蓝光钙钛矿发光二极管：机遇与挑战

doi:10.3866/PKU.WHXB202009002

物理化学学报 >> 2021, Vol. 37 >> Issue (4): 2009002.doi: 10.3866/PKU.WHXB202009002

所属专题：金属卤化物钙钛矿光电材料和器件

蓝光钙钛矿发光二极管：机遇与挑战

邹广锐兴¹, 陈梓铭¹^,²^,*(), 黎振超¹, 叶轩立¹^,*()

¹ 华南理工大学材料科学与工程学院，发光材料与器件国家重点实验室，广州 510641
² 华南理工大学环境与能源学院，广州 510006

收稿日期:2020-09-01 录用日期:2020-10-04 发布日期:2020-10-22
通讯作者: 陈梓铭,叶轩立 E-mail:chenziming@scut.edu.cn;msangusyip@scut.edu.cn
作者简介:陈梓铭，1991出生，博士导师为华南理工大学的叶轩立教授，现为华南理工大学博士后。主要研究钙钛矿光电器件的研发(包括发光二极管与太阳电池)，器件物理与光物理的解析等
叶轩立，1979出生，博士导师为西雅图华盛顿大学的任广禹教授，现为华南理工大学教授。主要研究钙钛矿及有机光电子材料及器件的研发，新应用领域的开拓，以及商业化的转化等
基金资助:
国家自然科学基金(21761132001);国家自然科学基金(51573057);国家自然科学基金(91733302);中国博士后科学基金(2019M650197);中国博士后科学基金(2020T130204)

Blue Perovskite Light-Emitting Diodes: Opportunities and Challenges

Guangruixing Zou¹, Ziming Chen¹^,²^,*(), Zhenchao Li¹, Hin-Lap Yip¹^,*()

¹ School of Materials Science and Engineering, South China University of Technology, State Key Laboratory of Luminescent Materials and Devices, Guangzhou 510641, China
² School of Environment and Energy, South China University of Technology, Guangzhou 510006, China

Received:2020-09-01 Accepted:2020-10-04 Published:2020-10-22
Contact: Ziming Chen,Hin-Lap Yip E-mail:chenziming@scut.edu.cn;msangusyip@scut.edu.cn
About author:Email: msangusyip@scut.edu.cn (H.Y.)
Email: chenziming@scut.edu.cn (Z.C.)
Supported by:
the National Natural Science Foundation of China(21761132001);the National Natural Science Foundation of China(51573057);the National Natural Science Foundation of China(91733302);the China Postdoctoral Science Foundation(2019M650197);the China Postdoctoral Science Foundation(2020T130204)

摘要/Abstract

摘要：

金属卤化钙钛矿由于具有优异的光电性能(如：高电子/空穴迁移率，高荧光量子产率，高色纯度，以及光色可调性等)，成为应用于发光二极管(LED)的理想材料。近年来，钙钛矿LED的发展十分迅速，红光和绿光钙钛矿LED的外量子效率(EQE)均已超过20%。然而，蓝光(尤其是深蓝光)钙钛矿LED的EQE以及稳定性依然相对落后，这严重制约了钙钛矿LED在高性能、广色域显示领域和高显色指数白光照明领域的应用。因此，总结现阶段蓝光钙钛矿LED的发展，并剖析其机遇与挑战，对未来蓝光甚至整个钙钛矿LED领域的发展至关重要。本文将蓝光钙钛矿LED根据光色细分为天蓝光、纯蓝光、深蓝光三大部分进行总结，回顾了三种LED器件的发展历程，并详细阐述了现阶段实现他们的主要手段以及相关的基础原理，最后分析了它们各自的问题并提出了相应的解决思路。

关键词: 金属卤化钙钛矿, 发光二极管, 蓝光, 策略, 挑战

Abstract:

Metal halide perovskites are considered as promising candidates for lighting applications owing to their excellent optoelectronic properties, such as high electron/hole mobility, high photoluminescence quantum yield, high color purity, and facile color tunability. In recent years, perovskite light-emitting diodes (LEDs) have developed rapidly, and their external quantum efficiencies (EQEs) have exceeded 20% for green and red emissions. However, the EQEs and stabilities of blue (particularly deep-blue) perovskite LEDs are still inferior to the green and red counterparts, which severely restricts the application of perovskite LEDs in high-performance and wide color gamut displays as well as white light illumination. Therefore, summarizing the development of blue perovskite LEDs and discussing the opportunities and challenges associated with their future applications will help to guide the further development of the entire perovskite LED field. In this review, according to the emission color, we divide the blue perovskite LEDs into three parts for a better discussion, i.e., the emissions in the sky-blue, pure-blue, and deep-blue regions. We introduce their developed history and discuss the basic strategies to achieve blue emission. There are three typical methods to obtain perovskite emitters with blue emission, i.e., (1) composition engineering, (2) dimensional engineering, and (3) synthesis of perovskite nanocrystals and quantum dots. For composition engineering, changing ions in perovskite ABX₃ structure can easily tune the perovskite emission color, particularly while changing the anions in "X" position. Therefore, modulating the ratio between the X-site anions of Br^- and Cl^- can cause perovskites to emit blue photons ranging from 420 to 490 nm, which almost covers the entire blue spectrum. For dimensional engineering, perovskite materials can form a series of low-dimensional structures (layered structures) with the insertion of organic ligands between the perovskite frameworks. This type of low-dimensional perovskite material typically exhibits better lighting properties than those exhibited by its three-dimensional counterpart owing to its unique charge or energy transfer process of charge carriers. Blue perovskite nanocrystals and quantum dots with high photoluminescence quantum yields are excellent candidates for realizing high-performance pure-blue and deep-blue devices because they can easily incorporate Cl^- in their crystals, which is considerably limited in perovskite thin films owing to the poor solubility of inorganic chloride sources in polar solvents. Furthermore, we discuss several challenges associated with blue perovskite LEDs, such as the inferior device performance in the pure-blue and deep-blue regions, difficulty in hole injection, electroluminescence (EL) instability of mixed halide perovskite systems, and lagged operation lifetime, and introduce potential solutions accordingly. Note that the challenges faced by blue perovskite LEDs are also the opportunities for research in this area. Therefore, this review is of a great reference value for the next evolution of blue perovskite LEDs.

Key words: Metal halide perovskite, Light-emitting diode, Blue emission, Strategy, Challenge

MSC2000:

O649.4

邹广锐兴, 陈梓铭, 黎振超, 叶轩立. 蓝光钙钛矿发光二极管：机遇与挑战[J]. 物理化学学报, 2021, 37(4): 2009002.

Guangruixing Zou, Ziming Chen, Zhenchao Li, Hin-Lap Yip. Blue Perovskite Light-Emitting Diodes: Opportunities and Challenges[J]. Acta Phys. -Chim. Sin., 2021, 37(4): 2009002.

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	Perovskites	Device structure	Ref.
3D perovskites	MAPb(Br_1–xCl_x)₃	ITO/PEDOT:PSS/perovskite/PCBM/Ag	37
	Cs₁₀(MA_0.17FA_0.83)_(100-x)PbCl_1.5Br_1.5	ITO/ZnO/perovskite/α-NPD/MoO₃/Al	38
	(Cs/Rb/FA/PEA/K)Pb(Cl/Br)₃	ITO/LiF/perovskite/LiF/Bphen /LiF/Al	13
Quasi-2D perovskites	4-PBA₂(CsPbBr₃)_n-1PbBr₄	ITO/ZnO/PEIE/perovskite/TFB/MoO₃/Al	39
	POEA₂MA_n–1Pb_nBr_3n+1	ITO/PEDOT:PSS/perovskite/TPBi/Ba/Al	19
	PEA₂Cs_n-1Pb_n(Cl_xBr_1-x)_{3n +1}	ITO/PEDOT:PSS/perovskite/TPBi/LiF/Al	42
	(EA)₂MA_n–1Pb_nBr_3n+1	ITO/PEDOT:PSS/perovskite/TmPyPB/CsF/Al	95
	BA₂[MAPbX₃]PbX₄	ITO/PEDOT:PSS/perovskite/TmPyPB/LiF/Al	57
	BA₂Cs_n-1Pb_n(Br/Cl)_{3n +1}	ITO/PEDOT:PSS/PVK/perovskite/TPBi/Al	90
	NaBr:PEA-CsPb(Br_1-xCl_x)₃	ITO/NiO_x/PTAA/PVK/perovskite/TPBi/LiF/Al	51
	PBABr_y(Cs_0.7FA_0.3PbBr₃)	ITO/NiO/TFB/PVK/perovskite/TPBi/LiF/Al	45
Perovskite quantum dots	CsPb(Cl/Br)₃	ITO/PEDOT:PSS/PVK/perovskite/TPBi/LiF/Al	59
	CsPbBr_xCl_3–x	ITO/PEDOT:PSS/TFB:PFI/perovskite/TPBi/LiF/Al	64
	CsPbCl_xBr_3–x	ITO/PEDOT:PSS/Poly-TPD/perovskite/TPBi/LiF/Al	62
	CsPb(Br/Cl)₃	ITO/PEDOT:PSS/Poly-TPD/CBP/perovskite/B3PYMPM/LiF/Al	102
	CsPb(Br/Cl)₃	ITO/PEDOT:PSS/TFB/perovskite/TPBi/Liq/Al	82

	Perovskites	EL peak/nm	Max. EQE/%	Max. Luminance/(cd∙m-2)	Ref.
Three-dimensional perovskites	Cs₁₀(MA_0.17FA_0.83)_(100–x)PbCl_1.5Br_1.5	475	1.7	3567	38
	Cs_x(MA_0.17FA_0.83)_(100–x)Pb(Br_3–xCl_x)₃	475	2.58	6426	89
	MAPb(Br_1–xCl_x)₃	482	< 0.1	1.7	37
	(Cs/Rb/FA/PEA/K)Pb(Cl/Br)₃	484	2.01	4015	13
Quasi-2D perovskites	PEA₂(Rb_0.6Cs_0.4)₂Pb₃Br₁₀	475	1.35	100.6	93
	PEA₂Cs_n–1Pb_n(Cl_xBr_1–x)_3n+1	480	5.7	3780	42
	PEOA₂MA_n–1Pb_nBr_3n+1	480, 494	1.1	19.25	19
	PBABr_y(Cs_0.7FA_0.3PbBr₃)	483	9.5	~700	45
	(BA_xPEA_1-x)2Cs_n-1Pb_n(Br_0.7Cl_0.3)_3n+1	485	7.84	1130	91
	(EA)₂MA_{n –1}Pb_nBr_3n+1	485	2.6	200	95
	PEACl:CsPbCl_xBr_3-x:YCl₃	485	11	9040	43
	BA₂Cs_n-1Pb_n(Br/Cl)_{3n +1}	487	6.2	3340	90
	PBA₂(Cs/MA/FA)_n–1Pb_nBr_3n+1	487, 493	4.34, 5.08	643.8, 1151	49
	PEA_xPA_2-x(CsPbBr₃)_n-1PbBr₄	488	7.51	1765	104
	PEA₂(Cs_1-xEA_xPbBr₃)₂PbBr₄	488	12.1	2191	44
	NaBr:PEA-CsPb(Br_1–xCl_x)₃	488	11.7	2060	51
	(IPA/PEA)-(MA/Cs)PbBr₃	490	1.5	2480	41
	4-PBA₂(CsPbBr₃)_n–1PbBr₄	491	0.015	186	39
	GABr, PEABr-CsPbBr₃	492	8.2	1687	92
	PA₂(CsPbBr₃)_n-1PbBr₄	492	1.45	5737	94
Perovskite quantum dots	CsPbBr₃	477	1.96	86.95	96
	CsPbBr₃	479	12.3	/	6
	CsPbBr₃ (nanoplates)	480	0.1	25	31
	Rb_xCs_1–xPbBr₃	490	0.87	186	105
	CsPb(Br_1–xCl_x)₃	490	1.9	35	46
	CsPb(Br_1–xCl_x)₃	495	0.075	750	97
	CsPbBr_2.4Cl_0.6	495	1.13	2452	98

	Perovskites	EL peak/nm	Peak EQE/%	Luminance/(cd·m^-2)	Ref.
Three-dimensional perovskites	RbCl-CsPbBr₃	468	0.062	112	48
Quasi-2D perovskites	BA₂Cs_{n -1}Pb_n(Br/Cl)_3n+1	465	2.4	962	90
	P-PDA, PEACs_{n –1}Pb_nBr_3n+1	465	2.6	211	50
	PBA₂(Cs/MA/FA)_n–1Pb_nBr_3n+1	465	2.34	144.9	49
	(BA)₂(MA)₂Pb₃Br₇Cl₃	468	0.01	21	100
	POEA-CsPbBr_xCl_3-x	468	0.71	122.1	99
	PBABr_y(Cs_0.7FA_0.3PbBr₃)	474	4	–	45
Perovskite quantum dots	(Rb_0.33Cs_0.67)_0.42-FA_0.58PbBr_1.75Cl_1.25	466	0.61	39	52
	CsMn_yPb_1–yBr_xCl_3–x	466	2.12	245	36
	CsPbBr_xCl_3–x	469	0.5	111	64
	Ni²⁺-CsPbCl_xBr_3–x	470	2.4	612	53
	CsPbCl_xBr_3–x	470	0.07	350	83
	CsPbCl_xBr_3–x	470	2.15	507	67
	CsPbBr_xCl_3–x	470	6.3	465	54

	Perovskites	EL peak/nm	Peak EQE/%	Luminance/(cd·m^-2)	Ref.
Three-dimensional perovskites	MAPb(Br_1-xCl_x)₃	425, 450	–	–	55
Quasi-2D perovskites	2D n(MAPbBr₃), n = 1/3/5	432, 456	0.004, 0.024	1.2，8.5	101
	BA₂[MAPbX₃]PbX₄	440	0.0054	–	57
	POEA₂MA_n-1Pb_nBr_3n+1	462	0.06	1.26	19
Perovskite quantum dots	CsPbBr_1.5Cl_1.5	445	1.38	2673	98
	CsPb(Cl/Br)₃	455	0.07	742	59
	CsPb(Cl/Br)₃	456	1.1	43.2	82
	CsPbCl_xBr_3-x	460	1.35	33	62
	CsPbBr₃@CsPbBr_x	463	–	–	60
	CsPb(Cl/Br)₃	463	3.3	569	63
	CsPbBr₃	463	0.124	62	61
	CsPb(Br/Cl)₃	463	1.4	318	102
	Rb_xCs_1-xPbBr₃	464	0.11	71	105
	2D CsPbBr₃	464	0.057	38	103
Perovskite Variant	Cs₃Cu₂I₅	445	1.12	262.6	16

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蓝光钙钛矿发光二极管：机遇与挑战

Blue Perovskite Light-Emitting Diodes: Opportunities and Challenges

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