Recent Progress on Structural and Functional Evolutions of Metal Halide Perovskites under High Pressure
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摘要: 过去10年里，金属卤素钙钛矿作为一种性能优异的新型功能材料被广泛应用，其研究取得了很多重要进展。压力作为一个基本的热力学变量，可以显著地影响材料的微观结构、原子间相互作用、电子轨道和化学键，是调节材料结构和性能的一个强大工具。与此同时，压力也为研究结构与性质之间的关系提供了新路径。结合金刚石对顶砧高压装置以及原位高压表征技术，总结了金属卤素钙钛矿在高压下的结构及性质变化，包括高压驱动结构相变，有序-无序转变，非晶化，局部结构演化，带隙、光致发光、光响应、电阻等性质在压力作用下的变化，以及高压下特有的奇特性质如金属化转变，系统分析了此类材料的结构-性质关系，并对未来的新型材料设计做出了展望。Abstract: Over the past decade, metal halide perovskites have been widely employed as the emerging active-materials for technological innovations, and their research has become one of the central goals in the field of energetic materials. Pressure, a new thermodynamic dimension, can tune microstructure, atomic interactions, electronic orbitals, and chemical bonds of materials, thus serves as a potent means to regulate the structures and properties of metal halide perovskites. In addition, pressure paves a novel avenue for probing and understanding the structure-property relationship. Taking the advantage of diamond anvil cell technology and in situ high-pressure characterization techniques, we have comprehensively summarized the pressure-induced evolutions of metal halide perovskites, encompassing structural phase transitions, order-disorder transitions, amorphization, and local structural evolution. We have examined alterations in properties, such as bandgap, photoluminescence, photoelectronic response, and electrical resistance, and other distinctive high-pressure phenomena. This review systematically analyzes the structure-property interplay within these known materials, and offers insights into the design of future novel materials.
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Key words:
- high-pressure /
- metal halide perovskite /
- structural evolution /
- semiconductor /
- diamond anvil cell
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图 2 MHPVs中压力驱动的非晶化、有序-无序转变、局部无序：(a) MASnI3在压缩和再压缩时压力驱动的结构演化[25]，(b) Cs2AgBiBr6在2.1 GPa时隐藏的局部无序[36]
Figure 2. Pressure-driven amorphous, ordered-disordered transition, local disorder: (a) pressure-driven structural evolution of MASnI3 during compression and recompression in MHPVs[25];(b) Cs2AgBiBr6 local disorder at 2.1 GPa[36]
图 3 高压实验条件及时间对结构和性能的影响：(a)不同传压介质（pressure-transmitting-medium，PTM）下MAPbBr3在同一压力时的结构[15]；高压下MAPbCl3的结构(b)和性能(c)的时间依赖[14]
Figure 3. Effect of high-pressure experimental conditions and time on structure and performance: (a) the structure of MAPbBr3 at the same pressure under different pressure-transmitting-media[15]; time dependence of structure (b) and performance (c) of MAPbCl3 under high pressure[14]
图 4 (a)～(b) 结合中红外峰证明压力下的有序-无序转变[69]，其中，FWHM为半峰宽，d为晶面间距，d0为常压下的晶面间距
Figure 4. (a)−(b) order-disordered transitions under pressure demonstrated by FWHM and d/d0 and mid-infrared peaks，where FWHM represent full width at half maximum, d represents the interplanar spacing under the current pressure, and d0 represents the interplanar spacing under ambient[69]
图 5 带隙的压力依赖性：(a) 不同卤素钙钛矿中的带隙演化[11, 26, 31, 41, 42, 55, 63, 69, 76, 85, 89, 97, 105, 107]，(b) 压缩下Pb―I―Pb键的键长和键角的变化[68]
Figure 5. Pressure dependence of band gap：(a) band gap evolution in different halogen perovskites[11, 26, 31, 41, 42, 55, 63, 69, 76, 85, 89, 97, 105, 107]; (b) changes of bond length and bond angle of Pb―I―Pb bonds under compression[68]
图 6 不同MHPVs PL的压力依赖：(a) MAPbI1.2Br1.8[9]的PL谱，(b) (2meptH2)PbCl4钙钛矿的PL压力依赖和压力下的光学图像[43]，(c) Cs2AgBiCl6[96]的PL谱，(d)～(e)常温常压和高压下自捕获激子发射的演化示意图[96]，(f) CsPbBr3单晶的PL压力依赖[106]
Figure 6. Pressure dependence of different MHPVs PL: (a) MAPbI1.2Br1.8[9]; (b) pressure dependence of PL and optical image of (2meptH2)PbCl4[43]; (c) Cs2AgBiCl6[96]; (d)–(e) schematic diagram of the evolution of self-captured exciton emission under environmental conditions and high pressure[38];(f) pressure dependence of PL in CsPbBr3 single crystal[106];
图 7 (a) MAPbI3的压力依赖PL衰减动力学[11]，(b) MAPbI3靠近价带顶的缺陷态在压力下变浅[11]，(c) MAPbI3的弱间接带隙[120]，(d) α-FAPbI3的压力依赖PL衰减动力学[26]，(e) 不同压力下MAPbI3 MC的压力依赖PL衰减动力学[19]，(f) MAPbI3 MC平均PL寿命和PL强度的压力依赖[19]，(g) CsPbBr3 NCs载流子寿命和带隙的压力依赖[29]
Figure 7. (a) MAPbI3 pressure-dependent PL attenuation kinetics[11]; (b) pressure dependence of defect states in MAPbI3[11]; (c) weak indirect bandgap of MAPbI3[120]; (d) α-FAPbI3 pressure-dependent PL attenuation kinetics[26]; (e) pressure-dependent PL decay kinetics of MAPbI3 MC[19]; (f) pressure dependence of average PL lifetime and PL intensity of MAPbI3 MC[19]; (g) pressure dependence of carrier lifetime and bandgap in CsPbBr3 NCs[29]
图 8 压力驱动的不同MHPVs的光电性质的演化：(a)～(b) MAPbBr3[23]，(c)～(d) MASnI3[25]，(e)～(g) MAPbBr3多晶的电输运性能[126]，(h)～(i) Cs3Bi2I9的增强的光电流和宽带光响应[65]，(j) Cs2PbI2Cl2在2 GPa下的显著的光电流增强[44]，(k)压力促进的激子解离示意图[44]
Figure 8. Pressure-driven evolution of photoelectric properties of different MHPVs: (a)–(b) MAPbBr3[23]; (c)–(d)MASnI3[25];(e)–(g) electrical transport performance of MAPbBr3 polycrystalline [126]; (h)–(i) enhanced photocurrent and broadband light response of Cs3Bi2I9[65]; (j) significant photocurrent enhancement at 2 GPa for Cs2PbI2Cl2[44]; (k) schematic diagram of stress-facilitated exciton dissociation[44]
图 9 高压下MHPVs的金属化：(a)～(b) MAPbI3带隙的压力依赖[13]，(c) 高压下MAPbI3的红外反射光谱[13]，(d) 高压下MAPbI3的电导率的温度依赖[13]，(e) Cs2In(Ⅰ)In(Ⅲ)Cl6高压原位拉曼光谱[127]，(f) Cs2In(I)In(III)Cl6的压力依赖光吸收光谱[127]，(g)～(h) 压力下CD3ND3PbI3的红外吸收光谱[18]，(i) 72 GPa压力下CD3ND3PbI3的带隙为零[18]
Figure 9. MHPVs metallization under high pressure: (a)–(b) pressure dependence of the MAPbI3 bandgap[13]; (c) infrared reflectance spectrum of MAPbI3 at high pressure[13]; (d) temperature dependence of MAPbI3 conductivity at high pressure[13]; (e) high-pressure in situ Raman of Cs2In(Ⅰ)In(Ⅲ )Cl6[127]; (f) pressure-dependent light absorption spectra of Cs2In(Ⅰ)In(Ⅲ )Cl6[127];(g)–(h) CD3ND3PbI3 IR absorption spectra under pressure[18]; (i) CD3ND3PbI3 with zero bandgap at 72 GPa[18]
图 10 不同MHPVs的压致发光行为：(a)～(c) Cs4PbBr6 NCs从3.01 GPa开始表现出明显的光发射[119]，(d) Cs4PbBr6 NCs的与压力相关的色度坐标[119]，(e)～(f) (BA)4AgBiBr8在高压下的PL光谱[39]，(g) (BA)4AgBiBr8的PL位置和PL强度的压力依赖[39]，(h) (BA)4AgBiBr8在高压下的光学图像（PL随压力的增加而变化）[39]，(i)～(j) C4N2H14SnBr4的压力依赖PL光谱和与压力相关的色度坐标[114]
Figure 10. Pressed luminescence of different MHPVS：(a)–(c) Cs4PbBr6 nanocrystals begin to exhibit significant emission at high pressure of 3.01GPa[119]; (d) pressure-dependent chromaticity coordinates of Cs4PbBr6 nanocrystals[119] ; (e)–(f) PL spectroscopy of (BA)4AgBiBr8 at high pressure[39]; (g) pressure dependence of PL position and PL strength of (BA)4AgBiBr8[39]; (h) the optical pattern of (BA)4AgBiBr8 at high pressure shows that PL varies with increasing pressure[39]; (i)–(j) pressure dependent PL spectrum and pressure-dependent chromaticity coordinates of C4N2H14SnBr4[114]
表 1 金属卤化物钙钛矿的压力诱导相变
Table 1. Pressure-induced phase transitions of metal halide perovskite
Material Phase transitions Ref. MAPbBr3 Pm$ \overline 3 $m (ambient pressure)→Im$ \overline 3 $ (0.4 GPa)→Pnma (1.8 GPa) [23] MAPbI3 I4/mcm (ambient pressure)→Imm2 (0.26 GPa) [8] MAPbCl3 Pm$ \overline 3 $m (ambient pressure)→Pm$ \overline 3 $m (0.8 GPa)→Pnma (2.0 GPa) [12] CD3ND3PbI3 I4/mcm (ambient pressure)→Imm2 (1.30 GPa)→Imm (2.57 GPa) [18] MASnI3 P4mm (ambient pressure)→Pnma (0.7 GPa) [25] MAPbI1.2Br1.8 Pm$ \overline 3 $m (ambient pressure)→Im$ \overline 3 $ (2.7 GPa) [9] MASnCl3 Pc (ambient pressure)→P1 (1 GPa)→amorphization (above 3 GPa) [24] MA3Bi2Br9 P$ \overline 3 $m1 (ambient pressure)→P21/a (5 GPa) [64] FAPbBr3 Pm$ \overline 3 $m (ambient pressure)→Im$ \overline 3 $ (0.53 GPa)→Pnma (2.2 GPa) [90] FAPbI3 No phase transitions below 7 GPa [26] FAPbI3 NCs Pm$ \overline 3 $m (ambient pressure)→Im$ \overline 3 $(0.6 GPa) [27] α-FAPbI3 Pm$ \overline 3 $m→Imm2 (0.3 GPa), Imm2→Immm (1.7 GPa) [28] (C9NH20)6Pb3Br12 No phase transitions below 80 GPa [38] DABCuCl4 P21/a (ambient pressure)→P2 (6.4 GPa) [63] BA2PbI4 Pbca (ambient pressure)→P21/a (2 GPa) [22] MHy2PbBr4 Pmn21→P21 (near 4 GPa) [74] Cy4BiBr7 No phase transitions below 20.13 GPa [84] CsPbBr3 Isostructural phase transition (about 1.2 GPa) [29] CsPbBr3 Isostructural phase transition (1.2 GPa) [98] CsPbBr3 Pbnm (ambient pressure)→Pm3m (1.7 GPa) [33] RP-CsPbBr3 Pbnm (ambient pressure)→P21/m (0.74 GPa ) [33] CsPbI3 Pnma (ambient pressure)→P21/m (5.6 GPa) [30] Cs2SnBr6 No phase transitions below 20 GPa [34] Cs2AgBiBr6 Fm$ \overline 3 $m (ambient pressure)→I4/m (4.5 GPa) [99] Cs3Bi2I9 No phase transitions below 12.7 GPa [97] Cs3Bi2I9 No phase transitions below 20.3 GPa [93] Cs3Bi2Br9 P$ \overline 3 $m1 (ambient pressure)→C2/c (10.1 GPa) [37] Cs2AgBiCl6 Fm$ \overline 3 $m (ambient pressure)→I4/m (5.6 GPa) [96] Cs2PbI2Cl2 I4/mmm (ambient pressure)→C2/m (2.8 GPa) [44] 
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表 2 不同MHPVs的PL发生和消失压力
Table 2. Pressures corresponding PL occurrence and disappearance for different MHPVs
Material Dimension Initial pressure of PL/GPa PL annihilation pressure/GPa Ref. MAPbCl3 3D Ambient 7.20 [108] MAPbBr3 3D Ambient 4.85 [108] MAPbBr3 3D Ambient 4.00 [109] MAPbI3 3D Ambient 2.70 [10] MAPbI1.2Br1.8 3D Ambient 1.60 [9] CsPb2Br5 3D Ambient 2.23 [40] CsPbBr3 3D Ambient 2.40 [106] Cs2AgBiCl6 3D Ambient 8.00 [96] (BA)2PbI4 2D Ambient 10.00 [110] (BA)2PbI4 2D Ambient 12.60 [22] (PEA)2PbBr4 2D Ambient 15.60 [41] (PEA)2PbI4 2D Ambient 7.60 [111] (HA)2(GA)Pb2I7 2D Ambient 9.48 [112] (BA)2(MA)Pb2I7 2D Ambient 4.70 [69] (GA)(MA)2Pb2I7 2D Ambient 7.00 [46] (BA)4AgBiBr8 2D 2.50 25.00 [39] C4N2H14PbBr4 1D Ambient 9.00 [91] C4N2H14PbBr4 1D Ambient 24.81 [113] C4N2H14SnBr4 1D 2.06 20.02 [114] CH3(CH2)2NH3PbBr3 1D Ambient 7.30 [115] CsCu2I3 1D Ambient 16.00 [116] (bmpy)9[ZnBr4]2[Pb3Br11] 0D Ambient 18.20 [117] (bmpy)6[Pb3Br12] 0D Ambient >80 [38] (MA)3Bi2I9 0D Ambient 9.00 [118] Cs4PbBr6 0D 3.01 18.23 [119] Cs3Bi2I9 0D Ambient 9.30 [97]
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