Anomalous alignment dependence of the third-order harmonic of H 2+ ions in intense laser fields

Abstract

We studied the high-harmonic generation of H2+ ions in an intense laser field by solving the time-dependent Schrödinger equation in prolate spheroidal coordinates. By analyzing the power spectra of the harmonics with the electric field polarized along the molecular axis, we found that the yield of the third-order harmonic drops by several orders of magnitude at a specified aligned angle between the laser polarization direction and the molecular axis. The laser polarization angle of the minimum depends on the internuclear distance and it disappears both in the separated- and united-atom limits. This infers that the minimum is associated with the molecular symmetry. By decomposing individual contributions of the σ and π states, we identified that the minimum is attributed to the cancellation of the induced dipole moments of the σ and π states, like a dynamical Cooper minimum, but the position of the minimum can be tuned by the laser intensity for a given internuclear distance. © 2012 American Physical Society.