锰离子掺杂纯无机钙钛矿纳米晶及应用 -

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锰离子掺杂纯无机钙钛矿纳米晶及应用

吉林大学化学学院超分子结构与材料国家重点实验室, 吉林长春 130012

基金项目:

中国国家重点研发计划2016YFB0401701

国家自然科学基金21773088

国家自然科学基金51425303

吉林大学科技创新研究团队2017TD-06

吉林省科技发展计划20190103024JH

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中图分类号:O631
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出版历程
- 收稿日期:2019-04-10
- 修回日期:2019-05-07
- 刊出日期:2019-10-01

Mn²⁺-doped CsPbX₃(X=Cl, Br and I) perovskite nanocrystals and their applications

doi:10.3788/CO.20191205.0933

State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun 130012, China

Funds:

the National Key Research and Development Program of China2016YFB0401701

National Natural Science Foundation of China21773088

National Natural Science Foundation of China51425303

JLU Science and Technology Innovative Research Team2017TD-06

the Jilin Province Science and Technology Research20190103024JH

More Information

Author Bio:
LIU Hui-wen (1993-), Ph.D.candidate, State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun.Her research interests are on the synthesis of perovskite nanocrystals and their applications in LEDs.E-mail:liuhuiwenjlu@163.com
ZHANG Hao (1976-), Professor, State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun.His research interests are on the synthesis and controllable self-assembly of photoelectric functional nanocrystals and polymer-based nanocomposites.E-mail:hao_zhang@jlu.edu.cn

Corresponding author:ZHANG Hao, E-mail:hao_zhang@jlu.edu.cn

摘要

摘要:胶体锰离子掺杂的纯无机钙钛矿纳米晶由于其优异的光电性质，使其作为一种新兴的荧光发射材料，被研究者们广泛研究。不仅如此，纯无机钙钛矿纳米晶的锰离子掺杂行为也揭示了由于掺杂过程和掺杂剂本身引起的新的光学性质。通过不同的合成方法和选择不同的锰前驱体可以实现不同的掺杂行为，以及由此引发不同的荧光性质。在高带隙钙钛矿主体中进行锰离子掺杂时，其中激发能量由钙钛矿主体转移到掺杂锰离子位点的d态，进而产生橙黄色d-d发射荧光。研究者们一直致力于理解锰离子掺杂过程并由此设计高效掺杂的纳米晶。这些锰离子掺杂的钙钛矿纳米晶由于具有独特的电子和光学特性使其在发光二极管和太阳能电池等应用中发挥了巨大的作用。结合之前的相关工作和进展，本综述重点总结了锰离子掺杂的纯无机钙钛矿纳米晶的合成方法、发光来源、发光机理和潜在应用的最新进展，并提出了未来潜在合理的研究方向。
- 钙钛矿/
- 荧光/
- 锰离子掺杂/
- 纯无机钙钛矿纳米晶
Abstract:Colloidal Mn ²⁺doped CsPbX ₃(X=Cl, Br, I) nanocrystals(NCs) are being explored extensively as alternative emitting materials, wherein highly efficient optical and optoelectronic processes can be achieved. Mn ²⁺doping in perovskite NCs also reveals several new fundamental aspects of doping and new dopant-induced optical properties through different methods of synthesis. Mn ²⁺doping exists in wide-band-gap perovskite hosts where the excitation energy is transferred to an Mn d-state, resulting in short-range tunable yellow-orange d-d emissions. Enormous efforts have been expended on understanding the doping process and designing highly efficient doped NCs. The unique electronic and fluorescent properties endow these Mn ²⁺doped perovskite NCs with various optoelectronic applications in light-emitting diodes(LEDs) and solar cells. Combining all these facts, this review focuses on the recent progress in synthesis methods, emission mechanism, and potential applications of Mn ²⁺doped CsPbX ₃perovskite NCs and provides an outline for plausible future studies.
- perovskite/
- fluorescence/
- Mn²⁺doped/
- CsPbX₃perovskite nanocrystals

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Figure 1.Summary of various synthesis methods for the synthesis of Mn²⁺-doped CsPbX₃NCs. (a)Sketch of the hot-injection method. (b)Scheme of LARP synthesis approach. (c)Room temperature post-synthesis method. (d)Microwave-assisted synthesis method. (e)Solvothermal synthesis method

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Figure 2.Summary of the selection of Mn sources for various synthesis methods of the Mn²⁺-doped CsPbX₃NCs. The most used MnCl₂(a) and (b)MnBr₂with the aid of HBr(c) MnAc₂with the aid of HCl(d) Mn-stearate(e) manganese acetate, manganese acetylacetonate, and manganese halides with the aid of benzoyl halide(f) as the Mn sources participated in the reaction

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Figure 3.(a) Sketch of 0D CsPbX₃QDs, (b) and (c)Mn²⁺-doped 0D CsPbX₃QDs, (d)sketch of 2D CsPbX₃NSs, (e) and (f)Mn²⁺-doped 2D CsPbX₃NSs or NPLs, (g-j) TEM images of NCs with different Mn²⁺substitution ratios(color version please see in the journal website)

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Figure 4.(a) The host CsPbX₃band gap and relative positions of Mn²⁺⁴T₁and⁶A₁states, (b)PDOS of CsPbCl₃, CsPb_0.875Mn_0.125Cl₃and CsPb_0.75Mn_0.25Cl₃, respectively, (c)the synthesis scheme of CsPb_xM_1-xBr₃NCs by triggering Cs₄PbBr₆NCs transformation with MnBr₂salts, (d-e)overview of enhanced stability in optical and structural properties of CsPb_xMn_1-xI₃NCs(color version please see in the journal website)

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Figure 5.(a) and (b) Mn²⁺-doped CsPbX₃NCs as color-converting materials for LEDs. (c)LEDs with white color emission. (d)Mn²⁺-doped CsPbBr₃NCs for electroluminescent LED devices. (e) and (f) Mn²⁺-doped CsPbX₃NCs for solar cells

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Table 1.Comparison of the performance parameters of PLEDs based on different Mn-substitution ratio

	V_on (V)	Max EQE(%)	Max.CE (cd·A^-1)	Max.PE (lm·W^-1)	Device structure
PLED-pure	3.6	0.81	3.71	0.70	ITO/poly-TPD orPVK/QDs/TPBI/LiF/Al
PLED-Mn2.6	3.5	0.95	4.33	0.72	ITO/poly-TPD orPVK/QDs/TPBI/LiF/Al
PLED-Mn3.8	4.2	1.49	6.41	1.14	ITO/poly-TPD orPVK/QDs/TPBI/LiF/Al

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Table 2.Comparison of the performance parameters of PSCs based on different CsPbBrI₂films

	J_sc(mA/cm²)	V_oc/V	FF/%	PCE/%	J_sc(EQE)(mA/cm²)
MnCl₂-0.5%	14.21	1.133	76.8	12.36	13.86
MnCl₂-1%	14.29	1.144	79.9	13.07	13.93
MnCl₂-2%	14.37	1.172	80.0	13.47	14.09

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Table 3.Key J-V parameters of PSCs with different coated layer thicknesses of CsPbCl₃:0.1Mn QDs

	QDs(mg/mL)	J_sc(mA/cm²)	V_oc/V	FF/%	PCE/%
CsPbCl₃-xMn	1	21.42	1.105	76.4	18.08
CsPbCl₃-xMn	5	22.03	1.105	76.3	18.57
CsPbCl₃-xMn	20	20.73	1.105	76.6	17.55

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