Research Progress on Structure Dimensional Regulation of Metal Halide Perovskite Single Crystal and Their Direct-Type X-Ray Detection Performance

doi:10.16553/j.cnki.issn1000-985x.2025.0108

Abstract

Abstract: X-ray detection has a wide application in critical fields such as medical diagnostics， security screening， industrial non-destructive testing， and environmental monitoring. Metal halide perovskite single crystals have emerged as promising candidates for developing low-cost， high-performance X-ray detection systems due to their compositional tunability， strong X-ray attenuation coefficients， high carrier mobility-lifetime product， and low-temperature solution-processable growth. This review focuses on the crystal structure dimensional regulation of metal halide perovskite single crystal and their effect on X-ray detection performance，and summarizing recent advances in perovskite single crystal-based direct X-ray detectors. Through a detailed analysis of crystal growth methods， semiconductor properties， and X-ray detection performance across perovskites with various dimensionalities， this review unveils the intrinsic relationship between crystal structural dimensionality and photoelectronic detection capabilities. Based on these discussions， challenges currently faced by perovskite single crystal X-ray detectors are critically examined. Future research directions are proposed to guide the design and growth of large-size high-quality perovskite single crystals and the realization of stable， high-sensitivity X-ray detection systems. This review provides both theoretical insights and practical guidelines for advancing perovskite-based X-ray detection technologies toward practical applications.

Key words: metal halide perovskite; single crystal; structure dimensional regulation; X-ray detection

CLC Number:

O641

DAI Yizhi, MA Lin, ZHANG Wenjie, LEI Wenxuan, XIAO Wen, ZHANG Junqi, WANG Wenyu, ZHANG Jinxing, LIU Yucheng. Research Progress on Structure Dimensional Regulation of Metal Halide Perovskite Single Crystal and Their Direct-Type X-Ray Detection Performance[J]. Journal of Synthetic Crystals, 2025, 54(8): 1305-1329.

Figures/Tables 14

Fig.1 Schematic illustration of crystal structure for the metal halides perovskite with different dimensions. （a） 3D structure；（b） 2D structure；（c） 1D structure；（d） 0D structure

Fig.2 Basic principles of single crystal growth by solution method. （a） Schematic diagram of homogeneous and heterogeneous nucleation during supersaturation of a solution；（b） relationship between the free energy for homogeneous nucleation and particle radius

Fig.3 Basic principles and methods of growth for perovskite single crystal. （a）~（c） The principles and methods for maintaining solution at supersaturation state；（d） slow cooling crystallization growth method in hydrohalic acid aqueous solution；（e） temperature increasing reaction crystallization growth method in organic solution；（f） reverse solvent diffusion assisted crystallization growth method；（g） solvent slow evaporation growth method

Fig.4 Single crystal growth of 3D structured perovskite. （a） Crystal structure of 3D perovskite；（b） MAPbI3 single crystal grown by slow cooling crystallization in aqueous solution［32］；（c）~（d） MAPbI3 single crystal grown by slow cooling crystallization of top seed crystal aqueous solution growing method［33］；（e） MAPbI3 and MAPbBr3 single crystal grown by reverse solvent diffusion assisted crystallization growing method［34］；（f） MAPbI3 and MAPbBr3 single crystal grown by temperature increasing reaction crystallization growing method［36，39］

Fig.5 Single crystal growth of inorganic 3D perovskite CsPbBr3. （a） Growth of inorganic perovskite CsPbBr3 single crystal and CsPbCl3 single crystal by high-temperature Bridgman growth method；（b） growth of high-quality inorganic perovskite CsPbBr3 single crystal by atmosphere-controlled edge-defined film-fed growth （EFG） method［43］；（c） growth of inorganic perovskite CsPbBr3 single crystal by solution method［44-49］

Fig.6 Single crystal growth of 2D structured perovskite. （a） Crystal structure of 2D （PEA）2PbI4［51］；（b） schematic diagram of the anti-solvent vapor-assisted crystallization and anti-solvent vapor-assisted capping crystallization process， and the optical images of PEA2PbI4 crystals obtained by these methods［52］；（c） schematic diagram of the induced peripheral crystallization procedure to grow 2D （PEA）2PbI4 single-crystalline membrane［54］；（d） schematic diagram of the crystallization process at different temperatures and the images of FPEA2PbI4 crystals［56］；（e） photographs of （BA）2（MA） n-1Pb n I3n+1 single crystals［60］

Fig.7 Single crystal growth of 1D structured perovskite. （a） Crystallographic packing diagrams of （BAH）BiI4 viewed along the a-axis， power XRD pattern of the top facet of （BAH）BiI4 single crystal and the powder XRD pattern of （BAH）BiI4 water-soaking for 60 d［63］；（b） photograph， SEM-EDS mapping， measured and simulated XRD patterns of CsCu2I3 single crystals［64］；（c） procedure for crystal growth and the photograph of （TMHD）SbBr5 single crystal［65］；（d） schematic procedures diagrams for the grow of CsAg x Cu2-x I3 （0≤x≤2） single crystals［22］

Fig.8 Single crystal growth of 0D structured perovskite. （a） Crystal structure of 0D perovskite A3M2I9［67］；（b） photographs of the perovskite A3M2I9 single crystals［68］；（c） Cs3Bi2I9 single crystal and wafers［69］；（d） solvent evaporation crystallization method to grow Cs3Bi2I9 single crystals［70］；（e） nucleation-controlled method to grow Cs3Bi2I9 single crystals［73］；（f） vertical Bridgman growth method and photographs of Cs3Bi2Br9 single crystals［78］；（g） continuously supplying of pre-crystallized solution to grow 329-type single crystals［80］

Fig.9 Device structure of different X-ray detectors. （a） Photoconductor X-ray detector；（b） photodiode X-ray detector；（c） phototransistor X-ray detector

Fig.10 3D perovskite single crystal X-ray detectors. （a） Photograph of a perovskite FA0.85MA0.1Cs0.05PbI2.55Br0.45 single crystal， detector structure and X-ray detection performance［12］；（b） schematic illustration of MSM and p-i-n MAPbI3 single crystal devices， the curves of dark current with respect to electric field and the current density as a function of incident dose rate of the devices［87］；（c） schematic illustration of the metal halide perovskite single crystals with different heterointerfaces and their X-ray detection performance［24］；（d） schematic illustration of the critical temperature field heating strategy and the ferroelastic domain wall distribution before and after the critical temperature field heating with 700 μm thick MAPbI3 single crystal， μτ product and sensitivity of detectors based on MAPbI3 single crystals without domain walls［88］；（e） photographs of the yellow-phase FAPbI3 single crystal rods， the detector structure， X-ray detection sensitivity and imaging［89］

Fig.11 2D perovskite single crystal X-ray detectors. （a） The device structure of （FPEA）2PbI4 single crystal X-ray detector and corresponding X-ray detection performance［57］；（b） schematic diagram of device structure and working mechanism of 2D and 3D/2D/3D single crystal X-ray detectors， detection sensitivity of 2D and 3D/2D/3D single crystal detectors， and X-ray image measured by the 3D/2D/3D single crystal detector［27］；（c） photograph and structure of CsPb2Br5 single crystals， and their X-ray detection performance［93］；（d） crystal structure of Ge0.5Pb0.5X6 octahedra， photograph of （PEA）2Ge0.5Pb0.5I4 single crystal， corresponding X-ray detection sensitivity and X-ray imaging［61］

Fig.12 1D perovskite single crystal X-ray detectors. （a） Photoconductivity， X-ray response and sensitivity statistics of （BAH）BiI4 single crystal device［63］；（b） structure， photoconductivity and sensitivity of CsCu2I3 single crystal device［64］；（c） structure， photoconductivity and sensitivity of （TMHD）SbBr5 single crystal device［65］；（d） structure， X-ray response current density and dark current of （ATZ）（EA）4Pb3I11 single crystal device［66］

Fig.13 0D perovskite single crystal X-ray detectors. （a） Photographs of MA3Bi2I9 single crystals， structure and sensitivity of the detector［72］；（b） photographs of MA3Bi2I9 single crystal， sensitivity and detection limit of the detector［74］；（c） structure of AG3Bi2I9， X-ray response current and sensitivity of the detector［81］；（d） photographs of Cs3Bi2I8Br and Cs3Bi2I3Br6 single crystal， sensitivity and detection limit of Cs3Bi2I8Br detector［96］；（e） images measured by the MA3Bi2I6Br3 single crystal linear array detector［80］

Table 1 Performance parameters comparison of 3D， 2D， 1D， 0D structure perovskite single crystal X-ray detector

维度	钙钛矿类型	迁移率-寿命积/（cm²·V^-1）	电阻率/（Ω·cm）	灵敏度/（μC·Gy^-1·cm^-2）	探测限/（nGy·s^-1）	参考文献
3D	MAPbI₃	5.30×10^-3	2.82×10⁷	2.31×10⁴	19 100	［85］
	DMAMAPbI₃	7.20×10^-3	3.04×10⁸	1.18×10⁴	16.9	［85］
	GAMAPbI₃	1.30×10^-2	2.05×10⁸	3.67×10³	16.9	［85］
	FAPbI₃			1.5×10⁵	267	［12］
	MAPbI₃	1.46×10^-3		5.2×10⁶	1.5	［86］
	Cs_0.1FA_0.85GA_0.05PbI_2.7Br_0.3	1.09×10^-2		2.5×10⁶	7.09	［87］
	MAPbBr₃/MAPbI₃	4.88×10^-2	2.22×10⁸	3.98×10⁵	12.2	［24］
	MAPbBr₃	7.01×10^-4	4.53×10⁶	2.90×10³		［24］
	MAPbI₃	1.06×10^-3	1.62×10⁷	3.05×10⁴		［24］
	CsPbBr₃	8.11×10^-4		46 180	10.81	［43］
	FAPbI₃	7.82×10^-2	2.31×10¹¹	2.16×10⁵	2	［89］
2D	（F-PEA）₂PbI₄	5.10×10^-4	1.36×10¹²	3 402	23	［57］
	（DGA）PbI₄	4.12×10^-3		4 869	95.4	［58］
	CsPb₂Br₅	2.53×10^-2	5.51×10¹⁰	8 865.6	12.7	［93］
	（PEA）₂Ge_0.5Pb_0.5I₄	3.64×10^-3	8.56×10⁹	13 488	8.23	［61］
	（PEA）₂PbI₄	3.31×10^-3	7.31×10¹⁰	840	12.9	［61］
	（PEA）₂GeI₄	2.23×10^-4	6.41×10⁹	1 527	18.9	［61］
1D	（BAH）BiI₄	1.95×10^-4	4.20×10¹¹	1 181.8	77	［63］
	DABCO-N₂H₅-Br₃		2.74×10¹⁰	1 143±10	2 680	［94］
	DABCO-N₂H₅-I₃		1.26×10¹⁰	1 187±9	2 880	［94］
	CsCu₂I₃	1.847×10^-2		424	0.93	［64］
	（TMHD）SbBr₅	8.33×10^-3		62.8		［65］
	（ATZ）（EA）₄Pb₃I₁₁	2.22×10^-4	1.94×10¹¹	1 356		［66］
0D	MA₃Bi₂I₉	2.87×10^-3	3.74×10¹⁰	1 947	83	［72］
	Cs₃Bi₂I₉	7.97×10^-4	2.79×10¹⁰	1 652.3	130	［73］
	MA₃Bi₂I₉	1.20×10^-3	5.27×10¹¹	10 620	0.62	［74］
	AG₃Bi₂I₉	7.94×10^-3	3.78×10¹⁰	5 791	2.6	［81］
	Cs₃Bi₂I₈Br		1.99×10¹⁰	1.33×10⁴	28.6	［96］

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