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Quantum interference during high-order harmonic generation from aligned molecules

Nature volume 435, pages 470–474 (2005)Cite this article

Abstract

High-order harmonic generation (HHG) from atoms and molecules offers potential application as a coherent ultrashort radiation source in the extreme ultraviolet and soft X-ray regions1,2,3. In the three-step model4,5,6 of HHG, an electron tunnels out from the atom and may recombine with the parent ion (emitting a high-energy photon) after undergoing laser-driven motion in the continuum. Aligned molecules7,8,9,10,11 can be used to study quantum phenomena in HHG associated with molecular symmetries; in particular, simultaneous observations of both ion yields and harmonic signals under the same conditions serve to disentangle the contributions from the ionization and recombination processes. Here we report evidence for quantum interference of electron de Broglie waves12,13,14 in the recombination process of HHG from aligned CO2 molecules. The interference takes place within a single molecule and within one optical cycle. Characteristic modulation patterns of the harmonic signals measured as a function of the pump–probe delay are explained with simple formulae determined by the valence orbital of the molecules. We propose that simultaneous observations of both ion yields and harmonic signals can serve as a new route to probe the instantaneous structure of molecular systems.

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Figure 1: The time evolution of the ion yield and the 23rd harmonic intensity from N 2 molecules.
Figure 2: The time evolution of the ion yield and the 23rd harmonic intensity from O 2 molecules.
Figure 3: The time evolution of the ion yield and the 23rd harmonic intensity from CO 2 molecules, and an illustration of the model of two point emitters.
Figure 4: The integrated signals of high-order harmonics measured as a function of the harmonic order.

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Acknowledgements

This work was supported by Grants-in-Aid from the Japan Society for the Promotion of Science and from the Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japan.

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  1. Department of Physics, Graduate School of Science, The University of Tokyo, 7-3-1, Hongo, Bunkyo-ku, Tokyo, 113-0033, Japan

    Tsuneto Kanai, Shinichirou Minemoto & Hirofumi Sakai

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  1. Tsuneto Kanai
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  3. Hirofumi Sakai
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Correspondence to Hirofumi Sakai.

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Kanai, T., Minemoto, S. & Sakai, H. Quantum interference during high-order harmonic generation from aligned molecules. Nature 435, 470–474 (2005). https://doi.org/10.1038/nature03577

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