High-efficiency Perovskite Light-Emitting Diodes via Novel Cobalt-based Hole Transporter Layer

QIN Xiang-qian; LI Ming-liang; ZHAO Ya-ping; ZHANG Qin; WEI Zhan-hua

doi:10.37188/CJL.20220377

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High-efficiency Perovskite Light-Emitting Diodes via Novel Cobalt-based Hole Transporter Layer

Updated：2023-01-04

- High-efficiency Perovskite Light-Emitting Diodes via Novel Cobalt-based Hole Transporter Layer Enhanced Publication
- Chinese Journal of Luminescence Vol.null, Issue null, (2023)
- Affiliations：
  
  Institute of Luminescent Materials and Information Displays， College of Materials Science and Engineering， Huaqiao University,Xiamen,China,361021;Institute of Chemical Materials， China Academy of Engineering Physics,Chengdu,China,610200
- Author bio：
- Funds：
  
  National Natural Science Foundation of China(U21A2078;51902110;22179042;12104170);the Natural Science Foundation of Fujian Province(2020J06021;2019J01057;2020J01064);Scientific Research Funds of Huaqiao University;Subsidized Project for Postgraduate's Innovative Fund in Scientific Research of Huaqiao University
- DOI：10.37188/CJL.20220377 CLC：
- Published Online：04 January 2023，
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秦向前,黎明亮,赵亚萍等.新型钴基空穴传输层助力高效钙钛矿发光二极管[J].发光学报,

QIN Xiang-qian,LI Ming-liang,ZHAO Ya-ping,et al.High-efficiency Perovskite Light-Emitting Diodes via Novel Cobalt-based Hole Transporter Layer[J].Chinese Journal of Luminescence,
秦向前,黎明亮,赵亚萍等.新型钴基空穴传输层助力高效钙钛矿发光二极管[J].发光学报, DOI：10.37188/CJL.20220377

QIN Xiang-qian,LI Ming-liang,ZHAO Ya-ping,et al.High-efficiency Perovskite Light-Emitting Diodes via Novel Cobalt-based Hole Transporter Layer[J].Chinese Journal of Luminescence, DOI：10.37188/CJL.20220377

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"）薄膜具有优异的光电特性，所以选其作为绿光Pero-LEDs的HTL。然而，纯的钴基底薄膜存在传输载流子能力较差、薄膜粗糙度较大等问题，因此，本文通过引入有机小分子添加剂乙醇胺（ETA），来有效调控传输层中Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "/Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "比例，提升传输层的导电能力。同时，因ETA的加入可以减缓退火过程中前驱体溶液的析出结晶速度，从而形成粗糙度较小的HTL薄膜，进而有利于形成高质量的钙钛矿薄膜。基于掺杂的HTL，其最优器件亮度高达45207 cd/m" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "，最大外量子效率（EQE）达到了15.08%，是一种性能较好的新型HTL。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "In the device structure of metal halide perovskite light-emitting diodes （Pero-LEDs）， the hole transport layer （HTL） is one of the critical factors affecting the efficiency of Pero-LEDs. Because cobalt acetate （Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "） film has excellent photoelectric properties， it has been selected as the HTL for green Pero-LEDs. However， the pure cobalt-based HTL films have problems such as poor carrier transport ability and large film roughness. Therefore， in this paper， by introducing the organic small molecule additive ethanolamine （ETA）， the proportion of Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "/Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": " in the transport layer is effectively regulated， and the conductivity of the transport layer is improved. At the same time， the addition of ETA can slow down the crystallization process of HTL precursor solution during the annealing process， bringing in a transport layer film with lower roughness， which is conducive to the deposition of high-quality perovskite films. Based on the doped Co-based HTL films， the optimal device brightness reaches 45，207 cd/m" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "， and the maximum external quantum efficiency （EQE） reaches 15.08%， proving that the Co-based compound is a novel HTL with good device performance." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "钙钛矿发光二极管" } ], [ { "name": "text", "data": "醋酸钴" } ], [ { "name": "text", "data": "乙醇胺" } ], [ { "name": "text", "data": "空穴传输材料" } ], [ { "name": "text", "data": "掺杂" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "Perovskite LEDs" } ], [ { "name": "text", "data": "Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] } ], [ { "name": "text", "data": "Ethanolamine" } ], [ { "name": "text", "data": "Hole Transport Layer" } ], [ { "name": "text", "data": "Doping" } ] ] } ], "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": "近年来，金属卤化物钙钛矿材料在太阳能电池" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "1", "type": "bibr", "rid": "R1", "data": [ { "name": "text", "data": "1" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "3", "type": "bibr", "rid": "R3", "data": [ { "name": "text", "data": "3" } ] } } ], "rid": [ "R1", "R2", "R3" ], "text": "1-3", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、光电探测器" }, { "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": "6", "type": "bibr", "rid": "R6", "data": [ { "name": "text", "data": "6" } ] } } ], "rid": [ "R4", "R5", "R6" ], "text": "4-6", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、激光器" }, { "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": "9", "type": "bibr", "rid": "R9", "data": [ { "name": "text", "data": "9" } ] } } ], "rid": [ "R7", "R8", "R9" ], "text": "7-9", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "和光催化" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "11", "type": "bibr", "rid": "R11", "data": [ { "name": "text", "data": "11" } ] } } ], "rid": [ "R10", "R11" ], "text": "10-11", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "等领域受到了广泛的关注，并且也取得了巨大的研究成果。又因其具有的高缺陷容忍度、高载流子迁移率、带隙连续可调、发光半峰宽窄和光致发光效率高等优异性能" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "12", "type": "bibr", "rid": "R12", "data": [ { "name": "text", "data": "12" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "15", "type": "bibr", "rid": "R15", "data": [ { "name": "text", "data": "15" } ] } } ], "rid": [ "R12", "R13", "R14", "R15" ], "text": "12-15", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，被视为最有希望的下一代照明和显示材料之一。短短几年时间内，钙钛矿发光二极管（Perovskite Light-Emitting Diodes, Pero-LEDs）的性能得到了大幅度的提升，特别是绿光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "16", "type": "bibr", "rid": "R16", "data": [ { "name": "text", "data": "16" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } } ], "rid": [ "R16", "R17", "R18", "R19", "R20" ], "text": "16-20", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、红光" }, { "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": "22", "type": "bibr", "rid": "R22", "data": [ { "name": "text", "data": "22" } ] } } ], "rid": [ "R21", "R22" ], "text": "21-22", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "和近红外光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "23", "type": "bibr", "rid": "R23", "data": [ { "name": "text", "data": "23" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "24", "type": "bibr", "rid": "R24", "data": [ { "name": "text", "data": "24" } ] } } ], "rid": [ "R23", "R24" ], "text": "23-24", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "Pero-LEDs的外量子效率（External Quantum Efficiency, EQE）" }, { "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": "均超过了20%，相对落后的蓝光Pero-LEDs的EQE也超过了12%" }, { "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": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "目前，Pero-LEDs的结构一般为“三明治”结构，由阳极、空穴传输层、钙钛矿发光层、电子传输层和阴极构成。总体而言，要实现高效率器件，不仅需要有高质量的钙钛矿薄膜，也需要合适的载流子传输层去平衡传递到钙钛矿发光层中的电子和空穴，所以选择合适的传输层也是制备高效率器件的重要条件之一" }, { "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": "。在Pero-LEDs器件中常用的空穴传输材料类型主要包含有机物和无机物。其中常见的有机材料有PTAA" }, { "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": "和PEDOT:PSS" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "29", "type": "bibr", "rid": "R29", "data": [ { "name": "text", "data": "29" } ] } } ], "rid": [ "R28", "R29" ], "text": "28-29", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "等，其中PEDOT:PSS水溶液呈酸性，会腐蚀氧化铟锡（Indium Tin Oxide, ITO）电极，释放大量激子猝灭原子（铟和锡），降低器件稳定性；并且PEDOT:PSS的较强亲水特性，会导致器件易吸收空气中的水分，进一步地降低器件稳定性" }, { "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": "。而常见的无机空穴传输材料有：硫氰酸亚铜(CuSCN)" }, { "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": "、碘化亚铜(CuI)" }, { "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": "和氧化镍(NiO" }, { "name": "sub", "data": [ { "name": "text", "data": "x" } ] }, { "name": "text", "data": ")" }, { "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": "等。虽然它们具有高光透过率、高稳定性和较高的载流子迁移率，但是其制备过程复杂，通常需要经过高温退火或高温喷涂等方式进行制备，时间成本、材料资源损耗较大。因此，开发一种低温制备工艺、性能优异且稳定的空穴传输材料是至关重要的。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "这里，我们引入了一种可水溶液法制备的新型空穴传输材料Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "。水溶液旋涂法制备钴基底空穴传输层的过程较为简单，只需将其水溶液以3000 r/min转速旋涂后，使用150℃退火30 min，即可得到致密的Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底薄膜。然后，通过有机小分子乙醇胺（Ethanolamine, ETA）对Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "薄膜进一步掺杂，有效地调控了Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底薄膜中Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "/Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "的比例，提升传输层的导电能力；同时，ETA的引入还能够减缓前驱体溶液中的晶体析出速度，形成粗糙度较小的薄膜，有利于钙钛矿前驱体溶液的沉积，形成高质量的钙钛矿薄膜。最终，基于掺杂的HTL，得到了亮度高达45207 cd/m" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "以及最大EQE为15.08%的Pero-LEDs。本文证明了Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "是一种优异的新型空穴传输材料，为实现Pero-LEDs固态照明和全彩显示的应用，提供一种新的材料选择。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2　实　　验" } ], "level": "1", "id": "s2" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.1　实验药品" } ], "level": "2", "id": "s2a" } }, { "name": "p", "data": [ { "name": "text", "data": "四水醋酸钴（Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " • 4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O）购买于阿拉丁试剂有限公司。聚（3,4-乙烯基二氧噻吩）:聚苯乙烯磺酸钠（PEDOT:PSS，Clevious P VP.Al 4083）购买于贺力氏有限公司。甲胺基氢溴酸盐（MABr）和甲脒氢溴酸盐（FABr）购买于格瑞特赛尔太阳能材料有限公司。2,7-双二苯基膦基-9,9′-螺芴（SPPO13）购买于西安宝莱特电子科技有限公司。4,6-双（3,5-二吡啶-3-基）-2-甲基嘧啶（B3PYMPM）购买于机光科技股份有限公司。除上述化学品外，其他药品均购买于西格玛奥德里奇（上海）贸易有限公司。所有材料未进一步提纯，直接使用。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.2　实验合成及器件制备" } ], "level": "2", "id": "s2b" } }, { "name": "p", "data": [ { "name": "text", "data": "Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "•4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O前驱体溶液制备。先配制6 mg/mL Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "•4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O水溶液，然后在1 mL Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "•4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O水溶液加入x μL（x =0, 0.25, 0.5, 1）体积量的ETA溶液，配制成不同掺杂浓度的前驱溶液。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "•4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O前驱体溶液等比放大实验。首先，将玻璃基底加热到150℃。然后，同时将掺杂和未掺杂ETA分子的Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "•4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O前驱体溶液各滴加200 μL溶液到玻璃基底上，退火5 min。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "粉末的合成。首先，将PbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "（10 mmol, 3.665 g）溶解于15 mL HBr溶液中。然后CsBr（10 mmol, 2.13 g）溶解于5 mL去离子水中。将CsBr水溶液逐滴加入PbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "溶液中，生成橘色沉淀，继续搅拌30 min。然后，将搅拌后的溶液抽滤，所得沉淀用无水乙醇清洗4次。最后，放置于60℃的真空干燥箱中真空干燥24 h以上，转移至氮气手套箱中备用。钙钛矿前驱体溶液配制。将CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "粉末、MABr和FABr（摩尔比为1:0.8:0.2）溶解在3 mL DMSO的溶液中，形成浓度为0.5 mol/L CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "前驱体溶液，溶液在室温下连续搅拌搅拌24 h后，静置沉降待用。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "Pero-LEDs的制备。首先，将刻蚀过的ITO玻璃用玻璃清洗剂、丙酮、异丙醇和无水乙醇分别用超声波清洗机处理20 min，然后通过普通压缩氮气进行干燥，最后再进行5 min等离子清洗处理。Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " HTL的制备：将配制的Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "•4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O水溶液以静态旋涂的方式，涂覆在ITO玻璃基底上（转速为3000 r/min，旋涂时间为30 s），而后在150℃的热台上退火30 min，再转移至氮气手套箱内备用；将PEDOT:PSS水溶液以静态旋涂的方式，涂覆在ITO玻璃基底上（转速4000 r/min，旋涂时间为40 s），而后在150℃的热台上退火15 min，再转移至氮气手套箱内备用。钙钛矿发光层的制备：将30 μL钙钛矿前驱体溶液以2000 r/min转速、70 s旋涂时间，涂覆在Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底和PEDOT:PSS基底，以及后面不同浓度掺杂的HTL上。在28 s时滴加400 μL 氯苯溶液作为反溶剂，然后立即滴加2次30 μL PVDF-HFP溶液（3 mg/mL，溶解在丙酮溶液里），随后再立即滴加42 μL SPPO13溶液（3 mg/mL，溶解在丙酮溶液里）。最后，使用真空热蒸发系统在低于5×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-4" } ] }, { "name": "text", "data": " Pa的真空条件下，依次沉积厚度为~40 nm的B3PYMPM层、~1 nm的LiF层和~100 nm的Al金属电极。器件活性面积为3 mm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " (2 mm×1.5 mm)。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.3　实验表征仪器" } ], "level": "2", "id": "s2c" } }, { "name": "p", "data": [ { "name": "text", "data": "Pero-LEDs性能测试。本论文中所有LED性能的表征均在氮气手套箱内进行。数字源表Keithley 2450为器件提供电压，并且记录器件工作过程中电流、电压的变化。积分球（GPS-4P-SL）与光纤光谱仪QE-Pro的集成系统用于记录器件工作时的亮度变化和发光光谱。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "薄膜性能表征。钙钛矿层和HTL的表面形貌和粗糙度分别用JSM-7610F场发射扫描电子显微镜（Scanning Electron Microscope, SEM）和Bruker Multimode8原子力显微镜（Atomic Force Microsco-pe, AFM）进行表征。薄膜透过率（Transmittance, T）和光致发光光谱（Photoluminescence, PL）使用积分球(GPS-4P-SL)、THORLABS光源与光纤光谱仪QE-Pro的集成系统测试。接触角（Contact Angle, CA）测试使用JC2000D1接触角测量仪获得。薄膜厚度使用台阶仪（KLA－Tencor/D－600）获得。红外光谱使用傅里叶变换红外（Fouriertransform infrared spectroscopy, FTIR）光谱仪（NICOLET iS 50 FTIR spectrometer）的衰减全反射模式下获得。时间分辨光致发光（Time-resolved photoluminescence, TRPL）光谱使用全功能荧光光谱仪（Edinburgh FLS920）来测试，激发光为405 nm激光。X射线光电子能谱（X-ray Photoelectron Spectrum, XPS）和紫外光电子能谱（Ultraviolet Photoelectron Spectroscopy, UPS）使用光电子能谱仪（Thermofisher ESCALAB Xi+）获得。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3　结果与讨论" } ], "level": "1", "id": "s3" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.1　PEDOT：PSS薄膜与Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "薄膜的性能比较" } ], "level": "2", "id": "s3a" } }, { "name": "p", "data": [ { "name": "text", "data": "首先，为了探究PEDOT:PSS和Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底对钙钛矿前驱体溶液的浸润性，我们采用DMSO溶液作为探针溶剂进行HTL接触角测试。如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(a-b)所示，在Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底上的接触角（CA=34" }, { "name": "sup", "data": [ { "name": "text", "data": "o" } ] }, { "name": "text", "data": "）小于PEDOT:PSS基底（CA=40" }, { "name": "sup", "data": [ { "name": "text", "data": "o" } ] }, { "name": "text", "data": "），表明钙钛矿前驱体溶液在Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底上有更好的浸润性，说明了在Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "传输层上有利于钙钛矿前驱体溶液的沉积。对于HTL而言，其光透过率也是一个重要的参考数据，透过率的高低会直接影响器件最终的出光性能。如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(c)所示在500~1000 nm的波长范围内，Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底的光透过率远高于PEDOT:PSS基底；同时，在Pero-LEDs的中心波长（527 nm）下，前者的透过率比后者高4.7%，表明前者对该波长范围的寄生吸收更少，更有利于Pero-LEDs的出光。此外，如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(d-e)所示，我们通过台阶仪测得到PEDOT:PSS和Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底的薄膜厚度分别为55.8 nm和6.9 nm，这也说明了薄的Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底吸收更少、透过率更高。所以，薄膜接触角以及透过率测试表明Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底具有有更好的浸润性和更高的光透过率，更有利于钙钛矿薄膜的制备以及器件的出光。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "PEDOT：PSS与Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "薄膜DMSO接触角（a-b），光透过率（c），厚度（d-e）；钙钛矿的PL曲线（f），TRPL曲线（g）；PEDOT：PSS与Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "薄膜的" }, { "name": "italic", "data": [ { "name": "text", "data": "I-V" } ] }, { "name": "text", "data": "曲线（h）（测试结构：ITO/HTL/Au），单载流子器件的" }, { "name": "italic", "data": [ { "name": "text", "data": "J-V" } ] }, { "name": "text", "data": "曲线（i）（单空穴器件结构：ITO/HTL/Perovskite/Au，单电子器件结构：ITO/B3PYMPM/Perovskite/B3PYMPM/LiF/Al）；Pero-LEDs的" }, { "name": "italic", "data": [ { "name": "text", "data": "L" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "曲线（j），" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "曲线（k），EQE-" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "曲线（l）。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.1" } ], "title": [ { "name": "text", "data": "DMSO contact angle （a-b）， Optical transmittance （c） and Thickness curves （d-e） of PEDOT：PSS and Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " films. PL （f）， TRPL curves （g） of perovskite films on PEDOT：PSS and Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " substrates. " }, { "name": "italic", "data": [ { "name": "text", "data": "I-V" } ] }, { "name": "text", "data": " curve （h）（test structure： ITO/HTL/Au）， " }, { "name": "italic", "data": [ { "name": "text", "data": "J-V" } ] }, { "name": "text", "data": " curve （i） of single carrier device of PEDOT：PSS and Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " film （single hole device structure： ITO/HTL/perovskite/Au， single electron device structure： ITO/B3PYMPM/Perovskite/B3PYMPM/LiF/Al）； " }, { "name": "italic", "data": [ { "name": "text", "data": "L-V" } ] }, { "name": "text", "data": " curve （j）， " }, { "name": "italic", "data": [ { "name": "text", "data": "J-V" } ] }, { "name": "text", "data": " curve （k）， EQE-" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": " curve （l） of Pero-LEDs." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275361&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275372&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275366&type=", "width": "162.79998779", "height": "106.20449829", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "为了进一步探究在两种基底上沉积的钙钛矿薄膜的光致发光性能，我们对两种薄膜进行了PL和TRPL的测试。如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(f)所示，相比于沉积在PEDOT:PSS基底上的钙钛矿薄膜来说，沉积在Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底上的钙钛矿薄膜的PL强度更高，表明沉积在Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底上的钙钛矿薄膜具有更高的结晶质量，更少的缺陷。TRPL测试也证明了这一点，如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(g)所示，在Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底上沉积的钙钛矿薄膜可以显著延长PL寿命(" }, { "name": "xref", "data": { "text": "表1", "type": "table", "rid": "T1", "data": [ { "name": "text", "data": "表1" } ] } }, { "name": "text", "data": "为具体的拟合数据)。其中，Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底上的钙钛矿薄膜（" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ave" } ] }, { "name": "text", "data": "=299 ns）表现出比PEDOT:PSS基底上的薄膜（" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ave" } ] }, { "name": "text", "data": "=113 ns）更长寿命，这表明Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底能有效减少钙钛矿前驱体溶液沉积时非辐射缺陷的生成，形成质量更高的薄膜。紧接着，我们针对两种基底的导电性进行了探索，按照实验部分的方法制备的两种基底，直接镀上金属电极测试其导电性。从" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(h)中我们可以看出，在相同的电压下，Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底的电流大于PEDOT:PSS基底，从而证实了Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底具有更强的导电性，更有助于空穴的注入。接下来，我们又通过制备单载流子器件来探索电子空穴注入的平衡，如图(i)所示，在较高电压下，Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底的载流子器件中电子和空穴注入更加平衡。基于以上的数据结果，我们可以发现Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底上的钙钛矿薄膜具有更好的光电特性，所以我们尝试制备了基于两种基底的Pero-LEDs去进一步评估器件性能。如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(j-k)所示，不同基底器件的" }, { "name": "italic", "data": [ { "name": "text", "data": "L-V" } ] }, { "name": "text", "data": "和" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "曲线表明Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底空穴传输层制备的Pero-LEDs具有更大电流密度和更高亮度。其中，" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "曲线表明基于两种基底的器件电流密度相差较大（在7 V下的Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "和PEDOT:PSS基底的器件流密度分别为188.79和20.26 mA/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "），表明Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底比PEDOT:PSS基底具有更强的导电性，更利于空穴的传输。" }, { "name": "italic", "data": [ { "name": "text", "data": "L" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "曲线显示，在Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底上制备的Pero-LEDs在6.5 V下的亮度为36490 cd/m" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "，是基于PEDOT:PSS基底器件亮度（1766 cd/m" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "）的20.7倍，主要是由于Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底有强的导电性和在该基底上沉积的钙钛矿薄膜缺陷复合中心减少，从而增加了器件中的辐射效率。相对于PEDOT:PSS基底的Pero-LEDs来说，基于Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底的Pero-LEDs在高亮度下存在高的EQE值，如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(l)所示，Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底制备的Pero-LEDs最大EQE为12.48%，大于PEDOT:PSS基底制备的器件效率（EQE=4.12%），表明Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底制备的Pero-LEDs性能更好。根据以上的数据表明，Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "薄膜比PEDOT:PSS薄膜更适合作为Pero-LEDs的HTL。" } ] }, { "name": "table", "data": { "id": "T1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "表1" } ], "title": [ { "name": "text", "data": "PEDOT：PSS与Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底上钙钛矿薄膜的TRPL数据" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Tab.1" } ], "title": [ { "name": "text", "data": "TRPL data of perovskite film on PEDOT：PSS and Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " substrates" } ] } ], "note": [], "table": [ { "head": [ [ { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "Substrates" } ] } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "A" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] } ] } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "（ns）" } ] } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "A" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] } ] } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "（ns）" } ] } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "A" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] } ] } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "（ns）" } ] } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "ave" } ] }, { "name": "text", "data": "（ns）" } ] } ] } ] ], "body": [ [ { "align": "center", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "PEDOT：PSS" } ] } ] }, { "align": "center", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "0.46" } ] } ] }, { "align": "center", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "3.89" } ] } ] }, { "align": "center", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "0.31" } ] } ] }, { "align": "center", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "35.11" } ] } ] }, { "align": "center", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "0.24" } ] } ] }, { "align": "center", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "144.50" } ] } ] }, { "align": "center", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "113" } ] } ] } ], [ { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] } ] } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "0.48" } ] } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "3.98" } ] } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "0.32" } ] } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "50.38" } ] } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "0.18" } ] } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "369.73" } ] } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "299" } ] } ] } ] ], "foot": [] } ], "graphics": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275380&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275378&type=", "width": "77.69584656", "height": "17.84652710", "fontsize": "" } } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.2　ETA掺杂Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " HTL" } ], "level": "2", "id": "s3b" } }, { "name": "p", "data": [ { "name": "text", "data": "通过以上对比，我们选择了性能更好的Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "作为Pero-LEDs的HTL，然而该传输层还存在着传输性能较差、薄膜表面粗糙和浸润性较低等不足。所以，我们通过ETA有机小分子对以上传输层的不足进行修饰，制备高质量的传输层薄膜。首先，我们将不同体积浓度ETA（x μL/mL, x=0, 0.25, 0.5, 1；当x=0 μL/mL时，为Control薄膜）加入Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2 " } ] }, { "name": "text", "data": "• 4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O前驱体溶液中，通过旋涂和低温退火，制备Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底HTL（如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "(a)）。如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "(b)所示，为了探究小分子添加剂ETA对Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " • 4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O前驱体溶液成膜后的影响，我们利用FTIR测试证明了ETA有机小分子与钴离子存在相互作用。在纯的ETA分子红外光谱中N-H键伸缩振动和变形振动所引起的红外峰分别为3318 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "和1657 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "。又由于ETA分子溶于Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " • 4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O前驱体溶液中会发生络合反应生成胺络合物，所以Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2 " } ] }, { "name": "text", "data": "+ ETA薄膜中红外光谱N-H键伸缩振动和变形振动形成的红外峰向低波数移动，分别为3243 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "和1630 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "（a）不同体积浓度ETA掺杂Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " • 4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O前驱体溶液制备Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底HTL；（b） Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "、Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " + ETA和ETA的傅里叶变换红外光谱；不同体积浓度ETA掺杂HTL的DMSO接触角0.25 μL/mL （c），0.5 μL/mL （d），1 μL/mL （e）（插图为相应掺杂浓度的Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " • 4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O前驱体溶液实物图）。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.2" } ], "title": [ { "name": "text", "data": "（a） Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " HTL prepared by ETA-doped Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " • 4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O precursor solution with different volume concentrations. （b） FTIR of Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "， Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " + ETA and ETA. DMSO contact angle of ETA-doped HTL with different volume concentrations 0.25 μL/mL （c）， 0.5 μL/mL （d）， 1 μL/mL （e）（the inset is the physical image of the corresponding doped concentration of Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " • 4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O precursor solution）." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275385&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275398&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275392&type=", "width": "86.54220581", "height": "107.44433594", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "为了更近一步探究ETA分子对Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底薄膜表面性质的影响，我们继续使用DMSO溶液作为测试接触角的探针溶剂。从" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(b)和" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "(c-e)可以看出，Control薄膜的DMSO接触角最大（CA=40.0" }, { "name": "sup", "data": [ { "name": "text", "data": "o" } ] }, { "name": "text", "data": "）。随着不同体积浓度ETA分子的加入，各HTL薄膜的接触角均变小，特别是掺杂体积浓度为0.25 μL/mL时，其接触角达到最小（CA=22.5" }, { "name": "sup", "data": [ { "name": "text", "data": "o" } ] }, { "name": "text", "data": "）。相比于Control薄膜来说，掺杂薄膜的接触角的减小，表明ETA分子的加入会改变Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底薄膜的浸润性，从而利于钙钛矿薄膜的沉积。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "此外，HTL薄膜粗糙度也是影响沉积钙钛矿发光层的一个重要参数。从" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "(a-d)所示，Control的薄膜表面粗糙度最大，RMS为4.75 nm。但随着不同体积浓度的ETA分子的加入，能有效地降低HTL薄膜的粗糙度。并且在掺杂浓度为0.25 μL/mL的条件下，薄膜的粗糙度降至最小（RMS=3.90 nm），这表明ETA分子改善了HTL薄膜表面形貌，使HTL薄膜更加平整。由于HTL是通过溶液旋涂法直接制备，所以在退火过程中是无法观察到ETA分子是如何影响HTL的形成过程。在此，我们通过采取一个等比放大实验去证明ETA分子在退火过程中起到的具体作用。从Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "来起传递作用。而从" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "(b-d)中可以看出，当加入ETA分子，在HTL中会有Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "出现，主要原因是ETA分子溶于Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " • 4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O前驱体溶液中会与Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "发生络合反应生成钴胺络合物，此时Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "发生sp" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "d" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "杂化轨道，使得其3d高能级轨道中存在一个未配对电子，不稳定，则Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "容易被氧化成Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "。而Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "在与ETA分子络合时发生d" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "sp" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "杂化轨道，形成的结构相对稳定。所以，在空气环境下制备HTL，氧气易于将钴胺络合物中的Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "氧化为Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "，从而增加了HTL中Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "离子的含量。而当掺杂浓度为0.25 μL/mL时，其Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "与Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "峰面积比达到最大（Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "/Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "=0.9596），意味着Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "在HTL的占比量增加，提升了HTL传递空穴的能力。为了验证这一实验结果，我们将不同掺杂ETA浓度的HTL进行导电性测试，根据" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "(e)所示，能直观地表明ETA的加入能改Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "的导电性，提升空穴传输的能力。接下来，通过制备单载流子器件来探索载流子注入的真实情况，如" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "(f)所示，掺杂ETA的HTL注入空穴能力加强的结论再一次得到验证，而电子注入量与空穴注入量相比相差较大。最终，数据表明掺杂ETA分子有利于调控HTL中Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "/Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "比例，提高HTL的导电能力。" } ] }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "不同体积浓度ETA掺杂HTLs的AFM图Control （a），0.25 μL/mL （b），0.5 μL/mL （c），1 μL/mL （d）；（e）掺杂与未掺杂ETA的Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " • 4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O前驱体溶液的退火过程。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.3" } ], "title": [ { "name": "text", "data": "AFM images of ETA-doped HTLs with different volume concentrations Control （a）， 0.25 μL/mL （b）， 0.5 μL/mL （c）， 1 μL/mL （d）. （e） Annealing process of Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " • 4H" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "O precursor solutions doped and undoped with ETA." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275404&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275412&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275408&type=", "width": "73.99500275", "height": "77.59300232", "fontsize": "" } ] } }, { "name": "fig", "data": { "id": "F4", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图4" } ], "title": [ { "name": "text", "data": "不同体积浓度ETA掺杂HTLs Co 2p的XPS曲线 Control （a），0.25 μL/mL （b），0.5 μL/mL （c），1 μL/mL （d）；不同体积浓度ETA掺杂HTL的" }, { "name": "italic", "data": [ { "name": "text", "data": "I-V" } ] }, { "name": "text", "data": "曲线（e），单载流子器件的" }, { "name": "italic", "data": [ { "name": "text", "data": "J-V" } ] }, { "name": "text", "data": "曲线（f）。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.4" } ], "title": [ { "name": "text", "data": "XPS curves of Co 2p of ETA-doped HTLs doped with different volume concentrations Control （a）， 0.25 μL/mL （b）， 0.5 μL/mL （c）， 1 μL/mL （d）. " }, { "name": "italic", "data": [ { "name": "text", "data": "I-V" } ] }, { "name": "text", "data": " curve （e）， " }, { "name": "italic", "data": [ { "name": "text", "data": "J-V" } ] }, { "name": "text", "data": " curve （f） of single carrier device of ETA-doped HTL doped with different volume concentrations." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275418&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275426&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275423&type=", "width": "77.69583130", "height": "93.78122711", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "基于对HTL的实验探究，我们得到了一个粗糙度较小、载流子传输性能较高的HTL薄膜。因此，我们继续探究不同体积浓度ETA掺杂HTL对钙钛矿薄膜表面形貌的影响。如" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "(a, e)所示，根据SEM数据，我们了解到Control薄膜最为粗糙，且表面存在较多的孔洞和不同大小的钙钛矿晶粒，使整个薄膜表面凹凸不平。为了进一步了解钙钛矿薄膜的粗糙度，我们对钙钛矿薄膜进行AFM测试，结果表明Control薄膜粗糙度最大，其RMS=24.6 nm。而" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "(b-d)所示，在不同掺杂体积浓度的HTL上，钙钛矿薄膜的粗糙度降低，特别是掺杂体积浓度为0.25 μL/mL的条件下，钙钛矿薄膜的粗糙度降低到最小（RMS=19.3 nm），表明在粗糙度较小的HTL上沉积出粗糙度较小钙钛矿薄膜。如" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "(e-h)所示，相比于Control薄膜的表面形貌，在掺杂ETA分子的HTL上沉积的钙钛矿薄膜孔洞减少。而在不同掺杂浓度条件下，钙钛矿薄膜形貌差异较大。在0.25 μL/mL的掺杂浓度下，钙钛矿薄膜呈现出最优的状态，钙钛矿晶粒较小且致密。随着掺杂浓度增加到1 μL/mL时，钙钛矿晶粒增大，薄膜的致密度降低。而在0.5 μL/mL的掺杂浓度时，钙钛矿薄膜处于过渡态，存在大晶粒和小晶粒的混合状态。总之，通过SEM和AFM两种表征数据，我们明确了在0.25 μL/mL的掺杂浓度下，钙钛矿薄膜的粗糙度较小，钙钛矿晶粒生长致密，更加证实了HTL对沉积钙钛矿薄膜的巨大影响。" } ] }, { "name": "fig", "data": { "id": "F5", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图5" } ], "title": [ { "name": "text", "data": "不同体积浓度ETA掺杂HTLs上钙钛矿薄膜的AFM图和SEM图Control （a， e），0.25 μL/mL （b， f），0.5 μL/mL （c， g），1 μL/mL （d， h）。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.5" } ], "title": [ { "name": "text", "data": "AFM and SEM images of perovskite films on HTLs with different volume concentrations of ETA Control （a， e）， 0.25 μL/mL （b， f）， 0.5 μL/mL （c， g）， 1 μL/mL （d， h）." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275432&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275439&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275435&type=", "width": "160.83099365", "height": "72.77799988", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "基于以上的数据结果，我们通过ETA分子掺杂Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底去改变钙钛矿薄膜的结晶形貌，得到致密的高质量钙钛矿薄膜。接下来，我们进一步探究了高质量钙钛矿薄膜的光电性能。首先，对钙钛矿薄膜进行PL测试，如" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "(a)中，清晰地展示了各浓度掺杂Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底上钙钛矿薄膜PL曲线。相较于Control薄膜而言，ETA分子的加入，增强了薄膜的PL强度，并且在掺杂浓度为0.25 μL/mL时，其PL强度增加到最大，但随着掺杂浓度的增加，薄膜的PL强度略微减小，但强度依旧高于Control薄膜，说明ETA分子的加入有提高钙钛矿薄膜质量的作用，使钙钛矿前驱体溶液在HTL上形成缺陷较少的钙钛矿薄膜。薄膜缺陷的减少，表明载流子在薄膜中的辐射复合量会增加。TRPL测试结果也印证了这样结论。如" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "(b)所示，ETA分子的加入能使钙钛矿薄膜平均寿命增长（掺杂浓度0.25 μL/mL、0.5 μL/mL和1 μL/mL ETA的样品薄膜平均寿命分别为421 ns、356 ns和324 ns，大于Control薄膜的平均寿命时间250 ns，如" }, { "name": "xref", "data": { "text": "表2", "type": "table", "rid": "T2", "data": [ { "name": "text", "data": "表2" } ] } }, { "name": "text", "data": "所示），表明ETA分子能降低载流子在钙钛矿薄膜上的非辐射复合，提升钙钛矿薄膜的成膜质量，使载流子平均寿命延长。我们一般使用三指数函数公式i=A" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "exp(-t/" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": ")+A" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "exp(-t/" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")+A" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "exp(-t/" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": ")拟合TRPL数据，其中" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "、" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "分别表示非辐射复合过程中缺陷捕获和俄歇复合，" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "则表示辐射复合过程中电子空穴对复合过程" }, { "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": "。TRPL测试结果与钙钛矿薄膜PL曲线数据的结论相吻合，证实ETA分子可以促进缺陷较少的钙钛矿薄膜生成。同时，我们采用空间电荷限制电流（Space Charge Limited Current, SCLC）方法对钙钛矿薄膜中的缺陷态密度进行估算，根据" }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "trap" } ] }, { "name": "text", "data": "的计算" }, { "name": "xref", "data": { "text": "公式（1）", "type": "disp-formula", "rid": "DF1", "data": [ { "name": "text", "data": "公式（1）" } ] } }, { "name": "text", "data": "：" } ] }, { "name": "fig", "data": { "id": "F6", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图6" } ], "title": [ { "name": "text", "data": "不同浓度ETA掺杂HTLs上钙钛矿薄膜的PL曲线（a），TRPL曲线（b）；（c）利用SCLC方法评估钙钛矿薄膜的缺陷态密度（器件结构：ITO/Co-based HTL/Perovskite/Au）；（d） Pero-LEDs器件结构示意图；Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " （e）和Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "+ETA （f）（最优掺杂浓度0.25 μL/mL ETA）的UPS曲线；不同浓度ETA掺杂HTL的Pero-LEDs的" }, { "name": "italic", "data": [ { "name": "text", "data": "J-V-L" } ] }, { "name": "text", "data": "曲线（g），EQE-" }, { "name": "italic", "data": [ { "name": "text", "data": "L " } ] }, { "name": "text", "data": "（h）（插图为0.25 μL/mL ETA掺杂HTL的Pero-LEDs器件在不同电压下的EL光谱），寿命测量结果曲线（i）。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.6" } ], "title": [ { "name": "text", "data": "PL curves （a）， TRPL curves （b） of perovskite films on HTLs doped with different concentrations of ETA. （c） Evaluation of the defect state density of perovskite films by SCLC method （Device structure： ITO/Co-based HTL/Perovskite/Au）. （d） Schematic diagram of the device structure of Pero-LEDs. Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " （e）， Co（OAc）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "+ETA （f） of UPS curves （optimal doping concentration 0.25 μL/mL ETA）. " }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "L " } ] }, { "name": "text", "data": "（g）， EQE-" }, { "name": "italic", "data": [ { "name": "text", "data": "L" } ] }, { "name": "text", "data": " curves （h）， Lifetime measurement result （i） of Pero-LEDs of HTLs doped with different concentrations of ETA （the inset is the EL spectrum of the device at different voltages）." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275442&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275454&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275449&type=", "width": "150.51026917", "height": "128.68025208", "fontsize": "" } ] } }, { "name": "table", "data": { "id": "T2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "表2" } ], "title": [ { "name": "text", "data": "不同浓度ETA掺杂HTLs上钙钛矿薄膜的TRPL数据" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Tab.2" } ], "title": [ { "name": "text", "data": "TRPL data of perovskite films on ETA-doped HTLs with different concentrations" } ] } ], "note": [], "table": [ { "head": [ [ { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "μL/mL" } ] } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "text", "data": "A" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] } ] } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "bold", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { 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N_{t r a p} = \frac{2 ε ε_{0} V_{T F L}}{e L^{2}}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275474&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=38275469&type=", "width": "23.45266724", "height": "7.61999989", "fontsize": "" } } }, { "name": "text", "data": "，" } ], "id": "DF1" } }, { "name": "p", "data": [ { "name": "text", "data": "可以看出" }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "trap" } ] }, { "name": "text", "data": "与" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "TFL" } ] }, { "name": "text", "data": "的大小成正比(其中，" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "TFL" } ] }, { "name": "text", "data": "表示缺陷极限填充电压，" }, { "name": "italic", "data": [ { "name": "text", "data": "ε" } ] }, { "name": "text", "data": "表示介电常数，" }, { "name": "italic", "data": [ { "name": "text", "data": "ε" }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] } ] }, { "name": "text", "data": "表示真空介电常数，" }, { "name": "italic", "data": [ { "name": "text", "data": "L" } ] }, { "name": "text", "data": "表示薄膜厚度，" }, { "name": "italic", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "表示电子电荷量常数)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "18", "type": "bibr", "rid": "R18", "data": [ { "name": "text", "data": "18" } ] } }, { "name": "text", "data": ", " }, { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。如" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "(c)所示，Control薄膜的" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "TFL" } ] }, { "name": "text", "data": "=2.37 V，表明该薄膜的缺陷态密度较大，存在缺陷较多。而ETA分子的加入能有效减少缺陷的生成，特别是当添加浓度为0.25 μL/mL时，其薄膜的" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "TFL" } ] }, { "name": "text", "data": "=1.11 V最小，表明该浓度掺杂下的钙钛矿薄膜的缺陷态密度最低，存在的缺陷最少，也近一步说明了ETA分子掺入Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "薄膜有利于制备高效率Pero-LEDs。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "在制备Pero-LEDs器件（Pero-LEDs结构如" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "(d)所示）之前，我们先利用UPS去了解Control薄膜和最优掺杂浓度0.25 μL/mL ETA HTL的能带位置。对于Pero-LEDs器件而言，空穴载流子使通过HTL价带顶注入到发光层价带，因此，一个匹配的价带位置，对器件性能也存在较大影响，如" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "(e-f)所示，我们能得到Control薄膜的价带位置处于4.14 eV，而最优掺杂浓度的Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "价带位置处于5.21 eV，这可能是因为ETA分子调节了HTL薄膜中Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "/Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "比例，从而对能级产生了影响，使得HTL的价带位置与发光层的价带（5.42 eV）" }, { "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": "更匹配，这也很好地解释了Pero-LEDs器件中空穴载流子注入的增大" }, { "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": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "最后，我们通过制备Pero-LEDs去进一步评估ETA掺杂HTL对器件性能的影响。从" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "(g)中的" }, { "name": "italic", "data": [ { "name": "text", "data": "J-V-L" } ] }, { "name": "text", "data": "曲线可以看出，掺杂ETA分子的Pero-LEDs相对应的电流密度和亮度均有增大，从而更加证实了ETA分子可以有效地调控HTL中Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "/Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "比例，提高其载流子传输能力；同时，其亮度的增加（最大器件亮度为45207 cd/m" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "大于Control器件亮度33490 cd/m" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "），也表明了ETA分子的加入有效地减少了非辐射复合以及缺陷的生成，从而起到了提升器件性能的作用。如" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "(h)所示，对比Control器件而言，当掺杂浓度为0.25 μL/mL时，其器件最大EQE为15.08%。ETA分子的加入，使器件的EQE整体提升（掺杂浓度为0.5 μL/mL和1 μL/mL的最大EQE分别为14.13%和13.71%大于Control最大EQE=12.48%）。其中，插图表示Pero-LEDs在不同电压下的EL光谱，可以看出在器件工作情况下，光谱稳定，发光中心波长未发生偏移。从以上的研究数据表明，ETA分子有助于钙钛矿前驱体溶液的高质量沉积，减少钙钛矿薄膜中缺陷的生成；有助于调控HTL中Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "和Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "比例，使其传输载流子能力增加。最终，在HTL最优掺杂浓度0.25 μL/mL条件下，使Pero-LEDs的EQE达到了15.08%。如" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "(i)所示，我们通过对掺杂和未掺杂HTL制备的器件进行寿命的测试，在恒定电流为0.01 mA的条件下，可以观察到最优掺杂浓度0.25 μL/mL的Pero-LEDs器件的寿命最长，表明该掺杂浓度下的器件性能最稳定。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4　结　　论" } ], "level": "1", "id": "s4" } }, { "name": "p", "data": [ { "name": "text", "data": "本文通过将两种空穴传输层PEDOT:PSS与Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "对比，发现Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "薄膜具有DMSO接触角更小和光透过率更强的优势，并且在Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "薄膜上钙钛矿薄膜具有更强的PL光谱，更长的平均寿命时间，所以Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "比PEDOT:PSS更适合作为Pero-LEDs的HTL。同时，通过进一步的ETA掺杂，有效地调控了传输层中Co" }, { "name": "sup", "data": [ { "name": "text", "data": "3+" } ] }, { "name": "text", "data": "和Co" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "的含量比例，提高了该HTL的载流子传输能力。并且ETA的掺入还能够改变前驱体溶液中晶体析出速度，使Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "薄膜更加平整均匀。同时，ETA分子还具有减小薄膜DMSO接触角和粗糙度的作用，使得HTL薄膜浸润性更好，沉积的钙钛矿薄膜质量更高。最后，基于掺杂的Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "基底薄膜，其最优掺杂浓度为0.25 μL/mL，其最优器件亮度为45207 cd/m" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "，最大EQE为15.08%。本研究在Pero-LEDs体系中引入了Co(OAc)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " HTL，并通过ETA分子的改性，进一步提升了该HTL的性能，丰富了Pero-LEDs体系的HTL种类，为制备不同体系的高效率Pero-LEDs提供一种新的选择。" } ] } ] } ], "footnote": [], "reflist": { "title": [ { "name": "text", "data": "参考文献" } ], "data": [ { "id": "R1", "label": "1", "citation": [ { "lang": "en", "text": [ { "name": "text", "data": "KOJIMA A" }, { "name": "text", "data": "， " }, { "name": "text", "data": "TESHIMA K" }, { "name": "text", "data": "， " }, { "name": "text", "data": "SHIRAI Y" }, { "name": "text", "data": "， " }, { "name": "text", "data": "et al" }, { "name": 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High-efficiency Perovskite Light-Emitting Diodes via Novel Cobalt-based Hole Transporter Layer Enhanced Publication