4.8 Article

Toward Bright Mid-Infrared Emitters: Thick-Shell n-Type HgSe/CdS Nanocrystals

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 46, 页码 19567-19575

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AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c09858

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资金

  1. National Science Foundation [DMR-2011854]
  2. ARO [W911NF-18-1-0207]
  3. Edith Barnard Memorial Fund from the Chemistry Department at the University of Chicago

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A new method was developed to grow thick, conformal CdS shells that preserve the optical properties of 5 nm HgSe cores, with the doping of the core/shell particles quantitatively tuned through a simple postsynthetic Cd treatment. The CdS shell greatly increases the intraband emission intensity and raises important questions about the fundamental limits to achievable slow intraband relaxation in quantum dots.
A procedure is developed for the growth of thick, conformal CdS shells that preserve the optical properties of 5 nm HgSe cores. The n-doping of the HgSe/CdS core/shell particles is quantitatively tuned through a simple postsynthetic Cd treatment, while the doping is monitored via the intraband optical absorption at 5 mu m wavelength. Photoluminescence lifetime and quantum yield measurements show that the CdS shell greatly increases the intraband emission intensity. This indicates that decoupling the excitation from the environment reduces the nonradiative recombination. We find that weakly n-type HgSe/CdS are the brightest solution-phase mid-infrared chromophores reported to date at room temperature, achieving intraband photoluminescence quantum yields of 2%. Such photoluminescence corresponds to intraband lifetimes in excess of 10 ns, raising important questions about the fundamental limits to achievable slow intraband relaxation in quantum dots.

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