X-ray Laser Pulses Research Articles

Simulation of the interaction of intense ultrashort X-ray laser pulses with micro-sized Al targets

We study the interaction of extremely short and high-intensity X-ray pulses with a 1.0μm thick Al foil. Four pulse lengths – 100 fs, 200 fs, 300 fs, and 400 fs – are considered. The photon energy is 1830 eV and the pulse intensity is 1017W/cm2. The interaction dynamics are calculated via a radiation hydrodynamic code. The X-ray laser pulse heats the target isochorically. It generates a homogeneous hot dense matter; electrons are hotter than ions. The simulation of the interaction of pump and probe pulses with a delay time in the fs scale provides that the probe pulse heats the target significantly. A Monte-Carlo method is used to provide a microscopic description; the electron distribution function shows a two-temperature system. The electron distribution has spikes at the energy difference between the k-edges of Al ions and the energy of incident photons. The energies of these spikes depend on the considered ionization depression model. The Chihara formula and the non-equilibrium random phase approximation are utilized to calculate the X-ray Thomson scattering spectrum (XRTS). For collective scattering, the plasmon peaks are a function of the pulse lengths and the electron distribution function. Therefore, when XRTS is fitted to a measured spectrum may give the target density, the target temperature, and the microscopic electron distribution function.

Linear Breit-Wheeler pair production by high-energy bremsstrahlung photons colliding with an intense x-ray laser pulse

A possible setup for the experimental verification of linear Breit-Wheeler pair creation of electrons and positrons in photon-photon collisions is studied theoretically. It combines highly energetic bremsstrahlung photons, which are assumed to be generated by an incident beam of GeV electrons penetrating through a high-$Z$ target, with keV photons from an x-ray laser field, which is described as a focused Gaussian pulse. We discuss the dependencies of the pair yields on the incident electron energy, target thickness, laser parameters, and collision geometry. It is shown that, for suitable conditions that are nowadays in reach at x-ray laser facilities, the resulting number of created particles seems to be well accessible for enabling the first experimental observation of the linear Breit-Wheeler process $\ensuremath{\gamma}\ensuremath{\gamma}\ensuremath{\rightarrow}{e}^{+}{e}^{\ensuremath{-}}$.

Nuclear-state population transfer using composite stimulated Raman adiabatic passage

Nuclear-state population transfer in three-level Λ-like nuclei that interact with two X-ray laser pulses using composite stimulated Raman adiabatic passage (CSTIRAP) technique is investigated theoretically. Due to the fact that the frequency of existing X-ray lasers is less than the frequency of gamma rays, so in this method the nuclei are accelerated and interact with two X-ray laser pulses with different frequencies. We use a series of pairs of delay pulses so that the phases of the pulses in each stage are different from the other one. In this method, the maximum values of the pump and Stokes laser pulses are adjusted so that the Rabi frequencies corresponding to the two pulses are equal during time evolution. We show that by properly selecting the phases as well as the order of the pulses in each stage, in single-photon and two-photon resonance cases, the population is completely transferred from the initial ground state to the final ground state. In this scheme, the number of steps is optional and as the number of steps increases, the required lasers intensities in each step decrease significantly.

Diffraction data from aerosolized Coliphage PR772 virus particles imaged with the Linac Coherent Light Source

Single Particle Imaging (SPI) with intense coherent X-ray pulses from X-ray free-electron lasers (XFELs) has the potential to produce molecular structures without the need for crystallization or freezing. Here we present a dataset of 285,944 diffraction patterns from aerosolized Coliphage PR772 virus particles injected into the femtosecond X-ray pulses of the Linac Coherent Light Source (LCLS). Additional exposures with background information are also deposited. The diffraction data were collected at the Atomic, Molecular and Optical Science Instrument (AMO) of the LCLS in 4 experimental beam times during a period of four years. The photon energy was either 1.2 or 1.7 keV and the pulse energy was between 2 and 4 mJ in a focal spot of about 1.3 μm x 1.7 μm full width at half maximum (FWHM). The X-ray laser pulses captured the particles in random orientations. The data offer insight into aerosolised virus particles in the gas phase, contain information relevant to improving experimental parameters, and provide a basis for developing algorithms for image analysis and reconstruction.

Ultrafast Real-Time Dynamics of CO Oxidation over an Oxide Photocatalyst

Femtosecond X-ray laser pulses synchronized with an optical laser were employed to investigate the reaction dynamics of the photooxidation of CO on the anatase TiO2(101) surface in real time. Our t...

URSA-PQ: A Mobile and Flexible Pump-Probe Instrument for Gas Phase Samples at the FLASH Free Electron Laser

We present a highly flexible and portable instrument to perform pump-probe spectroscopy with an optical and an X-ray pulse in the gas phase. The so-called URSA-PQ (German for ‘Ultraschnelle Röntgenspektroskopie zur Abfrage der Photoenergiekonversion an Quantensystemen’, Engl. ‘ultrafast X-ray spectroscopy for probing photoenergy conversion in quantum systems’) instrument is equipped with a magnetic bottle electron spectrometer (MBES) and tools to characterize the spatial and temporal overlap of optical and X-ray laser pulses. Its adherence to the CAMP instrument dimensions allows for a wide range of sample sources as well as other spectrometers to be included in the setup. We present the main design and technical features of the instrument. The MBES performance was evaluated using Kr M4,5NN Auger lines using backfilled Kr gas, with an energy resolution ΔE/E ≅ 1/40 in the integrating operative mode. The time resolution of the setup at FLASH 2 FL 24 has been characterized with the help of an experiment on 2-thiouracil that is inserted via the instruments’ capillary oven. We find a time resolution of 190 fs using the molecular 2p photoline shift and attribute this to different origins in the UV-pump—the X-ray probe setup.

Beyond integration: modeling every pixel to obtain better structure factors from stills

Most crystallographic data processing methods use pixel integration. In serial femtosecond crystallography (SFX), the intricate interaction between the reciprocal lattice point and the Ewald sphere is integrated out by averaging symmetrically equivalent observations recorded across a large number (104-106) of exposures. Although sufficient for generating biological insights, this approach converges slowly, and using it to accurately measure anomalous differences has proved difficult. This report presents a novel approach for increasing the accuracy of structure factors obtained from SFX data. A physical model describing all observed pixels is defined to a degree of complexity such that it can decouple the various contributions to the pixel intensities. Model dependencies include lattice orientation, unit-cell dimensions, mosaic structure, incident photon spectra and structure factor amplitudes. Maximum likelihood estimation is used to optimize all model parameters. The application of prior knowledge that structure factor amplitudes are positive quantities is included in the form of a reparameterization. The method is tested using a synthesized SFX dataset of ytterbium(III) lysozyme, where each X-ray laser pulse energy is centered at 9034 eV. This energy is 100 eV above the Yb3+ L-III absorption edge, so the anomalous difference signal is stable at 10 electrons despite the inherent energy jitter of each femtosecond X-ray laser pulse. This work demonstrates that this approach allows the determination of anomalous structure factors with very high accuracy while requiring an order-of-magnitude fewer shots than conventional integration-based methods would require to achieve similar results.

High-repetition-rate few-attosecond high-quality electron beams generated from crystals driven by intense X-ray laser

Advances in X-ray laser sources have paved the way to relativistic attosecond X-ray laser pulses and opened up the possibility of exploring high-energy-density physics with this technology. With particle-in-cell simulations, we investigate the interaction of realistic metal crystals with relativistic X-ray laser pulses of parameters that will be available in the near future. A wakefield of the order of TV/cm is excited in the crystal and accelerates trapped electrons stably even though the wakefield is locally modulated by the crystal lattice. Electron injection either occurs at the sharp crystal–vacuum boundary or is controlled by coating the crystal with a high-density film. High-repetition-rate attosecond (20 as) monoenergetic electron beams of energy 125 MeV, charge 100 fC, and emittance 1.6 × 10−9 m rad can be produced by shining MHz X-ray laser pulses of energy 2.1 mJ onto coated crystals several micrometers thick. Such a miniature crystal accelerator, which has high reproducibility and allows sufficient control of the parameters of the electron beams, greatly expands the applications of X-ray free electron lasers. For example, it could serve as an ideal electron source for ultrafast electron diffraction and ultrafast electron microscopy to achieve attosecond resolution.

Single-shot table-top coherent x-ray imaging with diffraction-limited resolution by nonlinear phase variations

We demonstrated single-shot high-numerical-aperture coherent diffraction imaging (CDI) with a diffraction-limited resolution using table-top x-ray laser at 13.9 nm. In order to achieve the diffraction-limited resolution, a nonlinear phase variation was introduced in a sample so that an asymmetric diffraction pattern with clear visibility could be extended to high spatial frequencies. From the diffraction signal, the sample image was successfully reconstructed with a resolution of 22 nm, which is close to the diffraction-limited resolution of 21 nm, using the phase retrieval procedure. The model calculation and simulations, performed to verify the experimental results, showed that the implementation of the nonlinear phase variation in the sample enhanced the resolution by a factor of about two, as compared to the case of a pure absorption sample. In addition, we examined the CDI with phase controllers introducing nonlinear phase variation illuminated by a table-top femtosecond Kr x-ray laser pulse at 32.8 nm that produced an asymmetric diffraction pattern extended to high spatial frequencies.

Laser-induced damage thresholds and mechanism of silica glass induced by ultra-short soft x-ray laser pulse irradiation.

Laser-induced damage thresholds (LIDTs) of silica glasses obtained by the femtosecond soft x-ray free-electron laser (SXFEL, 13.5 nm, 70 fs) and the picosecond soft x-ray laser (SXRL, 13.9 nm, 7 ps) are evaluated. The volume of the hydroxyl group in the silica glasses influenced its LIDTs. The LIDTs obtained in this research by the femtosecond SXFEL and the picosecond SXRL were nearly identical, but were different from that by the nanosecond soft x-ray pulse. The photoionization processes of silica glass in context of the laser-induced damage mechanism (LIDM) are also discussed. In the ultra-short soft x-ray pulse irradiation regime, the LIDM can be speculated to include the spallation process with a scission of bondings.

Density matrix formalism for femtosecond x-ray absorption and its excitonic enhancement

A reduced density matrix (RDM) formalism to simulate the dynamics of core-valence electronic excitation in a metal induced by a femtosecond x-ray laser pulse is presented. The theory is based on the time-dependent unrestricted Hartree–Fock (TDUHF) equation for a one-electron RDM combined with an off-diagonal collision term in the Born approximation (BA), where molecular orbitals (MOs) of a model cluster are used as a basis set. These MOs are calculated with a newly developed semiempirical method in the neglect of diatomic differential overlap approximation that takes into account atomic core structures and valence-orbital hybridization. The off-diagonal component of core-valence RDM is decomposed into a rapidly oscillating factor synchronizing with the x-ray field and a slowly varying envelope; time evolution of the latter yields induced electric polarization and complex electric susceptibility. As a numerical test, K-shell absorption near-edge spectra of copper are computed for a single-shot, weak femtosecond x-ray pulse. It is thereby shown that the attractive interaction between an excited electron and a core hole, described by the exchange part of the self-energy matrix, gives rise to excitonic enhancement of x-ray near-edge absorption. The TDUHF approximation significantly overestimates the excitonic enhancement; additional consideration of the screening of electron-hole interaction by valence electrons in BA leads to a prediction of absorption coefficients comparable to the existing experimental values.

Two-Color Soft X-Ray Lasing in a High-Density Nickel-like Krypton Plasma.

We report evidence of strong lasing on the 4p-4s transition at 62.7nm in nickel-like krypton occurring simultaneously with the usual 4d-4p lasing at 32.8nm. The gain dynamics of both transitions were experimentally and numerically investigated and found comparable. The two-color amplifier was seeded by the same harmonic pulse, therefore producing a short-duration coherent two-color soft x-ray laser pulse. Both transitions offer similar prospects of pulse energy and duration and could lead to the delivery of intense and ultrashort two-color coherent soft x-ray pulses with a controllable delay.

The Magnitude and Waveform of Shock Waves Induced by X-ray Lasers in Water

The high energy densities deposited in materials by focused X-ray laser pulses generate shock waves which travel away from the irradiated region, and can generate complex wave patterns or induce phase changes. We determined the time-pressure histories of shocks induced by X-ray laser pulses in liquid water microdrops, by measuring the surface velocity of the microdrops from images recorded during the reflection of the shock at the surface. Measurements were made with ~30 µm diameter droplets using 10 keV X-rays, for X-ray pulse energies that deposited linear energy densities from 3.5 to 120 mJ/m; measurements were also made with ~60 µm diameter drops for a narrower energy range. At a distance of 15 µm from the X-ray beam, the peak shock pressures ranged from 44 to 472 MPa, and the corresponding time-pressure histories of the shocks had a fast quasi-exponential decay with positive pressure durations estimated to range from 2 to 5 ns. Knowledge of the amplitude and waveform of the shock waves enables accurate modeling of shock propagation and experiment designs that either maximize or minimize the effect of shocks.

Demonstration of thin film compression for short-pulse X-ray generation

Thin film compression to the single-cycle regime combined with relativistic compression offers a method to transform conventional ultrafast laser pulses into attosecond X-ray laser pulses. These attosecond X-ray laser pulses are required to drive wakefields in solid density materials which can provide acceleration gradients of up to TeV/cm. Here we demonstrate a nearly 99% energy efficient compression of a 6.63 mJ, 39 fs laser pulse with a Gaussian mode to 20 fs in a single stage. Further, it is shown that as a result of Kerr-lensing, the focal spot of the system is slightly shifted on-axis and can be recovered by translating the imaging system to the new focal plane. This implies that with the help of wave-front shaping optics the focusability of laser pulses compressed in this way can be partially preserved.

Ultrahigh brightness attosecond electron beams from intense X-ray laser driven plasma photocathode

The emerging intense attosecond X-ray lasers can extend the Laser Wakefield Acceleration mechanism to higher plasma densities in which the acceleration gradients are greatly enhanced. Here we present simulation results of high quality electron acceleration driven by intense attosecond X-ray laser pulses in liquid methane. Ultrahigh brightness electron beams can be generated with 5-dimensional beam brightness over [Formula: see text]. The pulse duration of the electron bunch can be shorter than 20 as. Such unique electron sources can benefit research areas requiring crucial spatial and temporal resolutions.

Mesoscopic hierarchic polarization structure in the relaxor ferroelectrics Pb[(Mg1/3Nb2/3)1−xTix]O3

Mesoscopic polarization structures such as polar nanoregions and polarization domain walls are the key factors connecting microscopic fundamental polarization structures with macroscopic practical dielectric properties. A snapshot observation of the domain in the relaxor ferroelectrics $\mathrm{Pb}[{(\mathrm{M}{\mathrm{g}}_{1/3}\mathrm{N}{\mathrm{b}}_{2/3})}_{1\text{\ensuremath{-}}x}\mathrm{T}{\mathrm{i}}_{x}]{\mathrm{O}}_{3}$ just in the vicinity of morphotropic phase boundary region was performed by use of 7-ps single shot soft x-ray laser pulse. A self-assembled evolution of the oblique polarization domain was observed in $\mathrm{Pb}[{(\mathrm{M}{\mathrm{g}}_{1/3}\mathrm{N}{\mathrm{b}}_{2/3})}_{72.2}\mathrm{T}{\mathrm{i}}_{27.8}]{\mathrm{O}}_{3}$ under the sample temperature decreased with the thermal equilibrium condition. Based on energetic discussion, antiphase shift of domain wall pairs keeping flat boundaries was proposed for the dielectric response. A sharp enhancement in the dielectric response at the vicinity of morphotropic phase boundary region reported previously was recognized as evidence for the hierarchic nature of the present oblique polarization domain wall.

Sensitivity enhancement of poly(methyl methacrylate) upon exposure to picosecond-pulsed extreme ultraviolet

Short-pulse extreme ultraviolet (EUV) of a free-electron laser (FEL) is a prime candidate as a next-generation EUV lithography light source. However, the physical events and chemical reactions in resist materials, induced by the short-pulse EUV, have not yet been elucidated. In this study, the morphological and chemical changes in poly(methyl methacrylate) (PMMA) induced by picosecond-pulsed EUV were investigated using an X-ray laser (XRL) as a touchstone for next-generation EUV-FEL lithography. The XRL is suitable for the evaluation of resist materials in next-generation EUV-FEL lithography because of its short pulse width (7 ps) and high intensity (approximately 200 nJ/pulse at a maximum). The sensitivity of PMMA upon exposure to a 7 ps XRL pulse was enhanced by approximately 50 times in comparison with using conventional EUV sources, which have a typical pulse width of the order of nanoseconds. X-ray photoelectron spectroscopy revealed the decomposition of both the main and side chains of PMMA after XRL irradiation. These changes only occurred for relatively high doses of EUV irradiation at picosecond timescales. Thus, the results suggest the importance of a specific resist design for next-generation EUV-FEL lithography.

Science of High Energy, Single-Cycled Lasers

With the advent of the Thin Film Compression, high energy single-cycled laser pulses have become an eminent path to the future of new high-field science. An existing CPA high power laser pulse such as a commercially available PW laser may be readily converted into a single-cycled laser pulse in the 10PW regime without losing much energy through the compression. We examine some of the scientific applications of this, such as laser ion accelerator called single-cycle laser acceleration (SCLA) and bow wake electron acceleration. Further, such a single-cycled laser pulse may be readily converted through relativistic compression into a single-cycled, X-ray laser pulse. We see that this is the quickest and very innovative way to ascend to the EW (exawatt) and zs (zeptosecond) science and technology. We suggest that such X-ray laser pulses have a broad and new horizon of applications. We have begun exploring the X-ray crystal (or nanostructured) wakefield accelerator and its broad and new applications into gamma rays. Here, we make a brief sketch of our survey of this vista of the new developments.

Nondipole effects in helium ionization by intense soft x-ray laser pulses

We consider the helium atom exposed to laser pulses in soft-x regime at intensities of the order of 1017–1020 W/cm2. Two cases are investigated, first a pulse with a central frequency of 20 a.u. (~522.2eV) and a pulse with a central frequency of 50 a.u. (~1.36keV). We solve the time-dependent Schrodinger equation (TDSE), nondipole (retardation) effects are included up to O(1/c) (c being the velocity of light). We study the single photoionization of helium with a focus on nondipole effects. We calculate the total and partial photoelectron energy spectra, and the photoelectron angular distributions. The nondipole effects associated with the A·P and A2 coupling terms in the Hamiltonian (A denoting the vector potential of the field and P the momentum operator) are thoroughly analyzed in the region of one-photon resonance. We show that the nondipole contribution associated with A·P varies linearly with the intensity I while a three-photon transition involving A2 increases like I3, in agreement with lowest order perturbation theory (LOPT). At high intensities these contributions compete and the nondipole transition becomes nonlinear. The physical mechanisms associated with nondipole couplings are discussed, as well as their effects on photoelectron energy and angular distributions.

Breakdown of the nonrelativistic approximation in superintense laser-matter interactions

We study the breakdown of the nonrelativistic approximation in the multiphoton ionization of atomic hydrogen by some intense x-ray laser pulse, in a regime where the dipole approximation is no longer valid. To this end, both the time-dependent Dirac equation as well as its nonrelativistic counterpart, the time-dependent Schr\odinger equation, are solved within an ab initio numerical framework. It is demonstrated that a recently developed semirelativistic Schr\odinger equation for superintense laser fields [Lindblom et al., Phys. Rev. Lett. 121, 253202 (2018)] yields results in excellent agreement with the fully relativistic treatment. The semirelativistic equation is then used in an investigation of the role of higher-order beyond-dipole corrections to the laser-matter interaction. The result of the present study can be summarized into two main findings: (1) relativistic effects predict a blueshift of the multiphoton ionization spectrum, and (2) higher-order beyond dipole corrections (beyond the leading-order term) indicate a corresponding redshift of the photoelectron spectrum. However, the two shifts turn out to be of the same order of magnitude, effectively leading to a net cancellation of their respective contributions. This apparent cancellation effect raises an important question: Is the distinction between relativistic blueshifts and higher-order beyond dipole redshifts meaningful from an experimental point of view? The result of the present study indicates that the answer is negative because the two effects nonetheless cannot be measured separately. Therefore, instead, we suggest that the present findings should merely be taken as a demonstration that caution should be exercised when higher-order beyond-dipole and relativistic corrections are to be taken into account in approximation schemes in the modeling of superintense laser-matter interactions.