Electronic Properties of Ï€-conjugated Materials II - UniversitÃ¤t ...

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Invited Lectures – 8 π 2011 Ultrafast excited-state dynamics of multichromophoric systems Eric Vauthey University of Geneva Molecular systems containing several identical chromophoric units have found many types of applications, from artificial photosynthesis to DNA detection and molecular electronics. We will present some of our results obtained by ultrafast optical spectroscopy with various multichromophoric systems going from molecules with two chromophoric units to more complex systems with up to ten units. We will concentrate on two main processes that can take place in these arrays: excitation energy hopping and charge transfer. �e first one is common to most systems and takes place within a few picoseconds. We will show that the dynamics of energy hopping in a bichromophoric system intercalated into DNA can yield interesting conformational information.[1] Photoinduced charge separation (CS) between identical chromophoric units is less common and we will discuss some of our efforts to understand the direction of the charges in such symmetrybreaking process.[2] Finally, the excited-state dynamics of multichromophoric systems consisting of eight to ten coresubstituted naphtahlenediimide (NDI) chromophores covalently a�ached to a p-octiphenyl (POP) or an oligophenylethynyl (OPE) scaffold will be discussed. It will be shown that in a lipid bilayer, POP-NDI systems self-organise in a tetrameric architecture allowing photoinduced transmembrane electron transport.[3] Both POP-NDI and OPE-NDI systems also self-assemble on gold surfaces resulting to photocurrent generation.[4] All the CS pathways as well as the ensuing charge recombination (CR) channels have been elucidated.[5, 6] Our investigations reveal that, depending on the nature of the NDI core-substituents and on the scaffold, as well as on the excitation wavelength, either symmetry breaking CS between two NDI moieties or CS between the scaffold and a NDI unit take place. �ese processes result to charge-separated states with different lifetimes and thus different efficiencies for photocurrent generation. Although very long-lived charge separation (> ms) was not realised in these systems, this study opens several promising new avenues for ultrafast CS and slow CR. 36
π 2011 References Invited Lectures – 8 [1] A. Fürstenberg, M. D. Julliard, T. G. Deligeorgiev, N. I. Gadjev, A. A. Vassilev, E. Vauthey, J. Am. Chem. Soc. 128, 7661 (2006) [2] V. Markovic, D. Villamaina, I. Barabanov, L. M. Lawson Daku, E. Vauthey, Angew. Chem. Int. Ed. 50, 7596 (2011) [3] S. Bhosale, S. A. L., P. Talukdar, A. Fürstenberg, N. Banerji, E. Vauthey,G. Bollot, J. Mareda, C. Röger, F. Würthner, N. Sakai, S. Matile, Science 313, 84 (2006) [4] A. L. Sisson, N. Sakai, N. Banerji, A. Fürstenberg, E. Vauthey, S. Matile, Angew. Chem. Int. Ed. 47, 3727 (2008) [5] N. Banerji, A. Fürstenberg, S. Bhosale, A. L. Sisson, N. Sakai, S. Matile, E. Vauthey, J. Phys. Chem. B 112, 8912 (2008) [6] N. Banerji, G. Duvanel, A. Perez-Velasco, S. Maity, N. Sakai, S. Matile, E. Vauthey, J. Am. Chem. Soc. 128, 7661 (2006) N�� 37 Lectures
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