4.8 Article

Photoemission of Energetic Hot Electrons Produced via Up Conversion in Doped Quantum Dots

Journal

NANO LETTERS
Volume 16, Issue 11, Pages 7270-7275

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.6b03774

Keywords

photoemission; hot electron; Mn-doped quantum dot; exciton-to-hot-carrier up-conversion

Funding

  1. National Science Foundation [CBET-1264840]
  2. Robert A. Welch Foundation [A-1639]
  3. Div Of Chem, Bioeng, Env, & Transp Sys
  4. Directorate For Engineering [1264840] Funding Source: National Science Foundation

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The benefits of the hot electrons from semiconductor nanostructures in photocatalysis or photovoltaics result from their higher energy compared to that of the band-edge electrons facilitating the electron-transfer process. The production of high-energy hot electrons usually requires short-wavelength UV or intense multiphoton visible excitation. Here, we show that highly energetic hot electrons capable of above-threshold ionization are produced via exciton-to-hot-carrier up-conversion in Mn-doped quantum dots under weak band gap excitation (similar to 10 W/cm(2)) achievable with the concentrated solar radiation. The energy of hot electrons is as high as similar to 0.4 eV above the vacuum level, much greater than those observed in other semiconductor or plasmonic metal nanostructures, which are capable of performing energetically and kinetically more-challenging electron transfer. Furthermore, the prospect of generating solvated electron is unique for the energetic hot electrons from up-conversion, which can open a new door for long-range electron transfer beyond short-range interfacial electron transfer.

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