Strongly emissive individual DNA-encapsulated Ag nanoclusters as single-molecule fluorophores

Tom Vosch, Yasuko Antoku, Jung Cheng Hsiang, Chris I. Richards, Jose I. Gonzalez, Robert M. Dickson

Research output: Contribution to journalArticlepeer-review

437 Scopus citations

Abstract

The water-soluble, near-IR-emitting DNA-encapsulated silver nanocluster presented herein exhibits extremely bright and photostable emission on the single-molecule and bulk levels. The photophysics have been elucidated by intensity-dependent correlation analysis and suggest a heavy atom effect of silver that rapidly depopulates an excited dark level before quenching by oxygen, thereby conferring great photostability, very high single-molecule emission rates, and essentially no blinking on experimentally relevant time scales (0.1 to > 1,000 ms). Strong antibunching is observed from these biocompatible species, which emit >109 photons before photobleaching. The significant dark-state quantum yield even enables bunching from the emissive state to be observed as a dip in the autocorrelation curve with only a single detector as the dark state precludes emission from the emissive level. These species represent significant improvements over existing dyes, and the nonpower law blinking kinetics suggest that these very small species may be alternatives to much larger and strongly intermittent semiconductor quantum dots.

Original languageEnglish
Pages (from-to)12616-12621
Number of pages6
JournalProceedings of the National Academy of Sciences of the United States of America
Volume104
Issue number31
DOIs
StatePublished - Jul 31 2007

Keywords

  • Correlation
  • Fluorescence intermittency
  • Photophysics
  • Silver nanoclusters
  • Single-molecule spectroscopy

ASJC Scopus subject areas

  • General

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