Review on Impact of Film Preparation Method and Crystallization Behavior on the Imaging Performance of Halide Perovskite X-Ray Detectors

doi:10.16553/j.cnki.issn1000-985x.2025.0016

Abstract

Abstract: X-ray detectors play a vital role in medical diagnostics， security screening， industrial nondestructive testing， and scientific research. Halide perovskites （HPs） have garnered significant attention for high-performance X-ray detection due to their large X-ray absorption coefficient， long carrier diffusion length， and superior optical properties. Notably， the flexible synthesis of HPs enables facile fabrication into polycrystalline films， wafers， and other forms. However， differences in crystallization behavior induced by fabrication methods result in varied defect distributions within the active layer， such as crystallographic orientation， grain boundaries， cracks， and pinholes， which critically impact charge carrier transport and scintillation efficiency and degrade the device performance. Therefore， elucidating crystallization mechanisms under different fabrication conditions and developing tailored control strategies are imperative. Here we systematically review the recent advances in HPs X-ray detectors： 1） wet chemical synthesis approaches and crystallization regulation strategies； 2） crystallization regulation in pressing methods， ion migration suppression， and scintillator wafer development； 3） analyzing crystallization mechanisms in vapor deposition processes， strategies for enhancing scintillator performance， and exploratory efforts toward direct X-ray detection applications. Finally， we highlight existing challenges and future prospects for advancing HPs X-ray detectors.

Key words: halide perovskite; wet chemical method; pressing method; vapor deposition method; crystallization kinetics; crystallization regulation; X-ray imaging

CLC Number:

O795

XIE Hang, JIN Zhiwen. Review on Impact of Film Preparation Method and Crystallization Behavior on the Imaging Performance of Halide Perovskite X-Ray Detectors[J]. Journal of Synthetic Crystals, 2025, 54(7): 1100-1120.

Figures/Tables 8

Fig.1 Schematic diagram of X-ray detection principles. （a） Direct X-ray detection；（b） indirect X-ray detection

Fig.2 Schematic diagram of method for constructing the active of HPs X-ray detectors. （a） Spin-coating method；（b） blade-coating method；（c） spray coating method；（d） inkjet printing method；（e） pressing method；（f） vacuum evaporation method；（g） close-space sublimation method

Fig.3 Fabrication and characterization of X-ray detectors constructed via spin-coating method. Schematic diagram of the fabrication process （a） and cross-sectional SEM image of the polymer-encapsulated Cs4PbI6 device （b）［58］；（c） X-ray imaging process and images based on PAZE-NH4Br3·H?O film；（d） morphology SEM images under different magnifications［59］；（e） structural diagram of the porous PET substrate used for MFP；（f） cross-sectional SEM image of MFP based on MAPbI3［63］；（g） schematic diagram of X-ray imaging using Cs2ZrCl6@PDMS flexible scintillator films and corresponding X-ray images［67］；（h） schematic illustration of hot-casting of quasi-2D films on hole transport layer substrate prepared via spin-coating method；（i） cross-sectional SEM images of films cast form quasi-2D and 3D crystal structures［68］；（j） cross-sectional SEM images of 2D-RP films with different thickness；（k） CIWAXS maps of 2D-RP films with different thickness［69］

Fig.4 Characterization of X-ray detectors fabricated via blade-coating method. （a） Morphology SEM images of MA3Bi2I9 thick films with different concentrations of MACl additive， and cross-sectional image of the film with 10% MACl added；（b） dose rate-current density curves of device based on MA3Bi2I9 thick film with 10% MACl under different bias voltage［72］；（c） cross-sectional （left） and morphology （right） SEM images of FAMAC thick film［74］；（d） morphology （left） and cross-sectional （right） SEM images of MAPbI3 thick films with and without MASCN additive［77］；（e） schematic diagram of the crystallization process of wet films via spin-coating and blade-coating method［78］；（f） schematic diagram of the crystallization process for the wet films after blade-coating under different atmospheric conditions；（g） morphology （up） and cross-sectional （down） SEM images of thick films under different conditions；（h） X-ray images of metal letters at different dose rate［80］；（i） in situ optical microscopy images of the crystallization process of MTP2MnBr4 andBPP2MnBr4［81］；（j） illustration of MAPbI3 layer subjected to tensile or compressive stress induced by thermal changes on flexible and rigid substrates， respectively［84］

Fig.5 X-ray detectors based on inkjet printing and spraying methods and their characterization. Schematic diagram （a） and optical photograph （b） of the X-ray detection array based on CsPbI3 QDs via inkjet printing on a SiO2/Si wafer［87］；（c） cross-sectional SEM images of TCP devices printed on ITO substrates spin-coated with NiO x （left） and c-PEDOT∶PSS （right）［88］；（d） microscope images of different patterns of MAPbI3 via inkjet printing method［89］；（e） cross-sectional （top） and morphology （middle） SEM images of CsPbI2Br film with different cycles， constructed by the ALS method， and a schematic illustration of crystallization （bottom）［78］；（f） schematic diagram and cross-sectional and morphology SEM images of Cs3Bi2I9 thick films prepared by one step spraying （top） and two steps spraying （bottom）［90］；（g） in situ optical microscope images of MAPbI3 crystallization process in different DIW ink environments；（h） schematic diagram of the DIW crystallization process and final cross-sectional SEM image；（i） cross-sectional SEM images of MAPbI3 films printed by DIW method with different printing counts （form left to right：1~5 times）［91］

Fig.6 Characterization of X-ray detectors via pressing method. （a） Cross-sectional SEM images of the MAPbI3 with a precusor molar ratio of PbI2∶MAI=1∶1.15 during wafer formation at different pressing times （a-1 to a-6 represent 0， 5， 10， 20， 30， and 40 min respectively）；（b） relationship between the wafer thickness and the raw material mass， along with cross-sectional SEM images of wafer with different thickness［93］； optical image （c） and SEM morphology （left） and cross-sectional （right） images （d） of MA3Bi2I9 wafer［97］；（e） optical image of （F-PEA）3BiI6 wafer；（f） schematic illustration of crystal cell reorientation under pressure for （F-PEA） 3BiI6［98］；（g） TEM image of Cs4PbBr6 MCs， along with the corresponding selected-area electron diffraction pattern；（h） SEM images of Cs4PbBr6 MCs with different toluene injection speed；（i） SEM morphology （left） and cross-sectional （right） images of Cs4PbBr6 wafer［99］； optical image （j） and SEM morphology （left） and cross-sectional （right） images （k） of （C8H20N）2Cu2Br4 wafer；（l） optical image of the integrated circuit board used for imaging （left） and corresponding X-ray image （right）［100］；（m） optical images of MAPbI3 wafers at different pressing time， along with morphology （left 1 and 3） and cross-sectional （left 2 and 4） SEM images of opaque and transparent wafers［101］

Fig.7 Crystallization control and performance of X-ray detectors via vacuum deposition. SEM images of Cs3Cu2I5 film via vacuum deposition （a）， and MTF-spatial resolution function curve measured by the slanted-edge method （b）［105］； SEM （left） and cross-sectional （right） images of Cs3Cu2Cl5 film via sequential vacuum deposition （c）， and MTF curves measured by the slanted-edge method （d）［106］；（e） schematic illustration of light transmission and scattering within scintillator layers［107］；（f） SEM images of surfaces of CsI∶Tl film with different deposition stages；（g） film formation process of the CsI∶Tl；（h） generation of new crystal orientation in holes and cracks［109］； SEM images under different manifications （left 1 and 2） and cross-sectional image （right）（i）， and MTF-curves measured by the slanted-edge method （j）［110］；（k） SEM （left） and cross-sectional （right） images of FAPbI3 film；（l） schematic illustration of the device structure［111］；（m） SEM image of 400 nm-thick CsPbI2Br film［112］； SEM cross-sectional image of a MAPbI3 based photodiode （n） and schematic of the device structure （o）［113］

Fig.8 Crystallization control and scintillator performance via the near-space sublimation process. （a） SEM cross-sectional and morphology images of Rb2AgBr3 thick films prepared under different temperature conditions；（b） schematic illustration of dynamic imaging by Rb2AgBr3 thick film；（c） dynamic imaging images of chicken wings［114］；（d） cross-sectional SEM image of CsCu2I3 thick film；（e） schemic diagram of the seed crystal screening strategy；（f） SEM （1） and cross-sectional （2~4） images corresponding to different crystallization stages in the seed crystal screening strategy；（g） schematic of CsCu2I3 scintillator detector［115］；（h） schematic showing differences in dangling bonds and afterglow effects induced by different crystal structures；（i） afterglow comparison images under X-ray excitation；（j） cross-sectional SEM image and XRD pattern of Cs5Cu3Cl6I2 thick film with orientation growth；（k） demonstration images of angiography［116］

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