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Originally published in Science Express on 2 March 2006
Science 21 April 2006:
Vol. 312. no. 5772, pp. 424 - 427
DOI: 10.1126/science.1123904
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Reports

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. Marangos1*

We demonstrate a technique that uses high-order harmonic generation in molecules to probe nuclear dynamics and structural rearrangement on a subfemtosecond time scale. 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-femtosecond pulse, in a single laser shot. Measurements on molecular hydrogen and deuterium agreed well with calculations of ultrafast nuclear dynamics in the H2+ molecule, confirming the validity of the method. We then measured harmonic spectra from CH4 and CD4 to demonstrate a few-femtosecond time scale for the onset of proton rearrangement in methane upon ionization.

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.

* To whom correspondence should be addressed. E-mail: j.marangos{at}imperial.ac.uk

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