High Harmonic Generation from Multiple Orbitals in N 2 | Zendy

B. K. McFarland | Zendy; Joseph Farrell | Zendy; P. H. Bucksbaum | Zendy; Markus Gühr | Zendy

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High Harmonic Generation from Multiple Orbitals in N ₂

Author(s) -

B. K. McFarland,

Joseph Farrell,

P. H. Bucksbaum,

Markus Gühr

Publication year - 2008

Publication title -

science

Language(s) - English

Resource type - Journals

SCImago Journal Rank - 12.556

H-Index - 1186

eISSN - 1095-9203

pISSN - 0036-8075

DOI - 10.1126/science.1162780

Subject(s) - atomic physics , excited state , atomic orbital , high harmonic generation , molecular orbital , physics , electron , polarization (electrochemistry) , laser , molecule , molecular physics , chemistry , quantum mechanics

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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