Article (Scientific journals)
Coherent electronic and nuclear dynamics in a rhodamine heterodimer-DNA supramolecular complex
Cipolloni, M.; Fresch, B.; Occhiuto, I. et al.
2017In Physical Chemistry Chemical Physics, 19 (34), p. 23043-23051
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Abstract :
[en] 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. © 2017 the Owner Societies.
Research center :
Chimie Physique Theorique
Disciplines :
Chemistry
Author, co-author :
Cipolloni, M.;  Department of Chemical Sciences, University of Padova, via Marzolo 1, Padova, Italy
Fresch, B.;  Department of Chemical Sciences, University of Padova, via Marzolo 1, Padova, Italy, Theoretical Physical Chemistry, University of Liège, Allée du 6 Aout 11, Liège, Belgium
Occhiuto, I.;  Department of Chemical Sciences, University of Padova, via Marzolo 1, Padova, Italy
Rukin, P.;  Theoretical Physical Chemistry, University of Liège, Allée du 6 Aout 11, Liège, Belgium
Komarova, Ksenia G.;  Theoretical Physical Chemistry, University of Liège, Allée du 6 Aout 11, Liège, Belgium
Cecconello, A.;  Institute of Chemistry, Safra Campus, Hebrew University of Jerusalem, Jerusalem, Israel
Willner, I.;  Institute of Chemistry, Safra Campus, Hebrew University of Jerusalem, Jerusalem, Israel
Levine, Raphaël David;  Institute of Chemistry, Safra Campus, Hebrew University of Jerusalem, Jerusalem, Israel
Remacle, Françoise  ;  Université de Liège - ULiège > Département de chimie (sciences) > Laboratoire de chimie physique théorique
Collini, E.;  Department of Chemical Sciences, University of Padova, via Marzolo 1, Padova, Italy
Language :
English
Title :
Coherent electronic and nuclear dynamics in a rhodamine heterodimer-DNA supramolecular complex
Publication date :
2017
Journal title :
Physical Chemistry Chemical Physics
ISSN :
1463-9076
eISSN :
1463-9084
Publisher :
Royal Society of Chemistry
Volume :
19
Issue :
34
Pages :
23043-23051
Peer reviewed :
Peer Reviewed verified by ORBi
European Projects :
FP7 - 317707 - MULTI - MULTI-valued and parallel molecular logic
Name of the research project :
Multi valued and parallel molecular logic
Funders :
FET
CE - Commission Européenne [BE]
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