期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 49, 页码 17834-17842出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201911281
关键词
cation engineering; DFT simulation; perovskites; single crystal; X-ray detector
资金
- National Natural Science Foundation of China [11775120, 11535010, 21771114]
- MOE 111 [B12015]
- Natural Science Foundation of Tianjin [18JCYBJC17800, 17JCYBJC40900, 18YFZCGX00580]
- Recruitment Program of Global Youth Experts of China
- National Natural Science of China [21573022]
Metal halide perovskites have emerged as a new generation of X-ray detector materials. However, large-sized MAPbI(3) single crystals (SCs) still exhibit lower performance than MAPbBr(3) SCs in X-ray detection. DFT (density functional theory) simulations suggest the problem could be overcome by alloying large-sized cations at the A site. The alloyed process could notably decrease the electron-phonon coupling strength and increase the material defect formation energy. Accordingly, centimeter-sized alloyed DMAMAPbI(3) (DMA=dimethylammonium) and GAMAPbI(3) (GA=guanidinium) SCs are obtained. Electrical characterizations confirm the GAMAPbI(3) SCs display improved charge collection efficiency. It also exhibits a remarkable reduction of dark current, an important figure of merit for X-ray detectors. With a judiciously designed device architecture, the overall detector performance confirms GAMAPbI(3) SCs as one of the most sensitive perovskite X-ray detectors to date.
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