TY - JOUR
T1 - Decreasing Structural Dimensionality of Double Perovskites for Phase Stabilization toward Efficient X-ray Detection
AU - Chen, Da
AU - Niu, Guangda
AU - Hao, Shiqiang
AU - Fan, Liubing
AU - Zhao, Jing
AU - Wolverton, Christopher
AU - Xia, Mengling
AU - Liu, Quanlin
N1 - Funding Information:
The authors thank Zhengyang Zhou from the Shanghai Institute of Ceramics, Chinese Academy of Sciences, for the collection of the single-crystal X-ray diffraction data. This work was supported by the National Natural Science Foundation of China (51972021) and the Fundamental Research Funds for the Central Universities FRF-IDRY-19-005. S.H. and C.W. are supported by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences under award no. DE-SC0015520.
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/12/29
Y1 - 2021/12/29
N2 - Halide double perovskites have attracted substantial attention for optoelectronic applications owing to their low toxicity and high stability. However, double perovskites have strict requirements in terms of the halide type, thus rendering many of their properties unchangeable, including the band gap, atomic number, and carrier transport. By introducing long-chain organic amines, the chloride site of double perovskites can be completely replaced by bromide. Using this strategy, two dimensions silver-indium-bromide double perovskites (PEA)4AgInBr8 and (i-BA)4AgInBr8 were successfully synthesized [(PEA)+ = C6H5(CH2)2NH3+, (i-BA)+ = CH(CH3)2CH2NH3+]. Density functional theory calculations and spectroscopy characterizations were performed to unveil the semiconducting behaviors and photoluminescence properties of the title compounds. Electrical characterization confirms their good carrier-transport property (μτ product: 2.0 × 10-3 cm2 V-1) and low dark current. Moreover, the presence of heavy atoms, together with the ultrastable baseline contributes to a high X-ray detection sensitivity (185 μC Gyair-1 cm-2), greater than that of most previous double-perovskite detectors. Our work lays the foundation for broadening the family of potential double perovskites, creating a new path for the realization of long-sought perovskites with low toxicity and high stability that retain good optoelectronic performance.
AB - Halide double perovskites have attracted substantial attention for optoelectronic applications owing to their low toxicity and high stability. However, double perovskites have strict requirements in terms of the halide type, thus rendering many of their properties unchangeable, including the band gap, atomic number, and carrier transport. By introducing long-chain organic amines, the chloride site of double perovskites can be completely replaced by bromide. Using this strategy, two dimensions silver-indium-bromide double perovskites (PEA)4AgInBr8 and (i-BA)4AgInBr8 were successfully synthesized [(PEA)+ = C6H5(CH2)2NH3+, (i-BA)+ = CH(CH3)2CH2NH3+]. Density functional theory calculations and spectroscopy characterizations were performed to unveil the semiconducting behaviors and photoluminescence properties of the title compounds. Electrical characterization confirms their good carrier-transport property (μτ product: 2.0 × 10-3 cm2 V-1) and low dark current. Moreover, the presence of heavy atoms, together with the ultrastable baseline contributes to a high X-ray detection sensitivity (185 μC Gyair-1 cm-2), greater than that of most previous double-perovskite detectors. Our work lays the foundation for broadening the family of potential double perovskites, creating a new path for the realization of long-sought perovskites with low toxicity and high stability that retain good optoelectronic performance.
KW - X-ray detectors
KW - double perovskites
KW - hybrid halides
KW - layered compounds
KW - photoluminescence
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U2 - 10.1021/acsami.1c20234
DO - 10.1021/acsami.1c20234
M3 - Article
C2 - 34927414
AN - SCOPUS:85121902395
SN - 1944-8244
VL - 13
SP - 61447
EP - 61453
JO - ACS applied materials & interfaces
JF - ACS applied materials & interfaces
IS - 51
ER -