Excitation of H+2 with one-cycle laser pulses: shaped post-laser-field electronic oscillations, generation of higher- and lower-order harmonics

Abstract

ABSTRACTNon-Born–Oppenheimer quantum dynamics of H+2 excited by shaped one-cycle laser pulses linearly polarised along the molecular axis have been studied by the numerical solution of the time-dependent Schrödinger equation within a three-dimensional model, including the internuclear separation, R, and the electron coordinates z and ρ. Laser carrier frequencies corresponding to the wavelengths λl = 25 nm through λl = 400 nm were used and the amplitudes of the pulses were chosen such that the energy of H+2 was close to its dissociation threshold at the end of any laser pulse applied. It is shown that there exists a characteristic oscillation frequency ωosc ≃ 0.2265 au (corresponding to the period of τosc ≃ 0.671 fs and the wavelength of λosc ≃ 201 nm) that manifests itself as a ‘carrier’ frequency of temporally shaped oscillations of the time-dependent expectation values ⟨z ⟩ and ⟨∂V/∂z ⟩ that emerge at the ends of the laser pulses and exist on a timescale of at least 50 fs. Time-dependent expectation values ⟨ρ⟩ and ⟨∂V /∂ρ⟩ of the optically passive degree of freedom, ρ, demonstrate post-laser-field oscillations at two basic frequencies ωρ1 ≈ ωosc and ωρ2 ≈ 2ωosc. Power spectra associated with the electronic motion show higher- and lower-order harmonics with respect to the driving field.