Luminescence with Band-tail States and Thermal Disorder Analysis of CsFAMA Mixed Cationic Perovskite

ZHANG Gui-yin; WU Xiao-rui; WANG Ye; ZHAO Jin-jin; DANG Wei

doi:10.37188/CJL.20220268

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Luminescence with Band-tail States and Thermal Disorder Analysis of CsFAMA Mixed Cationic Perovskite

Synthesis and Properties of Materials | Updated：2023-02-13

- Luminescence with Band-tail States and Thermal Disorder Analysis of CsFAMA Mixed Cationic Perovskite Enhanced Publication
- Chinese Journal of Luminescence Vol.43, Issue 12, (2022)
- Affiliations：
  
  Department of Mathematics and Physics， North China Electric Power University,Baoding,China,071003;School of Materials Science and Engineering， Shijiazhuang Tiedao University,Shijiazhuang,China,050043;College of Physical Science and Technology， Hebei University,Baoding,China,071002;Hebei Provincial Center for Optical Sensing Innovation,Baoding,China,071002
- Author bio：
- Funds：
  
  Hebei Natural Science Foundation Project(F2017201136)
- DOI：10.37188/CJL.20220268 CLC： O482.31
- Published：05 December 2022，
  
  Received：11 July 2022，
  
  Revised：26 July 2022，
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张贵银,武晓蕊,王烨等.CsFAMA混合阳离子钙钛矿的带尾态发光和热无序度分析[J].发光学报,2022,43(12):1938-1947.

ZHANG Gui-yin,WU Xiao-rui,WANG Ye,et al.Luminescence with Band-tail States and Thermal Disorder Analysis of CsFAMA Mixed Cationic Perovskite[J].Chinese Journal of Luminescence,2022,43(12):1938-1947.
张贵银,武晓蕊,王烨等.CsFAMA混合阳离子钙钛矿的带尾态发光和热无序度分析[J].发光学报,2022,43(12):1938-1947. DOI： 10.37188/CJL.20220268.

ZHANG Gui-yin,WU Xiao-rui,WANG Ye,et al.Luminescence with Band-tail States and Thermal Disorder Analysis of CsFAMA Mixed Cationic Perovskite[J].Chinese Journal of Luminescence,2022,43(12):1938-1947. DOI： 10.37188/CJL.20220268.

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"name": "text", "data": "（以下简称CsFAMA混合阳离子钙钛矿）薄膜的发光过程进行研究。在245 K附近观测到相变引起的CsFAMA混合阳离子钙钛矿发光光谱红移现象。根据Saha‐Langmuir方程计算结果，确认温度高于65 K时电子空穴复合主导CsFAMA混合阳离子钙钛矿发光过程。利用带间发光与带尾态发光组合模型拟合CsFAMA混合阳离子钙钛矿的发光光谱，得到65~295 K温度范围内的带尾态扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "（0.023~0.045 eV）与载流子等效温度。根据CsFAMA混合阳离子钙钛矿的发光动力学曲线分析，确定电子空穴复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "随热力学温度升高（65~295 K）而不断降低。本文实验结果表明，热力学温度升高引起的晶格振动加剧，有利于实现自由载流子与晶格间的热交换，但增加了体系的热无序度，抑制了电子空穴的辐射复合，加快了载流子的非辐射复合速率。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "In this paper， the luminescence process of Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "0.05" } ] }, { "name": "text", "data": "FA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.81" } ] }, { "name": "text", "data": "MA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.14" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2.55" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "0.45" } ] }, { "name": "text", "data": "（hereinafter referred to as CsFAMA mixed cationic perovskite） thin film was studied by steady-state and transient photoluminescence（PL） spectroscopy. The phase transition induced PL spectra red shift was observed at about 245 K. According to the results of Saha-Langmuir equation， it is confirmed that electron hole recombination dominates the luminescence process of CsFAMA mixed cation perovskite when the temperature is higher than 65 K. The PL spectra of CsFAMA mixed cation perovskite were fitted by the combined model of interband luminescence and band tail luminescence. The band tail extendsion " }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "（0.023-0.045 eV） and the carrier equivalent temperature were obtained in the temperature range of 65-295 K. The experimental results show that the electron hole recombination rate constant " }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": " decreases with the increase of thermodynamic temperature（65-295 K） on the basis of analysis of the luminescence kinetics curve of CsFAMA mixed cationic perovskite. The increase of thermodynamic temperature causes the enhancement of lattice vibration， which is conducive to the heat exchange between free carriers and lattice. Meanwhile it increases the thermal disorder， leading to suppress of electron and hole radiative recombination and accelerate of carrier nonradiative recombination." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "发光" } ], [ { "name": "text", "data": "带尾态" } ], [ { "name": "text", "data": "热无序" } ], [ { "name": "text", "data": "相变" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "luminescence" } ], [ { "name": "text", "data": "band-tail state" } ], [ { "name": "text", "data": "thermal disorder" } ], [ { "name": "text", "data": "phase transition" } ] ] } ], "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": "有机金属卤化物钙钛矿材料（以下简称钙钛矿）结构式为" }, { "name": "italic", "data": [ { "name": "text", "data": "ABX" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "，其中" }, { "name": "italic", "data": [ { "name": "text", "data": "A" } ] }, { "name": "text", "data": "可以为CH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "NH" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "（MA）、HC（NH" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "）" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "（FA）、Cs，" }, { "name": "italic", "data": [ { "name": "text", "data": "B" } ] }, { "name": "text", "data": "可以为Pb、Sn，" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "text", "data": "可以为Cl、Br、I。低温溶液法制备的钙钛矿薄膜具有较大的光吸收系数、高电荷迁移率、可调带隙、较低的电子空穴结合能、较长的载流子寿命和较长的扩散长度等优点" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "1", "type": "bibr", "rid": "R1", "data": [ { "name": "text", "data": "1" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "3", "type": "bibr", "rid": "R3", "data": [ { "name": "text", "data": "3" } ] } } ], "rid": [ "R1", "R2", "R3" ], "text": "1-3", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。钙钛矿材料已经成功应用于光伏太阳能电池、发光二极管、光电探测器和激光器等领域" }, { "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": "9", "type": "bibr", "rid": "R9", "data": [ { "name": "text", "data": "9" } ] } } ], "rid": [ "R4", "R5", "R6", "R7", "R8", "R9" ], "text": "4-9", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。相对于MAPb" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "、FAPb" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "（" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "text", "data": "为Cl、Br、I），混合阳离子、混合卤素阴离子钙钛矿可以实现更加优异的光电性能。例如，FA/Cs混合离子钙钛矿可以拓展带隙调节范围和实现更高的载流子迁移率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "11", "type": "bibr", "rid": "R11", "data": [ { "name": "text", "data": "11" } ] } } ], "rid": [ "R10", "R11" ], "text": "10-11", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。在FA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.83" } ] }, { "name": "text", "data": "MA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.17" } ] }, { "name": "text", "data": "Pb（I" }, { "name": "sub", "data": [ { "name": "text", "data": "0.83" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "0.17" } ] }, { "name": "text", "data": "）" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "基础上引入Cs离子可以进一步减少缺陷态密度、提升载流子寿命" }, { "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": "。文献同时报道了（Cs,FA,MA）Pb（I,Br）" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "混合离子钙钛矿晶体结构的相变行为受到抑制" }, { "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": "。基于Cs、FA、MA三元阳离子钙钛矿太阳能电池的光电转换效率已经突破21%" }, { "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": "，且可以实现至少10 000 h的水-氧稳定性，1 000 h的光稳定性和出色的热稳定性" }, { "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": "。与此同时，混合离子钙钛矿的光物理性质也成为关注的焦点。例如，扫描隧道谱分析表明，FA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.79" } ] }, { "name": "text", "data": "MA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.16" } ] }, { "name": "text", "data": "Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "0.05" } ] }, { "name": "text", "data": "Pb（I" }, { "name": "sub", "data": [ { "name": "text", "data": "0.83" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "0.17" } ] }, { "name": "text", "data": "）" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "混合离子钙钛矿的束缚能级深度小于MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "16", "type": "bibr", "rid": "R16", "data": [ { "name": "text", "data": "16" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。在混合离子钙钛矿薄膜中，原子尺寸差异、电负性差异引入更多的结构无序和更加明显的带尾态" }, { "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": "。同时，Cs、K等碱金属阳离子" }, { "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": "或者混合卤素阴离子" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "19", "type": "bibr", "rid": "R19", "data": [ { "name": "text", "data": "19" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "还会延缓热载流子冷却过程，增加等效载流子温度。相比于MAPb" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "、FAPb" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "，混合离子钙钛矿具有更加无序的结构和更长的热载流子冷却时间。理解混合阳离子混合卤素离子钙钛矿材料的发光过程对于开发相关光电器件有重要意义，而目前还缺乏结构无序、带尾态对混合离子钙钛矿发光过程影响的系统研究。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "应用光致发光光谱可以快速、灵敏地表征钙钛矿薄膜的激发态特征。对稳态发光光谱的高能边拟合，可以得到其等效载流子温度" }, { "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": "，对发光光谱的低能边分析可以获得材料的带尾态信息。本文利用变温光致发光光谱和时间分辨发光光谱分析了CsFAMA混合阳离子钙钛矿的发光特征。首先根据Saha-Langmuir方程，确认不同热力学温度条件下的发光机制——激子发光或电子空穴复合发光。通过带间发光与带尾态发光组合模型拟合CsFAMA混合阳离子钙钛矿的光致发光光谱，得到带尾态在禁带中的扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "、等效载流子温度信息。然后，分析了CsFAMA混合阳离子钙钛矿荧光寿命、电子空穴复合速率常数随温度的变化行为。本文研究结果有助于从热无序和带尾态的角度理解混合阳离子混合卤素离子钙钛矿材料的发光特征。" } ] } ] }, { "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　CsFAMA混合阳离子钙钛矿薄膜制备" } ], "level": "2", "id": "s2a" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.1.1　石英片清洗" } ], "level": "3", "id": "s2a1" } }, { "name": "p", "data": [ { "name": "text", "data": "石英片依次在去离子水、丙酮和异丙酮混合溶液中超声清洗20 min。使用气枪将石英片上残留的异丙酮吹干。使用氧气等离子体处理石英片表面15 min，去除有机污染物，同时增加表面亲水性。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.1.2　Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "0.05" } ] }, { "name": "text", "data": "FA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.81" } ] }, { "name": "text", "data": "MA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.14" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2.55" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "0.45" } ] }, { "name": "text", "data": "溶液制备" } ], "level": "3", "id": "s2a2" } }, { "name": "p", "data": [ { "name": "text", "data": "A：1.21 mmol FAI，1.27 mmol PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "，0.2 mL DMSO+0.8 mL DMF；B：1.42 mmol MABr，1.5 mmol PbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "，0.2 mL DMSO+0.8 mL DMF；C：0.3 mmol CsI，0.4 mL DMSO。其中FAI、PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "、CsI、MABr、PbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "来自西安宝莱特光电科技有限公司，纯度均为99.99%；DMSO来自默克有限公司，纯度为99.99%；DMF来自北京百灵威科技有限公司，纯度为99.98%。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "取0.44 mL的A、0.066 mL的B和0.044 mL的C放到磁力搅拌器上室温旋转12 h，得到CsFAMA混合阳离子钙钛矿前驱体溶液。再取0.022 mL之前所得到的前驱体溶液，利用二步旋涂法（在2 000 r/min转速下10 s，在6 000 r/min转速下30 s）制备钙钛矿薄膜。在旋涂结束前10 s使用0.121 mL苯甲醚缓慢冲洗薄膜表面。将旋涂的钙钛矿薄膜转移到热板上，在110 ℃温度下退火20 min，并冷却到室温。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.2　实验表征方法" } ], "level": "2", "id": "s2b" } }, { "name": "p", "data": [ { "name": "text", "data": "采用紫外-近红外光谱仪（U4100，日立公司）测定了CsFAMA混合阳离子钙钛矿薄膜的透射光谱。薄膜的俯视SEM图谱由场发射扫描电子显微镜（Nova Nano SEM450）测得。薄膜的衍射峰采用XRD衍射仪（D8-Advance，布鲁克公司）进行测量。使用闭循环液氦制冷低温恒温器改变薄膜温度。光致发光（Photoluminescence-PL）实验光源采用532 nm连续激光。CsFAMA混合阳离子钙钛矿发射的荧光通过光谱仪（SP2500）和CCD探测器进行采集。时间分辨荧光光谱测量的光源为532 nm脉冲激光（超连续激光器NKT-super-12），数据采集由单光子雪崩探测模块（SPAD-PDM）和单光子计数器（Picoharp300）实现。" } ] } ] } ] }, { "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　CsFAMA混合阳离子钙钛矿薄膜的表面结构和光学表征" } ], "level": "2", "id": "s3a" } }, { "name": "p", "data": [ { "name": "text", "data": "从CsFAMA混合钙钛矿薄膜的俯视SEM图谱（" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "（a））可以看出，薄膜晶粒均匀，表面排列紧凑，无明显裂缝，颗粒的粒径介于几十纳米到上百纳米之间。利用表面轮廓仪（Dektak-XT Bruker）测量CsFAMA混合阳离子钙钛矿薄膜厚度约为（624±30） nm。CsFAMA混合阳离子钙钛矿为立方相，" }, { "name": "italic", "data": [ { "name": "text", "data": "Pm" } ] }, { "name": "text", "data": "3" }, { "name": "italic", "data": [ { "name": "text", "data": "m" } ] }, { "name": "text", "data": "点群。" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "（b）为CsFAMA混合阳离子钙钛矿薄膜的XRD谱，其主要特征峰为13.97°、19.91°、24.46°、28.31°、31.77°、34.96°、40.51°和 43.16°，分别对应（100）、（110）、（111）、（200）、（210）、（211）、（220）和（300）晶面" }, { "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": "。CsFAMA混合阳离子钙钛矿为直接带隙半导体材料" }, { "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": "。本文利用Tauc plot法（（" }, { "name": "italic", "data": [ { "name": "text", "data": "αhν" } ] }, { "name": "text", "data": "）" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "italic", "data": [ { "name": "text", "data": "=B" } ] }, { "name": "text", "data": "（" }, { "name": "italic", "data": [ { "name": "text", "data": "hν-E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "），其中" }, { "name": "italic", "data": [ { "name": "text", "data": "α" } ] }, { "name": "text", "data": "为吸收系数," }, { "name": "italic", "data": [ { "name": "text", "data": "B" } ] }, { "name": "text", "data": "为常数）外插（" }, { "name": "italic", "data": [ { "name": "text", "data": "αhν" } ] }, { "name": "text", "data": "）" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "italic", "data": [ { "name": "text", "data": "=" } ] }, { "name": "text", "data": "0，得到CsFAMA混合阳离子钙钛矿的带隙约为1.621 eV（" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "（c））。" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "（d）为不同热力学温度条件下CsFAMA混合阳离子钙钛矿薄膜光致发光光谱。随着温度升高，薄膜PL出现明显展宽现象和峰位移动。在15~225 K范围内，CsFAMA混合阳离子钙钛矿薄膜的PL峰位发生蓝移。当热力学温度大于245 K之后，PL峰位则出现红移。该温度接近MAPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "由四方相向立方相的转变温度" }, { "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": "。（FAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "）" }, { "name": "sub", "data": [ { "name": "text", "data": "0.85" } ] }, { "name": "text", "data": "（MAPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "）" }, { "name": "sub", "data": [ { "name": "text", "data": "0.15" } ] }, { "name": "text", "data": "的元素配比与本文研究的混合阳离子钙钛矿接近。通过变温X射线分析，Lidzey等发现证实（FAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "）" }, { "name": "sub", "data": [ { "name": "text", "data": "0.85" } ] }, { "name": "text", "data": "（MAPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "）" }, { "name": "sub", "data": [ { "name": "text", "data": "0.15" } ] }, { "name": "text", "data": "薄膜升温至260 K附近后发生伪四方相向伪立方相的晶体结构变化，同时薄膜禁带宽度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "略有减小" }, { "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": "。基于本文的实验测量结果和相关文献报道，可以推测CsFAMA混合阳离子钙钛矿PL峰位红移的现象源于薄膜相变行为。同时，文献报道MAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "、MAPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "、FAPbI" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "在相变过程中发光峰位红移，随温度升高峰位则呈现蓝移" }, { "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": "。而本文CsFAMA混合阳离子钙钛矿在相变后PL峰位只存在红移，并未出现峰位蓝移现象，这可能与本文测量温度范围有限有关。本文暂以低温相和高温相分别代指CsFAMA混合阳离子钙钛矿在低于和高于245 K条件下的晶体结构。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "（a）CsFAMA混合阳离子钙钛矿薄膜的SEM图像；（b）CsFAMA混合阳离子钙钛矿薄膜XRD谱；（c）（" }, { "name": "italic", "data": [ { "name": "text", "data": "αhν" } ] }, { "name": "text", "data": "）" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "与光子能量" }, { "name": "italic", "data": [ { "name": "text", "data": "hν" } ] }, { "name": "text", "data": "的关系，" }, { "name": "italic", "data": [ { "name": "text", "data": "α" } ] }, { "name": "text", "data": "为吸收系数；（d）典型温度条件下的光致发光谱。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.1" } ], "title": [ { "name": "text", "data": "（a）SEM picture of CsFAMA mixed cation perovskite films. （b）XRD pattern of CsFAMA mixed cation perovskite films. （c）The dependence of （" }, { "name": "italic", "data": [ { "name": "text", "data": "αhν" } ] }, { "name": "text", "data": "）" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " on photon energy " }, { "name": "italic", "data": [ { "name": "text", "data": "hν" } ] }, { "name": "text", "data": "， where " }, { "name": "italic", "data": [ { "name": "text", "data": "α" } ] }, { "name": "text", "data": " is absorption coefficient. （d）Photoluminescence spectra at some typical temperatures." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818575&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818583&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818578&type=", "width": "134.04223633", "height": "91.94767761", "fontsize": "" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.2　CsFAMA混合阳离子钙钛矿的发光机制：电子空穴复合、激子发光" } ], "level": "2", "id": "s3b" } }, { "name": "p", "data": [ { "name": "text", "data": "CsFAMA混合阳离子钙钛矿的主要发光机制包括电子空穴复合发光和激子发光。CsFAMA混合阳离子钙钛矿激发态中自由载流子占比可以使用Saha-Langmuir方程" }, { "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": "29", "type": "bibr", "rid": "R29", "data": [ { "name": "text", "data": "29" } ] } } ], "rid": [ "R27", "R28", "R29" ], "text": "27-29", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "描述：" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（1）" } ], "data": [ { "name": "math", "data": { "math": "

\frac{x^{2}}{1 - x} = \frac{1}{N} {(\frac{2 π m k_{B} T}{h^{2}})}^{3 / 2} e^{- \frac{E_{B}}{k_{B} T}}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818589&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818586&type=", "width": "42.50266647", "height": "9.05933285", "fontsize": "" } } }, { "name": "text", "data": "，" } ], "id": "DF1" } }, { "name": "p", "data": [ { "name": "text", "data": "其中，" }, { "name": "italic", "data": [ { "name": "text", "data": "x" } ] }, { "name": "text", "data": "表示自由载流子浓度相对于总激发密度的比例，" }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "text", "data": "表示平衡条件下的激发态密度，" }, { "name": "italic", "data": [ { "name": "text", "data": "m≈" } ] }, { "name": "text", "data": "0.15" }, { "name": "italic", "data": [ { "name": "text", "data": "m" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] } ] }, { "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": "，" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] }, { "name": "text", "data": "表示激子结合能，" }, { "name": "italic", "data": [ { "name": "text", "data": "h" } ] }, { "name": "text", "data": "表示普朗克常量，" }, { "name": "italic", "data": [ { "name": "text", "data": "k" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] }, { "name": "text", "data": "表示玻尔兹曼常数，" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "表示晶格温度。自由载流子占比" }, { "name": "italic", "data": [ { "name": "text", "data": "x" } ] }, { "name": "text", "data": "与激子结合能" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] }, { "name": "text", "data": "、热力学温度" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "以及平衡条件下激发态密度" }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "text", "data": "有关。文献报道CsFAMA混合阳离子钙钛矿的激子结合能较小，在19~24 meV之间" }, { "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": "。本文将根据Saha-Langmuir方程，计算不同热力学温度、连续光激发条件下自由载流子的占比" }, { "name": "italic", "data": [ { "name": "text", "data": "x" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "首先计算连续光激发条件下激发态密度" }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "text", "data": "。利用紫外-可见分光光度计测量薄膜在532 nm处的吸光度" }, { "name": "italic", "data": [ { "name": "text", "data": "A" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "abs" } ] }, { "name": "text", "data": "为2.354（" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

A_{a b s} = l g \frac{I_{0}}{I_{t}}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818596&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818594&type=", "width": "16.08666801", "height": "7.95866632", "fontsize": "" } } } ] }, { "name": "text", "data": "，" }, { "name": "italic", "data": [ { "name": "text", "data": "I" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "为样品的入射光强，" }, { "name": "italic", "data": [ { "name": "text", "data": "I" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "t" } ] }, { "name": "text", "data": "为样品的出射光强）。结合朗伯比尔定律" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

I_{t} = I_{0} e^{- α d}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818600&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818598&type=", "width": "14.05466747", "height": "4.06400013", "fontsize": "" } } } ] }, { "name": "text", "data": "，可得" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

α = \frac{A_{a b s} l n 10}{d}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818604&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818602&type=", "width": "19.13466644", "height": "7.28133297", "fontsize": "" } } } ] }, { "name": "text", "data": "。532 nm激光在CsFAMA混合阳离子钙钛矿中的穿透深度" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

\frac{1}{α}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818608&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818606&type=", "width": "2.87866688", "height": "7.28133297", "fontsize": "" } } } ] }, { "name": "text", "data": "约为115.1 nm。激光穿透深度小于薄膜厚度" }, { "name": "italic", "data": [ { "name": "text", "data": "d" } ] }, { "name": "text", "data": "（624 nm），因此，激光在CsFAMA混合阳离子钙钛矿中的激发体积应为" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

V = \frac{s}{α} = 1.66 \times 10^{- 15} m^{3}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818614&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818610&type=", "width": "37.25333405", "height": "7.28133297", "fontsize": "" } } } ] }, { "name": "text", "data": "，其中" }, { "name": "italic", "data": [ { "name": "text", "data": "s" } ] }, { "name": "text", "data": "为激光光斑面积（" }, { "name": "italic", "data": [ { "name": "text", "data": "s" } ] }, { "name": "text", "data": "≈1.44" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

\times

\frac{d N}{d t} = \frac{L}{V} - \frac{N}{τ} = 0

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818625&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818622&type=", "width": "26.50066566", "height": "7.36600018", "fontsize": "" } } } ] }, { "name": "text", "data": "，激发态密度" }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "text", "data": "可以表示为：" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（2）" } ], "data": [ { "name": "math", "data": { "math": "

N = \frac{L τ}{V}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818632&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818629&type=", "width": "11.43000031", "height": "7.28133297", "fontsize": "" } } }, { "name": "text", "data": "，" } ], "id": "DF2" } }, { "name": "p", "data": [ { "name": "text", "data": "其中" }, { "name": "italic", "data": [ { "name": "text", "data": "L" } ] }, { "name": "text", "data": "表示每秒光激发产生的激发态数量（包括电子空穴对和激子）。" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

L = \frac{W}{h ν} (1 - R) (1 - \frac{1}{e})

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818637&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818635&type=", "width": "35.56000137", "height": "7.36600018", "fontsize": "" } } } ] }, { "name": "text", "data": "，其中" }, { "name": "italic", "data": [ { "name": "text", "data": "W" } ] }, { "name": "text", "data": "为激发光功率，" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "text", "data": "为薄膜表面反射率（" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "text", "data": "=18.34%），" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

h ν

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818645&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818641&type=", "width": "3.64066648", "height": "2.62466669", "fontsize": "" } } } ] }, { "name": "text", "data": "表示光子能量。" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "text", "data": "表示CsFAMA混合阳离子钙钛矿的荧光寿命（此处取荧光动力学曲线从最大值衰减到最大值的" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

\frac{1}{e}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818654&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818650&type=", "width": "2.62466669", "height": "7.36600018", "fontsize": "" } } } ] }, { "name": "text", "data": "处所需时间）。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本文荧光寿命采用时间域时间分辨荧光光谱技术（Time resolved photoluminescence，TRPL）测量。激光单脉冲激发密度约为1.32" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

\times

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818660&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818658&type=", "width": "1.77800000", "height": "2.62466669", "fontsize": "" } } } ] }, { "name": "text", "data": "10" }, { "name": "sup", "data": [ { "name": "text", "data": "16 " } ] }, { "name": "text", "data": "/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "，远小于10" }, { "name": "sup", "data": [ { "name": "text", "data": "18 " } ] }, { "name": "text", "data": "/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "。因此，本文所得到CsFAMA混合阳离子钙钛矿的荧光寿命不受俄歇过程的影响" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "30", "type": "bibr", "rid": "R30", "data": [ { "name": "text", "data": "30" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。CsFAMA混合阳离子钙钛矿在不同热力学温度条件下的荧光寿命如" }, { "name": "xref", "data": { "text": "表1", "type": "table", "rid": "T1", "data": [ { "name": "text", "data": "表1" } ] } }, { "name": "text", "data": "所示，对应的荧光动力学曲线见" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（a）。根据" }, { "name": "xref", "data": { "text": "公式（2）", "type": "disp-formula", "rid": "DF2", "data": [ { "name": "text", "data": "公式（2）" } ] } }, { "name": "text", "data": "，在0.04 mW、532 nm激光连续激发条件下，CsFAMA混合阳离子钙钛矿体相内总的激发密度" }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "text", "data": "的数值见" }, { "name": "xref", "data": { "text": "表1", "type": "table", "rid": "T1", "data": [ { "name": "text", "data": "表1" } ] } }, { "name": "text", "data": "。" } ] }, { "name": "table", "data": { "id": "T1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "表1" } ], "title": [ { "name": "text", "data": "不同热力学温度下的荧光寿命" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "text", "data": "、激子结合能" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] }, { "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": "、平衡条件下激发态密度" }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "text", "data": "的数值" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Tab.1" } ], "title": [ { "name": "text", "data": "Values of fluorescence lifetime " }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "text", "data": "， exciton binding energy " }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] }, { "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": "and excitation density " }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "text", "data": " under equilibrium state at different thermodynamic temperatures" } ] } ], "note": [], "table": [ { "head": [ [ { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "/K" } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "text", "data": "/ns" } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] }, { "name": "text", "data": "/meV" } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "text", "data": "/m" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] } ] } ] ], "body": [ [ { "align": "center", "data": [ { "name": "text", "data": "15" } ] }, { "align": "center", "data": [ { "name": "text", "data": "1.872" } ] }, { "align": "center", "data": [ { "name": "text", "data": "21" } ] }, { "align": "center", "data": [ { "name": "text", "data": "6.26E+19" } ] } ], [ { "align": "center", "data": [ { "name": "text", "data": "45" } ] }, { "align": "center", "data": [ { "name": "text", "data": "2.461" } ] }, { "align": "center", "data": [ { "name": "text", "data": "21" } ] }, { "align": "center", "data": [ { "name": "text", "data": "8.22E+19" } ] } ], [ { "align": "center", "data": [ { "name": "text", "data": "75" } ] }, { "align": "center", "data": [ { "name": "text", "data": "4.952" } ] }, { "align": "center", "data": [ { "name": "text", "data": "21" } ] }, { "align": "center", "data": [ { "name": "text", "data": "1.65E+20" } ] } ], [ { "align": "center", "data": [ { "name": "text", "data": "105" } ] }, { "align": "center", "data": [ { "name": "text", "data": "5.18" } ] }, { "align": "center", "data": [ { "name": "text", "data": "21" } ] }, { "align": "center", "data": [ { "name": "text", "data": "1.73E+20" } ] } ], [ { "align": "center", "data": [ { "name": "text", "data": "135" } ] }, { "align": "center", "data": [ { "name": "text", "data": "6.14" } ] }, { "align": "center", "data": [ { "name": "text", "data": "21" } ] }, { "align": "center", "data": [ { "name": "text", "data": "2.05E+20" } ] } ], [ { "align": "center", "data": [ { "name": "text", "data": "165" } ] }, { "align": "center", "data": [ { "name": "text", "data": "8.716" } ] }, { "align": 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], [ { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "text", "data": "295" } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "text", "data": "3.144" } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "text", "data": "24" } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "text", "data": "1.05E+20" } ] } ] ], "foot": [] } ], "graphics": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818670&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818666&type=", "width": "77.69583130", "height": "47.40968323", "fontsize": "" } } }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "（a）连续光激发条件下自由载流子在总激发态密度中的占比" }, { "name": "italic", "data": [ { "name": "text", "data": "x" } ] }, { "name": "text", "data": "值；（b）室温下CsFAMA混合阳离子钙钛矿薄膜发光光谱及拟合曲线；（c）连续光激发、不同热力学温度条件下载流子的等效温度（黑色方块）与晶格温度（红色圆点）；（d）不同温度条件下CsFAMA混合阳离子钙钛矿带尾态在禁带中的扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.2" } ], "title": [ { "name": "text", "data": "（a）Percentage " }, { "name": "italic", "data": [ { "name": "text", "data": "x" } ] }, { "name": "text", "data": " of free carriers in total excitation state density under continuous laser excitation．（b）Photoluminescence spectrum of CsFAMA perovskite films at room temperature and its fitting．（c）Carrier equivalent temperatures（black square） and lattice temperatures（red circle） at different temperatures．（d）The extension degree of band tail states in the forbidden band " }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": " at different temperatures．" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818675&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818684&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818677&type=", "width": "141.00982666", "height": "105.86656189", "fontsize": "" } ] } }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "（a）典型热力学温度下CsFAMA钙钛矿薄膜的发光动力学曲线；（b）不同热力学温度下的荧光寿命；（c）不同热力学温度下电子空穴复合常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "的相对变化；（d）光致发光强度对温度的依赖关系。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.3" } ], "title": [ { "name": "text", "data": "（a）Photoluminescence dynamic curves of CsFAMA perovskite films at some typical thermodynamic temperatures．（b）Fluorescence lifetime at different thermodynamic temperatures．（c）Change trend of electron and hole recombination rate constant " }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": " at different thermodynamic temperatures．（d）The dependence of photoluminescence intensity on temperature." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818691&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818703&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818695&type=", "width": "146.79913330", "height": "106.17820740", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "将" }, { "name": "xref", "data": { "text": "表1", "type": "table", "rid": "T1", "data": [ { "name": "text", "data": "表1" } ] } }, { "name": "text", "data": "中的热力学温度" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "、激子结合能" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] }, { "name": "text", "data": "、激发态密度" }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "text", "data": "代入" }, { "name": "xref", "data": { "text": "公式（1）", "type": "disp-formula", "rid": "DF1", "data": [ { "name": "text", "data": "公式（1）" } ] } }, { "name": "text", "data": "，可计算总激发态密度中自由载流子的比例" }, { "name": "italic", "data": [ { "name": "text", "data": "x" } ] }, { "name": "text", "data": "，结果如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "（a）所示。从图中可以看出，当热力学温度低于35 K时，自由载流子占总激发态密度的比例小于0.5。在15～85 K范围内自由载流子占比迅速上升，其中45 K时自由载流子的占比接近80%，65 K时自由载流子占比接近100%。本文认为热力学温度高于65 K条件下，CsFAMA混合阳离子钙钛矿薄膜的发光主要来自电子和空穴复合发光。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.3　CsFAMA混合阳离子钙钛矿的带尾态发光分析" } ], "level": "2", "id": "s3c" } }, { "name": "p", "data": [ { "name": "text", "data": "根据Saha-Langmuir方程分析，热力学温度高于65 K条件下CsFAMA混合阳离子钙钛矿薄膜的发光机制为电子空穴复合发光。与单阳离子或单卤素离子钙钛矿相比，CsFAMA混合阳离子钙钛矿存在更加明显的结构无序度、带尾态以及更长的载流子热化时间" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "18", "type": "bibr", "rid": "R18", "data": [ { "name": "text", "data": "18" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "19", "type": "bibr", "rid": "R19", "data": [ { "name": "text", "data": "19" } ] } } ], "rid": [ "R18", "R19" ], "text": "18-19", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。为了详细了解结构无序和带尾态对CsFAMA混合阳离子钙钛矿发光过程的影响，本文利用带间发光与带尾态发光组合模型拟合实验发光光谱。根据该模型，CsFAMA混合阳离子钙钛矿发光光谱包括带间发光和带尾态发光两部分。带间跃迁发光强度表示为：" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（3）" } ], "data": [ { "name": "math", "data": { "math": "

S_{b u l k} (ћ ω) = \"{\"\begin{array}{c} A \sqrt[]{ћ w - E_{g}} e x p (- \frac{ћ ω - E_{g}}{k_{B} T}), ћ ω \geq E_{g} \\ 0, 其他 \end{array}\"\"

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818711&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818707&type=", "width": "72.81333160", "height": "15.32466698", "fontsize": "" } } }, { "name": "text", "data": "，" } ], "id": "DF3" } }, { "name": "p", "data": [ { "name": "text", "data": "其中，" }, { "name": "italic", "data": [ { "name": "text", "data": "S" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "bulk" } ] }, { "name": "text", "data": "为发光强度，" }, { "name": "italic", "data": [ { "name": "text", "data": "ћ" } ] }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

ω

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818717&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818714&type=", "width": "2.45533323", "height": "2.62466669", "fontsize": "" } } } ] }, { "name": "text", "data": "为光子能量，" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "g" } ] }, { "name": "text", "data": "为禁带宽度，" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "为自由载流子等效温度，" }, { "name": "italic", "data": [ { "name": "text", "data": "k" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "B" } ] }, { "name": "text", "data": "为玻尔兹曼常数，" }, { "name": "italic", "data": [ { "name": "text", "data": "A" } ] }, { "name": "text", "data": "为比例系数。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "带尾态密度可以表示为：" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（4）" } ], "data": [ { "name": "math", "data": { "math": "

D (E) = \frac{N_{0}}{E_{0}} e x p (- \frac{E_{g} - E}{E_{0}}),

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818724&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818721&type=", "width": "41.57133484", "height": "9.05933285", "fontsize": "" } } }, { "name": "text", "data": " " } ], "id": "DF4" } }, { "name": "p", "data": [ { "name": "text", "data": "其中，" }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "是禁带中局域能态的总数目，" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "代表这些局域能态在禁带中的扩展程度，" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "text", "data": "代表迁移率边的能量。带尾态的荧光强度为：" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（5）" } ], "data": [ { "name": "math", "data": { "math": "

S_{l o c a l} (ћ ω) = \"{\"\begin{array}{c} \frac{N_{e}}{E_{0}} e x p (\frac{ћ ω - E_{g}^{'}}{E_{0}}), ћ ω \leq E_{g}^{'} \\ 0, 其他 \end{array}\"\"

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818731&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818728&type=", "width": "60.79066849", "height": "15.32466698", "fontsize": "" } } }, { "name": "text", "data": "，" } ], "id": "DF5" } }, { "name": "p", "data": [ { "name": "text", "data": "其中，" }, { "name": "italic", "data": [ { "name": "text", "data": "S" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "local" } ] }, { "name": "text", "data": "为荧光强度，" }, { "name": "italic", "data": [ { "name": "text", "data": "N" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "是正比于局域能态密度的参量，而" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

E_{g}^{'}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818739&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818735&type=", "width": "3.38666677", "height": "4.06400013", "fontsize": "" } } } ] }, { "name": "text", "data": "是迁移率边，且近似条件下" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

E_{g}^{'} = E_{g}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818744&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818742&type=", "width": "11.17599964", "height": "4.06400013", "fontsize": "" } } } ] }, { "name": "text", "data": "。总的光谱荧光强度是以上两项相加，即" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（6）" } ], "data": [ { "name": "math", "data": { "math": "

S (ћ ω) = S_{b u l k} (ћ ω) + S_{l o c a l} (ћ ω) .

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818752&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818748&type=", "width": "46.31266785", "height": "4.57200003", "fontsize": "" } } }, { "name": "text", "data": " " } ], "id": "DF6" } }, { "name": "p", "data": [ { "name": "text", "data": "带间发光与带尾态发光组合模型可以很好地拟合CsFAMA混合阳离子钙钛矿薄膜的发光光谱（" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "（b））。本文通过发光光谱拟合获得了CsFAMA混合阳离子钙钛矿薄膜的等效载流子温度" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "以及带尾态的扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "。为了排除激子发光的干扰，本文选定65~295 K范围的光谱进行拟合。65 K条件下薄膜带尾态扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "约0.023 eV，在295 K条件下，" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "接近0.045 eV（" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "（d））。带尾态扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "随着热力学温度升高而不断增加。这表明高温条件下的晶格振动引发了更大的结构无序度，并导致带尾态的扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "增加。半导体带尾态扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "对温度的依赖关系可用下列公式描述" }, { "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": "：" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（7）" } ], "data": [ { "name": "math", "data": { "math": "

E_{0} (T) = E_{0} (0) + \frac{2 E_{0} (0)}{e x p (θ_{E} / T) - 1}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818762&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818756&type=", "width": "48.17533112", "height": "8.55133343", "fontsize": "" } } }, { "name": "text", "data": "，" } ], "id": "DF7" } }, { "name": "p", "data": [ { "name": "text", "data": "其中第一项" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "（0）为CsFAMA混合阳离子钙钛矿薄膜的静态无序度；而" }, { "name": "xref", "data": { "text": "公式（7）", "type": "disp-formula", "rid": "DF7", "data": [ { "name": "text", "data": "公式（7）" } ] } }, { "name": "text", "data": "中的第二项为动态分量，描述了声子对" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "数值的贡献，即声子密度的增加引起CsFAMA混合阳离子钙钛矿薄膜动态无序，导致材料的带尾态展宽。" }, { "name": "italic", "data": [ { "name": "text", "data": "T" } ] }, { "name": "text", "data": "为样品对应的晶格温度，" }, { "name": "italic", "data": [ { "name": "text", "data": "θ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "E" } ] }, { "name": "text", "data": "是爱因斯坦声子温度（声子态密度半填充时对应的温度）。利用" }, { "name": "xref", "data": { "text": "公式（7）", "type": "disp-formula", "rid": "DF7", "data": [ { "name": "text", "data": "公式（7）" } ] } }, { "name": "text", "data": "对带尾态的扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "进行拟合，如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "（d）所示。拟合曲线和实验曲线大体吻合，得到" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "（0）为0.023 eV，" }, { "name": "italic", "data": [ { "name": "text", "data": "θ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "E" } ] }, { "name": "text", "data": "为（367.08±5.17） K。另外当热力学温度超过200 K时，" }, { "name": "xref", "data": { "text": "公式（7）", "type": "disp-formula", "rid": "DF7", "data": [ { "name": "text", "data": "公式（7）" } ] } }, { "name": "text", "data": "拟合曲线和光谱拟合提取" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "的吻合程度变差。热力学温度高于245 K后" }, { "name": "xref", "data": { "text": "公式（7）", "type": "disp-formula", "rid": "DF7", "data": [ { "name": "text", "data": "公式（7）" } ] } }, { "name": "text", "data": "给出的" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "增幅小于实际增加幅度。变温PL光谱分析（" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "（d））已经证明CsFAMA混合阳离子钙钛矿在245 K附近存在低温相与高温相的转变。这种相变行为同样会影响带尾态的扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "随温度的变化规律，使得热力学温度高于200 K后" }, { "name": "xref", "data": { "text": "公式（7）", "type": "disp-formula", "rid": "DF7", "data": [ { "name": "text", "data": "公式（7）" } ] } }, { "name": "text", "data": "的拟合结果偏离光谱拟合所提取的" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "连续光激发条件下CsFAMA混合阳离子钙钛矿载流子等效温度以及晶格温度都会趋于稳定状态。变温实验中读取的薄膜温度与晶格温度近似相等（" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "（c）红色圆点）。根据CsFAMA混合阳离子钙钛矿带间发光拟合，本文可以得到不同热力学温度条件下载流子的等效温度，如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "（c）（黑色方块）所示。载流子与晶格的能量交换主要通过声子作用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } } ], "rid": [ "R32", "R33" ], "text": "32-33", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。晶格温度低于200 K时，薄膜体相内低声子密度限制了载流子与晶格的热交换速率，引起两者之间较大的差值，约30～90 K。晶格温度高于200 K时，薄膜体相内声子密度较高，可以实现载流子与晶格之间的充分热交换，因此载流子等效温度与晶格温度差值减小至20～30 K。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.4　CsFAMA混合阳离子钙钛矿载流子复合动力学分析" } ], "level": "2", "id": "s3d" } }, { "name": "p", "data": [ { "name": "text", "data": "在对CsFAMA混合阳离子钙钛矿中带尾态定量描述的基础上，本文进一步根据变温TRPL分析结构无序对载流子复合发光过程的影响。" } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（8）" } ], "data": [ { "name": "math", "data": { "math": "

\frac{d n}{d t} = - k_{1} n - R_{e h} n^{2}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818777&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818768&type=", "width": "28.10933495", "height": "7.36600018", "fontsize": "" } } }, { "name": "text", "data": "，" } ], "id": "DF8" } }, { "name": "p", "data": [ { "name": "text", "data": "其中" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "text", "data": "为自由载流子浓度；" }, { "name": "italic", "data": [ { "name": "text", "data": "k" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "为载流子的单分子复合速率常数，与载流子的非辐射复合过程有关；" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "表示电子空穴复合速率常数。CsFAMA混合阳离子钙钛矿的荧光寿命正比于" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

\frac{1}{k_{1} + R_{e h} n}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818785&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818780&type=", "width": "14.56266594", "height": "8.04333401", "fontsize": "" } } } ] }, { "name": "text", "data": "。随着热力学温度升高，钙钛矿材料的单分子复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "k" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "单调增加" }, { "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": "。本文推测电子空穴复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "减小是薄膜荧光寿命增加的主要原因。在时间分辨荧光光谱测量实验中，发光动力学曲线的峰值" }, { "name": "italic", "data": [ { "name": "text", "data": "PL" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "可以近似表示为" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "35", "type": "bibr", "rid": "R35", "data": [ { "name": "text", "data": "35" } ] } }, { "name": "text", "data": "]" } ] } ] }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "（9）" } ], "data": [ { "name": "math", "data": { "math": "

P L_{0} \approx R_{e h} n_{e} n_{h} = R_{e h} n_{0}^{2}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818790&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818786&type=", "width": "32.76599884", "height": "4.06400013", "fontsize": "" } } }, { "name": "text", "data": "，" } ], "id": "DF9" } }, { "name": "p", "data": [ { "name": "text", "data": "其中" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "为光激发瞬间的载流子密度，近似取光激发密度1.32×10" }, { "name": "sup", "data": [ { "name": "text", "data": "16 " } ] }, { "name": "text", "data": "/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "。" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "和" }, { "name": "italic", "data": [ { "name": "text", "data": "n" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "h" } ] }, { "name": "text", "data": "分别代表光激发瞬间的电子和空穴密度。根据发光动力学曲线的峰值变化，获得电子空穴复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "随温度变化行为，如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（c）所示。在65～165 K热力学温度范围内，电子空穴复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "逐渐减小。这表明电子空穴复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "的减小引发了65～165 K热力学温度范围内荧光寿命的增加。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本文进一步拟合了电子空穴复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "对温度的依赖关系（" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（c），温度小于100 K时的数据波动较大，为避免拟合误差，数据拟合从105 K开始）。CsFAMA混合阳离子钙钛矿的电子空穴复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "满足" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "∝" }, { "name": "italic", "data": [ { "name": "text", "data": "T " }, { "name": "sup", "data": [ { "name": "text", "data": "-" } ] } ] }, { "name": "sup", "data": [ { "name": "text", "data": "2.25" } ] }, { "name": "text", "data": "。对于直接带隙半导体，载流子迁移率满足" }, { "name": "italic", "data": [ { "name": "text", "data": "T " } ] }, { "name": "sup", "data": [ { "name": "text", "data": "-3/2" } ] }, { "name": "text", "data": "条件下，电子空穴复合系数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "满足" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "∝" }, { "name": "italic", "data": [ { "name": "text", "data": "T " }, { "name": "sup", "data": [ { "name": "text", "data": "-" } ] } ] }, { "name": "sup", "data": [ { "name": "text", "data": "3/2[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "36", "type": "bibr", "rid": "R36", "data": [ { "name": "text", "data": "36" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } } ], "rid": [ "R36", "R37" ], "text": "36-37", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Howard等报道Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "0.1" } ] }, { "name": "text", "data": "（MA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.17" } ] }, { "name": "text", "data": "FA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.83" } ] }, { "name": "text", "data": "）" }, { "name": "sub", "data": [ { "name": "text", "data": "0.9" } ] }, { "name": "text", "data": "Pb（I" }, { "name": "sub", "data": [ { "name": "text", "data": "0.84" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "0.16" } ] }, { "name": "text", "data": "）" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "的电子空穴复合速率常数满足" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "∝" }, { "name": "italic", "data": [ { "name": "text", "data": "T " } ] }, { "name": "sup", "data": [ { "name": "text", "data": "-3/2[" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。但Howard的拟合曲线只利用了4个温度条件的数据点，可能存在较大误差。本文认为温度升高引起载流子迁移率下降（" }, { "name": "italic", "data": [ { "name": "text", "data": "T " }, { "name": "sup", "data": [ { "name": "text", "data": "-" } ] } ] }, { "name": "sup", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "）仍然是CsFAMA混合阳离子钙钛矿电子空穴复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "减小的主要原因。同时本文所得幂因子为-2.25，略小于-3/2。这表明仍存在其他物理机制使得高温条件下" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "减小。这些物理机制包括载流子声子耦合形成极化子" }, { "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": "、Rashba效应" }, { "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": "、热无序引起的载流子局域化" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "41", "type": "bibr", "rid": "R41", "data": [ { "name": "text", "data": "41" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。CsFAMA混合阳离子钙钛矿存在更加明显的结构无序。随着热力学温度升高引起的热无序必然对电子空穴复合过程产生影响。本文谨慎推测热无序引起的载流子局域化是电子空穴复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "减小的另一主要原因。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "由" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "（b）还可以看出，热力学温度高于245 K后，CsFAMA混合阳离子钙钛矿的荧光寿命快速下降。在245~295 K范围内，电子空穴复合速率常数趋于稳定。因此，薄膜荧光寿命（正比于" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "

\frac{1}{k_{1} + R_{e h} n}

", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818797&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=39818795&type=", "width": "14.56266594", "height": "8.04333401", "fontsize": "" } } } ] }, { "name": "text", "data": "）的减小应主要来自单分子复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "k" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "的增加。根据前文分析，热力学温度高于245 K后带尾态在禁带中的扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "也存在明显的增加（" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "（d））。我们认为载流子单分子复合速率" }, { "name": "italic", "data": [ { "name": "text", "data": "k" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "的增加与材料的热无序度直接相关，即带尾态扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "加速了缺陷态辅助的载流子非辐射复合过程。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "4　结　　论" } ], "level": "1", "id": "s4" } }, { "name": "p", "data": [ { "name": "text", "data": "本文利用PL光谱技术、TRPL光谱技术对Cs" }, { "name": "sub", "data": [ { "name": "text", "data": "0.05" } ] }, { "name": "text", "data": "FA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.81" } ] }, { "name": "text", "data": "MA" }, { "name": "sub", "data": [ { "name": "text", "data": "0.14" } ] }, { "name": "text", "data": "PbI" }, { "name": "sub", "data": [ { "name": "text", "data": "2.55" } ] }, { "name": "text", "data": "Br" }, { "name": "sub", "data": [ { "name": "text", "data": "0.45" } ] }, { "name": "text", "data": "钙钛矿薄膜的发光过程进行了分析。首先通过Saha-Langmuir方程计算不同热力学温度条件下激发态中自由载流子的占比，证实温度高于65 K时CsFAMA混合阳离子钙钛矿的发光机制为电子空穴复合发光。本文进一步利用带间复合与带尾态组合模型对CsFAMA混合阳离子钙钛矿的发光光谱进行拟合，获得了等效载流子温度与带尾态扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "。光谱分析结果表明，随着热力学温度升高（65~295 K），CsFAMA混合阳离子钙钛矿的带尾态扩展程度" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "由0.023 eV升高至0.045 eV。CsFAMA混合阳离子钙钛矿的发光动力学分析表明，电子空穴复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "随温度升高而减小，同时晶格振动引发的热无序度增加也加速了载流子的非辐射复合。本文认为载流子迁移率降低、热无序诱导的载流子局域化是引起电子空穴复合速率常数" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "eh" } ] }, { "name": "text", "data": "减小的主要原因。同时，本文还发现CsFAMA混合阳离子钙钛矿在245 K附近发生低温相到高温相之间的转变。在高温相内薄膜的热无序度更加明显，扩大了带尾态的扩展程度，同时也加速了载流子的非辐射复合过程。本文的研究结果有助于更加全面理解混合阳离子混合卤素离子钙钛矿的发光过程。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本文专家审稿意见及作者回复内容的下载地址：" }, { "name": "extlink", "data": { "text": [ { "name": "text", "data": "http://cjl.lightpublishing.cn/thesisDetails#10.37188/" } ], "href": "http://cjl.lightpublishing.cn/thesisDetails#10.37188/" } } ] }, { "name": "p", "data": [ { "name": "text", "data": "CJL.20220268." } ] } ] } ], "footnote": [], "reflist": { "title": [ { "name": "text", "data": "参考文献" } ], "data": [ { "id": "R1", "label": "1", "citation": [ { "lang": "en", "text": [ { "name": "text", "data": "ZUO C T" }, { "name": "text", "data": "， " }, { "name": "text", "data": "BOLINK H J" }, { "name": "text", "data": "， " }, { "name": "text", "data": "HAN H W" }, { "name": "text", "data": "， " }, { "name": "text", "data": "et al" }, { "name": "text", "data": ". 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