The adiabatic approximation is a natural approach for the description of phenomena induced by low frequency laser radiation because the ratio of the laser frequency to the characteristic frequency of an atom or a molecule is a small parameter. Since the main aim of this work is the study of ionization phenomena, the version of the adiabatic approximation that can account for the transition from a bound state to the continuum must be employed. Despite much work in this topic, a universally accepted adiabatic approach of bound-free transitions is lacking. Hence, based on Savichev's modified adiabatic approximation [Sov. Phys. JETP 73, 803 (1991)], we first of all derive the most convenient form of the adiabatic approximation for the problems at hand. Connections of the obtained result with the quasiclassical approximation and other previous investigations are discussed. Then, such an adiabatic approximation is applied to single-electron ionization and non-sequential double ionization of atoms in a strong low frequency laser field. The momentum distribution of photoelectrons induced by single-electron ionization is obtained analytically without any assumptions on the momentum of the electrons. Previous known results are derived as special cases of this general momentum distribution. The correlated momentum distribution of two-electrons due to non-sequential double ionization of atoms is calculated semi-analytically. We focus on the deeply quantum regime -- the below intensity threshold regime, where the energy of the active electron driven by the laser field is insufficient to collisionally ionize the parent ion, and the assistance of the laser field is required to create a doubly charged ion. A special attention is paid to the role of Coulomb interactions in the process. The signatures of electron-electron repulsion, electron-core attraction, and electron-laser interaction are identified. The results are compared with available experimental data. Two-electron correlated spectra of non-sequential double ionization below intensity threshold are known to exhibit back-to-back scattering of the electrons, viz., the anticorrelation of the electrons. Currently, the widely accepted interpretation of the anticorrelation is recollision-induced excitation of the ion plus subsequent field ionization of the second electron. We argue that there exists another mechanism, namely simultaneous electron emission, when the time of return of the rescattered electron is equal to the time of liberation of the bounded electron (the ion has no time for excitation), that can also explain the anticorrelation of the electrons in the deep below intensity threshold regime. Finally, we study single-electron molecular ionization. Based on the geometrical approach to tunnelling by P. D. Hislop and I. M. Sigal [Memoir. AMS 78, No. 399 (1989)], we introduce the concept of a leading tunnelling trajectory. It is then proven that leading tunnelling trajectories for single active electron models of molecular tunnelling ionization (i.e., theories where a molecular potential is modelled by a single-electron multi-centre potential) are linear in the case of short range interactions and ``almost'' linear in the case of long range interactions. The results are presented on both the formal and physically intuitive levels. Physical implications of the proven statements are discussed.

The adiabatic approximation is a natural approach for the description of phenomena induced by low frequency laser radiation because the ratio of the laser frequency to the characteristic frequency of an atom or a molecule is a small parameter. Since the main aim of this work is the study of ionization phenomena, the version of the adiabatic approximation that can account for the transition from a bound state to the continuum must be employed. Despite much work in this topic, a universally accepted adiabatic approach of bound-free transitions is lacking. Hence, based on Savichev's modified adiabatic approximation [Sov. Phys. JETP 73, 803 (1991)], we first of all derive the most convenient form of the adiabatic approximation for the problems at hand. Connections of the obtained result with the quasiclassical approximation and other previous investigations are discussed. Then, such an adiabatic approximation is applied to single-electron ionization and non-sequential double ionization of atoms in a strong low frequency laser field. The momentum distribution of photoelectrons induced by single-electron ionization is obtained analytically without any assumptions on the momentum of the electrons. Previous known results are derived as special cases of this general momentum distribution. The correlated momentum distribution of two-electrons due to non-sequential double ionization of atoms is calculated semi-analytically. We focus on the deeply quantum regime -- the below intensity threshold regime, where the energy of the active electron driven by the laser field is insufficient to collisionally ionize the parent ion, and the assistance of the laser field is required to create a doubly charged ion. A special attention is paid to the role of Coulomb interactions in the process. The signatures of electron-electron repulsion, electron-core attraction, and electron-laser interaction are identified. The results are compared with available experimental data. Two-electron correlated spectra of non-sequential double ionization below intensity threshold are known to exhibit back-to-back scattering of the electrons, viz., the anticorrelation of the electrons. Currently, the widely accepted interpretation of the anticorrelation is recollision-induced excitation of the ion plus subsequent field ionization of the second electron. We argue that there exists another mechanism, namely simultaneous electron emission, when the time of return of the rescattered electron is equal to the time of liberation of the bounded electron (the ion has no time for excitation), that can also explain the anticorrelation of the electrons in the deep below intensity threshold regime. Finally, we study single-electron molecular ionization. Based on the geometrical approach to tunnelling by P. D. Hislop and I. M. Sigal [Memoir. AMS 78, No. 399 (1989)], we introduce the concept of a leading tunnelling trajectory. It is then proven that leading tunnelling trajectories for single active electron models of molecular tunnelling ionization (i.e., theories where a molecular potential is modelled by a single-electron multi-centre potential) are linear in the case of short range interactions and ``almost'' linear in the case of long range interactions. The results are presented on both the formal and physically intuitive levels. Physical implications of the proven statements are discussed.

The multiconfiguration time-dependent Hartree-Fock (MCTDHF) and multiconfiguration time-dependent Hartree (MCTDH) methods are employed to investigate nonperturbative multielectron dynamics in finite quantum systems. MCTDHF is a powerful tool that allows for the investigation of multielectron dynamics in strongly perturbed quantum systems. We have developed an MCTDHF code that is capable of treating problems involving three dimensional (3D) atoms and molecules exposed to strong laser fields. This code will allow for the theoretical treatment of multielectron phenomena in attosecond science that were previously inaccessible. These problems include complex ionization processes in pump-probe experiments on noble gas atoms, the nonlinear effects that have been observed in Ne atoms in the presence of an x-ray free-electron laser (XFEL) and the molecular rearrangement of cations after ionization. An implementation of MCTDH that is optimized for two electrons, each moving in two dimensions (2D), is also presented. This implementation of MCTDH allows for the efficient treatment of 2D spin-free systems involving two electrons; however, it does not scale well to 3D or to systems containing more that two electrons. Both MCTDHF and MCTDH were used to treat 2D problems in nanophysics and attosecond science. MCTDHF is used to investigate plasmon dynamics and the quantum breathing mode for several electrons in finite lateral quantum dots. MCTDHF is also used to study the effects of manipulating the potential of a double lateral quantum dot containing two electrons; applications to quantum computing are discussed. MCTDH is used to examine a diatomic model molecular system exposed to a strong laser field; nonsequential double ionization and high harmonic generation are studied and new processes identified and explained. An implementation of MCTDHF is developed for nonuniform tensor product grids; this will allow for the full 3D implementation of MCTDHF and will provide a means to investigate a wide variety of problems that cannot be currently treated by any other method. Finally, the time it takes for an electron to tunnel from a bound state is investigated; a definition of the tunnel time is established and the Keldysh time is connected to the wavefunction dynamics.

The multiconfiguration time-dependent Hartree-Fock (MCTDHF) and multiconfiguration time-dependent Hartree (MCTDH) methods are employed to investigate nonperturbative multielectron dynamics in finite quantum systems. MCTDHF is a powerful tool that allows for the investigation of multielectron dynamics in strongly perturbed quantum systems. We have developed an MCTDHF code that is capable of treating problems involving three dimensional (3D) atoms and molecules exposed to strong laser fields. This code will allow for the theoretical treatment of multielectron phenomena in attosecond science that were previously inaccessible. These problems include complex ionization processes in pump-probe experiments on noble gas atoms, the nonlinear effects that have been observed in Ne atoms in the presence of an x-ray free-electron laser (XFEL) and the molecular rearrangement of cations after ionization. An implementation of MCTDH that is optimized for two electrons, each moving in two dimensions (2D), is also presented. This implementation of MCTDH allows for the efficient treatment of 2D spin-free systems involving two electrons; however, it does not scale well to 3D or to systems containing more that two electrons. Both MCTDHF and MCTDH were used to treat 2D problems in nanophysics and attosecond science. MCTDHF is used to investigate plasmon dynamics and the quantum breathing mode for several electrons in finite lateral quantum dots. MCTDHF is also used to study the effects of manipulating the potential of a double lateral quantum dot containing two electrons; applications to quantum computing are discussed. MCTDH is used to examine a diatomic model molecular system exposed to a strong laser field; nonsequential double ionization and high harmonic generation are studied and new processes identified and explained. An implementation of MCTDHF is developed for nonuniform tensor product grids; this will allow for the full 3D implementation of MCTDHF and will provide a means to investigate a wide variety of problems that cannot be currently treated by any other method. Finally, the time it takes for an electron to tunnel from a bound state is investigated; a definition of the tunnel time is established and the Keldysh time is connected to the wavefunction dynamics.

Lorsqu'ils sont soumis à des pulses laser courts et intenses, des atomes peuvent perdre des électrons. Plusieurs canaux sont impliqués dans la double ionisation, comme la NSDI et le scénario associé de la recollision. La recollision est maintenant vue comme la “pierre d'angle de la physique en champ fort” pour les éclairages qu'elle donne dans l'organisation de la matière et en ce qu'elle constitue l'une des manifestations les plus flagrantes de la corrélation électron-électron dans la nature. Dans ce manuscrit, une analyse théorique des mécanismes de double ionisation est menée en utilisant la mécanique classique. Cette description complémente les modèles quantiques en observant la dynamique depuis un cadre de travail différent et avec l'éclairage de la dynamique nonlinéaire. L'analyse, menée dans l'espace des phases, permet l'identification des structures organisatrices qui régulent les différents mécanismes d'ionisation. Pour des champs laser polarisés linéairement, le mécanisme de la recollision est complété par l'image de l'électron interne. L'électron interne donne accès à une description fine de la dynamique de recollision et explique les différentes routes pour la double ionisation. Il permet également de faire des prédictions telles que l'intensité du coude dans la probabilité de double ionisation et explique complètement la RESI. En polarisation circulaire, il est communément cru que la recollision n'est pas possible, en dépit de résultats expérimentaux contradictoires. En fait, l'analyse de l'espace des phases montre que la recollision est possible mais pas accessible à tous les atomes, réconciliant par conséquent les contradictions expérimentales précédentes. / When subjected to strong and short laser pulses, atoms may lose electrons. Several ionization channels are involved in such double ionization events, like nonsequential double ionization (NSDI) and its associated recollision scenario. Recollision is now seen as the “keystone of strong field physics”, for its insights into the organization of matter, and is one of the most dramatic manifestations of electron-electron correlation in nature. In this manuscript a theoretical analysis of the double ionization mechanisms is carried out using classical mechanics. This description complements quantum treatments by observing the dynamics from a different framework, with the light of nonlinear dynamics, as both frameworks exhibit the main ingredient, i.e., strong electron-electron correlation. The analysis, carried out in phase space (e.g., through reduced models) enables the identification of the organizing structures that regulate the ionization channels. For linearly polarized lasers, the recollision mechanism is completed by the picture of the “inner” electron. The inner electron gives access to a fine description of the recollision dynamics and explains the routes to double ionization. It also enables verifiable predictions such as the location of the characteristic knee shape in the double ionization yield versus laser intensity and fully explains delayed ionizations like RESI. For circular polarization, it is commonly believed that recollision is not possible, despite apparently contradictory experimental results. In fact, the phase space analysis shows that recollision is possible but not accessible to all atoms, thus reconciling the previous experimental results.