High-intensity Femtosecond Laser Research Articles

(Sub-)Picosecond Surface Correlations of Femtosecond Laser Excited Al-Coated Multilayers Observed by Grazing-Incidence X-ray Scattering.

Femtosecond high-intensity laser pulses at intensities surpassing 1014 W/cm2 can generate a diverse range of functional surface nanostructures. Achieving precise control over the production of these functional structures necessitates a thorough understanding of the surface morphology dynamics with nanometer-scale spatial resolution and picosecond-scale temporal resolution. In this study, we show that single XFEL pulses can elucidate structural changes on surfaces induced by laser-generated plasmas using grazing-incidence small-angle X-ray scattering (GISAXS). Using aluminium-coated multilayer samples we distinguish between sub-picosecond (ps) surface morphology dynamics and subsequent multi-ps subsurface density dynamics with nanometer-depth sensitivity. The observed subsurface density dynamics serve to validate advanced simulation models representing matter under extreme conditions. Our findings promise to open new avenues for laser material-nanoprocessing and high-energy-density science.

Attosecond and nano-Coulomb electron bunches via the Zero Vector Potential mechanism

The commissioning of multi-petawatt class laser facilities around the world is gathering pace. One of the primary motivations for these investments is the acceleration of high-quality, low-emittance electron bunches. Here we explore the interaction of a high-intensity femtosecond laser pulse with a mass-limited dense target to produce MeV attosecond electron bunches in transmission and confirm with three-dimensional simulation that such bunches have low emittance and nano-Coulomb charge. We then perform a large parameter scan from non-relativistic laser intensities to the laser-QED regime and from the critical plasma density to beyond solid density to demonstrate that the electron bunch energies and the laser pulse energy absorption into the plasma can be quantitatively described via the Zero Vector Potential mechanism. These results have wide-ranging implications for future particle accelerator science and associated technologies.

Quantum mechanical modeling of high-intensity laser pulse interaction with hydrogen atom with considering the magnetic field and polarization

In the study of the non-relativistic interaction between high-intensity femtosecond laser pulses and atoms, the influence of the magnetic field is commonly overlooked. This work investigates the effects of the magnetic field in the high-intensity few-cycle laser pulses with non-relativistic intensity of 3.5×1014W/cm2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$3.5 \ imes 10^{14} { }\\;\\;{\ ext{W}}/{\ ext{cm}}^{2}$$\\end{document} at the center wavelength of 800 nm on the high-order harmonic generation (HHG), attosecond pulse train (APT), isolated attosecond pulse (IAP), and the electron trajectory in the hydrogen atom, employing the numerical solution of the time-dependent Schrödinger equation in three dimensions (3D-TDSE). Two polarizations, linear and circular, are considered. A comparison with the scenario where the magnetic field is not considered shows that the magnetic field can apply significant corrections to the results. Particularly, considering the magnetic field for circular polarization can make the cutoff frequency of HHG coincide with the semi-classical relationship of ħωc=Ip+3.17Up\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\hbar {\\upomega }_{{\ ext{c}}} = {\ ext{I}}_{{\ ext{p}}} + 3.17{\ ext{U}}_{{\ ext{p}}}$$\\end{document}, a case that for circular polarization does not exist without considering the magnetic field. Moreover, accounting for the magnetic field leads to a reduction in the attosecond pulse duration for circular polarization for APT (360as\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$360{\ ext{ as}}$$\\end{document} versus 241as\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$241{\ ext{ as}}$$\\end{document}) and for IAP (834as\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$834{\ ext{ as}}$$\\end{document} versus 602as\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$602{\ ext{ as}}$$\\end{document}). Additionally, the difference in production efficiency of HHG and APT between linear and circular polarization is reduced by two orders of magnitude, when magnetic field is considered. Although considering the magnetic field complicates the electron trajectory, especially for circular polarization, however, our quantum model provides enhanced insight into how the interaction works, especially when and where the electron collides with the parent nucleus. In this case, the quantum mechanical modeling largely covers the huge difference of not considering the magnetic field in the results predicted by other works.

A solid-state high harmonic generation spectrometer with cryogenic cooling.

Solid-state high harmonic generation (sHHG) spectroscopy is a promising technique for studying electronic structure, symmetry, and dynamics in condensed matter systems. Here, we report on the implementation of an advanced sHHG spectrometer based on a vacuum chamber and closed-cycle helium cryostat. Using an in situ temperature probe, it is demonstrated that the sample interaction region retains cryogenic temperature during the application of high-intensity femtosecond laser pulses that generate high harmonics. The presented implementation opens the door for temperature-dependent sHHG measurements down to a few Kelvin, which makes sHHG spectroscopy a new tool for studying phases of matter that emerge at low temperatures, which is particularly interesting for highly correlated materials.

The modeling non-sequential double ionization of helium atom under high-intensity femtosecond laser pulses with shielding charge approximation

In this study, we successfully extracted the ‘knee structure’ for non-sequential double ionization (NSDI) in the helium atom. To achieve this, for the first time, we solved the time-dependent Schrödinger equation in three dimensions for the helium atom, utilizing the shielding charge approximation. Our findings corroborate prior observations by Wang et al [Wang and Eberly, Phys. Rev. Lett. 105, 083001 (2010)], demonstrating that NSDI occurs within a narrower time window in circular polarization compared to linear polarization. As a result, the yield of linear polarization was higher than that of circular polarization, aligning with the previously reported results. Notably, in the case of circular polarization, the time window further narrows with increasing intensity, attributed to a decrease in the time-of-flight.

High-order harmonic generation, attosecond pulse, and non-sequential double ionization in the helium atom under high-intensity femtosecond laser pulses

High-order harmonic generation (HHG), attosecond pulse train (APT), isolated attosecond pulse (IAP), and non-sequential double ionization (NSDI) in the Helium atom under intense femtosecond laser pulses are computed using the time-dependent Schrodinger equation (TDSE) in one dimension (1D). By taking into account the electron–electron and electron-nucleus interactions, as well as determining the Helium atom’s ground state wave function through the imaginary time propagation (ITP) method, we are able to observe the widely recognized ‘knee structure’ in the ionization probability of the Helium atom as a function of intensity within an ionization boundary condition model. The results are in good agreement with the experimental data reported by (Walker et al (1994) Phys. Rev. Lett. 73, 1227).

High-quality micro/nano structures of 4H-SiC patterning by vector femtosecond laser

High-intensity femtosecond laser processing of hard and brittle materials such as silicon carbide (SiC) has poor surface quality and is prone to micro-cracks, making it difficult to meet the application requirements of silicon carbide microdevices. In this study, a method for fabricating high-quality micro-nanostructures of 4H-SiC using vector polarized light was proposed. The influences of linear polarization and vector polarization on the quality and surface morphology of processed SiC microgrooves were studied, and the micromachined size rule of microgrooves machined under different pulse numbers was summarized. The damage distribution of microstructures machined by linearly polarized light and vector polarized light were characterized by confocal Raman mapping. The study had shown that using vector beam, especially azimuthal polarization beam, can ensure the uniformity of the processing area, effectively reduce micro-cracks and chipping in the processing of hard and brittle materials, and obtain better processing quality. In addition, the vector polarized light can avoid the large microgroove taper during the processing, and ensure good structure size. Finally, a high-quality multi-ring structure was fabricated by an azimuthal polarization beam, which provides an accurate method for preparing microstructures with excellent performance.

Studies on Femtosecond Laser Textured Broadband Anti-reflective Hierarchical a-SiNx:H Thin Films for Photovoltaic Applications

Simple ultrafast laser writing for the fabrication of hierarchical silicon nitride (a-SiNx:H) microstructures is demonstrated as an effective antireflection coating. A wide range of Si-rich to N-rich a-SiNx:H thin films, having varied optical band gap (2.32–5.94 eV) and refractive index (2.8–1.7) of wavelength-ordered (∼λ/4) thickness, are deposited using the plasma-enhanced chemical vapor deposition technique. The high-intensity femtosecond laser (800 nm, 120 fs, 1 kHz) interaction with a-SiNx:H films resulted in diverse nano-/microstructures with systematic width and depth born out of nonlinear light–matter interactions. These experimentally demonstrated the extremely disordered micro–nano structures over a large area of ∼ 1 cm2 that exhibit significant light trapping and absorption capabilities over a broad spectral region of 200–1000 nm. The extensive reduction of reflection losses from 30 to 2.8% from pre- to post-laser texturing is a favorable condition for broadband anti-reflective coatings for enhanced light harvesting from prefabricated photovoltaic devices.

The Motion of a Charged Particle in the Electromagnetic Field of a Polarization-Modulated Wave

This article presents an exact solution of the equation of motion of a charged particle in the electromagnetic field of a high-intensity polarization-modulated wave. Expressions for the average kinetic energy of a particle without regard to its rest energy in the case of circular and linear polarization of a modulated wave are obtained. The motion of a charged particle in the field was analyzed and expressed in terms of dependences of its average kinetic energy on the electromagnetic wave intensity and on various types of modulation depths. The contribution of each type of modulation to the energy characteristics of a charged particle was demonstrated. Solving the equation of motion of a charged particle in the electromagnetic field of a plane wave opens up possibilities for various applications related, in particular, to various developments of multi-frequency lasers and laser modulation technology. This study was proposed due to the growing interest in experiments using high-intensity femtosecond laser radiation and high-temperature plasma

Nanoscale subsurface dynamics of solids upon high-intensity femtosecond laser irradiation observed by grazing-incidence x-ray scattering

Observing ultrafast laser-induced structural changes in nanoscale systems is essential for understanding the dynamics of intense light-matter interactions. For laser intensities on the order of 1014W/cm2, highly collisional plasmas are generated at and below the surface. Subsequent transport processes such as heat conduction, electron-ion thermalization, surface ablation, and resolidification occur at picosecond and nanosecond timescales. Imaging methods, e.g., using x-ray free-electron lasers (XFEL), were hitherto unable to measure the depth-resolved subsurface dynamics of laser-solid interactions with appropriate temporal and spatial resolution. Here we demonstrate picosecond grazing-incidence small-angle x-ray scattering (GISAXS) from laser-produced plasmas using XFEL pulses. Using multilayer (ML) samples, both the surface ablation and subsurface density dynamics are measured with nanometer depth resolution. Our experimental data challenges the state-of-the-art modeling of matter under extreme conditions and opens new perspectives for laser material processing and high-energy density science.Received 11 December 2021Accepted 23 May 2022DOI:https://doi.org/10.1103/PhysRevResearch.4.033038Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasHigh intensity laser-plasma interactionsHigh-energy-density plasmasPhysical SystemsPlasma sheaths & surfacesStrongly-coupled plasmasWarm-dense matterTechniquesHydrodynamicsLaser ablationParticle-in-cell methodsX-ray reflectivityX-ray scatteringPlasma PhysicsCondensed Matter, Materials & Applied Physics

Self-channeling of spatially modulated femtosecond laser beams in the post-filamentation region

The propagation of high-intensity femtosecond laser pulses in air under conditions of superposed spatial phase modulation is considered theoretically. The numerical simulations are carried out on the basis of the reduced form of a nonlinear Schrödinger equation for a time-averaged electric field envelope. Initial spatial modulations are applied to pulse wavefront profiling by a staggered ( T E M 22 ) phase plate, which is simulated numerically. The dynamics of laser pulse self-focusing, filamentation, and post-filamentation self-channeling after the phase plates with variable phase jumps is studied. We show that, with specific phase modulations, the pulse filamentation region in air can be markedly shifted further and elongated compared with a nonmodulated pulse. Moreover, during the post-filamentation propagation of spatially structured radiation, the highly localized light channels are formed, possessing enhanced intensity and reduced angular divergence, which enables post-filamentation pulse self-channeling on the distance multiple exceeding the Rayleigh range.

Investigation of hard x-ray emissions from terawatt laser-irradiated foils at the Matter in Extreme Conditions instrument of the Linac Coherent Light Source

In this technical report, we investigate the hard x-ray background produced at the Matter in Extreme Conditions (MEC) instrument of the Linac Coherent Light Source (LCLS) from the interaction of a high-intensity (∼1019 W/cm2) femtosecond laser with solid μm-thick aluminum and polypropylene targets. This background is dominated by bremsstrahlung from laser-generated relativistic electrons, and a measurement of the broadband x-ray spectrum via differential x-ray energy filtering was used to infer the existence of two electron distributions with electron temperatures of Thot = 500 ± 300 keV and Tcold = 5.0 ± 0.5 keV. Simultaneous single-shot measurements of the proton energies accelerated from laser-irradiated solid targets could be correlated with these measurements to further constrain the on-target laser parameters. Measurements of the hard x-ray photon background generated from laser-irradiated foils can be used to directly monitor and test the signal-to-background limits of silicon-based hybrid pixel array x-ray detectors at laser intensities approaching 1019 W/cm2.

Isolated attosecond pulse generation from helium atom irradiated by a three-color laser pulse

Isolated attosecond pulses enables the studying and controlling of ultrafast electron processes in atoms and molecules. High-order harmonic generation (HHG) is the most promising way to generate such pulses, benefiting from the broad plateau structure of the typical HHG spectrum. We theoretically investigate high-order harmonic and attosecond pulse generation from helium atom in a three-color laser field, which is synthesized by 16 fs/1600 nm, 15 fs/1100 nm and 5 fs/800 nm pulse laser. Compared with harmonic spectrum generated by a two-color laser field synthesized by 16 fs/1600 nm and 15 fs/1100 nm, the harmonic spectrum generated from the synthesized three-color field exhibits high conversion efficiency and broadband supercontinuum characteristics. The continuous spectrum range covers from 230th to 690th harmonics, and the generation of 128 attosecond isolated short pulses with higher intensity is realized after Fourier transform. This result is attributable to the fact that the synthesized three-color electric field exhibits high-intensity and few-cycle mid-infrared femtosecond pulse laser characteristics, which can effectively control atomic ionization and recombination occurring within an effective optical period of the mid-infrared femtosecond pulse. This scheme solves the problems faced by the current femtosecond pulse laser technology, i.e. the few-cycle mid-infrared femtosecond pulse laser cannot have both carrier envelope phase stability and high power output.

Wavelength dependence of the multiphoton ionization of CH3I by intense femtosecond laser pulses through Freeman resonances.

Multiphoton ionization (MPI) of methyl iodide, CH3I, has been investigated with the photoelectron imaging (PEI) technique, using high intensity femtosecond laser pulses at different central wavelengths. The use of high laser field strengths alters the way in which matter-radiation interaction takes place. This generates highly nonlinear phenomena, among which we can highlight the Stark shift effect. It can distort the potential energy surfaces of atoms and molecules, varying both the energy of electronic and rovibrational states of these systems and their ionization potentials. In this way, the Stark shift can generate resonances between intermediate states and an integer number of laser photons of a given wavelength, which would be absent in the low intensity regime. The main purpose of this work is the generation, detection and characterization of resonances produced by the Stark shift, commonly known as Freeman resonances, induced by multiphoton ionization of gas-phase CH3I at different laser wavelengths. The results obtained reveal that a multitude of resonances are induced in the ionization of CH3I in the range of intensities employed, involving several Rydberg states. Ionization pathways associated with different degrees of vibrational excitation in both the intermediate states and the molecular cation generated in each of the experiments are proposed.

Experimental investigation of size broadening of a K\u03b1 x-ray source produced by high intensity laser pulses

The size of a hard Kα x-ray source ({mathrm{E}}_{{rm{K}}_{rm{alpha }}} = 17.48 keV) produced by a high intensity femtosecond laser interacting with a solid molybdenum target is experimentally investigated for a wide range of laser intensity (I ~ 1017–2.8 × 1019 W/cm2) and for four values of the temporal contrast ratio (6.7 × 107 < CR < 3.3 × 1010). Results point out the size enlargement of the x-ray source with the increase of laser intensity and with the deterioration of temporal contrast. It amounts up to sixteen times the laser spot size at the highest laser intensity and for the lowest temporal contrast ratio. Using hydrodynamic simulations, we evaluate the density scale length of the pre-plasma L/λ just before the main pulse peak. This allows us to show that a direct correlation with the laser absorption mechanisms is not relevant to explain the large size broadening. By varying the thickness of the molybdenum target down to 4 µm, the impact of hot electron scattering inside the solid is also proved irrelevant to explain the evolution of both the x-ray source size and the Kα photon number. We deduce that the most probable mechanism yielding to the broadening of the source size is linked to the creation of surface electromagnetic fields which confine the hot electrons at the solid surface. This assumption is supported by dedicated experiments where the evolution of the size enlargement of the x-ray source is carefully studied as a function of the laser focal spot size for the highest contrast ratio.

Ultra-supercontinuum generation with high intense femtosecond pulses

Extreme spectral broadening has been theoretically simulated from the index of refraction changes from the envelope response to the fifth- and third-order susceptibilities from self-phase modulation (SPM) under the influence of an extremely high-intensity femtosecond laser pulse to potentially produce spectral broadening changes extending from extreme X-rays, UV, visible, THz down to DC. The theoretical results show that an extremely high-intensity pulse as high as on the order of 1014~1016 W/m2 can influence the fourth-order refractive index arising from fifth-order susceptibility large enough that the nonlinear n4I02 term to overtakes the n2I0 term from the third-order susceptibility to produce the ultra-supercontinuum broadening in the liquids such as CS2 and rare gas liquids and solids such as calcite, ZnO, Si, Argon, and Krypton. There has been experimental verification at lower intensities that the SC is symmetrical in frequency about laser frequency for say a Gaussian pulse extends from, UV visible, NIR, to MIR by many researchers using various states of matter. This paper provides an opportunity to extend the SPM model from X-rays to DC to form Ultra Supercontinuum Generation (USCG) using extreme intensity fs pulses in the four states of matter: gases, liquids, solids, and plasmas. At the highest intensity, a continuum with weaker intensity goes towards the X-ray region on the anti-Stokes side.

Absorption of high-intensity, high-contrast femtosecond laser pulses by a dielectric solid

Basic understanding of high-intensity femtosecond laser absorption by a solid is crucial for high-energy-density science. This multidimensional problem has many variables like laser parameters, solid target material, and geometry of the excitation. This study is important for a basic understanding of intense laser-matter interaction as well for applications such as ‘plasma mirror’. Here, we experimentally observe high-contrast femtosecond laser absorption by an optically polished fused silica target at near-relativistic laser intensities (∼1018 W cm−2). Laser absorption as a function of angle of incidence and incident energy is investigated for both p- and s-polarized pulses in detail, providing a strong indication of the presence of collisionless processes. At an optimum angle of incidence, almost 80% of the p-polarized laser energy gets absorbed by the target. We also observed high reflectivity (∼60%) at lower angle of incidence (30∘) for both the polarization of laser, indicating this study is fundamentally important for ‘plasma mirrors’ at near-relativistic intensities.

Femtosecond laser synthesis of nitrogen-doped luminescent carbon dots from acetonitrile

Carbon dots (CDs) is a novel promising class of nanomaterials with unique properties. Most of synthetic methods to obtain CDs employ hydrothermal synthesis, breaking down larger carbon materials by laser irradiation, arc discharge, ultrasonication or electrolysis. Here we describe a conceptually new bottom-up approach to nitrogen-rich carbonaceous nanoparticles via high intensity femtosecond laser irradiation of neat acetonitrile where the latter serves a source of the doping N atoms. Selected photophysical properties of the new material and mechanism of the photoluminescence (PL) are discussed.

Electric-field-induced second-harmonic generation using high-intensity femtosecond laser pulses over the observable optical breakdown threshold.

We investigated the performance of electric-field-induced second-harmonic generation (E-FISHG) by spectroscopic measurement using high-intensity femtosecond laser pulses. The second-harmonic intensity increased quadratically versus the applied electric field, as expected from the theory, up to 15 kV/cm with the laser energy up to 2.5 mJ, which is ∼5 times higher than the observable optical breakdown threshold. In addition, when the laser energy was 2.8 mJ, ∼80 times signal intensity at 0.23 mJ was obtained. These results suggest that the electric-field measurement by E-FISHG with high-intensity second harmonics is expected by using high-intensity laser pulses above the observable optical breakdown threshold. Spectroscopic measurement shows no E-FISHG of white light generated by self-phase modulation in laser-induced filament.

Complementary diagnostics of high-intensity femtosecond laser pulses via vacuum acceleration of protons and electrons

Taking advantage of complementary measurements of the characteristics of both protons and electrons accelerated by a laser in a vacuum, we propose an advanced diagnostics of the parameters of the tightly focused high-intensity femtosecond laser pulse. The laser field description is based on Stratton–Chu integrals, which allow simulating laser pulses with different spatial–temporal profiles focused by an off-axis parabolic mirror down to the diffraction limit. The free particles, whose dynamics are calculated by the test particle method, are accelerated from a rarefied gas (almost a vacuum). We analyze the dependence of the particle spectra on the laser parameters: the laser peak intensity, focal spot size, and pulse duration. The results show that diagnostics obtained by simultaneously using protons and electrons allow increasing the estimation accuracy of measuring the focal spot size and the peak intensity and thus allow evaluating the laser pulse duration in the femtosecond range. Our proposal is a response to the urgent need to measure pulse durations in the focal spot for new PW-level class lasers of super-short duration up to ∼10 to 20 fs, which clearly demonstrate a current trend in laser technology.