "rid": [ "R32", "R33", "R34", "R35", "R36", "R37" ], "text": "32-37", "type": "bibr" } }, { "name": "text", "data": "]" } ] } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211102&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211110&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21211105&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "另外，2020年，李振声课题组" }, { "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": "通过合理的分子设计和聚集态调控实现了分子内TADF和分子间TADF/磷光双发射特性。他们以苯甲酰为受体，二苯并噻吩和咔唑(衍生物)为双给体，制备了不对称D-A-D'有机分子CTM(化合物21)和tCTM(化合物22)，两个分子在溶液中均表现出分子内的TADF性质，而其晶体结构表现出双发射特性。化合物21的晶体表现出TADF-磷光双发射；而化合物22表现出双重TADF，这主要是因为咔唑单元之间的强相互作用使得其聚集态表现出橙色磷光，而被两个叔丁基取代后的咔唑单元削弱了其π-π堆积，使化合物22在分子间呈现TADF发射。这项工作从分子结构的角度为纯有机TADF-磷光/TADF材料提供了新的思路。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "由以上分析可知，目前双TADF材料还比较少见，但基于单分子的双TADF材料往往具有较好的生物相容性。更重要的是，双TADF发射材料的两种发射波长可以提供两个检测通道，其不同的发射颜色以及寿命可以精准定位细胞的不同区域。因此，这将为比率探针、双通道成像等提供很多可能性，从而推动生物探针和成像的发展。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3　总结与展望" } ], "level": "1", "id": "s3" } }, { "name": "p", "data": [ { "name": "text", "data": "纯有机TADF材料的研究刚刚十年左右，在分子设计方面，尽管目前基本有一致的设计原则，即:设计D-A构型的分子，缩小单重态和三重态之间的能级差以实现有效的RISC过程，但仍需要优化D、A与桥联单元的选择方法以及三者的键接方式，以同时获得理想的发光寿命和荧光量子产率，进一步根据每类分子独特的物理性能，拓展其在OLED、智能探针与传感、生物成像、三线态敏化、光催化剂等前沿领域的应用。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本文将基于TADF的双发射材料分为TADF-荧光双发射、TADF-磷光双发射和双TADF发射三种。事实上，到目前为止，基于TADF双发射的有机材料非常有限，能够在单分子层实现基于TADF的双发射主要依赖于化合物的结构，而影响结构的关键因素有:D单元的构型、A单元的构型、D单元和A单元的桥联基团、D单元和A单元的键接方式、D单元和A单元的扭转角度等。因此，在设计基于TADF的双发射材料时，应从以上几个方面寻找突破口。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "发光材料的结构和光物理性质决定了其应用。尽管已经报道的双发射材料在高效率OLED器件、比率探针、时间分辨生物成像、加密/解密等方面有一些简单应用，但聚集诱导熄灭、发光不稳定、应用前的预处理复杂、短波长的发射对生物体造成损害等问题依然限制了其更精确和更深入的应用。因此，进一步设计具有聚集诱导发光性质、近红外光发光、双相发射性质(在单分子态和聚集态均具有TADF双发射)的TADF双发射分子，将会给新型有机发光分子的设计合成、结构调控、应用探索等方面带来新的突破。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "总之，对基于TADF的双发射材料的研究仍处于早期阶段，现有分子设计理论还有限，因此需要建立新的分子策略以及更加详细的机制理论来发展基于TADF的双发射材料以及探索其光物理过程。我们相信，由于基于TADF的双发射分子具有丰富且独特的光物理性质，基于TADF的双发射材料将推动更多领域的进一步发展。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本文专家审稿意见及作者回复内容的下载地址:http://cjl.lightpublishing.cn/thesisDetails#10.37188/CJL.20210181." } ] } ] } ], "footnote": [], "reflist": { "title": [ { "name": "text", "data": "参考文献:" } ], "data": [ { "id": "R1", "label": "[1]", 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