Soft X-ray Pulses Research Articles

Correlation of Characteristic Ne SXR Signal Pulse With Computed Plasma Focus Dynamics in the Ne (97.5%)–Kr (2.5%) Admixtures of the INTI PF Machine at 12 kV

This paper shows the correlation of the characteristic Ne soft X-ray (SXR) signal pulse with computed dynamics of the plasma focus using doped neon in Ne (97.5%)/Kr (2.5%) admixtures. The Lee model code is coupled with a specifically designed correlation excel template. The results show that typically, the characteristic Ne SXR pulse signal starts after the start of the reflected shock (RS) and before the beginning of the pinch. Specifically, in the illustrated shot, the RS phase starts at $3.375~\mu \text{s}$ while the pinch phase starts at $3.384~\mu \text{s}$ . The characteristic Ne SXR signal pulse starts at $3.377~\mu \text{s}$ , which is 2 ns after the start of the RS and 7 ns before the pinch starts. There is a consistent trend of Ne SXR correlation with the computed dynamics in the Ne doped with Kr admixtures up to a doping level of 2.5%.

Computer simulation of hybrid quantum technologies of energy accumulation, storage, transformation and transfer in nanoenergy materials

Here we study hybrid quantum technologies of accumulation, storage, transformation and transfer of energy in nanomaterials using nanoelectromechanical systems as hybrid binary two-level quantum devices. In the diagram representation of the quantum kinetics processes, general results on the hybrid binary structure of nanoelectromechanical systems and their two-level quantum mechanisms of functioning in nano-energy materials are given. It is shown that a quantum nanoelectromechanical system is a hybrid of two parts: a compact nanomolecular subsystem of nuclei and electrons and a locking them electromechanical capsule as supercapacitor layer of quantum entangled pairs of excitons. The layer has a subatomic thickness. The energy processes of nanoelectromechanical system occur at two levels: through single-electron channels of femtosecond pulses in the nanomolecular system and through two-electron channels of attosecond pulses in the electromechanical capsule. Starting with the initial accumulation of the attosecond pulse of the electromagnetic field, a step-by-step diagram of the functioning of the nanoelectromechanical system as a nanoenergy device is given. The final part of the paper presents the results of computer simulation of the functioning of the energy device of a nanoelectromechanical system in the form of a 500-atom cube with (100) faces in an FCC nickel crystal at three temperature conditions (1 K, 77 K, 293 K). It is revealed that the energy of soft X-ray pulses with energy 590 eV is effectively accumulated in the nanoelectromechanical energy device. For hundreds of picoseconds, this energy is partially dissipated, undergoing quantum fluctuations of the thermal field of the condensed state of the material. In all computer experiments for the studied temperatures, three identical energy jumps were found in the range up to 0.5 ns. Energy losses occur as a result of three identical jumps in the shape of the electromechanical capsule and the configurations of the nuclear-electronic subsystem embedded in it. It is shown that in the nonequilibrium quasistationary state the 500 - atomic cuboid nanoelectromechanical systems (NEMS) of nickel has a high stored energy about 0.9 eV per atom as a result from large distortion of the NEMS capsule.

Atom-specific activation in CO oxidation.

We report on atom-specific activation of CO oxidation on Ru(0001) via resonant X-ray excitation. We show that resonant 1s core-level excitation of atomically adsorbed oxygen in the co-adsorbed phase of CO and oxygen directly drives CO oxidation. We separate this direct resonant channel from indirectly driven oxidation via X-ray induced substrate heating. Based on density functional theory calculations, we identify the valence-excited state created by the Auger decay as the driving electronic state for direct CO oxidation. We utilized the fresh-slice multi-pulse mode at the Linac Coherent Light Source that provided time-overlapped and 30 fs delayed pairs of soft X-ray pulses and discuss the prospects of femtosecond X-ray pump X-ray spectroscopy probe, as well as X-ray two-pulse correlation measurements for fundamental investigations of chemical reactions via selective X-ray excitation.

Ultrafast X-ray Transient Absorption Spectroscopy of Gas-Phase Photochemical Reactions: A New Universal Probe of Photoinduced Molecular Dynamics.

Time-resolved spectroscopic investigations of light-induced chemical reactions with universal detection capitalize recently on single-photon molecular probing using laser pulses in the extreme ultraviolet or X-ray regimes. Direct and simultaneous mappings of the time-evolving populations of ground-state reactants, Franck-Condon (FC) and transition state regions, excited-state intermediates and conical intersections (CI), and photoproducts in photochemical reactions utilize probe pulses that are broadband and energy-tunable. The limits on temporal resolution are set by the transit- or dwell-time of the photoexcited molecules at specific locations on the potential energy surface, typically ranging from a few femtoseconds to several hundred picoseconds. Femtosecond high-harmonic generation (HHG) meets the stringent demands for a universal spectroscopic probe of large regions of the intramolecular phase-space in unimolecular photochemical reactions. Extreme-ultraviolet and soft X-ray pulses generated in this manner with few-femtosecond or sub-femtosecond durations have enormous bandwidths, allowing the probing of many elements simultaneously through excitation or ionization of core-electrons, creating molecular movies that shed light on entire photochemical pathways. At free electron lasers (FELs), powerful investigations are also possible, recognizing their higher flux and tunability but more limited bandwidths. Femtosecond time-resolved X-ray transient absorption spectroscopy, in particular, is a valuable universal probe of reaction pathways that maps changes via the fingerprint core-to-valence resonances. The particular power of this method over valence-ionization probes lies in its unmatched element and chemical-site specificities. The elements carbon, nitrogen, and oxygen constitute the fundamental building blocks of life; photochemical reactions involving these elements are ubiquitous, diverse, and manifold. However, table-top HHG sources in the "water-window" region (280-550 eV), which encompasses the 1s-absorption edges of carbon (284 eV), nitrogen (410 eV), and oxygen (543 eV), are far from abundant or trivial. Recent breakthroughs in the laboratory have embraced this region by using long driving-wavelength optical parametric amplifiers coupled with differentially pumped high-pressure gas source cells. This has opened avenues to study a host of photochemical reactions in organic molecules using femtosecond time-resolved transient absorption at the carbon K-edge. In this Account, we summarize recent efforts to deploy a table-top carbon K-edge source to obtain crucial chemical insights into ultrafast, ultraviolet-induced chemical reactions involving ring-opening, nonadiabatic excited-state relaxation, bond dissociation and radical formation. The X-ray probe provides a direct spectroscopic viewport into the electronic characters and configurations of the valence electronic states through spectroscopic core-level transitions into the frontier molecular orbitals of the photoexcited molecules, laying fertile ground for the real-time mapping of the evolving valence electronic structure. The profound detail and mechanistic insights emerging from the pioneering experiments at the carbon K-edge are outlined here. Comparisons of the experimental methodology with other techniques employed to study similar reactions are drawn, where applicable and relevant. We show that femtosecond time-resolved X-ray transient absorption spectroscopy blazes a new trail in the study of nonadiabatic molecular dynamics. Despite table-top implementations being largely in their infancy, future chemical applications of the technique will set the stage for widely applicable, universal probes of photoinduced molecular dynamics with unprecedented temporal resolution.

Thermomechanical damage thresholds of tungsten as candidate first wall material under pulsed soft X-ray irradiations

In a Z-Pinch driven fusion-fission hybrid reactor (Z-FFR), a thin spherical metal shell and rare Ar buffer gas are introduced to mitigate the transient X-ray bursts to prevent the first wall from fatal damages by intense X-rays, which take almost 20% of the fusion energy yield (approximately 300 MJ). Thereby soft X-rays as well as the EUVs, are believed to become the dominant threatening sources that the first wall will suffer from. Tungsten is chosen to be the prime candidate material of the Z-FFR first wall, and has been tested on ‘QG-I’ facility to determine the single-shot thermomechanical damage thresholds under pulsed soft X-ray irradiations, as well as to verify and validate the modeling and calculating code ‘FWDR1D’. Several tens of tungsten samples as well as zirconium samples were exposed to a variety of X-ray fluences in the range of 0.1 to 0.7 J/cm2 and with an account of more than 20 shots. The theoretical and experimental results meet well, and analysis of the results indicates that tungsten has specific thermomechanical damage thresholds with X-ray fluences in the range of 0.15 to 0.21 J/cm2 under single-shot soft X-ray irradiations.

High-Quality Implosion of Overmassed <inline-formula> <tex-math notation="LaTeX">$Z$ </tex-math> </inline-formula>-Pinch in the Experiment With Magnetocumulative Generator

This paper presents the results of the experiment with an overmassed wire-array $Z$ -pinch load that is powered by a current pulse (amplitude ~4.3 MA and rise time $\sim 0.9~\mu \text{s}$ ) from a multidisk magnetocumulative generator. Interesting feature of the experimentally recorded soft X-ray (SXR) pulse is short (~10 ns) duration at a microsecond current rise time with total energy of several hundreds of kilojoules. Obtained results are the evidence of high-quality implosion of the current-carrying plasma. The 2-D magnetohydrodynamic code FLUX-rz was used for the numerical simulation and analysis of the obtained results. The calculations indicated that only ~30% of the initial load mass took part in the SXR generation. The main peculiarities of the overmassed $Z$ -pinch implosion are discussed in this paper.

Plasma impurities observed by a pulse height analysis diagnostic during the divertor campaign of the Wendelstein 7-X stellarator.

The paper reports on the optimization process of the soft X-ray pulse height analyzer installed on the Wendelstein 7-X (W7-X) stellarator. It is a 3-channel system that records X-ray spectra in the range from 0.6 to 19.6 keV. X-ray spectra, with a temporal and spatial resolution of 100 ms and 2.5 cm (depending on selected slit sizes), respectively, are line integrated along a line-of-sight that crosses near to the plasma center. In the second W7-X operation phase with a carbon test divertor unit, light impurities, e.g., carbon and oxygen, were observed as well as mid- to high-Z elements, e.g., sulfur, chlorine, chromium, manganese, iron, and nickel. In addition, X-ray lines from several tracer elements have been observed after the laser blow-off injection of different impurities, e.g., silicon, titanium, and iron, and during discharges with prefill or a gas puff of neon or argon. These measurements were achieved by optimizing light absorber-foil selection, which defines the detected energy range, and remotely controlled pinhole size, which defines photon flux. The identification of X-ray lines was confirmed by other spectroscopic diagnostics, e.g., by the High-Efficiency XUV Overview Spectrometer, HEXOS, and high-resolution X-ray imaging spectrometer, HR-XIS.

Pulse duration of a partially coherent soft X-ray laser estimated from far-field speckle statistics.

A novel method for estimating the pulse duration of partially coherent soft X-ray pulses from a far-field intensity pattern is presented. The method is based on intensity statistics at a single point in space and time, which allows the number of coherent longitudinal modes to be measured. Utilizing the knowledge of the coherence time of the radiation, either from the measurement of the spectral bandwidth or from numerical simulations, the duration of each individual pulse can be evaluated. This method was used to estimate the pulse duration of the laser-driven nickel-like molybdenum soft X-ray laser that is based on amplified spontaneous emission from a narrow plasma column and emits at a wavelength of 18.9nm. By varying the length of the gain medium, a clear dependence of the number of modes caused mainly by the spectral line narrowing was observed. Supported by simulations of radiative transfer and pulse propagation, the pulse duration at the end of a 3mm long gain medium was estimated to be 3.5ps. The experimental data from far-field intensity patterns were also analyzed by applying the generalized van Cittert-Zernike theorem, providing a lower bound of effective source size.

High-Power X-Ray Line Radiation of the Plasma Produced in a Collision of High-Energy Plasma Flows

Results are presented from experimental studies of a pulsed source of soft X-ray (SXR) emission with photon energies in the range of 0.4–1 keV and an output energy of 2–10 kJ. SXR pulses with a duration of 10–15 μs were generated in collisions of two plasma flows propagating toward one another in a longitudinal magnetic field. The plasma flows with velocities of (2–4) × 107 cm/s and energy contents of 70–100 kJ were produced by two electrodynamic coaxial accelerators with pulsed gas injection. Nitrogen and neon, as well as their mixtures with deuterium, were used as working gases. The diagnostic equipment is described, and the experimental results obtained under different operating conditions are discussed. In particular, X-ray spectroscopy was used to study the high-temperature plasma produced in a collision of two plasma flows. The observed intensities of spectral lines are compared with the results of detailed kinetic calculations performed in a steady-state approximation. The calculations of the nitrogen and neon kinetics have shown that the electron temperature of a nitrogen plasma can be most conveniently determined from the intensity ratio of the resonance lines of He- and H-like nitrogen ions, while that of a neon plasma, from the intensity ratio between the resonance line of He-like Ne IX ions and the 3p−2s line of Li-like Ne VIII ions. In the experiments with plasma flows containing nitrogen ions, the electron temperature was found to be ≈120 eV, whereas in the experiments with plasma flows containing neon ions, it was 160–170 eV.

Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment.

We present a general experimental concept for jitter-free pump and probe experiments at free electron lasers. By generating pump and probe pulse from one and the same X-ray pulse using an optical split-and-delay unit, we obtain a temporal resolution that is limited only by the X-ray pulse lengths. In a two-color X-ray pump and X-ray probe experiment with sub 70 fs temporal resolution, we selectively probe the response of orbital and charge degree of freedom in the prototypical functional oxide magnetite after photoexcitation. We find electronic order to be quenched on a time scale of (30 ± 30) fs and hence most likely faster than what is to be expected for any lattice dynamics. Our experimental result hints to the formation of a short lived transient state with decoupled electronic and lattice degree of freedom in magnetite. The excitation and relaxation mechanism for X-ray pumping is discussed within a simple model leading to the conclusion that within the first 10 fs the original photoexcitation decays into low-energy electronic excitations comparable to what is achieved by optical pump pulse excitation. Our findings show on which time scales dynamical decoupling of degrees of freedom in functional oxides can be expected and how to probe this selectively with soft X-ray pulses. Results can be expected to provide crucial information for theories for ultrafast behavior of materials and help to develop concepts for novel switching devices.

Generating femtosecond coherent X-ray pulses in a diffraction-limited storage ring with the echo-enabled harmonic generation scheme

To study ultrafast processes at the sub-picosecond level, novel methods based on coherent harmonic generation technologies have been proposed to generate ultrashort radiation pulses in existing ring-based light sources. Using the High Energy Photon Source as an example, we numerically test the feasibility of implementing one coherent harmonic generation technology, i.e., the echo-enabled harmonic generation (EEHG) scheme, in a diffraction-limited storage ring (DLSR). Two different EEHG element layouts are considered, and the effect of the EEHG process on the electron beam quality is also analyzed. Studies suggest that soft X-ray pulses, with pulse lengths of a few femtoseconds and peak powers of up to 1 MW, can be generated by using the EEHG scheme, while causing little perturbation to the regular operation of a DLSR.

Carrier-envelope phase controlled isolated attosecond pulses in the nm wavelength range, based on coherent nonlinear Thomson-backscattering

A proposal for a novel source of isolated attosecond XUV—soft x-ray pulses with a well controlled carrier-envelope phase difference (CEP) is presented in the framework of nonlinear Thomson-backscattering. Based on the analytic solution of the Newton–Lorentz equations, the motion of a relativistic electron is calculated explicitly, for head-on collision with an intense fs laser pulse. By using the received formulas, the collective spectrum and the corresponding temporal shape of the radiation emitted by a mono-energetic electron bunch can be easily computed. For certain suitable and realistic parameters, single-cycle isolated pulses of ca. 20 as length are predicted in the XUV—soft x-ray spectral range, including the 2.33–4.37 nm water window. According to our analysis, the generated almost linearly polarized beam is extremely well collimated around the initial velocity of the electron bunch, with considerable intensity and with its CEP locked to that of the fs laser pulse.

Real-time dynamics of Auger wave packets and decays in ultrafast charge migration processes

The Auger decay is a relevant recombination channel during the first few femtoseconds of molecular targets impinged by attosecond XUV or soft X-ray pulses. Including this mechanism in time--dependent simulations of charge--migration processes is a difficult task, and Auger scatterings are often ignored altogether. In this work we present an advance of the current state-of-the-art by putting forward a real--time approach based on nonequilibrium Green's functions suitable for first-principles calculations of molecules with tens of active electrons. To demonstrate the accuracy of the method we report comparisons against accurate grid simulations of one-dimensional systems. We also predict a highly asymmetric profile of the Auger wavepacket, with a long tail exhibiting ripples temporally spaced by the inverse of the Auger energy.

Complete reconstruction of ultra-broadband isolated attosecond pulses including partial averaging over the angular distribution.

Attosecond streaking is a powerful tool to investigate ultrafast electron dynamics on the attosecond time scale. To obtain the highest temporal resolution in a pump-probe experiment, soft-X-ray (SXR) and infrared (IR) pulses have to be carefully characterized. Here, we present a detailed description of our recent generalization of the Volkov-transform generalized projection algorithm (VTGPA) and its application to multiple overlapping photoelectron bands. This method allows for the complete temporal reconstruction of both IR and SXR pulses under the inclusion of accurate complex photoionization matrix elements (PMEs). In this article, we compare the performance of our new method with traditional algorithms. We particularly focus on the important role played by the photoelectron angular distribution (PAD) which needs to be taken into account for the highest fidelity of attosecond pulse reconstruction. For this purpose, we investigate numerically the influence of the finite collection angle of the electron spectrometer on the retrieval and the obtained pulse parameters. We further theoretically demonstrate the reliability of the reconstruction for pulse durations even shorter than the atomic unit of time.

Two-photon absorption of soft X-ray free electron laser radiation by graphite near the carbon K-absorption edge

We have examined the transmission of soft X-ray pulses from the FERMI free electron laser through carbon films of varying thickness, quantifying nonlinear effects of pulses above and below the carbon K-edge. At typical of soft X-ray free electron laser intensities, pulses exhibit linear absorption at photon energies above and below the K-edge, ∼308 and ∼260 eV, respectively; whereas two-photon absorption becomes significant slightly below the K-edge, ∼284.2 eV. The measured two-photon absorption cross section at 284.18 eV (∼6 × 10−48 cm4 s) is 7 orders of magnitude above what is expected from a simple theory based on hydrogen-like atoms – a result of resonance effects.

Dispersive soft x-ray absorption fine-structure spectroscopy in graphite with an attosecond pulse

Phase transitions of solids and structural transformations of molecules are canonical examples of important photo-induced processes, whose underlying mechanisms largely elude our comprehension due to our inability to correlate electronic excitation with atomic position in real time. Here, we present a decisive step towards such new methodology based on water-window-covering (284 eV to 543 eV) attosecond soft X-ray pulses that can simultaneously access electronic and lattice parameters via dispersive X-ray absorption fine-structure (XAFS) spectroscopy. We validate attoXAFS with an identification of the {\sigma}* and {\pi}* orbital contributions to the density of states in graphite simultaneously with its lattice's four characteristic bonding distances. This work demonstrates the concept of attoXAFS as a powerful real-time investigative tool which is equally applicable to gas-, liquid- and condensed phase.

Laser-plasma interactions in magnetized environment

Propagation and scattering of lasers present new phenomena and applications when the plasma medium becomes strongly magnetized. With mega-Gauss magnetic fields, scattering of optical lasers already becomes manifestly anisotropic. Special angles exist where coherent laser scattering is either enhanced or suppressed, as we demonstrate using a cold-fluid model. Consequently, by aiming laser beams at special angles, one may be able to optimize laser-plasma coupling in magnetized implosion experiments. In addition, magnetized scattering can be exploited to improve the performance of plasma-based laser pulse amplifiers. Using the magnetic field as an extra control variable, it is possible to produce optical pulses of higher intensity, as well as compress UV and soft x-ray pulses beyond the reach of other methods. In even stronger giga-Gauss magnetic fields, laser-plasma interaction enters a relativistic-quantum regime. Using quantum electrodynamics, we compute a modified wave dispersion relation, which enables correct interpretation of Faraday rotation measurements of strong magnetic fields.

Study of Plasma Flow Modes in Imploding Nested Arrays

Results from experimental studies of implosion of nested wire and fiber arrays at currents of up to 4 МА at the Angara-5-1 facility are presented. Depending on the ratio between the radii of the inner and outer arrays, different modes of the plasma flow in the space between the inner and outer arrays were implemented: the sub-Alfvenic (V r V А ) modes and a mode with the formation of the transition shock wave (SW) region between the cascades. By varying the material of the outer array (tungsten wires or kapron fibers), it is shown that the plasma flow mode between the inner and outer arrays depends on the ratio between the plasma production rates ṁin /ṁout in the inner and outer arrays. The obtained experimental results are compared with the results of one-dimensional MHD simulation of the plasma flow between the arrays. Stable implosion of the inner array plasma was observed in experiments with combined nested arrays consisting of a fiber outer array and a tungsten inner array. The growth rates of magnetic Rayleigh−Taylor (MRT) instability in the inner array plasma at different numbers of fibers in the outer array and different ratios between the radii of the inner and outer arrays are compared. Suppression of MRT instability during the implosion of the inner array plasma results in the formation of a stable compact Z-pinch and generation of a soft X-ray pulse. A possible scenario of interaction between the plasmas of the inner and outer arrays is offered. The stability of the inner array plasma in the stage of final compression depends on the character of interaction of plasma jets from the outer array with the magnetic field of the inner array.

Soft X-Ray Second Harmonic Generation as an Interfacial Probe.

Nonlinear optical processes at soft x-ray wavelengths have remained largely unexplored due to the lack of available light sources with the requisite intensity and coherence. Here we report the observation of soft x-ray second harmonic generation near the carbon K edge (∼284 eV) in graphite thin films generated by high intensity, coherent soft x-ray pulses at the FERMI free electron laser. Our experimental results and accompanying first-principles theoretical analysis highlight the effect of resonant enhancement above the carbon K edge and show the technique to be interfacially sensitive in a centrosymmetric sample with second harmonic intensity arising primarily from the first atomic layer at the open surface. This technique and the associated theoretical framework demonstrate the ability to selectively probe interfaces, including those that are buried, with elemental specificity, providing a new tool for a range of scientific problems.

X-ray diagnostics of plasma generated during collisions of plasma flows

Diagnostics of the high-temperature plasma formed during plasma flow collisions by comparing observable intensities of various x-ray spectral lines to accurate kinetic calculation results is discussed. Kinetic calculations have shown that using the resonance line intensity ratio of He-like Ne IX and 3p–2s Li-like Ne VIII is the most convenient way to measure neon-containing plasma temperatures. Experimental research results of the pulse soft (0.1–1 keV) x-ray source with a total energy up to 50 kJ are shown. The radiation pulse is generated during a head-on collision of two low-temperature plasma flows immersed in a longitudinal magnetic field. The plasma flows with the velocities up to 4 × 107 cm/s and total energy up to 200 kJ are formed by a coaxial accelerator operating in pulse gas puffing mode. Neon was used as an inflating gas. Electron temperature for a plasma containing Ne ions is about 160–170 eV. Electron density around the collision region is in the range 1016–1017 cm−3.