Low-Temperature Grown High-Quality MAPbI3 Perovskite Single Crystals and Its Photodetection Performance

doi:10.16553/j.cnki.issn1000-985x.2025.0215

Abstract

Abstract: Perovskite single crystals are regarded as highly promising materials for optoelectronic devices， owing to their low defect density， outstanding photovoltaic characteristics， high resistance to moisture， and effective suppression of ion migration. However， the efficiency of perovskite single crystals-based devices in applications such as photovoltaics and light-emitting diodes has remained inferior to that of polycrystalline thin-film counterparts， primarily due to limitations in material processing and crystal growth quality. To address these challenges， a low-temperature crystal growth strategy was developed using 2-methoxyethanol （2ME） as the solvent. This approach was designed to minimize thermal fluctuations during the crystallization process， thereby suppressing the formation of defect states. In addition， owing to the low boiling point of 2ME， solvent retention on the perovskite surface was significantly reduced. When compared with MAPbI₃ single crystals prepared using conventional gamma-butyrolactone （GBL） solvent， the 2ME-grown crystals exhibited a 2.7-fold enhancement in photoluminescence （PL） intensity and a 1.5-fold extension of carrier lifetime. A reduction in defect state density by 16% was achieved， along with a 19% increase in the activation energy for ion migration. Furthermore， a self-powered photodetector fabricated from 2ME-derived MAPbI₃ single crystals demonstrated a responsivity of 0.55 A·W^-1 and a specific detectivity of 0.80×10¹³ Jones at 0 V bias. These values exceed those of devices based on GBL-grown crystals by factors of 1.72 and 1.59， respectively. The response speed was also markedly improved， with rise and fall times of 2.1 ms and 3.2 ms—representing a 54% and 49% enhancement over the GBL-based device （~4.6 ms rise， ~6.3 ms fall）. This study establishes a reliable low-temperature pathway for the production of high-quality， low-defect MAPbI₃ single crystals via 2ME. The findings indicate that this method effectively enhances the optoelectronic performance and stability of perovskite single crystals， facilitating their application in advanced devices such as high-sensitivity imaging systems， optical communication modules， and quantum detection platforms.

Key words: perovskite single crystal; low-temperature growth; solvent residue; ion migration; self-powered; photodetector

CLC Number:

O782

LIU Dong, LI Yuxin, LI Dalin, LU Bin, GUO Zheng, CHEN Qian, ZHANG Xiaojing, WANG Yaxue, CHEN Danping, GUO Kexin, HE Tao. Low-Temperature Grown High-Quality MAPbI₃ Perovskite Single Crystals and Its Photodetection Performance[J]. Journal of Synthetic Crystals, 2026, 55(3): 349-358.

Figures/Tables 6

Fig.1 Controllable growth of MAPbI3 perovskite single crystals. （a） Schematic illustration of MAPbI3 perovskite single crystal growth using GBL and 2ME solvents；（b） optical microscopy image of MAPbI3 perovskite single crystals grown on ITO substrates from GBL and 2ME； XRD patterns （c） and ultraviolet-visible absorption （d） of MAPbI3 perovskite single crystals grown from GBL and 2ME， respectively；（e） UPS characterization of MAPbI3 perovskite single crystals；（f） AFM image of MAPbI3 perovskite single crystals grown from the two solvents

Fig.2 Structural characterization of MAPbI3 perovskite single crystals. （a） Structures and saturated vapor pressure （20 ℃） of GBL and 2ME solvents； EDS mapping images of MAPbI3 perovskite single crystals grown from GBL （b） and 2ME （c） solvents， respectively； XPS （d） and corresponding magnified view （e） of MAPbI3 perovskite single crystals grown from GBL；（f） XPS of MAPbI3 perovskite single crystals grown from 2ME

Fig.3 Characterization of crystal quality of MAPbI3 perovskite single crystals grown from GBL and 2ME. PL （a） and TRPL （b） spectra of MAPbI3 perovskite single crystals grown from GBL and 2ME solvents， respectively；（c） SCLC measurements for evaluating the trap density of MAPbI3 perovskite single crystals grown from the two solvents；（d） temperature-dependent conductivity measurements of MAPbI3 perovskite single crystals grown from GBL and 2ME； XRD rocking curves of MAPbI3 perovskite single crystals grown from GBL （e） and 2ME （f） solvents

Fig.4 Optoelectronic properties of MAPbI3 perovskite single crystals grown from GBL and 2ME. （a） Energy band diagram of the self-powered ITO/MAPbI3/Au photodetector；（b） dark and photoinduced （445 nm） I-V curves of the self-powered ITO/MAPbI3/Au photodetectors；（c） I-t photoresponse of GBL- and 2ME-grown crystals at 445 nm （0.01 mW·cm-2）；（d） I-t curves of the 2ME-grown crystal under 445 nm light at varying intensities；（e） relationship between photocurrent and optical power density of MAPbI3 single crystals grown in two solvents；（f） responsivity （R） and detectivity （D*） of the photodetectors based on MAPbI3 single crystals prepared using the two solvents

Table 1 Comparison of parameters with reported MAPI3 perovskite photodetectors

Device structure	Bias/V	R/（A·W^-1）	D^*/Jones	Reference
Au/MoO₃/MAPbI₃/ZnO/FTO	-6	10.8	3.5 × 10¹¹	［32］
MAPbI₃∶PC61BM/Au/ZnO	7	7	2.6 × 10¹²	［33］
ITO/PEDOT∶PSS/MAPbI₃（with ODT）/PC70BM/Al	-0.1	0.366	1.45 × 10¹²	［34］
ITO/NiO _x /MAPbI₃（with urea）/PCBM/BCP/Ag	-0.1	1.06	7.3 × 10¹²	［35］
ITO/PEDOT∶PSS/MAPbI₃/QD@APDEMS/PC70BM/Ag	-0.1	0.47	1.77 × 10¹²	［36］
ITO/NiO _x /MAPbI₃（TFTPN）/C60/BCP/Cu	0	0.503	9.44 × 10¹²	［36］
ITO/NiO _x /MAPbI₃（with PBFDO）/PCBM/BCP/Ag	0	0.49	8.1 × 10¹²	［36］
ITO/NiO _x /PMMA/MAPbI₃/PMMA/PCBM/ZnO/BCP/Al	0	0.415	1.30 × 10¹²	［37］
ITO/MAPbI₃/Au	0	0.55	0.80 ×10¹³	This work

Fig.5 Stability characterization of the photodetectors. After 1 000 on/off switching cycles， the I-t curves of the self-powered photodetectors based on GBL-grown （a） and 2ME-grown （b） MAPbI3 single crystals， respectively；（c） I-t curves of the self-powered photodetectors based on 2ME-grown MAPbI3 single crystals after one month aging； response time of the photodetectors fabricated with GBL-grown （d） and 2ME-grown （e） MAPbI3 single crystals， respectively

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Low-Temperature Grown High-Quality MAPbI₃ Perovskite Single Crystals and Its Photodetection Performance

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