Ultrafast coherence transfer in DNA-templated silver nanoclusters

Erling Thyrhaug; Sidsel Ammitzbøll Bogh; Miguel Carro; Charlotte Stahl Madsen; Tom André Jos Vosch; Donatas Zigmantas

doi:10.1038/ncomms15577

Ultrafast coherence transfer in DNA-templated silver nanoclusters

Erling Thyrhaug^*, Sidsel Ammitzbøll Bogh, Miguel Carro, Charlotte Stahl Madsen, Tom André Jos Vosch, Donatas Zigmantas

^*Corresponding author for this work

Department of Chemistry

31 Citations (Scopus)

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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.

Original language	English
Article number	15577
Journal	Nature Communications
Volume	8
Number of pages	7
ISSN	2041-1723
DOIs	https://doi.org/10.1038/ncomms15577
Publication status	Published - 2017

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title = "Ultrafast coherence transfer in DNA-templated silver nanoclusters",

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.",

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T1 - Ultrafast coherence transfer in DNA-templated silver nanoclusters

AU - Thyrhaug, Erling

AU - Bogh, Sidsel Ammitzbøll

AU - Carro, Miguel

AU - Madsen, Charlotte Stahl

AU - Vosch, Tom André Jos

AU - Zigmantas, Donatas

PY - 2017

Y1 - 2017

N2 - 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.

AB - 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.

U2 - 10.1038/ncomms15577

DO - 10.1038/ncomms15577

M3 - Journal article

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SN - 2041-1723

VL - 8

JO - Nature Communications

JF - Nature Communications

M1 - 15577

ER -

Ultrafast coherence transfer in DNA-templated silver nanoclusters

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