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Originally published in Science Express on 30 October 2008
Science 21 November 2008:
Vol. 322. no. 5905, pp. 1232 - 1235
DOI: 10.1126/science.1162780
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Reports

High Harmonic Generation from Multiple Orbitals in N2

Brian K. McFarland, Joseph P. Farrell, Philip H. Bucksbaum, Markus Gühr*

Molecular electronic states energetically below the highest occupied molecular orbital (HOMO) should contribute to laser-driven high harmonic generation (HHG), but this behavior has not been observed previously. Our measurements of the HHG spectrum of N2 molecules aligned perpendicular to the laser polarization showed a maximum at the rotational half-revival. This feature indicates the influence of electrons occupying the orbital just below the N2 HOMO, referred to as the HOMO-1. Such observations of lower-lying orbitals are essential to understanding subfemtosecond/subangstrom electronic motion in laser-excited molecules.

PULSE Institute, SLAC, Menlo Park, CA 94025, USA, and Departments of Physics and Applied Physics, Stanford University, Stanford, CA 94305, USA.

* To whom correspondence should be addressed. E-mail: mguehr{at}stanford.edu

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Science. ISSN 0036-8075 (print), 1095-9203 (online)