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• W2016048877 abstract "The DNA base adenine and four monomethylated adenines were studied in solution at room temperature by femtosecond pump−probe spectroscopy. Transient absorption at visible probe wavelengths was used to directly observe relaxation of the lowest excited singlet state (S1 state) populated by a UV pump pulse. In H2O, transient absorption signals from adenine decay biexponentially with lifetimes of 0.18 ± 0.03 ps and 8.8 ± 1.2 ps. In contrast, signals from monomethylated adenines decay monoexponentially. The S1 lifetimes of 1-, 3-, and 9-methyladenine are similar to one another and are all below 300 fs, while 7-methyladenine has a significantly longer lifetime (τ = 4.23 ± 0.13 ps). On this basis, the biexponential signal of adenine is assigned to an equilibrium mixture of the 7H- and 9H-amino tautomers. Excited-state absorption (ESA) by 9-methyladenine is 50% stronger than by 7-methyladenine. Assuming that ESA by the corresponding tautomers of adenine is unchanged, we estimate the population of 7H-adenine in H2O at room temperature to be 22 ± 4% (estimated standard deviation). To understand how the environment affects nonradiative decay, we performed the first solvent-dependent study of nucleobase dynamics on the ultrafast time scale. In acetonitrile, both lowest energy tautomers of adenine are present in roughly similar proportions as in water. The lifetimes of the 9-substituted adenines depend somewhat more sensitively on the solvent than those of the 7-substituted adenines. Transient signals for adenine in H2O and D2O are identical. These solvent effects strongly suggest that excited-state tautomerization is not an important nonradiative decay pathway. Instead, the data are most consistent with electronic energy relaxation due to state crossings between the optically prepared 1ππ* state and one or more 1nπ* states and the electronic ground state. The pattern of lifetimes measured for the monomethylated adenines suggests a special role for the 1nπ* state associated with the N7 electron lone pair." @default.
• W2016048877 created "2016-06-24" @default.
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• W2016048877 date "2003-10-10" @default.
• W2016048877 modified "2023-10-12" @default.
• W2016048877 title "Ultrafast Excited-State Dynamics of Adenine and Monomethylated Adenines in Solution: Implications for the Nonradiative Decay Mechanism" @default.
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• W2016048877 doi "https://doi.org/10.1021/ja035628z" @default.
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