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• W2094247157 startingPage "11225" @default.
• W2094247157 abstract "Electronic relaxation pathways in photoexcited nucleobases have received much theoretical and experimental attention due to their underlying importance to the UV photostability of these biomolecules. Multiple mechanisms with different energetic onsets have been proposed by ab initio calculations yet the majority of experiments to date have only probed the photophysics at a few selected excitation energies. We present femtosecond time-resolved photoelectron spectra (TRPES) of the DNA base adenine in a molecular beam at multiple excitation energies between 4.7−6.2 eV. The two-dimensional TRPES data is fit globally to extract lifetimes and decay associated spectra for unambiguous identification of states participating in the relaxation. Furthermore, the corresponding amplitude ratios are indicative of the relative importance of competing pathways. We adopt the following mechanism for the electronic relaxation of isolated adenine; initially the S2(ππ*) state is populated by all excitation wavelengths and decays quickly within 100 fs. For excitation energies below ∼5.2 eV, the S2(ππ*)→S1(nπ*)→S0 pathway dominates the deactivation process. The S1(nπ*)→S0 lifetime (1032−700 fs) displays a trend toward shorter time constants with increasing excitation energy. On the basis of relative amplitude ratios, an additional relaxation channel is identified at excitation energies above 5.2 eV." @default.
• W2094247157 created "2016-06-24" @default.
• W2094247157 creator A5020573040 @default.
• W2094247157 creator A5024661346 @default.
• W2094247157 date "2010-07-15" @default.
• W2094247157 modified "2023-09-30" @default.
• W2094247157 title "Wavelength Dependence of Electronic Relaxation in Isolated Adenine Using UV Femtosecond Time-Resolved Photoelectron Spectroscopy" @default.
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• W2094247157 doi "https://doi.org/10.1021/jp1029097" @default.
• W2094247157 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/20961159" @default.
• W2094247157 hasPublicationYear "2010" @default.
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