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Observation of Ultrafast Intersystem Crossing in Thymine by Extreme Ultraviolet Time-Resolved Photoelectron Spectroscopy

Wolf, Thomas J. A.; Parrish, Robert M; Myhre, Rolf Heilemann; Martinez, Todd J.; Koch, Henrik; Gühr, Marcus
Journal article, Peer reviewed
Accepted version
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URI
http://hdl.handle.net/11250/2626449
Date
2019
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  • Publikasjoner fra CRIStin - NTNU [26648]
Original version
Journal of Physical Chemistry A. 2019, 123 (32), 6897-6903.   https://doi.org/10.1021/acs.jpca.9b05573
Abstract
We studied the photoinduced ultrafast relaxation dynamics of the nucleobase thymine using gas-phase time-resolved photoelectron spectroscopy. By employing extreme ultraviolet pulses from high harmonic generation for photoionization, we substantially extend our spectral observation window with respect to previous studies. This enables us to follow relaxation of the excited state population all the way to low-lying electronic states including the ground state. In thymine, we observe relaxation from the optically bright 1ππ* state of thymine to a dark 1nπ* state within 80 ± 30 fs. The 1nπ* state relaxes further within 3.5 ± 0.3 ps to a low-lying electronic state. By comparison with quantum chemical simulations, we can unambiguously assign its spectroscopic signature to the 3ππ* state. Hence, our study draws a comprehensive picture of the relaxation mechanism of thymine including ultrafast intersystem crossing to the triplet manifold.
Publisher
American Chemical Society
Journal
Journal of Physical Chemistry A

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