Phase Purity Regulation of BA2MA3Pb4I13 and Its Influence on X-Ray Detection

doi:10.16553/j.cnki.issn1000-985x.2025.0018

Abstract

Abstract: Two-dimensional Ruddlesden-Popper （RP） layered perovskites have received lots of attention in recent years due to their excellent optoelectronic properties and good environmental stability. Their unique properties make them ideal candidates for applications in solar cells， light-emitting diodes， and X-ray detectors. However， two-dimensional RP-type layered perovskites synthesized by solution methods typically exhibit mixed phases with random inorganic layer numbers （i.e.， multiple n-values）， which hinders their application. In this study， the crystallization process of RP layered perovskites was regulated by replacing BAI with BAAc to achieve effective phase purification. The enhancement in phase purity was confirmed by characterization methods， and the phase-purified perovskite material exhibits reduced defects. Consequently， significantly improved carrier extraction and transport capabilities， along with suppressed ion migration were achieved. These structural improvements directly enhanced the performance of the X-ray detectors. The phase-purified detectors exhibit lower detection limits （160.24 nGy_air·s^-1） compared to the unpurified devices， demonstrating stronger capability in low-dose X-ray detection. Additionally， the phase-purified device shows good irradiation stability. Therefore， phase purification not only effectively improved the detection performance of two-dimensional perovskite X-ray detectors but also enhanced device stability， proving the broad application prospects of phase-purification technology in perovskite X-ray detectors.

Key words: regulated crystallization; two-dimensional perovskite; BAAc; phase purification; inhibition of ion migration; X-ray detector

CLC Number:

TL816

ZHANG Aiping, WEI Yazhou, ZHOU Changyao, YUAN Ruihan, WU Congcong, ZHENG Xiaojia. Phase Purity Regulation of BA₂MA₃Pb₄I₁₃ and Its Influence on X-Ray Detection[J]. Journal of Synthetic Crystals, 2025, 54(7): 1256-1264.

Figures/Tables 5

Fig.1 Schematic diagram of BA2MA3Pb4I13 perovskite

Fig.2 XRD patterns of BA2MA3Pb4I13 perovskite before and after phase purification

Fig.3 （a） UV-Vis absorption spectra of phase purified and unpurified BA2MA3Pb4I13 perovskites；（b） optical bandgap phase calculated by Tauc equation for purified and unpurified BA2MA3Pb4I13 perovskite nylon films； PL （c） and TRPL （d） results for phase purified and unpurified BA2MA3Pb4I13 perovskites

Fig.4 （a） Resistivity test of phase purified device and unpurified perovskite； bias-dependent photocurrents of unpurified （b） and pure phased （c） materials and corresponding μτ products；（d） mobility of holes and electrons in the phase purified material under different electric fields； ln（σT）-1 000/T curve of （e） phase purified device and （f） unpurified perovskite

Fig.5 （a） Response of phase purified and unpurified BA2MA3Pb4I13-LP detectors to X-rays at 210 V bias；（b） dose-dependent signal-to-noise ratio （SNR） of X-rays at 210 V bias； X-ray irradiation stability of unpurified devices （c） and phase purified devices （d）

References 28

[1]	BLASSE G. Scintillator materials［J］. Chemistry of Materials， 1994， 6（9）： 1465-1475.
[2]	SPAHN M. X-ray detectors in medical imaging［J］. Nuclear Instruments and Methods in Physics Research Section A： Accelerators， Spectrometers， Detectors and Associated Equipment， 2013， 731： 57-63.
[3]	HAFF R P， TOYOFUKU N. X-ray detection of defects and contaminants in the food industry［J］. Sensing and Instrumentation for Food Quality and Safety， 2008， 2（4）： 262-273.
[4]	SAKDINAWAT A， ATTWOOD D. Nanoscale X-ray imaging［J］. Nature Photonics， 2010， 4（12）： 840-848.
[5]	DUAN X H， CHENG J P， ZHANG L， et al. X-ray cargo container inspection system with few-view projection imaging［J］. Nuclear Instruments and Methods in Physics Research Section A： Accelerators， Spectrometers， Detectors and Associated Equipment， 2009， 598（2）： 439-444.
[6]	LI Z Z， ZHOU F G， YAO H H， et al. Halide perovskites for high-performance X-ray detector［J］. Materials Today， 2021， 48： 155-175.
[7]	ZHANG Y X， LIU Y C， XU Z， et al. Nucleation-controlled growth of superior lead-free perovskite Cs₃Bi₂I₉ single-crystals for high-performance X-ray detection［J］. Nature Communications， 2020， 11（1）： 2304.
[8]	KIM Y C， KIM K H， SON D Y， et al. Printable organometallic perovskite enables large-area， low-dose X-ray imaging［J］. Nature， 2017， 550（7674）： 87-91.
[9]	HEO J H， SHIN D H， PARK J K， et al. High-performance next-generation perovskite nanocrystal scintillator for nondestructive X-ray imaging［J］. Advanced Materials， 2018， 30（40）： 1801743.
[10]	董思吟，帖舒婕，袁瑞涵，等. 低维卤化物钙钛矿直接型X射线探测器研究进展［J］. 无机材料学报， 2023， 38（9）： 1017-1030.
	DONG S Y， TIE S J， YUAN R H， et al. Research progress on low-dimensional halide perovskite direct X-ray detectors［J］. Journal of Inorganic Materials， 2023， 38（9）： 1017-1030 （in Chinese）.
[11]	YUAN M J， QUAN L N， COMIN R， et al. Perovskite energy funnels for efficient light-emitting diodes［J］. Nature Nanotechnology， 2016， 11（10）： 872-877.
[12]	QUINTERO-BERMUDEZ R， GOLD-PARKER A， PROPPE A H， et al. Compositional and orientational control in metal halide perovskites of reduced dimensionality［J］. Nature Materials， 2018， 17（10）： 900-907.
[13]	TSAI H， LIU F Z， SHRESTHA S， et al. A sensitive and robust thin-film X-ray detector using 2D layered perovskite diodes［J］. Science Advances， 2020， 6（15）： eaay0815.
[14]	QUAN L N， YUAN M J， COMIN R， et al. Ligand-stabilized reduced-dimensionality perovskites［J］. Journal of the American Chemical Society， 2016， 138（8）： 2649-2655.
[15]	TSAI H， NIE W Y， BLANCON J C， et al. High-efficiency two-dimensional Ruddlesden-Popper perovskite solar cells［J］. Nature， 2016， 536（7616）： 312-316.
[16]	TSAI H， ASADPOUR R， BLANCON J C， et al. Design principles for electronic charge transport in solution-processed vertically stacked 2D perovskite quantum wells［J］. Nature Communications， 2018， 9： 2130.
[17]	HAN Y， PARK S， KIM C， et al. Phase control of quasi-2D perovskites and improved light-emitting performance by excess organic cations and nanoparticle intercalation［J］. Nanoscale， 2019， 11（8）： 3546-3556.
[18]	HE T W， LI S S， JIANG Y Z， et al. Reduced-dimensional perovskite photovoltaics with homogeneous energy landscape［J］. Nature Communications， 2020， 11（1）： 1672.
[19]	WANG Y K， MA D X， YUAN F L， et al. Chelating-agent-assisted control of CsPbBr₃ quantum well growth enables stable blue perovskite emitters［J］. Nature Communications， 2020， 11： 3674.
[20]	ZHOU M， FEI C B， SARMIENTO J S， et al. Manipulating the phase distributions and carrier transfers in hybrid quasi-two-dimensional perovskite films［J］. Solar RRL， 2019， 3（4）： 1800359.
[21]	SIDHIK S， LI W B， SAMANI M H K， et al. Memory seeds enable high structural phase purity in 2D perovskite films for high-efficiency devices［J］. Advanced Materials， 2021， 33（29）： 2007176.
[22]	LIU Y L， GAO C S， LI D， et al. Dynamic X-ray imaging with screen-printed perovskite CMOS array［J］. Nature Communications， 2024， 15（1）： 1588.
[23]	KASAP S， FREY J B， BELEV G， et al. Amorphous selenium and its alloys from early xeroradiography to high resolution X-ray image detectors and ultrasensitive imaging tubes［J］. Physica Status Solidi （b）， 2009， 246（8）： 1794-1805.
[24]	ZENTAI G， PARTAIN L D， PAVLYUCHKOVA R， et al. Mercuric iodide and lead iodide X-ray detectors for radiographic and fluoroscopic medical imaging［C］//Medical Imaging 2003： Physics of Medical Imaging. San Diego， CA. SPIE， 2003： 77.
[25]	DVORYANKIN V F， DVORYANKINA G G， KUDRYASHOV A A， et al. X-ray sensitivity of Cd_0.9Zn_0.1Te detectors［J］. Technical Physics， 2010， 55（2）： 306-308.
[26]	XIN D Y， ZHANG M， FAN Z H， et al. Low-dose and stable X-ray imaging enabled by low-dimensional dion-jacobson perovskites［J］. Advanced Functional Materials， 2024， 34（38）： 2402480.
[27]	LU X J， XIN D Y， LEI L， et al. High-performance flat-panel perovskite X-ray detectors enabled by defect passivation in ruddlesden-popper perovskites［J］. ACS Applied Materials & Interfaces， 2024， 16（11）： 14006-14014.
[28]	SHEARER D R， BOPAIAH M. Dose rate limitations of integrating survey meters for diagnostic X-ray surveys［J］. Health Physics， 2000， 79（2 ）： S20-S21.

Phase Purity Regulation of BA₂MA₃Pb₄I₁₃ and Its Influence on X-Ray Detection

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 5

References 28

Related Articles 3

Recommended Articles

Metrics

Comments

[1]	LI Ganggui, HUANG Danyang, ZHAO Xiaolong, CAI Yahui, HE Yongning. Study on the Process of Preparing ZnO Thick Film by Electrochemical Deposition Method [J]. JOURNAL OF SYNTHETIC CRYSTALS, 2024, 53(6): 1069-1077.
[2]	LI Zhiwei, TANG Huili, XU Jun, LIU Bo. Research Progress of Ultra-Wide Band Gap Semiconductor Ga₂O₃-Based X-Ray Detectors [J]. JOURNAL OF SYNTHETIC CRYSTALS, 2022, 51(3): 523-537.
[3]	WU Rui, FAN Donghai, KANG Yang, WAN Xin, GUO Chen, WEI Dengke, CHEN Donglei, WANG Tao, ZHA Gangqiang. Research Progress on Semiconductor Materials and Devices for Radiation Detection [J]. JOURNAL OF SYNTHETIC CRYSTALS, 2021, 50(10): 1813-1829.