Growth and X-Ray Detection Properties of High-Quality Perovskite Single Crystals

doi:10.16553/j.cnki.issn1000-985x.2025.0073

Abstract

Abstract: Metal halide perovskites （MHPs） single crystals have potential applications in the field of radiation detection due to their excellent optoelectronic properties. Additionally， suppressing defects both in the bulk during single crystal growth and on the surface after growth is expected to further improve the performance of semiconductor radiation detectors. In this study， high-quality MAPbBr₃ single crystals with dimensions exceeding 10 mm×10 mm were grown by inverse temperature crystallization （ITC） using the amphiphilic surfactant thiobetaine 10 as an additive. The mechanism of additive-optimized crystal growth was analyzed and characterized. The synergistic effect of sulfonic acid amphiphiles in crystallization control and defect passivation significantly suppressed defect formation. The full width at half maximum （FWHM） of the grown MAPbBr₃ single crystals reduces from 0.071° to 0.046°， while the long-chained alkyl groups make the surface of the crystals exhibit excellent hydrophobicity， increasing the surface contact angle increases from 84.04° to 96.25°. These results demonstrate an overall improvement in MHP single crystal quality. A device with Ni/Au-Ni/Au ring-symmetric electrodes was prepared， and the device resistivity increases from 2.08×10⁷ Ω·cm to 2.82×10⁸ Ω·cm， with a carrier mobility lifetime product of 1.81×10^-2 cm²·V^-1. Furthermore， MAPbBr₃ single crystals detector achieve an X-ray detection sensitivity of 1 459 μC·Gy_air^-1·cm^-2 under 50 kV X-ray irradiation and maintain stable operation over a 1 000 s test period. This strategy advances the practical application of perovskite single crystals in X-ray detection. Moreover， our strategy contributes to further progress in the practical application of perovskite single crystals in the field of X-ray detection.

Key words: perovskite single crystal; additive; X-ray detection; defect passivation; crystal growth; inverse temperature crystallization

CLC Number:

O782

XU Zhuangjie, BA Yanshuang, XI He, BAI Fuhui, CHEN Dazheng, ZHU Weidong, ZHANG Chunfu. Growth and X-Ray Detection Properties of High-Quality Perovskite Single Crystals[J]. Journal of Synthetic Crystals, 2025, 54(7): 1229-1237.

Figures/Tables 8

Fig.1 （a） Schematic growth of MAPbBr3 crystal and photographs of crystals grown with/without additives；（b） XRD patterns of MAPbBr3 single crystals grown with/without additives

Fig.2 High-resolution XRD rocking curves of grown crystal （001） plane with （a） / without （b） additives

Fig.3 Schematic diagram of surface growth and defect passivation mechanism of perovskite single crystal

Fig.4 Contact angle of water solution on the surface of grown single crystals with （a） /without （b） additive

Fig.5 FT-IR spectra （a） and XPS measurement result （b） of crystal grown with/without additive， and XPS of Pb 4f （c） and Br 3p （d）

Fig.6 （a） Photograph of device；（b） I-V curves of crystal devices grown with/without additives； light-dark current curves （c） and carrier mobility lifetime product （d） of crystal devices grown with/without additives

Fig.7 （a） Attenuation efficiency to 50 kV X-ray photons versus thickness of MAbBr3； J-t response of the grown crystal devices with （b）/without （c） additives under different biases； sensitivity of the grown crystal devices with （d） / without （e） additives under different biases；（f） I-t curves of the light-dark currents of the grown crystal devices with/without additives at a test period of 1 000 s

Table 1 Comparison of sensitivity performance of semiconductors

Device structure	X-ray source	Electric field/（V·cm^-1）	Sensitivity/（μC·Gy_air^-1·cm^-2）	Reference
α-Se	20 （keV）	—	20	［14］
Au/CZT/Au	120 （keV）	5 000	6 090	［23］
Au/MAPbBr₃/C₆₀/BCP/Au， Ag	50 （keV）	—	80	［24］
Au/MAPbBr₃/AZO	80 （kV_p）	50	529	［25］
Ag/MAPbBr₃/Ag	29 （kV）	10	140	［26］
Au/MoO₃/CsPbBr₃/Ag	50 （kV）	45	619	［27］
Au/Ni/MAPbBr₃/Ni/Au	50 （kV）	400	1 450	This work

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