金属离子掺杂提高全无机钙钛矿纳米晶发光性质的研究进展

于鹏; 曹盛; 曾若生; 邹炳锁; 赵家龙

doi:10.7498/aps.69.20200795

摘要

金属卤化物钙钛矿纳米晶由于其卓越的光电子性能, 在发光二极管、激光器、X射线成像、太阳能电池及光电探测等领域中受到了极大的关注. 与有机-无机杂化钙钛矿纳米晶相比, 全无机钙钛矿CsPbX₃(X = Cl, Br, I)纳米晶具有更优异的光电性能和更高的稳定性. 为进一步提高CsPbX₃纳米晶的光致发光量子效率和稳定性, 有研究已经着手调控纳米晶的微观结构, 减少作为非辐射复合中心的缺陷. 近年来, 在金属离子掺杂CsPbX₃纳米晶过程中, 发现不同种类和不同掺杂浓度的金属离子对其电子能带结构和光致发光性能有着巨大的影响, 基于金属离子掺杂取得了光致发光量子效率接近100%的CsPbX₃纳米晶. 本文综述了近年来在CsPbCl₃, CsPbBr₃, CsPbI₃和Mn²⁺掺杂CsPbX₃ (Mn²⁺:CsPbX₃)四种体系中通过金属离子掺杂提高全无机钙钛矿纳米晶光学性能的研究进展及其性能提升的物理机制. 此外, 提出了下一步还需要深入研究的一些问题和策略, 通过这些问题的深入研究, 希望能促使全无机钙钛矿纳米晶在各种光电器件中得到更广泛的应用.

关键词:

Abstract

Metal halide perovskite nanocrystals (NCs) have attracted great attention in the fields of light-emitting diodes, lasers, X-ray imaging, solar cells and photoelectric detectors due to their excellent optoelectronic properties. Compared with organic-inorganic hybrid perovskite NCs, all inorganic perovskite CsPbX₃ (X = Cl, Br, I) NCs have good photoelectric properties and high stability. To further improve the photoluminescence (PL) quantum yields (QYs) and stability of CsPbX₃ NCs, researchers reduced the defects as nonradiative recombination centers in NCs by the following strategies: 1) surface treatment with different ligands; 2) control of synthesis conditions with halide rich compounds; 3) doping of metal ions. Among them, metal doping is considered as a universal and effective way to adjust the optoelectronic properties of semiconductors. It is found that the type and the concentration of metal ions have great influence on the electronic band structure and PL performance of NCs after the metal ions have been doped into CsPbX₃ NCs. At the same time, compared with II-VI and III-V semiconductors, the unique structure of all inorganic perovskite NCs makes the doping of metal ions easier. Appropriate doping can not only enhance the intrinsic optical properties of the NCs without affecting their crystal structure, but also introduce new electronic energy levels into the NCs and new luminescent properties of doped metal ions. Based on metal ions doping strategy, the PLQYs of doped CsPbX₃ NCs have been enhanced to nearly 100%. In this work, we summarize recent advances in metal doping of the four typical kinds of perovskite NCs, including CsPbCl₃, CsPbBr₃, CsPbI₃, and Mn²⁺ doped CsPbX₃, and discuss the physical mechanisms of the improved properties through doping metal ions. It should be pointed out that the doping of some metal ions such as Ni²⁺ and Cd²⁺ into the above four kinds of NC systems can effectively passivate NC defects, thus improving the PL QY and stability of NCs. In addition, we put forward some personal perspectives on the future research subjects of interest and directions of metal doping for enhanced PL of CsPbX₃ NCs, which needs to be further explored in order to promote extensive application of perovskite NCs to various optoelectronic devices.

Keywords:

作者及机构信息

1.
广西大学物理科学与工程技术学院, 南宁　530004

2.
广西大学, 广西有色金属及特色材料加工重点实验室, 南宁　530004

通信作者: 曹盛, caosheng@gxu.edu.cn ; 赵家龙, zhaojl@ciomp.ac.cn

基金项目: 国家自然科学基金(批准号: 11774134)、广西八桂学者专项和广西高校引进海外高层次人才“百人计划”专项资助的课题

Authors and contacts

1.
School of Physical Science and Technology, Guangxi University, Nanning 530004, China

2.
Guangxi Key Laboratory of Processing for Non-Ferrous Metal and Featured Materials, Guangxi University, Nanning 530004, China

Corresponding author: Cao Sheng, caosheng@gxu.edu.cn ; Zhao Jia-Long, zhaojl@ciomp.ac.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 11774134), the Special Fund for “Guangxi Bagui Scholars”, China, and the “Guangxi Hundred-Talent Program”, China

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施引文献

图 1 纳米晶的形貌和晶体结构　(a)和(b)分别为Cu掺杂CsPbCl₃纳米晶前后的TEM图片, 插图为单个纳米晶的高分辨TEM图片^[49]; (c)为Cu掺杂CsPbCl₃纳米晶前后的XRD图谱^[49]

Fig. 1. Morphology and crystal structure of nanocrystals (NCs): (a), (b) TEM images of CsPbCl₃ and Cu doped CsPbCl₃ NCs, the inset shows high resolution TEM images of a single NC^[49]; (c) XRD patterns of CsPbCl₃ and Cu doped CsPbCl₃ NCs^[49].

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图 2 金属离子掺杂CsPbCl₃纳米晶的光学性能和晶体结构　(a) Cu掺杂CsPbCl₃纳米晶的吸收光谱和PL光谱^[49]; (b) BaCl₂掺杂CsPbCl₃纳米晶示意图^[50]; CdCl₂处理前后CsPbCl₃纳米晶的PL光谱(c)和PL衰减曲线(d), 图(c)的内插图为处理前后样品在紫外光激发下的数码照片^[52]; (e) Ni²⁺掺杂CsPbCl₃纳米晶的DFT计算掺杂能带结构和态密度图, 其中水平虚线表示费米能级^[53]

Fig. 2. Optical properties and crystal structure of metal ion doped CsPbCl₃ NCs. (a) Absorption and PL spectra of CsPbCl₃ and Cu-doped CsPbCl₃ NCs^[49]. (b) Schematic diagram of doping models for BaCl₂ doped CsPbCl₃^[50]. PL spectra (c) and PL decay curves (d) of CsPbCl₃ NCs before and after CdCl₂ treatment. The inset in panel (c) shows the photos of untreated and treated samples under a UV lamp^[52]. (e) Band structure and DOS of Ni²⁺:CsPbCl₃ by DFT calculation. The horizontal dotted line represents the Fermi level^[53]

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图 3 金属离子掺杂CsPbBr₃纳米晶的光学性能和晶体结构　(a) Sb³⁺掺杂CsPbBr₃示意图^[57]; (b) Ni²⁺掺杂CsPbBr₃纳米晶掺杂浓度与PLQY间的关系图^[59]; (c) Cu²⁺掺杂CsPbBr₃纳米晶掺杂浓度与PLQY之间的关系图^[60]; (d)和(e)分别为CsPbBr₃纳米在Cu²⁺掺杂前后能隙结构^[60]; (f) Mg²⁺掺杂CsPbCl₃, CsPbBr₃前后的PL谱及PLQY^[51]

Fig. 3. Optical properties and crystal structure of metal ion doped CsPbBr₃ NCs: (a) Schematic illustration of Sb³⁺ doped CsPbBr₃^[57]; (b) PLQY vs. Ni²⁺ doping concentration of CsPbBr₃ NCs^[59]; (c) PLQY vs. Cu²⁺ doping concentration of CsPbBr₃ NCs; electronic band structures before (d) and after (e) of Cu²⁺doped CsPbBr₃ NCs by DFT calculations^[60]; (f) PL spectra and PLQYs before and after Mg²⁺ doping of CsPbCl₃ and CsPbBr₃ NCs^[51]

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图 4 金属离子掺杂CsPbI₃纳米晶的光学性能　(a)不同Cu²⁺浓度的CsPbBrI₂纳米晶PLQY^[62]; (b)不同SrI₂掺杂浓度的CsPbI₃纳米晶PLQY随时间天数的变化^[63]; (c)不同Ni²⁺掺杂浓度的吸收和PL光谱^[64]; (d) Sb³⁺掺杂与(e)非掺杂CsPbI₃纳米晶薄膜PL强度随时间的变化^[65]; (f)不同Zn掺杂浓度下CsPbI₃纳米晶的吸收、PL光谱和PLQY^[66]

Fig. 4. Optical properties of metal ion doped CsPbI₃ NCs: (a) PLQY of CsPbBrI₂ NCs solution with different dopant concentration of Cu^2+[62]; (b) PLQY values as a function of aged days for unsubstituted and Sr²⁺-substituted CsPbI₃ NCs solutions^[63]; (c) absorption and PL spectra of as-synthesized Ni (II) doped CsPbI₃ NCs^[64]; successive PL spectra of Sb³⁺ doped (d) and undoped (e) CsPbI₃ NCs^[65]; (f) the absorption and PL peak maxima and PLQYs of CsPbI₃ NCs with different Zn-to-(Zn plus Pb) ratios^[66]

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图 5 Mn²⁺掺杂CsPbX₃纳米晶光学性能　(a) Mn²⁺掺杂前后CsPbCl₃纳米晶的PL光谱和UV光照下的数码照片^[67]; Mn²⁺掺杂CsPbCl₃纳米晶分别在340 K (b)和360 K (c)热处理下的PL强度及PL寿命随时间的变化^[69]

Fig. 5. Optical properties of Mn²⁺ doped CsPbI₃ NCs: (a) PL spectra and photographs under UV excitation of CsPbCl₃ NCs before and after Mn²⁺ doping^[67]; (b), (c) PL intensity and PL lifetime of Mn²⁺:CsPbCl₃ at different temperature (340 and 360 K) with different time^[69].

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图 6 金属离子和Mn²⁺掺杂CsPbX₃纳米晶的光学性能　(a) Mn²⁺:CsPbX₃纳米晶的PLQY与不同Ni/Pb比间的关系^[72];(b) CdCl₂溶液处理后Mn²⁺:CsPbX₃纳米晶的PL光谱和PL衰减曲线^[73]; (c) CdCl₂溶液处理后Mn²⁺:CsPbX₃纳米晶经过不同纯化次数在紫外激发下的数码照片^[73]

Fig. 6. Optical properties of CsPbX₃ NCs doped with metal ions and Mn²⁺: (a) PLQY of Mn²⁺ doped CsPbX₃ NCs vs. Ni/Pb ratios^[72]; (b) PL spectrum and PL decay curve of Mn²⁺ doped CsPbX₃ NCs after treatment with CdCl₂ solution^[73]; (c) digital photos of Mn²⁺ doped CsPbX₃ NCs before and after treatment with CdCl₂ solution under UV excitation with different purification times^[73].

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金属离子掺杂提高全无机钙钛矿纳米晶发光性质的研究进展