Journal
ADVANCED MATERIALS
Volume 32, Issue 50, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202004059
Keywords
free‐ carrier concentration; hydrogenation; plasmonic materials; quasi‐ metallic energy band; surface‐ enhanced Raman spectroscopy
Categories
Funding
- National Key Research and Development Program of China [2016YFA0200602, 2017YFA0303500, 2018YFA0208702]
- National Natural Science Foundation of China [21421063, 21473166, 21573211, 21633007, 21790350, 21803067, 91950207]
- Chinese Academy of Sciences [QYZDB-SSW-SLH018]
- Anhui Initiative in Quantum Information Technologies [AHY090200]
- USTC-NSRL Joint Funds [UN2018LHJJ]
- USTC Center for Micro-and Nanoscale Research and Fabrication
- Steady High Magnetic Field Facilities
- High Magnetic Field Laboratory
- Fundamental Research Funds for Central Universities of China
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The practical utilization of plasmon-based technology relies on the ability to find high-performance plasmonic materials other than noble metals. A key scientific challenge is to significantly increase the intrinsically low concentration of free carriers in metal-oxide materials. Here, a novel electron-proton co-doping strategy is developed to achieve uniform hydrogen doping in metal-oxide MoO3 at mild conditions, which creates a metal-like ultrahigh free-carrier concentration approaching that of noble metals (10(21) cm(-3) in H1.68MoO3 versus 10(22) cm(-3) in Au/Ag). This bestows giant and tunable plasmonic resonances in the visible region to this originally semiconductive material. Using ultrafast spectroscopy characterizations and first-principle simulations, the formation of a quasi-metallic energy band structure that leads to long-lived and strong plasmonic field is revealed. As verified by the surface-enhanced Raman spectra (SERS) of rhodamine 6G molecules on HxMoO3, the SERS enhancement factor reaches as high as 1.1 x 10(7) with a detection limit at concentration as low as 1 x 10(-9) mol L-1, representing the best among the hitherto reported non-metal systems. The findings not only provide a set of metal-like semiconductor materials with merits of low cost, tunable electronic structure, and plasmonic resonance, but also a general strategy to induce tunable ultrahigh free-carrier concentration in non-metal systems.
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