Signatures of nuclear motion in molecular high-order harmonics and in the generation of attosecond pulse trains by ultrashort intense laser pulses

Abstract

Non-Born–Oppenheimer time-dependent Shrödinger equation numerical simulations of the nonlinear nonperturbative response of 1D H2, H+2 molecules (and their isotopes) in few cycle intense 800 nm laser pulses are presented to study the effect of nuclear motion on molecular high-order harmonic generation. A time–frequency analysis is used to identify electron recollision and recombination times responsible for the generation of attosecond pulse trains during the nuclear motion. A very strong signature of nuclear motion is seen in the time profiles of high-order harmonics. In the case of high laser intensity (I ≃ 1015 W cm−2) the nuclear motion shortens the part of the attosecond pulse train originating from the first electron contribution and may enhance the onset of the second electron contribution for longer pulses. Molecular motion thus can act as an important ‘time-gating’ for controlling the length of generated attosecond pulses. The shape of time profiles of harmonics can thus be used for monitoring the nuclear motion. In the case of lower laser intensity, I ≃ 4 × 1014 W cm−2, we also find in time profiles a clear signature of electron excitation due to recollision of the returning electron.