Influence of asymmetry and nodal planes on high-harmonic generation in heteronuclear molecules

The relation between high-harmonic spectra and the geometry of the molecular orbitals in position and momentum space is investigated. In particular we choose two isoelectronic pairs of homonuclear and heteronuclear molecules, such that the highest occupied molecular orbital of the former exhibit at least one nodal plane. The imprint of such planes is a strong suppression in the harmonic spectra, for particular alignment angles. We are able to identify two distinct types of nodal planes. If the nodal planes are determined by the atomic wavefunctions only, the angle for which the yield is suppressed will remain the same for both types of molecules. In contrast, if they are determined by the linear combination of atomic orbitals at different centers in the molecule, there will be a shift in the angle at which the suppression occurs for the heteronuclear molecules, with regard to their homonuclear counterpart. This shows that, in principle, molecular imaging, which uses the homonuclear molecule as a reference and enables one to observe the wavefunction distortions in its heteronuclear counterpart, is possible.Comment: 14 pages, 7 figures. Figs. 3, 5 and 6 have been simplified in order to comply with the arXiv size requirement

Excitation, two-center interference and the orbital geometry in laser-induced nonsequential double ionization of diatomic molecules

We address the influence of the molecular orbital geometry and of the molecular alignment with respect to the laser-field polarization on laser-induced nonsequential double ionization of diatomic molecules for different molecular species, namely $\mathrm{N}_2$ and $\mathrm{Li}_2$. We focus on the recollision excitation with subsequent tunneling ionization (RESI) mechanism, in which the first electron, upon return, promotes the second electron to an excited state, from where it subsequently tunnels. We show that the electron-momentum distributions exhibit interference maxima and minima due to the electron emission at spatially separated centers. We provide generalized analytical expressions for such maxima or minima, which take into account $s$ $p$ mixing and the orbital geometry. The patterns caused by the two-center interference are sharpest for vanishing alignment angle and get washed out as this parameter increases. Apart from that, there exist features due to the geometry of the lowest occupied molecular orbital (LUMO), which may be observed for a wide range of alignment angles. Such features manifest themselves as the suppression of probability density in specific momentum regions due to the shape of the LUMO wavefunction, or as an overall decrease in the RESI yield due to the presence of nodal planes.Comment: 11 pages revtex, 2 figure

Local dynamics in high-order harmonic generation using Bohmian trajectories

We investigate high-order harmonic generation from a Bohmian-mechanical perspective, and find that the innermost part of the core, represented by a single Bohmian trajectory, leads to the main contributions to the high-harmonic spectra. Using time-frequency analysis, we associate this central Bohmian trajectory to an ensemble of unbound classical trajectories leaving and returning to the core, in agreement with the three step model. In the Bohmian scenario, this physical picture builds up non-locally near the core via the quantum mechanical phase of the wavefunction. This implies that the flow of the wavefunction far from the core alters the central Bohmian trajectory. We also show how this phase degrades in time for the peripheral Bohmian trajectories as they leave the core region.Comment: 7 pages, 3 figures; the manuscript has been considerably extended and modified with regard to the previous version

High-harmonic generation from a confined atom

The order of high harmonics emitted by an atom in an intense laser field is limited by the so-called cutoff frequency. Solving the time-dependent Schr\"odinger equation, we show that this frequency can be increased considerably by a parabolic confining potential, if the confinement parameters are suitably chosen. Furthermore, due to confinement, the radiation intensity remains high throughout the extended emission range. All features observed can be explained with classical arguments.Comment: 4 pages(tex files), 4 figures(eps files); added references and comment

Enhancement of bichromatic high-harmonic generation with a high-frequency field

Using a high-frequency field superposed to a linearly polarized bichromatic laser field composed by a wave with frequency $\omega$ and a wave with frequency $2\omega$, we show it is possible to enhance the intensity of a group of high harmonics in orders of magnitude. These harmonics have frequencies about 30% higher than the monochromatic-cutoff frequency, and, within the three-step-model framework, correspond to a set of electron trajectories for which tunneling ionization is strongly suppressed. Particular features in the observed enhancement suggest that the high-frequency field provides an additional mechanism for the electron to reach the continuum. This interpretation is supported by a time-frequency analysis of the harmonic yield. The additional high frequency field permits the control of this group of harmonics leaving all other sets of harmonics practically unchanged, which is an advantage over schemes involving only bichromatic fields.Comment: 6 pages RevTex, 5 figures (ps files), Changes in text, figures, references and equations include

Nonsequential Double Ionization with Polarization-gated Pulses

We investigate laser-induced nonsequential double ionization by a polarization-gated laser pulse, constructed employing two counter-rotating circularly polarized few cycle pulses with a time delay $T_{d}$. We address the problem within a classical framework, and mimic the behavior of the quantum-mechanical electronic wave packet by means of an ensemble of classical electron trajectories. These trajectories are initially weighted with the quasi-static tunneling rate, and with suitably chosen distributions for the momentum components parallel and perpendicular to the laser-field polarization, in the temporal region for which it is nearly linearly polarized. We show that, if the time delay $T_{d}$ is of the order of the pulse length, the electron-momentum distributions, as functions of the parallel momentum components, are highly asymmetric and dependent on the carrier-envelope (CE) phase. As this delay is decreased, this asymmetry gradually vanishes. We explain this behavior in terms of the available phase space, the quasi-static tunneling rate and the recollision rate for the first electron, for different sets of trajectories. Our results show that polarization-gating technique may provide an efficient way to study the NSDI dynamics in the single-cycle limit, without employing few-cycle pulses.Comment: 17 pages, 6 figure

Classical and quantum-mechanical treatments of nonsequential double ionization with few-cycle laser pulses

We address nonsequential double ionization induced by strong, linearly polarized laser fields of only a few cycles, considering a physical mechanism in which the second electron is dislodged by the inelastic collision of the first electron with its parent ion. The problem is treated classically, using an ensemble model, and quantum-mechanically, within the strong-field and uniform saddle-point approximations. In the latter case, the results are interpreted in terms of "quantum orbits", which can be related to the trajectories of a classical electron in an electric field. We obtain highly asymmetric electron momentum distributions, which strongly depend on the absolute phase, i.e., on the phase difference between the pulse envelope and its carrier frequency. Around a particular value of this parameter, the distributions shift from the region of positive to that of negative momenta, or vice-versa, in a radical fashion. This behavior is investigated in detail for several driving-field parameters, and provides a very efficient method for measuring the absolute phase. Both models yield very similar distributions, which share the same physical explanation. There exist, however, minor discrepancies due to the fact that, beyond the region for which electron-impact ionization is classically allowed, the yields from the quantum mechanical computation decay exponentially, whereas their classical counterparts vanish.Comment: 12 pages revtex, 12 figures (eps files