Journal
SCIENCE
Volume 306, Issue 5702, Pages 1765-1768Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1104038
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We present experimental and theoretical evidence for an excited-state deactivation mechanism specific to hydrogen-bonded aromatic dimers, which may account, in part, for the photostability of the Watson-Crick base pairs in DNA. Femtosecond time-resolved mass spectroscopy of 2-aminopyridine clusters reveals an excited-state lifetime of 65+/-10 picoseconds for the near-planar hydrogen-bonded dimer, which is significantly shorter than the lifetime of either the monomer or the 3- and 4-membered nonplanar clusters. Ab initio calculations of reaction pathways and potential-energy profiles identify the mechanism of the enhanced excited-state decay of the dimer: Conical intersections connect the locally excited (1)pipi* state and the electronic ground state with a (1)pipi* charge-transfer state that is strongly stabilized by the transfer of a proton.
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