Multiexcitons Recombination Dynamics Based on Large-scale Quantum Well Structure Enhanced Publication

{ "defaultlang": "zh", "titlegroup": { "articletitle": [ { "lang": "zh", "data": [ { "name": "text", "data": "基于大尺寸量子阱结构的多激子复合动力学" } ] }, { "lang": "en", "data": [ { "name": "text", "data": "Multiexcitons Recombination Dynamics Based on Large-scale Quantum Well Structure" } ] } ] }, "contribgroup": { "author": [ { "name": [ { "lang": "zh", "surname": "孟", "givenname": "竹", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "MENG", "givenname": "Zhu", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [ "corresp", "first-author" ], "corresp": [ { "rid": "cor1", "lang": "en", "text": "E-mail： 1183050408@qq.com", "data": [ { "name": "text", "data": "E-mail： 1183050408@qq.com" } ] } ], "bio": [ { "lang": "zh", "text": [ "孟竹（1991－），女，吉林四平人，博士，讲师，2021年于里昂第一大学获得博士学位。主要从事半导体纳米晶的制备以及其光学和闪烁性能的研究。 E-mail： 1183050408@qq.com" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733467&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733469&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733468&type=", "width": "17.83742714", "height": "25.40040588", "fontsize": "" } ], "data": [ [ { "name": "text", "data": "孟竹" }, { "name": "text", "data": "（1991－），女，吉林四平人，博士，讲师，2021年于里昂第一大学获得博士学位。主要从事半导体纳米晶的制备以及其光学和闪烁性能的研究。 E-mail： " }, { "name": "text", "data": "1183050408@qq.com" } ] ] } ], "email": "1183050408@qq.com", "deceased": false }, { "name": [ { "lang": "zh", "surname": "徐", "givenname": "豪", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "XU", "givenname": "Hao", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff2", "text": "2" } ], "role": [], "deceased": false } ], "aff": [ { "id": "aff1", "intro": [ { "lang": "zh", "label": "1", "text": "沈阳理工大学 理学院，辽宁 沈阳　110158", "data": [ { "name": "text", "data": "沈阳理工大学 理学院，辽宁 沈阳　110158" } ] }, { "lang": "en", "label": "1", "text": "School of Science， Shenyang Ligong University， Shenyang 110158， China", "data": [ { "name": "text", "data": "School of Science， Shenyang Ligong University， Shenyang 110158， China" } ] } ] }, { "id": "aff2", "intro": [ { "lang": "zh", "label": "2", "text": "沈阳大学 科技创新研究院，辽宁 沈阳　110003", "data": [ { "name": "text", "data": "沈阳大学 科技创新研究院，辽宁 沈阳　110003" } ] }, { "lang": "en", "label": "2", "text": "Institute of Innovation Science and Technology， Shenyang University， Shenyang 110003， China", "data": [ { "name": "text", "data": "Institute of Innovation Science and Technology， Shenyang University， Shenyang 110003， China" } ] } ] } ] }, "abstracts": [ { "lang": "zh", "data": [ { "name": "p", "data": [ { "name": "text", "data": "半导体纳米晶的多激子复合过程在激光器件、发光二极管和光伏等方面具有巨大的应用价值。但粒子体积的减小会加速多激子态的非辐射俄歇复合，这极大地阻碍了相关应用的发展。因此抑制俄歇复合成为纳米晶体领域一个重要的研究主题。在这里，我们基于球形量子阱结构CdS/CdSe/CdS，通过共格应变减小由材料间晶格失配引起的缺陷，制备出高荧光量子产率的大尺寸纳米晶。应用时间分辨荧光光谱技术，本文在光谱学以及动力学领域研究了大尺寸量子阱的多激子复合特性，分析了单激子及多激子的衰减寿命和谱线特征，并证实了大尺寸量子阱对俄歇复合的抑制作用。本研究有望促进纳米结构在多激子应用中的发展。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "Colloidal semiconductor nanocrystals present unique electronic and optical properties. The multiexcitons recombination process of semiconductor nanocrystals has attracted extensive attention motivated by the needs of prospective applications in lasing devices， light-emitting diodes， and photovoltaic cells. However， the reduction of particle size will accelerate the non-radiative Auger recombination of multiexcitons states， which significantly hinders the development of related applications. Therefore， suppressing Auger recombination has become an important research topic in the nanocrystal field. Increasing the volume of nanocrystals is considered to be an effective means to decrease Auger recombination. Here， we have synthesized a spherical quantum well structure CdS/CdSe/CdS by hot injection method. As a result of coherent strain， this sandwich like structure can diminish the strain on the interface which is caused by the material lattice mismatch， thus reducing dislocation defects and fabricating large-scale nanocrystals with quantum yield over 80%. By using time-resolved fluorescence spectroscopy， the multiexcitons recombination characteristics of large-scale quantum well are investigated in the fields of spectroscopy and dynamics. The decay lifetimes and spectral characteristics of single exciton， biexcitons and high-order multiexcitons are analyzed， and the suppression effect on Auger non-radiative recombination of large-scale quantum well is confirmed. The study of multiexcitons recombination and Auger process in large-scale quantum well is expected to promote the development of nanostructures in multiexcitons applications." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "大尺寸量子阱" } ], [ { "name": "text", "data": "多激子" } ], [ { "name": "text", "data": "时间分辨荧光光谱技术" } ], [ { "name": "text", "data": "非辐射复合" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "large-scale quantum well" } ], [ { "name": "text", "data": "multiexcitons" } ], [ { "name": "text", "data": "time-resolved fluorescence spectroscopy" } ], [ { "name": "text", "data": "non-radiative recombination" } ] ] } ], "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": "半导体纳米材料由于其独特的光学和电学性质一直是科学研究的热点" }, { "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": "。迄今为止，半导体纳米晶体已在发光二极管" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "4", "type": "bibr", "rid": "R4", "data": [ { "name": "text", "data": "4" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、激光增益介质" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "5", "type": "bibr", "rid": "R5", "data": [ { "name": "text", "data": "5" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "和太阳能电池" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "6", "type": "bibr", "rid": "R6", "data": [ { "name": "text", "data": "6" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "7", "type": "bibr", "rid": "R7", "data": [ { "name": "text", "data": "7" } ] } } ], "rid": [ "R6", "R7" ], "text": "6-7", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "等领域中显示出优异的应用前景。在过去的20年里，随着纳米晶体合成技术不断改进，使得制备各种尺寸、成分和形状的纳米晶体变成可能，这为改善纳米晶的性能和发展新型纳米材料提供了有效的途径。然而，纳米尺度上电子和空穴之间库仑相互作用的增强显著加快了非辐射俄歇复合速率，这已经成为纳米晶体在多载流子相关应用中的重要障碍" }, { "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": "9", "type": "bibr", "rid": "R9", "data": [ { "name": "text", "data": "9" } ] } } ], "rid": [ "R8", "R9" ], "text": "8-9", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，如何抑制非辐射俄歇复合效应成为了一个亟待解决的问题。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "研究表明，俄歇复合速率取决于波函数的约束程度、电子和空穴的空间分离程度以及界面能带梯度等因素的协同作用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。根据普遍接受的“体积比例缩放”理论，俄歇速率随纳米粒子体积的增长而减小" }, { "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": "。因此，抑制俄歇效应的一般结构为巨型核/壳量子点" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "12", "type": "bibr", "rid": "R12", "data": [ { "name": "text", "data": "12" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } } ], "rid": [ "R12", "R13" ], "text": "12-13", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "、合金结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "14", "type": "bibr", "rid": "R14", "data": [ { "name": "text", "data": "14" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "15", "type": "bibr", "rid": "R15", "data": [ { "name": "text", "data": "15" } ] } } ], "rid": [ "R14", "R15" ], "text": "14-15", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "或纳米棒" }, { "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": "。厚壳层量子点不仅可以减缓俄歇复合速率，在提高材料吸收截面方面也有着重要的作用。然而厚壳层量子点自身存在一定的结构局限性，不同材料间的固有晶格失配阻碍了该结构抑制俄歇复合的能力。当壳层达到一定厚度时，由于界面失配缺陷的形成会导致荧光量子效率(QY)严重降低。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本文中，我们利用球形量子阱结构CdS/CdSe/CdS" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "17", "type": "bibr", "rid": "R17", "data": [ { "name": "text", "data": "17" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "18", "type": "bibr", "rid": "R18", "data": [ { "name": "text", "data": "18" } ] } } ], "rid": [ "R17", "R18" ], "text": "17-18", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，通过外延生长出夹在两个CdS层之间的发射层CdSe。在发射层设计较薄的情况下，共格应变可克服壳层厚度的限制。由于壳层生长过程中结构应力的缓解，形成的晶格失配缺陷较少。这使得球形量子阱不同于传统核壳结构，随着壳层厚度的增加，球形量子阱依旧存在较高的荧光量子产率和较低的非辐射复合速率" }, { "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": "。基于此，本文制备了一种大尺寸高荧光量子产率的球形量子阱。通过在动力学和光谱学上分析不同激发条件下的时间分辨特性，研究了大尺寸量子阱的俄歇效应以及多激子复合过程。通过探索光谱和功率的依赖关系，并根据不同激发态独特的光谱和时间特性，实现了激发态的识别。我们观察到了强光泵浦下单激子，双激子以及高阶多激子的发射特征，并通过计算得到双激子的荧光量子效率及俄歇复合寿命。证实了大尺寸量子阱在抑制俄歇非辐射过程方面的优异表现。" } ] } ] }, { "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　实验药品与试剂" } ], "level": "2", "id": "s2a" } }, { "name": "p", "data": [ { "name": "text", "data": "1-十二硫醇(DDT, 99%)、硝酸镉(>99%)、三辛基膦(TOP, 97%)、十八烯(ODE, 90%)、氧化镉(CdO, 99.99%)、硒(99.99%)、硫(99.99%)、甲醇(98.5%)、甲苯( 99.9%)、油酸(OA, 90%)、油酸胺(OAm, 80-90%)、肉豆蔻酸钠(>98%)。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.2　前驱体制备" } ], "level": "2", "id": "s2b" } }, { "name": "p", "data": [ { "name": "text", "data": "Cd(myr)" }, { "name": "sub", "data": [ { "name": "text", "data": " 2" } ] }, { "name": "text", "data": "：9.3 g肉豆蔻酸钠溶解于750 mL甲醇中，搅拌至完全溶解。将溶解于120 mL甲醇的3.7 g硝酸镉混合到上述溶液中，缓慢搅拌以获得白色沉淀。用布氏漏斗过滤沉淀物，用甲醇冲洗数次，并在真空下干燥。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "0.25M S-ODE：70°C下20 mL ODE脱气30 min，在氩气下加入160 mg硫粉末。加热至140°C，直到硫粉末溶解，并保持在80°C备用。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "0.5M Cd(OA)" }, { "name": "sub", "data": [ { "name": "text", "data": " 2" } ] }, { "name": "text", "data": "：180°C下6.42 g CdO溶解于50 mL OA和50 mL ODE中。当混合物呈透明黄色时，温度降至120°C，对烧瓶进行脱气至P" }, { "name": "text", "data": "<" }, { "name": "text", "data": "0.3 mbar。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "2M TOPSe：1.58 g硒粉末加到10 mL TOP中,100°C持续4 h，直至完全溶解，反应在手套箱中进行。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.3　样品制备" } ], "level": "2", "id": "s2c" } }, { "name": "p", "data": [ { "name": "text", "data": "CdS内核的合成：1.5 mL 0.5M Cd(OA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "和27 mL ODE加入烧瓶，在氩气下加热至270°C后，注入1.5 mL 0.25M S-ODE。立即将温度降至250°C反应15 min。冷却至室温, 使用乙醇离心纯化后分散于正己烷中。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "CdSe层的合成：520 nmol CdS内核和5 mL ODE在65°C下脱气1 h。 0.1 M前体混合物(0.6 mL TOPSe、2.4 mL Cd(OA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "和9 mL ODE)在300°C下以6 mL/h的速度注入11 mL。冷却至室温, 使用乙醇离心纯化后分散于正己烷中。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "CdS壳层的合成：将156 nmol CdSe层、85 mg Cd(myr)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "和10 mL ODE在65°C下脱气30 min，然后加热至305°C，0.2 M前驱体溶液(1.58 mL DDT在31.42 mL ODE中稀释，13.2 mL Cd(OA)" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "溶解在15.8 mL ODE和4 mL OAm)以0.8 nm/h注入。退火30 min后冷却至室温,使用乙醇离心纯化后分散于正己烷中。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "2.4　实验设备" } ], "level": "2", "id": "s2d" } }, { "name": "p", "data": [ { "name": "text", "data": "形貌表征由透射电子显微镜(JEOL-JEM 2010)实现。吸收光谱通过AvaSpec-2048L光纤光谱仪测量，发射光谱由荧光分光光度计(FS5, Edinburgh Instruments)获得。时间分辨测量：450 nm, 500 kHz脉冲激光器(Edinburgh Instruments EPL-450)和PicoHarp300时间相关单光子计数获取衰减动力学曲线。405 nm, 500 kHz皮秒半导体激光器(Horiba DD-405L)和MCS6A多通道计数器用来测量并得到时间分辨光谱。所有测试均在室温下完成。" } ] } ] } ] }, { "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　样品的结构及表征" } ], "level": "2", "id": "s3a" } }, { "name": "p", "data": [ { "name": "text", "data": "本文采用了快速连续注入前驱体的合成方法" }, { "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": "。通过热注入合成半径为1.3 nm的CdS内核，然后滴入Cd和Se前驱体得到1.8 nm CdSe发射层，随后添加壳前驱体以形成大尺寸的纳米粒子。纳米晶的结构示意图如" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(a)所示，能带排列模式为准II型，类似于CdSe/CdS核/壳量子点，其中空穴完全限制在CdSe区域，电子在整个粒子上离域。样品的直径由透射电子显微镜(TEM)图像表征，平均尺寸约为24 nm，标准偏差为11%。颗粒呈现出多面和不规则的形状，这通常在大尺寸量子点中观察到(" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(b))" }, { "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": "21", "type": "bibr", "rid": "R21", "data": [ { "name": "text", "data": "21" } ] } } ], "rid": [ "R20", "R21" ], "text": "20-21", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。从不同尺寸CdS/CdSe/CdS的吸收光谱(" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(c))可以看出随着CdS壳层的生长，样品在紫外波段具有相当大的吸收截面，可以与钙钛矿量子点相媲美。同时CdS层作为光学天线，承担了吸收光子的责任，使得吸收光谱与发射光谱的重叠度随着外壳层的生长而逐渐减小，这将有助于减小样品由自吸收带来的损失。吸收光谱的二阶微分呈现出三个明显的跃迁特征，分别为634 nm处的1S" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1S" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "带边跃迁，575 nm处的1S" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-2S" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "跃迁,以及529 nm处涉及1P电子和空穴态的跃迁（1P" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1P" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "跃迁）。所制备量子阱的发射波长约为650 nm，半高宽约为30 nm，表明颗粒尺寸具有均一性。以oxazine 170为参比样品，通过相对方法测得溶液样品的荧光量子产率超过80%。样品中可能存在少量纯核CdS量子点，这对量子阱发光峰的性质不产生影响。通过绝对方法测试得到滴注形成的薄膜样品荧光量子产率约为50%，高于绝大多数目前所报道的实验值" }, { "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": "。这得益于壳层的包覆减小了外部环境对发射层的影响，同时厚壳层减小了颗粒之间的能量交换。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "大尺寸量子阱的表征。（a）量子阱的示意图及能带对齐方式 （b） 量子阱的透射电子显微镜图像 （c） 不同尺寸量子阱的吸收光谱以及24nm样品的发射光谱和吸收光谱的二阶微分。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 1" } ], "title": [ { "name": "text", "data": "Characterization of large-scale quantum well. （a） Schematic diagram and band alignment. （b） TEM image of large-scale quantum well. （c） The absorption spectra of quantum well with different sizes， PL spectrum and the second derivative of absorption spectrum of sample with a diameter of 24 nm." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733470&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733472&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733471&type=", "width": "162.79998779", "height": "40.70452881", "fontsize": "" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.2　不同激光功率下的动力学曲线" } ], "level": "2", "id": "s3b" } }, { "name": "p", "data": [ { "name": "text", "data": "将溶液滴注在硅片上，经自然干燥形成薄膜样品，以450 nm脉冲激光器为激发源进行研究，仪器的响应函数为400 ps。由于多激子态可以通过在高泵浦功率下快速连续吸收多个光子产生，因此识别激发态的最常用方法是分析它们的功率相关特性。首先根据理论方程: " }, { "name": "text", "data": "<" }, { "name": "text", "data": "N" }, { "name": "text", "data": ">" }, { "name": "text", "data": " = " }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733474&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733473&type=", "width": "8.38199997", "height": "8.12800026", "fontsize": "" } } } ] }, { "name": "text", "data": "，计算得到每个纳米晶的平均激子数，其中" }, { "name": "italic", "data": [ { "name": "text", "data": "P" } ] }, { "name": "text", "data": "，" }, { "name": "italic", "data": [ { "name": "text", "data": "f" } ] }, { "name": "text", "data": "分别是激光功率密度和频率，" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733476&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733475&type=", "width": "3.72533321", "height": "2.62466669", "fontsize": "" } } } ] }, { "name": "text", "data": "为激发光光子能量，" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733478&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733477&type=", "width": "2.28600001", "height": "2.62466669", "fontsize": "" } } } ] }, { "name": "text", "data": "表示样品在激发波长处的吸收截面" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "22", "type": "bibr", "rid": "R22", "data": [ { "name": "text", "data": "22" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。样品的吸收截面我们根据参考文献估算得到" }, { "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": "，直径为15 nm量子阱在400 nm激发光处的吸收截面约为8.3×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-14 " } ] }, { "name": "text", "data": "cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "。考虑到我们设置的激发波长以及颗粒的体积比例关系，得到所制备样品的吸收截面约为2×10" }, { "name": "sup", "data": [ { "name": "text", "data": "-13 " } ] }, { "name": "text", "data": "cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "，与钙钛矿结构纳米晶的吸收截面相近" }, { "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": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "我们首先分析带隙(650 nm)处的动力学特征，衰减曲线显示出强烈的功率依赖性，如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "(a)所示。在低功率下，每个纳米晶吸收的平均光子为" }, { "name": "text", "data": "<" }, { "name": "text", "data": "N" }, { "name": "text", "data": ">" }, { "name": "text", "data": "~ 0.06以确保不形成多激子，发射几乎完全来自单激子态。由于粒子带电效应通常是不可避免的，即使在激发光强度很低的情况下，整个衰减曲线仍然有一部分来自带电激子的贡献。衰减曲线可拟合得到18 ns和50 ns两个时间常数。我们在120 ns处对不同功率下的PL衰减曲线进行归一化。随着激发功率的增加，观察到曲线衰减的早期出现了额外的快速成分，我们推测其为多激子态发射。t " }, { "name": "text", "data": ">" }, { "name": "text", "data": " 120 ns后所有曲线重合在一起，这表明在此时间节点处快速成分已经完全衰减。为了量化多激子的寿命，我们从高功率下测量的曲线中减去缩放获得的单激子的贡献，分离出纯快速成分的动力学特征。如" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "(b)所示，" }, { "name": "text", "data": "<" }, { "name": "text", "data": "N" }, { "name": "text", "data": ">" }, { "name": "text", "data": "~ 3.8时，我们从动力学曲线中提取到一个新的时间常数3.56 ns。随着激发功率的进一步增加，还可以拟合得到超快的亚纳秒级衰减成分。" } ] }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "（a）不同激发功率下，在120 ns处归一化的衰减曲线。（b） ~ 3.8时，多激子衰减曲线通过从高功率衰减曲线中减去单激子贡献得到，用3.56 ns和17.8 ns的两个指数拟合。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 2" } ], "title": [ { "name": "text", "data": "（a） Normalized decay curves at 120 ns under different excitation power. （b） ~ 3.8， the multiexcitons decay curve is obtained by subtracting the single exciton contribution from the high-power decay curve， and is fitted with two exponents of 3.56 ns and 17.8 ns." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733479&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733481&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733480&type=", "width": "147.63800049", "height": "50.16500092", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "为了进一步探究快速成分的激子态类别，我们应用多指数函数拟合了所有的衰减曲线，并绘制了各个成分的PL强度与激发功率的关系，如" }, { "name": "xref", "data": { "text": "图3", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3" } ] } }, { "name": "text", "data": "所示。首先，时间常数为50 ns的激子态，其PL强度与激光强度成线性比例，这与单激子特性是一致的。而18 ns的成分同样随着功率的增大而线性增长，这证明了该成分并非多激子态，应为带电激子态。另一方面，我们观察到寿命为3.56 ns分量的PL强度与功率呈现近似二次(~1.8)依赖关系，表明在同一脉冲内至少有两个光子被单个纳米晶吸收形成多激子。因此，根据以上测量和分析，我们推测双激子(BX)寿命约为3.56 ns，而高阶多激子的时间常数在亚纳秒量级。" } ] }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "（a）不同激发功率下衰减曲线的拟合图。（b）不同分量发光强度与功率的关系。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.3" } ], "title": [ { "name": "text", "data": "（a） Fitting curves of decay dynamics under different excitation power. （b）The relationship between emission intensity and power of different components." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733482&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733484&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733483&type=", "width": "140.51098633", "height": "47.55400085", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "根据自由载流子的辐射衰减速率模型可以估算双激子量子产率" }, { "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": "，即" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733486&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733485&type=", "width": "14.73200035", "height": "3.89466691", "fontsize": "" } } } ] }, { "name": "text", "data": "/4，通过测量的单激子辐射寿命，能够得到双激子的辐射寿命" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733488&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733487&type=", "width": "6.01133299", "height": "3.72533321", "fontsize": "" } } } ] }, { "name": "text", "data": "约为12.5 ns。进而计算出双激子的量子产率约为29%。考虑到双激子寿命由辐射寿命和非辐射寿命组成" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733490&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733489&type=", "width": "24.89200020", "height": "4.14866638", "fontsize": "" } } } ] }, { "name": "sup", "data": [ { "name": "text", "data": " [" }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，可以得到了双激子的俄歇复合寿命" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "math": "", "graphicsData": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733492&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733491&type=", "width": "6.18066692", "height": "3.97933316", "fontsize": "" } } } ] }, { "name": "text", "data": "约为5 ns。我们对比了文献报道的不同类型纳米晶体的双激子性质" }, { "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": "27", "type": "bibr", "rid": "R27", "data": [ { "name": "text", "data": "27" } ] } } ], "rid": [ "R25", "R26", "R27" ], "text": "25-27", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。由" }, { "name": "xref", "data": { "text": "表1", "type": "table", "rid": "T1", "data": [ { "name": "text", "data": "表1" } ] } }, { "name": "text", "data": "可知，文献[" }, { "name": "xref", "data": { "text": "27", "type": "bibr", "rid": "R27", "data": [ { "name": "text", "data": "27" } ] } }, { "name": "text", "data": "]所用样品与本文具有相似的结构和尺寸，但由于其结构中存在巨型内核，导致了样品的荧光量子产率非常低，双激子的荧光量子产率也低于本文。此外，对于传统的准II型CdSe/CdS量子点，虽然可以得到QY较高的样品，但由于尺寸受限，对双激子俄歇复合的抑制作用较小。相对于具有大能量梯度界面的粒子，具有平滑界面的纳米晶体，例如CdSe/Cd" }, { "name": "sub", "data": [ { "name": "text", "data": "x" } ] }, { "name": "text", "data": "Zn" }, { "name": "sub", "data": [ { "name": "text", "data": "1-x" } ] }, { "name": "text", "data": "Se，CdSe/CdSe" }, { "name": "sub", "data": [ { "name": "text", "data": "x" } ] }, { "name": "text", "data": "S" }, { "name": "sub", "data": [ { "name": "text", "data": "1-x" } ] }, { "name": "text", "data": "/CdS等结构对俄歇作用的抑制较为显著。最高可以实现双激子QY为45%，俄歇寿命2.4 ns。相比之下，尽管本文样品不具有平滑的界面结构，但同样可以实现高QY和较好的俄歇复合抑制。" } ] }, { "name": "table", "data": { "id": "T1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "表1" } ], "title": [ { "name": "text", "data": "参考文献中不同类型纳米晶体双激子的性质" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Tab.1" } ], "title": [ { "name": "text", "data": "Properties of biexcitons in different types of nanocrystals in literature" } ] } ], "note": [ { "lang": "zh", "data": [ { "name": "p", "data": [ { "name": "text", "data": "*表示该数值为根据文献报道的数据计算得到" } ] } ] } ], "table": [ { "head": [ [ { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "text", "data": "样品类型" } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "text", "data": "样品直径/nm" } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "text", "data": "发光波长/nm" } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "text", "data": "荧光量子产率/%" } ] }, { "align": "center", "style": "border-top:solid;border-bottom:solid;", "data": [ { "name": "text", "data": "双激子荧光量子产率/%" } ] }, { "align": "center", "style": 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"border-bottom:solid;", "data": [ { "name": "text", "data": "650" } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "text", "data": "80" } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "text", "data": "29" } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "text", "data": "5" } ] }, { "align": "center", "style": "border-bottom:solid;", "data": [ { "name": "text", "data": "本文" } ] } ] ], "foot": [] } ], "graphics": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733494&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733493&type=", "width": "162.80000305", "height": "45.49623489", "fontsize": "" } } }, { "name": "p", "data": [ { "name": "text", "data": "为了更加深入地分析激子态的跃迁过程，本文以三激子为例，目前普遍接受的衰减模式为级联跃迁衰减：TX-" }, { "name": "text", "data": ">" }, { "name": "text", "data": "BX-" }, { "name": "text", "data": ">" }, { "name": "text", "data": "X-" }, { "name": "text", "data": ">" }, { "name": "text", "data": "X" }, { "name": "sub", "data": [ { "name": "text", "data": "0" } ] }, { "name": "text", "data": "基态，如" }, { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "所示。这里我们应用速率方程，在考虑多能级级联跃迁的情况下，根据实验参数和样品参数模拟了中性激子的发光强度随激发功率的变化情况。从模拟结果可以看出，单激子和双激子的PL强度与功率的关系与我们得到的较为一致。此外，我们还观察到高功率下，曲线会趋于饱和，这应该是由于泵浦速率远大于衰减速率导致的。" } ] }, { "name": "fig", "data": { "id": "F4", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图4" } ], "title": [ { "name": "text", "data": "三种激发态的发射强度与激发功率关系的模拟图，其中插图部分为级联跃迁示意图。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.4" } ], "title": [ { "name": "text", "data": "Simulation diagram of the relationship between emission intensity and excitation power of the three states， inset： a schematic diagram of cascade transition." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733495&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733497&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733496&type=", "width": "73.09600067", "height": "55.31600189", "fontsize": "" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "title": [ { "name": "text", "data": "3.3　不同激光功率下的时间分辨光谱" } ], "level": "2", "id": "s3c" } }, { "name": "p", "data": [ { "name": "text", "data": "除了用衰减曲线记录动力学过程外，本文还利用时间分辨光谱切片直接观察和分析谱线随激发强度的变化情况。为了研究具有超快复合特性的多激子，我们通过不同时间切片的积分光谱提取多激子的发射光谱。如" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "(a)所示，当入射光处于低功率时，从图中早期和晚期的时间切片光谱比较中，我们没有观察到光谱发射峰的明显变化，而据报道准II型量子点中双激子发射峰相对于单激子存在蓝移特征(排斥作用)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此相近的光谱谱线表明没有多激子复合的存在，也表明该样品的均匀性较好。若样品是多分散的，由于从小粒子到大粒子的能量转移，应观察到光谱显著的红移。当考虑高强度光激发时，光谱演化有明显的不同, 时间切片光谱如" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "(b)所示。谱线在能量高的一侧衰减初期出现明显的发射特征。随着时间的增加，这些特征峰迅速衰减直至消失，留下单激子光谱轮廓。这些发射峰有强烈地功率依赖性，这是多激子的典型特征。根据发射能量不同，这些发射峰可分为两种类型：发光层发射和壳层发射。" } ] }, { "name": "fig", "data": { "id": "F5", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图5" } ], "title": [ { "name": "text", "data": "（a）激发功率为9.3 nW时的时间切片光谱，（b）激发功率为35.8μW时的时间切片光谱。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 5" } ], "title": [ { "name": "text", "data": "（a） Time slice spectrum when the excitation power is 9.3 nW. （b） Time slice spectrum when the excitation power is 35.8μW." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733498&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733500&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733499&type=", "width": "146.84399414", "height": "52.33499908", "fontsize": "" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "我们首先对源自发光层的发射峰进行光谱分析。单激子的发射峰在650 nm处，0-0.8 ns光谱切片带隙处的发射峰（644.5 nm）与单激子相比约有5.5 nm蓝移(16 meV)。一般来说，双激子中激子-激子相互作用能约为10 meV，因此我们认为带隙处发射峰为带电激子和双激子的叠加。接下来，我们分析涉及高阶多激子复合的发射峰，从图中可以观察到615 nm和576 nm处的明显发射峰值。对于TX的级联衰减过程，从TX-" }, { "name": "text", "data": ">" }, { "name": "text", "data": "BX的具体流程存在很大争议。如" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "所示，有三种可能的重组途径，分别为1S" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1S" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "，1P" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1P" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "以及1P" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1S" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "。Katherine等人通过CdSe/CdS 纳米晶的三阶关联方法证明1S" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1S" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "跃迁路径在此过程中占主导地位" }, { "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": "。Lim等人" }, { "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": "发现1P激光阈值略低于1P" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1P" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "跃迁的理论值，他们将其归因于存在1P" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1S" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "复合路径。由于材料价带中相应能级非常接近，带边1S和1P空穴态的混合效应可能非常显著，从而允许了1P" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1S" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "跃迁。除此之外，关于带电双激子和三激子的许多其他报告也证明了这种跃迁的存在" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "12", "type": "bibr", "rid": "R12", "data": [ { "name": "text", "data": "12" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "30", "type": "bibr", "rid": "R30", "data": [ { "name": "text", "data": "30" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。然而在光谱轮廓中，很难区分这两种不同的P能级相关跃迁。基于以上分析，我们认为相对于单激子峰具有35 nm蓝移的峰值为1S" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1S" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "跃迁，涉及具有四个以上载流子的状态。而在576 nm处的较高能量发射峰源于P能级相关发射。通过与吸收光谱的二级微分对比（" }, { "name": "xref", "data": { "text": "图1", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1" } ] } }, { "name": "text", "data": "(c)），我们观察到1P能级发射峰与吸收峰的Stokes位移约为47 nm（大于1S能级相应的Stokes位移16 nm）。这种较大的Stokes位移说明了该发射峰中可能存在1P" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1S" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "跃迁。因为1P" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1S" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "的能量分离小于1P" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1P" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "跃迁，所以1P" }, { "name": "sub", "data": [ { "name": "text", "data": "e" } ] }, { "name": "text", "data": "-1S" }, { "name": "sub", "data": [ { "name": "text", "data": "3/2" } ] }, { "name": "text", "data": "跃迁的存在会使发光波长增大。最后，在高强度激发下，还观察到约512 nm处的另一个发射峰。由于其位置接近CdS带隙能量，我们推测其为与壳层相关的光学跃迁" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "25", "type": "bibr", "rid": "R25", "data": [ { "name": "text", "data": "25" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。当纳米颗粒中存在大量载流子时，一部分电子-空穴对不会热弛豫到发射层中，而是在壳层中直接复合发射高能光子。" } ] }, { "name": "fig", "data": { "id": "F6", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图6" } ], "title": [ { "name": "text", "data": "三激子的不同辐射复合路径示意图。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig.6" } ], "title": [ { "name": "text", "data": "Schematic diagram of different radiative recombination pathways of triexcitons." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733501&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733503&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=40733502&type=", "width": "62.52999878", "height": "57.32600021", "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，本文通过热注射法合成了形态均匀的大尺寸球形量子阱。应变外延生长所得的量子阱异质结构可以有效缓解厚壳层带来的结构缺陷，从而实现了纳米晶的高荧光量子产率(>80%)。通过时间分辨荧光光谱技术，我们在光谱及动力学方面完成了对不同功率激发下激子态种类的分析。根据不同激发态独特的时间和光谱特性，我们探究了单激子，双激子以及高阶多激子的发射特征。并通过计算得到双激子的荧光量子产率约为30%，俄歇复合寿命达到纳秒量级。这表明了大尺寸量子阱在抑制俄歇复合方面具有优异的性能，使得其在低阈值纳米激光的实现，载流子倍增效应的研究等领域将具有非常大的应用潜力。" } ] } ] } ], "footnote": [], "reflist": { "title": [ { "name": "text", "data": "参考文献" } ], "data": [ { "id": "R1", "label": "1", "citation": [ { "lang": "en", "text": [ { "name": "text", "data": "KLIMOV V I" }, { "name": "text", "data": ". 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