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有机发光二极管老化机制
特邀报告 | 更新时间：2023-02-16
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有机发光二极管老化机制 增强出版
- Degradation Mechanism of Organic Light-emitting Diodes
- 发光学报 2023年 44卷 第1期 (2023)
- 作者机构：华南理工大学 发光材料与器件国家重点实验室,广东,广州,510640
- 作者简介：
- 基金信息：国家自然科学基金(52103207);广东省自然科学基金(2022A1515011969)
- DOI：10.37188/CJL.20220317 中图分类号： TN312.8
纸质出版日期：2023-01-05，
收稿日期：2022-08-30，
修回日期：2022-09-15，
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引用本文
牛泉,郝洪敏,林雯欣等.有机发光二极管老化机制[J].发光学报,2023,44(01):186-197.
NIU Quan,HAO Hongmin,LIN Wenxin,et al.Degradation Mechanism of Organic Light-emitting Diodes[J].Chinese Journal of Luminescence,2023,44(01):186-197.
牛泉,郝洪敏,林雯欣等.有机发光二极管老化机制[J].发光学报,2023,44(01):186-197. DOI： 10.37188/CJL.20220317.
NIU Quan,HAO Hongmin,LIN Wenxin,et al.Degradation Mechanism of Organic Light-emitting Diodes[J].Chinese Journal of Luminescence,2023,44(01):186-197. DOI： 10.37188/CJL.20220317.
有机发光二极管老化机制 增强出版
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"data": "有机发光二极管（OLEDs）因在照明和显示领域的巨大潜在应用备受人们关注。在过去的三十年里，OLED器件的效率和寿命有了很大的提高，但对于商业应用而言提高器件寿命仍然是亟待解决的问题之一。为了进一步提升器件稳定性，则需要深入地研究OLED内部存在的老化机理。本文以小分子和聚合物OLEDs为例，综述了两种器件的老化机制。概括了OLED的一些外在和内在老化机制，并介绍了小分子和聚合物OLEDs老化机理的研究进展。对于小分子OLEDs，有研究提出其老化机理是激子与极化子的相互作用，形成陷阱导致器件老化。另一种理论认为激子与极化子的作用诱导分子聚集，促进界面老化。而对于聚合物OLEDs老化机理是激子与空穴相互作用，诱导空穴陷阱产生，导致了亮度、效率损失和驱动电压上升的现象。同时综述了目前一部分延长器件寿命的方案，为后续开发效率更高、寿命更长的OLED器件提供积极作用。"
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"data": "，已经初步满足中小尺寸平板显示的要求，成为继液晶显示之后第三代主流显示。虽然OLED在商业中的应用越来越广泛，但其使用寿命仍不能满足大尺寸显示、高亮度照明需求，尤其是蓝光OLED寿命远低于红光、绿光OLED，稳定性的提高是目前商业化亟需解决的问题。评估OLED器件的稳定性，往往是通过加速老化试验测量并计算器件寿命。在恒定电流驱动下，OLED器件寿命可以表达为器件亮度衰减至初始亮度的一定百分比所需的时间，例如亮度衰减至50%，则称为LT"
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"data": "OLED器件的老化机制可以分为本征老化与非本征老化。非本征老化指的是由外部因素引起的器件发光的失效，一般表现为“Dark spots”老化现象，或“Catastrophic failure”老化现象"
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"data": "。前者表现为器件发光区域内黑点的形成并随放置时间的延长而增加，导致OLED亮度降低，如"
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"data": "。例如水氧的入侵、基板不平整、微小颗粒的引入、金属阴极表面的小孔隙等，均会导致金属电极被氧化、有机层与金属阴极分层，影响电子的注入，产生不发光区域，即形成黑点"
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"data": "。有研究将OLED的金属阴极剥离，再重新蒸镀一层新的金属阴极，发现原本器件中的黑点消失，这种由电极剥落导致的老化现象为典型非本征老化，器件效率并不随时间改变"
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"data": "OLED本征老化指的是器件在电应力条件下工作时器件效率随时间不断衰减。在恒电流作用下，器件的老化现象表现为亮度逐渐下降、驱动电压逐渐上升。探索OLED本征老化机理，对进一步优化材料与器件设计，从材料创新和物理本源上提高器件稳定性具有重要意义。OLED根据发光材料与制备工艺的不同可分为基于蒸镀加工工艺的小分子OLED, 与基于聚合物发光半导体的可溶液加工的聚合物OLED（PLED）。由于制备工艺的不同，小分子OLED往往具有更加复杂的多层结构，比如包含了电荷注入层、电荷传输层、电荷/激子阻挡层、发光层等。这是因为蒸镀工艺对实现多层结构更为有利。而对于基于溶液加工的聚合物发光二极管，其结构往往较为简单，比如器件包含了电荷传输层与发光层。"
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"data": "因此，对于具有复杂结构的小分子OLED来说，老化过程则更为复杂，各个有机半导体层在老化过程中的变化导致解析器件本征老化机制较为困难。而对于具有简单结构甚至单层结构的聚合物OLED来说，器件模型的建构与老化机制的探索则相对较容易。因此本文基于复杂多层结构的小分子OLED以及结构简单的PLED两种器件，介绍老化机理的研究进展，对它们的内部与本征老化机理进行综述，并阐述介绍寿命提升方案。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2 小分子OLED本征老化机制"
}
],
"level": "1",
"id": "s2"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "在过去三十年，为了揭示小分子OLED的本征老化机制，人们进行了广泛的研究，提出了多种推论与解释，包括不稳定的阳离子分子、界面空间电荷累积、材料的化学降解、激子与极化子的相互作用导致器件老化等。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "8-羟基喹啉铝（Alq"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "）小分子是早期最广泛使用的荧光发光分子。1999年，Aziz等首先对以Alq"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "为发光材料的OLED进行了内在老化机制研究工作，提出了不稳定的阳离子分子理论。该理论认为进行空穴传输的Alq"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "形成了带阳离子的分子，这导致其荧光量子效率降低，并且作为荧光猝灭中心，导致器件电致发光性能降低。而参与电荷传输的带阴离子的分子对其荧光量子效率没有明显影响"
},
{
"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": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "受到上述理论启发，有研究进一步探究了在器件运行过程中空穴或电子的存在是否对器件老化发挥普遍作用。Kondakov等通过电容-电压测试，测量了器件运行中的电荷密度变化，发现随着电致老化时间延长，亮度减小，空穴传输层/电子传输层（HTM/ETM）界面处空间电荷密度增加，并且亮度与空间电荷密度呈线性相关"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "15",
"type": "bibr",
"rid": "R15",
"data": [
{
"name": "text",
"data": "15"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。于是推测器件在电应力作用下产生了空穴陷阱，陷阱捕获空穴形成空间电荷，被陷阱捕获的空穴与自由电子非辐射复合以及陷阱电荷对激子的猝灭导致亮度衰减"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "15",
"type": "bibr",
"rid": "R15",
"data": [
{
"name": "text",
"data": "15"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "16",
"type": "bibr",
"rid": "R16",
"data": [
{
"name": "text",
"data": "16"
}
]
}
}
],
"rid": [
"R15",
"R16"
],
"text": "15-16",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。该研究基于器件电学特性的测量与推论，并未进一步对陷阱形成量化，也未指出老化过程的关键物理化学过程。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "在器件老化过程中通过对陷阱形成进行物理模拟并进一步量化，同时利用检测手段对材料的化学降解产物进行追踪检测，将有利于为陷阱的形成与本源提供证据。有机半导体材料分子在OLED老化中的降解将在2.1节介绍。"
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "2.1 有机半导体分子化学降解"
}
],
"level": "2",
"id": "s2a"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "有机半导体材料分子的光电稳定性是制约器件寿命的重要因素之一。当OLED暴露在紫外可见光下，有机材料易通过光诱导氧化、裂解过程发生老化"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "17",
"type": "bibr",
"rid": "R17",
"data": [
{
"name": "text",
"data": "17"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。有机材料另一个重要的老化途径是电化学老化。通过载流子注入OLED器件，载流子在有机半导体内的传输从化学角度来看本质为发生连续的氧化还原过程，产生正、负极化子，同时载流子复合会生成激子，这些激子和极化子会导致有机材料处于不稳定状态"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "17",
"type": "bibr",
"rid": "R17",
"data": [
{
"name": "text",
"data": "17"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "18",
"type": "bibr",
"rid": "R18",
"data": [
{
"name": "text",
"data": "18"
}
]
}
}
],
"rid": [
"R17",
"R18"
],
"text": "17-18",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。研究认为OLED器件中有机电荷传输层、主体材料、发光材料的老化过程与有机半导体材料分子的键解离能（Bond dissociation energy，BDE）相关"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "19",
"type": "bibr",
"rid": "R19",
"data": [
{
"name": "text",
"data": "19"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。当有机半导体分子中具有较低BDE的化学键时，在OLED器件运行过程中相应功能层材料则易发生化学键的断裂，形成自由基，这些产物将进一步演变成非辐射复合中心或激子猝灭中心，从而影响电荷传输、电荷复合以及能量转移过程，导致OLED器件的老化"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "17",
"type": "bibr",
"rid": "R17",
"data": [
{
"name": "text",
"data": "17"
}
]
}
},
{
"name": "text",
"data": ", "
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "20",
"type": "bibr",
"rid": "R20",
"data": [
{
"name": "text",
"data": "20"
}
]
}
},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "23",
"type": "bibr",
"rid": "R23",
"data": [
{
"name": "text",
"data": "23"
}
]
}
}
],
"rid": [
"R20",
"R21",
"R22",
"R23"
],
"text": "20-23",
"type": "bibr"
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "2011年，Moraes等利用激光解吸飞行时间质谱（LDI-TOF-MS）技术研究了基于磷光小分子 Ir（ppy）"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3 "
}
]
},
{
"name": "text",
"data": "OLED的退化机制。如"
},
{
"name": "xref",
"data": {
"text": "图2",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2"
}
]
}
},
{
"name": "text",
"data": "（b）所示，该研究提出器件运行过程中磷光小分子键断裂，解离产物与空穴阻挡层形成稳定的配合物；化学解离反应过程如"
},
{
"name": "xref",
"data": {
"text": "图2",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2"
}
]
}
},
{
"name": "text",
"data": "（a）所示，配合物引起激子猝灭，这是导致器件退化的主要原因。采用不与发光材料发生反应形成配合物的空穴阻挡材料，可获得较高稳定性的器件"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "23",
"type": "bibr",
"rid": "R23",
"data": [
{
"name": "text",
"data": "23"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Lin等发现氧化膦基材料CzPO"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "在紫外光照射或电应力下，相对较弱的C—P键可在激发态和带电态发生解离，破坏OLED的稳定性"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "24",
"type": "bibr",
"rid": "R24",
"data": [
{
"name": "text",
"data": "24"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "bold",
"data": [
{
"name": "text",
"data": "。"
}
]
},
{
"name": "text",
"data": "随后他们在另一篇报道中又对有机发光材料中常见吸电子基团磺酰基、氧化膦和羰基等进行研究，认为器件运行中C—S、C—P、C—C键都会发生断裂导致器件退化"
},
{
"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": "。Hong等对咔唑-二苯并噻吩（Cz-DBT）中咔唑和二苯并噻吩之间的C—N键的断裂机制进行研究，提出C—N键的低键解离能（1.6 eV）是器件退化的主要原因"
},
{
"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": "。"
}
]
},
{
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"id": "F2",
"caption": [
{
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"label": [
{
"name": "text",
"data": "图2"
}
],
"title": [
{
"name": "text",
"data": "（a）磷光分子Ir（ppy）"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "在激发状态下的化学解离反应"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "xref",
"data": {
"text": "23",
"type": "bibr",
"rid": "R23",
"data": [
{
"name": "text",
"data": "23"
}
]
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "；（b）老化前后绿光磷光Ir（ppy）"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3 "
}
]
},
{
"name": "text",
"data": "OLED器件的光解吸飞行时间质谱"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "xref",
"data": {
"text": "23",
"type": "bibr",
"rid": "R23",
"data": [
{
"name": "text",
"data": "23"
}
]
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "；（c）CBP基OLED在器件老化过程中的化学反应"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
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"name": "xref",
"data": {
"text": "21",
"type": "bibr",
"rid": "R21",
"data": [
{
"name": "text",
"data": "21"
}
]
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": "；（d）CBP基OLED老化后的微分色谱"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
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"data": {
"text": "21",
"type": "bibr",
"rid": "R21",
"data": [
{
"name": "text",
"data": "21"
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]
}
},
{
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"data": "］"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
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"label": [
{
"name": "text",
"data": "Fig.2"
}
],
"title": [
{
"name": "text",
"data": "（a）Proposed chemical dissociation reaction of Ir（ppy）"
},
{
"name": "sub",
"data": [
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"data": "3"
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]
},
{
"name": "text",
"data": " after excitation"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "xref",
"data": {
"text": "23",
"type": "bibr",
"rid": "R23",
"data": [
{
"name": "text",
"data": "23"
}
]
}
},
{
"name": "text",
"data": "］"
}
]
},
{
"name": "text",
"data": ". （b）LDI-TOF mass spectra of the unaged and aged OLED based on the green phosphorescent emitter Ir（ppy）"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "［"
},
{
"name": "xref",
"data": {
"text": "22",
"type": "bibr",
"rid": "R22",
"data": [
{
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"data": "22"
}
]
}
},
{
"name": "text",
"data": "］"
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},
{
"name": "text",
"data": ". （c）Representative chemical reactions postulated to occur during operational degradation of CBP⁃based OLEDs"
},
{
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"data": [
{
"name": "text",
"data": "["
},
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"data": {
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"rid": "R21",
"data": [
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"data": "21"
}
]
}
},
{
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"data": "]"
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]
},
{
"name": "text",
"data": ". （d）Difference chromatogram of the operationally degradeddevice"
},
{
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"data": "["
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"data": "除了发光材料，在发光层中主体材料往往作为激子形成中心，并参与电荷传输与能量转移，是影响OLED器件稳定性的重要因素之一。研究认为，在激子、正负极化子作用下主体材料易发生老化。Kondakov等通过核磁共振与质谱分析，在老化过后的OLED器件中检测到主体材料4,4'-双（N-咔唑）-1,1'-联苯（CBP）的降解产物，如"
},
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"type": "fig",
"rid": "F2",
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{
"name": "text",
"data": "（d）所示，降解产物包含4-（N-咔唑）联苯（BPC）、咔唑等，这来源于CBP中弱C—N键的断裂。C—N键断裂继发产生一系列化学反应，如"
},
{
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"data": {
"text": "图2",
"type": "fig",
"rid": "F2",
"data": [
{
"name": "text",
"data": "图2"
}
]
}
},
{
"name": "text",
"data": "（c）所示，通过自由基加成反应产生中性自由基，成为非辐射复合中心和激子猝灭中心，影响器件寿命"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "20",
"type": "bibr",
"rid": "R20",
"data": [
{
"name": "text",
"data": "20"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。该团队在另一篇报道中利用化学分析、器件物理、光化学分析和电子顺磁共振，研究发现具有高激发态能量与低键解离能的OLED老化过程较快。器件运行过程中形成长寿命π自由基以带电或中性形式积累，作为非辐射复合中心和激子猝灭中心，造成OLED的退化"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "21",
"type": "bibr",
"rid": "R21",
"data": [
{
"name": "text",
"data": "21"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "对于电荷传输材料而言，键断裂会影响电子或空穴传输，导致电荷传输不平衡，影响OLED的稳定性。Sivasubramaniam等利用激光解吸电离设备并结合飞行时间质谱（LDI-TOF/MS）进行测量，提出器件运行期间空穴传输层三（4-咔唑基-9-基苯基）胺（TCTA）三苯胺中的C—N键发生了裂解"
},
{
"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": "。4,4'-环己基二[N,N-二（4-甲基苯基）苯胺]（TAPC）因其高三线态能级以及优异的空穴传输能力作为空穴传输材料，可实现高效率、低驱动电压的OLED器件，但器件在运行过程中易老化。Dong等利用高效液相色谱-质谱（HPLC-MS） 对TAPC进行理论和实验化学老化研究，发现 C（sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "）—N（sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "）键和C（sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "）—C（sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "）键发生断裂，并检测到环己烷的分解产物"
},
{
"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": "。通过分子设计工程，减少材料中的弱化学键，可以有效地提高器件寿命。例如，3,3-二（咔唑基）联苯（mCBP）中含有的C（sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "）—N（sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "）化学键的键解离能要高于TCTA、TAPC中的C（sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "）—N（sp"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "3"
}
]
},
{
"name": "text",
"data": "）化学键，因而有效提高了材料的稳定性，在器件寿命方面优于TAPC、TATC"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "29",
"type": "bibr",
"rid": "R29",
"data": [
{
"name": "text",
"data": "29"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。这说明化学键强弱和激发态能量是影响OLED器件运行稳定性的重要因素。"
}
]
}
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"title": [
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"data": "2.2 激子和极化子相互作用"
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"data": [
{
"name": "text",
"data": "随着OLED的不断发展，为进一步提升OLED器件效率与稳定性，功能层进一步堆叠。对于这种具有复杂结构的OLED，探究其本征老化机制是一大挑战。针对材料分子在OLED器件老化过程中的化学降解，有研究提出造成键断裂的原因是激子与极化子的相互作用。激子与极化子猝灭机制如"
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"data": {
"text": "图3",
"type": "fig",
"rid": "F3",
"data": [
{
"name": "text",
"data": "图3"
}
]
}
},
{
"name": "text",
"data": "所示，激子的能量转移到极化子中，这会产生一个高能量的极化子，在能量弛豫的过程中往往会破坏分子中的化学键"
},
{
"name": "sup",
"data": [
{
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"data": "["
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"name": "xref",
"data": {
"text": "30",
"type": "bibr",
"rid": "R30",
"data": [
{
"name": "text",
"data": "30"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。并推论极化子与激子的相互作用会诱导陷阱的生成，陷阱作为非辐射复合中心、激子猝灭中心以及深电荷陷阱，导致器件在电致发光过程中亮度效率下降、电压升高等老化现象"
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{
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"data": "["
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"name": "blockXref",
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"data": [
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"name": "xref",
"data": {
"text": "31",
"type": "bibr",
"rid": "R31",
"data": [
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"data": "31"
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"name": "text",
"data": "-"
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"data": {
"text": "32",
"type": "bibr",
"rid": "R32",
"data": [
{
"name": "text",
"data": "32"
}
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}
}
],
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"type": "bibr"
}
},
{
"name": "text",
"data": "]"
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]
},
{
"name": "text",
"data": "。还有理论认为激子与极化子相互作用会引起分子聚集在界面附近，影响载流子传输，增强激子猝灭，使器件效率降低"
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"data": {
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"data": "33"
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"data": {
"text": "34",
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"data": "2008年，Giebink等基于蓝光磷光OLED建立了激子-极化子诱导陷阱形成的数值计算模型，假设激子与极化子猝灭诱导主体分子HOMO与LUMO之间形成离散的深空穴陷阱。该老化模型可以有效描述OLED在恒电流电应力条件下工作亮度下降、电压上升现象，预设的老化模型与亮度和电压与老化时间的依赖关系数据相符合。当陷阱密度约为10"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "18 "
}
]
},
{
"name": "text",
"data": "cm"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-3"
}
]
},
{
"name": "text",
"data": "时，器件亮度下降程度"
},
{
"name": "text",
"data": ">"
},
{
"name": "text",
"data": "50%"
},
{
"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": "。随后该研究团队通过研究各种应力下单载流子器件的稳定性进一步验证了该理论。采用陷阱电荷限制电流模型（Trapped-charge-limited, TCL），并建立TCL电容公式，模拟磷光mCBP∶Ir（ppy）"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3 "
}
]
},
{
"name": "text",
"data": "OLED单载流子器件的电容、电流密度与电压依赖性。对单载流子器件分别施加恒电流应力、光照应力、以及恒电流与光照组合应力，通过器件模型模拟方法，发现在电应力作用下，带有阴离子的mCBP分子是不稳定的，结合光照应力，mCBP阴离子与Ir（ppy）"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "3 "
}
]
},
{
"name": "text",
"data": "激子相互作用加剧其不稳定性"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
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"name": "xref",
"data": {
"text": "31",
"type": "bibr",
"rid": "R31",
"data": [
{
"name": "text",
"data": "31"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。提出了OLED是由激子-极化子猝灭诱导陷阱的生成导致器件老化。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "但是以上模型并未对陷阱形成进行量化，同时关于陷阱类型的讨论还存在争议。Niu等采用瞬态响应电致发光（TEL）测试方法，研究了未老化与老化后的多层结构的N-杂环卡宾（NHC）铱金属配合物磷光OLED的电荷传输。在该器件中空穴由三[（3-苯基-1H-苯并咪唑-1-基-2（3H）-亚基）-1,2-亚苯基]铱（DPBIC）运输，电子由NHC发光材料运输，TEL测试结果表明，多层蓝光铱金属配合物磷光OLED器件电荷传输是以电子电流主导。老化器件中电流的减小与电子传输下降有关。最终提出电子陷阱形成导致电子传输下降，器件效率降低现象。电子陷阱在老化过程中还可表现为发光的猝灭剂，导致器件亮度降低"
},
{
"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": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "在界面处，由于界面势垒较高或者载流子传输不平衡，都会引起载流子在界面处的积累。这可能会导致激子与界面极化子相互作用，促进界面的老化，影响载流子注入，增强激子猝灭，使器件效率降低"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "34",
"type": "bibr",
"rid": "R34",
"data": [
{
"name": "text",
"data": "34"
}
]
}
},
{
"name": "text",
"data": ", "
},
{
"name": "xref",
"data": {
"text": "36",
"type": "bibr",
"rid": "R36",
"data": [
{
"name": "text",
"data": "36"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Wang等研究了单空穴器件中HTM/ETM界面在照明以及电流应力情况下的稳定性，发现在光照和空穴电流的同时作用下HTM/ETM界面严重老化，并且是由于HTM正极化子和HTM单线态激子之间的相互作用导致其与ETM界面发生老化。通过掺杂3,4,9,10-苝四甲酸二苯并咪唑（PTCBI）激子猝灭剂降低激子寿命和浓度，OLED恒流应力下驱动电压稳定性显著提高"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "36",
"type": "bibr",
"rid": "R36",
"data": [
{
"name": "text",
"data": "36"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。之后该研究团队通过研究器件处于长时间工作状态下的电致、光致发光光谱，发现老化后器件电致发光光谱出现500 nm左右的新发射峰，并证实其与激子-极化子相互作用诱导的聚集密切相关。说明电应力作用下激子和正极化子以高浓度存在时，激子与极化子相互作用诱导其主体材料分子聚集在HTM/ETM界面附近，并导致其界面老化。这种现象在多种宽带隙主体OLED器件中普遍存在"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "34",
"type": "bibr",
"rid": "R34",
"data": [
{
"name": "text",
"data": "34"
}
]
}
},
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"data": "]"
}
]
},
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"data": "。"
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]
},
{
"name": "text",
"data": "Cho等比较了溶液旋涂制备和真空沉积制备的OLED老化机理。同样认为在电应力作用下，器件发光层中激子和极化子之间的相互作用导致主体材料的聚集是器件退化的主要原因。并且研究发现，溶液加工器件相对于真空沉积器件的降解速度更快是因为溶液加工器件主体材料的聚集速度更快，进一步证实了材料聚集对器件稳定性的影响"
},
{
"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": "。"
}
]
}
]
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"data": {
"title": [
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"name": "text",
"data": "2.3 小分子OLEDs器件稳定性提升策略"
}
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"data": [
{
"name": "text",
"data": "材料稳定性是提高器件寿命的重要因素，提高材料的稳定性可以从分子设计工程入手"
},
{
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{
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"data": "["
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"data": [
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"data": {
"text": "37",
"type": "bibr",
"rid": "R37",
"data": [
{
"name": "text",
"data": "37"
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"name": "text",
"data": "-"
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"name": "xref",
"data": {
"text": "41",
"type": "bibr",
"rid": "R41",
"data": [
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"data": "41"
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"rid": [
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"type": "bibr"
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},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Shin等报道了以二苯并噻吩和咔唑基咔唑为基础的高三线态材料，作为蓝光磷光OLED的主体材料。该主体材料中咔唑与二苯并噻吩单元之间的C—N键在负极化子状态下的键解离能为1.7 eV，高于常用的主体材料mCBP中的C—N键（1.30 eV）。其次，该主体材料具有较高的玻璃转化温度，使器件有较好的热稳定性。利用该主体材料制备的器件寿命要比mCBP OLED提高5倍以上"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "40",
"type": "bibr",
"rid": "R40",
"data": [
{
"name": "text",
"data": "40"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Jeon等采用高化学稳定性的三嗪和咔唑基团来构建深蓝的热活化延迟荧光（TADF）分子，以二苯基三嗪为受体，二苯基咔唑为给体。由于二苯基咔唑给体能力较弱，引入两个苯基单元来扭曲给体单元，增强分子的电荷转移特性，稳定了电荷转移单线态激发态，实现了117 h的LT"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "50"
}
]
},
{
"name": "text",
"data": "寿命（初始亮度为1 000 cd/m"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "）"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "7",
"type": "bibr",
"rid": "R7",
"data": [
{
"name": "text",
"data": "7"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "通过降低激子寿命或者降低激子、极化子浓度可以有效提高器件寿命"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
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"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "42",
"type": "bibr",
"rid": "R42",
"data": [
{
"name": "text",
"data": "42"
}
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"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": "。TADF分子通过反向系间窜越（RISC）过程实现100%的激子利用率，有效提高了器件的效率。Noda等在5CzBN中几个咔唑单元引入苯环，从分子设计方面降低局域激发三线态的能量，增加了RISC速率并缩短了三线态激子寿命，将器件寿命LT"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "90"
}
]
},
{
"name": "text",
"data": "从30 h增加至450 h"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "44",
"type": "bibr",
"rid": "R44",
"data": [
{
"name": "text",
"data": "44"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Heimel等提出一种基于磷光敏化荧光材料，辐射衰减发光原理如"
},
{
"name": "xref",
"data": {
"text": "图4",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图4"
}
]
}
},
{
"name": "text",
"data": "（a）所示，通过三线态激发态快速的Förster共振能量转移至受体荧光分子的单线态，降低了激子寿命。减少了激子辐射衰减时间，有效延长了器件的寿命。从"
},
{
"name": "xref",
"data": {
"text": "图 4",
"type": "fig",
"rid": "F4",
"data": [
{
"name": "text",
"data": "图 4"
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},
{
"name": "text",
"data": "（b）中可以看到，在4 000 cd/m"
},
{
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"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "初始亮度下，器件LT"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "70"
}
]
},
{
"name": "text",
"data": "寿命从46 h提升至79 h，器件寿命提高了1.7倍，并且保持发光颜色不变"
},
{
"name": "sup",
"data": [
{
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"data": "["
},
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"data": {
"text": "45",
"type": "bibr",
"rid": "R45",
"data": [
{
"name": "text",
"data": "45"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。这为实现高效稳定的蓝光发光二极管提供了新路径。"
}
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"data": "（a）磷光给体敏化荧光受体的辐射衰减路径； （b）器件寿命与辐射衰减速率的关系"
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"label": [
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}
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"title": [
{
"name": "text",
"data": "（a）Schematic illustration of radiative decay paths of phosphor-sensitized fluorescence.（b）Correlation between lifetimes and radiative decay rates"
},
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"data": [
{
"name": "text",
"data": "平衡载流子以及扩展激子形成的区域也可以避免激子与极化子猝灭效应"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "blockXref",
"data": {
"data": [
{
"name": "xref",
"data": {
"text": "46",
"type": "bibr",
"rid": "R46",
"data": [
{
"name": "text",
"data": "46"
}
]
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},
{
"name": "text",
"data": "-"
},
{
"name": "xref",
"data": {
"text": "48",
"type": "bibr",
"rid": "R48",
"data": [
{
"name": "text",
"data": "48"
}
]
}
}
],
"rid": [
"R46",
"R47",
"R48"
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"type": "bibr"
}
},
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]
},
{
"name": "text",
"data": "。Zhang等在磷光OLED中采用梯度掺杂策略，该策略通过平衡载流子以减少额外的极化子，同时有效扩宽了复合区域，降低了激子密度，抑制激子-极化子湮灭过程。基于该策略的双单元蓝光磷光叠层OLED，在1 000 cd/m"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "初始亮度下器件LT"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "80"
}
]
},
{
"name": "text",
"data": "寿命为616 h，比当时传统的蓝色磷光OLED器件寿命提高了10倍"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "49",
"type": "bibr",
"rid": "R49",
"data": [
{
"name": "text",
"data": "49"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。另一种有效的方法是采用N型与P型材料混合作为主体材料。Sun等采用P型材料SiCzCz和N型材料SiTrzCz2作为蓝光磷光OLED混合主体材料，两种主体材料的混合平衡了载流子的传输，减少了剩余极化子的产生，制备的OLED器件在1 000 cd/m"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "初始亮度下器件LT"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "70"
}
]
},
{
"name": "text",
"data": "寿命为1 113 h"
},
{
"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": "。"
}
]
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "3 聚合物LED本征老化机制"
}
],
"level": "1",
"id": "s3"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "目前市场中的商用OLED显示屏都是由绿光、红光磷光小分子以及蓝光荧光小分子OLED制成，采用真空蒸镀技术，面临生产成本高、难以大面积、大规模生产等问题。随着有机平板显示市场份额逐年增大，为适应工业界大面积、规模化、低成本的生产需要，可溶液加工的聚合物发光二极管受到广泛关注"
},
{
"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": "。由于小分子OLED结构复杂，包含许多界面，器件老化的物理过程很难阐明；而PLED仅由夹在两个电极之间的空穴注入层、聚合物发光层组成，器件结构简单，可对其器件内部机理进行详细深入的研究。下文将对其本征老化机理展开综述。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "关于材料的化学降解，在2.1节已经大量概括了小分子OLED关于这方面的研究，聚合物材料也有类似的老化机理。有研究表明光氧化导致了聚合物中链断裂以及末端醛基生成。聚合物中这些缺陷通过电荷转移机制来解离激子，从而导致光致发光的衰减"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "52",
"type": "bibr",
"rid": "R52",
"data": [
{
"name": "text",
"data": "52"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Gassmann等基于PPV及其衍生物体系，系统地综述了电应力条件下有机半导体的分子量、化学或结构缺陷对器件性能的影响。并特别指出PPV中卤素相关缺陷对器件使用寿命有较大的负面影响"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "53",
"type": "bibr",
"rid": "R53",
"data": [
{
"name": "text",
"data": "53"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Nicolai等通过研究一系列半导体聚合物，发现所有聚合物的电子陷阱能级分布都是相同的，陷阱密度为3×10"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "23 "
}
]
},
{
"name": "text",
"data": "m"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-3"
}
]
},
{
"name": "text",
"data": "，陷阱能级位于-3.6 eV，陷阱态分布宽度为0.1 eV。这说明电子陷阱有一个共同的来源。推测其可能的来源，包括光氧化产物、卤素缺陷、水氧络合物。通过量子化学计算表明，水氧络合物可能是半导体聚合物中电子陷阱的起源。于是通过降低N型材料的最低未占轨道（LUMO）至-3.6 eV以下，则可以获得环境稳定的有机材料"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "54",
"type": "bibr",
"rid": "R54",
"data": [
{
"name": "text",
"data": "54"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "在早期的工作中，Parker等分别研究了基于OC"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "1"
}
]
},
{
"name": "text",
"data": "C"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "10"
}
]
},
{
"name": "text",
"data": "-PPV的单空穴器件以及单电子器件，发现单载流子器件在长时间运行条件下空穴迁移率没有明显变化，而电子迁移率降低，说明电子传输退化是引起PLED老化的关键过程。并根据这一现象推测老化过程中电子迁移率的降低是源于电子陷阱的生成"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "55",
"type": "bibr",
"rid": "R55",
"data": [
{
"name": "text",
"data": "55"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Slivestre等提出在恒流电应力作用下器件亮度降低、电压增加有一个共同起源，即陷阱的形成。陷阱作为非辐射复合中心，导致器件亮度下降；陷阱还增加了空间电荷，导致驱动电压的增加。作者还推导了器件在恒电流条件下运行过程中电压增加和亮度减小的第一近似模型，成功拟合了亮度、电压与时间的依赖关系"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "56",
"type": "bibr",
"rid": "R56",
"data": [
{
"name": "text",
"data": "56"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。2003年，Kim等采用原位拉曼光谱学研究了基于三芳胺基为核心的PFB的蓝光聚合物发光二极管的老化过程。研究发现PFB与PEDOT∶PSS之间发生了不可逆的电化学氧化，产生了稳定的带阳离子PFB分子，这一带电物质在激子扩散范围内称为发光猝灭中心，并且阻碍了空穴的注入，导致低驱动电压下电流密度显著降低"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "57",
"type": "bibr",
"rid": "R57",
"data": [
{
"name": "text",
"data": "57"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Stegmaier等通过使用飞行时间法（TOF）、线性增压载流子抽取法（CELIV）研究了多种PPV PLED老化前后的空穴传输，发现老化后PPV空穴迁移率降低，空穴迁移率与电压依赖性增强，空穴的色散传输特性增强。结合高斯无序模型，空穴传输的变化说明了材料无序度的增加，态密度分布宽度增大。同时通过实验验证了空穴传输仅在电子存在时退化，推测可能的原因是空穴陷阱的形成"
},
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"data": "["
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"data": {
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"type": "bibr",
"rid": "R58",
"data": [
{
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"data": "58"
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]
}
},
{
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"data": "]"
}
]
},
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"name": "text",
"data": "。以上研究进展多次提到了空穴陷阱的形成是老化的本征老化机制，但并未证实。近年来，PLED中电荷注入理论、电荷传输理论和郎之万复合、陷阱辅助复合理论成熟，单层PLED的器件模型已经基本完善，可以定量地描述未老化前PLED的电流密度-电压-亮度特性"
},
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"data": "["
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"data": {
"text": "59",
"type": "bibr",
"rid": "R59",
"data": [
{
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"data": "59"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Niu等的研究结合实验和器件物理模型证明了PLED的本征老化机理是由空穴陷阱导致，并对其进行一系列的量化，将空穴陷阱的形成与激子及极化子的相互作用联系起来，为实现高稳定性的聚合物发光二极管器件提供了理论指导"
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{
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"data": "["
},
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"data": [
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"data": {
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"type": "bibr",
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"data": "Niu等基于扩展高斯无序模型、漂移-扩散模型建立了SY-PPV PLED器件物理模型，其中载流子迁移率依赖于电场、温度以及载流子浓度，并将被陷阱捕获电子与自由空穴的陷阱辅助复合考虑在内"
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"data": {
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]
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"data": "。通过单载流子器件的电流密度与电压依赖性可以拟合得到迁移率、陷阱密度、陷阱能级分布等参数。在双载流子PLED器件中，需要考虑到两种复合过程，包括双分子型复合以及陷阱辅助复合，来描述PLED的电流密度以及光输出。器件效率与电压依赖性的模拟还需考虑阴极对激子的猝灭。通过以上方法建立了一个统一的描述未老化SY-PPV PLED的器件模型"
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"data": [
{
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}
},
{
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}
]
},
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"data": "。"
}
]
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"data": [
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"name": "text",
"data": "为建立老化后PLED统一的器件物理模型，需要分别改变器件参数，如注入势垒、载流子迁移率、电子陷阱、空穴陷阱等物理参量进行数据模拟来研究每一种物理参量对PLED退化的影响。由于光电转换效率与迁移率无依赖关系，首先排除了迁移率下降对器件效率的影响。其次，在实验中老化后器件未观察到内置电压"
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{
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"data": "V"
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},
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]
},
{
"name": "text",
"data": "（阴极与阳极功函数之差）降低现象，从而排除了注入势垒对器件老化的影响。随后通过在模拟中提高电子陷阱密度来研究电子陷阱的形成对PLED电学特性的影响。研究发现电子陷阱的增加对PLED电流电压特性影响较小，与实验结果不相符，电子陷阱增多假设无法解释老化现象。"
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]
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"data": [
{
"name": "text",
"data": "对比单空穴器件与老化后双载流子器件电流，可以发现老化后双载流子器件电流远低于空穴电流，这说明老化过程中空穴传输退化"
},
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"data": [
{
"name": "text",
"data": "["
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{
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"data": {
"text": "63",
"type": "bibr",
"rid": "R63",
"data": [
{
"name": "text",
"data": "63"
}
]
}
},
{
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"data": "]"
}
]
},
{
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"data": "。瞬态电致发光测试再次验证了老化过程中空穴传输的减少。于是在器件物理模型中引入空穴陷阱，并将被空穴陷阱捕获的空穴与自由电子的非辐射性复合考虑进去，得到陷阱辅助复合因子如"
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"data": "所示，包括电子陷阱（"
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"data": "）和空穴陷阱（"
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{
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"data": "考虑以上所有因素得到的器件物理模型可以有效地描述老化后PLED的电流密度、光电转换效率与电压的依赖性，验证了空穴陷阱的形成是导致PLEDs老化中电压升高、效率降低的关键原因"
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"type": "bibr",
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"data": " ，老化后器件工作原理如"
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"data": "所示。该器件物理模型为进一步量化空穴陷阱、明晰PLEDs的本征老化机理奠定了基础。"
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"data": "老化后PLED器件工作原理，复合过程包含辐射双分子复合过程以及电子陷阱和空穴陷阱发生的非辐射陷阱辅助复合过程。"
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"title": [
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"data": "Schematic representation of aged PLED device， three types of recombination processes are included： radiative Langevin recombination between free carriers， non-radiative trap-assisted recombination between trapped-electrons and free holes and trap-assisted recombination between trapped-holes and free electrons."
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"data": "PLED在电应力的作用下驱动电压升高现象与空穴陷阱捕获电荷形成空间电荷有直接关系。利用老化后PLED的器件物理模型可以拟合出恒流应力下不同驱动电压对应的空穴陷阱"
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"data": "），建立空穴陷阱密度与老化时间和电流的对应关系。研究发现老化前期空穴陷阱数量与时间成线性增加关系，老化后期与时间的0.5次方成线性关系。如"
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"data": "所示。利用器件模型模拟不同电流密度驱动下亮度随老化时间的变化，拟合效果较好，说明空穴陷阱形成理论可以将老化期间电压增加现象与被陷阱捕获的空穴非辐射复合导致的亮度损失联系起来"
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"data": "阻抗电容测试可以定量地检测老化后器件内部的陷阱密度，研究证实PLED器件在低频下观察到微分电容的负贡献来源于陷阱辅助复合"
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"data": "。而在恒电流应力下老化后得到器件随老化时间的增加负电容现象逐渐增强，并根据微分电容公式中弛豫时间计算的空穴陷阱浓度与上述器件物理模型中拟合得到的结果一致，这为支持上述老化理论提供了实验基础"
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"data": "为了进一步探究空穴陷阱形成的物理机制，从空穴陷阱形成速率入手，探究空穴陷阱与电流密度的幂律关系。由上述实验所观察到的经验公式"
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"data": "，结合激子密度与电流密度关系，推导得到空穴陷阱形成速率为："
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"data": "从上述公式观察到陷阱形成速率与激子密度与空穴浓度的乘积成正比，从而提出激子与空穴的相互作用导致空穴陷阱形成的老化理论。并通过对单空穴器件施加光应力实验进一步证明了激子与空穴同时存在是器件老化的必要因素，激子与自由空穴的相互作用导致空穴陷阱形成，造成器件发光效率逐渐降低，电压逐渐升高"
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{
"name": "text",
"data": "。激子与极化子相互作用形成空穴陷阱，与2.2节所提到的机制类似，激子的能量被转移到空穴，随后被激发到更高的能量状态，其中一些“热分子”会通过直接解离的途径导致分子键断裂并产生副产物，可能直接作为空穴陷阱或者通过与相邻分子相互作用形成空穴陷阱。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "关于空穴陷阱具体是如何猝灭激子的问题，Rörich等采用蒙特卡洛模拟以及瞬态光致发光光谱（TRPL）实验做出了解答。TRPL测量表明，老化后的PLED表现出激子寿命降低。通过蒙特卡洛模拟，量化了老化后器件以非辐射复合猝灭激子的数量，结果发现模拟得到的激子猝灭数量与前文提到的器件物理模型拟合得到的空穴陷阱数量一致。说明电致发光的减少是通过被陷阱捕获空穴与自由电子非辐射复合主导的，而光致发光的激子猝灭的途径是激子向空穴陷阱扩散，可能通过空穴转移导致激子猝灭"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "62",
"type": "bibr",
"rid": "R62",
"data": [
{
"name": "text",
"data": "62"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "定量描述老化后的PLED性能，以及本征老化机制的科学问题已基本解决，但是导致器件老化的激子类型还有待研究。Zee等通过混合聚合物材料与合适的功能小分子，控制单线态和三线态激子的能量和寿命，分别研究了这两种激子对PLED老化的影响。研究发现，通过加入低浓度的荧光材料来降低单线态能量并不影响PLED的稳定性，而当加入长寿命的三线态分子器件稳定性则显著降低。此外，加入有TADF特性的有机分子，降低三线态寿命，成功提高了PLED寿命。通过漂移-扩散模型提取了各个老化时间下的空穴陷阱密度，结合双分子复合以及原有电子陷阱和生成的空穴陷阱的非辐射复合模拟得到光输出的数值，该数值与老化实验中亮度随老化时间的下降对比，有较好的一致性。拟合得到的空穴陷阱密度与电流密度、老化时间的依赖性再一次证明了三线态激子-极化子相互作用是陷阱形成的关键老化机制"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "66",
"type": "bibr",
"rid": "R66",
"data": [
{
"name": "text",
"data": "66"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。简单的PLED器件结构有利于老化器件性能的定量分析，加深对老化机制的理解，这将为阐明更复杂器件结构OLED中的老化机制奠定基础。"
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "3.3 PLEDs的稳定性提升策略"
}
],
"level": "2",
"id": "s3c"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "为提高器件稳定性，可以提高迁移率、降低器件内载流子浓度、减少空穴陷阱的生成。例如，BEH-PPV空穴迁移率为3×10"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-9 "
}
]
},
{
"name": "text",
"data": "m"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "·V"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "·s"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "，SY-PPV零电场下空穴迁移率为3×10"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-12 "
}
]
},
{
"name": "text",
"data": "m"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "·V"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "·s"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "-1"
}
]
},
{
"name": "text",
"data": "，BEH-PPV空穴迁移率远高于SY-PPV。在相同的电流密度下，BEH-PPV中所含的空穴浓度要低于SY-PPV，激子与空穴相互作用弱，BEH-PPV PLED相比于SY-PPV PLED表现出更高的稳定性"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "60",
"type": "bibr",
"rid": "R60",
"data": [
{
"name": "text",
"data": "60"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "降低激子寿命和密度也是提高PLED器件稳定性的有效方法之一。例如，聚（2,7-9,9-二辛基芴）（PFO）中混合双二苯胺基苯基蒽醌（AQ（PhDPA）"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "），AQ（PhDPA）"
},
{
"name": "sub",
"data": [
{
"name": "text",
"data": "2"
}
]
},
{
"name": "text",
"data": "是TADF类型的分子，三线态激子通过反向系间窜越转为单线态激子，有效降低了激子寿命，并减少了PLED中三线态激子数量，从而提高了器件的寿命"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "66",
"type": "bibr",
"rid": "R66",
"data": [
{
"name": "text",
"data": "66"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "提高器件稳定性的另一种方法则是消除陷阱对器件性能的影响。2016年，Abbaszadeh运用陷阱稀释的方法，同时降低传输位点和陷阱位点的浓度，即在聚合物半导体中混入具有较宽带隙的绝缘性聚合物，从而减少了电子陷阱捕获电荷现象，降低了陷阱辅助复合，有效提高了器件效率"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "67",
"type": "bibr",
"rid": "R67",
"data": [
{
"name": "text",
"data": "67"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。Niu等同样运用陷阱稀释效应，降低空穴陷阱的形成对电荷运输和器件效率的影响，器件的稳定性得到提高，驱动电压在老化过程中几乎不变"
},
{
"name": "sup",
"data": [
{
"name": "text",
"data": "["
},
{
"name": "xref",
"data": {
"text": "60",
"type": "bibr",
"rid": "R60",
"data": [
{
"name": "text",
"data": "60"
}
]
}
},
{
"name": "text",
"data": "]"
}
]
},
{
"name": "text",
"data": "。"
}
]
}
]
}
]
},
{
"name": "sec",
"data": [
{
"name": "sectitle",
"data": {
"title": [
{
"name": "text",
"data": "4 总结与展望"
}
],
"level": "1",
"id": "s4"
}
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "本综述讨论了小分子OLED以及聚合物OLED在电应力作用下的老化机理，虽然两种器件材料不同、器件结构不同，但是二者的老化机理存在一定的共性，都提到了材料的稳定性、激子与极化子的相互作用、陷阱的形成对器件稳定性的影响。小分子OLED结构复杂，难以建立统一的模型对其进行描述。而PLED结构简单，成熟的器件物理模型有利于量化相关陷阱参数，明晰器件本征老化机理，可以为小分子OLED中老化机制的研究提供理论方法。同时，高效率、长寿命的小分子OLED也能指导PLED效率以及寿命的提升。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "针对目前所提出的老化理论进行材料设计以及器件结构优化，对抑制器件运行过程中的老化具有重要意义。从材料设计出发，设计稳定的、短激发态寿命的发光材料有利于提高器件稳定性；设计稳定的、高载流子传输能力的电荷传输层可以减少电荷积累，促进电荷平衡，抑制激子与极化子的相互作用，从而提高器件寿命；设计稳定的、双极电荷运输特性的主体材料，可以有效控制复合区域，延长器件的寿命。从器件结构优化出发，通过梯度掺杂策略、混合N型、P型主体材料，可以促进电荷平衡，扩宽复合区域，抑制激子与极化子的猝灭效应，提高器件稳定性；通过陷阱稀释效应，弱化陷阱对器件效率的影响，可以延长器件寿命。"
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "本文专家审稿意见及作者回复内容的下载地址："
},
{
"name": "extlink",
"data": {
"text": [
{
"name": "text",
"data": "http://cjl.lightpublishing.cn/thesisDetails#10.37188/"
}
],
"href": "http://cjl.lightpublishing.cn/thesisDetails#10.37188/"
}
}
]
},
{
"name": "p",
"data": [
{
"name": "text",
"data": "CJL.20220317."
}
]
}
]
}
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"data": "牛泉,郝洪敏,林雯欣等.有机发光二极管老化机制[J].发光学报,2023,44(01):186-197."
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