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We examine the dependences of the single and double ionization probabilities of NO radical on the angle between the NO axis and the laser polarization direction in an intense laser field (790 nm, 100 fs, 1–10 × 1014 W/cm2) and show that the double ionization is enhanced when the NO axis is parallel to the laser polarization direction. We reveal that the angular dependence of the sequential double ionization probability is determined by the shape of the 5σ orbital of NO+ from which the second photoelectron is emitted in the ionization from NO+ to NO2+. We also reveal that the fast oscillation in the probability of the tunnel ionization of NO originating from a coherent superposition of the two spin–orbit components in the electronic ground X2Π state is described well based on the molecular Ammosov-Delone-Krainov (MO-ADK) theory in which the time evolution of the electron density distribution of the 2π orbital is taken into account. [ABSTRACT FROM AUTHOR]

We numerically investigate the rotational dynamics of NO in the electronic ground X2Π state induced by an intense two-color laser field (10 TW/cm2) as a function of pulse duration (0.3–25 ps). In the short pulse duration of less than 12 ps, rotational Raman excitation is effectively induced and results in molecular orientation. On the contrary, when the pulse duration is longer than 15 ps, the rotational excitation is suppressed. In addition to the rotational excitation, we find that transitions between Λ-type doubling are induced. Significantly, the maximum coherent wave packet between Λ-type doubling in J = 0.5 is generated using the pulse duration of 19.8 ps. The wave packet changes to the eigenstates of Λ = +1 or −1 alternatively, where Λ is the projection of the electronic orbital angular momentum on the N–O axis, which is regarded as the unidirectional rotation of an unpaired 2π electron around the N–O axis in a space-fixed frame as well as in a molecule-fixed frame. The experimental method to observe the alternation of the rotational direction of the electron around the N–O axis is proposed. [ABSTRACT FROM AUTHOR]

We investigate the carrier-envelope phase (CEP) dependences of the single and double ionization processes of methanol (CH3OH) in an intense near-IR few-cycle laser field (2.1 × 1014 W/cm2) by the asymmetry in the ejection direction of CH3+ for the non-hydrogen migration channels and CH2+ for the hydrogen migration channels created through the C–O bond breaking after the ionization. Based on the absolute CEP values at the laser–molecule interaction point, calibrated by the method using intense few-cycle circularly polarized laser pulses [Fukahori et al., Phys. Rev. A 95, 053410-1–053410-14 (2017)], we confirm that methanol cations are produced by tunnel ionization and methanol dications are produced by the recollisional double ionization. We obtain the phase offset for the double ionization accompanying no hydrogen migration to be 1.85π as the absolute CEP at which the extent of the asymmetry becomes maximum. We interpret the phase shift of 0.85π from the phase offset of 1.0π for the tunnel ionization, estimated by a tunnel ionization model incorporating the chemical bond asymmetry, as the corresponding time delay associated with the electron recollisional ionization. The positive phase shift of 0.13π for the single ionization in the non-hydrogen migration channel is interpreted as the additional time (165 as) with which a methanol cation can be excited electronically prior to the decomposition. The additional phase shift of 0.22π for the single ionization in the hydrogen migration channel is interpreted as the additional time (280 as) required for a methanol cation to be excited electronically leading to the hydrogen migration prior to the decomposition. [ABSTRACT FROM AUTHOR]