Journal
JOURNAL OF PHYSICAL CHEMISTRY A
Volume 123, Issue 32, Pages 6897-6903Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.9b05573
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Funding
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division Office of Science Early Career Research Program through the Office of Basic Energy Sciences, U.S. Department of Energy [DE-SC0012376]
- Volkswagen foundation German National Academy of Sciences Leopoldina [LPDS2013-14]
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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 (1)pi pi* state of thymine to a dark (1)n pi* state within 80 +/- 30 fs. The (1)n pi* 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 (3)pi pi* state. Hence, our study draws a comprehensive picture of the relaxation mechanism of thymine including ultrafast intersystem crossing to the triplet manifold.
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