Temperature-dependent luminescence spectra of Ruddlesden-Popper quasi-2D perovskites Enhanced Publication

{ "defaultlang": "zh", "titlegroup": { "articletitle": [ { "lang": "zh", "data": [ { "name": "text", "data": "Ruddlesden-Popper型准二维钙钛矿温度依赖发光光谱研究" } ] }, { "lang": "en", "data": [ { "name": "text", "data": "Temperature-dependent luminescence spectra of Ruddlesden-Popper quasi-2D perovskites" } ] } ] }, "contribgroup": { "author": [ { "name": [ { "lang": "zh", "surname": "杜", "givenname": "子孝", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "DU", "givenname": "Zi-xiao", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" }, { "rid": "aff2", "text": "2" }, { "rid": "aff4", "text": "4" } ], "role": [ "first-author" ], "bio": [ { "lang": "zh", "text": [ "杜子孝（1998-），男，湖南张家界人，硕士研究生，学生，2020年于华中科技大学获得学士学位，主要从事钙钛矿发光机理方向的研究。E-mail： duzixiao@siom.ac.cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481344&type=", "small": 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[], "aff": [ { "rid": "aff1", "text": "1" }, { "rid": "aff2", "text": "2" } ], "role": [], "deceased": false }, { "name": [ { "lang": "zh", "surname": "刘", "givenname": "征征", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "LIU", "givenname": "Zheng-zheng", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [ "corresp" ], "corresp": [ { "rid": "cor1", "lang": "en", "text": "E-mail： liuzhengzheng@siom.ac.cn", "data": [ { "name": "text", "data": "E-mail： liuzhengzheng@siom.ac.cn" } ] } ], "bio": [ { "lang": "zh", "text": [ "刘征征（1991-），男，山东临沂人，博士，副研究员，2019年于中国科学院上海光学精密机械研究所获得博士学位，主要从事新型光电器件及发光物理机制研究。E-mail： liuzhengzheng@siom.ac.cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481350&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481352&type=", "big": 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"杜鹃（1980-），女，山东潍坊人，博士，研究员，博士生导师，2007年于中国科学院上海光学精密机械研究所获得博士学位，主要从事超短脉冲激光与功能材料相互作用（具体包括钙钛矿等纳米发光材料制备及器件）的研究。E-mail：dujuan@mail.siom.ac.cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481353&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481355&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481354&type=", "width": "23.04434204", "height": "23.04415894", "fontsize": "" } ], "data": [ [ { "name": "text", "data": "杜鹃" }, { "name": "text", "data": "（1980-），女，山东潍坊人，博士，研究员，博士生导师，2007年于中国科学院上海光学精密机械研究所获得博士学位，主要从事超短脉冲激光与功能材料相互作用（具体包括钙钛矿等纳米发光材料制备及器件）的研究。E-mail：" }, { "name": "text", "data": "dujuan@mail.siom.ac.cn" } ] ] } ], "email": "dujuan@mail.siom.ac.cn", "deceased": false }, { "name": [ { "lang": "zh", "surname": "冷", "givenname": "雨欣", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "LENG", "givenname": "Yu-xin", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" }, { "rid": "aff2", "text": "2" } ], "role": [ "corresp" ], "corresp": [ { "rid": "cor3", "lang": "en", "text": "lengyuxin@siom.ac.cn", "data": [ { "name": "text", "data": "lengyuxin@siom.ac.cn" } ] } ], "bio": [ { "lang": "zh", "text": [ "冷雨欣（1975-），男，上海人，博士，研究员，博士生导师，2002 年于中国科学院上海光学精密机械研究所获得博士学位，主要从事超强超短激光技术发展及其前沿重要应用等方面的研究。E-mail：lengyuxin@mail.siom.ac.cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481356&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481358&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481357&type=", "width": "23.37403870", "height": "23.37397766", "fontsize": "" } ], "data": [ [ { "name": "text", "data": "冷雨欣" }, { "name": "text", "data": "（1975-），男，上海人，博士，研究员，博士生导师，2002 年于中国科学院上海光学精密机械研究所获得博士学位，主要从事超强超短激光技术发展及其前沿重要应用等方面的研究。E-mail：" }, { "name": "text", "data": "lengyuxin@mail.siom.ac.cn" } ] ] } ], "email": "lengyuxin@mail.siom.ac.cn", "deceased": false } ], "aff": [ { "id": "aff1", "intro": [ { "lang": "zh", "label": "1", "text": "中国科学院上海光学精密机械研究所 强场激光物理国家重点实验室，上海　201800", "data": [ { "name": "text", "data": "中国科学院上海光学精密机械研究所 强场激光物理国家重点实验室，上海　201800" } ] }, { "lang": "en", "label": "1", "text": "State Key Laboratory of High Field Laser Physics and CAS Center for Excellence in Ultra-Intense Laser Science， Shanghai Institute of Optics and Fine Mechanics， Chinese Academy of Sciences， Shanghai 201800， China", "data": [ { "name": "text", "data": "State Key Laboratory of High Field Laser Physics and CAS Center for Excellence in Ultra-Intense Laser Science， Shanghai Institute of Optics and Fine Mechanics， Chinese Academy of Sciences， Shanghai 201800， China" } ] } ] }, { "id": "aff2", "intro": [ { "lang": "zh", "label": "2", "text": "国科大杭州高等研究院 物理与光电工程学院， 浙江 杭州　310024", "data": [ { "name": "text", "data": "国科大杭州高等研究院 物理与光电工程学院， 浙江 杭州　310024" } ] }, { "lang": "en", "label": "2", "text": "School of Physics and Optoelectronic Engineering， Hangzhou Institute for Advanced Study， UCAS， Hangzhou 310024， China", "data": [ { "name": "text", "data": "School of Physics and Optoelectronic Engineering， Hangzhou Institute for Advanced Study， UCAS， Hangzhou 310024， China" } ] } ] }, { "id": "aff3", "intro": [ { "lang": "zh", "label": "3", "text": "华中科技大学 光学与电子信息学院，湖北 武汉　430075", "data": [ { "name": "text", "data": "华中科技大学 光学与电子信息学院，湖北 武汉　430075" } ] }, { "lang": "en", "label": "3", "text": "Wuhan National Laboratory for Optoelectronics and School of Optical and Electronic Information， Huazhong University of Science and Technology， Wuhan 430074， China", "data": [ { "name": "text", "data": "Wuhan National Laboratory for Optoelectronics and School of Optical and Electronic Information， Huazhong University of Science and Technology， Wuhan 430074， China" } ] } ] }, { "id": "aff4", "intro": [ { "lang": "zh", "label": "4", "text": "中国科学院大学 材料与光电研究中心 北京100049", "data": [ { "name": "text", "data": "中国科学院大学 材料与光电研究中心 北京100049" } ] }, { "lang": "en", "label": "4", "text": "Materials and Optoelectronics Research Center， University of Chinese Academy of Sciences， Beijing 100049", "data": [ { "name": "text", "data": "Materials and Optoelectronics Research Center， University of Chinese Academy of Sciences， Beijing 100049" } ] } ] } ] }, "abstracts": [ { "lang": "zh", "data": [ { "name": "p", "data": [ { "name": "text", "data": "准二维Ruddlesden-Popper（R-P）卤化物钙钛矿具有优越的光电特性，在太阳能电池、发光二极管、激光器等光电器件中受到广泛关注，但严重影响载流子的弛豫和传输特性的激子-声子之间的相互作用，还未得到充分揭示。与广泛研究的三维钙钛矿结构相比，准二维钙钛矿存在天然形成的量子阱结构，具有更大的激子结合能，激子效应更加明显，但对其激子-声子相互作用的研究仍然较少。因此，我们通过溶液法制备了准二维R-P型钙钛矿 （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜，其增益系数高达~1090.62 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "，获得了低阈值（~12.48 μJ/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "）的放大的自发辐射。基于此，我们通过变温荧光光谱（77-300K）和瞬态吸收光谱技术研究了（PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜随温度变化的发光特性，以阐述其内部的激子-声子相互作用对其发光性能的影响，发现在低温域内（77-120 K），由激子-声子相互作用引起的带隙变化相对较弱，晶格热膨胀占主导地位；随着温度升高，激子-声子相互作用对带隙变化产生较大影响。另一方面，激子-声子相互作用会促使发光光谱线宽加宽，但我们在77-120 K的温度范围内观察到了反常线宽变窄现象，这归因于由局域化效应引起的多量子阱中的能量转移机制，直到120 K之后，激子-声子相互作用引起的谱线加宽才足以逆转这一趋势。本文中对准二维钙钛矿的激子-声子相互作用的研究，对于提高准二维钙钛矿光学性能及其发光应用具有指导价值。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "The quasi-2D Ruddlesden-Popper （R-P） halide perovskite has been widely used in solar cells， light-emitting diodes， lasers and other optoelectronic devices due to its excellent photoelectric properties. However， the exciton-phonon interaction， which seriously affects the relaxation and transport characteristics of carriers， has not been fully revealed. Compared with the widely studied 3D perovskite structure， quasi 2D perovskite has a naturally formed quantum well structure with greater exciton binding energy and more obvious exciton effect. However， the exciton-phonon interaction of quasi 2D perovskite is still less studied. Therefore， a quasi-2D R-P perovskite film （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": " has been prepared by solution method with a gain coefficient of ~1090.62 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": " and an amplified spontaneous emission of low threshold （~12.48 μJ/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "）. Based on this， we studied the luminescence properties of （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": " film with temperature variation by using variable temperature fluorescence spectroscopy （77-300K） and transient absorption spectroscopy， in order to elaborate the influence of exciton-phonon interaction on its luminescence properties. It was found that in the low temperature domain （77-120 K）， The bandgap change caused by exciton-phonon interaction is relatively weak， and the lattice thermal expansion is dominant. With the increase of temperature， the exciton-phonon interaction has a great influence on the change of bandgap. On the other hand， the exciton-phonon interaction causes the line width of the luminescence spectrum to widen， but we observed the abnormal line width narrowing in the temperature range of 77-120 K， which is attributed to an energy transfer mechanism in the multi-quantum well caused by the localization effect， until after 120 K， the line widening caused by the exciton-phonon interaction is sufficient to reverse this trend. In this paper， the exciton-phonon interaction of quasi 2D perovskite is of guiding value for improving the optical properties and luminescence applications of quasi 2D perovskite." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "激子-声子相互作用" } ], [ { "name": "text", "data": "准二维钙钛矿" } ], [ { "name": "text", "data": "光谱加宽" } ], [ { "name": "text", "data": "局域化效应" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "exciton-phonon interaction" } ], [ { "name": "text", "data": "quasi-2D perovskite" } ], [ { "name": "text", "data": "spectral broadening" } ], [ { "name": "text", "data": "localization effects" } ] ] } ], "highlights": [], "body": [ { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "1　引　　言" } ], "level": "1", "id": "s1" } }, { "name": "p", "data": [ { "name": "text", "data": "近年来，由于具有带隙可调、吸收能力强、增益系数高、光致发光量子产率高等优点，金属卤化物钙钛矿材料作为一种优异的光伏和发光材料吸引了越来越多的关注" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "1", "type": "bibr", "rid": "R1", "data": [ { "name": "text", "data": "1" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "2", "type": "bibr", "rid": "R2", "data": [ { "name": "text", "data": "2" } ] } } ], "rid": [ "R1", "R2" ], "text": "1-2", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。与三维钙钛矿材料相比，长链有机疏水阳离子，如萘甲胺（NMA）、苯乙胺（PEA）等的引入使得准二维钙钛矿具有更强的环境稳定性、更大的激子结合能和天然的量子阱结构，在发光器件中具有更广阔的应用前景" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "3", "type": "bibr", "rid": "R3", "data": [ { "name": "text", "data": "3" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "7", "type": "bibr", "rid": "R7", "data": [ { "name": "text", "data": "7" } ] } } ], "rid": [ "R3", "R4", "R5", "R6", "R7" ], "text": "3-7", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。准二维钙钛矿作为一种光增益介质，其大的激子结合能和内部固有的从小n相到大n相的“能量漏斗/级联”结构，使其具有高效的能量传输特性，进而载流子更多的在大n相聚集，提升发光效率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "8", "type": "bibr", "rid": "R8", "data": [ { "name": "text", "data": "8" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } } ], "rid": [ "R8", "R9", "R10" ], "text": "8-10", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。2018年，Li等人报道了增益系数高达300 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "的NMA基准二维钙钛矿薄膜，发现光致激发物在几个ps的时间范围内就可以在较低能带隙的量子阱上快速累积，从而便于建立粒子数的反转，最终实现了" }, { "name": "text", "data": "<" }, { "name": "text", "data": "20 μJ/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "的低阈值放大的自发辐射（ASE）" }, { "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": "。得益于准二维钙钛矿优异的光增益特性，不同形貌构成的微腔准二维钙钛矿激光得以迅速实现。薄膜增益介质的灵活性使其可以与外置谐振腔结合制备发光器件" }, { "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": "，但对准二维钙钛矿薄膜本身的发光光谱特性的研究有待进一步加强。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "最近的研究表明，钙钛矿材料具有较长的相干时间和稳定的无明显光谱扩散的发光等激子特性，然而，长的相干时间和窄的发射线宽均要求激子-声子耦合作用较弱" }, { "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": "。但目前较多的相关研究工作都是关注于三维钙钛矿中的激子-声子相互作用" }, { "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": "。与三维钙钛矿相比，大尺寸有机阳离子的存在使得准二维钙钛矿天然的量子阱结构使其具有强的限域效应，因此内部的激子效应更明显，不同n值钙钛矿对其发光特性影响较大" }, { "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": "16", "type": "bibr", "rid": "R16", "data": [ { "name": "text", "data": "16" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。但目前，基于准二维钙钛矿体系的激子-声子相互作用的研究仍然较少，激子-声子相互作用对其发光特性的影响机制仍有待探究。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本文中我们制备了具有较高增益(~1090.62 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": ")和较低ASE阈值(~12.48 μJ/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")的R-P型准二维钙钛矿(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜，并且通过分析其在T=77-300 K的光致发光(PL)温度依赖光谱和瞬态吸收光谱，研究了薄膜中的激子-声子相互作用。研究表明，在低温时（77-120K），准二维钙钛矿带隙改变主要受晶格热膨胀效应影响，激子-声子相互作用并不明显，随着温度的升高（" }, { "name": "text", "data": ">" }, { "name": "text", "data": "120 K），激子-声子相互作用的影响变大，其引起的发光中心红移将抵消掉一部分由晶格热膨胀引起的蓝移作用。另一方面，虽然激子-声子相互作用会贡献一定的光谱线宽加宽，但在77 -120 K的温度范围内，我们观察到了反常线宽窄化现象，这归因于准二维钙钛矿结构中局域化效应引起的多量子阱的能量转移机制。随着温度的升高（" }, { "name": "text", "data": ">" }, { "name": "text", "data": "120 K），激子-声子相互作用引起的谱线加宽才足以逆转这一趋势。本文详细解释了准二维钙钛矿内部的激子-声子相互作用与其他效应协同调控发光特性的作用机制，为基于准二维钙钛矿的光电器件的研究提供了物理基础。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2　实　　验" } ], "level": "1", "id": "s2" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.1　样品准备" } ], "level": "2", "id": "s2a" } }, { "name": "p", "data": [ { "name": "text", "data": "苯乙基溴化铵（PEABr）购自西安宝莱特。溴化铅（PbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "，99.999%）、溴化铯（CsBr，99.999%）和二甲亚砜（DMSO，无水，99.9%）购自阿拉丁试剂。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.2　钙钛矿薄膜的制备" } ], "level": "2", "id": "s2b" } }, { "name": "p", "data": [ { "name": "text", "data": "将1 mmol PbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "、1 mmol CsBr和0.6 mmol PEABr溶解在5mL DMSO中以制备钙钛矿前驱体溶液。在80℃下搅拌前驱体溶液8小时。同时，用去离子水、丙酮和异丙醇超声清洗玻璃基片，并在使用前用臭氧等离子体处理20分钟。然后，将钙钛矿前驱体溶液以3000 r.p.m的速度旋涂在玻璃基片上30秒，并在100℃的热板上热退火10分钟，以除去残留的溶剂。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.3　测试表征" } ], "level": "2", "id": "s2c" } }, { "name": "p", "data": [ { "name": "text", "data": "紫外-可见吸收光谱是在室温下用双光束紫外可见分光光度计（UV1901PCS，yoke，中国）在300 nm 到 800 nm 范围内测量。泵浦源是一个钛宝石再生放大器（800 nm，35 fs，1 kHz）。激发波长为400 nm的激光脉冲，由基频光通过在200 μm厚的BBO晶体中进行倍频产生。用柱面透镜聚焦泵浦光而得到的飞秒激光被用来测量荧光和 ASE光谱。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "对于变温光致发光光谱测量实验，样品被放入数字控温的真空低温器（MicrostatN2, Oxford Instruments）。激发光源是波长为405 nm的连续光，并由一个透镜聚焦（焦距f = 10 cm），信号收集器是一组具有背散射几何形状的透镜。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "变温瞬态吸收光谱实验是在一个商业化设备（Helios fire, ultrafast system）结合自建的温控系统进行的。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3　结果与讨论" } ], "level": "1", "id": "s3" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.1　样品发光性能表征" } ], "level": "2", "id": "s3a" } }, { "name": "p", "data": [ { "name": "text", "data": "我们通过溶液法制备了具有R-P结构的准二维钙钛矿(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜，在激发光照射下显示出优异的发光性能。" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "a是(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜在室温下的紫外-可见吸收光谱，显示了在402 nm、432 nm、460 nm和510 nm处有四个明显的激子吸收峰，分别对应于无机层数n=1、n=2、n=3和n≥5的量子阱，表明制备的准二维钙钛矿(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜中存在多量子阱结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "text", "data": ", " }, { "name": "xref", "data": { "text": "17", "type": "bibr", "rid": "R17", "data": [ { "name": "text", "data": "17" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "b显示了(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜在室温下的荧光和ASE光谱，荧光峰位~519 nm，与荧光谱相比，ASE峰位显示出明显的红移，峰位~536 nm。由于小n相载流子可以快速转移到最低能带，因此只能观察到属于n≥5相的荧光峰。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "准二维钙钛矿（PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜的光学特性。（a） 吸收光谱。（b） 荧光和ASE光谱。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.1" } ], "title": [ { "name": "text", "data": "Optical properties of the quasi-2D perovskite （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": " films. （a） Optical absorption spectrum. （b） PL and ASE spectra." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481359&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481361&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481360&type=", "width": "110.80941772", "height": "45.44785309", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "光学增益系数是评估材料发光性能的一个关键参数。(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜的光学增益系数可以通过可变条纹长度（VSL）方法测量，其中泵浦光被一个柱面透镜聚焦成一条长条纹线，其长度由一个可调节的狭缝控制" }, { "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": "，可通过调节狭缝宽度改变激发长度。如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "a所示，光谱发光强度随着狭缝宽度的增加而变大，当条纹长度超过0.009 cm时出现明显的ASE峰，这表示需要一定程度的光放大来克服传播损耗。" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "b描述了" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "a中发光强度与条纹长度的关系，可以用函数关系式描述为：" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "19", "type": "bibr", "rid": "R19", "data": [ { "name": "text", "data": "19" } ] } }, { "name": "text", "data": "]" } ] } ] }, { "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=39481363&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481362&type=", "width": "39.53932953", "height": "5.24933338", "fontsize": "" } } }, { "name": "text", "data": " " } ], "id": "DF1" } }, { "name": "p", "data": [ { "name": "text", "data": "其中" }, { "name": "italic", "data": [ { "name": "text", "data": "I" } ] }, { "name": "text", "data": "、" }, { "name": "italic", "data": [ { "name": "text", "data": "I" }, { "name": "sub", "data": [ { "name": "text", "data": "s" } ] } ] }, { "name": "text", "data": "、A、" }, { "name": "italic", "data": [ { "name": "text", "data": "G" } ] }, { "name": "text", "data": "和" }, { "name": "italic", "data": [ { "name": "text", "data": "L" } ] }, { "name": "text", "data": "分别是发光强度、单位体积的自发辐射率、激发体积的截面积、光学增益系数和条纹长度。根据" }, { "name": "xref", "data": { "text": "公式（1）", "type": "disp-formula", "rid": "DF1", "data": [ { "name": "text", "data": "公式（1）" } ] } }, { "name": "text", "data": "，我们拟合了L=0.001~0.01 cm的荧光强度-条纹长度曲线，可估算该薄膜光学增益系数G高达~1090.6 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "，在钙钛矿中居于前列，这非常有利于实现受激辐射光放大" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "23", "type": "bibr", "rid": "R23", "data": [ { "name": "text", "data": "23" } ] } } ], "rid": [ "R20", "R21", "R22", "R23" ], "text": "20-23", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "（a）不同条纹长度激发下的发光光谱。（b）发光强度与条纹长度的关系图。（c）泵浦光强度依赖性发光光谱。（d）发光强度和光谱线宽随泵浦光强度变化趋势。（e）不同温度下（PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜的发光强度随泵浦强度的变化趋势。（f）不同温度下ASE阈值，红色实线为拟合曲线。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.2" } ], "title": [ { "name": "text", "data": "（a） Luminescence spectra under excitation of different stripe lengths. （b） The relationship between luminescence intensity and stripe length. （c） Pump-fluence-dependent luminescence spectra. （d） The variation trend of luminescence intensity and spectral line width with pump intensity. （e） Trend of luminescence intensity of （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": " thin films with pump intensity at different temperatures （PEA）. （f） ASE threshold at different temperatures. The solid red line is fitting." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481364&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481366&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481365&type=", "width": "146.50900269", "height": "106.59200287", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "我们进一步研究了激发强度依赖的薄膜发光特性。如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "c所示，薄膜发光强度随着激发光能量密度的增大发生明显变化。在低能量密度激发下，发光光谱半高全宽（FWHM）为24.12 nm，强度线性增大，随着泵浦能量密度进一步增大，发光峰波长发生明显红移，FWHM窄化到5.03 nm，同时强度发生显著非线性增强，表明ASE的发生。" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "d具体描述了薄膜发光强度和FWHM随激发能量密度出现的明显阈值行为和增益导致的光谱窄化，其拐点激发能量密度为~12.48 μJ/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "，即ASE阈值。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "为了进一步研究(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜增益特性的温度依赖性，我们研究了不同的温度下薄膜的发光行为，" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "e显示了不同温度（77、100、150、200和300 K）下的薄膜ASE发光强度与相应泵浦强度的变化关系，发现薄膜的ASE阈值随着温度升高而略微增大，在77 K升温到300 K时，ASE阈值从4.32 μJ/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "增至13.38 μJ/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "。 这可以归因于随温度上升，准二维钙钛矿内激子发生解离，同时随着温度上升，纵向光学声子数增加，激子-声子耦合增强，均使得非辐射复合概率增大，导致发光效率变低，增大了ASE阈值" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "24", "type": "bibr", "rid": "R24", "data": [ { "name": "text", "data": "24" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。为了量化ASE阈值特性，ASE的阈值与温度的关系可以用指数函数表示，利用特征温度" }, { "name": "italic", "data": [ { "name": "text", "data": "T" }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] } ] }, { "name": "text", "data": "表示ASE阈值对温度变化的容忍能力。可用以下公式表示这种关系" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "25", "type": "bibr", "rid": "R25", "data": [ { "name": "text", "data": "25" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "26", "type": "bibr", "rid": "R26", "data": [ { "name": "text", "data": "26" } ] } } ], "rid": [ "R25", "R26" ], "text": "25-26", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "：" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（2）" } ], "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481368&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481367&type=", "width": "36.06800079", "height": "5.33400011", "fontsize": "" } } }, { "name": "text", "data": " " } ], "id": "DF2" } }, { "name": "p", "data": [ { "name": "text", "data": "其中" }, { "name": "italic", "data": [ { "name": "text", "data": "P" }, { "name": "sub", "data": [ { "name": "text", "data": "th" } ] }, { "name": "text", "data": "(T)" } ] }, { "name": "text", "data": "和" }, { "name": "italic", "data": [ { "name": "text", "data": "P" }, { "name": "sub", "data": [ { "name": "text", "data": "th,0" } ] } ] }, { "name": "text", "data": "分别为温度为" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": " K和低温时的受激辐射阈值，" }, { "name": "italic", "data": [ { "name": "text", "data": "T" }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] } ] }, { "name": "text", "data": "是特征温度。拟合得到该薄膜的特征温度为184.55 K（" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "f），这表明(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜的ASE特性对温度变化相对不敏感，具有非常好的稳定性" }, { "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": "。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.2　变温光致发光光谱分析" } ], "level": "2", "id": "s3b" } }, { "name": "p", "data": [ { "name": "text", "data": "为了研究(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜中晶格热膨胀和激子-声子耦合作用对其发光强度、发光波长及光谱半高宽的影响，我们利用功率为0.7 mW，波长为405 nm的连续光激发，测得其温度范围为77-300 K的荧光光谱。如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "a所示，在77 K到300 K的温度范围内，发光强度随着温度的升高而下降。这主要是因为随着温度的升高，纵向光学声子数增加，导致激子-声子耦合增强，从而提高了非辐射跃迁的概率，削弱了发光效率" }, { "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": "。相应的光谱积分强度随温度的变化如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "b所示，可根据" }, { "name": "xref", "data": { "text": "公式（3）", "type": "disp-formula", "rid": "DF3", "data": [ { "name": "text", "data": "公式（3）" } ] } }, { "name": "text", "data": "进行拟合" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "30", "type": "bibr", "rid": "R30", "data": [ { "name": "text", "data": "30" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "31", "type": "bibr", "rid": "R31", "data": [ { "name": "text", "data": "31" } ] } } ], "rid": [ "R30", "R31" ], "text": "30-31", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "：" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（3）" } ], "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481370&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481369&type=", "width": "29.37933159", "height": "7.87400007", "fontsize": "" } } }, { "name": "text", "data": " " } ], "id": "DF3" } }, { "name": "p", "data": [ { "name": "text", "data": "其中" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "是温度，" }, { "name": "italic", "data": [ { "name": "text", "data": "I(T)" } ] }, { "name": "text", "data": "和" }, { "name": "italic", "data": [ { "name": "text", "data": "I" }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] } ] }, { "name": "text", "data": "分别是温度为" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "和0 K（或低温）时的荧光光谱积分强度，" }, { "name": "italic", "data": [ { "name": "text", "data": "A" } ] }, { "name": "text", "data": "是常数，" }, { "name": "italic", "data": [ { "name": "text", "data": "k" }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] } ] }, { "name": "text", "data": "是玻尔兹曼常数，" }, { "name": "italic", "data": [ { "name": "text", "data": "E" }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] } ] }, { "name": "text", "data": "是热激活能。经过拟合（" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "b中红色曲线），可以得到其热激活能为44.46 meV，大于室温热能。相对大的" }, { "name": "italic", "data": [ { "name": "text", "data": "E" }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] } ] }, { "name": "text", "data": "值对于实现激子发光更加有利，因此，(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜中的激子相对比较稳定，适合用作光发射材料" }, { "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": "。" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "c显示了准二维钙钛矿薄膜的发光峰值能量的温度依赖性。可见，在77-120 K的温度范围内，薄膜的发射中心光子能量随着温度的升高而线性快速增大，然而在120至300K范围内，光子能量只变化了17.68 meV。在77-300 K的温度范围内，(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "准二维钙钛矿中的激子-声子相互作用主要是由Fröhlich耦合的纵向光学(LO)声子散射主导的，声学声子散射可以忽略不计。因此，我们采用了仅考虑LO声子影响的单振子模型进行分析" }, { "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": "。考虑到晶格体积随温度线性膨胀，晶格热膨胀和激子-声子耦合对PL峰值能量的共同影响可以用以下公式来拟合" }, { "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": "26", "type": "bibr", "rid": "R26", "data": [ { "name": "text", "data": "26" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "：" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（4）" } ], "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481372&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481371&type=", "width": "72.47466278", "height": "12.95400047", "fontsize": "" } } }, { "name": "text", "data": " " } ], "id": "DF4" } }, { "name": "p", "data": [ { "name": "text", "data": "其中T是温度，" }, { "name": "italic", "data": [ { "name": "text", "data": "E" }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] } ] }, { "name": "text", "data": "是0 K时的非重整化带隙能。" }, { "name": "italic", "data": [ { "name": "text", "data": "β" }, { "name": "sub", "data": [ { "name": "text", "data": "TE" } ] } ] }, { "name": "text", "data": "，" }, { "name": "italic", "data": [ { "name": "text", "data": "β" }, { "name": "sub", "data": [ { "name": "text", "data": "EP" } ] } ] }, { "name": "text", "data": "，" }, { "name": "italic", "data": [ { "name": "text", "data": "k" }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] } ] }, { "name": "text", "data": "，和" }, { "name": "italic", "data": [ { "name": "text", "data": "ћω" } ] }, { "name": "text", "data": "分别是晶格的热膨胀系数、激子-声子耦合作用系数、玻尔兹曼常数和声子能量。由于声子分布的影响，在0 K时会发生带隙重整，带隙重整化能𝐸" }, { "name": "sub", "data": [ { "name": "text", "data": "𝑔" } ] }, { "name": "text", "data": "(𝑇" }, { "name": "text", "data": "=0)=𝐸" }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "+𝛽" }, { "name": "sub", "data": [ { "name": "text", "data": "𝐸𝑃" } ] }, { "name": "text", "data": "，经过拟合，可得" }, { "name": "italic", "data": [ { "name": "text", "data": "E" }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] } ] }, { "name": "text", "data": "=2.42 eV，晶格热膨胀系数" }, { "name": "italic", "data": [ { "name": "text", "data": "β" }, { "name": "sub", "data": [ { "name": "text", "data": "TE" } ] } ] }, { "name": "text", "data": "=0.30 meV/K，激子-声子耦合作用系数" }, { "name": "italic", "data": [ { "name": "text", "data": "β" }, { "name": "sub", "data": [ { "name": "text", "data": "EP" } ] } ] }, { "name": "text", "data": "=-71.47 meV，以及平均光学声子能量" }, { "name": "italic", "data": [ { "name": "text", "data": "ћω" } ] }, { "name": "text", "data": "=43.59 meV。如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "c所示，当" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "=0 K时，对应薄膜中热膨胀对带隙没有贡献的重整化的带隙值，即𝐸" }, { "name": "sub", "data": [ { "name": "text", "data": "𝑔" } ] }, { "name": "text", "data": "(𝑇" }, { "name": "text", "data": "=0)=𝐸" }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "+𝛽" }, { "name": "sub", "data": [ { "name": "text", "data": "𝐸𝑃" } ] }, { "name": "text", "data": "=2.276 𝑒" }, { "name": "text", "data": "𝑉" }, { "name": "text", "data": "，" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "c中的黑色实线是其重整化带隙能。" } ] }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "（a）在波长为405 nm， 泵浦功率为0.7 mW的连续光激发下，（PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": " 薄膜从77到300 K的随温度变化的PL光谱。（b） PL积分强度与温度的关系，红线为非线性拟合曲线。（c） （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜发光峰峰值能量与温度的关系图。灰色和红色的虚线分别表示晶格热膨胀和激子-声子耦合相互作用的贡献。红色实线代表两者整体贡献。（d）发光谱的FWHM与温度之间的变化关系。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.3" } ], "title": [ { "name": "text", "data": "（a） Photoluminescence spectra of （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": " films with temperature from 77 to 300 K under continuous optical excitation at a wavelength of 405 nm with a pump power of 0.7 mW. （b） Integrated PL intensity as a function of temperature. The red line represents a nonlinear fitting. （c） Temperature-dependence of the peak energy of （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": " films. The gray and red dashed lines show the contributions of thermal expansion and exciton -phonon interaction， respectively. The solid red line is overall. （d） The function between temperature and FWHM." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481373&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481375&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481374&type=", "width": "105.84609985", "height": "89.93842316", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "具体地，不同温度条件下，准二维钙钛矿的带隙变化是由晶格热膨胀和激子-声子耦合效应共同影响的（分别由" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "c中黑色和红色虚线描述）。在低温条件下（77 K" }, { "name": "text", "data": "<" }, { "name": "text", "data": "T" }, { "name": "text", "data": "<" }, { "name": "text", "data": "120 K），考虑到纵向光学声子模式的数量接近零，发光带隙主要由晶格热膨胀效应而不是激子-声子耦合主导，这导致了峰值位置的线性蓝移和光子能量的线性增加。而随着温度的增加（T" }, { "name": "text", "data": ">" }, { "name": "text", "data": "120 K），声子模式的数量相应增加，导致激子-声子的相互作用变得显著。此时激子-声子耦合作用对PL光谱中心波长的影响快速增大，其引起的光谱红移，将抵消掉一部分由晶格热膨胀引起的蓝移作用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "36", "type": "bibr", "rid": "R36", "data": [ { "name": "text", "data": "36" } ] } } ], "rid": [ "R33", "R34", "R35", "R36" ], "text": "33-36", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，在晶格热膨胀和激子-声子相互作用的共同影响下，PL峰位首先线性蓝移，然后移速逐渐变缓，最后趋于稳定。" } ] }, { "name": "p", "data": [ { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "d显示了(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜的PL光谱的FWHM与温度的关系。在低温条件下（77 K-120 K），FWHM从54.00 meV下降到49.42 meV，出现反常的光谱窄化，而在高温条件下（120 K-300 K），FWHM增加到89.04 meV，总体呈现出\"√\"形的变化趋势。不同温度下(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "的发光光谱谱宽主要是由于晶体中的晶格振动引起的，这些由形变势、压电和Fröhlich相互作用导致的振动以不同的方式扰动激子的运动。表示如下" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } } ], "rid": [ "R37", "R38" ], "text": "37-38", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "：" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（5）" } ], "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481377&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481376&type=", "width": "86.27533722", "height": "8.80533314", "fontsize": "" } } }, { "name": "text", "data": "，" } ], "id": "DF5" } }, { "name": "p", "data": [ { "name": "text", "data": "其中第一项" }, { "name": "italic", "data": [ { "name": "text", "data": "Γ" }, { "name": "sub", "data": [ { "name": "text", "data": "inh" } ] } ] }, { "name": "text", "data": "是由激子-激子相互作用和晶体的无序性引起的散射产生的不均匀展宽，是一个与温度无关的常数。第二项中T是温度，" }, { "name": "italic", "data": [ { "name": "text", "data": "φ" }, { "name": "sub", "data": [ { "name": "text", "data": "AC" } ] } ] }, { "name": "text", "data": "是激子-声学声子耦合相互作用系数，主要与形变势相互作用有关，与温度呈线性相关。第三项中" }, { "name": "italic", "data": [ { "name": "text", "data": "φ" }, { "name": "sub", "data": [ { "name": "text", "data": "LO" } ] } ] }, { "name": "text", "data": "是激子-纵向光学声子耦合相互作用系数（Fröhlich相互作用系数），它与LO声子的玻色-爱因斯坦分布有关，即" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481379&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481378&type=", "width": "22.01333237", "height": "7.19666624", "fontsize": "" } } } ] }, { "name": "text", "data": "，这里" }, { "name": "italic", "data": [ { "name": "text", "data": "E" }, { "name": "sub", "data": [ { "name": "text", "data": "LO" } ] } ] }, { "name": "text", "data": "是LO声子的平均能量，" }, { "name": "italic", "data": [ { "name": "text", "data": "k" } ] }, { "name": "text", "data": "是玻尔兹曼常数，" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "是温度。最后一项" }, { "name": "italic", "data": [ { "name": "text", "data": "φ" }, { "name": "sub", "data": [ { "name": "text", "data": "imp" } ] } ] }, { "name": "text", "data": "是杂质项，它是由于完全电离杂质的散射而产生的线宽，大小由它们的平均结合能" }, { "name": "italic", "data": [ { "name": "text", "data": "E" }, { "name": "sub", "data": [ { "name": "text", "data": "b" } ] } ] }, { "name": "text", "data": "决定。考虑到(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜的杂质非常少，可以忽略杂质引起的光谱展宽变化，即" }, { "name": "italic", "data": [ { "name": "text", "data": "Γ" }, { "name": "sub", "data": [ { "name": "text", "data": "imp" } ] } ] }, { "name": "text", "data": "=0。又考虑到声学声子能很小， 因此激子与声学声子散射导致的光谱变化也可忽略。在此条件下，从120 K到300 K的实验数据被拟合为" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "d中的红色曲线。其中，与温度无关的非均匀增宽项" }, { "name": "italic", "data": [ { "name": "text", "data": "Г" }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] } ] }, { "name": "text", "data": "=45.48 meV，激子-纵向光学声子耦合系数" }, { "name": "italic", "data": [ { "name": "text", "data": "φ" }, { "name": "sub", "data": [ { "name": "text", "data": "LO" } ] } ] }, { "name": "text", "data": "=195.42 meV，纵向光学声子能量" }, { "name": "italic", "data": [ { "name": "text", "data": "E" }, { "name": "sub", "data": [ { "name": "text", "data": "LO" } ] } ] }, { "name": "text", "data": "=43.50 meV，与平均光学声子能相当。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.3　瞬态吸收动力学研究" } ], "level": "2", "id": "s3c" } }, { "name": "p", "data": [ { "name": "text", "data": "为了进一步研究(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜的光谱加宽机制，我们分析了其内部的载流子动力学行为。" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "a是在100 K的温度下，(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜的瞬态吸收光谱（TAS），" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "b是不同时间下的吸收变化光谱，可以看到在432 nm和517 nm附近处有两个由态填充效应引起的基态漂白（GSB）峰（负信号），分别对应小n项（n=2）和大n项（n≥5）的量子阱。如" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "c所示，n=2相的GSB信号在0.50皮秒内发生迅速衰减，并在~13.10皮秒内衰减到零，而n≥5相在1.30皮秒内迅速建立，发生了明显的从高能带隙的量子阱到低能带隙的量子阱的超快载流子转移过程。小n相较长的衰减寿命表明在低温下载流子传输的不充分，会引起载流子局域聚集。而在300 K时，如" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "d-f所示，最低带隙n≥5的GSB信号仍然存在，建立时间小于1 皮秒，但n=2相的GSB信号变得很弱，这归因于当温度升高到300 K后，载流子在低维相的局域效应减弱，而在较低低能带隙的量子阱上累积。" } ] }, { "name": "fig", "data": { "id": "F4", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图4" } ], "title": [ { "name": "text", "data": "（a）100 K温度下（PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": " 薄膜的TAS。（b）选定时间尺度的TAS（T=100 K）。（c）432 nm和517 nm处的动力学曲线（T=100 K）。（d）300 K温度下薄膜的TAS。（e）选定时间尺度的TAS（T=300 K）。（f） 433 nm和514 nm处的动力学曲线（T=300 K）。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.4" } ], "title": [ { "name": "text", "data": "TA spectra of （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": " films. （a） TA spectra of the film （T=100 K）. （b） TA spectra at selected timescales （T=100 K）. （c） Kinetic curves at 432 nm and 517 nm （T=100 K）. （d） TA spectra of the film （T=300 K）. （e） TA spectra at selected timescales （T=300 K）. （f） Kinetic curves at 433 nm and 514 nm （T=300 K）." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481380&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481382&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481381&type=", "width": "162.79998779", "height": "93.14813232", "fontsize": "" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.4　载流子局域化效应" } ], "level": "2", "id": "s3d" } }, { "name": "p", "data": [ { "name": "text", "data": "准二维钙钛矿中随温度升高光谱线宽变窄的现象与材料内部的多量子阱结构和能量转移密切相关，可以用局域化效应来解释，主要因为在材料内部存在一种载流子转移机制。具体地说，在低温条件(77 K" }, { "name": "text", "data": "<" }, { "name": "text", "data": "T" }, { "name": "text", "data": "<" }, { "name": "text", "data": "120 K)下，载流子随机地分布在能量最低位之间（" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "a）。随着温度的升高，接近120 K时，小n项量子阱处的载流子逐渐变少，同时弱局域化的载流子被热激活，并通过跳跃弛豫达到饱和再分布到强局域化状态的其他低能量区域（" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "b）。在这个过程中，线宽会明显变窄。之后，随着温度进一步升高（" }, { "name": "text", "data": ">" }, { "name": "text", "data": "120 K），载流子的热化开始变得更加关键，激子声子耦合效应逐渐占据主导作用，导致了线宽的显著增加。这在传统的半导体材料如InGaN/GaN量子阱中也观察到类似的光谱线宽变窄现象" }, { "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": "。" } ] }, { "name": "fig", "data": { "id": "F5", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图5" } ], "title": [ { "name": "text", "data": "不同温度下载流子在多量子阱结构中转移的可能机制。（a）-（c）分别表示载流子在低、中、高温下的分布情况。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.5" } ], "title": [ { "name": "text", "data": "The possible mechanism of carriers transferring in the MQWs structure at different temperatures. （a）-（c） represent the distribution of carriers at low， medium， and high temperatures， respectively." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481383&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481385&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481384&type=", "width": "77.69583130", "height": "19.48111916", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "a显示在增大了激发功率后（～1.1 mW），测得的变温荧光光谱（77-300 K），PL强度随着温度的升高而下降，这与" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "a表现出的现象一致。然而我们提取了随温度变化的FWHM信息绘制在" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "b中，发现" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "d中的从77 K到120 K的FWHM反常窄化消失了，这可以归因于激发光功率的增加，即载流子浓度的增加，削弱了局域化效应的影响。在T" }, { "name": "text", "data": ">" }, { "name": "text", "data": "120 K后，FWHM与低激发功率下（~0.7 mW）的变化趋势相似，可以归因于载流子的热效应占主导地位，而局域化效应对FWHM的影响相对较弱。说明当激发光功率增加时，由于局域化效应的减弱，导致与温度有关的光谱窄化幅度变小，异常的光谱窄化现象消失，谱线宽度随着温度的升高在整个温度域内单调增加。" } ] }, { "name": "fig", "data": { "id": "F6", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图6" } ], "title": [ { "name": "text", "data": "（a） 在波长为405 nm， 泵浦功率为1.1 mW的连续光激发下，从77到300 K的（PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜随温度变化的光致发光光谱。（b） （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜PL谱的FWHM与温度之间的函数关系。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.6" } ], "title": [ { "name": "text", "data": "Photoluminescence spectra of （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": " films with temperature from 77 to 300 K under continuous optical excitation at a wavelength of 405 nm and a pump power of 1.1 mW. （b） The function between temperature and FWHM of （PEA）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": " films." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481386&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481388&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39481387&type=", "width": "100.90731812", "height": "47.33421707", "fontsize": "" } ] } } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4　结　　论" } ], "level": "1", "id": "s4" } }, { "name": "p", "data": [ { "name": "text", "data": "综上所述，准二维钙钛矿(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜表现出了优异的光增益特性，具有~1090.62 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "的高光增益系数和~12.48 μJ/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "的低ASE阈值。通过进一步研究温度依赖发光光谱，分析晶格热膨胀和激子-声子耦合对(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜的发光带隙和线宽的影响。发现准二维钙钛矿(PEA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "n-1" } ] }, { "name": "text", "data": "Pb" }, { "name": "sub", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "3n+1" } ] }, { "name": "text", "data": "薄膜中存在的多量子阱结构和能量漏斗效 应，这种强局域化的能量转移机制，可以抑制低温下光谱线宽增加。研究结果可以为提升准二维钙钛矿材料与器件光学性能提供有力指导。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本文（补充文件及）专家审稿意见和作者回复内容下载地址：" }, { "name": "extlink", "data": { "text": [ { "name": "text", "data": "http://cjl.lightpublishing.cn/thesisDetails#10.37188/CJL.20220" } ], "href": "http://cjl.lightpublishing.cn/thesisDetails#10.37188/CJL.20220" } }, { "name": "text", "data": "***." } ] } ] } ], "footnote": [], "reflist": { "title": [ { "name": "text", "data": "参考文献" } ], "data": [ { "id": "R1", "label": "1", "citation": [ { "lang": "en", "text": [ { "name": "text", "data": "LIU X K" }, { "name": "text", "data": "， " }, { "name": "text", "data": "XU W" }, { "name": "text", "data": "， " }, { "name": "text", "data": "BAI S" }, { "name": "text", "data": "， " }, { "name": "text", "data": "et al" }, { "name": "text", "data": ". 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