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Phys. Rev. Lett. 92, 083002 (2004) [4 pages]

Superexcited State Dynamics Probed with an Extreme-Ultraviolet Free Electron Laser

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Wen Li1,2, Robert R. Lucchese3, Adnan Doyuran4, Zilu Wu4, Henrik Loos4, Gregory E. Hall2, and Arthur G. Suits1,2,*
1Department of Chemistry, Stony Brook University, Stony Brook, New York 11794, USA
2Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973, USA
3Department of Chemistry, P.O. Box 30012, Texas A&M University, College Station, Texas 77842, USA
4National Synchrotron Light Source, Brookhaven National Laboratory, Upton, New York 11973, USA

Received 14 August 2003; published 27 February 2004

We present the first experimental results obtained with a high-gain harmonic generation extreme ultraviolet free electron laser. The experiment probes decay dynamics of superexcited states of methyl fluoride via ion pair imaging spectroscopy. Velocity mapped ion images of the fluoride ion, obtained with excitation via intense, coherent, subpicosecond pulses of 86–89 nm radiation, reveal low translational energy, implying very high internal excitation in the methyl cation cofragment. Angular distributions show changing anisotropy as the excitation energy is tuned through this region. The dynamics underlying the dissociation are discussed with the aid of theoretical calculations.

© 2004 The American Physical Society

URL:
http://link.aps.org/doi/10.1103/PhysRevLett.92.083002
DOI:
10.1103/PhysRevLett.92.083002
PACS:
33.80.Rv, 33.80.Eh, 34.50.Gb, 41.60.Cr

*Permanent address: Department of Chemistry, Wayne State University, Detroit, MI 48202, USA.

Electronic address: asuits@chem.wayne.edu