High harmonic generation from multiple orbitals in N2 |
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| Authors: | McFarland Brian K Farrell Joseph P Bucksbaum Philip H Gühr Markus |
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| Affiliation: | PULSE Institute, SLAC, Menlo Park, CA 94025, USA, and Departments of Physics and Applied Physics, Stanford University, Stanford, CA 94305, USA. |
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| Abstract: | 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. |
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