1. Transient resonant Auger-Meitner spectra of photoexcited thymine
- Author
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Wolf, Thomas J. A., Paul, Alexander C., Folkestad, Sarai D., Myhre, Rolf H., Cryan, James P., Berrah, Nora, Bucksbaum, Phil H., Coriani, Sonia, Coslovich, Giacomo, Feifel, Raimund, Martinez, Todd J., Moeller, Stefan P., Mucke, Melanie, Obaid, Razib, Plekan, Oksana, Squibb, Richard J., Koch, Henrik, Guehr, Markus, Wolf, Thomas J. A., Paul, Alexander C., Folkestad, Sarai D., Myhre, Rolf H., Cryan, James P., Berrah, Nora, Bucksbaum, Phil H., Coriani, Sonia, Coslovich, Giacomo, Feifel, Raimund, Martinez, Todd J., Moeller, Stefan P., Mucke, Melanie, Obaid, Razib, Plekan, Oksana, Squibb, Richard J., Koch, Henrik, and Guehr, Markus
- Abstract
We present the first investigation of excited state dynamics by resonant Auger-Meitner spectroscopy (also known as resonant Auger spectroscopy) using the nucleobase thymine as an example. Thymine is photoexcited in the UV and probed with X-ray photon energies at and below the oxygen K-edge. After initial photoexcitation to a pi pi* excited state, thymine is known to undergo internal conversion to an n pi* excited state with a strong resonance at the oxygen K-edge, red-shifted from the ground state pi* resonances of thymine (see our previous study Wolf, et al., Nat. Commun., 2017, 8, 29). We resolve and compare the Auger-Meitner electron spectra associated both with the excited state and ground state resonances, and distinguish participator and spectator decay contributions. Furthermore, we observe simultaneously with the decay of the n pi* state signatures the appearance of additional resonant Auger-Meitner contributions at photon energies between the n pi* state and the ground state resonances. We assign these contributions to population transfer from the n pi* state to a pi pi* triplet state via intersystem crossing on the picosecond timescale based on simulations of the X-ray absorption spectra in the vibrationally hot triplet state. Moreover, we identify signatures from the initially excited pi pi* singlet state which we have not observed in our previous study.
- Published
- 2021
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