Proton-coupled energy transfer in molecular triads.

Autor: Pettersson Rimgard B; Department of Chemistry - Ångström Laboratory, Uppsala University, SE 75120 Uppsala, Sweden., Tao Z; Department of Chemistry, Yale University, New Haven, CT 06520, USA., Parada GA; Department of Chemistry, Yale University, New Haven, CT 06520, USA.; Department of Chemistry, College of New Jersey, Ewing, NJ 08628, USA., Cotter LF; Department of Chemistry, Yale University, New Haven, CT 06520, USA., Hammes-Schiffer S; Department of Chemistry, Yale University, New Haven, CT 06520, USA., Mayer JM; Department of Chemistry, Yale University, New Haven, CT 06520, USA., Hammarström L; Department of Chemistry - Ångström Laboratory, Uppsala University, SE 75120 Uppsala, Sweden.
Jazyk: angličtina
Zdroj: Science (New York, N.Y.) [Science] 2022 Aug 12; Vol. 377 (6607), pp. 742-747. Date of Electronic Publication: 2022 Jul 21.
DOI: 10.1126/science.abq5173
Abstrakt: We experimentally discovered and theoretically analyzed a photochemical mechanism, which we term proton-coupled energy transfer (PCEnT). A series of anthracene-phenol-pyridine triads formed a local excited anthracene state after light excitation at a wavelength of ~400 nanometers (nm), which led to fluorescence around 550 nm from the phenol-pyridine unit. Direct excitation of phenol-pyridine would have required ~330-nm light, but the coupled proton transfer within the phenol-pyridine unit lowered its excited-state energy so that it could accept excitation energy from anthracene. Singlet-singlet energy transfer thus occurred despite the lack of spectral overlap between the anthracene fluorescence and the phenol-pyridine absorption. Moreover, theoretical calculations indicated negligible charge transfer between the anthracene and phenol-pyridine units. We construe PCEnT as an elementary reaction of possible relevance to biological systems and future photonic devices.
Databáze: MEDLINE
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