Journal
MATTER
Volume 4, Issue 3, Pages 1054-1071Publisher
CELL PRESS
DOI: 10.1016/j.matt.2020.12.024
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Funding
- Strategic Priority Research Program of CAS [XDB36000000]
- Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China [51888103]
- National Natural Science Foundation of China [21872043, 21573049, 21422303]
- National Basic Research Plan of China [2018YFB1502000, 2016YFA0201600]
- Beijing Natural Science Foundation [2142036]
- Fundamental Research Funds for the Central Universities [NJ2020048]
- Startup Fund from Nanjing University of Aeronautics and Astronautics [56SYAH19047]
- Knowledge Innovation Program of CAS
- Youth Innovation Promotion Association of CAS
- Special Program of One Belt One Road'' of CAS
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Single-crystal (Ga1-xZnx)(N1-xOx) nanowires were synthesized with fully tunable compositions using a customized chemical vapor deposition strategy. The existence of a strong clustering tendency at the nanometer scale in the synthesized nanowires was verified through X-ray absorption fine structure analysis, which plays a dominant role in determining the electronic band structures and ultimately affects the water-splitting activity. Atomic arrangement engineering provides an additional tool for band-gap engineering of semiconductor alloys, benefiting the development of new functional materials for energy conversion applications.
We synthesized single-crystal (Ga1-xZnx)(N1-xOx) nanowires with fully tunable compositions (0 < x < 1) using a customized chemical vapor deposition strategy. Despite the uniform distributions of component elements at the nanometer scale, X-ray absorption fine structure analysis in combination with ab initio multiple -scattering calculation verified the existence of a strong clustering tendency, i.e., the energetic preference of the valence-matched Ga-N and Zn-O pairs, in the synthesized nanowires. The strong clustering tendency plays a dominant role in determining the electronic band structures of the nanowires, causing a continuous band-gap reduction with increasing ZnO content, which is interpreted via a type II band alignment among the intracrystalline heterojunctions formed between the incorporated clusters and the host material. This, ultimately, makes the sample with the highest ZnO content show the highest water-splitting activity. Atomic arrangement engineering will provide an additional tool for band-gap engineering of semiconductor alloys, greatly benefiting the development of new functional materials for energy conversion applications.
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