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Theory of high-order harmonic generation from molecules by intense laser pulses

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Anh-Thu Le1, R Della Picca2, P D Fainstein2, D A Telnov3, M Lein4 and C D Lin1

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We show that high-order harmonics generated from molecules by intense laser pulses can be expressed as the product of a returning electron wave packet and the photo-recombination cross section where the electron wave packet can be obtained from the simple strong-field approximation (SFA) or from a companion atomic target. Using these wave packets but replacing the photo-recombination cross sections obtained from SFA or from the atomic target by the accurate cross sections from molecules, the resulting high-order harmonic spectra are shown to agree well with the benchmark results from direct numerical solution of the time-dependent Schrödinger equation, for the case of H+2 in laser fields. The result illustrates that these powerful theoretical tools can be used for obtaining high-order harmonic spectra from molecules. More importantly, the results imply that the photo-recombination cross section extracted from laser-induced high-order harmonic spectra can be used for time-resolved dynamic chemical imaging of transient molecules with temporal resolutions down to a few femtoseconds.


PACS

33.80.-b Photon interactions with molecules

31.15.-p Calculations and mathematical techniques in atomic and molecular physics

42.65.Ky Frequency conversion; harmonic generation, including higher-order harmonic generation

Subjects

Atomic and molecular physics

Computational physics

Optics, quantum optics and lasers

Dates

Issue 8 (28 April 2008)

Received 15 February 2008

Published 3 April 2008



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