We demonstrate a simple method to improve the Lewenstein model for the description of high-order harmonic generation (HHG). It is shown that HHG spectra can be expressed as the product of a returning electron wave packet and the photo-recombination cross sections, where the former can be extracted from the Lewenstein model. By replacing plane waves with scattering waves in the calculation of recombination matrix elements, we showed that the resulting HHG spectra agree well with those from solving the time-dependent Schrödinger equation. The improved model can be used for quantitative calculations of high harmonics generated by molecules.
A recent paper reported elliptically polarized high-order harmonics from aligned N$_2$ using a linearly polarized driving field [X. Zhou \emph{et al.}, Phys. Rev. Lett. \textbf{102}, 073902 (2009)]. This observation cannot be explained in the standard treatment of the Lewenstein model and has been ascribed to many-electron effects or the influence of the Coulomb force on the continuum electron. We show that non-vanishing ellipticity naturally appears within the Lewenstein model when using a multi-center stationary phase method for treating the dynamics of the continuum electron. The reason for…
The nonlinear ionization with accompanied photorecombination on closely located center has been considered. The radiation spectrum has been calculated in the frame of the Lewenstein-Corkum approach. The dependence of radiation on the distance between ionization point and the recombination center, and the frequency and laser field strength has been investigated.
High-order harmonic responses from three $C_{20}$ isomers: fullerene, ring, and bowl, are calculated within the modified Lewenstein model for molecular systems. Spectra for all three structures exhibit intense modulations of the harmonic spectrum along the plateau and some of them can be interpreted as a consequence of multi-center interference effects. Each structure shows characteristic modulation patterns in peak harmonic intensities, which are directly related to zeroes in the recombination matrix element as a function of the three components of momentum. Different C$_{20}$ isomers lead to…
The generation of harmonics by atoms or ions in a two-color, coplanar field configuration with commensurate frequencies is investigated through both, an analytical calculation based on the Lewenstein model and the numerical ab initio solution of the time-dependent Schroedinger equation of a two-dimensional model ion. Through the analytical model, selection rules for the harmonic orders in this field configuration, a generalized cut-off for the harmonic spectra, and an integral expression for the harmonic dipole strength is provided. The numerical results are employed to test the predictions of…
We introduce a semi-classical wavefunction (SCWF) model for strong-field physics and attosecond science. When applied to high harmonic generation (HHG), this formalism allows one to show that the natural time-domain separation of the contribution of ionization, propagation and recollisions to the HHG process leads to a frequency-domain factorization of the harmonic yield into these same contributions, for any choice of atomic or molecular potential. We first derive the factorization from the natural expression of the dipole signal in the temporal domain by using a reference system, as in the q…
We present a novel ab-initio single-electron approach to correlated electron dynamics in strong laser fields. By writing the electronic wavefunction as a product of a marginal one-electron wavefunction and a conditional wavefunction, we show that the exact harmonic spectrum can be obtained from a single-electron Schrödinger equation. To obtain the one-electron potential in practice, we propose an adiabatic approximation, i.e. a potential is generated that depends only on the position of one electron. This potential, together with the laser interaction, is then used to obtain the dynamics of th…
We present a generic approach for treating the effect of nuclear motion in the high-order harmonic generation from polyatomic molecules. Our procedure relies on a separation of nuclear and electron dynamics where we account for the electronic part using the Lewenstein model and nuclear motion enters as a nuclear correlation function. We express the nuclear correlation function in terms of Franck-Condon factors which allows us to decompose nuclear motion into modes and identify the modes that are dominant in the high-order harmonic generation process. We show results for the isotopes CH$_4$ and…
We investigate the connection of recently identified fine-scale oscillations in the dependence of the yield of the high-harmonic generation (HHG) on wavelength lambda of a few-cycle laser pulse [K. Schiessl, K.L. Ishikawa, E. Persson, and J. Burgdorfer, Phys. Rev. Lett. 99, 253903 (2007)] to the well-known channel closing (CC) effect. Using the Lewenstein model of HHG, we identify the origin of the oscillations as quantum interference of many rescattering trajectories. By studying the simultaneous variations with intensity and wavelength, different models for the interference of channel closin…
We investigate the electron quantum path interference effects during high harmonic generation in atomic gas medium driven by ultrashort chirped laser pulses. To achieve that, we identify and vary the different experimentally relevant control parameters of such a driving laser pulse influencing the high harmonic spectra. Specifically, the impact of the pulse duration, peak intensity and instantaneous frequency is studied in a self-consistent manner based on Lewenstein formalism. Simulations involving macroscopic propagation effects are also considered. The study aims to reveal the microscopic b…
We investigate high-order harmonic generation from a Bohmian-mechanical perspective, and find that the innermost part of the core, represented by a single Bohmian trajectory, leads to the main contributions to the high-harmonic spectra. Using time-frequency analysis, we associate this central Bohmian trajectory to an ensemble of unbound classical trajectories leaving and returning to the core, in agreement with the three step model. In the Bohmian scenario, this physical picture builds up non-locally near the core via the quantum mechanical phase of the wavefunction. This implies that the flow…
We report theoretical investigations of the tomographic procedure suggested by Itatani {\it et al.} [Nature, {\bf 432} 867 (2004)] for reconstructing highest occupied molecular orbitals (HOMO) using high-order harmonic generation (HHG). Using the limited range of harmonics from the plateau region, we found that under the most favorable assumptions, it is still very difficult to obtain accurate HOMO wavefunction, but the symmetry of the HOMO and the internuclear separation between the atoms can be accurately extracted, especially when lasers of longer wavelengths are used to generate the HHG. W…
The relation between high-harmonic spectra and the geometry of the molecular orbitals in position and momentum space is investigated. In particular we choose two isoelectronic pairs of homonuclear and heteronuclear molecules, such that the highest occupied molecular orbital of the former exhibit at least one nodal plane. The imprint of such planes is a strong suppression in the harmonic spectra, for particular alignment angles. We are able to identify two distinct types of nodal planes. If the nodal planes are determined by the atomic wavefunctions only, the angle for which the yield is suppre…
We analyze the imprint of nodal planes in high-order harmonic spectra from aligned diatomic molecules in intense laser fields whose components exhibit orthogonal polarizations. We show that the typical suppression in the spectra associated to nodal planes is distorted, and that this distortion can be employed to map the electron's angle of return to its parent ion. This investigation is performed semi-analytically at the single-molecule response and single-active orbital level, using the strong-field approximation and the steepest descent method. We show that the velocity form of the dipole op…
We investigate the quantum dynamics of two bosons, trapped in a two-dimensional harmonic trap, upon quenching arbitrarily their interaction strength thereby covering the entire energy spectrum. Utilizing the exact analytical solution of the stationary system we derive a closed analytical form of the expansion coefficients of the time-evolved two-body wavefunction, whose dynamics is determined by an expansion over the postquench eigenstates. The emergent dynamical response of the system is analyzed in detail by inspecting several observables such as the fidelity, the reduced one-body densities,…
We make a detailed assessment of which form of the dipole operator to use in calculating high order harmonic generation within the framework of the strong field approximation, and look specifically at the role the form plays in the inclusion of multielectron effects perturbatively with regard to the contributions of the highest occupied molecular orbital. We focus on how these corrections affect the high-order harmonic spectra from aligned homonuclear and heteronuclear molecules, exemplified by $\mathrm{N}_2$ and CO, respectively, which are isoelectronic. We find that the velocity form incorre…
The Qprop package is presented. Qprop has been developed to study laser-atom interaction in the nonperturbative regime where nonlinear phenomena such as above-threshold ionization, high order harmonic generation, and dynamic stabilization are known to occur. In the nonrelativistic regime and within the single active electron approximation, these phenomena can be studied with Qprop in the most rigorous way by solving the time-dependent Schrödinger equation in three spatial dimensions. Because Qprop is optimized for the study of quantum systems that are spherically symmetric in their initial, un…
Exponential localization of wavefunctions in lattices, whether in real or synthetic dimensions, is a fundamental wave interference phenomenon. Localization of Bloch-type functions in space-periodic lattice, triggered by spatial disorder, is known as Anderson localization and arrests diffusion of classical particles in disordered potentials. In time-periodic Floquet lattices, exponential localization in a periodically driven quantum system similarly arrests diffusion of its classically chaotic counterpart in the action-angle space. Here we demonstrate that nonlinear optical response allows for …
Generation of high-order harmonics in gases enabled to probe the attosecond electron dynamics in atoms and molecules with unprecedented resolution. Extending the techniques developed originally for atomic and molecular gases to solid state materials requires a fundamental understanding of the physics that has been partially addressed theoretically. Here we employ time-dependent density-functional theory to investigate how the electron dynamics resulting in high-harmonic emission in monolayer hexagonal boron nitride is affected by the presence of vacancies. We show how these realistic spin-pola…
