Strong antenna-enhanced fluorescence of a single light-harvesting complex shows photon anti-bunching

E. Wientjes, J. Renger, A.G. Curto, R. Cogdell, N.F. van Hulst

Research output: Contribution to journalArticleAcademicpeer-review

68 Citations (Scopus)

Abstract

The nature of the highly efficient energy transfer in photosynthetic light-harvesting complexes is a subject of intense research. Unfortunately, the low fluorescence efficiency and limited photostability hampers the study of individual light-harvesting complexes at ambient conditions. Here we demonstrate an over 500-fold fluorescence enhancement of lightharvesting complex 2 (LH2) at the single-molecule level by coupling to a gold nanoantenna. The resonant antenna produces an excitation enhancement of circa 100 times and a fluorescence lifetime shortening to B20 ps. The radiative rate enhancement results in a 5.5-fold-improved fluorescence quantum efficiency. Exploiting the unique brightness, we have recorded the first photon antibunching of a single light-harvesting complex under ambient conditions, showing that the 27 bacteriochlorophylls coordinated by LH2 act as a nonclassical single-photon emitter. The presented bright antenna-enhanced LH2 emission is a highly promising system to study energy transfer and the role of quantum coherence at the level of single complexes.
Original languageEnglish
Article number4236
Number of pages7
JournalNature Communications
Volume5
DOIs
Publication statusPublished - 2014
Externally publishedYes

Keywords

  • pigment-protein complexes
  • purple bacterial lh2
  • exciton delocalization
  • molecule fluorescence
  • energy-transfer
  • optical antennas
  • nanoantennas
  • dynamics
  • spectroscopy
  • dna

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