Quantum
dynamics of H2
+ excited by two-cycle laser pulses with laser
carrier frequencies corresponding to the wavelengths λl = 800 and 200 nm (corresponding to the periods τl = 2.667 and 0.667 fs, respectively) and being linearly polarized
along the molecular axis have been studied by the numerical solution
of the non-Born–Oppenheimer time-dependent Schrödinger
equation within a three-dimensional (3D) model, including the internuclear
distance R and electron coordinates z and ρ. The amplitudes of the pulses have been chosen such
that the energies of H2
+ after the ends of the laser pulses, ⟨E⟩ ≈ −0.515 au, were close to the dissociation
threshold of H2
+. It is found that there exists a certain characteristic oscillation
frequency ωosc = 0.2278 au (corresponding to the
period τosc = 0.667 fs and the wavelength λosc = 200 nm) that plays the role of a “carrier”
frequency of temporally shaped oscillations of the expectation values
⟨−∂V/∂z⟩ emerging after the ends of the laser pulses, both at λl = 800 nm and at λl = 200 nm. Moreover, at
λl = 200 nm, the expectation value ⟨z⟩ also demonstrates temporally shaped oscillations
after the end of the laser pulse. In contrast, at λl = 800 nm, the characteristic oscillation frequency ωosc = 0.2278 au appears as the frequency of small-amplitude oscillations
of the slowly varying expectation value ⟨z⟩ which makes, after the end of the pulse, an excursion with
an amplitude of about 4.5 au along the z axis and
returns back to ⟨z⟩ ≈ 0 afterward.
It is found that the period of the temporally shaped post-field oscillations
of ⟨−∂V/∂z⟩ and ⟨z⟩, estimated as τshp ≈ 30 fs, correlates with the nuclear motion. It
is also shown that vibrational excitation of H2
+ is accompanied by the formation
of “hot” and “cold” vibrational ensembles
along the R degree of freedom. Power spectra related
to the electron motion in H2
+ calculated for both the laser-driven z and optically passive ρ degrees of freedom in the
acceleration form proved to be very interesting. In particular, both
odd and even harmonics can be observed.