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We report on‐the‐fly surface‐hopping dynamics simulations of single adenine embedded in solvated DNA oligomers, (dA)10 and (dA)10·(dT)10. Both model systems are found to decay from the S1 to the S0 state via distinct monomeric channels, on account of the strong hydrogen‐bonding interactions between the Watson–Crick pair in the double‐stranded oligomer. Surprisingly, the decay times (several picoseconds)...
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