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

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 light-harvesting 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 ~20 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 non-classical 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.
- Geballe Laboratory for Advanced Materials
- Institute of Photonic Sciences Spain
- FUNDACIO INSTITUT DE CIENCIES FOTONIQUES Spain
- Stanford University United States
- Wageningen University & Research Netherlands
spectroscopy, Photons, purple bacterial lh2, exciton delocalization, pigment-protein complexes, Light-Harvesting Protein Complexes, optical antennas, dynamics, dna, Fluorescence, Nanostructures, Rhodopseudomonas, energy-transfer, nanoantennas, Bacterial Proteins, Energy Transfer, molecule fluorescence, Gold
spectroscopy, Photons, purple bacterial lh2, exciton delocalization, pigment-protein complexes, Light-Harvesting Protein Complexes, optical antennas, dynamics, dna, Fluorescence, Nanostructures, Rhodopseudomonas, energy-transfer, nanoantennas, Bacterial Proteins, Energy Transfer, molecule fluorescence, Gold
citations This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).114 popularity This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.Top 1% influence This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).Top 10% impulse This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.Top 1% download downloads 14 - 14downloads
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