High Harmonic Generation from Multiple Orbitals in N2

Journal Article · Thu Mar 05 00:00:00 EST 2009 · Science 322:1232-1235,2008

OSTI ID:1018525

McFarland, B; Farrell, Joseph P; Bucksbaum, Philip H; Guehr, Markus

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 N{sub 2} 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 N{sub 2} 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.

• Research Organization: SLAC National Accelerator Lab., Menlo Park, CA (United States)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC02-76SF00515
• OSTI ID: 1018525
• Report Number(s): SLAC-PUB-13406; SCEHDK; TRN: US201114%%45
• Journal Information: Science 322:1232-1235,2008, Vol. 322, Issue 5905; ISSN 0193-4511
• Country of Publication: United States
• Language: English

Related Subjects

71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
ELECTRONS
HARMONIC GENERATION
LASERS
POLARIZATION
Other
OPTICS