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In the rapidly evolving field of structured light, the self-torque has been recently defined as an intrinsic property of light beams carrying time-dependent orbital angular momentum. In particular, extreme-ultraviolet (EUV) beams with self-torque -- exhibiting a topological charge that continuously varies on the subfemtosecond timescale -- are naturally produced in high-order harmonic generation (HHG) when driven by two time-delayed intense infrared vortex beams with different topological charges. Until now, the polarization state of such EUV beams carrying self-torque has been restricted to linear states due to the drastic reduction in the harmonic up-conversion efficiency with increasing the ellipticity of the driving field. In this work, we theoretically demonstrate how to control the polarization state of EUV beams carrying self-torque, from linear to circular. The extremely high sensitivity of HHG to the properties of the driving beam allows us to propose two different driving schemes to circumvent the current limitations to manipulate the polarization state of EUV beams with self-torque. Our advanced numerical simulations are complemented with the derivation of selection rules of angular momentum conservation, which enable precise tunability over the angular momentum properties of the harmonics with self-torque. The resulting high-order harmonic emission, carrying time-dependent orbital angular momentum with a custom polarization state, can expand the applications of ultrafast light-matter interactions, particularly in areas where dichroic or chiral properties are crucial, such as magnetic materials or chiral molecules.

We present a numerical experiment that demonstrates the possibility to capture topological phase transitions via an x-ray absorption spectroscopy scheme. We consider a Chern insulator whose topological phase is tuned via a second-order hopping. We perform time-dynamics simulations of the out-of-equilibrium laser-driven electron motion that enables us to model a realistic attosecond spectroscopy scheme. In particular, we use an ultrafast scheme with a circularly polarized IR pump pulse and an attosecond x-ray probe pulse. A laser-induced dichroism-type spectrum shows a clear signature of the topological phase transition. We are able to connect these signatures with the Berry structure of the system. This work extend the applications of attosecond absorption spectroscopy to systems presenting a non-trivial topological phase.

High-order harmonic generation driven by intense extreme ultraviolet (EUV) fields merges quantum optics and attosecond science, giving rise to an appealing route for the generation of coherent EUV and soft X-ray light for high-resolution imaging and spectroscopies. We theoretically investigate ultrafast resonant dynamics during the interaction of He atoms with strong extreme ultraviolet pulses. At high driving intensities, we identify record fast attosecond Rabi oscillations imprinting observable signatures in the high harmonic spectrum. At field strengths suppressing the Coulomb potential barrier for all the bounded states, we demonstrate the survival of the attosecond two-level dynamics for several Rabi cycles. Consequently, this intense EUV laser-atom interaction reveals a new strong-field scenario where the resonant coupling of two-level bound-bound transitions prevails, contrasting with the dominance of bound-continuum transitions in the conventional strong-field infrared regimes. These findings set an interesting perspective for extreme attosecond nonlinear optics with intense short-wavelength fields., Comment: Main text (6 pages) and supplementary materials (5 pages)

High harmonic generation 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 > 5000, that emerge as a bright supercontinuum that spans the entire electromagnetic spectrum from the ultraviolet to > 1.6 keV, allowing in-principle the generation of pulses as short as 2.5 attoseconds. The multi-atmosphere gas pressures required for bright, phase matched emission also supports 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 high harmonic generation encounter other atoms during the emission process., Comment: 32 pages, 9 figures (4 in main text, 5 in supplemental materials)

The landscape of ultrafast structured light pulses has recently evolved driven by the capability of high-order harmonic generation (HHG) to up-convert orbital angular momentum (OAM) from the infrared to the extreme-ultraviolet (EUV) spectral regime. Accordingly, HHG has been proven to produce EUV vortex pulses at the femtosecond timescale. Here we demonstrate the generation of attosecond vortex pulse trains, i.e. a succession of attosecond pulses with a helical wavefront, resulting from the synthesis of a comb of EUV high-order harmonics with the same OAM. By driving HHG with a polarization tilt-angle fork grating, two spatially separated circularly polarized high-order harmonic beams with order-independent OAM are created. Our work opens the route towards attosecond-resolved OAM light-matter interactions., Comment: Main text (1-14 pages) and supplemental material (14-16 pages)

Structured ultrafast laser beams offer unique opportunities to explore the interplay of the angular momentum of light with matter at the femtosecond scale. Linearly polarized vector beams are paradigmatic examples of structured beams whose topology is characterized by a well-defined Poincar\'e index. It has been demonstrated that the Poincar\'e index is a topological invariant during high-order harmonic generation from isotropic targets, such as noble gases. As a result, harmonics are produced as extreme-ultraviolet vector beams, with the same topology as the driver. We demonstrate that this simple conservation rule does not apply to crystalline solids, characterized by their anisotropic non-linear response to the driving excitation. In this context, we identify the topological properties of the harmonic field as unique probes, sensitive to both the microscopic and macroscopic features of the target's complex non-linear response. Our simulations, performed in single-layer graphene but extendable to other solid targets, show that the harmonic field is split into a multi-beam structure whose topology -- different from that of the driver -- encodes information about laser-driven electronic dynamics. Our work opens the route towards using the topological analysis of the high-order harmonic field as a novel spectroscopic tool to reveal the coupling of light and target symmetries in the non-linear response of matter.

Vigorous efforts to harness the topological properties of light have enabled a multitude of novel applications. Translating the applications of structured light to higher spatial and temporal resolutions mandates their controlled generation, manipulation, and thorough characterization in the short-wavelength regime. Here, we resort to high-order harmonic generation (HHG) in a noble gas to upconvert near-infrared (IR) vector, vortex, and vector-vortex driving beams that are tailored respectively in their Spin Angular Momentum (SAM), Orbital Angular Momentum (OAM), and simultaneously in their SAM and OAM. We show that HHG enables the controlled generation of extreme-ultraviolet (EUV) vector beams exhibiting various spatially-dependent polarization distributions, or EUV vortex beams with a highly twisted phase. Moreover, we demonstrate the generation of EUV vector-vortex beams (VVB) bearing combined characteristics of vector and vortex beams. We rely on EUV wavefront sensing to unambiguously affirm the topological charge scaling of the HHG beams with the harmonic order. Interestingly, our work shows that HHG allows for a synchronous controlled manipulation of SAM and OAM. These EUV structured beams bring in the promising scenario of their applications at nanometric spatial and sub-femtosecond temporal resolutions using a table-top harmonic source., Comment: 13 pages, 6 figures

Ultrafast laser pulses provide unique tools to manipulate magnetization dynamics at femtosecond timescales, where the interaction of the electric field -- such as excitation of spin carriers to non-equilibrium states, generation of localized charge currents, demagnetization, or inverse Faraday effect -- dominates over the magnetic field. Recent proposals using structured laser beams have enlightened the possibility to generate intense femtosecond magnetic fields, spatially isolated from the electric field. Here we demonstrate the relevance of this novel scenario to femtomagnetism, unveiling the purely precessional, non-linear, chiral response of the magnetization when subjected to circularly polarized magnetic fields. This fundamental result not only opens an avenue in the study of laser-induced ultrafast magnetization dynamics, but also sustains technological implications as a route to promote all-optical non-thermal magnetization switching both at shorter timescales -- towards the attosecond regime -- and at THz frequencies.

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 wavefunction, 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 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., Comment: Submitted to Science Advances

Twisted light fields carrying orbital angular momentum (OAM) provide powerful capabilities for applications in optical communications, microscopy, quantum optics and microparticle rotation. Here we introduce and experimentally validate a new class of light beams, whose unique property is associated with a temporal OAM variation along a pulse: the self-torque of light. Self-torque is a phenomenon that can arise from matter-field interactions in electrodynamics and general relativity, but to date, there has been no optical analog. In particular, the self-torque of light is an inherent property, which is distinguished from the mechanical torque exerted by OAM beams when interacting with physical systems. We demonstrate that self-torqued beams in the extreme-ultraviolet (EUV) naturally arise as a necessary consequence of angular momentum conservation in non-perturbative high-order harmonic generation when driven by time-delayed pulses with different OAM. In addition, the time-dependent OAM naturally induces an azimuthal frequency chirp, which provides a signature for monitoring the self-torque of high-harmonic EUV beams. Such self-torqued EUV beams can serve as unique tools for imaging magnetic and topological excitations, for launching selective excitation of quantum matter, and for manipulating molecules and nanostructures on unprecedented time and length scales., Comment: 24 pages, 4 figures

We report a novel scheme to generate laser-induced, ultrafast, intense (Tesla scale), spatially isolated, magnetic fields. Three-dimensional particle-in-cell simulations show that a femtosecond azimuthally-polarized infrared vector beam, aimed to a conducting circular aperture, produces an intense axially polarized tip-shaped femtosecond magnetic field, extending over micrometer distances and being isolated from the electric field. Our results are backed-up by an analytic model, demonstrating the underlying physics and guiding for optimal parameters. In particular, we find the conditions under which the magnetic nanoprobe is substantially enhanced, reaching 4 T when driven by a $10^{11}$ W/cm$^2$ laser field, which reflects a selective enhancement by a factor of $\sim$6. Our scheme offers a promising tool to control, probe and tailor magnetic nanodomains in femtosecond timescales through pure magnetic interaction by using structured laser beams.

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, momentum, and spin and orbital angular momentum. Here we present theoretical simulations which demonstrate that this process also conserves a mixture of the latter, the torus-knot angular momentum $J_\gamma$, by producing high-order harmonics with driving pulses that are invariant under coordinated rotations. We demonstrate that the charge $J_\gamma$ 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., Comment: Accepted Manuscript

In this work we study the impact of chromatic focusing of few-cycle laser pulses on high-order harmonic generation (HHG) through analysis of the emitted extreme ultraviolet (XUV) radiation. Chromatic focusing is usually avoided in the few-cycle regime, as the pulse spatio-temporal structure may be highly distorted by the spatiotemporal aberrations. Here, however, we demonstrate it as an additional control parameter to modify the generated XUV radiation. We present experiments where few-cycle pulses are focused by a singlet lens in a Kr gas jet. The chromatic distribution of focal lengths allows us to tune HHG spectra by changing the relative singlet-target distance. Interestingly, we also show that the degree of chromatic aberration needed to this control does not degrade substantially the harmonic conversion efficiency, still allowing for the generation of supercontinua with the chirped-pulse scheme, demonstrated previously for achromatic focussing. We back up our experiments with theoretical simulations reproducing the experimental HHG results depending on diverse parameters (input pulse spectral phase, pulse duration, focus position) and proving that, under the considered parameters, the attosecond pulse train remains very similar to the achromatic case, even showing cases of isolated attosecond pulse generation for near single-cycle driving pulses., Comment: 8 pages, 7 figures

Plasmon resonances are known to amplify the electromagnetic fields near metallic nanostructures. Therefore, they are considered to provide a promising scheme to generate extreme-ultraviolet harmonics, using low power drivings. During high-order harmonic generation (HHG), the driving and harmonic fields accumulate a phase difference as they propagate through the target. In a typical set-up -a laser focused into a gas jet or cell- the propagation distances amount to several wavelengths, and the cumulative phase-mismatch affects strongly the efficiency and properties of the harmonic emission. In contrast, HHG in metallic nanostructures is considered to overcome this limitations, as the common sources of phase mismatch -optical density and focusing geometry- are negligible for subwavelength propagation distances. Nevertheless, in this letter we demonstrate that phase matching still plays a relevant role in HHG from nanostructures. Our computations attribute this to the non-perturbative character of HHG, that links the phase of the harmonics to the intensity distribution of the driving field. We also show that widely used applications of phase matching control, such as quantum path selection and the increase of contrast in attosecond pulse generation, are also feasible at the nanoscale., Comment: 9 pages, 7 figures

Tanabe et al (Phys. Rev. A {\bf 82} 040101(R) 2010) have experimentally demonstrated that the emission properties of unstable atoms in entangled and product states are different. The authors define an apparent decay time as a fitting parameter which falls below the lifetime of the single atom for entangled pairs. We argue that their results about coincidence time spectra are correct, but those concerning lifetimes cannot be considered conclusive because they assume the emission of photons by the two atoms to be independent processes, a doubtful hypothesis for entangled states. We suggest an improved evaluation of the lifetimes based on a rigorous approach, which demands some modifications of the experimental procedure.

Light beams carrying orbital angular momentum, such as Laguerre-Gaussian beams, give rise to the violation of the standard dipolar selection rules during the interaction with matter yielding, in general, an exchange of angular momentum larger than hbar per absorbed photon. By means of ab initio 3D numerical simulations, we investigate in detail the interaction of a hydrogen atom with intense Gaussian and Laguerre-Gaussian light pulses. We analyze the dependence of the angular momentum exchange with the polarization, the orbital angular momentum, and the carrier-envelope phase of light, as well as with the relative position between the atom and the light vortex. In addition, a quantum-trajectory approach based on the de Broglie-Bohm formulation of quantum mechanics is used to gain physical insight into the absorption of angular momentum by the hydrogen atom.

We analyse the influence of entanglement on the emission properties of atoms. To this end, first, we propose a scheme for the preparation of a pair of entangled Helium atoms, one in the ortho and the other in the para spin configuration. We discuss a realistic scenario for this process, based in the double ionization of He by intense laser fields. These states are used to analyse disentanglement and the role of entanglement in the spontaneous emission from the pair. In particular, we show that the decaying rate of an entangled atom is different from that in a product state, modifying the temporal emission distribution and lifetime of the atoms., Comment: Accepted in JPB

We analyze superpositions of ortho- and para-Helium states, considering the possible existence of stationary and metastable states in the system. In particular, the metastable superposition of 1s2s ortho and para states seems to be accessible to experimental scrutiny.

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 Schroedinger equation restricted to the one-dimensional soft-core approximation are presented. Our results show a clear transition from non-sequential to sequential double ionization for increasing intensities. Non sequential 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 the evidence of the influence of the exclusion principle in the underlying rescattering mechanism.

We present a study of the interaction of a relativistically planar channeled electron with an intense electromagnetic field. Using a S-Matrix approach in the Strong Field Approximation, it is shown that the crystal periodicity affects drastically the excitation process, suppressing the possibility of multiphoton absorption except for some particular cases. This selective excitation opens the possibility to control the dynamics of the channeling process by means of an external field. Explicit expressions for the S-matrix N-photon excitation rates together with the corresponding conservation laws are obtained from the relativistic quantum mechanical Dirac equation., Comment: Accepted for publication in Phys. Rev. A