Following a chemical reaction using high-harmonic interferometry

H. J. Wörner, J. B. Bertrand, D. V. Kartashov, P. B. Corkum and D. M. Villeneuve ()
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H. J. Wörner: Joint Laboratory for Attosecond Science, National Research Council of Canada and University of Ottawa, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada
J. B. Bertrand: Joint Laboratory for Attosecond Science, National Research Council of Canada and University of Ottawa, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada
D. V. Kartashov: Joint Laboratory for Attosecond Science, National Research Council of Canada and University of Ottawa, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada
P. B. Corkum: Joint Laboratory for Attosecond Science, National Research Council of Canada and University of Ottawa, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada
D. M. Villeneuve: Joint Laboratory for Attosecond Science, National Research Council of Canada and University of Ottawa, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada

Nature, 2010, vol. 466, issue 7306, 604-607

Abstract: Reaction tracking with high-harmonic spectroscopy New methods are emerging that aim to image chemical reactions as they occur, using X-ray diffraction, electron diffraction or laser-induced recollision. But none of these methods offer spectral selection, which allows a laser pulse with light of one wavelength to initiate a reaction, and a second pulse with another, appropriately selected wavelength to monitor the reacting molecules. Wörner et al. now show that this apparent limitation offers exciting opportunities for recollision-based high-harmonic spectroscopy: due to the coherent nature of the attosecond high-harmonic pulse generation, unexcited molecules can act as local oscillators against which structural and electronic dynamics is observed on an attosecond timescale. High-harmonic spectroscopy thus seems ideally suited to measure coupled electronic and nuclear dynamics in fast photochemical reactions, or to characterize short-lived transition states.

Date: 2010
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DOI: 10.1038/nature09185

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