Ultrafast coherence transfer in DNA-templated silver nanoclusters

Erling Thyrhaug (), Sidsel Ammitzbøll Bogh, Miguel R Carro-Temboury, Charlotte Stahl Madsen, Tom Vosch and Donatas Zigmantas ()
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Erling Thyrhaug: Chemical Physics and NanoLund, Lund University
Sidsel Ammitzbøll Bogh: University of Copenhagen
Miguel R Carro-Temboury: University of Copenhagen
Charlotte Stahl Madsen: University of Copenhagen
Tom Vosch: University of Copenhagen
Donatas Zigmantas: Chemical Physics and NanoLund, Lund University

Nature Communications, 2017, vol. 8, issue 1, 1-7

Abstract: Abstract DNA-templated silver nanoclusters of a few tens of atoms or less have come into prominence over the last several years due to very strong absorption and efficient emission. Applications in microscopy and sensing have already been realized, however little is known about the excited-state structure and dynamics in these clusters. Here we report on a multidimensional spectroscopy investigation of the energy-level structure and the early-time relaxation cascade, which eventually results in the population of an emitting state. We find that the ultrafast intramolecular relaxation is strongly coupled to a specific vibrational mode, resulting in the concerted transfer of population and coherence between excited states on a sub-100 fs timescale.

Date: 2017
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DOI: 10.1038/ncomms15577

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