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Title: Involvement of a low-lying Rydberg state in the ultrafast relaxation dynamics of ethylene

We present a measurement of the time-resolved photoelectron kinetic energy spectrum of ethylene using 156 nm and 260 nm laser pulses. The 156 nm pulse first excites ethylene to the {sup 1}B{sub 1u} (ππ{sup ∗}) electronic state where 260 nm light photoionizes the system to probe the relaxation dynamics with sub-30 fs resolution. Recent ab initio calculations by Mori et al. [J. Phys. Chem. A 116, 2808-2818 (2012)] have predicted an ultrafast population transfer from the initially excited state to a low-lying Rydberg state during the relaxation of photoexcited ethylene. The measured photoelectron kinetic energy spectrum reveals wave packet motion on the valence state and shows indications that the low-lying π3s Rydberg state is indeed transiently populated via internal conversion following excitation to the ππ{sup ∗} state, supporting the theoretical predictions.
Authors:
 [1] ;  [2] ; ;  [3] ;  [3] ;  [2] ;  [3] ;  [4] ;  [3] ;  [2]
  1. Graduate Group in Applied Science and Technology, University of California, Berkeley, California 94720 (United States)
  2. (United States)
  3. Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)
  4. (China)
Publication Date:
OSTI Identifier:
22493615
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 144; Journal Issue: 1; Other Information: (c) 2016 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ETHYLENE; EXCITATION; INTERNAL CONVERSION; KINETIC ENERGY; LASER RADIATION; PHOTOIONIZATION; PROBES; RELAXATION; RYDBERG STATES; TIME RESOLUTION; TRANSIENTS; VALENCE; VISIBLE RADIATION; WAVE PACKETS