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Phys Rev Lett. 2007 May 18;98(20):203007. Epub 2007 May 17.

Probing orbital structure of polyatomic molecules by high-order harmonic generation.

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Blackett Laboratory, Imperial College London, London SW7 2BW, United Kingdom.

Erratum in

  • Phys Rev Lett. 2007 Jun 8;98(23):239903.


The effects of electronic structure and symmetry are observed in laser driven high-order harmonic generation for laser aligned conjugated polyatomic molecular systems. The dependence of the harmonic yield on the angle between the molecular axis and the polarization of the driving laser field is seen to contain the fingerprint of the highest occupied molecular orbitals in acetylene and allene, a good quantitative agreement with calculations employing the strong field approximation was found. These measurements support the extension of the recently proposed molecular orbital imaging techniques beyond simple diatomic molecules to larger molecular systems.

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