Non-classical high harmonic generation in graphene driven by linearly-polarized laser pulses.

Recent studies in high-order harmonic generation (HHG) in solid targets reveal new scenarios of extraordinary rich electronic dynamics, in comparison to the atomic and molecular cases. For the later, the main aspects of the process can be described semiclassically in terms of electrons that recombine when the trajectories revisit the parent ion. HHG in solids has been described by an analogous mechanism, in this case involving electron-hole pair recombinations. However, it has been recently reported that a substantial part of the HHG emission corresponds to situations where the electron and hole trajectories do not overlap in space. According to the present knowledge, HHG from this imperfect recollisions reflects the quantum nature of the process, arising in systems with large Berry curvatures or for elliptically polarized driving fields. In this work, we demonstrate that imperfect recollisions are also relevant in the more general case. We show the signature of such recollisions in the HHG spectrum from monolayer graphene -a system with null Berry curvature- irradiated by linearly polarized driving fields. Our calculations also reveal that imperfect multiple-order recollisions contribute to the harmonic emission when electron-hole excursion times exceed one cycle of the driving field. We believe that our work adds a substantial contribution to the full understanding of the sub-femtosecond dynamics of HHG in solid systems.

Necklace-structured high-harmonic generation for low-divergence, soft x-ray harmonic combs with tunable line spacing.

The extreme nonlinear optical process of high-harmonic generation (HHG) makes it possible to map the properties of a laser beam onto a radiating electron wave function and, in turn, onto the emitted x-ray light. Bright HHG beams typically emerge from a longitudinal phased distribution of atomic-scale quantum antennae. Here, we form a transverse necklace-shaped phased array of linearly polarized HHG emitters, where orbital angular momentum conservation allows us to tune the line spacing and divergence properties of extreme ultraviolet and soft x-ray high-harmonic combs. The on-axis HHG emission has extremely low divergence, well below that obtained when using Gaussian driving beams, which further decreases with harmonic order. This work provides a new degree of freedom for the design of harmonic combs-particularly in the soft x-ray regime, where very limited options are available. Such harmonic beams can enable more sensitive probes of the fastest correlated charge and spin dynamics in molecules, nanoparticles, and materials.

Transverse phase matching of high-order harmonic generation in single-layer graphene.

The efficiency of high-harmonic generation (HHG) from a macroscopic sample is strongly linked to the proper phase matching of the contributions from the microscopic emitters. We develop a combined micro+macroscopic theoretical model that allows us to distinguish the relevance of high-order harmonic phase matching in single-layer graphene. For a Gaussian driving beam, our simulations show that the relevant HHG emission is spatially constrained to a phase-matched ring around the beam axis. This remarkable finding is a direct consequence of the non-perturbative behavior of HHG in graphene-whose harmonic efficiency scaling is similar to that already observed in gases- and bridges the gap between the microscopic and macroscopic HHG in single-layer graphene.

Trains of attosecond pulses structured with time-ordered polarization states.

Ultrafast laser pulses generated at the attosecond timescale represent a unique tool to explore the fastest dynamics in matter. An accurate control of their properties, such as polarization, is fundamental to shape three-dimensional laser-driven dynamics. We introduce a technique to generate attosecond pulse trains whose polarization state varies from pulse to pulse. This is accomplished by driving high-harmonic generation with two time-delayed bichromatic counter-rotating fields with proper orbital angular momentum (OAM) content. Our simulations show that the evolution of the polarization state along the train can be controlled via OAM, pulse duration, and time delay of the driving fields. We, thus, introduce an additional control into structured attosecond pulses that provides an alternative route to explore ultrafast dynamics with potential applications in chiral and magnetic materials.

High harmonic generation in armchair carbon nanotubes.

We study high-order harmonic generation (HHG) in armchair-type single-wall carbon nanotubes (SWNTs) driven by ultrashort, mid-infrared laser pulses. For a SWNT with chiral indices (n, n), we demonstrate that HHG is dominated by bands |m| = n - 1 and that the cut-off frequency saturates with intensity, as it occurs in the case of single layer graphene. As a consequence, HHG in SWNTs can be described effectively as a one-dimensional periodic system, whose high-frequency emission can be modified through the proper control of the structural parameters. Additionally, we show that the HHG mechanism in nanotubes has some similarities to that previously reported in single layer graphene. However, as a main difference, the electron-hole pair excitation in SWNTs is connected to the non-adiabatic crossing through the first van Hove singularity of the |m| = n - 1 bands, instead of the crossing through the Dirac point that takes place in graphene.

Generation of extreme-ultraviolet beams with time-varying orbital angular momentum.

Light fields carrying orbital angular momentum (OAM) provide powerful capabilities for applications in optical communications, microscopy, quantum optics, and microparticle manipulation. We introduce a property of light beams, manifested as a temporal OAM variation along a pulse: the self-torque of light. Although self-torque is found in diverse physical systems (i.e., electrodynamics and general relativity), it was not realized that light could possess such a property. We demonstrate that extreme-ultraviolet self-torqued beams arise in high-harmonic generation driven by time-delayed pulses with different OAM. We monitor the self-torque of extreme-ultraviolet beams through their azimuthal frequency chirp. This class of dynamic-OAM beams provides the ability for controlling magnetic, topological, and quantum excitations and for manipulating molecules and nanostructures on their natural time and length scales.

Conservation of Torus-knot Angular Momentum in High-order Harmonic Generation.

High-order harmonic generation stands as a unique nonlinear optical up-conversion process, mediated by a laser-driven electron recollision mechanism, which has been shown to conserve energy, linear momentum, and spin and orbital angular momentum. Here, we present theoretical simulations that demonstrate that this process also conserves a mixture of the latter, the torus-knot angular momentum J_{γ}, by producing high-order harmonics with driving pulses that are invariant under coordinated rotations. We demonstrate that the charge J_{γ} of the emitted harmonics scales linearly with the harmonic order, and that this conservation law is imprinted onto the polarization distribution of the emitted spiral of attosecond pulses. We also demonstrate how the nonperturbative physics of high-order harmonic generation affect the torus-knot angular momentum of the harmonics, and we show that this configuration harnesses the spin selection rules to channel the full yield of each harmonic into a single mode of controllable orbital angular momentum.

Optical anisotropy of non-perturbative high-order harmonic generation in gapless graphene.

High harmonic generation in atomic or molecular targets stands as a robust mechanism to produce coherent ultrashort pulses with controllable polarization in the extreme-ultraviolet. However, the production of elliptically or circularly-polarized harmonics is not straightforward, demanding complex combinations of elliptically or circularly-polarized drivers, or the use of molecular alignment techniques. Nevertheless, recent studies show the feasibility of high-harmonic generation in solids. In contrast with atoms and molecules, solids are high-density targets and therefore more efficient radiation sources. Among solid targets, 2D materials are of special interest due to their particular electronic structure, which conveys special optical properties. In this paper, we present theoretical calculations that demonstrate an extraordinary complex light-spin conversion in single-layer graphene irradiated at non perturbative intensities. Linearly-polarized drivings result in the emission of elliptically-polarized harmonics, and elliptically-polarized drivings may result in linearly-polarized or ellipticity-reversed harmonics. In addition, we demonstrate the ultrafast temporal modulation of the harmonic ellipticity.

Controlling the polarization and vortex charge of attosecond high-harmonic beams via simultaneous spin-orbit momentum conservation.

Optical interactions are governed by both spin and angular momentum conservation laws, which serve as a tool for controlling light-matter interactions or elucidating electron dynamics and structure of complex systems. Here, we uncover a form of simultaneous spin and orbital angular momentum conservation and show, theoretically and experimentally, that this phenomenon allows for unprecedented control over the divergence and polarization of extreme-ultraviolet vortex beams. High harmonics with spin and orbital angular momenta are produced, opening a novel regime of angular momentum conservation that allows for manipulation of the polarization of attosecond pulses-from linear to circular-and for the generation of circularly polarized vortices with tailored orbital angular momentum, including harmonic vortices with the same topological charge as the driving laser beam. Our work paves the way to ultrafast studies of chiral systems using high-harmonic beams with designer spin and orbital angular momentum.

Nonperturbative Twist in the Generation of Extreme-Ultraviolet Vortex Beams.

High-order harmonic generation (HHG) has been recently proven to produce extreme-ultraviolet (XUV) vortices from the nonlinear conversion of infrared twisted beams. Previous works have demonstrated a linear scaling law of the vortex charge with the harmonic order. We demonstrate that this simple law hides an unexpectedly rich scenario for the buildup of orbital angular momentum (OAM) due to the nonperturbative behavior of HHG. The complexity of these twisted XUV beams appears only when HHG is driven by nonpure vortex modes, where the XUV OAM content is dramatically increased. We explore the underlying mechanisms for this diversity and derive a general conservation rule for the nonperturbative OAM buildup. The simple scaling found in previous works corresponds to the collapse of this scenario for the particular case of pure (single-mode) OAM driving fields.

Tomographic reconstruction of circularly polarized high-harmonic fields: 3D attosecond metrology.

Bright, circularly polarized, extreme ultraviolet (EUV) and soft x-ray high-harmonic beams can now be produced using counter-rotating circularly polarized driving laser fields. Although the resulting circularly polarized harmonics consist of relatively simple pairs of peaks in the spectral domain, in the time domain, the field is predicted to emerge as a complex series of rotating linearly polarized bursts, varying rapidly in amplitude, frequency, and polarization. We extend attosecond metrology techniques to circularly polarized light by simultaneously irradiating a copper surface with circularly polarized high-harmonic and linearly polarized infrared laser fields. The resulting temporal modulation of the photoelectron spectra carries essential phase information about the EUV field. Utilizing the polarization selectivity of the solid surface and by rotating the circularly polarized EUV field in space, we fully retrieve the amplitude and phase of the circularly polarized harmonics, allowing us to reconstruct one of the most complex coherent light fields produced to date.

Ultraviolet surprise: Efficient soft x-ray high-harmonic generation in multiply ionized plasmas.

High-harmonic generation is a universal response of matter to strong femtosecond laser fields, coherently upconverting light to much shorter wavelengths. Optimizing the conversion of laser light into soft x-rays typically demands a trade-off between two competing factors. Because of reduced quantum diffusion of the radiating electron wave function, the emission from each species is highest when a short-wavelength ultraviolet driving laser is used. However, phase matching--the constructive addition of x-ray waves from a large number of atoms--favors longer-wavelength mid-infrared lasers. We identified a regime of high-harmonic generation driven by 40-cycle ultraviolet lasers in waveguides that can generate bright beams in the soft x-ray region of the spectrum, up to photon energies of 280 electron volts. Surprisingly, the high ultraviolet refractive indices of both neutral atoms and ions enabled effective phase matching, even in a multiply ionized plasma. We observed harmonics with very narrow linewidths, while calculations show that the x-rays emerge as nearly time-bandwidth-limited pulse trains of ~100 attoseconds.

Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers.

High harmonic generation driven by femtosecond lasers makes it possible to capture the fastest dynamics in molecules and materials. However, to date the shortest subfemtosecond (attosecond, 10(-18) s) pulses have been produced only in the extreme UV region of the spectrum below 100 eV, which limits the range of materials and molecular systems that can be explored. Here we experimentally demonstrate a remarkable convergence of physics: when midinfrared lasers are used to drive high harmonic generation, the conditions for optimal bright, soft X-ray generation naturally coincide with the generation of isolated attosecond pulses. The temporal window over which phase matching occurs shrinks rapidly with increasing driving laser wavelength, to the extent that bright isolated attosecond pulses are the norm for 2-µm driving lasers. Harnessing this realization, we experimentally demonstrate the generation of isolated soft X-ray attosecond pulses at photon energies up to 180 eV for the first time, to our knowledge, with a transform limit of 35 attoseconds (as), and a predicted linear chirp of 300 as. Most surprisingly, advanced theory shows that in contrast with as pulse generation in the extreme UV, long-duration, 10-cycle, driving laser pulses are required to generate isolated soft X-ray bursts efficiently, to mitigate group velocity walk-off between the laser and the X-ray fields that otherwise limit the conversion efficiency. Our work demonstrates a clear and straightforward approach for robustly generating bright isolated attosecond pulses of electromagnetic radiation throughout the soft X-ray region of the spectrum.

Attosecond extreme ultraviolet vortices from high-order harmonic generation.

We present a theoretical study of high-order harmonic generation (HHG) and propagation driven by an infrared field carrying orbital angular momentum (OAM). Our calculations unveil the following relevant phenomena: extreme-ultraviolet harmonic vortices are generated and survive to the propagation effects, vortices transport high-OAM multiples of the corresponding OAM of the driving field and, finally, the different harmonic vortices are emitted with similar divergence. We also show the possibility of combining OAM and HHG phase locking to produce attosecond pulses with helical pulse structure.

Bright coherent ultrahigh harmonics in the keV x-ray regime from mid-infrared femtosecond lasers.

High-harmonic generation (HHG) traditionally combines ~100 near-infrared laser photons to generate bright, phase-matched, extreme ultraviolet beams when the emission from many atoms adds constructively. Here, we show that by guiding a mid-infrared femtosecond laser in a high-pressure gas, ultrahigh harmonics can be generated, up to orders greater than 5000, that emerge as a bright supercontinuum that spans the entire electromagnetic spectrum from the ultraviolet to more than 1.6 kilo-electron volts, allowing, in principle, the generation of pulses as short as 2.5 attoseconds. The multiatmosphere gas pressures required for bright, phase-matched emission also support laser beam self-confinement, further enhancing the x-ray yield. Finally, the x-ray beam exhibits high spatial coherence, even though at high gas density the recolliding electrons responsible for HHG encounter other atoms during the emission process.

Ab initio calculation of the double ionization of helium in a few-cycle laser pulse beyond the one-dimensional approximation.

We present ab initio computations of the ionization of two-electron atoms by short pulses of intense linearly polarized Ti:sapphire laser radiation beyond the one-dimensional approximation. In the model the electron correlation is included in its full dimensionality, while the center-of-mass motion is restricted along the polarization axis. Our results exhibit a rich double ionization quantum dynamics in the direction transversal to the field polarization, which is neglected in the previous models based on the one-dimensional approximation.

Non-linear Young's double-slit experiment.

The Young's double slit experiment is recreated using intense and short laser pulses. Our experiment evidences the role of the non-linear Kerr effect in the formation of interference patterns. In particular, our results evidence a mixed mechanism in which the zeroth diffraction order of each slit are mainly affected by self-focusing and self-phase modulation, while the higher orders propagate linearly. Despite of the complexity of the general problem of non-linear propagation, we demonstrate that this experiment retains its simplicity and allows for a geometrical interpretation in terms of simple optical paths. In consequence, our results may provide key ideas on experiments on the formation of interference patterns with intense laser fields in Kerr media.

Lithium ionization by a strong laser field.

We study ab initio computations of the interaction of lithium with a strong laser field. Numerical solutions of the time-dependent fully correlated three-particle Schrodinger equation restricted to the one-dimensional soft-core approximation are presented. Our results show a clear transition from nonsequential to sequential double ionization for increasing intensities. Nonsequential double ionization is found to be sensitive to the spin configuration of the ionized pair. This asymmetry, also found in experiments of photoionization of Li with synchrotron radiation, shows evidence of the influence of the exclusion principle on the underlying rescattering mechanism.