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Issue 34, 2017
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Coherent electronic and nuclear dynamics in a rhodamine heterodimer–DNA supramolecular complex

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Abstract

Elucidating the role of quantum coherences in energy migration within biological and artificial multichromophoric antenna systems is the subject of an intense debate. It is also a practical matter because of the decisive implications for understanding the biological processes and engineering artificial materials for solar energy harvesting. A supramolecular rhodamine heterodimer on a DNA scaffold was suitably engineered to mimic the basic donor–acceptor unit of light-harvesting antennas. Ultrafast 2D electronic spectroscopic measurements allowed identifying clear features attributable to a coherent superposition of dimer electronic and vibrational states contributing to the coherent electronic charge beating between the donor and the acceptor. The frequency of electronic charge beating is found to be 970 cm−1 (34 fs) and can be observed for 150 fs. Through the support of high level ab initio TD-DFT computations of the entire dimer, we established that the vibrational modes preferentially optically accessed do not drive subsequent coupling between the electronic states on the 600 fs of the experiment. It was thereby possible to characterize the time scales of the early time femtosecond dynamics of the electronic coherence built by the optical excitation in a large rigid supramolecular system at a room temperature in solution.

Graphical abstract: Coherent electronic and nuclear dynamics in a rhodamine heterodimer–DNA supramolecular complex

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Publication details

The article was received on 01 Mar 2017, accepted on 11 Jul 2017 and first published on 17 Aug 2017


Article type: Paper
DOI: 10.1039/C7CP01334E
Citation: Phys. Chem. Chem. Phys., 2017,19, 23043-23051
  • Open access: Creative Commons BY-NC license
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    Coherent electronic and nuclear dynamics in a rhodamine heterodimer–DNA supramolecular complex

    M. Cipolloni, B. Fresch, I. Occhiuto, P. Rukin, K. G. Komarova, A. Cecconello, I. Willner, R. D. Levine, F. Remacle and E. Collini, Phys. Chem. Chem. Phys., 2017, 19, 23043
    DOI: 10.1039/C7CP01334E

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