Ultrafast coherence transfer in DNA-templated silver nanoclusters

TY - JOUR

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

C2 - 28548085

AN - SCOPUS:85020006548

SN - 2041-1723

VL - 8

JO - Nature Communications

JF - Nature Communications

M1 - 15577

ER -