Upconversion Luminescence in Quantum Dots Enhanced Publication

{ "defaultlang": "zh", "titlegroup": { "articletitle": [ { "lang": "zh", "data": [ { "name": "text", "data": "上转换发光量子点" } ] }, { "lang": "en", "data": [ { "name": "text", "data": "Upconversion Luminescence in Quantum Dots" } ] } ] }, "contribgroup": { "author": [ { "name": [ { "lang": "zh", "surname": "刘", "givenname": "秀", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "LIU", "givenname": "Xiu", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [ "first-author" ], "bio": [ { "lang": "zh", "text": [ "刘秀(1988-)，男，山东莱芜人，博士，2017年于钢铁研究总院获得博士学位，主要从事量子点材料及其显示应用方向的研究。E-mail: liuxiu44@163.com" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656869&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656874&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656879&type=" } ], "data": [ [ { "name": "text", "data": "刘秀" }, { "name": "text", "data": "(1988-)，男，山东莱芜人，博士，2017年于钢铁研究总院获得博士学位，主要从事量子点材料及其显示应用方向的研究。E-mail: " }, { "name": "text", "data": "liuxiu44@163.com" } ] ] } ], "email": "liuxiu44@163.com", "deceased": false }, { "name": [ { "lang": "zh", "surname": "车", "givenname": "艳玲", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "CHE", "givenname": "Yan-ling", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [], "deceased": false }, { "name": [ { "lang": "zh", "surname": "杨", "givenname": "高岭", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "YANG", "givenname": "Gao-ling", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff1", "text": "1" } ], "role": [ "corresp" ], "corresp": [ { "rid": "cor1", "lang": "en", "text": "*E-mail: glyang@bit.edu.cn", "data": [ { "name": "text", "data": "*E-mail: glyang@bit.edu.cn" } ] } ], "bio": [ { "lang": "zh", "text": [ "杨高岭(1987-)，男，河南鹿邑人，博士，副研究员，2016年于北京理工大学获得博士学位，主要从事微纳光刻与智能显示方向的研究。E-mail: glyang@bit.edu.cn" ], "graphic": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656884&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656889&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656893&type=" } ], "data": [ [ { "name": "text", "data": "杨高岭" }, { "name": "text", "data": "(1987-)，男，河南鹿邑人，博士，副研究员，2016年于北京理工大学获得博士学位，主要从事微纳光刻与智能显示方向的研究。E-mail: " }, { "name": "text", "data": "glyang@bit.edu.cn" } ] ] } ], "email": "glyang@bit.edu.cn", "deceased": false }, { "name": [ { "lang": "zh", "surname": "钟", "givenname": "海政", "namestyle": "eastern", "prefix": "" }, { "lang": "en", "surname": "ZHONG", "givenname": "Hai-zheng", "namestyle": "eastern", "prefix": "" } ], "stringName": [], "aff": [ { "rid": "aff2", "text": "2" } ], "role": [], "deceased": false } ], "aff": [ { "id": "aff1", "intro": [ { "lang": "zh", "label": "1", "text": "北京理工大学　光电学院，北京　100081", "data": [ { "name": "text", "data": "北京理工大学　光电学院，北京　100081" } ] }, { "lang": "en", "label": "1", "text": "School of Optics and Photonics, Beijing Institute of Technology, Beijing 100081, China", "data": [ { "name": "text", "data": "School of Optics and Photonics, Beijing Institute of Technology, Beijing 100081, China" } ] } ] }, { "id": "aff2", "intro": [ { "lang": "zh", "label": "2", "text": "北京理工大学　材料学院，北京　100081", "data": [ { "name": "text", "data": "北京理工大学　材料学院，北京　100081" } ] }, { "lang": "en", "label": "2", "text": "School of Materials Science & Engineering, Beijing Institute of Technology, Beijing 100081, China", "data": [ { "name": "text", "data": "School of Materials Science & Engineering, Beijing Institute of Technology, Beijing 100081, China" } ] } ] } ] }, "abstracts": [ { "lang": "zh", "data": [ { "name": "p", "data": [ { "name": "text", "data": "光子上转换是一种重要的非线性反斯托克斯发光现象，在激光、显示、光伏、信息安全以及生物成像与诊疗等领域具有应用前景。与研究较多的有机分子三重态-三重态湮灭和稀土掺杂纳米颗粒上转换发光材料相比，上转换量子点可以在宽光谱激发范围内实现上转换发光，具有频谱吸收宽、发光效率高、近红外可吸收、能带可调、尺寸小以及稳定性高等特点，引起了领域内的关注。本文介绍了上转换发光的种类及机理，对近年来上转换发光量子点的研究进展进行了总结，重点分析了基于激发态吸收的半导体双量子点的类型和设计原理，探讨了上转换发光量子点在发光二极管(LED)、光电探测、生物标记、太阳能电池等方面的应用潜力，特别是未来发展面临的挑战和前景。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "Photon upconversion(UC), a nonlinear optical process that converts multiple low-energy photons into a single high-energy photon, is of significant importance in many fields, such as laser, display, photovoltaic, information security, bioimaging and diagnosis. In compare with the well developed lanthanide-doped nanocrystals and triple-triple annihilation, UC quantum dots can achieve UC luminescence under a wide spectral excitation range, which are emerging as promising candidates for many photonic applications due to their wide spectral absorption, high luminous efficiency, near-infrared absorption, tunable energy band, small size and high stability. In this short review, we summarize the progress of upconversion semiconductor quantum dots with the description of basic mechanisms, recent progress of different types of UC quantum dots, especially UC dual quantum dots that based on excited state absorption, discuss the application potential of UC quantum dots in light-emitting diodes, detectors, solar cells and biomarkers, then we conclude with a brief prespective about the challenges and future prospects in this field." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "上转换发光" } ], [ { "name": "text", "data": "量子点" } ], [ { "name": "text", "data": "能带调控" } ], [ { "name": "text", "data": "半导体纳米晶" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "upconversion luminescence" } ], [ { "name": "text", "data": "quantum dots" } ], [ { "name": "text", "data": "energy band engineering" } ], [ { "name": "text", "data": "semiconductor nanocrystals" } ] ] } ], "highlights": [], "body": [ { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "1" } ], "title": [ { "name": "text", "data": "引言" } ], "level": "1", "id": "s1" } }, { "name": "p", "data": [ { "name": "text", "data": "近年来，上转换发光因其独特的反斯托克斯发光特性引起了人们的广泛关注，并在光伏、生物成像与诊疗、信息存储与安全、激光、以及三维显示等领域展现出了广阔的应用前景" }, { "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": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } } ], "rid": [ "R1", "R2", "R3", "R4", "R5", "R6", "R7", "R8", "R9", "R10" ], "text": "1-10", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。与传统的斯托克斯发射(短波激发、长波发射)相比，上转换发光可以将低频光子转化成高频光子，通常是近红外光激发、可见光发射，因此在长波长特别是近红外光的利用方面具有极大的优势。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "现阶段研究最多的上转换体系主要有两种，稀土掺杂的纳米颗粒和基于三重态-三重态湮灭(Triplet-triplet annihilation,TTA)的上转换发光有机分子体系，这也是迄今为止两种最为经典的上转换体系。镧系元素掺杂的上转换纳米粒子由于其低毒性、高化学稳定性、窄带发射以及长荧光寿命等优点，已经被越来越多地应用于药物递送、生物成像、信息存储以及三维显示等领域" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "11", "type": "bibr", "rid": "R11", "data": [ { "name": "text", "data": "11" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "15", "type": "bibr", "rid": "R15", "data": [ { "name": "text", "data": "15" } ] } } ], "rid": [ "R11", "R12", "R13", "R14", "R15" ], "text": "11-15", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。然而，由于稀土元素吸收截面比较小且吸收波长比较固定，约束了镧系元素掺杂上转换纳米粒子的量子产率及可利用波长范围，因此其在实际应用中受到了一定的限制。与稀土元素掺杂上转换相比，TTA体系可在较低的激发功率密度(" }, { "name": "text", "data": "<" }, { "name": "text", "data": "0.1 W/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")下实现较高量子产率(" }, { "name": "text", "data": ">" }, { "name": "text", "data": "10%)的上转换发光，甚至可以在太阳光下工作，因而TTA上转换在光催化以及太阳能发电等方面具有应用前景" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "16", "type": "bibr", "rid": "R16", "data": [ { "name": "text", "data": "16" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } } ], "rid": [ "R16", "R17", "R18", "R19", "R20" ], "text": "16-20", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。然而，由于TTA体系发光过程涉及三线态激子的迁移和湮灭，因此极易受到氧气分子的破坏导致发光猝灭；此外，有机分子的不稳定性及应用时固载困难的问题也进一步约束了TTA在更多领域中的应用。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "量子点是一种半径接近或小于激子玻尔半径的半导体纳米颗粒，具有频谱吸收宽、发光效率高、能带连续可调、尺寸小以及稳定性高等特点" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "21", "type": "bibr", "rid": "R21", "data": [ { "name": "text", "data": "21" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "25", "type": "bibr", "rid": "R25", "data": [ { "name": "text", "data": "25" } ] } } ], "rid": [ "R21", "R22", "R23", "R24", "R25" ], "text": "21-25", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，同时还具有优异的溶液加工特性，已经成为照明与显示领域研究及应用的热门材料" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "26", "type": "bibr", "rid": "R26", "data": [ { "name": "text", "data": "26" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } } ], "rid": [ "R26", "R27", "R28", "R29", "R30", "R31", "R32" ], "text": "26-32", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。如果能实现半导体量子点的上转换发光，将有望彻底解决目前主流上转换材料难以实现宽频谱上转换的问题，突破上转换发光技术在光电子领域的应用瓶颈。2013年，以色列魏兹曼科学研究院的Oron等通过构筑半导体双量子点首次实现了基于激发态吸收的量子点上转换发光，开启了全无机胶体半导体量子点上转换发光的新篇章" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。到目前为止，利用胶体化学合成的方法，研究人员已经实现了基于不同上转换发光机理的上转换量子点的构筑，如激发态吸收、声子辅助、量子点敏化TTA、量子点复合镧系纳米颗粒等，其上转换发光特性也得到了广泛的研究" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } } ], "rid": [ "R33", "R34", "R35", "R36", "R37" ], "text": "33-37", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。利用上转换量子点的溶液可加工性能和宽频谱吸收特性，研究者也探究了上转换量子点在固态照明与显示、太阳能电池、生物成像等领域的应用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "36", "type": "bibr", "rid": "R36", "data": [ { "name": "text", "data": "36" } ] } }, { "name": "text", "data": "," }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "40", "type": "bibr", "rid": "R40", "data": [ { "name": "text", "data": "40" } ] } } ], "rid": [ "R38", "R39", "R40" ], "text": "38-40", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "上转换发光量子点是近年来发展起来的新型上转换发光体系，能够充分利用量子点材料较高的发光效率、近红外可吸收、可调的吸收和发射、尺寸小以及无机材料的高稳定性等特点，在上转换应用领域极具潜力。近年来，虽然对于上转换发光量子点的研究不断深入，但是关于量子点上转换的综述较少。基于此，我们简要介绍了近年来上转换发光量子点的研究进展，总结了上转换发光量子点在发光二极管(Light emitting diode,LED)、生物标记、太阳能电池等方面的应用，并阐述了该领域面临的挑战和未来可能的发展方向。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "2" } ], "title": [ { "name": "text", "data": "上转换发光机理" } ], "level": "1", "id": "s2" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "2.1" } ], "title": [ { "name": "text", "data": "同时激发上转换发光过程" } ], "level": "2", "id": "s2a" } }, { "name": "p", "data": [ { "name": "text", "data": "实现上转换发光的基本方法主要有两种：同时激发和连续激发。其中，二次谐波(Second harmonic generation,SHG)是最标准的将低能光子转换成高能光子的同时激发方法，这是一种基本的二阶非线性光学现象，也称倍频效应" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "41", "type": "bibr", "rid": "R41", "data": [ { "name": "text", "data": "41" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "42", "type": "bibr", "rid": "R42", "data": [ { "name": "text", "data": "42" } ] } } ], "rid": [ "R41", "R42" ], "text": "41-42", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。如" }, { "name": "xref", "data": { "text": "图1(a)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(a)" } ] } }, { "name": "text", "data": "所示，它是指两个基频光光子与非线性晶体材料相互作用之后，产生一个光子的过程，新产生的光子频率两倍于基频光光子" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "43", "type": "bibr", "rid": "R43", "data": [ { "name": "text", "data": "43" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。倍频效应可以看作是一种特殊的和频现象，它可以使波长位于近红外光的激光转化成可见光，在激光频率转换方面发挥了重要作用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "44", "type": "bibr", "rid": "R44", "data": [ { "name": "text", "data": "44" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "48", "type": "bibr", "rid": "R48", "data": [ { "name": "text", "data": "48" } ] } } ], "rid": [ "R44", "R45", "R46", "R47", "R48" ], "text": "44-48", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。但是，这种基于二次谐波的上转换通常需要很高的激发强度(" }, { "name": "text", "data": ">" }, { "name": "text", "data": "10" }, { "name": "sup", "data": [ { "name": "text", "data": "6" } ] }, { "name": "text", "data": " W/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")，因此在实际应用方面受限很大" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "47", "type": "bibr", "rid": "R47", "data": [ { "name": "text", "data": "47" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "上转换发光机理。(a)二次谐波；(b)双光子吸收；(c)激发态吸收；(d)能量传递；(e)光子雪崩。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 1" } ], "title": [ { "name": "text", "data": "UC luminescence mechanism. (a)Second harmonic generation, SHG. (b)Two photon absorption, TPA. (c)Excited stated absorption, ESA. (d)Energy transfer, ET. (e)Photon avalanche, PA." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656900&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656910&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656906&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "另一种常见的同时激发的方法是双光子吸收(Two photon absorption,TPA)，这一类上转换是指在强光的激发下，荧光分子同时吸收两个光子，跃迁到能量是激发光能量两倍的激发态，然后产生跃迁，得到上转换荧光的过程，如" }, { "name": "xref", "data": { "text": "图1(b)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(b)" } ] } }, { "name": "text", "data": "所示。双光子吸收与传统荧光分子吸收的差别在于它是通过一个中间虚态，使得荧光分子得到双倍的能量而产生上转换发光。自1961年首次在掺杂稀土离子的CdF∶Eu" }, { "name": "sup", "data": [ { "name": "text", "data": "2+" } ] }, { "name": "text", "data": "晶体中观察到双光子荧光现象后" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "48", "type": "bibr", "rid": "R48", "data": [ { "name": "text", "data": "48" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，人们对双光子吸收现象进行了大量的研究，在半导体晶体、有机染料、掺杂有机染料固体介质、有机生色团等材料中都观察到了双光子吸收现象" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "49", "type": "bibr", "rid": "R49", "data": [ { "name": "text", "data": "49" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "55", "type": "bibr", "rid": "R55", "data": [ { "name": "text", "data": "55" } ] } } ], "rid": [ "R49", "R50", "R51", "R52", "R53", "R54", "R55" ], "text": "49-55", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。但是，由于双光子吸收需要很强的激发能量和超快光源，因此在向实际应用发展过程中所面临的挑战依旧很大" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "56", "type": "bibr", "rid": "R56", "data": [ { "name": "text", "data": "56" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "57", "type": "bibr", "rid": "R57", "data": [ { "name": "text", "data": "57" } ] } } ], "rid": [ "R56", "R57" ], "text": "56-57", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "2.2" } ], "title": [ { "name": "text", "data": "连续激发上转换发光过程" } ], "level": "2", "id": "s2b" } }, { "name": "p", "data": [ { "name": "text", "data": "通常来讲，真正意义上的上转换发光采用的是连续激发的机理。连续激发的上转换发光是指体系受激后，激发能量能够存储在一个真实的态中，这与二次谐波或双光子吸收中的虚态截然不同，这个真实的态有足够长的寿命能够再吸收一个光子从而跃迁到更高的能级。与同时激发的方法相比，这种连续激发的上转换过程所需的激发能量很小，极具应用优势。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "基于这种连续激发的机理主要有激发态吸收、能量传递和光子雪崩三种类型" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "58", "type": "bibr", "rid": "R58", "data": [ { "name": "text", "data": "58" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。激发态吸收(Excited stated absorption,ESA)是指电子吸收光子后从基态跃迁到激发态，在跃迁回基态之前再吸收一个或多个光子，从而跃迁到更高的能级的过程。如" }, { "name": "xref", "data": { "text": "图1(c)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(c)" } ] } }, { "name": "text", "data": "所示，位于基态能级E" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "的电子，吸收光子后跃迁到亚稳态能级E" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "上，电子在稳态能级上再吸收一个光子从而跃迁到更高能级E" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "上，当电子从E" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "能级向下跃迁回E" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "能级时就会产生高能量光子。能量传递(Energy transfer,ET)通常是离子间相互作用的方式之一，当足够多的离子被激发到中间态能级上之后，在满足能级匹配的条件下，处于激发态的离子之间发生能量传递，其中一个离子无辐射弛豫到较低能级态，另一个离子则被激发到高能态进而产生高能光子的辐射跃迁，如" }, { "name": "xref", "data": { "text": "图1(d)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(d)" } ] } }, { "name": "text", "data": "所示。光子雪崩(Photon avalanche,PA)的原理如" }, { "name": "xref", "data": { "text": "图1(e)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(e)" } ] } }, { "name": "text", "data": "所示，当E" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "和E" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "能级间的能量差与泵浦光子能量相等时，处于E" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "能级上的粒子由于激发态吸收，跃迁到更高的E" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "能级上，接着E" }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "与E" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "能级上的粒子通过交叉弛豫过程，分别布局到E" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "能级上，如此周而复始，粒子数呈几何倍数增加，如同雪崩一样地在E" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "能级上迅速积累，这样的过程被称为光子雪崩。光子雪崩是激发态吸收和能量传递相结合的过程，只是能量传递发生在同种离子之间。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "3" } ], "title": [ { "name": "text", "data": "上转换发光量子点" } ], "level": "1", "id": "s3" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "3.1" } ], "title": [ { "name": "text", "data": "激发态吸收上转换发光量子点" } ], "level": "2", "id": "s3a" } }, { "name": "p", "data": [ { "name": "text", "data": "2013年，以色列魏兹曼科学研究院的Oron课题组首次提出并证实了双量子点中存在基于激发态吸收机理的上转换发光过程" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。他们所采用的量子点体系如" }, { "name": "xref", "data": { "text": "图2(a)", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2(a)" } ] } }, { "name": "text", "data": "所示，低能级态的Te∶CdSe量子点是光子吸收体，高能级态的CdSe量子点是光子发射体，双量子点间的CdS的作用是形成两者间的势垒。这种双量子点(Te∶CdSe/CdS/CdSe)中的两个独立的发光量子点(Te∶CdSe,CdSe)在短波长激发下可以产生双峰发射(" }, { "name": "xref", "data": { "text": "图2(b)", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2(b)" } ] } }, { "name": "text", "data": ")，且由于非常近的空间距离，二者之间存在电子耦合现象。当用680 nm的泵浦光激发后，可以观测到高能光子的发射，如" }, { "name": "xref", "data": { "text": "图2(c)", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2(c)" } ] } }, { "name": "text", "data": "所示；且上转换发光光谱与用405 nm激发产生的光谱几乎一致，说明上转换发光来自于高能量子点的直接带隙复合。上转换需要吸收两个低能量光子，因此在较低激发强度时，上转换发光强度与激发强度成二次方关系，饱和之后二者成线性关系，如" }, { "name": "xref", "data": { "text": "图2(d)", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2(d)" } ] } }, { "name": "text", "data": "所示。这是对上转换半导体双量子点体系的首次报道，但该结构的上转换发光效率却非常低(0.1%)。基于这种激发态吸收的上转换发光量子点通常由三种不同的半导体材料组成，分别作为上转换发光中所需的吸收体、势垒、发光体，且三种半导体材料需封闭在同一纳米晶中才可实现半导体材料的室温上转换发光。由于其中的吸收体和发光体一般是独立的不同能级的量子点体系，因而，这种新型的兼具两种不同量子点材料的上转换量子点体系也被称之为半导体双量子点" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "59", "type": "bibr", "rid": "R59", "data": [ { "name": "text", "data": "59" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "半导体双量子点上转换发光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。(a)双量子点能带结构；(b)吸收与发射光谱；(c)上转换发光光谱；(d)激发能量密度与上转换发光强度关系示意图。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 2" } ], "title": [ { "name": "text", "data": "Description of the UC double QDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (a)Schematic depiction of dual emitting quantum dot. (b)Ensemble absorption(blue) and emission(red) spectra. (c)Emission spectrum of UC luminescence excited at 680 nm(blue) closely resembles the ensemble emission spectrum excited at 405 nm(red). (d)Excitation energy density dependence of the UC luminescence(blue circles) together with quadratic(red) and linear(green) fits to the respective parts of the curve." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656916&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656924&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656920&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "半导体量子点材料的上转换发光效率主要是由两个因素决定的：上转换效率和荧光量子产率。上转换效率即激子从低能级量子点跃迁到高能级量子点的效率，这个过程通常被热激子重新冷却到低能级所限制。因此，为了提高半导体量子点的上转换效率，可以通过采用长荧光寿命的量子点(如PbSe、PbS等)作为吸收体，或通过能级调控来限制载流子回流来实现。如洛斯阿拉莫斯国家实验室的Makarov等采用长荧光寿命(" }, { "name": "text", "data": ">" }, { "name": "text", "data": "2 μs)的PbSe量子点做光子吸收体，在较低的激发强度(" }, { "name": "text", "data": "<" }, { "name": "text", "data": "1 W/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")下实现了PbSe/CdSe量子点的上转换发光，上转换发光效率为0.2%" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "35", "type": "bibr", "rid": "R35", "data": [ { "name": "text", "data": "35" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。魏兹曼科学研究院的Teitelboim等在PbSe量子点外进一步通过生长CdSe(ZB)/CdSe(WZ)量子阱结构(如" }, { "name": "xref", "data": { "text": "图3(d)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(d)" } ] } }, { "name": "text", "data": "所示)，有效地将上转换荧光量子产率提升到了0.7%，实现了光子从近红外区域(可达1.7 μm)到可见光(630~700 nm可调)的上转换" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "60", "type": "bibr", "rid": "R60", "data": [ { "name": "text", "data": "60" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。能带调控策略是另一种提高上转换效率的方法，Milleville等在Te∶CdSe/CdS/CdSe量子点的基础上利用合金化的策略进一步优化了上转换效率，他们发现采用均相核与合金化的棒时，如" }, { "name": "xref", "data": { "text": "图3(e)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(e)" } ] } }, { "name": "text", "data": "所示，由于表面缺陷和载流子回流受限，上转换发光性能可以提升100倍" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "61", "type": "bibr", "rid": "R61", "data": [ { "name": "text", "data": "61" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Yang等发展了PbS/CdS-CdSe/ZnS半Type-Ⅰ/反Type-Ⅰ双量子点体系，其能带结构如" }, { "name": "xref", "data": { "text": "图3(f)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(f)" } ] } }, { "name": "text", "data": "所示，利用能带调控和尺寸调控相结合的方式，将半导体量子点的上转换发光效率提高到2.17%。他们认为深空穴限域和长中间态寿命共同作用，会大大提高半导体双量子点的光子上转换效率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "62", "type": "bibr", "rid": "R62", "data": [ { "name": "text", "data": "62" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "量子点上转换发光效率调控。(a)上转换核壳量子点" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "66", "type": "bibr", "rid": "R66", "data": [ { "name": "text", "data": "66" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(b)上转换纳米棒" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "66", "type": "bibr", "rid": "R66", "data": [ { "name": "text", "data": "66" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(c)上转换纳米片" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "67", "type": "bibr", "rid": "R67", "data": [ { "name": "text", "data": "67" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(d)PbSe/CdSe/CdS 上转换量子点能带结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "60", "type": "bibr", "rid": "R60", "data": [ { "name": "text", "data": "60" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(e)CdSe(Te)/CdS" }, { "name": "sub", "data": [ { "name": "text", "data": "1-" }, { "name": "italic", "data": [ { "name": "text", "data": "x" } ] } ] }, { "name": "text", "data": "Se" }, { "name": "sub", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "x" } ] } ] }, { "name": "text", "data": "/CdSe 上转换纳米棒能带结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "61", "type": "bibr", "rid": "R61", "data": [ { "name": "text", "data": "61" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(f)PbS/CdS-CdSe/ZnS上转换量子点能带结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "62", "type": "bibr", "rid": "R62", "data": [ { "name": "text", "data": "62" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 3" } ], "title": [ { "name": "text", "data": "Engineering efficient photon upconversion in semiconductor heterostructures. (a)Core/multishell QDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "66", "type": "bibr", "rid": "R66", "data": [ { "name": "text", "data": "66" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (b)Dots in rod nanocrystals" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "66", "type": "bibr", "rid": "R66", "data": [ { "name": "text", "data": "66" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (c)CdSe/CdS/CdTe core/barrier/crown nanoplatelets" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "67", "type": "bibr", "rid": "R67", "data": [ { "name": "text", "data": "67" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (d)Schematic band alignment of PbSe/CdSe/CdS QDs-quantum well heterostructure" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "60", "type": "bibr", "rid": "R60", "data": [ { "name": "text", "data": "60" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (e)Band diagram of a complete CdSe(Te)/CdS" }, { "name": "sub", "data": [ { "name": "text", "data": "1-" }, { "name": "italic", "data": [ { "name": "text", "data": "x" } ] } ] }, { "name": "text", "data": "Se" }, { "name": "sub", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "x" } ] } ] }, { "name": "text", "data": "/CdSe upconverting nanostructure" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "61", "type": "bibr", "rid": "R61", "data": [ { "name": "text", "data": "61" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (f)Schematic illustration of the band alignment of PbS/CdS-CdSe/ZnS UC QDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "62", "type": "bibr", "rid": "R62", "data": [ { "name": "text", "data": "62" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656928&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656940&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656934&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "高能态量子点的荧光量子产率对量子点的上转换发光效率也至关重要。影响量子点发光效率的因素主要有两个：一个是缺陷态，量子点的非辐射复合主要是由表面缺陷引起的；另一个更重要的影响因素其实是Förster能量共振转移。一方面，我们需要吸收体和发射体之间存在电子耦合现象；但是，另一方面，由于发射体在能量共振转移中通常是供体分子，所以对上转换来说，如何有效地避免Förster能量共振转移是我们所必须考虑的。最基本的调控手段就是增加吸收体和发射体之间的距离，这在半导体量子点中比较容易实现，因为维度调控是量子点发展过程中一个非常重要的方向，目前已经可以通过溶液法合成多种维度的胶体量子点材料" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "63", "type": "bibr", "rid": "R63", "data": [ { "name": "text", "data": "63" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "65", "type": "bibr", "rid": "R65", "data": [ { "name": "text", "data": "65" } ] } } ], "rid": [ "R63", "R64", "R65" ], "text": "63-65", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。已有不同方法的工作报道利用维度调控来抑制Förster能量共振，比如采用纳米棒状或者片状结构(" }, { "name": "xref", "data": { "text": "图3(b)、(c)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(b)、(c)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "66", "type": "bibr", "rid": "R66", "data": [ { "name": "text", "data": "66" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "67", "type": "bibr", "rid": "R67", "data": [ { "name": "text", "data": "67" } ] } } ], "rid": [ "R66", "R67" ], "text": "66-67", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，增强发射体的发光强度，进而提升量子点的上转换发光效率(" }, { "name": "xref", "data": { "text": "图3(a)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(a)" } ] } }, { "name": "text", "data": ")。除了调节吸收体和发射体的空间距离以外，通过减少发射峰与吸收曲线之间的重叠也可以有效地抑制Förster能量共振转移。有研究表明，Type-Ⅱ量子点的吸收发射重合最小，能量共振也最小" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "68", "type": "bibr", "rid": "R68", "data": [ { "name": "text", "data": "68" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。基于此，北京理工大学Yang等报道了上转换Type-Ⅱ/Type-Ⅰ半导体双量子点" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "69", "type": "bibr", "rid": "R69", "data": [ { "name": "text", "data": "69" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，利用ZnTe/CdSe Type-Ⅱ量子点做光子吸收体，用CdSe/ZnSe Type-Ⅰ量子点作为光子发射体，将这两种量子点封闭成双量子点体系，使可见光的荧光量子产率提升到了50%，最终大大提高了半导体双量子点材料的上转换发光效率。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "基于激发态吸收的上转换发光量子点，其上转换发光过程是先通过带间吸收在低能级态生成一个限域的空穴和一个相对离域的电子，随后空穴通过直接吸收或间接吸收第二个光子越过势垒到达高能级态上，进而与离域的电子复合产生上转换发光。根据第二个吸收光子种类的不同，我们可以将上转换分成两种类型：直接带内吸收和俄歇辅助吸收，如" }, { "name": "xref", "data": { "text": "图4(a)、(b)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(a)、(b)" } ] } }, { "name": "text", "data": "所示。双光子吸收与上转换过程类似，都能激发出相同的高能量发光，但它是一个瞬时过程，不涉及在激发光子处存在吸收共振。如" }, { "name": "xref", "data": { "text": "图4(c)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(c)" } ] } }, { "name": "text", "data": "所示，在相似的激发能量密度下，用820 nm共振激发与1 064 nm非共振激发产生的上转换荧光强度的能量密度依赖性是截然不同的" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "69", "type": "bibr", "rid": "R69", "data": [ { "name": "text", "data": "69" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。而对于非共振 1 064 nm 激发情况，上转换产率与激发波长成二次方，这与双光子过程所预期的一样。更重要的是，即使在较低的能量下，820 nm 激发的相关性也近似线性数量级，低至1 mJ/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "。这说明上转换发光与双光子吸收过程完全不同，两者的横截面吸收存在明显差异。Yang等进一步通过泵浦探测实验发现，当探测能量密度超过约 400 mJ/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "时，探测到的上转换发射明显增加；低于该阈值，探测贡献很小，如" }, { "name": "xref", "data": { "text": "图4(d)", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4(d)" } ] } }, { "name": "text", "data": "所示" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "69", "type": "bibr", "rid": "R69", "data": [ { "name": "text", "data": "69" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。考虑到与谐振激发功率相比，非共振激发贡献仅在400 mJ/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "时才变得显著，并且由于空穴的带内吸收在这两个波长之间预计不会有如此显著的差异，他们认为820 nm 处激发主导上转换的发光机制，可能是通过在两个连续的带内吸收形成双激子后，发生俄歇复合上转换。" } ] }, { "name": "fig", "data": { "id": "F4", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图4" } ], "title": [ { "name": "text", "data": "基于激发态吸收的上转换发光过程" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "69", "type": "bibr", "rid": "R69", "data": [ { "name": "text", "data": "69" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。(a)带内吸收上转换发光机理：带内吸收(过程1)生成的热空穴越过势垒(过程2)到达第二个量子点上；(b)俄歇复合上转换发光：俄歇复合(过程2)发生在第二个带内吸收(过程1)之后，产生的热空穴随后跃迁到第二个量子点上(过程3)；(c)不同激发波长下上转换发光强度的能量依赖特性；(d)上转换发光强度的泵浦依赖特性。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 4" } ], "title": [ { "name": "text", "data": "Two possible mechanisms that contribute to UC in double QDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "69", "type": "bibr", "rid": "R69", "data": [ { "name": "text", "data": "69" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (a)Direct intraband hole absorption mechanism of UC: a hot hole formed due to intraband absorption(1) crosses above the barrier to the second dot(2). (b)Auger-mediated UC: a second intraband absorption event(1) is followed by Auger recombination, leading to a formation of a hot hole(2), which then crosses above the barrier to the second dot(3). (c)Energy density dependence of 635 nm emission upon resonant(820 nm) excitation and nonresonant(1 064 nm) excitation. (d)Dependence of UC luminescence intensity on probe pulse energy for pump-probe measurement and probe-only measurement." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656946&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656955&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656949&type=" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "3.2" } ], "title": [ { "name": "text", "data": "声子辅助上转换发光量子点" } ], "level": "2", "id": "s3b" } }, { "name": "p", "data": [ { "name": "text", "data": "声子辅助上转换能够通过吸收声子(晶格振动)的方式发射出能量高于激发光的光子。其发光过程如" }, { "name": "xref", "data": { "text": "图5(a)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(a)" } ] } }, { "name": "text", "data": "所示，电子吸收入射光子能量(" }, { "name": "italic", "data": [ { "name": "text", "data": "hω" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "Exc" } ] }, { "name": "text", "data": ")和一个或多个声子能量(" }, { "name": "inlineformula", "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656959&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656968&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656962&type=" } } } ] }, { "name": "text", "data": ")后跃迁到一个真实的电子态能级| X" }, { "name": "text", "data": ">" }, { "name": "text", "data": "，之后辐射复合产生一个高能光子发射(" }, { "name": "italic", "data": [ { "name": "text", "data": "hω" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "Det" } ] }, { "name": "text", "data": " ≥ " }, { "name": "italic", "data": [ { "name": "text", "data": "hω" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "Exc" } ] }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "70", "type": "bibr", "rid": "R70", "data": [ { "name": "text", "data": "70" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。与双光子吸收或二次谐波等同时激发的上转换机理不同，声子辅助上转换所需的额外能量(Δ" }, { "name": "italic", "data": [ { "name": "text", "data": "E" } ] }, { "name": "text", "data": "=" }, { "name": "italic", "data": [ { "name": "text", "data": "hω" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "Det" } ] }, { "name": "text", "data": "-" }, { "name": "italic", "data": [ { "name": "text", "data": "hω" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "Exc" } ] }, { "name": "text", "data": ")主要来源于由晶格振动产生的热能(声子)。声子辅助上转换在多种材料中都已被发现，如稀土掺杂纳米颗粒、有机染料、碳纳米管、半导体纳米带、半导体量子点以及钙钛矿等等" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "," }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "71", "type": "bibr", "rid": "R71", "data": [ { "name": "text", "data": "71" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "73", "type": "bibr", "rid": "R73", "data": [ { "name": "text", "data": "73" } ] } } ], "rid": [ "R71", "R72", "R73" ], "text": "71-73", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。如" }, { "name": "xref", "data": { "text": "图5(b)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(b)" } ] } }, { "name": "text", "data": "所示，Aguila等在钙钛矿量子点中发现了上转换发光现象" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "70", "type": "bibr", "rid": "R70", "data": [ { "name": "text", "data": "70" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，当用高能激光(2.71 eV)和低于发光中心的能量(2.33,2.20,1.96 eV)激发钙钛矿量子点时，可以观测到极强的上转换发光峰。进一步通过光谱分析，以及强度和温度依赖的光谱研究证实了钙钛矿量子点中的上转换发光是通过声子辅助完成的。" } ] }, { "name": "fig", "data": { "id": "F5", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图5" } ], "title": [ { "name": "text", "data": "声子辅助上转换发光。(a)声子辅助上转换发光机理" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "70", "type": "bibr", "rid": "R70", "data": [ { "name": "text", "data": "70" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(b)CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "量子点在不同能量激发下的上转换发光光谱" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "70", "type": "bibr", "rid": "R70", "data": [ { "name": "text", "data": "70" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(c)基于缺陷能级的声子辅助上转换发光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(d)PbS/CdS/ZnS 量子点的上转换发光与激发光谱" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(e)CdSe量子点在不同激发波长下的飞秒荧光光谱" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(f)CdSe量子点的上转换单分子荧光光谱" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 5" } ], "title": [ { "name": "text", "data": "Phonon-assisted UC photoluminescence. (a)Schematic diagram for phonon-assisted UC photoluminescence" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "70", "type": "bibr", "rid": "R70", "data": [ { "name": "text", "data": "70" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (b)Normalized room-temperature UC photoluminescence spectra of CsPbBr" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": " NCs under different excitation energies" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "70", "type": "bibr", "rid": "R70", "data": [ { "name": "text", "data": "70" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (c)Schematic diagram of phonon-assisted single photon UC photoluminescence of PbS/CdS/ZnS QDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (d)UC luminescent spectra of PbS, PbS/CdS, and PbS/CdS/ZnS QDs excited by a 980 nm laser and the UC luminescent excitation spectrum" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (e)Normalized femtosecond-resolved photoluminescence spectra monitored at 630 nm under different excitation wavelengths" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (f)Normalized UC photoluminescence and down-conversion photoluminescence spectra of a typical single CdSe QD" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656974&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656983&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656980&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "量子点的上转换发光可以借助于能带中的缺陷能级实现，" }, { "name": "xref", "data": { "text": "图5(c)、(d)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(c)、(d)" } ] } }, { "name": "text", "data": "所示为基于PbS/CdS/ZnS核壳量子点的上转换发光，在长波长近红外光的激发下，价带中的电子先被激发到PbS量子点的导带，再通过耦合声子到达带内的缺陷能级，从而实现上转换。在980 nm的近红外光激发下，PbS/CdS/ZnS量子点在820 nm处展现出良好的上转换发光，上转换发光效率可达4.6%(100 mW/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。最近，浙江大学Ye等发现，在几乎没有缺陷的核壳结构量子点中上转换发光能够高效地进行，并且其上转换荧光量子产率与下转换一致，均接近100%" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。进一步研究表明，通过超快荧光光谱测得量子点上转换过程的时间常数" }, { "name": "text", "data": "<" }, { "name": "text", "data": "200 fs，远快于一般的辐射复合以及缺陷捕获速率，如" }, { "name": "xref", "data": { "text": "图5(e)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(e)" } ] } }, { "name": "text", "data": "所示。量子点的上、下转换的发光性质在集合体和单颗粒水平上都是完全一致的，如" }, { "name": "xref", "data": { "text": "图5(f)", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5(f)" } ] } }, { "name": "text", "data": "所示，这说明上、下转换拥有相同的电声子耦合电子态。因此，研究人员认为高效的上转换发光主要来源于声子辅助，无需借助缺陷能级来实现，并提出了基于本征电声子耦合能级的上转换发光机制。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "3.3" } ], "title": [ { "name": "text", "data": "量子点敏化TTA上转换发光" } ], "level": "2", "id": "s3c" } }, { "name": "p", "data": [ { "name": "text", "data": "相比于有机生色团来说，无机半导体量子点更加稳定，且其吸收光谱可从可见波段调节到近红外波段，非常适宜作为光子吸收体" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "21", "type": "bibr", "rid": "R21", "data": [ { "name": "text", "data": "21" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "25", "type": "bibr", "rid": "R25", "data": [ { "name": "text", "data": "25" } ] } } ], "rid": [ "R21", "R22", "R23", "R24", "R25" ], "text": "21-25", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。此外，有机分子通过单线态裂分产生的三重态激子与量子点之间可以实现能量相互转移(" }, { "name": "xref", "data": { "text": "图6(a)", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6(a)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "74", "type": "bibr", "rid": "R74", "data": [ { "name": "text", "data": "74" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，量子点可以作为TTA上转换发光过程中的敏化剂" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "75", "type": "bibr", "rid": "R75", "data": [ { "name": "text", "data": "75" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。量子点敏化上转换发光系统通常由三部分组成：量子点光子吸收敏化剂、量子点表面介质、发光染料分子。由于量子点表面配体通常采用脂肪组长链分子来提供胶体稳定性并钝化表面缺陷，因此在溶液中想要实现从量子点到发光体的三重态能量转移几乎是不可能的。量子点的表面介质的使用可以有效地增加短程三重态能量传递的速率和效率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "76", "type": "bibr", "rid": "R76", "data": [ { "name": "text", "data": "76" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。上转换发生过程如" }, { "name": "xref", "data": { "text": "图6(b)", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6(b)" } ] } }, { "name": "text", "data": "所示，PbS量子点吸收近红外光产生激子，在室温下激子具有单线态和三重态的特性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "77", "type": "bibr", "rid": "R77", "data": [ { "name": "text", "data": "77" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。5-羧酸并四苯(5-CT)介质的存在使量子点与介质之间的三重态能量传递成为可能(TET1)，随后介质通过第二步三重态能量传递(TET2)将三重态激发态能量传导到红荧烯发光体上，进而通过红荧烯分子间的三重态湮灭过程实现上转换的发光过程。" } ] }, { "name": "fig", "data": { "id": "F6", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图6" } ], "title": [ { "name": "text", "data": "量子点TTA上转换发光。(a)并四苯与量子点之间的单线态三线态能量传递" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "74", "type": "bibr", "rid": "R74", "data": [ { "name": "text", "data": "74" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(b)TTA上转换发光体系：量子点(PbS)/介质(5-CT)/发光体(rubrene)" }, { "name": "sup", "data": [ { "name": "text", "data": " [" }, { "name": "xref", "data": { "text": "77", "type": "bibr", "rid": "R77", "data": [ { "name": "text", "data": "77" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": " ;(c)利用空穴路径改变策略提高量子点敏化TTA上转换发光效率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "85", "type": "bibr", "rid": "R85", "data": [ { "name": "text", "data": "85" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": " ;(d)基于Si量子点的上转换发光过程" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "86", "type": "bibr", "rid": "R86", "data": [ { "name": "text", "data": "86" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": " ;(e)基于钙钛矿量子点体系的TTA上转换发光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "89", "type": "bibr", "rid": "R89", "data": [ { "name": "text", "data": "89" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": " ;(f)基于PbS量子点TTA上转换的固态装置示意图" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "95", "type": "bibr", "rid": "R95", "data": [ { "name": "text", "data": "95" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 6" } ], "title": [ { "name": "text", "data": " TTA UC sensitized by colloidal QDs. (a)Singlet excitons in tetracene first undergo singlet fission then triplet transfer to the nanocrystal" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "74", "type": "bibr", "rid": "R74", "data": [ { "name": "text", "data": "74" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (b)Schematic of the QD(PbS)/mediator(5-CT)/emitter(rubrene) photon upconversion system" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "77", "type": "bibr", "rid": "R77", "data": [ { "name": "text", "data": "77" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (c)Electronic-doped QDs sensitized TTA-UC by using hole rerouting strategy" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "85", "type": "bibr", "rid": "R85", "data": [ { "name": "text", "data": "85" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (d)Schematic of photon UC based on Si QDs" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "86", "type": "bibr", "rid": "R86", "data": [ { "name": "text", "data": "86" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (e)Scheme for TTA-UC sensitized by inorganic perovskite nanocrystals" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "89", "type": "bibr", "rid": "R89", "data": [ { "name": "text", "data": "89" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (f)Solid-state device structures of TTA UC" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "95", "type": "bibr", "rid": "R95", "data": [ { "name": "text", "data": "95" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656990&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656999&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25656995&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "利用胶体量子点作为TTA上转换发光过程中的敏化剂最早是由加州大学滨河分校的Huang等报道，他们分别利用CdSe/9-ACA/DPA(9,10-DPA,9,10-二苯基蒽)体系和PbSe/RUB(RUB，红荧烯)体系实现了可见光和近红外光的上转换" }, { "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": "。随后又有相当多的工作通过改变量子点的尺寸、形貌、配体、核壳结构、掺杂、表面介质等条件进一步改善上转换发光效率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "78", "type": "bibr", "rid": "R78", "data": [ { "name": "text", "data": "78" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "85", "type": "bibr", "rid": "R85", "data": [ { "name": "text", "data": "85" } ] } } ], "rid": [ "R78", "R79", "R80", "R81", "R82", "R83", "R84", "R85" ], "text": "78-85", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。如Ronchi等提出通过电子掺杂的策略引入能级高于9-蒽甲酸(9ACA)介质HOMO能级的中间带，可以有效地提升能量传递效率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "85", "type": "bibr", "rid": "R85", "data": [ { "name": "text", "data": "85" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。他们利用Au掺杂的CdSe量子点，得到了量子点激子与有机介质三重态之间接近100%的能量传递，最终实现了24%的上转换发光荧光量子产率(" }, { "name": "xref", "data": { "text": "图6(c)", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6(c)" } ] } }, { "name": "text", "data": ")。除了最常用的镉基、铅基量子点外，开发基于绿色环保型量子点的TTA上转换体系也在持续进行中" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "86", "type": "bibr", "rid": "R86", "data": [ { "name": "text", "data": "86" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "88", "type": "bibr", "rid": "R88", "data": [ { "name": "text", "data": "88" } ] } } ], "rid": [ "R86", "R87", "R88" ], "text": "86-88", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。如" }, { "name": "xref", "data": { "text": "图6(d)", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6(d)" } ] } }, { "name": "text", "data": "所示，Xia等利用硅量子点与有机发光体之间的自旋三线态激子传输，实现了上转换发光效率为7%的红光上转换，且该体系可以很好地掺入水溶性胶束中进行生物医用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "86", "type": "bibr", "rid": "R86", "data": [ { "name": "text", "data": "86" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。大连物化所Lai等报道了基于InP体系的量子点TTA绿色环保体系，其上转换效率接近10%" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "87", "type": "bibr", "rid": "R87", "data": [ { "name": "text", "data": "87" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。通过对无毒CuInS" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "上转换体系进行研究，Han等也发现自陷域激子的长寿命可以有效地提升量子点与基质之间的能量传递效率(高达92.3%)，从而提高荧光上转换发光量子产率(18.6%)" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "88", "type": "bibr", "rid": "R88", "data": [ { "name": "text", "data": "88" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。作为一种新兴的材料体系，钙钛矿具备极高的缺陷容忍度和载流子迁移率，这也使其成为TTA上转换光子吸收体的优选材料之一" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "89", "type": "bibr", "rid": "R89", "data": [ { "name": "text", "data": "89" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "92", "type": "bibr", "rid": "R92", "data": [ { "name": "text", "data": "92" } ] } } ], "rid": [ "R89", "R90", "R91", "R92" ], "text": "89-92", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。日本九州大学Mase等首次报道了基于钙钛矿量子点的TTA上转换体系(" }, { "name": "xref", "data": { "text": "图6(e)", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6(e)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "89", "type": "bibr", "rid": "R89", "data": [ { "name": "text", "data": "89" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，之后He等进一步利用具有量子效应的钙钛矿量子点实现了10%的上转换发光量子产率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "90", "type": "bibr", "rid": "R90", "data": [ { "name": "text", "data": "90" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。开发固态上转换发光材料体系对于太阳能电池和光电探测器集成应用具有重要意义。Wu等将有机发光分子热蒸镀到PbS量子点膜上" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "93", "type": "bibr", "rid": "R93", "data": [ { "name": "text", "data": "93" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，制备得到的固态装置在808 nm近红外光激发下可以实现1.2%的上转换发光效率。之后，他们又通过对器件结构的改进和量子点表面配体优化，使固态上转换效率达到了7%" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "94", "type": "bibr", "rid": "R94", "data": [ { "name": "text", "data": "94" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "95", "type": "bibr", "rid": "R95", "data": [ { "name": "text", "data": "95" } ] } } ], "rid": [ "R94", "R95" ], "text": "94-95", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "3.4" } ], "title": [ { "name": "text", "data": "量子点复合镧系上转换发光" } ], "level": "2", "id": "s3d" } }, { "name": "p", "data": [ { "name": "text", "data": "将量子点与镧系掺杂纳米晶复合可以实现上转换发光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "," }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "96", "type": "bibr", "rid": "R96", "data": [ { "name": "text", "data": "96" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "101", "type": "bibr", "rid": "R101", "data": [ { "name": "text", "data": "101" } ] } } ], "rid": [ "R96", "R97", "R98", "R99", "R100", "R101" ], "text": "96-101", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。福建物构所Zheng等利用稀土纳米晶到CsPb" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿量子点的辐射能量传递" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，首次实现了CsPb" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "量子点在低功率半导体激光器(" }, { "name": "text", "data": "<" }, { "name": "text", "data": "10" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": " W/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": ")激发下的高效(10" }, { "name": "sup", "data": [ { "name": "text", "data": "-3" } ] }, { "name": "text", "data": "~10" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "text", "data": ")上转换发光，如" }, { "name": "xref", "data": { "text": "图7(a)", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7(a)" } ] } }, { "name": "text", "data": "所示。通过稳态/瞬态上转换光谱和上转换发光绝对量子产率测试等手段，证明了稀土纳米晶/CsPb" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "量子点复合材料存在非常高效的辐射能量传递上转换(Radiative energy transfer upconversion,RETU)过程，其内转换(能量传递)效率接近100%，上转换发光效率在0.33%~0.45%范围内，接近纯镧系元素掺杂的纳米颗粒。比利时根特大学的Zeng等利用原位生长策略合成了量子点/镧系掺杂复合纳米颗粒" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "97", "type": "bibr", "rid": "R97", "data": [ { "name": "text", "data": "97" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，上转换镧系纳米晶与钙钛矿量子点之间的能量传递也接近100%，实现了复合材料有效的上转换发射。中科院长春应化所Du等利用种子生长法将CsPb" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "钙钛矿量子点成功修饰到上转换纳米颗粒(UCNPs)表面，得到的纳米复合材料在980 nm激光激发下产生可调的上转换发光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "98", "type": "bibr", "rid": "R98", "data": [ { "name": "text", "data": "98" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。他们认为非辐射荧光共振能量转移(Förster resonance energy transfer,FRET)和辐射光子再吸收(Photon reabsorption,PR)均参与了能量传递过程，使其能量传递效率接近100%，如" }, { "name": "xref", "data": { "text": "图7(b)", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7(b)" } ] } }, { "name": "text", "data": "所示。为了改善钙钛矿量子点/上转换纳米复合材料的稳定性，新加坡国立大学张勇团队采用中间过渡相的策略合成出了包覆立方相钙钛矿量子点的六方相镧系掺杂上转换纳米晶，所制备的复合纳米颗粒展现出了良好的水溶性和光稳定性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "98", "type": "bibr", "rid": "R98", "data": [ { "name": "text", "data": "98" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F7", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图7" } ], "title": [ { "name": "text", "data": "量子点复合镧系上转换发光。(a)基于辐射能量转移上转换过程的量子点/镧系掺杂纳米复合材料" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(b)基于辐射光子再吸收与非辐射能量共振转移共激发的量子点/镧系掺杂上转换纳米颗粒" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "97", "type": "bibr", "rid": "R97", "data": [ { "name": "text", "data": "97" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(c)980 nm激发下量子点/镧系掺杂纳米复合材料的上转换荧光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 7" } ], "title": [ { "name": "text", "data": "UC luminescence from QDs/lanthanide-doped hybrid nanocomposites. (a)Schematic representation of the radiative energy transfer upconversion processes in all-inorganic CsPb" }, { "name": "italic", "data": [ { "name": "text", "data": "X" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": " perovskite QDs through sensitization by lanthanide-doped nanoparticles" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (b)Schematic diagrams of energy levels for upconversion processes and the energy transfer mechanism radiative photon reabsorption(PR) and nonradiative Förster resonance energy transfer(FRET) processes in the excited at 980 nm" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "97", "type": "bibr", "rid": "R97", "data": [ { "name": "text", "data": "97" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (c)Photographs of QDs/lanthanide-doped hybrid nanocomposites UC luminescence under 980 nm illumination" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25657003&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25657012&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25657010&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "将量子点与稀土离子掺杂的纳米颗粒复合，得到的复合材料结合了稀土离子和量子点的发光优点，不仅可以在紫外激发下提供下转换发光，而且在近红外光激发下产生多色可调的上转换发光(" }, { "name": "xref", "data": { "text": "图7(c)", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7(c)" } ] } }, { "name": "text", "data": ")" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，弥补了稀土离子因能级分立而无法全光谱连续调控的不足。在这种体系中，光子上转换过程在镧系掺杂纳米颗粒中完成，量子点主要起光转换的作用。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "4" } ], "title": [ { "name": "text", "data": "上转换发光量子点应用" } ], "level": "1", "id": "s4" } }, { "name": "p", "data": [ { "name": "text", "data": "如前所述，上转换发光的典型光学特性是反斯托克斯发射和近红外可吸收，同时相比于镧系掺杂和TTA，量子点的上转换发光半峰宽很窄、色纯度极高。与此同时，量子点可以实现覆盖整个可见光区的可调窄带发射，使其在宽色域三维显示领域展示出巨大的潜力；上转换发光量子点在近红外区域具有高效的吸收，在太阳能利用领域呈现出潜在的应用价值；量子点的尺寸通常小于10 nm，这使其相比于镧系掺杂纳米颗粒更适宜用于生物成像与治疗领域。" } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "4.1" } ], "title": [ { "name": "text", "data": "照明与显示" } ], "level": "2", "id": "s4a" } }, { "name": "p", "data": [ { "name": "text", "data": "众所周知，光致发光和电致发光在我们的日常生活中起着极其重要的作用，特别是在信息的展示、获取和通讯方面。现阶段的发光装置通常是采用下转换发光，这就要求激发光能量要大于发射光子的能量。单单就照明而言，下转换发光就消耗了全球接近15%的电量，通过热耗散的形式造成了相当严重的能源损失。此外，热耗散还会缩短器件使用寿命，增加制造成本，造成全球温室效应，并存在严重的安全隐患。Ye等将量子点的上转换发光与电致发光结合起来，器件结构示意图如" }, { "name": "xref", "data": { "text": "图8(a)", "type": "fig", "rid": "F8", "data": [ { "name": "text", "data": "图8(a)" } ] } }, { "name": "text", "data": "所示" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。利用100 mW的商用AlGaInP红光二极管激发，封装在石英玻璃管中的量子点可以产生橘色上转换光发射，可以将电致发光的光谱宽度有效地向短波段拓宽了接近100%。进一步通过采用不同波长发光峰的上转换量子点，研究人员构建了具有高显色性(CRI" }, { "name": "text", "data": ">" }, { "name": "text", "data": "90)的高效白光照明光源，实现了接近连续的高显色性的白光光谱，能量转换效率可达104%。将上转换发光材料均匀分散在三维空间中，通过近红外光激发和三维调制，可以发出多种不同颜色的可见光，用裸眼即可直接观察到彩色三维图形，从而实现真正意义上的立体三维彩色显示" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "11", "type": "bibr", "rid": "R11", "data": [ { "name": "text", "data": "11" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。与稀土掺杂的纳米颗粒相比，半导体量子点的单峰发射使其色彩纯度更高，更适合应用于三维显示领域。Yang和Meir等通过简单的成膜方式" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "69", "type": "bibr", "rid": "R69", "data": [ { "name": "text", "data": "69" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "xref", "data": { "text": "2", "type": "bibr", "rid": "R2", "data": [ { "name": "text", "data": "2" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，实现了量子点的固态上转换发光，初步验证了上转换量子点在三维成像领域应用的可能性。" } ] }, { "name": "fig", "data": { "id": "F8", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图8" } ], "title": [ { "name": "text", "data": "上转换发光量子点应用。(a)上转换复合光源" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(b)上转换光电探测器" }, { "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": ";(c)上转换太阳能电池" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "66", "type": "bibr", "rid": "R66", "data": [ { "name": "text", "data": "66" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ";(d)上转换生物成像" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 8" } ], "title": [ { "name": "text", "data": "Applications of UC devices. (a)Schematic diagram for the hybrid light source" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "37", "type": "bibr", "rid": "R37", "data": [ { "name": "text", "data": "37" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (b)Infrared imaging using flexible UC devices" }, { "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": ". (c)Schematic of an UC solar cell" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "66", "type": "bibr", "rid": "R66", "data": [ { "name": "text", "data": "66" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": ". (d)Schematic diagram of low-power LED light excited UC bioimaging " }, { "name": "italic", "data": [ { "name": "text", "data": "in vivo" } ] }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25657020&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25657026&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=25657023&type=" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "4.2" } ], "title": [ { "name": "text", "data": "探测成像" } ], "level": "2", "id": "s4b" } }, { "name": "p", "data": [ { "name": "text", "data": "近红外光电探测与成像器件在信息通讯、军事、气象、生物检测等领域具有重要作用。传统的成像器件需要红外光电探测器与读出电路集成，复杂的集成工艺限制了红外成像系统的发展。通过频率上转换的方法将红外图像信息转换到可见光波段，然后采用性能优、价格低、制备工艺成熟的可见光波段硅基图像探测器采集信号，可以将红外光直接转化为可见光成像。红外上转换光电探测是解决红外图像探测的一种行之有效的方法，不但可以提升硅基探测器对红外光探测成像的响应特性，还有望拓展多种新功能器件" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "3", "type": "bibr", "rid": "R3", "data": [ { "name": "text", "data": "3" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "105", "type": "bibr", "rid": "R105", "data": [ { "name": "text", "data": "105" } ] } } ], "rid": [ "R3", "R4", "R5", "R6", "R7", "R8", "R9", "R10", "R11", "R12", "R13", "R14", "R15", "R16", "R17", "R18", "R19", "R20", "R21", "R22", "R23", "R24", "R25", "R26", "R27", "R28", "R29", "R30", "R31", "R32", "R33", "R34", "R35", "R36", "R37", "R38", "R39", "R40", "R41", "R42", "R43", "R44", "R45", "R46", "R47", "R48", "R49", "R50", "R51", "R52", "R53", "R54", "R55", "R56", "R57", "R58", "R59", "R60", "R61", "R62", "R63", "R64", "R65", "R66", "R67", "R68", "R69", "R70", "R71", "R72", "R73", "R74", "R75", "R76", "R77", "R78", "R79", "R80", "R81", "R82", "R83", "R84", "R85", "R86", "R87", "R88", "R89", "R90", "R91", "R92", "R93", "R94", "R95", "R96", "R97", "R98", "R99", "R100", "R101", "R102", "R103", "R104", "R105" ], "text": "3-105", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Yan等利用CdSe/NaYF" }, { "name": "sub", "data": [ { "name": "text", "data": "4" } ] }, { "name": "text", "data": "∶Yb,Er 复合上转换材料构筑的光电器件" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "101", "type": "bibr", "rid": "R101", "data": [ { "name": "text", "data": "101" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，在980 nm光照射下，探测到了明显的光电流信号。Zhou等以胶体量子点材料为基础，制备出一种新型、低成本、高探测率的红外上转换器件，如" }, { "name": "xref", "data": { "text": "图8(b)", "type": "fig", "rid": "F8", "data": [ { "name": "text", "data": "图8(b)" } ] } }, { "name": "text", "data": "所示" }, { "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": "。这种红外上转换器件的红外吸收层和可见光发射层均采用了量子点材料。基于这种胶体量子点的红外探测器外量子效率可以达到8000%，探测率达到6×10" }, { "name": "sup", "data": [ { "name": "text", "data": "12" } ] }, { "name": "text", "data": " Jones，响应速度在毫秒量级。进一步将这种高效率的红外光电探测器和胶体量子点发光二极管结合起来，制备了红外上转换器件，并获得了6.5%的光子转换效率。将该器件用于生物医学成像领域，在红外光照射下，研究人员可以清晰地分辨出正常组织和癌变组织，展现了红外上转换器件在生物成像领域良好的应用前景。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "4.3" } ], "title": [ { "name": "text", "data": "太阳能利用" } ], "level": "2", "id": "s4c" } }, { "name": "p", "data": [ { "name": "text", "data": "在太阳能利用领域，上转换过程可以将低于带隙能量的近红外光子转换成大于带隙能量的光子来最小化光伏器件中的非吸收能量损失，这种设计与反射层结合，可以有效地实现对近红外波段太阳能充分利用的目的，如" }, { "name": "xref", "data": { "text": "图8(c)", "type": "fig", "rid": "F8", "data": [ { "name": "text", "data": "图8(c)" } ] } }, { "name": "text", "data": "所示" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "66", "type": "bibr", "rid": "R66", "data": [ { "name": "text", "data": "66" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，上转换太阳能电池也是现阶段最有可能打破单节电池的Schockley-Queisser效率极限的方法之一。镧系掺杂的纳米晶和TTA上转换分子已经与光伏装置集成来提升光伏效率" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "106", "type": "bibr", "rid": "R106", "data": [ { "name": "text", "data": "106" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。但是，由于这些材料的上转换通常是基于离散的原子、离子或分子，在近红外光谱区域的吸收带非常窄，因此通过使用上转换进行太阳能收集依然非常困难且效率相当低。Milleville等通过对量子点能带进行调控，在等效太阳光能量的激发下实现了量子点的上转换发光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "61", "type": "bibr", "rid": "R61", "data": [ { "name": "text", "data": "61" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Sellers等用动力学速率模型预测了上转换量子点太阳能电池的工作效率，当上转换过程光子能量损失在1.3~1.75 eV之间时，他们用带隙在1.3~1.75 eV的上转换层构筑的太阳能电池，最高太阳能转换效率可以超过39%" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "107", "type": "bibr", "rid": "R107", "data": [ { "name": "text", "data": "107" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。这个相对恒定的太阳能转换效率范围是上转换量子效率和光子能量损耗之间权衡的结果，较高的上转换量子效率增加了低能量入射光子转化成高能光子的数量，但是增加光子能量损耗减少了上转换量子点层可以收集的低能量太阳能光子的数量。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "4.4" } ], "title": [ { "name": "text", "data": "生物成像" } ], "level": "2", "id": "s4d" } }, { "name": "p", "data": [ { "name": "text", "data": "众所周知，红区(600~700 nm)和近红外光谱范围(近红外一区700~900 nm，近红外二区1 000~1 700 nm)通常被称为生物组织的“光学窗口”，生物组织的光散射更低，活体成像效果更佳" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "108", "type": "bibr", "rid": "R108", "data": [ { "name": "text", "data": "108" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。因此，将激发和发射峰引入光学窗口，对体内生物成像具有重要的意义。上转换发光材料的激发光源为近红外光，因此具有较深的组织穿透力、无自发荧光背景、发射峰窄且在可见到近红外范围内可调、对生物组织几乎无损伤等优势。过去几十年中，镧系掺杂纳米颗粒突破了有机染料分子的许多限制，被广泛应用于生物成像、光动力治疗、光激活药物释放、荧光传感器和光遗传学等技术" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "10", "type": "bibr", "rid": "R10", "data": [ { "name": "text", "data": "10" } ] } }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "9", "type": "bibr", "rid": "R9", "data": [ { "name": "text", "data": "9" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "112", "type": "bibr", "rid": "R112", "data": [ { "name": "text", "data": "112" } ] } } ], "rid": [ "R9", "R10", "R11", "R12", "R13", "R14", "R15", "R16", "R17", "R18", "R19", "R20", "R21", "R22", "R23", "R24", "R25", "R26", "R27", "R28", "R29", "R30", "R31", "R32", "R33", "R34", "R35", "R36", "R37", "R38", "R39", "R40", "R41", "R42", "R43", "R44", "R45", "R46", "R47", "R48", "R49", "R50", "R51", "R52", "R53", "R54", "R55", "R56", "R57", "R58", "R59", "R60", "R61", "R62", "R63", "R64", "R65", "R66", "R67", "R68", "R69", "R70", "R71", "R72", "R73", "R74", "R75", "R76", "R77", "R78", "R79", "R80", "R81", "R82", "R83", "R84", "R85", "R86", "R87", "R88", "R89", "R90", "R91", "R92", "R93", "R94", "R95", "R96", "R97", "R98", "R99", "R100", "R101", "R102", "R103", "R104", "R105", "R106", "R107", "R108", "R109", "R110", "R111", "R112" ], "text": "9-112", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。然而，稀土掺杂上转换存在激发功率高、纳米颗粒尺寸大等缺点。近年来，量子点上转换在生物医用领域有了很大的进展。复旦大学李富友团队利用PbS/CdS/ZnS上转换发光量子点做体内成像探针，在980 nm光照射下，当激发强度为8 mW/cm" }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "时即可观测到极为明显的上转换近红外光发射，比镧系掺杂纳米颗粒小了一个数量级，如" }, { "name": "xref", "data": { "text": "图8(d)", "type": "fig", "rid": "F8", "data": [ { "name": "text", "data": "图8(d)" } ] } }, { "name": "text", "data": "所示" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。研究人员用低功率LED即可激发上转换光发射，实现体内不同组织的高效成像，且照射过程相比于激光照射几乎无明显的热产生，进一步说明了上转换量子点在低能量激发应用时的安全性。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "5" } ], "title": [ { "name": "text", "data": "结论与展望" } ], "level": "1", "id": "s5" } }, { "name": "p", "data": [ { "name": "text", "data": "在过去的十几年里，研究者们报道了大量的基于量子点材料的上转换发光体系，包括利用量子点可调发射特性的镧系掺杂复合体系、利用量子点宽吸收特性的TTA上转换、借助声子辅助的上转换发光量子点以及基于激发态吸收机理的半导体双量子点体系。量子点上转换在近红外区域具有较大的吸收系数，发射光谱可调谐且可以覆盖整个可见光和近红外区域。因此，依赖于可调的半导体量子点异质结构和光物理特性，上转换发光量子点表现出比其他上转换发光材料更大的应用潜力。尽管上转换发光量子点在近几年有了较大的进展，但是上转换的内在机制还尚未完全解释清楚，同时该领域的研究也存在一些亟待解决的问题和未来可以重点研究的方向：" } ] }, { "name": "p", "data": [ { "name": "text", "data": "(1)上转换发光效率。与镧系掺杂和TTA上转换发光体系相比，基于激发态吸收的量子点上转换发光效率依然很低，这主要是由于受激的热载流子在中间态能级的寿命不足所致(通常小于10 μs)。因此，如何提高量子点自身的中间态寿命，或通过表面等离子体共振、光子晶体等外部增强方式" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "11", "type": "bibr", "rid": "R11", "data": [ { "name": "text", "data": "11" } ] } }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "3", "type": "bibr", "rid": "R3", "data": [ { "name": "text", "data": "3" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "115", "type": "bibr", "rid": "R115", "data": [ { "name": "text", "data": "115" } ] } } ], "rid": [ "R3", "R4", "R5", "R6", "R7", "R8", "R9", "R10", "R11", "R12", "R13", "R14", "R15", "R16", "R17", "R18", "R19", "R20", "R21", "R22", "R23", "R24", "R25", "R26", "R27", "R28", "R29", "R30", "R31", "R32", "R33", "R34", "R35", "R36", "R37", "R38", "R39", "R40", "R41", "R42", "R43", "R44", "R45", "R46", "R47", "R48", "R49", "R50", "R51", "R52", "R53", "R54", "R55", "R56", "R57", "R58", "R59", "R60", "R61", "R62", "R63", "R64", "R65", "R66", "R67", "R68", "R69", "R70", "R71", "R72", "R73", "R74", "R75", "R76", "R77", "R78", "R79", "R80", "R81", "R82", "R83", "R84", "R85", "R86", "R87", "R88", "R89", "R90", "R91", "R92", "R93", "R94", "R95", "R96", "R97", "R98", "R99", "R100", "R101", "R102", "R103", "R104", "R105", "R106", "R107", "R108", "R109", "R110", "R111", "R112", "R113", "R114", "R115" ], "text": "3-115", "type": "bibr" } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，提升量子点的上转换发光效率，是上转换发光量子点进一步研究的重要科学问题之一。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "(2)生物医用上转换发光量子点。上转换发光材料用于生物成像、药物运输、光动力疗法等生命科学领域时，不仅要具有较小的尺寸、较高的上转换发光效率、形貌和发光颜色可控等条件，还要求有良好的水溶性、表面有与生物分子相偶联的活性基团。目前制备的上转换发光量子点表面多为疏水性基团，无法与生物分子偶联，还不能很好地满足生物医学应用的这些要求。因此需要对上转换发光量子点进行表面修饰，置换或者修饰量子点表面的有机配体，将量子点表面的配体改为亲水基团来提高量子点的水溶性和生物兼容性。此外，目前上转换发光的相关研究主要集中在近红外光激发可见光发射，如何实现近红外区域的上转换发射对于上转换发光研究特别是其在生物成像等领域的应用同样具有重要的意义。量子点在近红外发光区域的可选择性比较大，通过能带调控和组分调控，有望实现更加高效的上转换近红外发光。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "(3)固态上转换微纳集成。溶液状态下高性能上转换发光量子点的结构设计与制备已获得了相当大的突破。但是要想将上转换应用到太阳能电池、荧光聚光器、显示和传感等光电子领域，就必须实现上转换发光量子点与光电子器件的有效集成。其中，固态上转换发光的性能调制与机理探索是难点。虽然已有一些研究实现了量子点的固态上转换发光，然而其上转换效率依然很低，且相关机理研究仍不清晰。因此，如何实现高效固态上转换发光，并将其与光电子器件集成应用是上转换发光量子点研究的重点方向之一。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "总之，量子点作为一种全新的上转换发光材料，在宽光谱吸收和可调发射方面具有无可比拟的优势。相信不久的将来，上转换发光量子点必将在照明显示、生物医用、增强探测、太阳能光伏等领域扮演更重要的角色。" } ] }, { "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：http://cjl.lightpublishing.cn/thesisDetails#10.37188/CJL.20210394." } ] } ] } ], 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