Estimating the plasmonic field enhancement using high-order harmonic generation: The role of inhomogeneity of the fields

In strong field laser physics it is a common practice to use the high-order harmonic cutoff to estimate the laser intensity of the pulse that generates the harmonic radiation. Based on the semiclassical arguments it is possible to find a direct relationship between the maximum value of the photon energy and the laser intensity. This approach is only valid if the electric field driving HHG is spatially homogenous. In laser-matter processes driven by plasmonics fields, the enhanced fields present a spatial dependence that strongly modifies the electron motion and consequently the laser driven phenomena. As a result, this method should be revised in order to more realistically estimate the field. In this work, we demonstrate how the inhomogeneity of the fields will effect this estimation. Furthermore, by employing both quantum mechanical and classical calculations, we show how one can obtain a better estimation for the intensity of the enhanced field in plasmonic nanostructure.Comment: 7 pages and 2 figure

Excitation, two-center interference and the orbital geometry in laser-induced nonsequential double ionization of diatomic molecules

We address the influence of the molecular orbital geometry and of the molecular alignment with respect to the laser-field polarization on laser-induced nonsequential double ionization of diatomic molecules for different molecular species, namely $\mathrm{N}_2$ and $\mathrm{Li}_2$. We focus on the recollision excitation with subsequent tunneling ionization (RESI) mechanism, in which the first electron, upon return, promotes the second electron to an excited state, from where it subsequently tunnels. We show that the electron-momentum distributions exhibit interference maxima and minima due to the electron emission at spatially separated centers. We provide generalized analytical expressions for such maxima or minima, which take into account $s$ $p$ mixing and the orbital geometry. The patterns caused by the two-center interference are sharpest for vanishing alignment angle and get washed out as this parameter increases. Apart from that, there exist features due to the geometry of the lowest occupied molecular orbital (LUMO), which may be observed for a wide range of alignment angles. Such features manifest themselves as the suppression of probability density in specific momentum regions due to the shape of the LUMO wavefunction, or as an overall decrease in the RESI yield due to the presence of nodal planes.Comment: 11 pages revtex, 2 figure

Laser-induced nonsequential double ionization at and above the recollision-excitation-tunneling threshold

We perform a detailed analysis of the recollision-excitation-tunneling (RESI) mechanism in laser-induced nonsequential double ionization (NSDI), in which the first electron, upon return, promotes a second electron to an excited state, from which it subsequently tunnels, based on the strong-field approximation. We show that the shapes of the electron momentum distributions carry information about the bound-state with which the first electron collides, the bound state to which the second electron is excited, and the type of electron-electron interaction. Furthermore, one may define a driving-field intensity threshold for the RESI physical mechanism. At the threshold, the kinetic energy of the first electron, upon return, is just sufficient to excite the second electron. We compute the distributions for helium and argon in the threshold and above-threshold intensity regime. In the latter case, we relate our findings to existing experiments. The electron-momentum distributions encountered are symmetric with respect to all quadrants of the plane spanned by the momentum components parallel to the laser-field polarization, instead of concentrating on only the second and fourth quadrants.Comment: 14 pages, 7 figure

Coherent XUV generation driven by sharp metal tips photoemission

It was already experimentally demonstrated that high-energy electrons can be generated using metal nanotips as active media. In addition, it has been theoretically proven that the high-energy tail of the photoemitted electrons is intrinsically linked to the recollision phenomenon. Through this recollision process it is also possible to convert the energy gained by the laser-emitted electron in the continuum in a coherent XUV photon. It means the emission of harmonic radiation appears to be feasible, although it has not been experimentally demonstrated hitherto till now. In this paper, we employ a quantum mechanical approach to model the electron dipole moment including both the laser experimental conditions and the bulk matter properties and predict is possible to generate coherent UV and XUV radiation using metal nanotips as sources. Our quantum mechanical results are fully supported by their classical counterparts.Comment: arXiv admin note: substantial text overlap with arXiv:1309.034

A rigorous treatment of excitation and quantum interference in laser-induced nonsequential double ionization of atoms and molecules

Electron-electron correlation, excitation and quantum interference are generally important in attosecond physics, especially for imaging of atoms and molecules. These are the main topics addressed in this thesis, in the context of laser-induced nonsequential double ionization (NSDI). Excitation is the most extensive topic of this work and is addressed within a rigorous, semi-analytic study of the recollision-excitation with subsequent tunneling ionization (RESI) mechanism in laser-induced nonsequential double ionization (NSDI). This is the most comprehensive study of this mechanism performed in the context of the strong-field approximation to the preset date. Subsequently, we investigate potential imaging applications, by computing electron momentum distributions of atoms and molecules. For atoms, we show that the RESI electron momentum distributions depends very critically on the bound state wave function. For molecules, we address the influence of the molecular orbital geometry and of the molecular alignment with respect to the laser-field polarization, by computing the electron momentum distributions of N2 and Li2. We show that the electron-momentum distributions exhibit interference maxima and minima, either due to the electron emission at spatially separated centers, or to the orbital geometry, such as nodes of the atomic wavefunction. In this latter case, we do not restrict ourself only to RESI, and we also compute the electron momentum distributions of N2 for electron-impact ionization, in which we also observe two-center interference patterns when the molecule is aligned along the laserfield polarization direction. The above-mentioned momentum constraints, together with the strong dependence of the distributions on the bound states involved, the molecular orbital geometry and the molecular alignment angle may be important for singling out the RESI mechanism in actual physical situations and using NSDI in ultra-fast imaging. In the final chapter, we present the first step taken by us in order to address the above-stated issues using an approach beyond the strong field approximation

Causality and quantum interference in time-delayed laser-induced nonsequential double ionization

We perform a detailed analysis of the importance of causality within the strong-field approximation and the steepest-descent framework for the recollision-excitation with subsequent tunneling ionization (RESI) pathway in laser-induced nonsequential double ionization (NSDI). In this time-delayed pathway, an electron returns to its parent ion and, by recolliding with the core, gives part of its kinetic energy to excite a second electron at a time t′. The second electron then reaches the continuum at a later time t by tunneling ionization. We show that, if t′ and t are complex, the condition that recollision of the first electron occurs before tunnel ionization of the second electron translates into boundary conditions for the steepest-descent contours and thus puts constraints on the saddles to be taken when computing the RESI transition amplitudes. We also show that this generalized causality condition has a dramatic effect on the shapes of the RESI electron momentum distributions for few-cycle laser pulses. Physically, causality determines how the dominant sets of orbits of an electron returning to its parent ion can be combined with the dominant orbits of a second electron tunneling from an excited state. All features encountered are analyzed in terms of such orbits and their quantum interference

Time-delayed nonsequential double ionization with few-cycle laser pulses: importance of the carrier-envelope phase

We perform theoretical investigations of laser-induced nonsequential double ionization with few cycle pulses, with particular emphasis on the dependence of the electron-momentum distributions on the carrier-envelope phase. We focus on the recollision-excitation with subsequent tunneling ionization (RESI) pathway, in which a released electron, upon return to its parent ion, gives part of its kinetic energy to promote a second electron to an excited state. At a subsequent time, the second electron is freed through tunneling ionization. We show that the RESI electron-momentum distributions vary dramatically with regard to the carrier-envelope phase. By performing a detailed analysis of the dynamics of the two active electrons in terms of quantum orbits, we relate the shapes and the momentum regions populated by such distributions to the dominant set of orbits along which rescattering of the first electron and ionization of the second electron occurs. These orbits can be manipulated by varying the carrier-envelope phase. This opens a wide range of possibilities for controlling correlated attosecond electron emission by an adequate pulse choice.Comment: 12 pages, 7 figures, 1 tabl