Band Gap and Defect Engineering Enhanced Scintillation from Ce3+-Doped Nanoglass Containing Mixed-Type Fluoride Nanocrystals

Chengxi Luo; Yue Jing; Zhehao Hua; Zexuan Sui; Ci Wang; Peng Hu; Lirong Zheng; Sen Qian; Luyun Yang; Xinyuan Sun; Gao Tang; Hua Cai; Yao Zhu; Huiyun Ban; Jifeng Han; Zhile Wang; Xvsheng Qiao; Jing Ren; Jianzhong Zhang

doi:10.1021/acsami.3c09230

Band Gap and Defect Engineering Enhanced Scintillation from Ce³⁺-Doped Nanoglass Containing Mixed-Type Fluoride Nanocrystals

ACS Appl Mater Interfaces. 2023 Oct 4;15(39):46226-46235. doi: 10.1021/acsami.3c09230. Epub 2023 Sep 22.

Authors

Chengxi Luo^{1

2}, Yue Jing¹, Zhehao Hua³, Zexuan Sui^{1

3}, Ci Wang¹, Peng Hu³, Lirong Zheng³, Sen Qian³, Luyun Yang², Xinyuan Sun⁴, Gao Tang⁵, Hua Cai⁶, Yao Zhu¹, Huiyun Ban⁷, Jifeng Han⁸, Zhile Wang⁹, Xvsheng Qiao¹⁰, Jing Ren¹, Jianzhong Zhang¹

Affiliations

¹ Key Laboratory of In-fiber Integrated Optics, Ministry Education of China, Harbin Engineering University, Harbin 150001, China.
² Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, China.
³ Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China.
⁴ Department of Physics, Jinggangshan University, Ji'an 343009, China.
⁵ College of Materials and Chemistry, China Jiliang University, Hangzhou 310018, China.
⁶ China Building Materials Academy, Beijing 100024, China.
⁷ Beijing Glass Research Institute, Beijing 101111, China.
⁸ Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, Sichuan University, Chengdu 610065, China.
⁹ Department of Electronic Science and Technology, Harbin Institute of Technology, Harbin 150001, China.
¹⁰ School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027 China.

PMID: 37738374
DOI: 10.1021/acsami.3c09230

Abstract

Much can be learned from the research and development of scintillator crystals for improving the scintillation performance of glasses. Relying on the concept of "embedding crystalline order in glass", we have demonstrated that the scintillation properties of Ce³⁺-doped nanoglass composites (nano-GCs) can be optimized via the synergistic effects of Gd³⁺-sublattice sensitization and band-gap engineering. The nano-GCs host a large volume fraction of KY_xGd_1-xF₄ mixed-type fluoride nanocrystals (NCs) and still retain reasonably good transparency at Ce³⁺-emitting wavelengths. The light yield of 3455 ± 20 ph/MeV is found, which is the largest value ever reported in fluoride NC-embedded nano-GCs. A comprehensive study is given on the highly selective doping of Ce³⁺ in the NCs and its positive effect on the scintillation properties. The favorable influence of the Y³⁺/Gd³⁺ mixing on the suppression of defects is accounted for by density functional theory and borne out experimentally. As a proof-of-concept, X-ray imaging with a good spatial resolution (7.9 lp/mm) is demonstrated by employing Ce³⁺-doped nano-GCs. The superior radiation hardness, repeatability, and thermal stability of the designed scintillators bode well for their long-term practical applications.

Keywords: X-ray imaging; band-gap engineering; fast scintillator; mixed crystal; nanoglass composite.