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基于LiF修饰层的喷墨打印钙钛矿发光二极管
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基于LiF修饰层的喷墨打印钙钛矿发光二极管
- Inkjet Printed Perovskite Light-emitting Diode Based on LiF Modification Layer
- 发光学报 2021年 42卷 第5期 (2021)
- 作者机构：福州大学 物理与信息工程学院，平板显示技术国家地方联合工程实验室,福建,福州,350108
- 作者简介：
- 基金信息：国家自然科学基金(62075043)
- DOI：10.37188/CJL.20210058 中图分类号： TN312.8
纸质出版日期：2021-05-01，
收稿日期：2021-02-09，
修回日期：2021-02-23，
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引用本文
郑春波, 郑鑫, 冯晨, 等. 基于LiF修饰层的喷墨打印钙钛矿发光二极管[J]. 发光学报, 2021, 42(5):565-574.
Chun-bo ZHENG, Xin ZHENG, Chen FENG, et al. Inkjet Printed Perovskite Light-emitting Diode Based on LiF Modification Layer[J]. Chinese Journal of Luminescence, 2021, 42(5):565-574.
郑春波, 郑鑫, 冯晨, 等. 基于LiF修饰层的喷墨打印钙钛矿发光二极管[J]. 发光学报, 2021, 42(5):565-574. DOI： 10.37188/CJL.20210058.
Chun-bo ZHENG, Xin ZHENG, Chen FENG, et al. Inkjet Printed Perovskite Light-emitting Diode Based on LiF Modification Layer[J]. Chinese Journal of Luminescence, 2021, 42(5):565-574. DOI： 10.37188/CJL.20210058.
基于LiF修饰层的喷墨打印钙钛矿发光二极管
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"data": "金属卤化物钙钛矿材料由于具有高光致发光量子产率、高色纯度、带隙可调等优良光学性能，作为发光材料广泛用于制备钙钛矿电致发光二极管(PeLEDs)。虽然已经取得了较好的研究进展，但是其大面积商业化的进程还比较缓慢，尚需进一步研究。为了实现钙钛矿薄膜发光二极管的大面积制备，本文使用喷墨打印技术，研究了不同基板结构对于钙钛矿前驱液的铺展与结晶成膜的影响及器件性能的比较，引入了具有空穴阻挡能力的无机小分子材料氟化锂(LiF)作为缓冲层沉积于空穴传输层TFB上，获得了像素化的均匀分布的钙钛矿薄膜，从而得到发光均匀的最高亮度为4 861 cd/m"
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"data": "显示技术与我们的生活息息相关，在通讯、娱乐、工业生产等行业都能见到它的应用。研究表明人的各种感觉器官从外界获得的信息中视觉占了60%，显示产业已然成为了信息时代不可或缺的基础设施。近年来，卤素钙钛矿材料由于其优异的光学性能，主要包括高光致发光量子产率 (Photoluminescence quantum yield,PLQY)"
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"type": "bibr"
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "，而广泛地应用于钙钛矿电致发光二极管(Perovskite light-emitting diodes,PeLEDs)。短短几年时间内，绿光的 PeLED 外量子效率(External quantum efficiency,EQE)从0.1%跃升到了20.3%"
},
{
"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": ",EQE为20.9%的红光钙钛矿发光二极管"
},
{
"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": "和EQE超过10%的蓝光钙钛矿发光二极管"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "26",
"type": "bibr",
"rid": "R26",
"data": [
{
"name": "text",
"data": "26"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "27",
"type": "bibr",
"rid": "R27",
"data": [
{
"name": "text",
"data": "27"
}
]
}
}
],
"rid": [
"R26",
"R27"
],
"text": "26-27",
"type": "bibr"
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "也相继问世，展现了其在显示和照明方面优异的前景。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "与已经开始进入商用试验阶段的有机发光二极管和无机量子点发光二极管"
},
{
"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": "相比,PeLEDs除了具备比它们更出色的色纯度及发光波长在可见光区连续可调外，还可以通过低廉简便的溶液法制备，尤其是钙钛矿薄膜前驱液的稳定性也是非常的出色。同时经过 5 年的研究，目前基于三维钙钛矿材料为发光层的 PeLEDs的EQE已超过20%，实现了较高的性能，有望成为新一代的发光光源。然而，旋涂法制备工艺虽然操作简单、设备成本低，但是该方法的材料利用率低，且不适用于大面积的样品制作，只适用于材料的评测与表征。喷墨打印技术作为一种传统印刷手段，能方便地实现图案化，材料利用率高且易于大面积制备"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "29",
"type": "bibr",
"rid": "R29",
"data": [
{
"name": "text",
"data": "29"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "37",
"type": "bibr",
"rid": "R37",
"data": [
{
"name": "text",
"data": "37"
}
]
}
}
],
"rid": [
"R29",
"R30",
"R31",
"R32",
"R33",
"R34",
"R35",
"R36",
"R37"
],
"text": "29-37",
"type": "bibr"
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "，使得其在显示方面具有很大的应用前景。而且对于钙钛矿的喷墨打印已经有了一些研究成果，例如钙钛矿单晶阵列的制备"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "38",
"type": "bibr",
"rid": "R38",
"data": [
{
"name": "text",
"data": "38"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "41",
"type": "bibr",
"rid": "R41",
"data": [
{
"name": "text",
"data": "41"
}
]
}
}
],
"rid": [
"R38",
"R39",
"R40",
"R41"
],
"text": "38-41",
"type": "bibr"
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "、钙钛矿的图案化标签"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "42",
"type": "bibr",
"rid": "R42",
"data": [
{
"name": "text",
"data": "42"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "45",
"type": "bibr",
"rid": "R45",
"data": [
{
"name": "text",
"data": "45"
}
]
}
}
],
"rid": [
"R42",
"R43",
"R44",
"R45"
],
"text": "42-45",
"type": "bibr"
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "、钙钛矿太阳能电池的制备"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "46",
"type": "bibr",
"rid": "R46",
"data": [
{
"name": "text",
"data": "46"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "49",
"type": "bibr",
"rid": "R49",
"data": [
{
"name": "text",
"data": "49"
}
]
}
}
],
"rid": [
"R46",
"R47",
"R48",
"R49"
],
"text": "46-49",
"type": "bibr"
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "等。对于喷墨打印制备大面积发光二极管，目前研究尚浅。最近，华南理工大学彭俊彪课题组实现了对绿光钙钛矿量子点发光二极管的喷墨打印"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "xref",
"data": {
"text": "50",
"type": "bibr",
"rid": "R50",
"data": [
{
"name": "text",
"data": "50"
}
]
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "，表现出1 233 cd/m"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "的亮度并且器件的外量子效率为2.8%，峰值电流效率为10.3 cd/A。对于将钙钛矿前驱液应用于喷墨打印发光二极管尚无报道，因为它的常用溶剂二甲基甲酰胺(DMF)或二甲基亚砜(DMSO)在多种有机基材上有较大的接触角，例如聚(4-丁基苯基二苯胺)(poly-TPD)、聚(9-乙烯咔唑)(PVK)和聚［(9,9-二辛基芴-2,7-二基)-共-(4,4'-(N-(4-仲丁基苯基)二苯胺)］(TFB);另一方面，由于DMF及DMSO高沸点的特点，使得在水性基底无法实现三相线钉扎，成膜较差。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "本文将钙钛矿薄膜的前驱液应用于喷墨打印制备发光二极管，针对其中遇到的问题研究了钙钛矿前驱液墨水在不同基底上的铺展与结晶成膜情况，并揭示了它们对器件性能的影响。最后采用在TFB界面层上制备一层LiF修饰层来实现钙钛矿前驱液的均匀铺展成膜，获得了发光均匀的最高亮度为4 861 cd/m"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "且最大电流效率为5.41 cd/A的印刷钙钛矿绿光二极管。"
}
]
}
]
},
{
"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 像素化基板制备及清洁"
}
],
"level": "2",
"id": "s2a"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "本文中用到的玻璃基板由深圳华南湘城科技有限公司加工而成，其中大小为30 mm×30 mm，有效发光区域为2 mm×2 mm。在制备器件前，首先用玻璃清洁剂擦洗后冲洗掉玻璃表面的清洁剂，依次浸入丙酮、异丙醇、去离子水中，在超声仪中超声清洗15 min;最后将基板放入70 ℃烘箱中烘干。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "对于打印器件，我们需要对清洗好的基板进行光刻，得到像素凹槽，以用于后续的喷墨印刷。本文中的像素化基板通过光刻方法实现，采用紫外线曝光与湿法刻蚀的方法。像素化后的基板最好放在氮气手套箱中用培养皿保存好，以防被环境中的灰尘污染。由于光刻胶容易溶于丙酮等有机溶剂，因此若像素化基板受到轻微污染需要清洗，只需在去离子水中超声5 min，然后用氮气吹干基板即可。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2.2 样品制备"
}
],
"level": "2",
"id": "s2b"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "首先对像素化的基板进行臭氧处理10 min，以提高ITO的功函数。接下来，制备各功能层。本文中有4种器件结构，分别是ITO/CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "(70 nm)/TPBi(40 nm)/LiF(1 nm)/Al(100 nm)、ITO/PEDOT∶PSS(40 nm)/CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "(45 nm)/TPBi(40 nm)/LiF(1 nm)/Al(100 nm)、ITO/PEDOT∶PSS/TFB(30 nm)/CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "(45 nm)/TPBi(40 nm)/LiF(1 nm)/Al(100 nm)和ITO/PEDOT∶PSS(40 nm)/TFB(30 nm)/LiF/CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "/TPBi(40 nm)/LiF(1 nm)/Al(100 nm)。对于上述器件，首先，对于PEDOT∶PSS 层，用PEDOT∶PSS溶液旋涂在ITO基板上，高速3 000 r/min持续40 s并在120 ℃退火 20 min后自然冷却待用。对于TFB层，用配制好的TFB溶液旋涂制备TFB空穴传输层(3 000 r/min,40 s)并在120 ℃退火20 min。对于发光层，利用配制好的钙钛矿前驱体(CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": ")溶液，在空气中，由喷墨打印机(JetlabⅡ的纳米材料薄膜沉积设备,MicroFab公司)精准地印刷在像素基板上，随后将样品置于手套箱过渡舱中(10"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "4"
}
]
},
{
"name": "text",
"data": " Pa(10"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": " bar))抽气10 min，使dimethysulfoxide (DMSO,Aladdin)溶剂充分挥发。其中,PEDOT∶PSS溶液(聚3,4-乙烯二氧基噻吩∶聚苯乙烯磺酸,Heraeus Clevios PVP. Al 4083)需要经过0.45 μm水性过滤头过滤后使用。TFB溶液是将TFB (poly(9,9-dioctylfluorene-co-N-(4-butylphenyl)diphenylamine)(西安宝莱特光电科技有限公司，纯度 99%)按5 mg/mL溶解于氯苯(Alfa Aesar，纯度 99%)中。CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": " 溶液是由溴化铅(PbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "，西安宝莱特光电科技有限公司，纯度"
},
{
"name": "text",
"data": ">"
},
{
"name": "text",
"data": "99.99%)、溴化铯(CsBr,Alfa Aesar，纯度99.999%)和溴化苯乙胺(PEABr，西安宝莱特光电科技有限公司，纯度"
},
{
"name": "text",
"data": ">"
},
{
"name": "text",
"data": "99.99%)按照量比1∶1∶0.4 溶解于 DMSO 中，溶液的浓度为0.1 mmol/mL，前驱液在基板上结晶成膜形成二维钙钛矿薄膜("
},
{
"name": "xref",
"data": {
"text": "图1",
"type": "fig",
"rid": "F1",
"data": [
{
"name": "text",
"data": "图1"
}
]
}
},
{
"name": "text",
"data": ")。最后，将样品传入真空热蒸镀系统(SPECTROS 150,Kurt J. Lesker公司)，在背景真空为1.066×10"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-4"
}
]
},
{
"name": "text",
"data": " Pa(8×10"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-7"
}
]
},
{
"name": "text",
"data": " torr)下，蒸镀Tris-［1-phenyl-1H-benzimidazole］(TPBi)、氟化锂(LiF)和铝(Al)。"
}
]
},
{
"name": "fig",
"data": {
"id": "F1",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图1"
}
],
"title": [
{
"name": "text",
"data": "苯基溴化胺在钙钛矿周围形成配体示意图"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.1"
}
],
"title": [
{
"name": "text",
"data": "Schematic diagram of phenylamine bromide forming ligands around perovskite"
}
]
}
],
"subcaption": [],
"note": [],
"graphics": [
{
"print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=21350016&type=",
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{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2.3 器件性能测试"
}
],
"level": "2",
"id": "s2c"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "使用接触角测试仪(SL200 KS,Kono,USA)测试钙钛矿前驱液在不同基底的接触角。使用荧光显微镜(Olympus BX51M)对钙钛矿薄膜进行宏观的形貌表征，以确定墨滴有无落入像素槽中、墨水是否完好成膜，以及检验薄膜是否有缺陷、孔洞等。器件的电流密度(Current density)、亮度(Luminance)、外量子效率(External quantum efficiency,EQE)以及电流效率(Current efficiency,CE)通过由积分球、海洋光学(Ocean optics)USB 2000+光纤光谱仪、Keithley 6485电源搭建的"
},
{
"name": "italic",
"data": [
{
"name": "text",
"data": "I-V-L"
}
]
},
{
"name": "text",
"data": "测试系统采集，利用积分球对器件发光时产生的光通量进行收集。上述所有测试都是在室温大气环境中进行。"
}
]
}
]
}
]
},
{
"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 钙钛矿前驱液对于不同基底的成膜情况探究及对应PeLEDs性能"
}
],
"level": "2",
"id": "s3a"
}
},
{
"name": "p",
"data": [
{
"name": "xref",
"data": {
"text": "图2",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2"
}
]
}
},
{
"name": "text",
"data": "给出了不同基底上的钙钛矿前驱液的接触角，前驱液在ITO和TFB基板上呈现出较大的接触角，不利于墨水的铺展，故对ITO和TFB做了等离子处理，增加墨水的浸润性。这里需要补充一点，因为前驱液的溶剂DMSO是种高沸点液体且不易挥发，本文采用真空抽滤的方式将溶剂抽干使得钙钛矿快速结晶成膜。"
}
]
},
{
"name": "fig",
"data": {
"id": "F2",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图2"
}
],
"title": [
{
"name": "text",
"data": "钙钛矿前驱液在不同基底上的接触角。(a)ITO基底;(b)PEDOT∶PSS基底;(c)TFB基底。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.2"
}
],
"title": [
{
"name": "text",
"data": "Contact angles of perovskite precursors on different substrates. (a)ITO substrate. (b)PEDOT∶PSS substrate. (c)TFB substrate."
}
]
}
],
"subcaption": [],
"note": [],
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"name": "p",
"data": [
{
"name": "text",
"data": "如"
},
{
"name": "xref",
"data": {
"text": "图3",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3"
}
]
}
},
{
"name": "text",
"data": "所示，基于不同基底的钙钛矿前驱液结晶成膜截然不同。通常传统旋涂器件的钙钛矿薄膜是在PEDOT∶PSS界面上的,2018年，华侨大学魏展画课题组用MABr壳层钝化CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "晶体，实现了外量子效率为20.3%的钙钛矿LED"
},
{
"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": "。但是,PEDOT∶PSS薄膜是水性的，同时前驱液的溶剂是水性的DMSO，使得其在PEDOT∶PSS上的接触角较小，为了不使前驱液外溢，在像素坑bank外做了疏水处理(PDMS转印疏水层材料TFB于bank外)。打印完后的薄膜结晶情况如"
},
{
"name": "xref",
"data": {
"text": "图3(a)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(a)"
}
]
}
},
{
"name": "text",
"data": "所示，可以看出虽然疏水层有效地阻止了前驱液的外溢，但是原位液在PEDOT∶PSS上的结晶薄膜并不平整，薄膜中存在许多孔洞，不利于器件的电致发光。这些孔洞的出现是由于在PEDOT∶PSS上,DMSO溶液的三相接触线无法钉扎，使得在抽滤溶剂的过程中发生液体流动。"
},
{
"name": "xref",
"data": {
"text": "图3(b)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(b)"
}
]
}
},
{
"name": "text",
"data": "显示了等离子处理后ITO上钙钛矿成膜情况，薄膜成膜较为平整，且前驱液几乎无外溢。而"
},
{
"name": "xref",
"data": {
"text": "图3(c)",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3(c)"
}
]
}
},
{
"name": "text",
"data": "显示，在等离子后的TFB上的成膜情况则表现为前驱液外溢严重，会影响到附近的像素点，不利于器件的制备;但是无等离子处理的TFB层又不利于前驱液的铺展。"
}
]
},
{
"name": "fig",
"data": {
"id": "F3",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图3"
}
],
"title": [
{
"name": "text",
"data": "钙钛矿前驱液在PEDOT∶PSS上结晶成膜(a)，等离子处理后ITO上结晶成膜(b)，等离子后的TFB上结晶成膜(c)，比例尺为50 μm。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.3"
}
],
"title": [
{
"name": "text",
"data": "Perovskite precursor solution is crystallized to form a film on PEDOT∶PSS(a), ITO after plasma treatment(b), TFB after plasma(c). The scale is 50 μm."
}
]
}
],
"subcaption": [],
"note": [],
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"data": [
{
"name": "text",
"data": "下面将对这3种器件的性能进行比较。3种器件的结构示意图如"
},
{
"name": "xref",
"data": {
"text": "图4",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4"
}
]
}
},
{
"name": "text",
"data": "所示，从图中我们看出器件1是没有空穴注入层和空穴传输层的，类似于发光电化学电池的结构，而CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "自身又是比较好的传输层材料，拥有不错的空穴传输能力。这就要求钙钛矿层厚度需要比较厚，使得载流子能在其中完成传输并复合。而器件2则是比较传统的钙钛矿薄膜的器件结构，除了上述提到的钙钛矿前驱液在PEDOT∶PSS上成膜不均匀外,PEDOT∶PSS对于器件的稳定性也有一定的影响，这是因为PEDOT∶PSS 本身呈酸性 (pH值约为12)"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "xref",
"data": {
"text": "51",
"type": "bibr",
"rid": "R51",
"data": [
{
"name": "text",
"data": "51"
}
]
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "，对ITO电极存在腐蚀作用，不利于器件的长期储存。而且PEDOT∶PSS的HOMO能级(-5.0~-5.1 eV)与钙钛矿价带最大值Vbmax(-5.8~5.9 eV)之间的能级不匹配导致空穴注入不如电子注入。而器件3则沿用了传统有机发光二极管的结构，更有利于发光器件电荷的注入平衡。"
}
]
},
{
"name": "fig",
"data": {
"id": "F4",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图4"
}
],
"title": [
{
"name": "text",
"data": "3种打印器件的结构示意图"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.4"
}
],
"title": [
{
"name": "text",
"data": "Schematic diagrams of the three types of printing devices"
}
]
}
],
"subcaption": [],
"note": [],
"graphics": [
{
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{
"name": "p",
"data": [
{
"name": "xref",
"data": {
"text": "图5",
"type": "fig",
"rid": "F5",
"data": [
{
"name": "text",
"data": "图5"
}
]
}
},
{
"name": "text",
"data": "显示了3个器件的器件性能，我们可以看出器件1由于没有空穴注入及空穴传输层，只能由CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "自身充当空穴传输层，但是ITO/CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "较大的界面注入势垒使得空穴容易聚集在该界面，这使得形成的激子与空穴发生相互作用而引起俄歇复合，影响器件的电致发光性能。而器件2由于CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "薄膜的不平整存在大量孔隙的原因，使得器件发光性能较差。虽然器件3的结构更有利于电荷注入平衡，但是等离子对于TFB层及其上的钙钛矿层的具体影响尚不清楚。从"
},
{
"name": "xref",
"data": {
"text": "图5(a)",
"type": "fig",
"rid": "F5",
"data": [
{
"name": "text",
"data": "图5(a)"
}
]
}
},
{
"name": "text",
"data": "来看,TFB的存在使得电流上升更快，更有利于空穴的注入，使得器件3在2.9 V启亮，较器件1和2的3 V启亮更早。但是，器件3在达到4.5 V后亮度开始衰减，可能是前驱液在等离子后的TFB上铺展更大，某些区域薄膜过薄产生漏电流影响了后续的发光。但是，我们认为TFB等离子不适合喷墨打印的最大原因是因为TFB层等离子后会使在其上印刷前驱液发生严重外溢行为;另外,TFB在等离子后增加浸润性也有一个失效时间。"
},
{
"name": "xref",
"data": {
"text": "图6",
"type": "fig",
"rid": "F6",
"data": [
{
"name": "text",
"data": "图6"
}
]
}
},
{
"name": "text",
"data": "给出了TFB基底在等离子后不同时间的墨水接触角，这使得若要在TFB基底上完成打印，需要在打印前再进行基板处理，这在商业应用上不方便并且不好把控基底的实际浸润性。为此，我们决定在TFB上沉积一层LiF修饰层来代替等离子作用完成前驱液的铺展成膜。"
}
]
},
{
"name": "fig",
"data": {
"id": "F5",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图5"
}
],
"title": [
{
"name": "text",
"data": "不同器件结构的打印器件性能分析。(a)3种器件的电压与亮度和电流密度关系曲线;(b)3种器件的电压与亮度和电流效率关系曲线。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.5"
}
],
"title": [
{
"name": "text",
"data": "Performance analysis of printed devices with different device structures. (a)Relationship curves of the voltage, brightness and current density of the three devices. (b)Relationship curves of the voltage, brightness and current efficiency of the three devices."
}
]
}
],
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"note": [],
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"caption": [
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"lang": "zh",
"label": [
{
"name": "text",
"data": "图6"
}
],
"title": [
{
"name": "text",
"data": "TFB基底等离子后的放置时间对墨水接触角的影响。(a)刚结束等离子;(b)等离子后3 min;(c)等离子后6 min;(d)等离子后10 min。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.6"
}
],
"title": [
{
"name": "text",
"data": "Effect of placement time on ink contact angle after plasma of TFB substrate. (a)Just after plasma. (b)3 min after plasma. (c)6 min after plasma. (d)10 min after plasma."
}
]
}
],
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{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "3.2 基于LiF修饰层的钙钛矿二极管成膜及性能"
}
],
"level": "2",
"id": "s3b"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "由于TFB等有机空穴传输层自身对DMSO溶剂的不亲润性，这里采用蒸镀一层LiF修饰TFB表面，使得前驱液能铺展开来("
},
{
"name": "xref",
"data": {
"text": "图7(b)",
"type": "fig",
"rid": "F7",
"data": [
{
"name": "text",
"data": "图7(b)"
}
]
}
},
{
"name": "text",
"data": ")。为了探究LiF厚度对器件性能的影响，我们制备了不同厚度LiF修饰层的发光器件，通过比较器件的效率来确认最合适的LiF修饰层厚度。器件的结构、薄膜荧光特性及器件性能测试结果如"
},
{
"name": "xref",
"data": {
"text": "图7",
"type": "fig",
"rid": "F7",
"data": [
{
"name": "text",
"data": "图7"
}
]
}
},
{
"name": "text",
"data": "所示，其中"
},
{
"name": "xref",
"data": {
"text": "图7(a)",
"type": "fig",
"rid": "F7",
"data": [
{
"name": "text",
"data": "图7(a)"
}
]
}
},
{
"name": "text",
"data": "为该打印器件的器件结构，与传统的器件结构相比，我们去除了PEDOT∶PSS层。因为PEDOT∶PSS是酸性的，对ITO电极会有腐蚀作用，对于器件的长期保存是不利的，同时我们发现去除PEDOT∶PSS层对于器件的效率几乎没有影响，并且已有相当多的报道在制备钙钛矿发光二极管时舍去了PEDOT∶PSS层"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "52",
"type": "bibr",
"rid": "R52",
"data": [
{
"name": "text",
"data": "52"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "58",
"type": "bibr",
"rid": "R58",
"data": [
{
"name": "text",
"data": "58"
}
]
}
}
],
"rid": [
"R52",
"R53",
"R54",
"R55",
"R56",
"R57",
"R58"
],
"text": "52-58",
"type": "bibr"
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "。"
},
{
"name": "xref",
"data": {
"text": "图7(c)",
"type": "fig",
"rid": "F7",
"data": [
{
"name": "text",
"data": "图7(c)"
}
]
}
},
{
"name": "text",
"data": "为前驱液在LiF修饰的TFB层上的结晶成膜荧光图像，显示了像素阵列中钙钛矿薄膜的均匀分布。随后我们将该薄膜制备了相应的器件。"
}
]
},
{
"name": "fig",
"data": {
"id": "F7",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图7"
}
],
"title": [
{
"name": "text",
"data": "基于LiF修饰层的打印钙钛矿发光器件。(a)打印器件结构示意图;(b)墨水在LiF上的接触角;(c)在LiF修饰层上印刷钙钛矿薄膜的像素阵列的PL显微图像，比例尺为50 μm。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.7"
}
],
"title": [
{
"name": "text",
"data": "Printed perovskite light-emitting device based on LiF modified layer. (a)Schematic diagram of the printed device structure. (b)Contact angles of perovskite precursors on LiF substrate. (c)PL microscopic image of a pixel array printed with a perovskite film on the LiF modified layer. The scale is 50 μm."
}
]
}
],
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"data": {
"text": "图8(a)",
"type": "fig",
"rid": "F8",
"data": [
{
"name": "text",
"data": "图8(a)"
}
]
}
},
{
"name": "text",
"data": "为器件的电致发光光谱及电致点亮图，展现出优异的发光性能。"
},
{
"name": "xref",
"data": {
"text": "图8(b)",
"type": "fig",
"rid": "F8",
"data": [
{
"name": "text",
"data": "图8(b)"
}
]
}
},
{
"name": "text",
"data": "和"
},
{
"name": "xref",
"data": {
"text": "图9(a)、(b)",
"type": "fig",
"rid": "F9",
"data": [
{
"name": "text",
"data": "图9(a)、(b)"
}
]
}
},
{
"name": "text",
"data": "分别展示了不同LiF修饰层厚度的器件的性能对比。从"
},
{
"name": "xref",
"data": {
"text": "图8(b)",
"type": "fig",
"rid": "F8",
"data": [
{
"name": "text",
"data": "图8(b)"
}
]
}
},
{
"name": "text",
"data": "可以看出,LiF修饰层厚度的微小变化对于器件的电流密度及亮度变化几乎没有影响;但是从"
},
{
"name": "xref",
"data": {
"text": "图9(a)、(b)",
"type": "fig",
"rid": "F9",
"data": [
{
"name": "text",
"data": "图9(a)、(b)"
}
]
}
},
{
"name": "text",
"data": "的器件效率来看,LiF修饰层的厚度应该影响了空穴-电子的复合位置，从而影响了激子的发光辐射复合率。一般来说，器件的性能与器件的结构和薄膜的质量息息相关，而且发光层的厚度对于性能也有一定的影响。从接触角来分析，墨水在LiF上的接触角比在等离子后的TFB上要大，薄膜厚度大，那么该器件出现漏电流的可能性就会小很多，使得器件亮度能上升到4 800 cd/m"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "。从图中我们可以知道，随着LiF修饰层厚度的增加，器件的外量子效率及电流效率逐渐下降。接下来我们从激子复合效应示意图来解释LiF修饰层对于器件性能的影响。"
}
]
},
{
"name": "fig",
"data": {
"id": "F8",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图8"
}
],
"title": [
{
"name": "text",
"data": "不同LiF修饰层厚度的打印钙钛矿发光器件性能。(a)打印器件的电致发光光谱及电致发光图;(b)不同LiF修饰层厚度器件的电压与亮度及电流密度关系曲线。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.8"
}
],
"title": [
{
"name": "text",
"data": "Performance of printed perovskite light-emitting devices with different LiF modified layer thicknesses. (a)Electroluminescence spectrum and electroluminescence diagrams of the printed device. (b)Voltage,brightness and current density curves of devices with different LiF modified layer thicknesses."
}
]
}
],
"subcaption": [],
"note": [],
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"lang": "zh",
"label": [
{
"name": "text",
"data": "图9"
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],
"title": [
{
"name": "text",
"data": "不同LiF修饰层厚度的打印钙钛矿发光器件性能。(a)不同LiF修饰层厚度器件的亮度与外量子效率关系曲线;(b)不同LiF修饰层厚度器件的亮度与电流效率关系曲线。"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.9"
}
],
"title": [
{
"name": "text",
"data": "Performance of printed perovskite light-emitting devices with different LiF modified layer thicknesses. (a)Relationship curves between brightness and external quantum efficiency of devices with different LiF modified layer thicknesses. (b) Relationship between brightness and current efficiency of devices with different LiF modified layer thicknesses."
}
]
}
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{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "3.3 LiF界面处的激子复合效应"
}
],
"level": "2",
"id": "s3c"
}
},
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"data": [
{
"name": "xref",
"data": {
"text": "图10",
"type": "fig",
"rid": "F10",
"data": [
{
"name": "text",
"data": "图10"
}
]
}
},
{
"name": "text",
"data": "给出了LiF修饰层的器件的激子复合效应示意图。高极性的介电材料LiF除了改善TFB界面使钙钛矿前驱液能有效铺展，作为空穴阻挡层，它对于空穴也有一定的阻挡作用。 LiF层处于TFB与CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "的界面处，空穴在该界面处发生积累可明显降低复合发光区域内的电场，从而减少从TFB层进入CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "复合发光区域的空穴，但并不影响从阴极端过来的电子的传输，使得激子复合区域更靠近LiF修饰层。由于PEDOT∶PSS的HOMO能级较TFB更高，虽然去除了PEDOT∶PSS而少了些空穴的注入，但是PEDOT∶PSS/CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "的界面注入势垒较TFB/CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "更大，使得空穴和电子仍能约束在CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "发光层。然而，随着LiF修饰层厚度的增加，空穴更多地被阻挡在LiF/CsPbBr"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "界面处，更多的电子迁移到LiF界面处发生复合，降低了激子的发光辐射复合率，进而降低了PeLEDs的性能。"
}
]
},
{
"name": "fig",
"data": {
"id": "F10",
"caption": [
{
"lang": "zh",
"label": [
{
"name": "text",
"data": "图10"
}
],
"title": [
{
"name": "text",
"data": "激子界面复合效应示意图"
}
]
},
{
"lang": "en",
"label": [
{
"name": "text",
"data": "Fig.10"
}
],
"title": [
{
"name": "text",
"data": "Schematic diagram of exciton interface recombination effect"
}
]
}
],
"subcaption": [],
"note": [],
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},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "4 结论"
}
],
"level": "1",
"id": "s4"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "本文利用在TFB传输层上沉积一层LiF修饰层，有效实现了钙钛矿前驱体溶液的铺展与平整成膜，获得了最大亮度为4 816 cd/m"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "、最大外量子效率为1.73%、最大电流效率为5.41 cd/A的绿光PeLEDs。经研究表明,LiF修饰层的引入，实现了像素化的均匀分布的钙钛矿薄膜，同时LiF层对于空穴有一定的阻挡作用，对于器件的电荷注入平衡的实现提供了一种可供参考的方法。本文为钙钛矿薄膜实现大面积打印提供了一种可供借鉴的、行之有效的制备方式。"
}
]
}
]
}
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"history": {
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"revised": "2021-02-23",
"ppub": "2021-05-01",
"opub": "2021-10-22"
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"data": [],
"year": "2021"
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"appendix": [],
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"supplementary": [],
"journalTitle": "发光学报",
"issue": "05",
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}
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