二维有机-无机杂化钙钛矿铁电材料的研究进展

doi:10.6023/A20080375

化学学报 ›› 2021, Vol. 79 ›› Issue (1): 23-35.DOI: 10.6023/A20080375 上一篇下一篇

综述

二维有机-无机杂化钙钛矿铁电材料的研究进展

徐豪杰^a^,^b, 韩世国^a^,^b, 孙志华^a^,^*(), 罗军华^a

a 中国科学院福建物质结构研究所福州 350002)
(
b 中国科学院大学北京 101408

投稿日期:2020-08-18 发布日期:2020-10-20
通讯作者: 孙志华

作者简介:

徐豪杰, 本科毕业于湖北大学材料科学与工程学院, 获学士学位. 目前就读于中国科学院福建物质结构研究所, 主要从事新型铁电材料的探索与性能研究.

韩世国, 2018年毕业于青岛大学物理科学学院, 获硕士学位. 目前在中国科学院福建物质结构研究所攻读博士学位. 当前的研究兴趣为新型光铁电体材料与光电应用探索.

孙志华, 中国科学院福建物质结构研究所研究员, 博士生导师. 主要从事极性光电功能材料的结构设计、化学合成与性能表征, 研究兴趣包括光敏铁电体、铁电半导体及材料的光电性能耦合与调控等.

罗军华, 中国科学院福建物质结构研究所研究员, 博士生导师, 上海科技大学特聘教授, 国家杰出青年基金获得者. 当前的主要研究方向为非中心对称结构的光电功能材料.

* E-mail: sunzhihua@fjirsm.ac.cn

基金资助:
国家自然科学基金(Nos. 21875251); 国家自然科学基金(21833010); 国家自然科学基金(21525104); 国家自然科学基金(21971238); 国家自然科学基金(21975258); 国家自然科学基金(61975207); 国家自然科学基金(21921001); 中科院基础前沿项目(ZDBS-LY-SLH024); 福建省自然科学基金(2018H0047); 中科院先导项目(XDB20010200)

Recent Advances of Two-dimensional Organic-Inorganic Hybrid Perovskite Ferroelectric Materials

Haojie Xu^a^,^b, Shiguo Han^a^,^b, Zhihua Sun^a^,^*(), Junhua Luo^a

a Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China)
(
b University of Chinese Academy of Sciences, Beijing 101408, China

Received:2020-08-18 Published:2020-10-20
Contact: Zhihua Sun
Supported by:
the National Natural Science Foundation of China(Nos. 21875251); the National Natural Science Foundation of China(21833010); the National Natural Science Foundation of China(21525104); the National Natural Science Foundation of China(21971238); the National Natural Science Foundation of China(21975258); the National Natural Science Foundation of China(61975207); the National Natural Science Foundation of China(21921001); the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences(ZDBS-LY-SLH024); the Natural Science Foundation of Fujian Province(2018H0047); the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB20010200)

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摘要/Abstract

铁电性通常是指电介质材料的自发极化取向随着外加电场发生变化的性能. 以自发极化为核心, 铁电材料表现出优异的介电响应、热释电性、压电性、电光效应和非线性光学效应等, 是一类具有广阔应用前景的功能材料. 近年来, 二维有机-无机杂化钙钛矿化合物在铁电研究领域崭露头角, 逐渐发展为铁电材料的重要组成部分. 此类材料具有独特的结构兼容性与可调控性, 能够实现多种功能的共存或耦合, 是发展新型多功能材料的理想体系. 本综述基于居里原理的对称性方法, 以铁电材料的结构相变为基础, 阐述了铁电体的晶体学对称性破缺现象. 具体结合二维有机-无机杂化钙钛矿铁电体的典型实例, 揭示材料铁电性能的结构来源及光电性能调控的潜在途径, 最后对该铁电材料体系的发展趋势和应用前景提出了展望.

关键词: 铁电体, 对称性破缺, 二维结构, 杂化钙钛矿, 光电性能

Ferroelectric materials, characterized by the reversible switching of spontaneous polarization by an applied electric field, exhibit excellent physical properties including dielectric response, pyroelectricity, piezoelectricity, electro-optics, and nonlinear optical effects, etc. All these physical properties have been widely used for diverse practical applications. In recent years, two-dimensional (2D) organic-inorganic hybrid perovskites have emerged as an important family of ferroelectrics. Benefitting from unique structural compatibility and tunability, this 2D class of ferroelectrics enable the coexistence and/or coupling of multiple functions, which become an ideal platform for the development of new multifunctional candidates. Based on the Curie symmetry principle, this work illuminates the crystallographic symmetry breaking and highlights the source of ferroelectricity in 2D hybrid perovskite ferroelectrics, as well as potential strategies to modulate their photoelectric properties. Finally, we propose the development trend and application prospects of these 2D hybrid perovskite ferroelectric materials.

Key words: ferroelectric, symmetry breaking, two-dimensional structure, hybrid perovskite, photoelectric property

引用此文

徐豪杰, 韩世国, 孙志华, 罗军华. 二维有机-无机杂化钙钛矿铁电材料的研究进展[J]. 化学学报, 2021, 79(1): 23-35.

Haojie Xu, Shiguo Han, Zhihua Sun, Junhua Luo. Recent Advances of Two-dimensional Organic-Inorganic Hybrid Perovskite Ferroelectric Materials[J]. Acta Chimica Sinica, 2021, 79(1): 23-35.

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图/表 17

三斜晶系	F1 (1)
单斜晶系	2 F1 (2/2); mF1 (2/2); 2/ mF1 (2); 2/ mFm (1); 2/ mF2 (1)
正交晶系	222 F1 (4/2); 222 F2 (1); mm2 F1 (4/2); mm2 Fm (2/2); mmmF1 (4); mmmFm (2); mmmFmm2 (1)
四方晶系	4 F1 (4/2); F1 (4/2); F2 (1); 4/ mF1 (4); 4/ mFm (2); 4/ mF4 (1); 422 F1 (8/2); 422 F2( s) (2); 422 F4 (1); 4 mmF1 (8/2); 4 mmFm (4/2); 2 mF1 (8/2); 2 mF2( s) (2); 2 mFm (4/2); 2 mFmm2 (1); 4/ mmmF1 (8); 4/ mmmFm( s) (4); 4/ mmmFm( p) (4); 4/ mmmFmm2( s) (2); 4/ mmmF4 mm (1)
三方晶系	3 F1 (3/2); F1 (3); F3 (1); 32 F1 (6/2); 32 F2 (3/2); 32 F3 (1); 3 mF1 (6/2); 3 mFm (3/2); mF1 (6); mF2 (3); mFm (3); mF3 m (1)
六方晶系	6 F1 (6/2); F1 (6/2); Fm (3/2); F3 (1); 6/ mF1 (6); 6/ mFm (3); 6/ mF6 (1); 622 F1 (12/2); 622 F2( s) (3); 622 F6 (1); 6 mmF1 (12/2); 6 mmFm (6/2); m2 F1 (12/2); m2 Fm( s) (6/2); m2 Fm( p) (6/2); m2 Fmm2 (3/2); m2 F3 m (1); 6/ mmmF1 (12); 6/ mmmFm( s) (6); 6/ mmmFm( p) (6); 6/ mmmFmm2( s) (3); 6/ mmmF6 mm (1)
立方晶系	23 F1 (12/2); 23 F2 (3); 23 F3 (4/2); mF1 (12); mFm (6); mFmm2 (3); mF3 (4); 432 F1 (24/2); 432 F2( s) (6); 432 F4 (3); 432 F3 (4); 3 mF1 (24/2); 3 mFm (12/2); 3 mFmm2 (3); 3 mF3 m (4/2); mmF1 (24); mmFm( s) (12); mmFm( p) (12); mmFmm2 (6); mmF4 mm (3); mmF3 m (4)

表1. 88种可能存在的铁电相变类型

Table 1. 88 species of potential paraelectric-to-ferroelectric phase transitions

图1. 有机阳离子层沿着<100>、<110>、<111>方向排布形成的二维层状钙钛矿结构类型

Figure 1. The organic cation layer is arranged along the <100>, <110>, and <111> directions to form a two-dimensional layered perovskite structure.

图2. (a)化合物1的铁电相结构和顺电相结构; (b)不同温度下的电滞回线; (c)介电性能随温度的变化趋势

Figure 2. (a) The ferroelectric phase and paraelectric phase structures of compound 1; (b) P-E hysteresis loops measured at different temperatures; (c) temperature dependence of the dielectric properties

图3. 化合物1的对称性破缺示意图

Figure 3. Schematic diagram of the symmetry breaking of compound 1

图4. (a)化合物2的铁电相和顺电相结构; (b)不同温度下 P-E电滞回线; (c)不同光照条件下的铁电体光伏效应

Figure 4. (a) The ferroelectric phase and paraelectric phase structures of compound 2; (b) P-E hysteresis loops collected at different temperatures; (c) ferroelectric photovoltaic effects under the different illumination intensities

图5. (a)化合物3的 R型和 S型晶体结构; (b)二阶非线性光学信号随温度的变化趋势; (c)紫外可见吸收光谱

Figure 5. (a) R-type and S-type crystal structures of compound 3; (b) variable-temperature second harmonic generation signals; (c) the ultraviolet-visible absorption spectra different type compounds

图6. (a)化合物4的铁电相结构和顺电相结构; (b)不同温度下测量 P-E电滞回线; (c)偏振光探测性能

Figure 6. (a) The ferroelectric phase and paraelectric phase structures of compound 4; (b) P-E hysteresis loop collected at different temperatures; (c) the polarized-light detection performance

图7. (a)化合物5的铁电相和顺电相结构; (b)不同温度下P-E电滞回线; (c)双光子吸收效应的开孔Z-扫描曲线

Figure 7. (a) The ferroelectric phase and paraelectric phase structures of compound 5; (b) P-E hysteresis loops measured at different temperatures; (c) the aperture Z-scan curve for two-photon absorption

图8. (a)化合物6的铁电相和顺电相结构; (b)不同温度下P-E电滞回线; (c)光电性能

Figure 8. (a) Ferroelectric phase and paraelectric phase structures of compound 6; (b) P-E hysteresis loops collected at different temperatures; (c) the photoelectric properties

图9. (a)化合物7的铁电相结构和顺电相结构; (b)不同温度下P-E电滞回线; (c)光电导响应性能

Figure 9. (a) Ferroelectric phase and paraelectric phase structures of compound 7; (b) P-E hysteresis loops collected at different temperatures; (c) the photoelectric properties

图10. (a)化合物8的铁电相结构和顺电相结构; (b)不同温度下P-E电滞回线; (c)自驱动光电探测性能

Figure 10. (a) The ferroelectric and paraelectric phase structures of compound 8; (b) P-E hysteresis loops measured at different temperatures; (c) self-powered photoelectric detection performance

图11. (a)化合物9的铁电相结构和顺电相结构; (b)沿着不同晶体学方向的P-E电滞回线; (c)铁电体光伏效应

Figure 11. (a) Ferroelectric phase and paraelectric phase structures of compound 9; (b) P-E hysteresis loops measured along the different crystal axes; (c) ferroelectric bulk photovoltaic effects

图12. (a)化合物10的铁电相结构和顺电相结构; (b)铁电相的P-E电滞回线; (c)反铁电相的P-E电滞回线

Figure 12. (a) The ferroelectric and paraelectric phase structures of compound 10; (b) the P-E hysteresis loops of the ferroelectric phase; (c) the P-E hysteresis loops of the antiferroelectric phase

图13. (a)化合物11在298 K、330 K和373 K温度下的晶体结构; (b)介电性能随温度的变化趋势; (c)压电力显微镜图像

Figure 13. (a) The crystal structures of compound 11 at 298 K, 330 K and 373 K; (b) the temperature dependence of dielectric properties; (c) piezoelectric force microscope image

图14. (a)化合物12的铁电相结构和顺电相结构; (b)P-E电滞回线; (c)室温下的Rashba效应

Figure 14. (a) Ferroelectric phase and paraelectric phase structures of compound 12; (b) P-E hysteresis loop; (c) the Rashba effect observed at room temperature

图15. (a)化合物13的铁电相结构和顺电相结构; (b)铁电相的P-E电滞回线与I-V曲线; (c) X-射线照射下的I-V曲线

Figure 15. (a) Ferroelectric phase and paraelectric phase structures of compound 13; (b) P-E hysteresis loop and I-V curve of ferroelectric phase; (c) I-V curve obtained under the X-ray irradiation

分类	材料组分		铁电相变类型	P _s/ (μC•cm ^–2)	E _g/eV	Ref.
A' ₂ MX ₄	(benzylammonium) ₂PbCl ₄	438	mmmFmm2	13	3.65	[25]
	(cyclohexylaminium) ₂ PbBr ₄	364	mmmFmm2	6.8	2.95	[28, 29]
	( n-butylammonium) ₂PbCl ₄	328	mmmFmm2	2.1		[3]
	[2-fluorobenzylammonium] ₂PbCl ₄	448	4/ mmmFmm2	5.35	3.62	[26]
	[ R-1-(4-chlorophenyl)ethylammonium] ₂PbI ₄ [ S-1-(4-chlorophenyl)ethylammonium] ₂PbI ₄	487 473.2	422 F1		2.34	[31]
	(4,4-difluorocyclohexylammonium) ₂PbI ₄	377	mmmFmm2	ca.4.5	2.38	[49]
	(4-aminotetrahydropyran) ₂PbBr ₄	503		5.36	3.12	[50]
	(4,4-difluoropiperidinium) ₂PbI ₄	428.5	4/ mmmFmm2	10.0	2.24	[51]
	(4,4-difluorohexahydroazepine) ₂PbI ₄	454	4?2 mF2	1.1	2.32	[52]
A' ₂ AM ₂ X ₇	( n-butylammonium) ₂CsPb ₂Br ₇	412	mmmFmm2	4.2	2.7	[35]
	( n-butylammonium) ₂(formamidinium)Pb ₂Br ₇	322	mmmFmm2	3.8	2.35	[33]
	( n-butylammonium) ₂(methylammonium)Pb ₂Br ₇	352	mmmFmm2	3.6	2.55	[32]
	(isobutylammonium) ₂CsPb ₂Br ₇	353	反铁电	ca.6.3		[53]
A' ₂ A ₂ M ₃ X ₁₀	( n-butylammonium) ₂(methylammonium) ₂Pb ₃Br ₁₀	315	mmmFmm2	2.9	2.41	[37]
	(ethylammonium) ₂(methylammonium) ₂Pb ₃Br ₁₀	375	4/ mmmFmm2	3.7	2.7	[38]
	(ethylammonium) ₄Pb ₃Cl ₁₀	415	4/ mmmFmm2	4.5	3.39	[54]
	( n-butylammonium ) ₂EA ₂Pb ₃Br ₁₀	380	4/ mmmFmm2	5	2.55	[55]
	(ethylammonium) ₄Pb ₃Br ₁₀	384	4/ mmmFmm2	3.5/5.9	2.7	[41]
	( n-butylammonium) ₂(ethylammonium) ₂Pb ₃I ₁₀	363	4/ mmmFmm2	5.6	1.9	[42]
	(allyammonium) ₂(ethylammonium) ₂Pb ₃Br ₁₀	378	4/ mmmFmm2		2.71	[56]
	( n-butylammonium) ₂(methylammonium) ₂Sn ₃Br ₁₀	318	mmmFmm2		2.22	[44]
其他	(4-(aminomethyl)piperidinium)PbI ₄	352	2/ mFm	9.8	2.38	[47]
	( R/ S-3-hydroxylquinuclidinium) ₄KCe(NO ₃) ₈	320	222 F2	4.1		[57]
	( n-propylammonium) ₂CsAgBiBr ₇	222	2/ mF2	1.5	2.25	[58]
	(chloropropylammonium) ₄AgBiBr ₈	305	mmmFm	3.2	2.69	[48]

分类	材料组分		铁电相变类型	P _s/ (μC•cm ^–2)	E _g/eV	Ref.
A' ₂ MX ₄	(benzylammonium) ₂PbCl ₄	438	mmmFmm2	13	3.65	[25]
	(cyclohexylaminium) ₂ PbBr ₄	364	mmmFmm2	6.8	2.95	[28, 29]
	( n-butylammonium) ₂PbCl ₄	328	mmmFmm2	2.1		[3]
	[2-fluorobenzylammonium] ₂PbCl ₄	448	4/ mmmFmm2	5.35	3.62	[26]
	[ R-1-(4-chlorophenyl)ethylammonium] ₂PbI ₄ [ S-1-(4-chlorophenyl)ethylammonium] ₂PbI ₄	487 473.2	422 F1		2.34	[31]
	(4,4-difluorocyclohexylammonium) ₂PbI ₄	377	mmmFmm2	ca.4.5	2.38	[49]
	(4-aminotetrahydropyran) ₂PbBr ₄	503		5.36	3.12	[50]
	(4,4-difluoropiperidinium) ₂PbI ₄	428.5	4/ mmmFmm2	10.0	2.24	[51]
	(4,4-difluorohexahydroazepine) ₂PbI ₄	454	4?2 mF2	1.1	2.32	[52]
A' ₂ AM ₂ X ₇	( n-butylammonium) ₂CsPb ₂Br ₇	412	mmmFmm2	4.2	2.7	[35]
	( n-butylammonium) ₂(formamidinium)Pb ₂Br ₇	322	mmmFmm2	3.8	2.35	[33]
	( n-butylammonium) ₂(methylammonium)Pb ₂Br ₇	352	mmmFmm2	3.6	2.55	[32]
	(isobutylammonium) ₂CsPb ₂Br ₇	353	反铁电	ca.6.3		[53]
A' ₂ A ₂ M ₃ X ₁₀	( n-butylammonium) ₂(methylammonium) ₂Pb ₃Br ₁₀	315	mmmFmm2	2.9	2.41	[37]
	(ethylammonium) ₂(methylammonium) ₂Pb ₃Br ₁₀	375	4/ mmmFmm2	3.7	2.7	[38]
	(ethylammonium) ₄Pb ₃Cl ₁₀	415	4/ mmmFmm2	4.5	3.39	[54]
	( n-butylammonium ) ₂EA ₂Pb ₃Br ₁₀	380	4/ mmmFmm2	5	2.55	[55]
	(ethylammonium) ₄Pb ₃Br ₁₀	384	4/ mmmFmm2	3.5/5.9	2.7	[41]
	( n-butylammonium) ₂(ethylammonium) ₂Pb ₃I ₁₀	363	4/ mmmFmm2	5.6	1.9	[42]
	(allyammonium) ₂(ethylammonium) ₂Pb ₃Br ₁₀	378	4/ mmmFmm2		2.71	[56]
	( n-butylammonium) ₂(methylammonium) ₂Sn ₃Br ₁₀	318	mmmFmm2		2.22	[44]
其他	(4-(aminomethyl)piperidinium)PbI ₄	352	2/ mFm	9.8	2.38	[47]
	( R/ S-3-hydroxylquinuclidinium) ₄KCe(NO ₃) ₈	320	222 F2	4.1		[57]
	( n-propylammonium) ₂CsAgBiBr ₇	222	2/ mF2	1.5	2.25	[58]
	(chloropropylammonium) ₄AgBiBr ₈	305	mmmFm	3.2	2.69	[48]

表2. 二维钙钛矿结构铁电化合物的基本性能

Table 2. Basic properties of two-dimensional perovskite structure ferroelectric compounds

表2. 二维钙钛矿结构铁电化合物的基本性能

Table 2. Basic properties of two-dimensional perovskite structure ferroelectric compounds

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二维有机-无机杂化钙钛矿铁电材料的研究进展

Recent Advances of Two-dimensional Organic-Inorganic Hybrid Perovskite Ferroelectric Materials

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