High-intensity Ultrashort Laser Pulses Research Articles

Femtosecond Laser Ablation-Induced Magnetic Phase Transformations in FeRh Thin Films

In this study, we present a novel investigation into the magnetic and morphological properties of equiatomic B2-ordered FeRh thin films irradiated with single high-intensity ultrashort laser pulses. The goal is to elucidate the effect of femtosecond laser ablation on the magnetic properties of FeRh. We employed Scanning Magneto-Optical Kerr Effect (S-MOKE) microscopy to examine the magnetic phase after laser processing, providing high spatial resolution and sensitivity. Our results for the first time demonstrated the appearance of a magneto-optical signal from the bottom of ablation craters, suggesting a transition from antiferromagnetic to ferromagnetic behavior. Fluence-resolved measurements clearly demonstrate that the ablation threshold coincides with the threshold of the antiferromagnet-to-ferromagnet phase transition. The existence of such a magnetic phase transition was independently confirmed by temperature-dependent S-MOKE measurements using a CW laser as a localized heat source. Whereas the initial FeRh film displayed a reversible antiferromagnet-ferromagnet phase transition, the laser-ablated structures exhibited irreversible changes in their magnetic properties. This comprehensive analysis revealed the strong correlation between the femtosecond laser ablation process and the magnetic phase transformation in FeRh thin films.

Enhanced target normal sheath acceleration with a grooved hydrocarbon target

The interaction of a high-intensity ultrashort laser pulse with a few micrometers-thick hydrocarbon target is known to accelerate protons/ions to multi-MeV, on the rear side of the target, via the mechanism of target normal sheath acceleration. Micro-structuring the target front is one of the promising approaches to enhance the cutoff energy as well as to reduce the divergence of accelerated protons/ions. In this paper, the interaction of a normally incident intense laser pulse with targets having single micrometer-sized grooves, at their front side, of semi-circular, triangular, and rectangular shapes has been studied by using two-dimensional particle-in-cell simulations. It is observed that as compared to a flat target for targets with a rectangular groove at the front side the focused hot electron beam at the rear side results in an approximately fourfold increase in the cutoff energy of accelerated protons. For triangular and semi-circular groove targets, the cutoff energy remains comparatively lower (higher than the flat target though). The angular divergence of the accelerated protons/ions is also found to be relatively much lower in the case of a rectangular groove.

Nanoscale Control of Structure and Composition for Nanocrystalline Fe Thin Films Grown by Oblique Angle RF Sputtering.

The use of Fe films as multi-element targets in space radiation experiments with high-intensity ultrashort laser pulses requires a surface structure that can enhance the laser energy absorption on target, as well as a low concentration and uniform distribution of light element contaminants within the films. In this paper, (110) preferred orientation nanocrystalline Fe thin films with controlled morphology and composition were grown on (100)-oriented Si substrates by oblique angle RF magnetron sputtering, at room temperature. The evolution of films key-parameters, crucial for space-like radiation experiments with organic material, such as nanostructure, morphology, topography, and elemental composition with varying RF source power, deposition pressure, and target to substrate distance is thoroughly discussed. A selection of complementary techniques was used in order to better understand this interdependence, namely X-ray Diffraction, Atomic Force Microscopy, Scanning and Transmission Electron Microscopy, Energy Dispersive X-ray Spectroscopy and Non-Rutherford Backscattering Spectroscopy. The films featured a nanocrystalline, tilted nanocolumn structure, with crystallite size in the (110)-growth direction in the 15–25 nm range, average island size in the 20–50 nm range, and the degree of polycrystallinity determined mainly by the shortest target-to-substrate distance (10 cm) and highest deposition pressure (10−2 mbar Ar). Oxygen concentration (as impurity) into the bulk of the films as low as 1 at. %, with uniform depth distribution, was achieved for the lowest deposition pressures of (1–3) × 10−3 mbar Ar, combined with highest used values for the RF source power of 125–150 W. The results show that the growth process of the Fe thin film is strongly dependent mainly on the deposition pressure, with the film morphology influenced by nucleation and growth kinetics. Due to better control of film topography and uniform distribution of oxygen, such films can be successfully used as free-standing targets for high repetition rate experiments with high power lasers to produce Fe ion beams with a broad energy spectrum.

Ghost-imaging-enhanced noninvasive spectral characterization of stochastic x-ray free-electron-laser pulses

High-intensity ultrashort X-ray free-electron laser (XFEL) pulses are revolutionizing the study of fundamental nonlinear x-ray matter interactions and coupled electronic and nuclear dynamics. To fully exploit the potential of this powerful tool for advanced x-ray spectroscopies, a noninvasive spectral characterization of incident stochastic XFEL pulses with high resolution is a key requirement. Here we present a methodology that combines high-acceptance angle-resolved photoelectron time-of-flight spectroscopy and ghost imaging to enhance the quality of spectral characterization of x-ray free-electron laser pulses. Implementation of this noninvasive high-resolution x-ray diagnostic can greatly benefit the ultrafast x-ray spectroscopy community by functioning as a transparent beamsplitter for applications such as transient absorption spectroscopy in averaging mode as well as covariance-based x-ray nonlinear spectroscopies in single-shot mode where the shot-to-shot fluctuations inherent to a self-amplified spontaneous emission (SASE) XFEL pulse are a powerful asset.

Multiscale study of high energy attosecond pulse interaction with matter and application to proton\u2013Boron fusion

For several decades, the interest of the scientific community in aneutronic fusion reactions such as proton–Boron fusion has grown because of potential applications in different fields. Recently, many scientific teams in the world have worked experimentally on the possibility to trigger proton–Boron fusion using intense lasers demonstrating an important renewal of interest of this field. It is now possible to generate ultra-short high intensity laser pulses at high repetition rate. These pulses also have unique properties that can be leveraged to produce proton–Boron fusion reactions. In this article, we investigate the interaction of a high energy attosecond pulse with a solid proton–Boron target and the associated ion acceleration supported by numerical simulations. We demonstrate the efficiency of single-cycle attosecond pulses in comparison to multi-cycle attosecond pulses in ion acceleration and magnetic field generation. Using these results we also propose a path to proton–Boron fusion using high energy attosecond pulses.

Subcycle terahertz field waveforms clocked by attosecond high-harmonic pulses from relativistic laser plasmas

A high-intensity ultrashort laser pulse interacting with a thin plasma target is shown to couple to plasma electrons, driving electron oscillations within the plasma and making these electrons bounce back and forth between plasma boundaries. Each time these recirculating electrons traverse the plasma boundary, they emit bright subcycle terahertz (THz) field waveforms via laser-driven coherent transition radiation. As a concurrent process, laser-driven electrons near the front surface of the plasma target are accelerated to relativistic velocities to emit high-order harmonics (HHs), giving rise to attosecond pulses of vacuum-ultraviolet radiation. These attosecond pulses are shown to provide a high-precision clock for subcycle THz field waveforms. We demonstrate that the delay time between HH pulses and THz waveforms can be tuned with an attosecond precision by varying the thickness of the plasma target, thus opening an avenue toward HH-pump–THz-probe studies of ultrafast processes on the attosecond time scale with table-top laser sources.

Diagnostic of laser wakefield acceleration with ultra – Short laser pulse by using SMILEI PIC code

• Generation of high energy beam with LWFA is the most efficient and low in cost as compared with conventional accelerator. • In LWFA, we firstly performed this acceleration with the combination of up ramp and down ramp density region. • We firstly performed the work related with production of high energy beam with self-injected electrons. • We firstly performed the work with ultra – short laser pulse and polygonal plasma density profile for LWFA. High-energy particle beam is used to probe the local or long range structure and properties of materials. Particle accelerators are also used in material science to understand radiation damage, particularly in studies of structural material to be applied in fusion power generator and satellites. Laser Wakefield Acceleration (LWFA) is a promising technique to build compact and powerful particle accelerators for generating multi-GeV electron beams. The efficient coupling of laser energy with plasma is very important to generate high energy electrons, which is the subject to optimum laser and plasma profiles. In this article, we have used high intensity ultra-short laser pulse and a polygon plasma density profile to analyse the behaviour of LWFA in the bubble regime, which corresponds to the evacuation of plasma electrons in the wake of the laser pulse. Many electrons get self-injected in this wakefield and get accelerated behind the laser pulse up to very high energies, producing high energy beam useful for material processing along with their other applications. We have diagnosed some parameters such as electron density variation, wakefield magnitude and energy spectrum of the electrons accelerated in this mechanism.

Ultrafast Adsorbate Excitation Probed with Subpicosecond-Resolution X-Ray Absorption Spectroscopy.

We use a pump-probe scheme to measure the time evolution of the C K-edge x-ray absorption spectrum from CO/Ru(0001) after excitation by an ultrashort high-intensity optical laser pulse. Because of the short duration of the x-ray probe pulse and precise control of the pulse delay, the excitation-induced dynamics during the first picosecond after the pump can be resolved with unprecedented time resolution. By comparing with density functional theory spectrum calculations, we find high excitation of the internal stretch and frustrated rotation modes occurring within 200fs of laser excitation, as well as thermalization of the system in the picosecond regime. The ∼100 fs initial excitation of these CO vibrational modes is not readily rationalized by traditional theories of nonadiabatic coupling of adsorbates to metal surfaces, e.g., electronic frictions based on first order electron-phonon coupling or transient population of adsorbate resonances. We suggest that coupling of the adsorbate to nonthermalized electron-hole pairs is responsible for the ultrafast initial excitation of the modes.

Photoluminescence of Point Defects in Silicon Dioxide by Femtosecond Laser Exposure

The nature of the radiation‐induced point defects in amorphous silica is investigated through online photoluminescence (PL) under high intensity ultrashort laser pulses. Using 1030 nm femtosecond laser pulses with a repetition rate of 1 kHz, it is possible to study the induced color centers through their PL signatures monitored during the laser exposure. Their generation is driven by the nonlinear absorption of the light related to the high pulse peak powers provided by femtosecond laser, allowing to probe the optical properties of the laser exposed region. The experiment is conducted as a function of the laser pulse power in samples with different OH contents. The results highlight the different interaction regimes attained by varying the irradiation conditions for various chemical compositions. Moreover, the online measurements are combined with postmortem characterization of the damaged area, via phase contrast microscopy, Raman and steady‐state PL spectroscopies, highlighting the potential of these online femtosecond tests to provide additional knowledge to the postmortem technique ones.

Accurate spectra for high energy ions by advanced time-of-flight diamond-detector schemes in experiments with high energy and intensity lasers

Time-Of-Flight (TOF) methods are very effective to detect particles accelerated in laser-plasma interactions, but they show significant limitations when used in experiments with high energy and intensity lasers, where both high-energy ions and remarkable levels of ElectroMagnetic Pulses (EMPs) in the radiofrequency-microwave range are generated. Here we describe a novel advanced diagnostic method for the characterization of protons accelerated by intense matter interactions with high-energy and high-intensity ultra-short laser pulses up to the femtosecond and even future attosecond range. The method employs a stacked diamond detector structure and the TOF technique, featuring high sensitivity, high resolution, high radiation hardness and high signal-to-noise ratio in environments heavily affected by remarkable EMP fields. A detailed study on the use, the optimization and the properties of a single module of the stack is here described for an experiment where a fast diamond detector is employed in an highly EMP-polluted environment. Accurate calibrated spectra of accelerated protons are presented from an experiment with the femtosecond Flame laser (beyond 100 TW power and ~ 1019 W/cm2 intensity) interacting with thin foil targets. The results can be readily applied to the case of complex stack configurations and to more general experimental conditions.

Energy deposition parameters revealed in the transition from 3D to 1D femtosecond laser ablation of fluorite at high-NA focusing

Ultrashort-pulse laser surface and bulk nano- and micromachining of dielectrics have multiple promising applications in micro-optics, microfluidics, and memory storage. The fundamental principles relate intrinsic inter-band multi-photon (MPA) and laser-induced intra-band free-carrier absorption (FCA) to particular ablation mechanisms and features. These principles are yet to be quantified into a complete set of basic experimental laser-matter interaction parameters, describing photoexcitation, relaxation, and final ablation. In this study, we considered the characteristic double-crater structure of single-shot ablation spots on dielectric surfaces and single-shot transmission spectra to extract crucial information about the underlying basic processes of ultrafast photoexcitation and laser energy deposition. Specifically, energy-dependent crater profiles and accompanying prompt self-phase modulation (SPM) spectral broadening were studied in single-shot surface ablation experiments on fluorite (CaF2) surface photo-excited by tightly focused 515- or 1030-nm, 300-fs laser pulses. Crater size dependence demonstrated two slopes, scaling proportionally to the squared focal 1/e-radius at higher energies (intensities) for larger ablated spots, and a much smaller squared 1/e-radius at lower energies (intensities) for (sub) micron-wide ablated spots, indicating a transition from 1D to 3D-ablation. As a result, these slopes were related to lower-intensity wavelength-dependent multi-photon inter-band transitions and wavelength-independent higher-intensity linear absorption in the emerging near-critical electron-hole plasma (EHP), respectively. Crater depth dependences on the local laser intensity fitted in the corresponding ranges by multi- and one-photon absorption provided the corresponding absorption coefficients. Spectral broadening measurements indicated even values for the red and blue shoulders of the laser pulse spectrum, representing the SPM effect in the weakly excited fluorite at the leading pulse front and providing the corresponding Kerr coefficient. In the second regime, the blue-shoulder broadening value saturated, indicating the appearance of near-critical plasma screening at the trailing pulse front, which is consistent with our calculations. These complementary experiments and related analysis provided an important set of key basic parameters, characterizing not only surface ablation, but also propagation of high-intensity ultrashort laser pulses in bulk fluorite, and enabling precise forecasting of optimal energy deposition for high-efficiency ultrashort-laser micro-structuring of this dielectric material.

Time-resolved characterization of ultrafast electrons in intense laser and metallic-dielectric target interaction.

High-intensity ultrashort laser pulses interacting with thin solid targets are able to produce energetic ion beams by means of extremely large accelerating fields set by the energetic ejected electrons. The characterization of such electrons is thus important in view of a complete understanding of the acceleration process. Here, we present a complete temporal-resolved characterization of the fastest escaping hot electron component for different target materials and thicknesses, using temporal diagnostics based on electro-optical sampling with 100 fs temporal resolution. Experimental evidence of scaling laws for ultrafast electron beam parameters have been retrieved with respect to the impinging laser energy (0.4-4 J range) and to the target material, and an empirical law determining the beam parameters as a function of the target thickness is presented.

Direct observation of ultrafast electrons generated by high-intensity laser-matter interaction

High intensity ultrashort laser pulses interacting with thin solid targets are able to produce energetic protons and ions by means of extremely large accelerating fields, generated by escaping electrons. The characterization of such electrons is thus a key factor for the understanding of the accelerating potential temporal evolution. Here, we present temporally resolved measurements of the ultrafast escaping electron component. The charge, electric field, and temporal duration of the emitted ultrafast electron beams are determined using temporal diagnostics with a 100 fs temporal resolution. Experimental evidence of scaling laws for the ultrafast electron beam parameters with respect to the incident laser pulse energy is retrieved and compared with theoretical models, showing an excellent agreement.

Diffraction-ray tube analysis of ultrashort high-intensity laser pulse filamentation in air

The results of theoretical simulation of femtosecond Ti:Sapphire laser pulse propagation in air in the self-focusing and filamentation regimes are presented. The self-focusing of pulsed radiation was analyzed based on the diffraction-ray tracing method, within which the beam power propagates within specific light structures, known as the diffraction-ray tubes. These tubes do not intersect in space and do not exchange their energy, but the changes in their shape and cross-section reflect the physical effects occurring with the radiation during its propagation through the medium. This allows discovering the formation of specific light structures in a laser beam during its self-focusing. One of these structures is the energy-replenishing diffraction-ray tube (ERT), which provides the filamentation domain with the necessary light energy and exists also in the form of a high-intensity light channel during the post-filamentation propagation of a pulse. The dependences of the radius and power of this energy-replenishing tube on the initial beam radius and peak radiation power at a fixed pulse length are derived. It is revealed that the radiation energy expenditure for filamentation decreases as the beam radius increases. The peak power in ERT does not exceed the critical self-focusing power for a Gaussian beam during the post-filamentation propagation of a pulse and weakly depends on the initial pulse parameters.

Energy transfer from intense laser pulse to dielectrics in time-dependent density functional theory

Energy transfer processes from a high-intensity ultrashort laser pulse to electrons in simple dielectrics, silicon, diamond, and $\alpha$-quartz are theoretically investigated by first-principles calculations based on time-dependent density functional theory (TDDFT). Dependences on frequency as well as intensity of the laser pulse are examined in detail, making a comparison with the Keldysh theory. Although the Keldysh theory reliably reproduces the main features of the TDDFT calculation, we find some deviations between results by the two theories. The origin of the differences is examined in detail.

Symplectic integration and physical interpretation of time-dependent coupled-cluster theory.

The formulation of the time-dependent Schrödinger equation in terms of coupled-cluster theory is outlined, with emphasis on the bivariational framework and its classical Hamiltonian structure. An indefinite inner product is introduced, inducing physical interpretation of coupled-cluster states in the form of transition probabilities, autocorrelation functions, and explicitly real values for observables, solving interpretation issues which are present in time-dependent coupled-cluster theory and in ground-state calculations of molecular systems under the influence of external magnetic fields. The problem of the numerical integration of the equations of motion is considered, and a critical evaluation of the standard fourth-order Runge-Kutta scheme and the symplectic Gauss integrator of variable order are given, including several illustrative numerical experiments. While the Gauss integrator is stable even for laser pulses well above the perturbation limit, our experiments indicate that a system-dependent upper limit exists for the external field strengths. Above this limit, time-dependent coupled-cluster calculations become very challenging numerically, even in the full configuration interaction limit. The source of these numerical instabilities is shown to be rapid increases of the amplitudes as ultrashort high-intensity laser pulses pump the system out of the ground state into states that are virtually orthogonal to the static Hartree-Fock reference determinant.

Ultrafast excitation of conduction-band electrons by high-intensity ultrashort laser pulses in band-gap solids: Vinogradov equation versus Drude model

Heating of conduction-band electrons is one of the major processes of energy absorption and transfer in high-intensity ultrafast laser–solid interactions. It is frequently simulated by assuming a high rate of electron-particle collisions. We explore the approximation of low-rate electron–phonon collisions based on the Vinogradov equation for the intraband absorption rate by conduction-band electrons performing laser-driven oscillations. Band-structure modification by the ponderomotive energy of the ultrafast oscillations is taken into account. The Vinogradov equation combined with the Keldysh formula for the interband transition rate delivers a highly nonequilibrium energy distribution of the conduction electrons. Reported results suggest a substantial revision of the traditional models of ultrafast free-carrier heating by intense laser pulses.

Direct electron acceleration for diagnostics of a laser pulse focused by an off-axis parabolic mirror

We develop a theoretical basis for a new method of high-intensity ultrashort laser pulse diagnostics via vacuum electron acceleration from an ultrathin foil. A laser pulse is focused by an off-axis parabolic mirror, which has practical interest for most experiments with high-intensity pulses. The field description is based on Stratton–Chu integrals, which allow covering all focusing ranges up to the diffraction limit where the six-component laser field is correctly described. The theoretical approach uses a test particle method applicable for quite thin foils and rarefied gases, where the plasma fields do not substantially affect electron acceleration. The diagnostic method is to use measurements of angular-spectrum characteristics of laser accelerated or scattered electrons to compare them with the theory developed here. The proposed method can diagnose not only the intensity but also the quality of a laser pulse.

Ultrafast modification of band structure of wide-band-gap solids by ultrashort pulses of laser-driven electron oscillations

The electric field of high-intensity ultrashort laser pulses substantially perturbs an electron subsystem of a crystal and affects its band structure. Laser-driven oscillations of electrons and holes are frequently referred to as a major mechanism of the perturbation in dielectrics and semiconductors. New physical effects arise when the band structure is modified by an ultrashort pulse of the oscillations driven by a few-cycle laser pulse. Assuming the laser-pulse envelope varies slowly compared to the carrier frequency, we derive analytical relations for the laser-modified band structure by utilizing the Keldysh cycle-averaged nonperturbative approach under the approximation of constant effective mass. Formation of indirect-gap transient bands, suppression of the nonlinear absorption on the leading edge of a laser pulse, and cycle-averaged photocurrent generation driven by the pulse envelope are predicted. Analytical scaling with six laser and material parameters is obtained. The reported results establish the limits of validity of the Keldysh photoionization model and advance understanding of the fundamental effects involved in high-intensity ultrafast laser-solid interactions.

Laser induced ablation of aluminum nanoparticle: a molecular dynamics study

We investigate ablation of Aluminum nanoparticle due to ultrashort high-intensity laser pulse. Molecular dynamics simulation is used to follow the evolution of the system and observe thermodynamics together with cluster properties. The energy given from the laser to the system is 1.5 eV/atom which is above ablation threshold and modelled using instantaneous and homogenous energization at the beginning of simulation. The evolution of the system shows a highly non-equilibrium state after the irradiation. Expansion of the sphere indicated that the system cannot survive from the temporary high tensile pressure that leads to ablation. While the high temperature consecutively responsible for the formation of cluster, it also indicated that the system is relaxed at the end of the simulation.