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Ultrafast Dynamics of Nonrigid Zinc-Porphyrin Arrays Mimicking the Photosynthetic "Special Pair".
Moretti, Luca; Kudisch, Bryan; Terazono, Yuichi; Moore, Ana L; Moore, Thomas A; Gust, Devens; Cerullo, Giulio; Scholes, Gregory D; Maiuri, Margherita.
Afiliación
  • Moretti L; IFN-CNR, Dipartimento di Fisica, Politecnico di Milano, P.za Leonardo da Vinci 32, 20133 Milan, Italy.
  • Kudisch B; Department of Chemistry, Princeton University, Princeton, New Jersey 08540, United States.
  • Terazono Y; Department of Chemistry, Princeton University, Princeton, New Jersey 08540, United States.
  • Moore AL; School of Molecular Sciences, Arizona State University, Tempe, Arizona 85287, United States.
  • Moore TA; School of Molecular Sciences, Arizona State University, Tempe, Arizona 85287, United States.
  • Gust D; School of Molecular Sciences, Arizona State University, Tempe, Arizona 85287, United States.
  • Cerullo G; School of Molecular Sciences, Arizona State University, Tempe, Arizona 85287, United States.
  • Scholes GD; IFN-CNR, Dipartimento di Fisica, Politecnico di Milano, P.za Leonardo da Vinci 32, 20133 Milan, Italy.
  • Maiuri M; Department of Chemistry, Princeton University, Princeton, New Jersey 08540, United States.
J Phys Chem Lett ; 11(9): 3443-3450, 2020 May 07.
Article en En | MEDLINE | ID: mdl-32290662
Conjugated porphyrin arrays are heavily investigated as efficient molecular systems for photosynthesis and photocatalysis. Recently, a series of one-, two-, and six-zinc-porphyrin arrays, noncovalently linked through benzene-based hubs, have been synthesized with the aim of mimicking the structure and function of the bacteriochlorophyll "special pair" in photosynthetic reaction centers. The excitonically coupled porphyrin subunits are expected to activate additional excited state relaxation channels with respect to the monomer. Here, we unveil the appearance of such supramolecular electronic interactions using ultrafast transient absorption spectroscopy with sub-25 fs time resolution. Upon photoexcitation of the Soret band, we resolve energy trapping within ∼150 fs in a delocalized dark excitonic manifold. Moreover, excitonic interactions promote an additional fast internal conversion from the Q-band to the ground state with an efficiency of up to 60% in the hexamer. These relaxation pathways appear to be common loss channels that limit the lifetime of the exciton states in noncovalently bound molecular aggregates.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem Lett Año: 2020 Tipo del documento: Article País de afiliación: Italia Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem Lett Año: 2020 Tipo del documento: Article País de afiliación: Italia Pais de publicación: Estados Unidos