Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 135, Issue 38, Pages 14142-14150Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja404599g
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Funding
- NREL LDRD Director's Fellowship Program
- Solar Photochemistry program of the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC36-08GO28308]
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We have developed a colloidal synthesis of 4-10 nm diameter indium nitride (InN) nanocrystals that exhibit both a visible absorption onset (similar to 1.8 eV) and a strong localized surface plasmon resonance absorption in the mid-infrared (similar to 3000 nm). Chemical oxidation and reduction reversibly modulate both the position and intensity of this plasmon feature as well as the band-to-band absorption onset. Chemical oxidation of InN nanocrystals with NOBF, is found to red-shift the absorption onset to similar to 1.3 eV and reduce the plasmon absorption energy (to 3550 nm) and intensity (by an order of magnitude at 2600 nm). Reduction of these oxidized species with Bu4NBH4 fully recovers the original optical properties. Calculations suggest that the carrier density in these InN nanocrystals decreases upon oxidation from 2.89 x 1020 cm(-3) to 2.51 X 10(20) cm(-3), consistent with the removal of similar to 4 electrons per nanocrystal. This study provides a unique example of the ability to tune the optical properties of colloidal nanomaterials, and in particular the LSPR absorption, with reversible redox reactions that do not affect the semiconductor chemical composition or phase.
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