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Title: Electronic coherences in nonadiabatic molecular photophysics revealed by time-resolved photoelectron spectroscopy
Time-resolved photoelectron spectroscopy (TRPES) signals that monitor the relaxation of the RNA base uracil upon optical excitation are simulated. Distinguishable signatures of coherence dynamics at conical intersections are identified, with temporal and spectral resolutions determined by the duration of the ionizing probe pulse. The frequency resolution of the technique, either directly provided by the signal or retrieved at the data-processing stage, can magnify the contribution from molecular coherences, enabling the extraction of most valuable information about the nonadiabatic molecular dynamics. The predicted coherence signatures in TRPES could be experimentally observed with existing ultrashort pulses from high-order harmonic generation or free-electron lasers.  more » « less
Award ID(s):
1953045
PAR ID:
10340557
Author(s) / Creator(s):
; ;
Date Published:
Journal Name:
Proceedings of the National Academy of Sciences
Volume:
119
Issue:
11
ISSN:
0027-8424
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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