No Arabic abstract
If one-electron observables of a many-electron system are of interest, a many-electron dynamics can be represented exactly by a one-electron dynamics with effective potentials. The formalism for this reduction is provided by the Exact Electron Factorization (EEF). We study the time-dependent features of the EEF effective potentials for a model of an atom ionized by an ultrastrong and ultrashort laser pulse, with the aim of understanding what is needed to develop computationally feasible approximations. It is found that the simplest approximation, the so-called time-independent conditional amplitude (TICA) approximation, is complementary to single-active electron (SAE) approaches as it reproduced the exact dynamics well for high photon frequencies of the laser field or large Keldysh parameter. For relatively low frequencies of the laser field or for smaller Keldysh parameters, we find that excited state dynamics in the core region of the atom leads to a time-dependent ionization barrier in the EEF potential. The time-dependence of the barrier needs to be described accurately to correctly model many-electron effects, and we conclude that a multi-state extension of the TICA approximation is a possible route how this can be achieved. In general, our study sheds a different light on one-electron pictures of strong-field ionization and shows that many-electron effects for such processes may be included by solving a one-electron Schrodinger equation, provided the core dynamics can be modeled successfully.
We report on the observation of discrete structures in the electron energy distribution for strong field double ionization of Argon at 394 nm. The experimental conditions were chosen in order to ensure a non-sequential ejection of both electrons with an intermediate rescattering step. We have found discrete ATI (above-threshold ionization) like peaks in the sum energy of both electrons, as predicted by all quantum mechanical calculations. More surprisingly however is the observation of two ATI combs in the energy distribution of the individual electrons.
We present an exact single-electron picture that describes the correlated electron dynamics in strong laser fields. Our approach is based on the factorization of the electronic wavefunction as a product of a marginal and a conditional amplitude. The marginal amplitude, which depends only on one electronic coordinate and yields the exact one-electron density and current density, obeys a time-dependent Schrodinger equation with an effective time-dependent potential. The exact equations are used to derive an approximation that is a step towards a general and feasible ab-initio single-electron approximation for molecules. The derivation also challenges the usual interpretation of the single-active electron approximation. From the study of model systems, we find that the exact and approximate single-electron potentials for processes with negligible two-electron ionization lead to a qualitatively similar dynamics, but that the ionization barrier may be explicitly time-dependent.
Hartree-Fock atom in a strong electric static field is considered. It is demonstrated that exchange between outer and inner electrons, taken into account by the so-called Fock term affects strongly the long-range behavior of the inner electron wave function. As a result, it dramatically increases its probability to be ionized. A simple model is analyzed demonstrating that the decay probability, compared to the case of a local (Hartree) atomic potential, increases by many orders of magnitude. As a result of such increase, the ratio of inner to outer electrons ionization probability became not too small. It is essential that the effect of exchange upon probability of inner electron ionization by strong electric field is proportional to the square of the number of outer electrons. It signals that in clusters the inner electron ionization by strong field, the very fact of which is manifested by e.g. high energy quanta emission, has to be essentially increased as compared to this process in gaseous atomic objects.
This work presents an algorithm to evaluate Coulomb and exchange matrices in Fock operator using range separation techniques at various aspects. This algorithm is particularly favorable for the scenario of (1) all-electron calculations or (2) computing exchange matrix for a large number of $mathbf{k}$-point samples. An all electron Hartree-Fock calculation with 110k basis functions is demonstrated in this work.
We study light absorption in many-electron interacting systems beyond the linear regime by using a {em single} broadband impulse of an electric field in the instantaneous limit. We determine non-pertubatively the absorption cross section from the Fourier transform of the time-dependent induced dipole moment, which can be obtained from the time evolution of the wavefunction. We discuss the dependence of the resulting cross section on the magnitude of the impulse and we highlight the advantages of this method in comparison with perturbation theory working on a one-dimensional model system for which numerically exact solutions are accessible. Thus we demonstrate that the considered non pertubative approach provides us with an effective tool for investigating fluence-dependent nonlinear optical excitations.