Abstract

A quantum description of the one-electron triangular H${}_{3}^{2+}$ molecular ion, beyond the Born-Oppenheimer approximation, is used to study the full influence of the nuclear motion on the high-intensity photoionization and harmonic generation processes. A detailed analysis of electron and proton motions and their time-dependent acceleration allows for identification of the main electron recollision events as a function of time-dependent configuration of the protons. High-order-harmonic generation photons are shown to be produced by single-electron recollision in the second half of the pulse envelope, which also induces a redshift in the harmonics, due to the rapid few-femtosecond motions of protons. Perpendicular harmonics are produced, in general, with a linearly polarized laser pulse parallel to a bond of the triangular molecule, and, in particular, the harmonics in the cutoff region are elliptically polarized. When the laser-pulse polarization is parallel to a symmetry axis of the triangular molecular ion, creation and destruction of the chemical bond perpendicular to the polarization is predicted on a near-femtosecond time scale.

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