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D. Milošević, W. Becker

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.

M. Busuladžić, A. Gazibegović-Busuladži, A. Čerkić, D. Milošević

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.

S. Kovacevic, A. Čerkić, M. Busuladžić, D. Milošević

S-matrix theory is used in order to analyze the energy spectra of electron-atom potential scattering assisted by a bicircular (two-component circularly polarized) laser field having corotating field components. The double scattering (rescattering) is also included in the analysis by applying the second Born approximation in the expansion of the S-matrix element. We have investigated how the energy spectrum of scattered electrons is affected by the scattering angle. We have also analyzed the sensitivity of the energy spectrum to the relative phase and intensity ratio of the laser-field components. The calculated energy spectra are characterized by the plateau-like oscillatory structures with abrupt cutoffs. Positions of these cutoffs in the energy spectra are confirmed by a classical analysis. Rescattering effects can be observed in the calculated energy spectra for certain values of the scattering angle. These effects are represented by the second plateau in the energy spectrum. This is different from the process of above-threshold ionization/detachment by a bicircular laser field, where the (re)scattering effects in the photoelectron energy spectra cannot be observed in the case of corotating laser-field components.

A. Jašarević, E. Hasović, R. Kopold, W. Becker, D. Milošević

The quantum-mechanical transition amplitude of an ionization process induced by a strong laser field is typically expressed in the form of an integral over the ionization time of a highly oscillatory function. Within the saddle-point (SP) approximation this integral can be represented by a sum over the contributions of the solutions of the SP equation for complex ionization time. It is shown that, for the general case of an elliptically polarized polychromatic laser field, these solutions can be obtained as zeros of a trigonometric polynomial of the order n and that there are exactly n relevant solutions, which are to be included in the sum. The results obtained are illustrated by examples of various tailored laser fields that are presently used in strong-field physics and attoscience. For some critical values of the parameters two SP solutions can coalesce and the topology of the ‘steepest descent’ integration contour changes so that some SPs are bypassed. Around the critical parameters a uniform approximation should be used instead of the SP method.

A. Gazibegović-Busuladžić, D. Habibović, M. Busuladžić, D. Milošević

Molecular strong-field approximation is applied to above-threshold detachment of homonuclear diatomic molecular negative ions. Differences between the photodetachment amplitudes for neutral diatomic molecules and diatomic anions, for both direct and rescattered electrons, are examined. Numerical results for the photoelectron spectra of $ {\rm C}_2^ - $C2− molecular anions for different intensities and wavelengths of a linearly polarized laser field and different molecular anion orientations are shown and discussed. Two-center destructive interference minima (suppression regions) in the rescattering part of the photoelectron spectra are observed. For molecules with molecular orientation defined by the angle $ {\theta _L} $θL with respect to the laser-field polarization axis, these minima manifest as two parallel straight lines in the distribution of the photoelectron yield presented in the photoelectron momentum plane. These lines make the angle $ {90^ \circ } - {\theta _L} $90∘−θL, with the momentum component parallel to the laser-field polarization axis. Focal-averaged photoelectron spectra are also presented and analyzed.

D. Milošević, W. Becker

High-order harmonic generation by orthogonally polarized two-color (OTC) laser fields is analysed using strong-field approximation and quantum-orbit theory. Results for the field components frequency ratio of 2:1 and 3:1 are presented and compared. We have shown that, depending on the relative phase between the field components, the shape of the high-harmonic spectrum can be very different from that obtained by a monochromatic linearly polarized laser field. It is also shown that it is possible to generate elliptically polarized high-order harmonics with very high photon energies using OTC laser field with the frequency ratio of 3:1 and a long fundamental wavelength. An effective relative phase control of the harmonic emission is demonstrated. The obtained results are explained using the quantum-orbit theory.

B. Fetić, Wilhelm Becker, D. Milošević, D. Milošević

Over the past three decades numerous numerical methods for solving the time-dependent Schr\"odinger equation within the single-active electron approximation have been developed for studying ionization of atomic targets exposed to an intense laser field. In addition, various numerical techniques for extracting the photoelectron spectra from the time-dependent wave function have emerged. In this paper we compare photoelectron spectra obtained by either projecting the time-dependent wave function at the end of the laser pulse onto the continuum state having the proper incoming boundary condition or by using the window-operator method. Our results for three different atomic targets show that the boundary condition imposed onto the continuum states plays a crucial role for obtaining correct spectra accurate enough to resolve fine details of the interference structures of the photoelectron angular distribution.

A. Gazibegović-Busuladžić, M. Busuladžić, A. Čerkić, E. Hasović, W. Becker, D. Milošević

We investigate strong-field ionization of linear molecules by a two-color laser field of frequencies rω and sω having coplanar counterrotating or corotating elliptically polarized components (ω is the fundamental laser field frequency and r and s are integers). Using the improved molecular strong-field approximation we analyze direct above-threshold ionization (ATI) and high-order ATI (HATI) spectra. More precisely, reflection and rotational symmetries of these spectra for linear molecules aligned in the laser-field polarization plane are considered. The reflection symmetries for particular molecular orientations, known to be valid for a bicircular field (this is the field with circularly polarized counterrotating components), are valid also for arbitrary component ellipticities. However, specific rotational symmetries that are satisfied for HATI by a bicircular field, are violated for an arbitrary elliptically polarized field with counterrotating components. For the corotating case and the N2 molecule we analyze molecular-orientation-dependent interferences and plateau structures for various ellipticities.

High-order harmonics generated by a linearly polarized laser field are also linearly polarized. Having in mind that for various application, such as the exploration of magnetic materials, chiral molecules etc., we need circularly polarized high harmonics which serve as coherent soft x-rays, we explore high-order harmonic generation by the so-called bicircular laser field. This field consists of two coplanar counter-rotating circularly polarized fields of different frequencies equal to integer multiples of a fundamental frequency ω. High harmonics generated by such field are circularly polarized with helicity alternating between +1 and −1. Combining a group of such harmonics, instead of obtaining a circularly polarized attosecond pulse train, one obtains a pulse with unusual polarization properties. But, if the harmonics of particular helicity are stronger, i.e., if we have helicity asymmetry in a high-harmonic energy interval, then it is possible to generate an elliptical or even circular pulse train. We theoretically investigated a wide range of bicircular field-component intensities (I1 and I2) and found regions where both the harmonic intensity is high and the helicity asymmetry is large. Particular attention is devoted to the ω−2ω and ω−3ω bicircular fields and atoms having the s and p ground states. In our calculations we use strong-field approximation and quantum-orbit theory. We show that, even in the extreme case of I2 = 8I1, for an ω−3ω bicircular field, high-order harmonic generation is more efficient than in the I2 = I1 case. The obtained results are explained analyzing the relevant electron trajectories and velocities, which follow from the quantum-orbit theory. For the atoms having p ground state the helicity asymmetry parameter is large for a wide range of high-harmonic photon energies, while for the atoms having s ground state the helicity asymmetry parameter can be large only for low harmonics. We confirm this by averaging the obtained results over the intensity distribution in the laser focus.

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