通向钙钛矿电泵浦激光的研究进展 增强出版

{ "defaultlang": "zh", "titlegroup": { "articletitle": [ { "lang": "zh", "data": [ { "name": "text", "data": "通向钙钛矿电泵浦激光的研究进展" } ] }, { "lang": "en", "data": [ { "name": "text", "data": "Research Progress Towards Perovskite Electrical Driven Lasers" } ] } ] }, "contribgroup": { "author": [ { "name": [ { "lang": "zh", "surname": "魏", "givenname": "衍福", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "WEI", "givenname": "Yan-fu", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "" } ], "role": [ "first-author" ], "bio": [ { "lang": "zh", "text": [ "魏衍福（1995-），男，湖北十堰人，硕士研究生，2018年于长江大学获得学士学位，主要从事钙钛矿微型激光器方面的研究。 E-mail： 2413671678@qq.com" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471884&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471891&type=", "big": 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liguohui@tyut.edu.cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471896&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471905&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471900&type=", "width": "24.89199829", "height": "29.88732910", "fontsize": "" } ], "data": [ [ { "name": "text", "data": "李国辉" }, { "name": "text", "data": "（1984-），男，四川广元人，博士，副教授，硕士生导师，2011年于华东师范大学获得博士学位，主要从事包括钙钛矿激光器、表面等离激元纳米器件、有机及钙钛矿光电探测器等的研究。E‐mail: liguohui@tyut.edu.cn" } ] ] } ], "email": "liguohui@tyut.edu.cn", "deceased": false }, { "name": [ { "lang": "zh", "surname": "潘", "givenname": "登", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "PAN", "givenname": "Deng", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "" } ], "role": [], "deceased": false }, { "name": [ { "lang": "zh", "surname": "温", "givenname": 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"eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "" } ], "role": [ "corresp" ], "corresp": [ { "rid": "cor2", "lang": "en", "text": "yanxiacui@tyut.edu.cn", "data": [ { "name": "text", "data": "yanxiacui@tyut.edu.cn" } ] } ], "note": [ { "rid": "fna1", "lang": "zh", "text": "崔艳霞（1984-），女，山西吕梁人，博士，教授，博士生导师，2011年于浙江大学获得博士学位，主要从事包括表面等离激元纳米器件、有机及钙钛矿光电探测器及钙钛矿激光器等的研究。 E-mail： yanxiacui@tyut.edu.cn", "data": [ { "name": "text", "data": "崔艳霞（1984-），女，山西吕梁人，博士，教授，博士生导师，2011年于浙江大学获得博士学位，主要从事包括表面等离激元纳米器件、有机及钙钛矿光电探测器及钙钛矿激光器等的研究。 E-mail： yanxiacui@tyut.edu.cn" } ] } ], "bio": [ { "lang": "zh", "text": [ "李国辉（1984-），女，山西吕梁人，博士，教授，博士生导师，2011 年于浙江大学获得博士学位，主要从事包括表面等离激元纳米器件、有机及钙钛矿光电探测器及钙钛矿激光器等的研究。E-mail：yanxiacui@tyut. edu. cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471918&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471918&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471918&type=", "width": "24.89199829", "height": "29.88732910", "fontsize": "" } ], "data": [ [ { "name": "text", "data": "李国辉" }, { "name": "text", "data": "（1984-），女，山西吕梁人，博士，教授，博士生导师，2011 年于浙江大学获得博士学位，主要从事包括表面等离激元纳米器件、有机及钙钛矿光电探测器及钙钛矿激光器等的研究。E-mail：" }, { "name": "text", "data": "yanxiacui@tyut. edu. cn" } ] ] } ], "email": "yanxiacui@tyut. edu. cn", "deceased": false } ], "aff": [ { "id": "aff1", "intro": [ { "lang": "zh", "text": "太原理工大学 物理与光电工程学院， 山西 太原　030024", "data": [ { "name": "text", "data": "太原理工大学 物理与光电工程学院， 山西 太原　030024" } ] }, { "lang": "en", "text": "College of Physics and Optoelectronics， Taiyuan University of Technology， Taiyuan 030024， China", "data": [ { "name": "text", "data": "College of Physics and Optoelectronics， Taiyuan University of Technology， Taiyuan 030024， China" } ] } ] } ] }, "abstracts": [ { "lang": "zh", "data": [ { "name": "p", "data": [ { "name": "text", "data": "可溶液法制备的钙钛矿拥有优异的光学、电学性能，是一类极具潜力的电泵浦激光增益介质。近年来，基于钙钛矿材料的室温连续光泵浦激光以及大电流电致发光器件陆续被报道，在通向钙钛矿电泵浦激光的研究上取得了可喜进展，本文以此为主题展开综述。首先，介绍了钙钛矿材料实现电泵浦激光的优势。接着，梳理了现阶段通向钙钛矿电泵浦激光的两大问题，即非辐射复合损耗高和热效应严重，同时给出了改善这两大问题可采取的一些有效策略。然后，给出了电荷注入平衡化、降低光学损耗、促进粒子数反转等补充手段，它们有力推动了通向钙钛矿电泵浦激光研究向前发展。此外，还介绍了钙钛矿表面等离激元激光、钙钛矿激子极化激元激光等有望实现低阈值钙钛矿电泵浦激光的新机制。最后，总结全文，并对电泵浦钙钛矿激光未来研究做出了展望。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "Solution-processed perovskites， having excellent optical and electrical properties， can serve as a kind of promising electrically driven laser gain medium. In recent years， progresses towards electrically driven lasers based on perovskite materials have been made. For instance， a series of room-temperature continuous-wave optically-pumped perovskite lasers along with a few high-current perovskite light emitting diodes（LEDs） have been reported. This paper takes this topic as the review subject. Firstly， the advantages of perovskite materials for developing electrical driven lasers are introduced. Then， the two major constraints towards electrical driven perovskite lasers at the present stage， including high non-radiative recombination loss and serious thermal effect， are introduced， and some strategies to break through these constraints are given. Subsequently， this paper gives supplementary means such as balancing the charge injection， reducing optical loss， and promoting population inversion， which have effectively promoted the development of perovskite electrical pumped laser research. This paper also introduces the recent progresses of surface plasmon polariton lasers， exciton polariton lasers， " }, { "name": "italic", "data": [ { "name": "text", "data": "etc" } ] }, { "name": "text", "data": ".， based on perovskite materials， which possess the potential to reduce the laser thresholds， as alternatives for realizing electrical driven perovskite lasers. Finally， the full text is summarized， and the future research towards electrical driven perovskite lasers is prospected." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "钙钛矿" } ], [ { "name": "text", "data": "激光器" } ], [ { "name": "text", "data": "电泵浦" } ], [ { "name": "text", "data": "激光阈值" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "perovskite" } ], [ { "name": "text", "data": "laser" } ], [ { "name": "text", "data": "electrical driven" } ], [ { "name": "text", "data": "lasing threshold" } ] ] } ], "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": "微型激光器，特别是微型电泵浦激光器，在光通信" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "1", "type": "bibr", "rid": "R1", "data": [ { "name": "text", "data": "1" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、光计算" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "2", "type": "bibr", "rid": "R2", "data": [ { "name": "text", "data": "2" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、光存储" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "3", "type": "bibr", "rid": "R3", "data": [ { "name": "text", "data": "3" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "等领域具有十分重要的研究价值。最早被用于太阳电池的钙钛矿半导体材料，由于可通过溶液法制备出缺陷态密度极低的晶体，且具有光吸收系数高、载流子扩散距离长、发光效率高等特性，在发光二极管（Light emitting diode，LED）、激光领域引起了研究人员的广泛关注" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "4", "type": "bibr", "rid": "R4", "data": [ { "name": "text", "data": "4" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "5", "type": "bibr", "rid": "R5", "data": [ { "name": "text", "data": "5" } ] } } ], "rid": [ "R4", "R5" ], "text": "4-5", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。自2014年Xing等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "6", "type": "bibr", "rid": "R6", "data": [ { "name": "text", "data": "6" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "报道了钙钛矿材料中脉冲光泵浦的放大的自发辐射（Amplified spontaneous emission，ASE）以来，基于钙钛矿纳米片" }, { "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": "、钙钛矿纳米线" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "8", "type": "bibr", "rid": "R8", "data": [ { "name": "text", "data": "8" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、以及钙钛矿分布式反馈（Distributed feedback，DFB）" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "9", "type": "bibr", "rid": "R9", "data": [ { "name": "text", "data": "9" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、钙钛矿分布式布拉格反射（Distributed Bragg reflection，DBR）" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、钙钛矿光子晶体" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "11", "type": "bibr", "rid": "R11", "data": [ { "name": "text", "data": "11" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "等结构形式的激光器中均实现了低阈值脉冲光泵浦激光。并且，钙钛矿的高密度光泵浦激光器阵列以及光子集成器件也陆续被报道" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "12", "type": "bibr", "rid": "R12", "data": [ { "name": "text", "data": "12" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，为开发钙钛矿电泵浦激光奠定了良好的基础。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "要实现钙钛矿电泵浦激光，首先需要实现钙钛矿材料在连续（Continuous-wave, CW）光泵浦下的激光输出。低温下CW泵浦的ASE以及激光的实现，推进了钙钛矿电泵浦激光器的研制。最近，钙钛矿CW光泵浦激光的工作温度进一步提高到了室温" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。并且，CW光泵浦的极化激元激光也被报道" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "14", "type": "bibr", "rid": "R14", "data": [ { "name": "text", "data": "14" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "15", "type": "bibr", "rid": "R15", "data": [ { "name": "text", "data": "15" } ] } } ], "rid": [ "R14", "R15" ], "text": "14-15", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，通过该机制有望实现阈值更低的钙钛矿电泵浦激光。钙钛矿电泵浦激光的原理类似LED，空穴与电子从电极两端注入至钙钛矿内辐射复合发出光子，额外引入谐振腔对光学模式进行选择，便可产生激光。根据CW光泵浦下激光输出时钙钛矿材料中光生载流子的浓度，可以预估出其产生电泵浦激光阈值载流子浓度下限" }, { "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": "。据预测，电泵浦激光的阈值载流子浓度应当比CW泵浦下激光输出时的光生载流子浓度至少高出一个数量级" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "15", "type": "bibr", "rid": "R15", "data": [ { "name": "text", "data": "15" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "17", "type": "bibr", "rid": "R17", "data": [ { "name": "text", "data": "17" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，通向电泵浦激光研究中的一个重要前提是实现大电流工作钙钛矿LED。目前，钙钛矿LED的外量子效率（EQE）已经超过20%" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "18", "type": "bibr", "rid": "R18", "data": [ { "name": "text", "data": "18" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。在钙钛矿LED的EQE滚降前，器件对电流的承受能力从最开始报道的数百mA·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "已经提升到了数千A·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "19", "type": "bibr", "rid": "R19", "data": [ { "name": "text", "data": "19" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } } ], "rid": [ "R19", "R20" ], "text": "19-20", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。值得一提的是，近期研究人员将光栅结构与电注入结构相结合，虽然并未实现电泵浦激光，但研究表明该器件允许的工作电流高达10 kA·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "，对应的注入载流子浓度为7.5 × 10" }, { "name": "sup", "data": [ { "name": "text", "data": "17" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "，与该器件实现光泵浦激光的载流子浓度十分接近（7.97× 10" }, { "name": "sup", "data": [ { "name": "text", "data": "17" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "）" }, { "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": "。这些进展为电泵浦钙钛矿激光器的研制铺平了道路。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本文以通向钙钛矿电泵浦激光研究进展为主题展开综述。首先，介绍了钙钛矿材料实现电泵浦激光的优势。接着，梳理了现阶段通向钙钛矿电泵浦激光的两大主要制约因素，即非辐射复合损耗高与热效应严重，并给出了研究人员为改善这些问题所采取的一些有效策略。然后，给出了平衡电荷注入、降低光学损耗、促进粒子数反转等补充措施，它们对于降低激光阈值十分有益。此外，还介绍了表面等离激元、极化激元激光等新机制钙钛矿激光器，它们的阈值更低，为钙钛矿电泵浦激光的实现提供了更大的可能性。最后，总结全文，并对通向电泵浦钙钛矿激光研究的未来做出了展望。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2　钙钛矿实现电泵浦激光的优势" } ], "level": "1", "id": "s2" } }, { "name": "p", "data": [ { "name": "text", "data": "钙钛矿材料作为一类新兴的激光增益介质，从众多可溶液法制备的低成本半导体材料中脱颖而出。较之无机胶体纳米晶材料或有机半导体材料，钙钛矿材料凭借电学、光学方面的性能指标，有望开发出性能更优越的电泵浦激光。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "首先，钙钛矿材料的缺陷态密度低于无机胶体纳米晶，最低达到10" }, { "name": "sup", "data": [ { "name": "text", "data": "8" } ] }, { "name": "text", "data": "量级" }, { "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": "。因此，钙钛矿材料具有更低的非辐射复合损耗与激光阈值。众所周知，半导体材料的强激子结合能、短激子扩散长度会导致激子-激子湮灭的发生，不利于激光的发射。该问题在有机半导体材料中尤为显著，如单重态激子-三重态激子湮灭现象。研究表明，准二维、二维钙钛矿材料中也会存在这类激子-激子湮灭现象" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。不过，准二维、二维钙钛矿材料的激子扩散长度较之有机半导体材料大一至两个数量级，对激子-激子湮灭有一定的抑制效果" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "22", "type": "bibr", "rid": "R22", "data": [ { "name": "text", "data": "22" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。三维钙钛矿材料相对于有机半导体材料，具有更低的激子结合能，因而其激子浓度较低，相应地，其激子-激子湮灭几率也较低" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "22", "type": "bibr", "rid": "R22", "data": [ { "name": "text", "data": "22" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。目前，在三维钙钛矿材料中，尚未发现有关三重态激子的湮灭损耗问题。此外，CsPb" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿材料中的三重态激子表现出极快的辐射发光速率，这使得受激辐射过程较之非辐射复合过程具有更高的竞争力" }, { "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": "。相比而言，无机半导体材料中的三重态激子普遍呈“暗态”，不具有辐射复合发光的能力" }, { "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": "。基于该特性有望开发出高性能激光器件。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "另外，较之有机半导体材料，钙钛矿的载流子迁移率更高，这有助于降低电注入器件中载流子的传导损耗，提高载流子注入效率。已有报道表明，CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿胶体纳米晶的载流子迁移率高达 4 500 cm" }, { "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": "xref", "data": { "text": "24", "type": "bibr", "rid": "R24", "data": [ { "name": "text", "data": "24" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，接近Ⅲ-Ⅴ族无机半导体材料的相应指标。并且，钙钛矿材料中的光学增益极高，已经达到3 000 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "–1[" }, { "name": "xref", "data": { "text": "25", "type": "bibr", "rid": "R25", "data": [ { "name": "text", "data": "25" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，并不逊色于无机半导体材料，且远高于有机半导体材料中已实现的光学增益，保证了优良的光放大效果。这些都进一步铺平了通向钙钛矿电泵浦激光的道路。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3　通向钙钛矿电泵浦激光的主要矛盾及缓解策略" } ], "level": "1", "id": "s3" } }, { "name": "p", "data": [ { "name": "text", "data": "钙钛矿CW光泵浦激光的实现，验证了该材料具有维持激光输出所需的极高光增益的能力。不过，同样暴露出了以高非辐射复合损耗、大的热效应为主的限制激光器件运转的问题。这些问题在电泵浦激光中变得更为严重。根据伯纳德-杜拉福德（Bernard-Duraffourg）条件，钙钛矿材料在室温下要实现激射，要求载流子浓度至少在10" }, { "name": "sup", "data": [ { "name": "text", "data": "18" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "以上" }, { "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": "。为了达到这个值，钙钛矿激光器的注入电流密度" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "与EQE（" }, { "name": "italic", "data": [ { "name": "text", "data": "η" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "EQE" } ] }, { "name": "text", "data": "）的乘积需要达到一定的阈值。在材料辐射复合系数一定的情况下，注入载流子浓度的平方与器件的" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "×" }, { "name": "italic", "data": [ { "name": "text", "data": "η" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "EQE" } ] }, { "name": "text", "data": "成正比" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "27", "type": "bibr", "rid": "R27", "data": [ { "name": "text", "data": "27" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } } ], "rid": [ "R27", "R28" ], "text": "27-28", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，理论可预测" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "×" }, { "name": "italic", "data": [ { "name": "text", "data": "η" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "EQE" } ] }, { "name": "text", "data": "的阈值超过100 A·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2[" }, { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。在电荷平衡注入情况下" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "th" } ] }, { "name": "text", "data": "与" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "成正比，" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "需要在1 kA·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "以上" }, { "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": "，这使得器件会因为焦耳加热而工作在更高的温度。目前，在大工作电流的钙钛矿发光器件中，过高的非辐射复合损耗与严重的热效应共同降低了材料内部的电-光转换效率，使更多能量被转化为热量而进一步加剧了热效应，最终对器件造成不可逆的损伤。这两个方面构成了制约钙钛矿电泵浦激光实现的核心矛盾，研究人员针对这些问题开展了深入的研究并提出了一些有效的应对策略。" } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.1　非辐射复合损耗及其抑制" } ], "level": "2", "id": "s3a" } }, { "name": "p", "data": [ { "name": "text", "data": "在钙钛矿材料中，光生载流子的衰减满足以下公式：" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（1）" } ], "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471942&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471938&type=", "width": "41.82533264", "height": "7.36600018", "fontsize": "" } } }, { "name": "text", "data": "，" } ], "id": "DF1" } }, { "name": "p", "data": [ { "name": "text", "data": "其中" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "为光生载流子密度，" }, { "name": "italic", "data": [ { "name": "text", "data": "G" } ] }, { "name": "text", "data": "为产生项。" }, { "name": "italic", "data": [ { "name": "text", "data": "k" }, { "name": "sub", "data": [ { "name": "text", "data": "i" } ] } ] }, { "name": "text", "data": "，" }, { "name": "italic", "data": [ { "name": "text", "data": "i" } ] }, { "name": "text", "data": "=1，2，3分别描述俘获在势阱中的单个载流子（电子或空穴）发生复合的几率、内禀的电子-空穴辐射复合几率、俄歇复合发生的几率。其中，陷阱辅助的单分子复合和俄歇复合组成了非辐射复合。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "钙钛矿材料中，表面电荷陷阱主要表现为元素空位、Pb" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "失配等具有低形成能的点缺陷，比体缺陷态密度更高" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "6", "type": "bibr", "rid": "R6", "data": [ { "name": "text", "data": "6" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "30", "type": "bibr", "rid": "R30", "data": [ { "name": "text", "data": "30" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，钙钛矿与相邻材料的界面处发生的陷阱复合更为严重。为了降低表面陷阱态密度，除了严格控制钙钛矿化学计量比，还可以对钙钛矿的表面缺陷加以钝化" }, { "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": "。目前，在钙钛矿材料表面引入的钝化剂种类大致分为有机、有机-无机杂化、无机三种类型。在大电流电致发光（EL）器件中，前两类钝化剂不适宜引入（如环氧树脂、PMMA、PEABr等），因为它们的导电性较差。相比而言，金属卤化物 （如PbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "、K" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "text", "data": "，" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "text", "data": "=Cl, Br, I等）" }, { "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": " 以及硫氰酸盐（NaSCN、NH" }, { "name": "sub", "data": [ { "name": "text", "data": "4" } ] }, { "name": "text", "data": "SCN ）" }, { "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": "等结构小的全无机化合物钝化剂，在有效钝化了缺陷的前提下，保证了良好的电荷传输性能。2020年，Zou等" }, { "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": "在LED中引入PEABr及KBr分别作为CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "的钝化剂。在施加同等电压时，添加KBr器件的电流密度相对更高。还需指出的是，钝化剂的引入有可能造成钙钛矿的EL猝灭。最近，Zhao等" }, { "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": "发现引入KI的MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": " 的大电流LED中出现了反常的EL猝灭现象。他们认为这可能是在KI参与下，外加电场诱发了I" }, { "name": "sup", "data": [ { "name": "text", "data": "–" } ] }, { "name": "text", "data": "以及I" }, { "name": "sup", "data": [ { "name": "text", "data": "3-" } ] }, { "name": "text", "data": "从钙钛矿层中扩散至邻近材料中，产生了电荷陷阱。总之，为了有效地抑制钙钛矿材料中的单分子复合，引入钝化剂十分必要，但必须通过钝化剂的优选以最小化它们对EL过程所造成的负面影响。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "俄歇复合被认为是钙钛矿LED器件中导致EQE滚降的主要原因之一。当三维钙钛矿材料中的载流子浓度达到10" }, { "name": "sup", "data": [ { "name": "text", "data": "16" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "量级时，会出现俄歇复合，如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "（a）所示" }, { "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": "；注入载流子浓度大于10" }, { "name": "sup", "data": [ { "name": "text", "data": "18" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "时，俄歇复合将占据载流子总复合的50%以上，成为主要的非辐射复合通道" }, { "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": "。在大电流密度下，载流子浓度上升所导致的俄歇复合变得更加严重。研究表明，钙钛矿LED在大电流下的EQE较之小电流下会降低一到两个数量级" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } }, { "name": "text", "data": "," }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "27", "type": "bibr", "rid": "R27", "data": [ { "name": "text", "data": "27" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } } ], "rid": [ "R27", "R28" ], "text": "27-28", "type": "bibr" } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "34", "type": "bibr", "rid": "R34", "data": [ { "name": "text", "data": "34" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "（a）三维钙钛矿中不同的载流子复合机制（辐射复合、缺陷辅助复合、俄歇复合）对应的载流子寿命随注入载流子浓度变化的关系曲线" }, { "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": "；（b）准二维钙钛矿中的单重态激子与三重态激子的能量转移过程" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.1" } ], "title": [ { "name": "text", "data": "（a）Carrier lifetime corresponding to different carrier recombination mechanisms（radiation recombination， defect assisted recombination， Auger recombination） varies with the injected carrier density in 3D perovskite" }, { "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": ". （b）Energy transfer process of singlet excitons and triplet excitons in quasi-2D perovskite of （NMA/PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "FA" }, { "name": "italic", "data": [ { "name": "sub", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "sub", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "italic", "data": [ { "name": "sub", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "italic", "data": [ { "name": "sub", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "sub", "data": [ { "name": "text", "data": "+1" } ] }, { "name": "text", "data": "， " }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "=8" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471945&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471950&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471947&type=", "width": "152.78582764", "height": "39.45811462", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "高的俄歇复合几率通常与特殊的能带结构相关联。首先，大的自旋-轨道耦合会使导带能级发生分裂，当分裂能级与导带底的能量差（即分裂能）小于或等于材料带隙能量时，复合过程会促成载流子落入这些分裂能级而非辐射光子，对应较高的俄歇复合损耗" }, { "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": "39", "type": "bibr", "rid": "R39", "data": [ { "name": "text", "data": "39" } ] } } ], "rid": [ "R38", "R39" ], "text": "38-39", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。其次，晶格畸变打破了自旋简并，导致带边自旋简并带发生Rashba分裂，新的分裂能级可以参与俄歇复合，进而俘获载流子" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "40", "type": "bibr", "rid": "R40", "data": [ { "name": "text", "data": "40" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "41", "type": "bibr", "rid": "R41", "data": [ { "name": "text", "data": "41" } ] } } ], "rid": [ "R40", "R41" ], "text": "40-41", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。在MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "这样一种典型的钙钛矿材料中，上述两种能带结构情形均有报道，且由自旋-轨道耦合引发的俄歇复合比由晶格畸变引发的更为严重" }, { "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": "。对于前者，可参考传统无机半导体材料中的策略，通过掺入重金属原子，将分裂能提高到带隙能之上来缓解" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "39", "type": "bibr", "rid": "R39", "data": [ { "name": "text", "data": "39" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。对于后者，可以通过优化晶格结构来应对。立方相钙钛矿材料具有更加稳定的晶格结构。2019年，Ščajev等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "42", "type": "bibr", "rid": "R42", "data": [ { "name": "text", "data": "42" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "通过组分工程将Cs离子添加入混合离子钙钛矿中，获得了几近理想立方相的晶格结构，稳定了能带，弱化了Rashba分裂，有效抑制了俄歇复合。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "在准二维钙钛矿中，由于载流子迁移（参见第4.2节）引发局部载流子浓度升高，因此其俄歇复合损耗较之三维钙钛矿更为严重" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "43", "type": "bibr", "rid": "R43", "data": [ { "name": "text", "data": "43" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。另外，准二维钙钛矿通常具有大的激子结合能，因此电子与空穴库仑作用力较强，所以电性相反的两种载流子更易发生聚集，提高俄歇复合几率" }, { "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": "。2021年， Jiang等在基于PEA有机阳离子的二维钙钛矿中，通过氟取代增强了PEA阳离子的极性，弱化了电子-空穴间的库仑相互作用，进而降低了激子结合能，使俄歇复合几率降低了一个数量级" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "43", "type": "bibr", "rid": "R43", "data": [ { "name": "text", "data": "43" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "需要指出的是，准二维钙钛矿中由于引入了有机阳离子基团，其激子中包含了大量的三重态激子" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "45", "type": "bibr", "rid": "R45", "data": [ { "name": "text", "data": "45" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "46", "type": "bibr", "rid": "R46", "data": [ { "name": "text", "data": "46" } ] } } ], "rid": [ "R45", "R46" ], "text": "45-46", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，这与有机半导体中的情形一致。由于三重态激子的寿命较长（20~50 ns）" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "45", "type": "bibr", "rid": "R45", "data": [ { "name": "text", "data": "45" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，这也促成了它们的大量累积。三重态激子的累积不仅会对单重态辐射复合发出光子产生负面的重吸收效应，并且会与单重态激子发生激子-激子湮灭，严重降低发光效率。在谐振腔中，三重态寿命会进一步延长" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "45", "type": "bibr", "rid": "R45", "data": [ { "name": "text", "data": "45" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。最终，单重态激子密度不断降低，直至激射停止" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "因此，在准二维钙钛矿电注入器件中，对三重态激子进行有效管理是实现电泵浦激光的前提。2020年，Qin等设计了一种能够对三重态激子实施优化管理的措施，基于此制成的准二维钙钛矿LED性能优越，并且实现了室温CW光泵浦的单重态激子激光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "47", "type": "bibr", "rid": "R47", "data": [ { "name": "text", "data": "47" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。他们对三重态激子管理的本质是利用不同能量转移机制实现了单重态激子与三重态激子在空间上的分离，具体原理如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "（b）所示，其中引入NMA/PEA有机配体的材料为" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "=8的NMA" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "FA" }, { "name": "italic", "data": [ { "name": "sub", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "sub", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "italic", "data": [ { "name": "sub", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "italic", "data": [ { "name": "sub", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "sub", "data": [ { "name": "text", "data": "+1" } ] }, { "name": "text", "data": "（N2F8）及PEA" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "FA" }, { "name": "italic", "data": [ { "name": "sub", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "sub", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "italic", "data": [ { "name": "sub", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "italic", "data": [ { "name": "sub", "data": [ { "name": "text", "data": "n" } ] } ] }, { "name": "sub", "data": [ { "name": "text", "data": "+1" } ] }, { "name": "text", "data": "（P2F8）。单重态激子的转移过程参见4.2节的描述，它们转移至最大的" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "值域后辐射发出光子。对于三重态激子来说，由于[PbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "6" } ] }, { "name": "text", "data": "]" }, { "name": "sup", "data": [ { "name": "text", "data": "4–" } ] }, { "name": "text", "data": "的单/三重态能级低于PEA的三重态能级、高于NMA的三重态能级，因此，[PbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "6" } ] }, { "name": "text", "data": "]" }, { "name": "sup", "data": [ { "name": "text", "data": "4–" } ] }, { "name": "text", "data": "中的三重态能量更易通过直接交换电子的方式（即Dexter能量转移）转移至NMA中，而非PEA。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.2　热效应及其优化" } ], "level": "2", "id": "s3b" } }, { "name": "p", "data": [ { "name": "text", "data": "钙钛矿材料的热导率普遍较低，通常在1 W·m" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "·K" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "以下。例如，MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "的热导率约为0.5 W·m" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "·K" }, { "name": "sup", "data": [ { "name": "text", "data": "-1[" }, { "name": "xref", "data": { "text": "48", "type": "bibr", "rid": "R48", "data": [ { "name": "text", "data": "48" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。低热导率引发热量累积，造成器件温度大幅升高。在电泵浦条件下，激光阈值处器件的温升Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "=" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "s" } ] }, { "name": "text", "data": "（" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "J" } ] }, { "name": "italic", "data": [ { "name": "text", "data": "I" } ] }, { "name": "text", "data": "+" }, { "name": "italic", "data": [ { "name": "text", "data": "RI" } ] }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "）" }, { "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": "，其中" }, { "name": "italic", "data": [ { "name": "text", "data": "I" } ] }, { "name": "text", "data": "为注入电流，" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "s" } ] }, { "name": "text", "data": "为器件的等效热阻，" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "为结压。依据该公式，注入电流越大，器件升温越高。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "发光过程会造成钙钛矿器件温度升高；反过来，温度升高又会导致其EL性能的严重退化。究其原因，温度上升导致钙钛矿材料中空穴与电子发生复合的几率下降" }, { "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": "。2021年，Allegro等" }, { "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": "测试了混合离子钙钛矿薄膜的双分子复合系数与温度之间的关系曲线，如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "（a）所示，二者满足" }, { "name": "italic", "data": [ { "name": "text", "data": "k" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471953&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471951&type=", "width": "2.37066650", "height": "2.62466669", "fontsize": "" } } } ] }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "sup", "data": [ { "name": "text", "data": "-3/2" } ] }, { "name": "text", "data": "的关系。此外，温度升高导致材料需要更高的注入载流子浓度以满足粒子数反转条件。2019年，Jia等" }, { "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": "发现MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿激光的阈值载流子浓度随温度升高而非线性升高，如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "（b）所示。总而言之，温度升高既降低了发光效率，又抬升了激光阈值，甚至会造成激光“死亡”，即激射在持续一段时间后停止" }, { "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": "53", "type": "bibr", "rid": "R53", "data": [ { "name": "text", "data": "53" } ] } } ], "rid": [ "R52", "R53" ], "text": "52-53", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。例如，Jia等的研究表明，基于MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿材料的CW光泵浦，在持续100 ns左右便出现了激光“死亡”现象。当泵浦源为脉冲光时，由于瞬时能量更大，材料内部升温更快，发生激光死亡的时间更早（~25 ns）" }, { "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": "。经理论预测，以蓝宝石为散热基底的钙钛矿激光器件要避免激光死亡，其载流子浓度不能超过10" }, { "name": "sup", "data": [ { "name": "text", "data": "19" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "量级（如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "（c）所示），在" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "×" }, { "name": "italic", "data": [ { "name": "text", "data": "η" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "EQE" } ] }, { "name": "text", "data": "必须符合最低阈值的前提下，这一约束对器件的EQE又提出了更高的要求。显而易见，降低工作温度至室温以下，更有利于获得电泵浦激光。原因在于，第一，低温下电子填充更低的能态，更易达成粒子数反转；第二，低温下复合寿命延长且非辐射复合更低，有助于产生更大的载流子浓度。因此，早期的钙钛矿CW光泵浦激光大多工作在低温条件下" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "26", "type": "bibr", "rid": "R26", "data": [ { "name": "text", "data": "26" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "55", "type": "bibr", "rid": "R55", "data": [ { "name": "text", "data": "55" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。对于钙钛矿材料，低温下的电泵浦激光或当首先被突破。" } ] }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "温度对钙钛矿发光器件性能的影响规律。 （a）混合离子钙钛矿薄膜的双分子复合系数随温度的变化关系" }, { "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": "；（b）MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿的阈值载流子浓度随温度的变化关系" }, { "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": "；（c）蓝宝石/硅为衬底的不同钙钛矿器件在不同温度下的激光死亡阈值" }, { "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": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.2" } ], "title": [ { "name": "text", "data": "Effect of temperature on the performances of perovskite light emitting devices. （a）The bimolecular recombination coefficient of mixed ion perovskite films varies with temperature" }, { "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": ". （b）The threshold carrier density of MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": " perovskite varies with temperature" }, { "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": ". （c）Laser death thresholds of different perovskite devices based on sapphire and silicon substrates at different temperatures" }, { "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": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471956&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471960&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471958&type=", "width": "153.47198486", "height": "37.37193298", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "焦耳热同样也限制了钙钛矿激光器件的长期稳定性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "56", "type": "bibr", "rid": "R56", "data": [ { "name": "text", "data": "56" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "57", "type": "bibr", "rid": "R57", "data": [ { "name": "text", "data": "57" } ] } } ], "rid": [ "R56", "R57" ], "text": "56-57", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。已报道的钙钛矿CW光泵浦激光器的稳定工作时间均短于1 h。此外，高温条件下，光照、水、氧等的叠加作用，会进一步加剧钙钛矿材料的降解" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "58", "type": "bibr", "rid": "R58", "data": [ { "name": "text", "data": "58" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，诱发钙钛矿激光器失效的实际温度远低于其本身的升华温度" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "59", "type": "bibr", "rid": "R59", "data": [ { "name": "text", "data": "59" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。如对于MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "材料，这个温度低于358 K" }, { "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": "。对钙钛矿材料表面的悬挂键进行封装，有利于减轻钙钛矿在泵浦温升以及水、氧环境多重作用下导致的材料降解行为。例如，Li等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "61", "type": "bibr", "rid": "R61", "data": [ { "name": "text", "data": "61" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "在MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "纳米片的上方引入一种有机π-共轭小分子，即四苯基二苯并二茚并芘（DBP），封装了样品表面悬挂的Pb" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "键，减小了钙钛矿材料在泵浦工作时的降解速率，延长了其持续输出激光脉冲的时间。但是，封装层也会面临高温退化失效的问题" }, { "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": "因此，对于钙钛矿发光器件，抑制其在泵浦注入时的温升十分必要。两条途径可以实现该目的，即降低产热和提升散热。小器件尺寸有利于降低器件产热，更低重复频率、更短脉宽的泵浦源也有利于钙钛矿发光器件短时间升温后，有足够的间隔时间将热量弛豫掉。2018年，Kim等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "27", "type": "bibr", "rid": "R27", "data": [ { "name": "text", "data": "27" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "研究了脉冲型电泵浦源激励下LED器件的瞬态EL发光性能，其中有源区的半径较小（控制在200 μm以下）。他们发现，在注入电流为 203 A·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "–2" } ] }, { "name": "text", "data": " 、重复频率为389 Hz、脉冲宽度为2 μs条件下，电流密度在激励起始之后百纳秒时间内达到稳定。但激励持续时间在微秒尺度时，会引发50 K以上的器件温升，致使EL强度持续下降。他们的研究表明，若将脉冲宽度控制在百纳秒甚至更短尺度，器件产热将更匹配其散热能力，更有利于电泵浦激光的实现。需要指出的是，寄生电容的存在使得钙钛矿LED器件的发光过程无法跟上泵浦源的快速变化，限制了最小脉宽，无法保证热量的高效耗散" }, { "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": "。针对这一问题，需要降低器件的寄生电容以提升其响应速度。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "利用高导电的传输层与散热强的电极修饰材料有利于提升器件的散热。2020年，Zhao等" }, { "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": "在MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": " LED器件中同时采用了这两类手段，获得了优良的热管理效果。其器件结构如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（a）所示。通过对载流子传输层进行掺杂，有效地提升了器件的电导率。不过，以玻璃为基底的情况下器件在1 kA·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "的电流注入下升温达到473 K，如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（b）所示。通过在Ag电极顶部粘合高热导率的石墨膜，可以提升器件的散热效率。他们对比了不同尺寸以及结合石墨膜散热的器件的升温，如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（c）所示，结合石墨膜散热的小尺寸器件升温控制效果更明显。上述热管理措施综合改善了器件的EL特性，在脉宽为800 ns的脉冲电泵浦源激励下，MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": " LED器件的EL几乎无衰减。在此基础上，他们进一步使用载流子迁移率更高的传输层材料，同时添加了碘化钾以钝化碘离子缺陷，最终器件的EQE提升了近2倍" }, { "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": "。并且在脉宽短至30 ns的电脉冲泵浦激励下，器件的EL无衰减。同时还使用了一种能够降低串联电阻的阳极设计方案（如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（d）），使器件响应速度达到1.2 ns，这样有利于采用更短的脉宽，使器件有足够的间隔时间将热量弛豫掉。该器件在引入选模光栅后获得了窄化的EL线宽，如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（e）所示。EQE-" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "曲线（" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（f））表明，他们的器件获得了最高10 kA·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "的注入电流密度与对应1%的EQE，相应的" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "×" }, { "name": "italic", "data": [ { "name": "text", "data": "η" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "EQE" } ] }, { "name": "text", "data": "值达100 A·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "，远高于Kim等所报道的器件" }, { "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": "。经估算，此时的电泵浦载流子浓度为7.5×10" }, { "name": "sup", "data": [ { "name": "text", "data": "17" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "，已经十分接近光泵浦激光阈值载流子浓度（7.97× 10" }, { "name": "sup", "data": [ { "name": "text", "data": "17" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "）。" } ] }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "（a）采用热管理策略的钙钛矿LED示意图" }, { "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": "；（b）在脉冲模式下工作的钙钛矿LED从高能电致发光尾部提取的载流子温度" }, { "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": "；（c）具有不同几何形状和散热的钙钛矿型LED中，载流子温度作为恒电流密度的函数" }, { "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": "；（d）集成二阶DFB光栅的PeLED示意图" }, { "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": "；（e）脉冲电流密度为10 kA·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "时，有或无DFB光栅的PeLEDs的EL光谱" }, { "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": "；（f）脉冲模式下驱动的PeLEDs的EQE-" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "曲线" }, { "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": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.3" } ], "title": [ { "name": "text", "data": "（a）Schematic diagram of a perovskite LED（PeLEDs） employing thermal management strategies" }, { "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": ". （b）Carrier temperature extracted from the high-energy electroluminescence tail for perovskite LEDs operated in the pulsed mode" }, { "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": ". （c）Carrier temperature for perovskite LEDs with various geometry and heat spreaders as a function of constant current density" }, { "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": ". （d）Schematic diagram of the PeLED with the integration of a second-order DFB grating" }, { "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": ". （e）EL spectra of PeLEDs driven at pulsed current density of 10 kA·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "， with or without a DFB grating" }, { "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": ". （f）EQE-" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": " curves of PeLEDs driven in pulsed mode" }, { "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": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471961&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471968&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471965&type=", "width": "158.21197510", "height": "82.08557129", "fontsize": "" } ] } } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4　通向钙钛矿电泵浦激光的补充措施" } ], "level": "1", "id": "s4" } }, { "name": "p", "data": [ { "name": "text", "data": "除了前一节描述的两种核心制约因素外，钙钛矿电注入型发光器件中还面临电荷注入不平衡、光学损耗高、增益能力不足等问题。例如，现有的电注入结构设计与制备方案，包括钙钛矿有源区的设计与制备、载流子传输层的设计与制备等尚未优化到最佳状态，器件中伴随有电荷注入不平衡等问题，降低了载流子的注入效率，增加了电泵浦激光实现的难度。此外，实现激光的最低要求是增益大于损耗，即净增益大于零。而现有电注入结构中光学散射、电极寄生吸收等会引起高光学损耗，不利于高性能激光的实现" }, { "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": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "64", "type": "bibr", "rid": "R64", "data": [ { "name": "text", "data": "64" } ] } } ], "rid": [ "R63", "R64" ], "text": "63-64", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。不仅如此，钙钛矿的设计与制备直接影响了其光学增益能力。促进粒子数反转是弥补低增益的有效手段，两种泵浦源皆通过注入能量以产生超过阈值的载流子密度形成粒子数反转。但是，由于电泵浦激光器中载流子注入效率低，依据光泵浦激光阈值载流子密度仅仅能估算电泵浦激光阈值下限。因此，需要有效地利用注入至钙钛矿层内的载流子促成粒子数反转。针对这些方面，研究人员提出了平衡电荷注入、降低光学损耗、促进粒子数反转等策略，有助于钙钛矿电泵浦激光器件性能的提升。" } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4.1　电荷平衡注入" } ], "level": "2", "id": "s4a" } }, { "name": "p", "data": [ { "name": "text", "data": "典型的电注入结构是由阳极、空穴传输层（HTL）、钙钛矿层、电子传输层（ETL） 和阴极堆叠构成。理想的电注入效果是使载流子平衡、高效地注入至钙钛矿层中发生复合，当电子与空穴的注入不平衡时，具有低注入效率的那类载流子会在靠近钙钛矿与其传输层的界面处发生积聚，加剧非辐射复合损耗与器件升温。电注入器件中的空穴传输层在传输空穴的同时，也具有阻挡电子进入的功能，双重功能可通过多层材料的组合来实现。类似地，电子传输层传输电子的同时，也具有阻挡空穴的功能。为了提高发光效率，载流子从发光层到向电极运动的通道应当完全被阻断，当HTL阻挡载流子的势垒过低时，会引发载流子泄露，泄露的载流子降低了电注入器件的发光效率。此外，钙钛矿材料中的针孔及粗糙的表面也会导致载流子分流，还会导致光学损耗，需要对钙钛矿表面加以修饰，见4.2节的讨论。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "由于钙钛矿材料的价带较深，研究人员需要设计具有宽带隙HTL的钙钛矿电注入器件以提升其空穴注入效率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "65", "type": "bibr", "rid": "R65", "data": [ { "name": "text", "data": "65" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。2020年，Zou等" }, { "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": "对比了不同HTL构成的CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿电注入型发光器件的空穴注入性能。器件结构如" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "（a），他们选取了三种电子阻挡势垒高度接近的HTL设计，即PEDOT∶PSS（A）、PEDOT∶PSS/TFB/PVK（B）、poly-TPD/PVK（C）。由于poly-TPD的注入势垒低于PEDOT∶PSS，因而C器件具有更高的空穴注入效率。" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "（b）、（c）显示C器件的导电效果更好、EQE最高。Yin等" }, { "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": "发现K" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "掺杂的HTL可以提高电导率。2021年，Shen等" }, { "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": "在K" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "改性的HTL上也制备了钙钛矿薄膜。如" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "（d），由于 K" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "与钙钛矿中卤离子之间存在强偶极相互作用，因此所制得的钙钛矿薄膜具备更高表面覆盖率与更一致的晶粒取向，从而大幅降低了界面电荷陷阱。并且器件的阻抗谱（" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "（e））显示，电荷转移电阻显著降低；结合" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "（f），K" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "改性HTL器件的响应速度更快，表明实现了更平衡的电荷注入效果。对钙钛矿层进行K" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "修饰，也可以得到类似的效果。2020年，Yang等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "68", "type": "bibr", "rid": "R68", "data": [ { "name": "text", "data": "68" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "用K" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "替代钙钛矿纳米晶中的有机长链配体，使得K" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "与纳米晶表面的卤离子相结合，形成了锚定在钙钛矿纳米晶表面的金属配体，从而提升了电荷从HTL层注入至钙钛矿中的效率。并且，由于K" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "替代了有机配体，所以钙钛矿纳米晶的表面粗糙度也得到改善，明显降低了器件的漏电流，最终带来器件发光性能的显著改善。" } ] }, { "name": "fig", "data": { "id": "F4", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图4" } ], "title": [ { "name": "text", "data": "（a）钙钛矿LED器件结构示意图" }, { "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": "；（b）～（c）A、B、C结构的" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "、EQE-" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "图" }, { "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": "；（d）K" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "改性的PEDOT∶PSS基底上钙钛矿结构和晶体生长示意图" }, { "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": "；（e）偏置电压为4.5 V器件的阻抗谱" }, { "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": "；（f）占空比为20%的瞬态EL衰减曲线" }, { "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": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.4" } ], "title": [ { "name": "text", "data": "（a）Schematic device architecture of PeLEDs" }, { "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": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "V" } ] }, { "name": "text", "data": "（b）， and EQE-" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "（c） data of structures A， B and C" }, { "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": ". （d）Schematic device architecture， and crystal growth of perovskite grains on K" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "-modified PEDOT∶PSS substrate" }, { "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": ". （e）Impedance spectra of the devices biased at 4.5 V" }, { "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": ". （f）Transient EL decay curves with 20% duty cycle" }, { "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": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471972&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471981&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471977&type=", "width": "156.74475098", "height": "73.90795898", "fontsize": "" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4.2　降低光学损耗" } ], "level": "2", "id": "s4b" } }, { "name": "p", "data": [ { "name": "text", "data": "在钙钛矿激光器件中，具有光滑表面的钙钛矿样品可以有效抑制光散射（" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "（a）），提高器件的净增益。广泛使用的溶液旋涂法制备出的钙钛矿薄膜粗糙度比较高，且不可避免地出现针孔（" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（b）），引发相对严重的光散射损耗，不利于激光的实现。2020年，Cho等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "采用真空沉积法和溶液旋涂法分别制备了CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "薄膜，所制得的样品的表面粗糙度分别为2 nm与20 nm，测试表明只有前者才能激发ASE。优化制备工艺可进一步降低钙钛矿薄膜的光散射损耗。2019年，Li等" }, { "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": "利用两步气相沉积法工艺，制备了粗糙度约1 nm的单晶MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿纳米片，腔品质因子为 2 600。最近，Li等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "61", "type": "bibr", "rid": "R61", "data": [ { "name": "text", "data": "61" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "在PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "纳米片向MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "纳米片的气相转化过程中，利用残留的PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "对钙钛矿表面进行修饰。与完全转化样品相比，修饰后的样品具有更低的表面粗糙度（低至0.7 nm）。基于此，PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "残留样品进一步抑制了散射损耗，表现出极高的腔品质因子（7 810）。" } ] }, { "name": "fig", "data": { "id": "F5", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图5" } ], "title": [ { "name": "text", "data": "（a）钙钛矿中放大自发辐射（ASE）过程中两种主要的光学损耗机制示意图：光学散射和电极寄生吸收" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "；（b）钙钛矿薄膜表面存在大量针孔，导致强烈的光学散射损耗" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "71", "type": "bibr", "rid": "R71", "data": [ { "name": "text", "data": "71" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "；（c）引入重结晶过程前后，钙钛矿薄膜PL强度随传播距离的变化关系" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "70", "type": "bibr", "rid": "R70", "data": [ { "name": "text", "data": "70" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "；（d）具有不同光学增益的钙钛矿波导模式对应的PL强度与距离的乘积随传输距离的变化关系" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.5" } ], "title": [ { "name": "text", "data": "（a）Schematic diagram of two main optical loss mechanisms， " }, { "name": "italic", "data": [ { "name": "text", "data": "i" } ] }, { "name": "text", "data": ". " }, { "name": "italic", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": ".， optical scattering and electrode parasitic absorption， in the process of amplified spontaneous emission（ASE） in perovskites" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": ". （b）A large number of pinholes exist on the surface of perovskite films， resulting in strong optical scattering loss" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "71", "type": "bibr", "rid": "R71", "data": [ { "name": "text", "data": "71" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": ". （c）Variation of PL intensity of perovskite films with the propagating length before and after introducing the recrystallization process" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "70", "type": "bibr", "rid": "R70", "data": [ { "name": "text", "data": "70" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": ". （d）The product of PL intensity and propagating distance of perovskite waveguide modes with different optical gains varies with the propagating distance" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471984&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471989&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471987&type=", "width": "130.45581055", "height": "82.78271484", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "在溶液法制备钙钛矿薄膜的过程中添加钝化剂可有效降低样品的表面粗糙度。Liang等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "69", "type": "bibr", "rid": "R69", "data": [ { "name": "text", "data": "69" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "在MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿溶液法成膜过程中添加了具有小体积有机阳离子基团的钝化剂，促使其薄膜粗糙度从3.06 nm降低至1.14 nm。最近，Liang等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "70", "type": "bibr", "rid": "R70", "data": [ { "name": "text", "data": "70" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "提出了一种溶剂辅助重结晶制备钙钛矿薄膜的方法以降低表面针孔，将薄膜粗糙度从2.17 nm降低至0.46 nm。进一步测试表明，引入重结晶过程的钙钛矿薄膜的散射损耗是参比器件的1/3（如" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "（c）所示），这使得光泵浦下激光器的ASE阈值降低为参比器件的一半，低至1.44 μJ·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "电注入器件中，电极寄生吸收会削弱材料光增益能力。Cho等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "在低粗糙度CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿薄膜与 TPBi电子传输层、银电极制成的三层结构中，观测了光泵浦下不同波导模式的PL强度随传输距离变化的关系曲线，结果如" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "（d）所示。具有更高增益的PL" }, { "name": "sub", "data": [ { "name": "text", "data": "550-570" } ] }, { "name": "text", "data": "在波导模式传播过程中，弥补了一定的寄生吸收损耗后仍然具有较高的净增益，传播距离更远。他们还发现，随着TPBi层的厚度降低，电极寄生吸收损耗逐渐加剧，PL" }, { "name": "sub", "data": [ { "name": "text", "data": "550-570" } ] }, { "name": "text", "data": "的传输距离也随之逐渐缩短。次年，Cho等" }, { "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": "对比了有/无电极的两种器件的光泵浦ASE阈值，含电极器件的阈值为180 μJ·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "，高于无电极的情况（140 μJ·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "）。根据计算，该器件最大注入电流条件下（" }, { "name": "italic", "data": [ { "name": "text", "data": "J" } ] }, { "name": "text", "data": "=840 A·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "），注入的载流子浓度（6.4 × 10" }, { "name": "sup", "data": [ { "name": "text", "data": "17" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "）仅达到了光泵浦阈值180 μJ·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "对应的载流子浓度（2.0 × 10" }, { "name": "sup", "data": [ { "name": "text", "data": "19" } ] }, { "name": "text", "data": " cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "）的3%，不足以实现粒子数反转。他们指出，适当增加波导光限制能力或者利用小接触面积的纳米结构电极，可以降低电极寄生吸收损耗" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "17", "type": "bibr", "rid": "R17", "data": [ { "name": "text", "data": "17" } ] } }, { "name": "text", "data": ", " }, { "name": "xref", "data": { "text": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4.3　促进粒子数反转" } ], "level": "2", "id": "s4c" } }, { "name": "p", "data": [ { "name": "text", "data": "钙钛矿材料中存在一些新奇的载流子转移机制，对其加以利用，可提升局部激发态密度，促进粒子数反转" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "72", "type": "bibr", "rid": "R72", "data": [ { "name": "text", "data": "72" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "73", "type": "bibr", "rid": "R73", "data": [ { "name": "text", "data": "73" } ] } } ], "rid": [ "R72", "R73" ], "text": "72-73", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。2015年，Neutzner等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "72", "type": "bibr", "rid": "R72", "data": [ { "name": "text", "data": "72" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "发现载流子转移伴随材料相变产生。具体地，当MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "随着环境温度从100 K上升至160 K，材料会从原来的正交相转变为正交相与四方相共存的混合相。由于四方相MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿的带隙（~1.43 eV）小于正交相的带隙（~1.6 eV）" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "74", "type": "bibr", "rid": "R74", "data": [ { "name": "text", "data": "74" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，两个相的界面可以发生载流子转移，其转移效率在~150 K的温度时达到最高。" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "（a）给出了该混合相MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿在150 K下光生载流子填充状态随时间演化的光漂白特征，显示此时正交相（瞬态吸收峰730 nm）到四方相（对应760 nm）的载流子转移在13 ps内基本完成，比俄歇复合寿命还要短，有利于对光生载流子的充分利用。此外，粒径更小的正交相MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "晶粒中的载流子扩散到四方相晶粒所需的时间更短，利用这一特性还可进一步提升载流子转移效率。2017年，Jia等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "75", "type": "bibr", "rid": "R75", "data": [ { "name": "text", "data": "75" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "利用这一载流子转移机制，实现了低温下的MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿CW光泵浦激光。" } ] }, { "name": "fig", "data": { "id": "F6", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图6" } ], "title": [ { "name": "text", "data": "（a）混合相MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "（正交相与四方相共存）的瞬态吸收谱" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "72", "type": "bibr", "rid": "R72", "data": [ { "name": "text", "data": "72" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "；（b）不同钙钛矿薄膜在不同延迟时间下的去卷积瞬态吸收光漂白特征，其中钙钛矿薄膜包含域排列高度有序的两种准二维钙钛矿（ " }, { "name": "italic", "data": [ { "name": "text", "data": "n " } ] }, { "name": "text", "data": "= 2 或 " }, { "name": "italic", "data": [ { "name": "text", "data": "n " } ] }, { "name": "text", "data": "= 3）以及三维钙钛矿" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "77", "type": "bibr", "rid": "R77", "data": [ { "name": "text", "data": "77" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "；（c）准二维钙钛矿中载流子从小" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "值域向大" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "值域发生逐级转移过程示意图" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "73", "type": "bibr", "rid": "R73", "data": [ { "name": "text", "data": "73" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.6" } ], "title": [ { "name": "text", "data": "（a）Transient absorption spectra of mixed phase MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "72", "type": "bibr", "rid": "R72", "data": [ { "name": "text", "data": "72" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": " at different delay time. （b）The de-convolved transient absorption photobleaching features in different perovskites， including highly-ordered-domain-arranged quasi-2D perovskites with " }, { "name": "italic", "data": [ { "name": "text", "data": "n " } ] }, { "name": "text", "data": "= 2 and " }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": " = 3 as well as the 3D phases perovskite" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "77", "type": "bibr", "rid": "R77", "data": [ { "name": "text", "data": "77" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": ". （c）Schematic diagram of carrier transfer from small " }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "-value domain to large " }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "-value domain in quasi-2D perovskites" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "73", "type": "bibr", "rid": "R73", "data": [ { "name": "text", "data": "73" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471992&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471996&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471993&type=", "width": "142.43565369", "height": "107.43508911", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "在准二维钙钛矿中，也发现了一种特殊的载流子转移现象。在这类材料中，存在不同" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "值的量子阱，即不同" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "值的域。其中" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "为某量子阱中两个有机层之间[" }, { "name": "italic", "data": [ { "name": "text", "data": "BX" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "6" } ] }, { "name": "text", "data": "]" }, { "name": "sup", "data": [ { "name": "text", "data": "4-" } ] }, { "name": "text", "data": "的层数。如" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "（c）所示，不同" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "值域的带隙随" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "的增大而减小" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "73", "type": "bibr", "rid": "R73", "data": [ { "name": "text", "data": "73" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。正因为如此，载流子可以从小" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "值域到大" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "值域之间逐级转移" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "76", "type": "bibr", "rid": "R76", "data": [ { "name": "text", "data": "76" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，这种像漏斗一样载流子逐级转移的时间跨度大约在100 ps以内" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "73", "type": "bibr", "rid": "R73", "data": [ { "name": "text", "data": "73" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。2020年，Lei等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "77", "type": "bibr", "rid": "R77", "data": [ { "name": "text", "data": "77" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "利用溶剂工程分别制备了呈现有序域分布与无序域分布的准二维钙钛矿薄膜，前者激光阈值比后者降低了1个数量级。这是因为，域分布无序使得载流子俘获位置分布无序，导致局域载流子浓度降低；其次，在域分布无序薄膜中，不同" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "值域之间存在结晶行为差异，容易在晶界及边缘处引入缺陷致使表面粗糙程度升高，带来相对严重的光学/电学损耗" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "78", "type": "bibr", "rid": "R78", "data": [ { "name": "text", "data": "78" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。反之，高度有序的域排列使这种逐级载流子传递时间降低至亚皮秒尺度（" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "（b））。超快的逐级载流子转移弱化了缺陷对载流子的俘获效果，带来了器件净增益的提高，最终降低了激光阈值" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "77", "type": "bibr", "rid": "R77", "data": [ { "name": "text", "data": "77" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。需要指出的是，这种载流子逐级转移机制能否兼顾电驱动下的电荷注入平衡，值得进行深入探究" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "5　钙钛矿激光新机制" } ], "level": "1", "id": "s5" } }, { "name": "p", "data": [ { "name": "text", "data": "基于经典的激光工作原理制成的钙钛矿激光器往往具有较高的阈值，一定程度上限制了钙钛矿电泵浦激光。为了突破这一限制，一些基于新物理机制的钙钛矿激光被陆续报道，包括表面等离激元（SPP）" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "79", "type": "bibr", "rid": "R79", "data": [ { "name": "text", "data": "79" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、 Mie共振" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "80", "type": "bibr", "rid": "R80", "data": [ { "name": "text", "data": "80" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、激子极化激元" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "81", "type": "bibr", "rid": "R81", "data": [ { "name": "text", "data": "81" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "82", "type": "bibr", "rid": "R82", "data": [ { "name": "text", "data": "82" } ] } } ], "rid": [ "R81", "R82" ], "text": "81-82", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、连续域束缚态（BIC）" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "83", "type": "bibr", "rid": "R83", "data": [ { "name": "text", "data": "83" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": " 等。其中，基于激子极化激元" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "81", "type": "bibr", "rid": "R81", "data": [ { "name": "text", "data": "81" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "82", "type": "bibr", "rid": "R82", "data": [ { "name": "text", "data": "82" } ] } } ], "rid": [ "R81", "R82" ], "text": "81-82", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "的钙钛矿室温CW激光已经实现，为通向电泵浦激光研究提供了一些颇为有效的备选方案。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "SPP模式是金属表面自由电子发生集体振荡的一类光学模式，该模式在金属/介质界面处场强最高" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "84", "type": "bibr", "rid": "R84", "data": [ { "name": "text", "data": "84" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "85", "type": "bibr", "rid": "R85", "data": [ { "name": "text", "data": "85" } ] } } ], "rid": [ "R84", "R85" ], "text": "84-85", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。区别于介质波导中激发的腔共振型光子模式或光子晶体引发的布洛赫光子模式，SPP模式的优势是利用光与物质的强相互作用获得低激光阈值" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "85", "type": "bibr", "rid": "R85", "data": [ { "name": "text", "data": "85" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。2018年，Wu等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "86", "type": "bibr", "rid": "R86", "data": [ { "name": "text", "data": "86" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "构建了CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "纳米线-Ag膜-SiO" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "三层结构的激光器。发现同一尺寸器件中，SPP模式激光阈值均低于光子模式激光。研究还表明，优化金属层与钙钛矿层之间的间隙，还可以进一步降低阈值。2019年，Wu等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "87", "type": "bibr", "rid": "R87", "data": [ { "name": "text", "data": "87" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "在MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "薄膜上依次制备了PMMA间隔层与金纳米棒，当间隔层厚度小于8 nm时，非辐射复合能量转移引起的猝灭逐渐占据主导，导致ASE阈值升高；反之，激子与等离子体之间的耦合强度降低，阈值升高。在钙钛矿SPP激光器中，介质间隔层的厚度在5~20 nm 范围内才能达成最佳表面等离激元增强效果" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "88", "type": "bibr", "rid": "R88", "data": [ { "name": "text", "data": "88" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "SPP激光机制有助于激光器件的小型化。为了降低功耗、实现高密度集成，器件的小型化是必要的。然而，小型激光器需要更高的光学增益来克服腔损耗。目前，SPP激光机制可以实现更紧凑、光限制更强的激光器。事实上，大的光限制因子对应大的净模式增益。最近，Cho等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "89", "type": "bibr", "rid": "R89", "data": [ { "name": "text", "data": "89" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "基于亚微米尺度的三维钙钛矿微结构，实现了三个维度光限制的SPP激光器，如" }, { "name": "xref", "data": { "text": "图 7", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图 7" } ] } }, { "name": "text", "data": "（a）所示，电场在间隔层中最强。他们还发现可通过SPP模式在微腔中的强边界反射补偿掉金属吸收损耗，进一步提升净增益。另外，钙钛矿光子模式激光寿命在30 ps以内" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "90", "type": "bibr", "rid": "R90", "data": [ { "name": "text", "data": "90" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，而等离子体受激发射寿命为1.6 ps" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "91", "type": "bibr", "rid": "R91", "data": [ { "name": "text", "data": "91" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，比光子模式快了一个数量级。超快的受激辐射过程有效避免了与俄歇复合过程的竞争，提高了净增益。" } ] }, { "name": "fig", "data": { "id": "F7", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图7" } ], "title": [ { "name": "text", "data": "（a）上图为基于CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "-pNE-Au的表面等离激元激光器结构，下图为激光器结构中的光场分布" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "89", "type": "bibr", "rid": "R89", "data": [ { "name": "text", "data": "89" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "；（b）上图为CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "纳米立方的Mie共振激光器结构，下图为Mie共振模式分布" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "80", "type": "bibr", "rid": "R80", "data": [ { "name": "text", "data": "80" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "； （c）极化激元激光不同温度下的群速度-光子能量曲线，插图为SEM下纳米线形貌" }, { "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": "；（d）准BIC激光理论" }, { "name": "italic", "data": [ { "name": "text", "data": "Q" } ] }, { "name": "text", "data": "值，插图为BIC激光器结构示意图" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "83", "type": "bibr", "rid": "R83", "data": [ { "name": "text", "data": "83" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.7" } ], "title": [ { "name": "text", "data": "（a）Top： surface plasmonic laser structure based on CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "-pNE-Au. Bottom： the light field distribution in this laser structure" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "89", "type": "bibr", "rid": "R89", "data": [ { "name": "text", "data": "89" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": ". （b）Top： the structure of CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": " Mie resonance laser. Bottom： the Mie resonance mode distribution" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "80", "type": "bibr", "rid": "R80", "data": [ { "name": "text", "data": "80" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": ". （c）The group velocity photon energy curve of polariton laser at different temperatures. The inset shows the morphology of nanowires under SEM" }, { "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": ". （d）The theoretical " }, { "name": "italic", "data": [ { "name": "text", "data": "Q" } ] }, { "name": "text", "data": " value of quasi-BIC laser. The inset is the structural diagram of BIC laser" }, { "name": "sup", "data": [ { "name": "text", "data": "［" }, { "name": "xref", "data": { "text": "83", "type": "bibr", "rid": "R83", "data": [ { "name": "text", "data": "83" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36471999&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36472003&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=36472001&type=", "width": "135.72767639", "height": "131.06272888", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "由于SPP激光器中的金属欧姆损耗较高，限制了其激光性能的提高。与金属纳米结构相比，由高折射率介质构成的纳米结构激发的Mie共振可避免这一点，在激光应用方面具有很大的吸引力。类似于SPP共振，基于Mie共振也可实现纳米尺度的光场局域，也能增强光与物质相互作用，实现突破衍射极限的相干辐射源" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "92", "type": "bibr", "rid": "R92", "data": [ { "name": "text", "data": "92" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。钙钛矿材料具有足够高的折射率，并且它们的微结构形式多样，因此基于钙钛矿材料的Mie共振激光引起了研究人员的关注。最近，Tiguntseva等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "80", "type": "bibr", "rid": "R80", "data": [ { "name": "text", "data": "80" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "制备出了尺寸~310 nm的亚波长尺度CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿立方颗粒，如" }, { "name": "xref", "data": { "text": "图7", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7" } ] } }, { "name": "text", "data": "（b）所示，进一步基于单个CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "立方颗粒实现了基于Mie共振的室温脉冲光泵浦激光，但其" }, { "name": "italic", "data": [ { "name": "text", "data": "Q" } ] }, { "name": "text", "data": "值较低，处于500~1 600。截至目前，钙钛矿Mie共振激光的报道还相对较少，它们的潜力尚需挖掘。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "当分子中的激子与光子能量的波函数相互作用程度足够强、使得耦合强度超过衰减速率时，该相互作用将进入强耦合状态，形成一种新的混合态，称之为激子极化激元。激子极化激元具有非常强的非线性特性，促成了激子极化激元凝聚的发生，基于这种凝聚态产生的稳态相干光为激子极化激元激光。2018年，Evans等在CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "纳米线中观察到CW光激发下的激子极化激元激光" }, { "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": "。2020年，Shang等" }, { "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": "揭示了基于CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "纳米线的激子极化激元激光具有低阈值的机理。他们发现，在降温过程中，激子极化激元激光谱移向激子振荡能，模式光的群折射率逐渐上升，出现了慢光效应（如" }, { "name": "xref", "data": { "text": "图 7", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图 7" } ] } }, { "name": "text", "data": "（c）所示），进而带来更好的光限制作用，促使激子极化激元态的激子特性逐渐增强，最终获得低温CW激光。需要指出的是，当运转温度上升或注入载流子浓度高于该材料的激子离解阈值（Mott浓度）时，激子极化激元激光会过渡至光子激光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "14", "type": "bibr", "rid": "R14", "data": [ { "name": "text", "data": "14" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "93", "type": "bibr", "rid": "R93", "data": [ { "name": "text", "data": "93" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，采用具有更大激子结合能的钙钛矿材料有助于将这种激光机制应用于室温条件下。较之CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "，MAPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "单晶的激子结合能更高。2019年，Tian等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "94", "type": "bibr", "rid": "R94", "data": [ { "name": "text", "data": "94" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "利用空间限制法直接在一对DBR反射镜之间生长出高质量单晶MAPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "薄膜，该薄膜的激子寿命长达426 ns。他们利用VCSEL光腔进一步增强了光与物质相互作用，并获得了室温CW光泵浦激光，其阈值为34 mW·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "，是目前阈值最低的室温钙钛矿CW激光。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "BIC是连续域中保持局域化的谐振模式。当系统表现出反射或旋转对称性时，不同对称态的模式会完全解耦，因此BIC波函数不会与连续域的辐射波耦合，而被有效地“保护”起来。所以BIC具有零泄露特征，从而具有无限大的" }, { "name": "italic", "data": [ { "name": "text", "data": "Q" } ] }, { "name": "text", "data": "品质因子。不过，这也意味着BIC是具有无限辐射寿命的“暗态”。然而，实际应用中，结构设计、材料制备中往往会引入打破对称性的扰动因素，如材料折射率的变化，从而使BIC与连续域耦合，并坍缩为具有光发射特性的高" }, { "name": "italic", "data": [ { "name": "text", "data": "Q" } ] }, { "name": "text", "data": "值准BIC（Quasi-BIC），理论上该" }, { "name": "italic", "data": [ { "name": "text", "data": "Q" } ] }, { "name": "text", "data": "值可以达到10" }, { "name": "sup", "data": [ { "name": "text", "data": "10" } ] }, { "name": "text", "data": "以上" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "83", "type": "bibr", "rid": "R83", "data": [ { "name": "text", "data": "83" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。这一点在激光领域上具有重要的应用价值。最近，BIC工作机制也被引入到钙钛矿激光器中。2020年，Huang等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "83", "type": "bibr", "rid": "R83", "data": [ { "name": "text", "data": "83" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "利用MAPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "薄膜构造出超表面（如" }, { "name": "xref", "data": { "text": "图7", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7" } ] } }, { "name": "text", "data": "（d）所示），在脉冲光泵浦下调控不同区域的钙钛矿增益能力产生差别，从而打破其中的BIC对称保护，实现了基于准BIC的超低阈值激光，阈值为4.2 μJ·cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": "，" }, { "name": "italic", "data": [ { "name": "text", "data": "Q" } ] }, { "name": "text", "data": "值为5 560。此外，Tiguntseva等提出借助BIC能够改善钙钛矿Mie共振激光的" }, { "name": "italic", "data": [ { "name": "text", "data": "Q" } ] }, { "name": "text", "data": "值，进一步实现CW激光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "80", "type": "bibr", "rid": "R80", "data": [ { "name": "text", "data": "80" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "6　总结与展望" } ], "level": "1", "id": "s6" } }, { "name": "p", "data": [ { "name": "text", "data": "总之，通向钙钛矿电泵浦激光研究已经取得了一系列可喜的进展。过去的几年中，研究人员们针对阻碍钙钛矿电泵浦激光实现的一系列问题，提出了解决方案，助力通向钙钛矿电泵浦激光的发展。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "钙钛矿表面存在大量的缺陷，通过引入合适的钝化剂可有效削弱缺陷辅助的单分子复合。为了抑制钙钛矿中的俄歇复合损耗，可以通过掺杂重金属元素提升自旋-轨道耦合导致的分裂能，以降低由自旋-轨道耦合分裂诱发的俄歇复合，亦可利用组分工程获得更紧密的钙钛矿晶格结构，以弱化Rashba能带分裂，从而降低由此引发的俄歇复合。二维钙钛矿中的三重态激子复合损耗十分严重，利用不同载流子转移机制实现单重态激子与三重态激子在空间上的分离，是一种降低三重态激子复合损耗十分有效的措施。钙钛矿激光器中的热效应严重，可通过缩小器件面积、用短脉冲源激励、提高器件各功能层导电性、引入高散热电极等方法，缓解其中的热效应问题。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "此外，在电注入器件的结构设计方面，可借鉴的优化策略包括：选用与钙钛矿能级更为匹配的载流子传输材料，提升各功能层的电荷传输能力，优化功能薄膜的质量与界面质量等。在光学结构设计方面，首先是降低散射损耗，在制备表面粗糙度低的薄膜的前提下，引入重结晶策略可有效降低表面粗糙度并减少针孔。其次是降低金属电极的寄生吸收，可通过增强载流子传输层的光限制能力或者纳米结构电极来达到该目的。促进粒子数反转是实现电泵浦激光的一个有益补充，可采取的措施包括：在三维钙钛矿中利用材料的相变，构建载流子俘获点以获得局部高载流子浓度；制备有序域分布的准二维钙钛矿，保证载流子从不同域间的有效传输与聚集。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "目前，3D和准二维钙钛矿均实现了室温CW激光与大电流LED。对于准二维钙钛矿，材料不利于跨有机层的电荷传输；相对3D钙钛矿，准二维钙钛矿的俄歇阈值更低。不过，这类材料具有比3D钙钛矿材料更高的稳定性、更高效的激子复合。因此，两类材料都具有通向电泵浦激光的独特优势与前景。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "未来的研究中新机制激光器也十分值得关注，为钙钛矿电泵浦激光的实现提供了崭新的平台。基于钙钛矿的激子极化激元激光器已经实现了CW光泵浦激光，SPP激光器也得到了广泛研究。但是与光子激光不同的是，SPP激光器中额外存在金属固有损耗，需要进一步解决。SPP激光器的性能依然有较大的提升空间。激子极化激元机制的优势是可以实现比光子模式激光更低的阈值，基于该机制已经实现目前室温钙钛矿连续激光的最低阈值。不过，钙钛矿微腔的质量限制了激子极化激元激光的性能。并且，将这种微腔引入电泵浦激光中时需要用到干法转移，因此还需进一步优化转移工艺，尽可能降低对微腔的损伤。目前，基于Mie共振、BIC的钙钛矿激光器研究才刚刚兴起。这些新工作机制具有输出低阈值、高" }, { "name": "italic", "data": [ { "name": "text", "data": "Q" } ] }, { "name": "text", "data": "值激光的潜力，因而需要加大对这些新机制激光器的研究。未来，它们将在通向钙钛矿电泵浦激光研究中占据十分重要的位置。" } ] }, { "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": 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