Strongly Luminescent Cyclometalated Gold(III) Complexes Supported by Bidentate Ligands Displaying Intermolecular Interactions and Tunable Emission Energy

Chan Kaai Tung; Tong Glenna So Ming; Wan Qingyun; Cheng Gang; Yang Chen; Che Chi‐Ming

摘要

Abstract > A series of charge‐neutral Au III complexes, which comprise a dicarbanionic C‐deprotonated biphenyl ligand and bidentate ancillary ligands ([Au(C^C)(L^X)]; L^X=β‐diketonate and relatives (O^O), quinolinolate and relatives (N^O), and diphosphino (P^P) ligands), were prepared. All the complexes are emissive in degassed CH <sub>2</sub> Cl <sub>2</sub> solutions and in thin‐film samples with Φ <sub>em</sub> up to 18 and 35?%, respectively, except for 5 and 6 , which bear (N^O)‐type ancillary ligands. Variation of the electronic characteristics of the β‐diketonate ancillary ligand was demonstrated to be a viable route for tuning the emission color from blue‐green (peak λ <sub>em</sub> at ca. 466?nm for 1 and 2 ; 501?nm for 4?a and 4?b ) to orange (peak λ <sub>em</sub> at 585?nm for 3 ), in contrast to the common observations that the ancillary ligand has a negligible effect on the excited‐state energy of the Au III complexes reported in the literature. DFT/time‐dependent (TD) DFT calculations revealed that the energies of the 3 ππ*(C^C) and the 3 ILCT(O^O) excited states (ILCT=intraligand charge transfer) switch in order on going from O^O=acetylacetonate (acac) to aryl‐substituted β‐diketonate ligands. Solution‐processed and vacuum‐deposited organic light‐emitting diode (OLED) devices of selected complexes were prepared. The vacuum‐deposited OLED fabricated with 2 displays a sky‐blue emission with a maximum external quantum efficiency (EQE) of 6.71?% and CIE coordinates of (0.22, 0.40). The crystal structures of 7 and 9 reveal short intermolecular Au III ???Au III contacts, with intermetal distances of 3.408 and 3.453??, respectively. DFT/TDDFT calculations were performed on 7 and 9 to account for the noncovalent interactions. Solid samples of 1 , 3 , and 9 exhibit excimeric emission at room temperature, which is rarely reported in Au III complexes. </abstract> </span> <span class="z_kbtn z_kbtnclass hoverxs" style="display: none;">展开▼</span> </div> <div class="translation abstracttxt"> <span class="zhankaihshouqi fivelineshidden" id="abstract"> <span>机译：</span><Abstract XMLNS =“http://www.wiley.com/namespaces/wiley”type =“main”xml：lang =“en”> <标题类型=“main”>抽象</ title> > 一系列充电中性Au iii </ sup> 复合物，其包含DicarbanionIOc C-反驳的联苯基配体和二齿辅助配体（[Au（c 1℃）（l ^ x）]; l ^ x =β-二酮和亲属（O ^ O），喹啉酸盐和亲属（n制备^ O）和二磷基（P→P）配体）。所有复合物都在脱气的CH中发光 <sub> 2 </ sub> CL. <sub> 2 </ sub> 解决方案和薄膜样品 φ</ i> <sub> Em </ sub> 除了 5 </ b> 和 6 </ b> ，哪些熊（n ^ o）型辅助配体。 β-二通酸酯配套配体的电子特性的变化被证明是从蓝绿色调整发光颜色的可行途径（峰值 λ</ i> <sub> Em </ sub> 在加利福尼亚州。 466？nm for 1 </ b> 和 2 </ b> ; 501？nm for 4？a </ b> 和 4？b </ b> ）到橙色（峰值 λ</ i> <sub> Em </ sub> 在585？nm for 3 </ b> 相反，与辅助配体对Au的兴奋状态能量具有可忽略不计的常见观察结果相比 iii </ sup> 复合物在文献中报道。 DFT /时间依赖（TD）DFT计算透露了这种能量 3 </ sup> ΠΠ*（c ^ c）和 3 </ sup> ILCT（O ^ O）激发态（ILCT = Intraligand电荷转移）按顺序开关，从O ^ O =乙酰丙酮（ACAC）转移到芳基取代的β-二酮酸盐配体中。制备溶液处理和真空沉积的选定配合物的有机发光二极管（OLED）装置。真空沉积的OLED制造 2 </ b> 显示天蓝色发射，最大外部量子效率（EQE）为6.71Ω％和CIE坐标（0.22,0.40）。晶体结构 7 </ b> 和 9 </ b> 揭示短分子间Au iii </ sup> ??? au. iii </ sup> 触点，分别为3.408和3.453的内部间距。进行DFT / TDDFT计算 7 </ b> 和 9 </ b> 考虑非价相互作用。固体样品 1 </ b> 那 3 </ b> ，和 9 </ b> 在室温下表现出良好的发射，在Au中很少报道 iii </ sup> 复合物。 </ p> </摘要> </span> <span class="z_kbtn z_kbtnclass hoverxs" style="display: none;">展开▼</span> </div> </div> <div class="record"> <h2 class="all_title" id="enpatent33" >著录项</h2> <ul> <li> <span class="lefttit">来源</span> <div style="width: 86%;vertical-align: text-top;display: inline-block;"> <a href='/journal-foreign-16161/'>《Chemistry, an Asian journal》</a> <b style="margin: 0 2px;">|</b><span>2017年第16期</span><b style="margin: 0 2px;">|</b><span>共17页</span> </div> </li> <li> <div class="author"> <span class="lefttit">作者</span> <p id="fAuthorthree" class="threelineshidden zhankaihshouqi"> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Chan Kaai Tung&option=202" target="_blank" rel="nofollow">Chan Kaai Tung;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Tong Glenna So Ming&option=202" target="_blank" rel="nofollow">Tong Glenna So Ming;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Wan Qingyun&option=202" target="_blank" rel="nofollow">Wan Qingyun;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Cheng Gang&option=202" target="_blank" rel="nofollow">Cheng Gang;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Yang Chen&option=202" target="_blank" rel="nofollow">Yang Chen;</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=Che Chi‐Ming&option=202" target="_blank" rel="nofollow">Che Chi‐Ming;</a> </p> <span class="z_kbtnclass z_kbtnclassall hoverxs" id="zkzz" style="display: none;">展开▼</span> </div> </li> <li> <div style="display: flex;"> <span class="lefttit">作者单位</span> <div style="position: relative;margin-left: 3px;max-width: 639px;"> <div class="threelineshidden zhankaihshouqi" id="fOrgthree"> <p>State Key Laboratory of Synthetic ChemistryThe University of Hong KongPokfulam Road Hong Kong SAR China;</p> <p>State Key Laboratory of Synthetic ChemistryThe University of Hong KongPokfulam Road Hong Kong SAR China;</p> <p>State Key Laboratory of Synthetic ChemistryThe University of Hong KongPokfulam Road Hong Kong SAR China;</p> <p>State Key Laboratory of Synthetic ChemistryThe University of Hong KongPokfulam Road Hong Kong SAR China;</p> <p>State Key Laboratory of Synthetic ChemistryThe University of Hong KongPokfulam Road Hong Kong SAR China;</p> <p>State Key Laboratory of Synthetic ChemistryThe University of Hong KongPokfulam Road Hong Kong SAR China;</p> </div> <span class="z_kbtnclass z_kbtnclassall hoverxs" id="zhdw" style="display: none;">展开▼</span> </div> </div> </li> <li > <span class="lefttit">收录信息</span> <span style="width: 86%;vertical-align: text-top;display: inline-block;"></span> </li> <li> <span class="lefttit">原文格式</span> <span>PDF</span> </li> <li> <span class="lefttit">正文语种</span> <span>eng</span> </li> <li> <span class="lefttit">中图分类</span> <span><a href="https://www.zhangqiaokeyan.com/clc/159.html" title="化学">化学;</a></span> </li> <li class="antistop"> <span class="lefttit">关键词</span> <p style="width: 86%;vertical-align: text-top;"> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=gold&option=203" rel="nofollow">gold;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=luminescence&option=203" rel="nofollow">luminescence;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=noncovalent interactions&option=203" rel="nofollow">noncovalent interactions;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=organic light-emitting diodes&option=203" rel="nofollow">organic light-emitting diodes;</a> <a style="color: #3E7FEB;" href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=photophysics&option=203" rel="nofollow">photophysics;</a> </p> <div class="translation"> 机译：金;发光;非价相互作用;有机发光二极管;光学; </div> </li> </ul> </div> </div> <div class="literature cardcommon" id="literaturereference" style="display:none"> <div class="similarity "> <h3 class="all_title" id="enpatent111">引文网络</h3> <div class="referencetab clearfix"> <ul id="referencedaohang"> <li dataid="referenceul">参考文献</li> <li dataid="citationul">引证文献</li> <li dataid="commonreferenceul">共引文献</li> <li dataid="commoncitationul">同被引文献</li> <li dataid="tworeferenceul">二级参考文献</li> <li dataid="twocitationul">二级引证文献</li> </ul> </div> <div class="reference_details" id="referenceList"> <ul id="referenceul"></ul> <ul id="citationul"></ul> <ul id="commonreferenceul"></ul> <ul id="commoncitationul"></ul> <ul id="tworeferenceul"></ul> <ul id="twocitationul"></ul> 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王尧宇</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=王欣&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,王欣</a> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=史启祯&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor">,史启祯</a> <span> <a href="/conference-cn-31710/" target="_blank" rel="nofollow" class="tuijian_authcolor"> . 第四届全国配位化学会议 </a> <span> <span> . 2001</span> </span> </div> </li> <li> <div> <b>7. </b><a class="enjiyixqcontent" href="/academic-degree-domestic_mphd_thesis/020315787111.html">含氮杂环配体多齿配位基金属(Cu(I), Au(III))配合物的结构、发光机制和效率的量子化学研究</a> <b>[A] </b> <span> <a href="/search.html?doctypes=4_5_6_1-0_4-0_1_2_3_7_9&sertext=沈璐&option=202" target="_blank" rel="nofollow" class="tuijian_auth tuijian_authcolor"> . 沈璐</a> <span> . 2020</span> </span> </div> </li> </ul> <ul style="display: none;"> <li> <div> <b>1. </b><a class="enjiyixqcontent" 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