We present a numerical method for investigating the non-perturbative quantum mechanical interaction of light with atoms in two dimensions, without a basis expansion. This enables us to investigate intense laser-atom interactions with light of arbitrary polarization without approximation. Results are presented for the dependence of ionization and high harmonic generation on ellipticity seen in recent experiments. Strong evidence of stabilization in circular polarization is found.
The relativistic theory of above-threshold ionization (ATI) of hydrogen-like atoms in ultrastrong radiation fields, taking into account the photoelectron induced rescattering in the continuum spectrum is developed. It is shown that the contribution of the latter in the multiphoton ionization probability even in the Born approximation by Coulomb field is of the order of ATI probability in the scope of Keldysh-Faisal-Reiss ansatz.
The alignment dependence of the ionization behavior of H$_2$ exposed to intense ultrashort laser pulses is investigated on the basis of solutions of the full time-dependent Schrödinger equation within the fixed-nuclei and dipole approximation. The total ionization yields as well as the energy-resolved electron spectra have been calculated for a parallel and a perpendicular orientation of the molecular axis with respect to the polarization axis of linear polarized laser pulses. For most, but not all considered laser peak intensities the parallel aligned molecules are easier to ionize. Furthermo…
We describe a efficient way to photoionize strontium atoms in a linear radio-frequency trap. We use a 2-photon second order process to excite the autoionization resonance (4d2 + 5p2) 1D2. A doubled pulsed Ti:Saphire laser system is used at 431nm to provide 100fsec pulses at 82Mhz. The fabrication of the laser systems for addressing the Sr+ transitions necessary for laser cooling and excitation of quantum jumps, vacuum system and ion trap structure are also described in detail. With the current setup a easy and repeatable trapping of linear ion chains is achieved at UHV pressures.
In this paper we study the response in time of N$_2$, O$_2$ and F$_2$ to laser pulses having a wavelength of 390nm. We find single ionization suppression in O$_2$ and its absence in F$_2$, in accordance with experimental results at $λ= 800$nm. Within our framework of time-dependent density functional theory we are able to explain deviations from the predictions of Intense-Field Many-Body $S$-Matrix Theory (IMST). We confirm the connection of ionization suppression with destructive interference of outgoing electron waves from the ionized electron orbital. However, the prediction of ionization s…
Spin effects in the tunneling regime of strong field ionization of hydrogenlike highly charged ions in linearly as well as circularly polarized laser fields are investigated. The impact of the polarization of a laser field on the spin effects are analyzed. Spin-resolved differential ionization rates are calculated employing the relativistic Coulomb-corrected strong-field approximation (SFA) developed in the previous paper of the series. Analytical expressions for spin asymmetries and spin flip probability, depending on the laser's polarization, are obtained for the photoelectron momentum corre…
We develop a relativistic Coulomb-corrected strong field approximation (SFA) for the investigation of spin effects at above-threshold ionization in relativistically strong laser fields with highly charged hydrogen-like ions. The Coulomb-corrected SFA is based on the relativistic eikonal-Volkov wave function describing the ionized electron laser-driven continuum dynamics disturbed by the Coulomb field of the ionic core. The SFA in different partitions of the total Hamiltonian is considered. The formalism is applied for direct ionization of a hydrogen-like system in a strong linearly polarized l…
The generation of electron vortex states in ionization by intense and short laser pulses is analyzed under the scope of the lowest-order Born approximation. For near infrared laser fields and nonrelativistic intensities of the order of $10^{16}$~W/cm$^2$, we show that one has to modify the nonrelativistic treatment of ionization by accounting for recoil and mass relativistic corrections. By using the corrected quasi-relativistic theory, the requirements for the observation of electron vortex states with non-negligible probability and large topological charge are determined.
We present experimental results for the ionization of aniline and benzene molecules subjected to intense ultrashort laser pulses. Measured parent molecular ions yields were obtained using a recently developed technique capable of three-dimensional imaging of ion distributions within the focus of a laser beam. By selecting ions originating from the central region of the focus, where the spatial intensity distribution is nearly uniform, volumetric-free intensity-dependent ionization yields were obtained. The measured data revealed a previously unseen resonant-like multiphoton ionization process.…
The two- and three-body Coulomb explosion of carbonyl sulfide (OCS) by 790 nm, 50 fs laser pulses focussed to $\approx $ 10$^{16}$ Wcm$^{-2}$ has been investigated by three-dimensional covariance mapping technique. For the first time in a triatomic molecule, a single charge state, in this case the trication, has been observed to dissociate into two distinct energy channels. With the aid of a three dimensional visualization technique to reveal the ionization hierarchy, evidence is presented for the existence of two sets of ionization pathways resulting from these two initial states. While one g…
Spin effects in above-threshold ionization of hydrogenlike highly charged ions in super-strong laser fields are investigated. Spin-resolved ionization rates in the tunneling regime are calculated by employing two versions of a relativistic Coulomb-corrected strong-field approximation (SFA). An intuitive simple-man model is developed which explains the derived scaling laws for spin-flip and spin-asymmetry effects. The intuitive model as well as our ab initio numerical simulations support the analytical results for the spin effects obtained in the dressed SFA where the impact of the laser field …
The effect of the Pauli exclusion principle on double ionization of He atoms by strong, linearly polarized laser pulses is analyzed. We show that correlated electron escape, with electron momenta symmetric with respect to the field polarization axis, is suppressed if atoms are initially prepared in the metastable state 3S. The effect is a consequence of selection rules for the transition to the appropriate outgoing two-electron states. We illustrate the suppression in numerical calculations of electron and ion momentum distributions within a reduced dimensionality model.
A theoretical study of the intense-field single ionization of molecular hydrogen or deuterium oriented either parallel or perpendicular to a linear polarized laser pulse (400 nm) is performed for different internuclear separations and pulse lengths in an intensity range of $(2-13)\times10^{13} $W cm$^{-2}$. The investigation is based on a non-perturbative treatment that solves the full time-dependent Schrödinger equation of both correlated electrons within the fixed-nuclei and the dipole approximation. The results for various internuclear separations are used to obtain the ionization yields of…
Aiming at the investigation of above-threshold ionization in super-strong laser fields with highly charged ions, we develop a Coulomb-corrected strong field approximation (SFA). The influence of the Coulomb potential of the atomic core on the ionized electron dynamics in the continuum is taken into account via the eikonal approximation, treating the Coulomb potential perturbatively in the phase of the quasi-classical wave function of the continuum electron. In this paper the formalism of the Coulomb-corrected SFA for the nonrelativistic regime is discussed employing velocity and length gauge. …
Recent attoclock experiments using the attsecond angular streaking technique enabled the measurement of the tunneling time delay during laser induced strong field ionization. Theoretically the tunneling time delay is commonly modelled by the Wigner time delay concept which is derived from the derivative of the electron wave function phase with respect to energy. Here, we present an alternative method for the calculation of the Wigner time delay by using the fixed energy propagator. The developed formalism is applied to the nonrelativistic as well as to the relativistic regime of the tunnel-ion…
Classically allowed transport is shown to compete with quantum tunneling during the ionization of atoms by ultrashort and intense laser pulses, despite Keldysh parameters smaller than unity. This is done by comparing exact probability densities with the ones obtained from purely classical propagation using the Truncated Wigner Approximation. Not only is classical transport capable of moving trajectories away from the core, but it can also furnish ionization probabilities of the same order as the quantum ones for intensities currently employed in experiments. Our results have implications rangi…
The processes of ionization and energy transfer in a quantum system composed of two distant H atoms with an initial internuclear separation of 100 atomic units (5.29 nm) have been studied by the numerical solution of the time-dependent Schrödinger equation beyond the Born-Oppenheimer approximation. Thereby it has been assumed that only one of the two H atoms was excited by temporally and spatially shaped laser pulses at various laser carrier frequencies. The quantum dynamics of the extended H-H system, which was taken to be initially either in an unentangled or an entangled ground state, has b…
We report on tunnel ionization of Xe by 2-cycle, intense, infrared laser pulses and its dependence on carrier-envelope-phase (CEP). At low values of optical field ($E$), the ionization yield is maximum for cos-like pulses with the dependence becoming stronger for higher charge states. At higher $E$-values, the CEP dependence either washes out or flips. A simple phenomenological model is developed that predicts and confirms the observed results. CEP effects are seen to persist for 8-cycle pulses. Unexpectedly, electron rescattering plays an unimportant role in the observed CEP dependence. Our r…
The outgoing electrons in non-sequential multiple ionization in intense laser fields are strongly correlated. The correlations can be explained within a classical model for interacting electrons in the presence of the external field. Here we extend the previous analysis for two and three electrons to cases with up to eight electrons and identify the saddle configurations that guard the channels for non-sequential multiple ionization. For four and fewer electrons the electrons in the dominant configuration are equivalent, for six and more electrons this is no longer the case. The case of five e…
Visualizing intense laser field driven electron dynamics in a multielectron molecule: dynamic electron localization, bonding properties and multiple ionization bursts
