We consider high-order above-threshold ionization (HATI) of polyatomic molecules ionized by a strong linearly polarized laser field. Improved molecular strong-field approximation by which the HATI process on polyatomic molecular species can be described is developed. Using this theory we calculate photoelectron angular-energy spectra for different triatomic molecules. Special attention is devoted to the minima that are observed in the calculated high-energy electron spectra of the ozone and carbon dioxide molecules. A key difference between these minima and minima that are observed in the corresponding spectra of diatomic molecules are presented.

Processes of above-threshold ionization (ATI) and high-order harmonic generation (HHG) for heteronuclear diatomic molecules are investigated. By analyzing the HHG and ATI spectra for different molecular orientation with respect to the main laser polarization axis and for different values of the photon energies and electron energies and emission angle, we are able to draw some conclusions about the molecular structure. The partial elliptic dichroism effect in HHG spectra is also analyzed. Regarding the ATI spectra, two-center interference minima are visible, even for a circularly polarized laser field. The positions of the minima depend on the internuclear distance, on the relative contributions of the atomic orbitals to the highest occupied molecular orbital and on the laser field parameters.

S-matrix theory is used to analyze different atomic and molecular processes in a linearly polarized few-cycle laser field. The energy spectra of high-order above-threshold ionization (HATI) are presented. Electron-atom potential scattering assisted by a few-cycle laser pulse is also analyzed. It is shown that the plateau structures in the energy spectra of the electron-atom potential scattering are dependent on the carrier-envelope phase (CEP) of the laser pulse, so that the cutoff positions of the plateaus can be controlled by changing the CEP. Regarding our analysis of the molecular HATI process, the angle-resolved spectra, obtained by different theoretical approaches, are also presented.

Additional support for the concept of ”quantum orbits” is presented that emphasizes in particular the importance of ”long orbits” where the time between ionization and rescattering may be many periods of the laser field. Two examples are discussed, above-threshold ionization by an elliptically polarized laser field and intensity-dependent enhancements of certain spectral regions within the backscattering plateau, where we compare experimental data and the theoretical quantum-orbit simulations. In both cases, good agreement is obtained.

Rresonancelike enhancement of groups of adjacent peaks in the photoelectron spectrum of high-order above-threshold ionization has been well documented for noble-gas atoms subjected to intense infrared laser pulses. However, its physical origin is still under debate. In this Rapid Communication, we investigate experimentally and theoretically high-order above-threshold ionization of diatomic nitrogen and oxygen molecules in order to shed more light on the underlying mechanism. The resonancelike enhancement is experimentally observed for N-2 but is absent for O-2 molecules. A simulation on the basis of S-matrix theory and the strong-field approximation reproduces the experimental observations. This implies that the resonancelike enhancement can be attributed to the channel-closing effect. The specific molecular structure plays a decisive role for the presence or absence of this enhancement in molecular systems.

We theoretically investigate high-order above-threshold ionization (HATI) of heteronuclear diatomic molecules applying the molecular strong-field approximation which includes dressing of the molecular bound state. We consider HATI of nitrogen monoxide molecules, which are characterized by the π symmetry of their highest occupied molecular orbital. We show that the HATI spectra of NO exhibit characteristic interference structures. We analyze the differences and similarities of the HATI spectra of NO molecules and the spectra of CO (σ symmetry) and O(2) (π(g) symmetry) molecules. The symmetry properties of the molecular HATI spectra governed by linearly and elliptically polarized fields are considered in detail. The yields of high-energy electrons, contributing to the plateau region of the photoelectron spectra, strongly depend on the employed ellipticity.

We present a quantum-mechanical laser-assisted scattering theory and show how the rescattering effects can be described within the second Born approximation. Also, we use two versions of the atomic (molecular) strong-field approximation in order to describe high-order above-threshold ionization. In the improved strong-field approximation, the rescattering of the ionized electron off the parent ion is described within the first-order Born approximation. A better approximation is the so-called low-frequency approximation in which the elastic rescattering amplitude is calculated exactly.

In this paper, we present a quantum-mechanical theory in order to describe laser-induced and laser-assisted atomic and molecular processes with an emphasis on an elliptically polarized strong laser field. The features of the high-energy regions of spectra and their cutoffs are analyzed in detail for different values of ellipticity, laser intensities and various atomic and molecular species. Our theoretical study is focused on the ellipticity dependence of the plateau structures that appear in the energy spectra of atomic and molecular processes in strong laser fields.

The molecular strong-field approximation (MSFA), which includes dressing of the molecular bound state, is introduced and applied to above-threshold ionization of heteronuclear diatomic molecules. Expressions for the laser-induced molecular dipole and polarizability as functions of the laser parameters (intensity and frequency) and molecular parameters [molecular orientation, dipole, and parallel and perpendicular polarizabilities of the highest occupied molecular orbital (HOMO)] are presented. Our previous MSFA theory, which incorporates the rescattering effects, is generalized from homonuclear to heteronuclear diatomic molecules. Angle- and energy-resolved high-order above-threshold ionization spectra of oriented heteronuclear diatomic molecules, exemplified by the carbon monoxide (CO) molecule, exhibit pronounced minima, which can be related to the shape of their HOMO-electron-density distribution. For the CO molecule we have found an analytical condition for the positions of these minima. We have also shown that the effect of the dressing of the HOMO is twofold: (i) the laser-induced Stark shift decreases the ionization yield and (ii) the laser-induced time-dependent dipole and polarizability change the oscillatory structure of the spectra.

Above-threshold ionization of diatomic molecules by infrared carrier-envelope phase (CEP) stable few-cycle laser pulses is analyzed both experimentally and theoretically. The theoretical approach is based on the recently developed molecular improved strong-field approximation (ISFA), generalized to few-cycle pulses. Instead of using the first Born approximation, the rescattering matrix element in the ISFA is now calculated exactly. This modification leads to the appearance of characteristic minima in the differential cross section as a function of the scattering angle. Experimental angle-resolved photoelectron spectra of N{sub 2} and O{sub 2} molecules are obtained using the velocity map imaging technique. A relatively good agreement of experimental and simulated angle-resolved spectra, CEP-dependent asymmetry maps, and extracted electron-molecular ion elastic scattering differential cross sections is obtained.

We investigate how various versions of the molecular strong-field approximation (MSFA) agree with the experiment by Grasbon et al. [Phys. Rev. A 63, 041402(R) (2001)], in which the suppression of the ionization yield in the low-energy spectrum of the ${\mathrm{O}}_{2}$ molecule, compared to the spectrum of its companion atom Xe, was observed. In this experiment, it was also found that the spectrum of the ${\mathrm{N}}_{2}$ molecule is comparable to the corresponding spectrum of its companion atom Ar. We show that the length-gauge version of the MSFA with the initial state dressed by the laser field gives the best agreement with the experimental data for both ${\mathrm{O}}_{2}$ and ${\mathrm{N}}_{2}$ molecules.