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Published Online March 2, 2006
Science DOI: 10.1126/science.1123904

Reports

Submitted on December 15, 2005
Accepted on February 13, 2006

Probing Proton Dynamics in Molecules on an Attosecond Time Scale

S. Baker 1, J. S. Robinson 1, C. A. Haworth 1, H. Teng 1, R. A. Smith 1, C. C. Chirila 2, M. Lein 2, J. W. G. Tisch 1, J. P. Marangos 1*

1 Blackett Laboratory, Imperial College London, Prince Consort Road, South Kensington, London SW7 2BZ, UK.
2 Max Planck Institute for Nuclear Physics, Saupfercheckweg 1, 69117 Heidelberg, Germany.

We demonstrate a new technique using high order harmonic generation in molecules to probe nuclear dynamics and structural rearrangement on a sub-femtosecond timescale. The chirped nature of the electron wavepacket produced by laser ionization in a strong field gives rise to a similar chirp in the photons emitted upon electron-ion recombination. Use of this chirp in the emitted light allows information about nuclear dynamics to be gained with 100 attosecond temporal resolution, from excitation by an 8 fs pulse, in a single laser shot. Measurements on H2 and D2 agree well with calculations of ultra-fast nuclear dynamics in the H2+ molecule, confirming the validity of the method. Guided by this result, we have measured harmonic spectra from CH4 and CD4 to demonstrate a few-femtosecond timescale for the onset of proton rearrangement in methane upon ionization.


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