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.

Scattering of electrons off diatomic molecules in a bichromatic elliptically polarised laser field is considered by applying the S-matrix theory within the second Born approximation. Two characteristic plateaus appear in the energy spectrum of scattered electrons. The higher plateau is observed in the low-energy part of the spectrum and describes the single scattering, while the lower plateau extends to the high-energy part of the spectrum and describes the double scattering. Scattering and rescattering of electrons off molecular targets may occur at any molecular centre and in any order. Interference of contributions results in increasing/decreasing the differential cross section in particular regions of the energy spectrum of scattered electrons. Two contributions for single scattering and four contributions for double scattering exist in the case of diatomic molecules. For some molecular orientations, a sequence of declining maxima may be observed instead of the plateaus in the electron energy spectrum. We have also observed parabolic structures in the angle-resolved energy spectra. Analytical formulas that explain these structures have been provided. We have also explored the impact of the laser-field ellipticity on the scattered-electron energy spectra. The bichromatic ω– and ω– laser fields have been considered. GRAPHICAL ABSTRACT

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.

Above-threshold ionization spectra from cesium are measured as a function of the carrier-envelope phase (CEP) using laser pulses centered at 3.1  μm wavelength. The directional asymmetry in the energy spectra of backscattered electrons oscillates three times, rather than once, as the CEP is changed from 0 to 2π. Using the improved strong-field approximation, we show that the unusual behavior arises from the interference of few quantum orbits. We discuss the conditions for observing the high-order CEP dependence, and draw an analogy with time-domain holography with electron wave packets.

Using our theory which is based on the strong-field approximation we analyze high-order above-threshold ionization and high-order harmonic generation processes for the case of the homonuclear diatomic molecules exposed to an orthogonally polarized two-color (OTC) laser field. The OTC field represents a superposition of two linearly polarized fields with mutually orthogonal polarizations and different frequencies. We analyze the photoelectron energy spectra and the harmonic ellipticity as a function of the ratio of the intensities of the OTC laser-field components and the relative phase. Some combinations of the values of these parameters lead to the high-energy electrons, while the harmonic ellipticity depends strongly on the ratio of the intensities of the laser-field components. It is possible to find the value of this ratio for which the ellipticity of the emitted harmonics is large. The signes of ellipticity are opposite for the molecular orientations which are connected through the reflection with respect to the axis along the first OTC field component. This symmetry is explained using the expression which relates the T-matrix element and the harmonic ellipticity.

International Physics Conference in Bosnia and Herzegovina (PHYCONBA 2020) Organizer: Physical Society in Federation of Bosnia and Herzegovina with support of the Academy of Sciences and Arts of Bosnia and Herzegovina Date: October 19, 2020 Venue: Premises of The Academy of Sciences and Arts of Bosnia and Herzegovina, 7 Bistrik street, Sarajevo, Bosnia and Herzegovina. Memebers of Organizing committee: 1. Maja Đekić (Faculty of Science, University of Sarajevo), chairwoman, 2. Mirza Hadžimehmedović (Faculty of Science, University of Tuzla), member, 3. Rifat Omerović (Faculty of Science, University of Tuzla), member, 4. Ena Žunić-Ćejvanović, member, 5. Amra Salčinović Fetić, (Faculty of Science, University of Sarajevo), Technical secretary, 6. Benjamin Fetić (Faculty of Science, University of Sarajevo), member Members of Scientific committee: 1. Dejan Milošević (Faculty of Science, University of Sarajevo, Academy of Sciences and Arts of BiH), chairman, 2. Dijana Dujak (Faculty of Electrical Engineering, University of Sarajevo), member, 3. Hedim Osmanović (Faculty of Science, University of Tuzla), member, 4. Siniša Ignjatović (Faculty of Natural Sciences and Mathematics, University of Banja Luka), member.

High-harmonic generation by aligned diatomic molecules in orthogonally po-larized two-color laser fields is considered using the molecular strong-field approximation. Regions of the parameter space with large harmonic ellipticity are identified.

We investigate emission rate and ellipticity of high-order harmonics generated exposing a homonuclear diatomic molecule, aligned in the laser-field polarization plane, to a strong orthogonally polarized two-color (OTC) laser field. The linearly polarized OTC-field components have frequencies rω and sω, where r and s are integers. Using the molecular strong-field approximation with dressed initial state and undressed final state, we calculate the harmonic emission rate and harmonic ellipticity for frequency ratios 1:2 and 1:3. The obtained quantities depend strongly on the relative phase between the laser-field components. We show that with the OTC field it is possible to generate elliptically polarized high-energy harmonics with high emission rate. To estimate the relative phase for which the emission rate is maximal we use the simple man’s model. In the harmonic spectra as a function of the molecular orientation there are two types of minima, one connected with the symmetry of the molecular orbital and the other one due to destructive interference between different contributions to the recombination matrix element, where we take into account that the electron can be ionized and recombine at the same or different atomic centers. We derive a condition for the interference minima. These minima are blurred in the OTC field except in the cases where the highest occupied molecular orbital is modeled using only s or only p orbitals in the linear combination of the atomic orbitals. This allows us to use the interference minima to assess which atomic orbitals are dominant in a particular molecular orbital. Finally, we show that the harmonic ellipticity, presented in false colors in the molecular-orientation angle vs. harmonic-order plane, can be large in particular regions of this plane. These regions are bounded by the curves determined by the condition that the harmonic ellipticity is approximately zero, which is determined by the minima of the T-matrix contributions parallel and perpendicular to the fundamental component of the OTC field.

We consider the problem of the choice of gauge in nonrelativistic strong-laser-field physics. For this purpose, we use the phase-space path-integral formalism to obtain the momentum-space matrix element of the exact time-evolution operator. With the assumption that the physical transition amplitude corresponds to transitions between eigenstates of the physical energy operator rather than the unperturbed Hamiltonian H0=(−i∂/∂r)2/2+V(r), we prove that the aforementioned momentum-space matrix elements obtained in velocity gauge and length gauge are equal. These results are applied to laser-assisted electron-ion radiative recombination (LAR). The transition amplitude comes out identical in length gauge and velocity gauge, and the expression agrees with the one conventionally obtained in length gauge. In addition to the strong-field approximation (SFA), which is the zeroth-order term of our expansion, we present explicit results for the first-order and the second-order terms, which correspond to LAR preceded by single and double scattering, respectively. Our general conclusion is that in applications to atomic processes in strong-field physics the length-gauge version of the SFA (and its higher-order corrections) should be used. Using the energy operator as the basis-defining Hamiltonian, we have shown that the resulting transition amplitude is gauge invariant and agrees with the form commonly derived in length gauge.

Based on the strong-field approximation, we report results for high-order harmonic generation by bi-elliptical orthogonally polarized two-color (BEOTC) fields with frequency ratios of 2:1 and 3:1 and fundamental wavelengths of 800 and 1800 nm. A BEOTC field denotes the superposition of two copropagating counter-rotating elliptically polarized fields with different wavelengths and orthogonal semimajor axes. Its two limiting cases are the bicircular field and the linearly polarized orthogonal two-color field [D. B. Milo\ifmmode \check{s}\else \v{s}\fi{}evi\ifmmode \acute{c}\else \'{c}\fi{} and W. Becker, Phys. Rev. A 100, 031401(R) (2019)]. A detailed analysis of the high-order harmonic intensities and ellipticities as functions of the harmonic order, the ellipticity, and the relative phase between the two driving-field components is presented. Regions of the parameter space are identified where the harmonic ellipticities are very high. Surprisingly, this can be the case already for very small ellipticity (as small as $\ensuremath{\varepsilon}=0.01$) of the driving field. This can be important for practical applications. In the opposite limit where the BEOTC field is close to bicircular, the selection rules that govern the latter case can also be very quickly invalidated. For the 2:1 case, this can result in an apparent shift of the selection rules by one harmonic order.

By analyzing angular and energy distributions of the photoelectrons emitted in strong-laser-field-induced ionization of molecules, one can obtain information about the molecular structure and the ground-state symmetry. High-energy part of the photoelectron spectra in the above-threshold ionization (ATI) is characterized by a plateau region in which the ionization probability is practically energy independent. The photoelectron yield drops off exponentially for electron energies higher than some critical energy, i.e. the mentioned plateau is followed by an abrupt cutoff. We investigate the influence of the molecular ground state symmetry on this plateau region and show that, analyzing the corresponding high-order ATI spectra, one can obtain information about the highest occupied molecular orbitals (HOMOs) of the considered molecules. We present results for different homonuclear diatomic molecules: N2, O2, Ar2 and C2 having, respectively, the σ g , π g , σ u and π u symmetries of the HOMO. Particular attention is devoted to the C2 molecule since high-order ATI spectra for this molecule have not been analyzed yet. We consider ATI by a linearly polarized laser field for which the mentioned plateau can be well-developed, depending on the orientation of the molecular axis with respect to the laser-field polarization axis. The HOMO-symmetry-dependent (dis)appearance of the plateau is particularly pronounced for the parallel and perpendicular orientations. Our findings are valid for a wide range of the laser-field intensities and wavelengths, which is important for realization of the suggested experiments. Using the improved molecular strong-field approximation, the theory which is particularly suitable for the analysis of high-energy ATI spectra, for the case of the C2 molecule and different molecular and laser parameters, we investigate various features of the plateau, such as its length and the interference minima and their positions.