Intense Ultrashort Laser Pulses Research Articles

Interaction of intense ultrashort laser pulses with solid targets: A systematic analysis using first-principles calculations

Interaction of intense ultrashort laser pulses with solid targets: A systematic analysis using first-principles calculations

Spatiotemporal reshaping of femtosecond laser pulses on interaction with gas sheath at ionization saturation intensity regime

Interaction of intense ultrashort laser pulse with gases generates a transient spatiotemporal electron density distribution via field ionization, which may lead to the spatiotemporal reshaping of the pulse, viz., its beam profile, pulse width, etc. Here, we present an experimental study on ultrashort laser pulse interaction with argon gas sheath in an ionization saturation intensity regime (∼1015–1017 W/cm2). The present investigation has been performed using a 6 mJ, 1 kHz, and 55−60 fs Ti:Sapphire laser pulse interaction with a ∼2.5 mm long argon sheath. After the laser gas interaction, the laser spatial profile exhibits a multi-ring structure around a central maximum spot. Laser gas interaction parameters, such as laser intensity, gas pressure, etc., affect the ring pattern significantly. Under optimum parameter conditions, the laser pulse has two rings in spatial profile, and the pulse width of the central spot is self-compressed to ∼35 fs. A theoretical calculation reveals that the laser beam’s spatiotemporal profile evolves as it propagates inside the gas sheath. The calculation also demonstrates that the gas ionization profile plays a crucial role in the spatiotemporal reshaping and self-compression of the laser beam. The calculation also shows that the generation of concentric ring patterns in the spatial profile is mainly due to the ionization of argon atoms into Ar+, Ar2+, and Ar3+ species in the interaction region. Such self-compressed laser pulses with concentric ring beam profiles may be useful for high-harmonic generation and shorter attosecond pulse trains.

Collimated hot electron generation from sub-wavelength grating target irradiated by a femtosecond laser pulse of relativistic intensity

We investigate the production of hot electrons from the interaction of relativistically intense (I>1018 W/cm2) ultrashort (25 fs) laser pulses with sub-wavelength grating target. We measure the hot electron angular distribution and energy spectra for grating target and compare them with those from a planar mirror target. We observe that hot electrons are emitted in a collimated beam along the specular direction of the grating target. From the measurements, we see fast electron temperature and flux for grating are higher than those for mirror due to a stronger coupling with the laser. We performed numerical simulations, which are in good agreement with experimental results, and offer insights into the acceleration mechanism by resulting electric and magnetic fields. Such collimated fast electron beams have a wide range of applications in applied and fundamental science.

Controlling the photoelectron holography with shaped intense ultrashort laser pulses

We perform a theoretical investigation on the control of photoelectron holography with shaped intense ultrashort laser pulses. By adjusting the π phase-flip position in the frequency domain, the shape of the time-dependent envelope of the input laser electric field changes from Gaussian to trapezoidal and finally to double-peak pulse. The photoelectron momentum spectra for different pulse shapes are calculated by both three-dimensional time-dependent Schrödinger equation (TDSE) method and Quantum-trajectory Monte Carlo (QTMC) model, and good agreement is achieved between results calculated by the two methods. Interference pattern in photoelectron holography exhibits a strong dependence on the shape of the electric field. Analysis shows that adjacent and nonadjacent intercycle interference as well as intracycle interference are all effectively regulated by the shaped pulse.

Ionization of hydrogen atom driven by ultrashort intense laser pulses: study in momentum space of phase-dependent effects

Ionization of hydrogen atom driven by ultrashort intense laser pulses: study in momentum space of phase-dependent effects

Effect of pulse duration on the above-threshold ionization of a hydrogen atom irradiated by a 400 nm intense laser.

The photoelectron emission spectra generated by the interaction between ultrashort intense laser pulses and atoms can reveal the ultrafast dynamics of electrons. By using the numerical solution of the time-dependent Schrödinger equation in momentum space, the photoelectron emission spectra of atoms irradiated by 400 nm intense lasers with different durations of the pulse has been investigated. In the photoelectron emission spectrum, in addition to the above-threshold ionization peaks due to ionization interference in multiple cycles and the sideband peaks mainly due to the interference of ionized electrons at different moments along the rising edge of the laser pulse envelope, additional peaks of photoelectron emission whose intensity appears to oscillate with the increasing duration of the laser pulse can also be observed. Based on strong-field approximation and the population's analysis of the bound state, it is found that these photoelectron peaks originate from the ionization of the excited state and the oscillations of these peaks are due to the superposition of their peak energy positions with the sideband energy positions. Furthermore, it is demonstrated that the energy positions of the maximum intensity of the photoelectron emission spectra move towards the higher energy end as the duration of the driving laser pulse extends. This phenomenon can be attributed to the fact that the main moment of ionization of atoms changes with the increasing duration of the driving laser pulse, thus allowing the real-time ionization of atoms to be probed using photoelectron emission spectra.

Ion acceleration from a multispecies nanostructured target using a high-intensity laser: a simulation study

The use of nanostructured targets can enhance the energy and quality of accelerated electron and ion beams compared to conventional flat foil targets. Ion acceleration from plastic foil targets having sub-micron thickness embedded with rods of nanometre length using ultra-short intense laser pulses of intensity W cm−2 is investigated using particle-in-cell simulations. The laser and target parameters are tuned to achieve better performance with nanostructured targets compared to flat foils. Several novel features of the ion acceleration process are revealed in this study. A hybrid radiation pressure acceleration-target normal sheath acceleration mechanism using a linearly polarised (LP) laser is found to play a key role in accelerating protons upto ∼300 MeV of energy. The effects of multiple ion species on the acceleration of protons has been studied, and a narrow peak in the proton energy spectrum around ∼100 MeV is observed, which is attributed to the presence of heavier ions in the target.

Torsional Wave-Packet Dynamics in 2-Fluorobiphenyl Investigated by State-Selective Ionization-Detected Impulsive Stimulated Raman Spectroscopy.

We report the creation and observation of vibrational wave packets pertinent to torsional motion in a biphenyl derivative in its electronic ground-state manifold. Adiabatically cooled molecular samples of 2-fluorobiphenyl were irradiated by intense nonresonant ultrashort laser pulses to drive impulsive stimulated Raman excitation of torsional motion. Spectral change due to the nonadiabatic vibrational excitation is probed in a state-selective manner using resonance-enhanced two-photon ionization through the S1 ← S0 electronic transition. The coherent nature of the excitation was exemplified by adopting irradiation with a pair of pump pulses: observed signals for excited torsional levels exhibit oscillatory variations against the mutual delay between the pump pulses due to wave-packet interference. By taking the Fourier transform of the time course of the signals, energy intervals among torsional levels with v = 0-3 were determined and utilized to calibrate a density functional theory (DFT)-calculated torsional potential-energy function. Time variation of populations in the excited torsional levels was assessed experimentally by measuring integrated intensities of the corresponding transitions while scanning the delay. Early time enhancement of the population (up to ∼2 ps) and gradual degradation of coherence (within ∼20 ps) appears. To explain the observed distinctive features, we developed a four-dimensional (4D) dynamical calculation in which one-dimensional (1D) quantum-mechanical propagation of the torsional motion was followed by solving the time-dependent Schrödinger equation, whereas three-dimensional (3D) molecular rotation was tracked by classical trajectory calculations. This hybrid approach enabled us to reproduce experimental results at a reasonable computational cost and provided a deeper insight into rotational effects on vibrational wave-packet dynamics.

Intensity delivery to the focal area with tight focusing of a femtosecond laser beam in a gas environment

We propose a comprehensive approach to describe the propagation regime of a tightly focused intense ultrashort laser pulse in a gaseous medium under conditions of its ionization, based on the use of a discrete aberration-free quasi-optical approximation. The proposed approach provides a good match of calculation results with available experimental data for air and helium. We have demonstrated that the use of the second harmonic ensures a noticeable advantage for all the discussed radiation parameters in the focal zone compared to the fundamental radiation. The developed integrated approach can be used to predict the intensity of an ultrashort laser pulse in the focal volume of a gas medium.

Influence of embedded NiO-nanoparticles on the nonlinear absorption of tungsten disulfide nanolayers

2D transition metal dichalcogenides possess fascinating properties due to their direct bandgap, strong spin-orbit coupling, and promising electronic/mechanical properties. In this work, we synthesized pure tungsten disulfide (WS2) nanolayers and NiO nanoparticles (NPs) decorated in few-layered WS2 and measured the third-order nonlinear optical properties using femtosecond Z-scan measurements. The open aperture Z-scan data illustrated that the inclusion of NiO nanoparticles into the WS2 layers increases the nonlinear absorption at 800 and 400 nm wavelengths. Furthermore, we observed the switchability of the nonlinear absorption from saturable absorption to two-photon absorption or reverse saturable absorption by changing the pump intensity. Thus, the embedded NiO NPs played a crucial role in the variation of intensity-dependent nonlinear absorption mechanism of WS2 nanolayers and thus can be helpful for various optical applications such as laser pulse compression and optical limiting to prevent over-exposure of protective photosensitive sensors by intense ultrashort laser pulses.

Electrical topological defects induced by terahertz laser pulses

Recent experimental evidence and theoretical simulations have shown that electrical polarization can be tuned and even deterministically controlled in ferroelectrics by applying laser pulses having a frequency that is higher than that of the main polarization (soft) mode. Here, by using ab initio computations, we further discover that such pulses can also create nontrivial topological polar phases in bulk ferroelectric materials. Such a phenomenon is found to originate from nonthermal quenching process in which the applied intense ultrashort laser pulse first squeezes the ferroelectric phase into a cubic-like paraelectric phase at a moderate temperature and then to a renucleation process akin to the Kibble-Zurek mechanism creating nontrivial topological polar defects in the bulk ferroelectric ground-state phase. Our work therefore presents a novel and optical mean of creating topological defects in ferroelectrics.

Generation of synchronized x-rays and mid-infrared pulses by Doppler-shifting of relativistically intense radiation from near-critical-density plasmas

It is shown that when relativistically intense ultrashort laser pulses are reflected from the boundary of a plasma with a near-critical density, the Doppler frequency shift leads to generation of intense radiation in both the high-frequency (up to the x-ray) and low-frequency (mid-infrared) ranges. The efficiency of energy conversion into the wavelength range above 3 µm can reach several percent, which makes it possible to obtain relativistically intense pulses in the mid-infrared range. These pulses are synchronized with high harmonics in the ultraviolet and x-ray ranges, which opens up opportunities for high-precision pump–probe measurements, in particular, laser-induced electron diffraction and transient absorption spectroscopy.

Shock Waves in Weakly Relativistic e-p-i Plasma: Application to Plasma Created by Ultraintense Short Pulse Laser

In this article, the role of the positrons shock waves generation in weakly relativistic laser-created plasma is investigated. The plasma considered is generated on the rear face of a target, irradiated by a high intensity short pulse laser, in the framework of target normal sheath acceleration (TNSA) mechanism. This plasma is composed of Boltzmann distributed positrons, hot and cold super-thermal electrons, and dynamic ions. Kinematic viscosity among the plasma constituents has been also considered. With the purpose of studying the behavior of nonlinear ion acoustic shock waves (IASHWs), the reductive perturbation method (RPM) has been employed and Korteweg-de Vries Burgers equation has been derived. It was observed that different plasma parameters (namely, electrons super-thermality, number of positrons, ion temperature, kinematic viscosity, etc.) have a real impact on the propagation of IASHWs. As electron–positron plasmas with ion possessing relativistic velocities are often detected in laboratory experiments, astrophysical, and space environments, the present work will help to explain the different types of collective processes and instabilities in regions where e-p-i plasmas can exist.

Light-Induced Ultrafast Molecular Dynamics: From Photochemistry to Optochemistry.

By precisely controlling the waveform of ultrashort laser fields, electronic and nuclear motions in molecules can be steered on extremely short time scales, even in the attosecond regime. This new research field, termed “optochemistry”, presents the light field in the time-frequency domain and opens new avenues for tailoring molecular reactions beyond photochemistry. This Perspective summarizes the ultrafast laser techniques employed in recent years for manipulating the molecular reactions based on waveform control of intense ultrashort laser pulses, where the chemical reactions can take place in isolated molecules, clusters, and various nanosystems. The underlying mechanisms for the coherent control of molecular dynamics are explicitly explored. Challenges and opportunities coexist in the field of optochemistry. Advanced technologies and theoretical modeling are still being pursued, with great prospects for controlling chemical reactions with unprecedented spatiotemporal precision.

Determination of geometrical structure of CCl3+ by trapped-ion electron diffraction

A trapped-ion electron diffraction (TIED) apparatus has been developed. By sufficient suppression of the background signals originating from electrons scattered by residual gases and those originating from the back-scattered and secondary electrons generated at a Faraday cup, the gas electron diffraction pattern of CCl3+, generated through the dissociative ionization of CCl4 by near-IR ultrashort intense laser pulses, is recorded using the TIED apparatus at the electron acceleration voltage of 18.8 keV. The determined internuclear distances, r(C-Cl) = 1.66(2) Å and r(Cl⋯Cl) = 2.87(2) Å, which are consistent with theoretically calculated values, confirm that CCl3+ takes a planar geometry.

Ultrahızlı Optik Darbeler Kullanılarak Azot Molekülünden Yüksek Mertebeli Harmonik Üretimi

Generation of coherent extreme ultraviolet (XUV) pulses is a nonlinear process of high harmonic generation (HHG). HHG produced in molecular nitrogen (N2) medium has been obtained using ultrashort intense laser pulses. The strong laser field was focused onto a gas cell to produce short wavelengths having photon energy up to 54 eV. The highest photon energy is experimentally observed as the 35th order. The absorption of harmonics restricts the harmonic yield efficiency. The harmonic yield is affected by the interaction length and medium pressure. The harmonic yield changes with the medium parameters. The simulation for the absorption length was performed using the Mathematica program. Variation of the harmonic signal has been attributed to the absorption of harmonics, and it is compared with the absorption length.

Two-body dissociation of formic acid following double ionization by ultrafast laser pulses

We studied the fragmentation of planar formic acid (HCOOH) molecules following their double ionization by intense ultrashort laser pulses. Deuterium tagging (i.e., HCOOD) combined with coincidence momentum imaging measurements of all fragment ions enabled determination of the role of the hydroxyl and carboxyl hydrogen atoms in the breakup. Specifically, we observe a strong preference for the hydroxyl (OD) group to remain intact in a ${\mathrm{HCOOD}}^{2+}\ensuremath{\rightarrow}\phantom{\rule{4pt}{0ex}}{\mathrm{OD}}^{+}+{\mathrm{HCO}}^{+}$ fragmentation, which is an order of magnitude more likely than ${\mathrm{OH}}^{+}+{\mathrm{DCO}}^{+}$. An even larger preference for breaking the H-C bond over the O-H bond is observed in the ${\mathrm{H}}^{+}+{\mathrm{DCO}}_{2}^{+}$ and ${\mathrm{D}}^{+}+{\mathrm{HCO}}_{2}^{+}$ deprotonation channels. Bond rearrangement, leading to ${\mathrm{H}}_{2}^{+}$ or ${\mathrm{H}}_{2}{\mathrm{O}}^{+}$ formation, exhibits no isotopic preference. The kinetic-energy-release distributions of the ${\mathrm{OH}}^{+}+{\mathrm{DCO}}^{+}$ and ${\mathrm{O}}^{+}+{\mathrm{H}}_{2}{\mathrm{CO}}^{+}$ breakup channels suggest that more than one process contributes to these final products, although further theoretical work is needed to identify the specific paths.

Intense Laser Pulse Interaction With Graphene and Graphene Ribbons

In this work we investigate quantum mechanically the interaction of an intense ultrashort laser pulse with the graphene monolayer as well as with the armchair graphene ribbons of different widths. We consider a tight binding (TB) Hamiltonian of the monolayer graphene and give two rules for deriving the dispersion relations of the armchair graphene ribbons of any width, N, from the TB eigenvalues of the monolayer. The band structure of the monolayer and the armchair ribbons of different widths are discussed with illustrations. The time-dependent wavefunctions of the systems and the expectation values of interest are determined by solving the coupled equations of the band amplitudes “exactly” (numerically). First, simulations are made for the population excitation in the conduction band (CB) from the valence band (BV), the VB-CB interband correlation (or “coherence”), the intraband, the interband and the total currents in the monolayer graphene. The graphene currents are compared with the corresponding currents induced in an armchair ribbon (width, N = 3). The change from the 2D monolayer to the 1D ribbon shows a remarkable transition of the dominance of the intraband current that leads to a near steady total current in the monolayer, to a dominance of the interband current in the ribbon that induces an oscillatory current in the ribbon beyond the pulse duration. The difference observed might be a combined effect of the “confinement” in one dimention and a finite band-gap minimum in the case of the ribbon. However, this transition should be further investigated for better clarity. A brief comparison of the radiation spectra emitted from the monolayer and from the ribbon is also made. They show a grossly similar structure and a relative insensitivity with respect to the detailed structure of the targets chosen. This might be due to the dominance of virtual continuum-continuum transitions, to and from the bands states, that lie behind the fundamental quantum process of high harmonic emissions. Lastly, the dependence of the charge currents, induced in a ribbon of unit width (N = 1), on the carrier-envelope-phase (CEP) of the incident laser pulse is investigated. It is seen that the shape of the main part of the current produced in the ribbon can be fully reversed by changing the CEP of the ultrashort laser pulse from 0 to π. More generally, it is suggested that the pulse shape of the charge carriers in the ribbon could be designed by similarly tailoring the form of the vector potential of the incident laser pulse.

Electrostatic shock waves driven by electron vortices in laser–plasma interactions

Nonlinear structures such as shock waves and vortices widely exist in nature and the Universe. They have also been separately observed in laser–plasma interactions. We show for the first time that two perpendicularly propagated collisionless electrostatic shock waves (CESs) can be excited by a moving electron vortex (EV). The latter is driven by an ultrashort intense laser pulse propagating through a sandwich nonuniform underdense plasma slab and is found to move perpendicularly to the density gradient. Two CESs are observed on both sides of the passing route of the EVs. The left-side CES is induced by a high-density electron layer, which originates from the vortex front and is compressed and accelerated during the EV motion. The right-side CES is induced by supersonic ions accelerated by the EVs directly. Ion acceleration by such CESs along the directions perpendicular to the vortex propagation is also observed. This study reveals the transformation of nonlinear structures and provides new routes for laser energy dissipation in plasmas.

Optical Properties of Gold After Intense Short-Pulse Excitations

Intense ultrashort laser pulses can create highly excited matter with extraordinary properties. Experimental and theoretical investigations of these extreme conditions are very complex and usually intertwined. Here, we report on a theoretical approach for the electron scattering rates and the optical properties in gold at elevated temperatures. Our theory is based on the degree of occupancy of the conduction band as well as inputs from ab initio simulations and experimental data. After the electron system has reached a quasi-equilibrium, the occupancy is fully determined by the electron temperature. Thus, our approach covers the important relaxation stage after fast excitations when the two-temperature model can be applied. Being based on the electronic structure of solids, the model is valid for lattice temperatures up to melting but the electron temperature might exceed this limit by far. Our results agree well with recent experimental data for both the collision frequencies and the conductivity of highly excited gold. Scattering of sp-electrons by d-electrons is found to be the dominant damping mechanism at elevated electron temperatures and depends strongly on the number of conduction electrons, hence, revealing the microscopic origin of the conductivity change after heating. The supportive benchmarks with experiments are very valuable as the underlying scattering rates determine a number of other transport, optical and relaxation properties of laser-excited matter.