Tuning the electronic band structure of metal surfaces for enhancing high-order harmonic generation

High harmonic generation (HHG) from condensed matter phase holds promise to promote future cutting-edge research in the emerging field of attosecond nanoscopy. The key for the progress of the field relies on the capability of the existing schemes to enhance the harmonic yield and to push the photon energy cutoff to the extreme ultraviolet (XUV, 10-100 eV) regime and beyond towards the spectral "water window" region (282-533 eV). Here, we demonstrate a coherent control scheme of HHG, which we show to give rise to quantum modulations in the XUV region. The control scheme is based on exploring surface states in transition-metal surfaces, and specifically by tuning the electronic structure of the metal surface itself together with the use of optimal chirped pulses. Moreover, we show that the use of such pulses having moderate intensities permits to push the harmonic cutoff further to the spectral water window region, and that the extension is found to be robust against the change of the intrinsic properties of the material. The scenario is numerically implemented using a minimal model by solving the time-dependent Schrodinger equation for the metal surface Cu(111) initially prepared in the surface state. Our findings elucidate the importance of metal surfaces for generating coherent isolated attosecond XUV and soft-x-ray pulses and for designing compact solid-state HHG devices.Comment: 9 pages, 4 figure

Coherent electron displacement for quantum information processing using attosecond single cycle pulses

Coherent electron displacement is a conventional strategy for processing quantum information, as it enables to interconnect distinct sites in a network of atoms. The efficiency of the processing relies on the precise control of the mechanism, which has yet to be established. Here, we theoretically demonstrate a new route to drive the electron displacement on a timescale faster than that of the dynamical distortion of the electron wavepacket by utilizing attosecond single-cycle pulses. The characteristic feature of these pulses relies on a vast momentum transfer to an electron, leading to its displacement following a unidirectional path. The scenario is illustrated by revealing the spatiotemporal nature of the displaced wavepacket encoding a quantum superposition state. We map out the associated phase information and retrieve it over long distances from the origin. Moreover, we show that a sequence of such pulses applied to a chain of ions enables attosecond control of the directionality of the coherent motion of the electron wavepacket back and forth between the neighbouring sites. An extension to a two-electron spin state demonstrates the versatility of the use of these pulses. Our findings establish a promising route for advanced control of quantum states using attosecond single-cycle pulses, which pave the way towards ultrafast processing of quantum information as well as imaging.publishedVersio

Femtosecond Single Cycle Pulses Enhanced the Efficiency of High Order Harmonic Generation

High-order harmonic generation is a nonlinear process that converts the gained energy during light-matter interaction into high-frequency radiation, thus resulting in the generation of coherent attosecond pulses in the XUV and soft x-ray regions. Here, we propose a control scheme for enhancing the efficiency of HHG process induced by an intense near-infrared (NIR) multi-cycle laser pulse. The scheme is based on introducing an infrared (IR) single-cycle pulse and exploiting its characteristic feature that manifests by a non-zero displacement effect to generate high-photon energy. The proposed scenario is numerically implemented on the basis of the time-dependent Schrödinger equation. In particular, we show that the combined pulses allow one to produce high-energy plateaus and that the harmonic cutoff is extended by a factor of 3 compared to the case with the NIR pulse alone. The emerged high-energy plateaus is understood as a result of a vast momentum transfer from the single-cycle field to the ionized electrons while travelling in the NIR field, thus leading to high-momentum electron recollisions. We also identify the role of the IR single-cycle field for controlling the directionality of the emitted electrons via the IR-field induced electron displacement effect. We further show that the emerged plateaus can be controlled by varying the relative carrier-envelope phase between the two pulses as well as the wavelengths. Our findings pave the way for an efficient control of light-matter interaction with the use of assisting femtosecond single-cycle fields.publishedVersio

High-order photoelectron holography in the midinfrared-wavelength regime

We study the dynamical photoelectron holography of an excited hydrogen atom with a strong midinfrared laser field using numerical solutions of the three-dimensional time-dependent Schr\uf6dinguer equation. A clear holographic interference pattern of first and high order (hologram) is recorded in the two-dimensional (2D) momentum distribution of the photoelectron. The patterns are well reproduced by additional quantitative calculations based on the Lippmann-Schwinger equation. Here, the high-order interference effect is linked to the multsicattering of low-momentum electrons driven by the midinfrared laser field prior to ejection. The phenomenon manifests by low-momentum structures in 2D momentum distributions and is found to be sensitive to the change of the optical carrier-envelope phase (CEP). By analyzing the temporal evolution of the buildup of the hologram, we show that this sensitivity results from the birth time of the continuum wave packet with an offset in time during the subcycle dynamics, thus encoding information about the ionization mechanism which is mapped into the CEP-resolved 2D momentum distributions and angle-resolved photoelectron spectra. It is indeed an indicator that the ejected electrons exhibit a memory of their birth-time. These findings suggest that the CEP-resolved photoelectron holography serves as a tool for a direct measurement of attosecond dynamics. Furthermore, the effects due to such multiple scattering electron paths can be used to design new atom interferometers to highlight mechanisms that require higher accuracy

Simultaneous Excitation of Helium by Means of an Electron and a Photon: A Joined Experimental and Theoretical Study

We report on a joined experimental and theoretical study of differential cross-sections resulting from inelastic scattering of a monoenergetic electron by helium atoms in the presence of an intense carbon dioxide laser. In particular, we measured the signals of the scattered electrons during the simultaneous electron–photon excitation of He 21P state for the first three microseconds of the laser pulse. The signals were measured for an incident electron energy of 45 eV and showed a structure that emerged at small scattering angles. The latter was found to be sensitive to the nature of the transferred photons, as well as the intensity of the laser field. The experimental findings were supported by quantum calculations based on the second-order Born approximation in which the correlated electron–electron interactions were taken into account.publishedVersio

Atomic collisional data for neutral beam modeling in fusion plasmas

The injection of energetic neutral particles into the plasma of magnetic confinement fusion reactors is a widely-accepted method for heating such plasmas; various types of neutral beam are also used for diagnostic purposes. Accurate atomic data are required to properly model beam penetration into the plasma and to interpret photoemission spectra from both the beam particles themselves (e.g. beam emission spectroscopy) and from plasma impurities with which they interact (e.g. charge exchange recombination spectroscopy). This paper reviews and compares theoretical methods for calculating ionization, excitation and charge exchange cross sections applied to several important processes relevant to neutral hydrogen beams, including H + Be4+ and H + H+. In particular, a new cross section for the proton-impact ionization of H (1s) is recommended which is significantly larger than that previously accepted at fusion-relevant energies. Coefficients for an empirical fit function to this cross section and to that of the first excited states of H are provided and uncertainties estimated. The propagation of uncertainties in this cross section in modeling codes under JET-like conditions has been studied and the newly-recommended values determined to have a significant effect on the predicted beam attenuation. In addition to accurate calculations of collisional atomic data, the use of these data in codes modeling beam penetration and photoemission for fusion-relevant plasma density and temperature profiles is discussed. In particular, the discrepancies in the modeling of impurities are reported. The present paper originates from a Coordinated Research Project (CRP) on the topic of fundamental atomic data for neutral beam modeling that the International Atomic Energy Agency (IAEA) ran from 2017 to 2022; this project brought together ten research groups in the fields of fusion plasma modeling and collisional cross section calculations. Data calculated during the CRP is summarized in an appendix and is available online in the IAEA’s atomic database, CollisionDB

Theoretical studies of electronic processes in atomic and molecular collisions : non perturbative approaches

Deux domaines différents de la physique des collisions ont fait l’objet de mes travaux de thèse réalisés dans le cadre d'une cotutelle entre l'Université Moulay Ismail, Meknes-Maroc et l'Université Pierre et Marie Curie, Paris-France: le premier concerne les collisions ion-atome/molécule dans le régime des énergies intermédiaires (keV), alors que le second vise le domaine des collisions électron-atome assistées par un champ laser intense. Bien que distincts, les deux thèmes sont interconnectés puisqu'il s'agit principalement d'étudier, dans des approches non-perturbatives, les phénomènes de diffusion et la dynamique électronique des collisions de cibles atomiques et moléculaires soumis à de fortes et très courtes perturbations. La première partie porte spécifiquement sur la modélisation des processus de transfert électronique et d'ionisation induits lors de collisions d'ions et de cibles atomiques et moléculaires. L'étude porte particulièrement sur les phénomènes d'interférences de type Young, de multi-diffusion et de diffraction Fraunhofer observés au cours de ces processus. La deuxième partie de thèse repose sur une étude des processus de diffusion élastiques et inélastiques induits lors de collisions assistées par un champ laser intense. L'étude s’appuie sur l’analyse spécifique des transitions "libre-libre" au cours lesquelles la cible reste dans son état fondamental après la collision, et des phénomènes de résonance dans le processus d'excitation simultanée électron-photon de la cible.This work has been performed as a joint PhD between Université Moulay Ismail, Meknes-Morocco, and Université Pierre et Marie Curie, Paris-France. It concerns two different areas of collision physics: the first part of my research covers the study of ion-atom/molecule collisions in the intermediate energies (keV) , while the second deals with laser-assisted electron-atom scattering. The two subjects are interconnected since both concern the description of electronic processes occurring in scattering events and the study of highly non linear response of atomic and molecular targets to high or short time-dependent perturbations. The first part of the thesis focuses specifically on the modeling of electron transfer and ionization processes induced in collisions of ions and atomic/molecular targets. My work concentrates mainly on the phenomena of Young-type interferences, multi-scattering and Fraunhofer diffraction observed during these processes. The second part concerns the study of elastic and inelastic processes induced in electron-atom collisions in the presence of a strong laser field. The investigations focus on free, free transitions, in which the target remains in its initial state after the collision, and resonance phenomena in more complex processes where the target is simultaneously excited by the the electron-projectile and the radiation and when collisional and radiative interactions are strong enough to concurrently modify the internal state of the targe

Quantum control and characterization of ultrafast ionization with orthogonal two-color laser pulses

We study ultrafast ionization dynamics using orthogonally polarized two-color (OTC) laser pulses involving the resonant “first plus second” (ω + 2ω) scheme. The scheme is illustrated by numerical simulations of the time-dependent Schrödinger equation and recording the photoelectron momentum distribution. On the basis of the simulations of this resonant ionization, we identify signatures of the dynamic Autler-Townes effect and dynamic interference, in which their characterization is not possible in the spectral domain. Taking advantage of the OTC scheme we show that these dynamical effects, which occur at the same time scale, can be characterized in momentum space by controlling the spatial quantum interference. In particular, we show that with the use of this control scheme, one can tailor the properties of the control pulse to lead to enhancement of the ionization rate through the Autler-Townes effect without affecting the dynamic interference. This enhancement is shown to result from constructive interferences between partial photoelectron waves having opposite-parity, and found to manifest by symmetry-breaking of the momentum distribution. The scenario is investigated for a prototype of a hydrogen atom and is broadly applicable to other systems. Our findings may have applications for photoelectron interferometers to control the electron dynamics in time and space, and for accurate temporal characterization of attosecond pulses

étude théorique des processus électroniques ayant lieu au cours de collisions atomiques et moléculaires: approches non perturbatives

This work has been performed as a joint PhD between Université Moulay Ismail, Meknes-Morocco, and Université Pierre et Marie Curie, Paris-France. It concerns two different areas of collision physics: the first part of my research covers the study of ion-atom/molecule collisions in the intermediate energies (keV) , while the second deals with laser-assisted electron-atom scattering. The two subjects are interconnected since both concern the description of electronic processes occurring in scattering events and the study of highly non linear response of atomic and molecular targets to high or short time-dependent perturbations. The first part of the thesis focuses specifically on the modeling of electron transfer and ionization processes induced in collisions of ions and atomic/molecular targets. My work concentrates mainly on the phenomena of Young-type interferences, multi-scattering and Fraunhofer diffraction observed during these processes. The second part concerns the study of elastic and inelastic processes induced in electron-atom collisions in the presence of a strong laser field. The investigations focus on free-free transitions, in which the target remains in its initial state after the collision, and resonance phenomena in more complex processes where the target is simultaneously excited by the the electron-projectile and the radiation and when collisional and radiative interactions are strong enough to concurrently modify the internal state of the target.Deux domaines différents de la physique des collisions ont fait l'objet de mes travaux de thèse réalisés dans le cadre d'une cotutelle entre l'Université Moulay Ismail, Meknes-Maroc et l'Université Pierre et Marie Curie, Paris-France: le premier concerne les collisions ion-atome/molécule dans le régime des énergies intermédiaires (keV), alors que le second vise le domaine des collisions électron-atome assistées par un champ laser intense. Bien que distincts, les deux thèmes sont interconnectés puisqu'il s'agit principalement d'étudier, dans des approches non-perturbatives, les phénomènes de diffusion et la dynamique électronique des collisions de cibles atomiques et moléculaires soumis à de fortes et très courtes perturbations. La première partie porte spécifiquement sur la modélisation des processus de transfert électronique et d'ionisation induits lors de collisions d'ions et de cibles atomiques et moléculaires. L'étude porte particulièrement sur les phénomènes d'interférences de type Young, de multi-diffusion et de diffraction Fraunhofer observés au cours de ces processus. La deuxième partie de thèse repose sur une étude des processus de diffusion élastiques et inélastiques induits lors de collisions assistées par un champ laser intense. L'étude s'appuie sur l'analyse spécifique des transitions "libre-libre" au cours lesquelles la cible reste dans son état fondamental après la collision, et des phénomènes de résonance dans le processus d'excitation simultanée électron-photon de la cible