脉冲激光沉积制备卤化物钙钛矿薄膜研究进展

doi:10.15541/jim20250449

摘要/Abstract

摘要：

脉冲激光沉积(Pulsed Laser Deposition, PLD)是一种清洁且用途广泛的薄膜制备技术, 该方法可精确控制薄膜厚度、结晶取向并实现精确的化学计量比转移, 常用于制备各种复杂组分的功能薄膜材料。卤化物钙钛矿材料因其优异的光电特性而备受关注, 已在太阳能电池、光电探测器、发光二极管等领域取得巨大进展。然而, 传统多晶薄膜的高缺陷密度严重制约了器件性能的进一步提升。本文系统综述了利用PLD技术制备卤化物钙钛矿薄膜的最新研究进展, 重点探讨了如何通过外延生长策略克服多晶薄膜的固有缺陷并获得高质量薄膜及相关光电器件。首先, 概述了PLD的基本原理及其在钙钛矿多晶薄膜沉积中的工艺调控与器件应用, 随后聚焦于PLD外延生长单晶钙钛矿薄膜的前沿进展, 围绕晶格匹配、应力调控与低缺陷界面构筑等关键科学问题, 阐述了在不同衬底上实现高质量钙钛矿薄膜外延生长的策略及应用。最后, 分析了PLD在钙钛矿半导体薄膜光电集成、叠层电池及柔性器件等领域所面临的挑战与未来发展方向, 以期为相关研究提供一些帮助与指导。

关键词: 脉冲激光沉积, 卤化物钙钛矿薄膜, 外延生长, 光电器件, 综述

Abstract:

Pulsed laser deposition (PLD) is a clean and versatile technique for thin film fabrication. This method provides precise control over film thickness and crystalline orientation while ensuring accurate transfer of chemical stoichiometry. It is commonly used to fabricate various functional thin film materials with complex compositions. Halide perovskite materials have attracted significant attention due to their exceptional optoelectronic properties, leading to remarkable progress in applications such as solar cells, photodetectors, and light-emitting diodes. However, the high defect density in conventional polycrystalline perovskite films severely limits further improvements in device performance. This review systematically summarizes recent progress in preparing halide perovskite thin films via PLD, with a particular focus on epitaxial growth strategies designed to overcome the intrinsic limitations of polycrystalline films. First, the basic principles of PLD and their application in depositing polycrystalline perovskite films are outlined, including process control and device integration. Next, the article concentrates on advanced research in the epitaxial growth of single-crystal perovskite films using PLD. Key issues such as lattice matching, strain engineering, and the construction of low-defect interfaces are discussed, along with strategies for achieving high-quality epitaxy on various substrates. Finally, we analyze the challenges and future directions of PLD for applications in integrated optoelectronics, tandem solar cells, and flexible devices, with the aim of providing assistance and guidance for relevant researchers.

Key words: pulsed laser deposition, halide perovskite thin film, epitaxial growth, optoelectronic device, review

中图分类号:

TB43

曹丙强, 李兴牧, 魏浩铭, 单衍苏. 脉冲激光沉积制备卤化物钙钛矿薄膜研究进展[J]. 无机材料学报, 2026, 41(9): 1178-1192.

CAO Bingqiang, LI Xingmu, WEI Haoming, SHAN Yansu. Research Advances in the Preparation of Halide Perovskite Thin Films by Pulsed Laser Deposition[J]. Journal of Inorganic Materials, 2026, 41(9): 1178-1192.

图/表 12

图1 典型钙钛矿晶体结构示意图[16]

Fig. 1 Schematic diagrams of typical perovskite crystal structure[16] (a) Crystal structure of a 3D perovskite lattice; (b) Crystal structure of the cubic perovskite phase

图2 典型的钙钛矿薄膜制备方法[27-35]

Fig. 2 Typical preparation methods for perovskite thin films[27-35] (a) One-step spin-coating method[27]; (b) Two-step spin-coating method[28]; (c) Single-source and dual-source thermal evaporation methods[29-34]; (d) Chemical vapor deposition method[35]

图3 钙钛矿薄膜PLD示意图[36-38]

Fig. 3 Schematic diagrams of PLD of perovskite films[36-38]

图4 通过PLD“离轴”沉积MAPbI3薄膜, PLD与旋涂法结合制备MAPbI3薄膜及在纹理化硅片上生长的CsxFA1-xPbI3薄膜[41-43]

Fig. 4 Fabrication of MAPbI3 films via off-axis PLD, MAPbI3 films by hybrid PLD/spin-coating, and CsxFA1-xPbI3 films on textured silicon substrates[41-43] (a) Schematic illustration of the “off-axis” substrate arrangement in PLD[41]; (b) Schematic of the perovskite solar cell structure[41]; (c) J-V curves of the perovskite solar cell under forward and reverse scans[41]; (d) Schematic of the hybrid PLD and spin-coating method for MAPbI3 film fabrication[42]; (e) XRD patterns of MAPbI3 films prepared by the hybrid PLD method (blue) and conventional spin-coating (red)[42]; (f) SEM images of CsxFA1-xPbI3 films grown on textured silicon wafers at different laser frequencies[43]

图5 不同工艺参数下PLD生长的MAPbI3薄膜[49]

Fig. 5 MAPbI3 thin films grown by PLD with different parameters[49] (a) Schematic illustration of plume morphologies during PLD at different deposition pressures; (b) XRD patterns of films fabricated from targets with PbI2 to MAI ratios of 1 : 1, 1 : 6, and 1 : 8; (c) Cross-sectional SEM image of a glass/ITO/SnO2/PCBM device; (d) Conformal growth of MAPbI3 film on textured silicon substrate; (e) AFM images of films deposited with different laser spot sizes: RMS roughness of 33.9 nm (1.0 mm2), 18.7 nm (2.0 mm2), and 12.4 nm (2.5 mm2)

图6 垂直型MSM结构CsPbBr3薄膜光电探测器结构及性能[51]

Fig. 6 Structure and performance of a vertical MSM photodetector based on a CsPbBr3 thin film[51] (a) Schematic diagram of MSM-type CsPbBr3 thin film photodetectors with different structures; (b, c) Response time graph of planar/vertical MSM-type CsPbBr3 thin film photodetector; (d) Photocurrent and dark current graph of vertical/planar MSM-type CsPbBr3 thin film photodetector under 450 nm laser illumination; (e) Comparison of the device I-T curves for corresponding devices under a -20 V bias; (f) Simulated dark current curves of vertical structure CsPbBr3 thin film photodetectors under different interface defect state densities; (g) After adding a layer of NiOx, simulated I-V curves showing total current, electron current, and hole current for CsPbBr3/NiOx thin film devices; (h) After adding a layer of TiO2, simulated I-V curves showing total current, electron current, and hole current for CsPbBr3/TiO2 thin film devices

图7 通过CVD在STO(100)衬底上外延生长CsPbBr3(100)薄膜, CVD远程外延生长CsPbBr3薄膜[54-55]

Fig. 7 Epitaxial growth of CsPbBr3 (100) on STO (100) by CVD and remote epitaxial growth of CsPbBr3 via CVD[54-55] (a) Lattice matching between CsPbBr3 (100) and STO (100) crystallographic planes[54]; (b) Optical microscopy image of the CsPbBr3 film grown on the STO substrate[54]; (c) (110) pole figure of the 7 μm CsPbBr3 SCTF sample[54]; (d) Deposition process of the CsPbBr3 film (Amorphous carbon is deposited on NaCl via PLD, and then CsPbBr3 film is epitaxially grown on a-C/NaCl. The right inset shows a photograph of the as-grown CsPbBr3 film on a-C/NaCl)[55]; (e) X-ray φ scan of CsPbBr3 (224) and NaCl (224) reflections[55]; (f) SEM image of cross-sectional CsPbBr3/a-C/NaCl[55]; (g) HRTEM image of as-grown CsPbBr3 film. Inset shows corresponding fast Fourier transform results[55]

图8 MBE外延生长CsPbBr3薄膜[62]

Fig. 8 MBE epitaxial growth of CsPbBr3[62] (a, b) RHEED patterns collected on clean Si (111), and after the deposition of ~10 nm of CsPbBr3; (c) HAADF image and Pb, Br, and Cs EDX elemental maps of 300 nm CsPbBr3 MBE film grown on SiO2/Si (111) substrate; (d, e) Cross-sectional HAADF-STEM image and elemental maps of the CsPbBr3 MBE film; (f, g) SEM images of the epitaxial CsPbBr3 film. In (f) markers indicate the size of terraces and other surface features. In (g) the dashed circle and ellipse mark a small interstitial grain and a 1D structure, respectively

图9 通过PLD在晶格匹配的衬底上外延生长卤化物钙钛矿薄膜的示意图[73-74]

Fig. 9 Schematic diagram of the epitaxial growth of halide perovskite thin films on lattice-matched substrates via PLD[73-74]

表1 外延生长钙钛矿薄膜及相关器件文献总结[52,54-55,61-62,81-91]

Table 1 Literature survey of epitaxially grown perovskite thin films and related devices[52,54-55,61-62,81-91]

Preparation process	Material	Substrate	Mismatch ratio	Film property	Device structure; performance	Ref.
Spin coating	MAPbI₃	KCl	0.3%	Pseudomorphic epitaxy	KCl/MAPbI₃/Au; R: 20.7 A/W, D^*: 6.5×10¹³ Jones	[52]
Spin coating	α-FAPbI₃	MAPbCl_xBr_3-_x	6.3%	Incommensurate epitaxy	-	[81]
Spin coating	MAPbBr₃	MAPbBr₃ single-crystal	-	Homoepitaxial growth	-	[82]
CVD	CsPbBr₃	SrTiO₃	0.47%	Pseudomorphic epitaxy	STO/CsPbBr₃/Au	[54]
CVD	CsSnBr₃	NaCl	2.8%	Incommensurate epitaxy	-	[83]
CVD	CsPbBr₃	a-C/NaCl	-	Remote epitaxy	-	[55]
Magnetron sputtering	BaTiO₃	MgAl₂O₄/Si	2.37%	Incommensurate epitaxy	-	[84]
Magnetron sputtering	BiFeO₃	SrTiO₃	-	Incommensurate epitaxy	-	[85]
MBE	CsPbBr₃	Au	1.9%	Pseudomorphic epitaxy	-	[61]
MBE	CsSnBr₃	Au	0.9%	Pseudomorphic epitaxy	-	[61]
MBE	CsPbBr₃	Si	7%	Incommensurate epitaxy	-	[62]
PLD	α-MAPbI₃	KCl	0.16%-0.60%	Pseudomorphic epitaxy	-	[86]
PLD	CsPbBr₃	Si	6.8%	Incommensurate epitaxy	Al/p-Si/n-CsPbBr₃/Au; R: 780 mA/W, D^*: 2.41×10¹⁴ Jones	[87]
PLD	CsPbBr₃	SrTiO₃	0.12%	Pseudomorphic epitaxy	-	[88]
PLD	CsPbBr₃	Muscovite	-	Van der Waals epitaxy	Muscovite/CsPbBr₃/Au; D^*: 2.41×10¹⁴ Jones	[89]
PLD	Cs₂AgBiBr₆	SrTiO₃	3.9%	Incommensurate epitaxy	STO/Cs₂AgBiBr₆/Au; R: 1.2 A/W, D^*: 4.63×10¹² Jones	[90]
PLD	CsSnBr₃	Si	6.3%	Incommensurate epitaxy	Al/n-Si/p-CsSnBr₃/Au; R: 0.125 mA/W, D^*: 2.1×10⁹ Jones	[91]

图10 PLD生长CsPbBr3外延薄膜[87,89]

Fig. 10 Epitaxial growth of CsPbBr3 by PLD[87,89] (a) Schematic illustration of the epitaxial CsPbBr3 thin film on Si (100) substrate and the crystal lattice matching between CsPbBr3 and Si[87]; (b) XRD patterns of CsPbBr3 films grown on Si substrates at different temperatures[87]; (c, d) HAADF-STEM and iDPC-STEM images of the CsPbBr3/Si interface, revealing an interfacial transition layer of approximately 2 nm thickness[87]; (e) Cross-sectional SEM image of the CsPbBr3 film in false color[89]; (f) Photo of the CsPbBr3 photodetector[89]; (g) Responsivity and specific detectivity of the photodetector under various light intensity values[89]

图11 通过PLD生长CsSnBr3(100)、α-MAPbI3、Cs2AgBiBr6外延薄膜[86,90-91]

Fig. 11 Epitaxial thin films of CsSnBr3(100), α-MAPbI3, and Cs2AgBiBr6 grown by PLD[86,90-91] (a) Lattice matching between single-crystal Si (100) substrate and CsSnBr3 (100) epitaxial thin films[91]; (b) SEM image of CsSnBr3 on Si substrate[91]; (c) Schematic illustration of α-MAPbI3 epitaxy on KCl substrate[86]; (d) Specular XRD patterns of MAPbI3 films with different thicknesses on KCl substrate[86]; (e) Structural insights from X-ray reciprocal space mapping (RSM): left to right-RSM of bare KCl substrate (420) asymmetric plane (black arrow indicates substrate position), RSM of 70 nm-thick MAPbI3 film on KCl, and RSMs of 70 nm film along φ =90° ((240) reflection) and φ =180° ((420) reflection) directions, while the azimuthal direction represents φ, with a range of 0°-360°[86]; (f) Schematic diagram of the PLD epitaxial growth process of Cs2AgBiBr6 epitaxial films; (g) RSM pattern of the Cs2AgBiBr6 epitaxial film corresponding to the (100) direction[90]; (h) I-V curves of device at varying irradiation power densities[90]

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