The contributions of two energetically highest molecular orbitals to the harmonic emission rate are analysed for a two-component laser field. For diatomic molecules exposed to the elliptically polarised field, the emission from the highest-occupied molecular orbital (HOMO) is dominant for various molecular orientations with respect to the laser field. However, the contribution of the lower molecular orbital (HOMO-1) can become significant or even dominant for some molecular orientations. We introduce the ratio of the coherent over the incoherent sum of the HOMO and HOMO-1 contributions as a quantitative measure of the significance of the particular molecular orbital. Also, the gaseous medium response is different for the left and right elliptically polarised light and the molecular characteristics are imprinted into this difference. Moreover, for the orthogonally polarised two-colour (OTC) laser field the relative contributions of HOMO and HOMO-1 depend to a great extent on the relative phase between the field components. The importance of the HOMO-1 can be assessed by the relative error which is made if the harmonic spectra are obtained only with the HOMO contribution. Finally, we investigate the interference of the contributions of two highest molecular orbitals. We show that, for the OTC field, the destructive interference depends linearly on the intensity of the field components. Also, the interference minima shift towards the higher energies with the increase of the component wavelength.

Nondipole effects occurring in the process of atomic ionization by an intense, mid‐infrared, counter‐rotating bicircular laser field are investigated using the strong‐field approximation with leading‐order nondipole corrections. The time integrals appearing in the expression for the differential ionization rate are computed in two ways: numerically, and by applying the saddle‐point approximation. The nondipole corrections introduce an asymmetry in the photoelectron momentum distribution along the field propagation direction. The asymmetry is quantified by the partial average value of the propagation‐direction momentum component of the photoelectrons and by the normalized difference of the differential ionization rates computed including and excluding the nondipole corrections. Using the saddle‐point approximation, it is investigated how the nondipole corrections change the solutions for direct photoelectrons and how this affects the momentum spectra. The impact of nondipole corrections increases with increasing photoelectron energy. Analysis of the complete photoelectron spectra including both direct and rescattered photoelectrons shows that, in the low‐energy region, a shift against the propagation direction occurs. The partial average of the propagation–direction momentum component in the rescattering region exhibits a plateau structure and also a local minimum structure that was recently observed in an experiment with a linearly polarized laser field (Lin et al., Phys Rev. Lett. 128, 023201 (2022)).

Using the CO molecule as target, we investigate high-order harmonic generation by a bichromatic elliptically polarized laser field. This field consists of two elliptically polarized components with the commensurable frequencies and mutually orthogonal semi-major axes. Both odd and even harmonics are emitted and their ellipticity can be large depending on the values of the laser-field parameters. It is often the case that the ellipticity of subsequent odd and even harmonics is substantially different so that, in order to produce a series of high-order harmonics with similar ellipticity, it is beneficial if the emission of odd or even harmonics is suppressed. In this paper we explore how this can be achieved using the ellipticity of the laser-field components and the relative phase as control parameters. For some values of these parameters it is possible to produce a comb of odd or even harmonics with similar ellipticity. These harmonics can later be employed for various applications the example of which is the generation of an elliptically polarized attosecond pulse train.

Nondipole effects in processes assisted by a THz field having the strength of a few MV/cm can be significant due to its long wavelength. We illustrate this for strong-laser-field-induced ionization assisted by a THz field. To this end, we generalize our strong-field-approximation theory so that it includes the first-order term in a 1/c expansion of the vector potential. We show that in this case, in addition to a shift of the maximum of the photoelectron momentum distribution, the differential ionization probability as well as the cutoff energy can be significantly increased. For an explanation of these unexpected results we use the saddle-point method adjusted to include nondipole effects.

We address ionization of a diatomic molecule by a bichromatic elliptically polarized field with co-rotating components. Using the strong-field approximation we investigate symmetry properties of the photoelectron momentum distribution and explore the minima which appear in the photoelectron spectra. We distinguish two types of minima: (i) two-center interference minima which appear due to the destructive interference of the contributions of two electron wave packets emitted from the two centers of the diatomic molecule and (ii) the one-center minima which are caused by the interference of the parts of the wave packet emitted from the same atomic center at different times. The position of the two-center interference minima depends on the molecular orientation. When a molecular orbital is modelled using the atomic orbitals of a specific parity, the position of the two-center interference minima does not depend on the ellipticity of our driving field. However, when a molecular orbital consists of both odd and even atomic orbitals the interference of their contributions and the position of the minima depend on the ellipticity. The position of the interference minima in the photoelectron momentum plane is confirmed using the saddle-point method. The position and the number of the one-center minima do not depend on the molecular orientation, but they strongly depend on the ellipticity of the field components. Finally, comparing the photoelectron spectra of the CO molecule with the spectra of homonuclear molecules and the NO molecule we show that the electron probability density distribution plays a significant role for the high-energy rescattered electrons.

Generation of an elliptically polarized attosecond pulse train by an orthogonally polarized two-color (OTC) laser field is investigated theoretically and simulated numerically. The OTC field consists of two linearly polarized fields with orthogonal polarizations and frequencies that are integer multiples of the fundamental frequency ω. For the ω−3ω OTC field, the emitted harmonics are elliptically polarized so that they may form an elliptically polarized attosecond pulse train provided that a group of harmonics is phase-locked. This is the case if only one quantum orbit generates the corresponding part of the harmonic spectrum. If so, then two attosecond pulses are emitted per optical cycle due to the dynamical symmetry of the ω−3ω OTC field. Atomic targets with an s ground state only generate attosecond pulses with almost linear polarization. Using, however, targets with a p ground state, attosecond pulses with substantial ellipticity can be produced because ground states with opposite magnetic quantum numbers m=+1 and m=−1 produce harmonics with opposite helicities at different rates. In this case, the harmonic intensity and harmonic ellipticity are different for the ground states with the magnetic quantum number m=±1. These differences are the source of the attosecond pulse ellipticity and can be controlled using the relative phase as a control parameter. In addition, by choosing a particular group of harmonics, one can select the desired ellipticity of the attosecond pulse train.

Using the strong-field approximation we systematically investigate the selection rules for high-order harmonic generation and the symmetry properties of the angle-resolved photoelectron spectra for various atomic and molecular targets exposed to one-component and two-component laser fields. These include bicircular fields and orthogonally polarized two-color fields. The selection rules are derived directly from the dynamical symmetries of the driving field. Alternatively, we demonstrate that they can be obtained using the conservation of the projection of the total angular momentum on the quantization axis. We discuss how the harmonic spectra of atomic targets depend on the type of the ground state or, for molecular targets, on the pertinent molecular orbital. In addition, we briefly discuss some properties of the high-order harmonic spectra generated by a few-cycle laser field. The symmetry properties of the angle-resolved photoelectron momentum distribution are also determined by the dynamical symmetry of the driving field. We consider the first two terms in a Born series expansion of the T matrix, which describe the direct and the rescattered electrons. Dynamical symmetries involving time translation generate rotational symmetries obeyed by both terms. However, those that involve time reversal generate reflection symmetries that are only observed by the direct electrons. Finally, we explain how the symmetry properties, imposed by the dynamical symmetry of the driving field, are altered for molecular targets.

The molecular strong-field approximation is employed to study high-order harmonic generation by linear and planar polyatomic molecules exposed to an orthogonally polarized two-color laser field, which consists of two orthogonal linearly polarized components with commensurable frequencies. For such a driving field, we find that the harmonic emission rate and the shape of the spectrum strongly depend on the laser-field parameters including the relative phase and the ratio of the intensities of the two components. The values of the relative phase that correspond to the optimal harmonic emission rate, as well as the cutoff position, can be assessed using a classical model. The possible production of an isolated attosecond pulse is investigated. For suitable symmetry of the laser field an attosecond pulse train with only one attosecond pulse per cycle can be generated. Depending on the frequencies of the two field components, the molecular symmetry properties and the orientation of the molecule with respect to the field, the even harmonics can be absent from the spectrum, which can be used to determine the molecular orientation. The emitted harmonics are elliptically polarized and their ellipticity depends on the molecular orientation.