Increasing ellipticity usually suppresses the recollision probability drastically. In contrast, we report on a recollision channel with large return energy and a substantial probability, regardless of the ellipticity. The laser envelope plays a dominant role in the energy gained by the electron, and in the conditions under which the electron comes back to the core. We show that this recollision channel efficiently triggers various nonlinear and nonperturbative phenomena-such as multiple ionization-with an elliptically polarized pulse.
We study double ionization of Mg by electron impact through the vantage point of classical mechanics. We consider all electron-electron correlations in a Coulomb four-body problem, where three electrons belong to the atom and the fourth electron causes the impact ionization. From our model we compute the double-ionization probability of Mg for impact energies from 15 to 125 eV. Double ionization occurs through eight double-ionization mechanisms, which we classify into four categories: inner shell capture, direct, delay, and ionized inner shell mechanisms. We show that delay and ionized inner shell mechanisms require electron-electron correlations among the four electrons, and are responsible for the second increase in the double-ionization probability. Furthermore, we show that our theoretical prediction about the relative prominence of certain double-ionization mechanisms is in agreement with experimental results on the relative prominence of non-first-over first-order mechanisms.
We study the double ionization of atoms subjected to circularly polarized (CP) laser pulses. We analyze two fundamental ionization processes: the sequential (SDI) and nonsequential (NSDI) double ionization in the light of the rotating frame (RF) which naturally embeds nonadiabatic effects in CP pulses. We use and compare two adiabatic approximations: The adiabatic approximation in the laboratory frame (LF) and the adiabatic approximation in the RF. The adiabatic approximation in the RF encapsulates the energy variations of the electrons on subcycle timescales happening in the LF and this, by fully taking into account the ion-electron interaction. This allows us to identify two nonadiabatic effects including the lowering of the threshold intensity at which over-the-barrier ionization happens and the lowering of the ionization time of the electrons. As a consequence, these nonadiabatic effects facilitate over-the-barrier ionization and recollision-induced ionizations. We analyze the outcomes of these nonadiabatic effects on the recollision mechanism. We show that the laser envelope plays an instrumental role in a recollision channel in CP pulses at the heart of NSDI.
We investigate the role of the Coulomb interaction in strong field processes. We find that the Coulomb field of the ion makes its presence known even in highly intense laser fields, in contrast to the assumptions of the strong field approximation. The dynamics of the electron after ionization is analyzed with four models for an arbitrary laser polarization: the Hamiltonian model in the dipole approximation, the strong field approximation, the Coulomb-corrected strong field approximation and the guiding center. These models illustrate clearly the Coulomb effects, in particular Coulomb focusing and Coulomb asymmetry. We show that the Coulomb-corrected strong field approximation and the guiding center are complementary, in the sense that the Coulomb-corrected strong field approximation describes well short time scale phenomena (shorter than a laser cycle) while the guiding center is well suited for describing long time scale phenomena (longer than a laser cycle) like Coulomb-driven recollisions and Rydberg state creation.
We study the behavior of reduced models for the propagation of intense laser pulses in atomic gases. The models we consider incorporate ionization, blueshifting, and other nonlinear propagation effects in an ab initio manner, by explicitly taking into account the microscopic electron dynamics. Numerical simulations of the propagation of ultrashort linearly-polarized and elliptically-polarized laser pulses over experimentally-relevant propagation distances are presented. We compare the behavior of models where the electrons are treated classically with those where they are treated quantum-mechanically. A classical equivalent to the ground state is found, which maximizes the agreement between the quantum and classical predictions of the single-atom ionization probability as a function of laser intensity. We show that this translates into quantitative agreement between the quantum and classical models for the laser field evolution during propagation through gases of ground-state atoms. This agreement is exploited to provide a classical perspective on low- and high-order harmonic generation in linearly-polarized fields. In addition, we demonstrate the stability of the polarization of a nearly-linearly-polarized pulse using a two-dimensional model.
We consider the theoretical description of intense laser pulses propagating through gases. Starting from a first-principles description of both the electromagnetic field and the electron motion within the gas atoms, we derive a hierarchy of reduced models. We obtain a parallel set of models, where the atomic electrons are treated classically on the one hand, and quantum-mechanically on the other. By working consistently in either a Lagrangian formulation or a Hamiltonian formulation, we ensure that our reduced models preserve the variational structure of the parent models. Taking advantage of the Hamiltonian formulation, we deduce a number of conserved quantities of the reduced models.
We consider the dynamics of electrons in combined strong laser and Coulomb fields. Under a timescale separation condition, we reduce this dynamics to a guiding-center framework. More precisely, we derive a hierarchy of models for the guiding-center dynamics based on averaging over the fast motion of the electron using Lie transforms. The reduced models we obtain describe well the different ionization channels, in particular, the conditions under which an electron is rescattered by the ionic core or is directly ionized. The comparison between these models highlights the models which are best suited for a qualitative and quantitative agreement with the parent dynamics.
Electron motion in combined strong laser and Coulomb fields is central to laser-matter interactions. By mapping this problem onto the motion of a guiding center, we derive a reduced model which naturally embeds important Coulomb effects such as focusing and asymmetry, and clearly distinguishes direct versus rescattered electron ionization processes. We demonstrate the power of this tool by unraveling the bifurcation in photoelectron momentum distributions seen in experiments.
We present a classical model for high-order harmonic generation during the propagation of an intense laser pulse through an atomic gas. Numerical simulations of the model show excellent quantitative agreement with the corresponding quantum model for the blueshift and intensity reduction of the propagating laser pulse over experimentally realistic propagation distances. We observe a significant extension of the high-order harmonic cutoff due to propagation effects. A phase-space analysis of our classical model uncovers the mechanism behind this extension.
We consider electron impact-driven single and double ionization of magnesium in the 10-100 eV energy range. Our classical Hamiltonian model of these (e, 2e) and (e, 3e) processes sheds light on their total cross sections and reveals the underlying ionization mechanisms. Two pathways are at play in single ionization: Delayed and direct. In contrast, only the direct process is observed in double ionization, ruling out the excitation-autoionization channel. We also provide evidence that the so-called TS2 (Two-Step 2) mechanism predominates over the TS1 (Two-Step 1) mechanism, in agreement with experiments.
We investigate the process of circularly polarized high harmonic generation in molecules using a bicircular laser field. In this context, we show that molecules offer a very robust framework for the production of circularly polarized harmonics, provided their symmetry is compatible with that of the laser field. Using a discrete time-dependent symmetry analysis, we show how all the features (harmonic order and polarization) of spectra can be explained and predicted. The symmetry analysis is generic and can easily be applied to other target and/or field configurations.
We revisit the stabilization of ionization of atoms subjected to a superintense laser pulse using nonlinear dynamics. We provide an explanation for the lack of complete ionization at high intensity and for the decrease of the ionization probability as intensity is increased. We investigate the role of each part of the laser pulse (ramp-up, plateau, ramp-down) in this process. We emphasize the role of the choice for the ionization criterion, energy versus distance criterion.
Over a century after Bohr's the initial quantization of hydrogen, the semiclassical quantization of atomic systems still represents a challenge. In the present paper, we re-examine the semiclassical quantization of hydrogen asking the question: How can hydrogen be quantized without making use of its separability? The approach adopted was to explicitly a construct transformation from the physical variable to the action-angle variables. The initial difficulty encountered is the lack of an equilibrium point on the potential energy surface. To surmount this diffi culty, it is noted that the circular periodic orbits are relative equilibria. In a rotating frame, the relative equilibria become critical points in the phase fl ow. It is shown that the fl ow in the vicinity of the critical point is stable. The Lie–Deprit transformation is then used to transform the system into normal form, following which the semiclassical quantization is straightforward.
Using numerical simulations, we show that atomic high order harmonic generation (HHG) with a circularly polarized laser field offers an ideal framework for quantum-classical correspondence in strong field physics. With an appropriate initialization of the system, corresponding to a superposition of ground and excited state(s), simulated HHG spectra display a narrow strip of strong harmonic radiation preceded by a gap of missing harmonics in the lower part of the spectrum. In specific regions of the spectra, HHG tends to lock to circularly polarized harmonic emission. All these properties are shown to be closely related to a set of key classical periodic orbits that organize the recollision dynamics in an intense, circularly polarized field.
We present a purely classical recollision scenario, i.e., without tunneling, which, in contrast to the standard three-step model, takes into account the ionic core potential fully at all stages of the recollision process and is valid at all intensities. We find that a key periodic orbit drives the recollisions by guiding electrons away and back to the core. At sufficiently high intensity, we connect our scenario to the three-step model, and explain why the three-step model leads to good agreement with the cutoff in high harmonic generation despite neglecting the core potential after tunneling.
We show that a family of key periodic orbits drives the recollision process in a strong circularly polarized laser field. These orbits, coined recolliding periodic orbits, exist for a wide range of parameters, and their relative influence changes as the laser and atomic parameters are varied. We find the necessary conditions for recollision-driven nonsequential double ionization to occur. The outlined mechanism is universal in that it applies equally well beyond atoms: The internal structure of the target species plays a minor role in the recollision process.
Classical models in strong field physics typically require a careful selection of initial conditions which correspond accurately to the state selection. We compare two such procedures, the (many) pilot atom technique and the microcanonical strategy. We show that for some range of parameters, the pilot atom strategy may lead to artifacts due to the correlations between the different initial conditions. On the other hand, the microcanonical strategy is, by design, free of such artifacts for all admissible parameters.
We analyze the dynamics of a valence electron of the buckminsterfullerene molecule (C60) subjected to a circularly polarized laser field by modeling it with the motion of a classical particle in an annular billiard. We show that the phase space of the billiard model gives rise to three distinct trajectories: "whispering gallery orbits," which hit only the outer billiard wall; "daisy orbits," which hit both billiard walls (while rotating solely clockwise or counterclockwise for all time); and orbits that only visit the downfield part of the billiard, as measured relative to the laser term. These trajectories, in general, maintain their distinct features, even as the intensity is increased from 10(10) to 10(14) Wcm-2. We attribute this robust separation of phase space to the existence of twistless tori.