Journal article · Preprint article
Transient resonant Auger-Meitner spectra of photoexcited thymine
SLAC National Accelerator Laboratory1
University of Potsdam2
Norwegian University of Science and Technology3
University of Connecticut4
Stanford University School of Medicine5
Department of Chemistry, Technical University of Denmark6
University of Gothenburg7
Uppsala University Hospital8
Sincrotrone Trieste9
Scuola Normale Superiore di Pisa10
...and 0 moreWe 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 ππ* excited state, thymine is known to undergo internal conversion to an nπ* excited state with a strong resonance at the oxygen K-edge, red-shifted from the ground state π* 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 nπ* state signatures the appearance of additional resonant Auger-Meitner contributions at photon energies between the nπ* state and the ground state resonances.
We assign these contributions to population transfer from the nπ* state to a ππ* 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 ππ* singlet state which we have not observed in our previous study.
Language: | English |
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Publisher: | The Royal Society of Chemistry |
Year: | 2021 |
Pages: | 555-570 |
ISSN: | 13645498 and 13596640 |
Types: | Journal article and Preprint article |
DOI: | 10.1039/d0fd00112k |
ORCIDs: | 0000-0002-0641-1279 , 0000-0002-7547-445X , 0000-0002-7776-0919 , 0000-0003-3231-1164 , Coriani, Sonia , 0000-0001-5234-3935 , 0000-0002-4798-8947 , 0000-0002-1759-4752 and 0000-0002-8367-8727 |