Auger ionization beats photo-oxidation of semiconductor quantum dots: extended stability of single-molecule photoluminescence

Angew Chem Int Ed Engl. 2015 Mar 23;54(13):3892-6. doi: 10.1002/anie.201501131. Epub 2015 Feb 27.

Abstract

Despite the bright and tuneable photoluminescence (PL) of semiconductor quantum dots (QDs), the PL instability induced by Auger recombination and oxidation poses a major challenge in single-molecule applications of QDs. The incomplete information about Auger recombination and oxidation is an obstacle in the resolution of this challenge. Here, we report for the first time that Auger-ionized QDs beat self-sensitized oxidation and the non-digitized PL intensity loss. Although high-intensity photoactivation insistently induces PL blinking, the transient escape of QDs into the ultrafast Auger recombination cycle prevents generation of singlet oxygen ((1) O2 ) and preserves the PL intensity. By the detection of the NIR phosphorescence of (1) O2 and evaluation of the photostability of single QDs in aerobic, anaerobic, and (1) O2 scavenger-enriched environments, we disclose relations of Auger ionization and (1) O2 -mediated oxidation to the PL stability of single QDs, which will be useful during the formulation of QD-based single-molecule imaging tools and single-photon devices.

Keywords: Auger ionization; photochemistry; quantum dots; single-molecule studies; singlet oxygen.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Free Radical Scavengers
  • Luminescence
  • Nanotechnology
  • Oxidation-Reduction
  • Oxygen / chemistry
  • Photochemical Processes
  • Quantum Dots*
  • Reactive Oxygen Species
  • Semiconductors*
  • Spectroscopy, Near-Infrared

Substances

  • Free Radical Scavengers
  • Reactive Oxygen Species
  • Oxygen