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Excitation Dynamics in Hetero‐bichromophoric Calixarene Systems
Authors:Dr Irene Tosi  Dr Mireia Segado Centellas  Dr Elisa Campioli  Dr Alessandro Iagatti  Dr Andrea Lapini  Dr Cristina Sissa  Prof Laura Baldini  Prof Chiara Cappelli  Dr Mariangela Di Donato  Prof Francesco Sansone  Dr Fabrizio Santoro  Prof Francesca Terenziani
Institution:1. Dipartimento di Chimica, Università di Parma, Parco Area delle Scienze 17/a, Parma, Italy;2. Scuola Normale Superiore, Pisa, Italy;3. LENS (European Laboratory for Non Linear Spectroscopy), Sesto Fiorentino (FI), Italy;4. INO (Istituto Nazionale di Ottica), Firenze, Italy;5. Dipartimento di Chimica “Ugo Schiff”, Università di Firenze, Sesto Fiorentino (FI), Italy;6. CNR-Consiglio Nazionale delle Ricerche, Istituto di Chimica dei Composti Organo Metallici (ICCOM-CNR), Pisa, Italy
Abstract:In this work, the dynamics of electronic energy transfer (EET) in bichromophoric donor–acceptor systems, obtained by functionalizing a calix4]arene scaffold with two dyes, was experimentally and theoretically characterized. The investigated compounds are highly versatile, due to the possibility of linking the dye molecules to the cone or partial cone structure of the calix4]arene, which directs the two active units to the same or opposite side of the scaffold, respectively. The dynamics and efficiency of the EET process between the donor and acceptor units was investigated and discussed through a combined experimental and theoretical approach, involving ultrafast pump–probe spectroscopy and density functional theory based characterization of the energetic and spectroscopic properties of the system. Our results suggest that the external medium strongly determines the particular conformation adopted by the bichromophores, with a direct effect on the extent of excitonic coupling between the dyes and hence on the dynamics of the EET process itself.
Keywords:density functional calculations  donor–  acceptor systems  energy transfer  solvent effects  ultrafast spectroscopy
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