Soft X-ray Pulses Research Articles

The soft X-ray and XUV split-and-delay unit at beamlines FL23/24 at FLASH2.

A split-and-delay unit for the extreme ultraviolet and soft X-ray spectral regions has been built which enables time-resolved experiments at beamlines FL23 and FL24 at the Free-electron LASer in Hamburg (FLASH). Geometric wavefront splitting at a sharp edge of a beam splitting mirror is applied to split the incoming soft X-ray pulse into two beams. Ni and Pt coatings at grazing incidence angles have been chosen in order to cover the whole spectral range of FLASH2 and beyond, up to hν = 1800 eV. In the variable beam path with a grazing incidence angle of ϑd = 1.8°, the total transmission (T) ranges are of the order of 0.48 < T < 0.84 for hν < 100 eV and T > 0.50 for 100 eV < hν < 650 eV with the Ni coating, and T > 0.06 for hν < 1800 eV for the Pt coating. For a fixed beam path with a grazing incidence angle of ϑf = 1.3°, a transmission of T > 0.61 with the Ni coating and T > 0.23 with a Pt coating is achieved. Soft X-ray pump/soft X-ray probe experiments are possible within a delay range of -5 ps < Δt < +18 ps with a nominal time resolution of tr = 66 as and a measured timing jitter of tj = 121 ± 2 as. First experiments with the split-and-delay unit determined the averaged coherence time of FLASH2 to be τc = 1.75 fs at λ = 8 nm, measured at a purposely reduced coherence of the free-electron laser.

Ultrafast X-ray Spectroscopy of Intersystem Crossing in Hexafluoroacetylacetone: Chromophore Photophysics and Spectral Changes in the Face of Electron-Withdrawing Groups.

Intersystem crossings between singlet and triplet states represent a crucial relaxation pathway in photochemical processes. Herein, we probe the intersystem crossing in hexafluoro-acetylacetone with ultrafast X-ray transient absorption spectroscopy at the carbon K-edge. We observe the excited state dynamics following excitation with 266 nm UV light to the 1ππ* (S2) state with element and site-specificity using a broadband soft X-ray pulse produced by high harmonic generation. These results are compared to X-ray spectra computed from orbital optimized density functional theory methods. It is found that the electron-withdrawing fluorine atoms decongest the X-ray absorption spectrum by enhancing separation between features originating from different carbon atoms. This facilitates the elucidation of structural and electronic dynamics at the chromophore. The evolution of the core-to-valence resonances at the carbon K-edge reveals an ultrafast population transfer between the 1nπ* (S1) and 3ππ* (T1) states on a 1.6 ± 0.4 ps time scale, which is similar to the 1.5 ps time scale earlier observed for acetylacetone [ J. Am. Chem. Soc. 2017, 139, 16576-16583, DOI: 10.1021/jacs.7b07532]. It therefore appears that terminal fluorination has little influence on the intersystem crossing rate of the acetylacetone chromophore. In addition, the significant role of hydrogen-bond opened and twisted rotational isomers is elucidated in the excited state dynamics by comparison of the experimental transient X-ray spectra with theory.

Optical beat notes assisted attosecond soft X-ray pulse generation in high-gain free electron lasers

Abstract Attosecond soft X-ray pulses are of great importance for the study of ultrafast electronic phenomena. In this paper, a feasible method is proposed to generate isolated fully coherent attosecond soft X-ray free electron laser via optical frequency beating. Two optical lasers with the opposite frequency chirps are used to induce a gradient frequency energy modulation, which helps to generate a gradually varied spacing electron pulse train. Subsequently, the undulator sections with electron beam delay lines are used to amplify the target ultra-short radiation. Numerical start-to-end simulations have been performed and the results demonstrate that an isolated soft X-ray pulse with the peak power of 330 GW and pulse duration of 620 as can be achieved by the proposed technique.

Sensitivity of EEHG simulations to dynamic beam parameters

Currently, the Free electron laser user facility FLASH at DESY is undergoing a significant upgrade involving the complete transformation of one of its beamlines to allow external seeding. With the Echo-Enabled Harmonic Generation (EEHG) seeding method, we aim for the generation of fully coherent XUV and soft X-ray pulses at wavelengths down to 4 nm. The generated FEL radiation is sensitive to various electron beam properties, e.g., its energy profile imprinted either deliberately or by collective effects such as Coherent Synchrotron Radiation (CSR). In dedicated particle tracking simulations, one usually makes certain assumptions concerning the beam properties and the collective effects to simplify implementation and analysis. Here, we estimate the influence of some of the common assumptions made in EEHG simulations on the properties of the output FEL radiation, using the example of FLASH and its proposed seeding beamline. We conclude that the inherent properties of the FLASH1 beam, namely the negatively chirped energy profile, has dominant effect on the spectral intensity profile of the radiators output compare to that of the CSR induced chirp.

Tracking the surface atomic motion in a coherent phonon oscillation

X-ray photoelectron diffraction is a powerful tool for determining the structure of clean and adsorbate-covered surfaces. Extending the technique into the ultrafast time domain will open the door to studies as diverse as the direct determination of the electron-phonon coupling strength in solids and the mapping of atomic motion in surface chemical reactions. Here we demonstrate time-resolved photoelectron diffraction using ultrashort soft x-ray pulses from the free electron laser FLASH. We collect Se $3d$ photoelectron diffraction patterns over a wide angular range from optically excited $\mathrm{Bi}{}_{2}\mathrm{Se}{}_{3}$ with a time resolution of 140 fs. Combining these with multiple scattering simulations allows us to track the motion of near-surface atoms within the first 3 ps after triggering a coherent vibration of the ${A}_{1g}$ optical phonons. Using a fluence of $4.2\phantom{\rule{0.28em}{0ex}}\mathrm{mJ}/{\mathrm{cm}}^{2}$ from a 1.55 eV pump laser, we find the resulting coherent vibrational amplitude in the first two interlayer spacings to be on the order of 0.01 \AA{}.

Resonant double-core excitations with ultrafast, intense X-ray pulses

Intense few-to-sub-femtosecond soft X-ray pulses can produce neutral, two-site excited double-core-hole states by promoting two core electrons to the same unoccupied molecular orbital. We theoretically investigate double nitrogen K-edge excitations of nitrous oxide (N 2 O) with multiconfigurational electronic structure calculations. We show that the second core-excitation energy is reduced with respect to its ground state value. A site-selective double core-excitation mechanism using intense few-femtosecond x-rays is investigated using time-dependent Schrödinger equation (TDSE) simulations. The subsequent two-step Auger–Meitner and two-electrons-one-electron decay spectra of the double core-excited states are analysed using a Mulliken population analysis of the multiconfirational wavefunctions. The change in the electron emission lineshape between the absorption of 1 or 2 photons in the resonant core-excitation is predicted by combining this approach with the TDSE simulations. We examine the possibility of resolving the double core-excited states with X-ray pump-probe techniques by calculating the chemical shifts of the core-electron binding energy of the core-excited states and decay products.

Isolated attosecond X-ray pulses from superradiant thomson scattering by a relativistic chirped electron mirror

Time-resolved investigation of electron dynamics relies on the generation of isolated attosecond pulses in the (soft) X-ray regime. Thomson scattering is a source of high energy radiation of increasing prevalence in modern labs, complementing large scale facilities like undulators and X-ray free electron lasers. We propose a scheme to generate isolated attosecond X-ray pulses based on Thomson scattering by colliding microbunched electrons on a chirped laser pulse. The electrons collectively act as a relativistic chirped mirror, which superradiantly reflects the laser pulse into a single localized beat. As such, this technique extends chirped pulse compression, developed for radar and applied in optics, to the X-ray regime. In this paper we theoretically show that, by using this approach, attosecond soft X-ray pulses with GW peak power can be generated from pC electron bunches at tens of MeV electron beam energy. While we propose the generation of few cycle X-ray pulses on a table-top system, the theory is universally scalable over the electromagnetic spectrum.

Time-resolved resonant soft X-ray scattering combined with MHz synchrotron X-ray and laser pulses at the Photon Factory.

A picosecond pump-probe resonant soft X-ray scattering measurement system has been developed at the Photon Factory storage ring for highly efficient data collection. A high-repetition-rate high-power compact laser system has been installed to improve efficiency via flexible data acquisition to a sub-MHz frequency in time-resolved experiments. Data are acquired by gating the signal of a channel electron multiplier with a pulse-counting mode capable of discriminating single-bunch soft X-ray pulses in the dark gap of the hybrid operation mode in the storage ring. The photoinduced dynamics of magnetic order for multiferroic manganite SmMn2O5 are clearly demonstrated by the detection of transient changes in the resonant soft X-ray scattering intensity around the Mn LIII- and O K-edges.

Saturable Absorption of Free-Electron Laser Radiation by Graphite near the Carbon K-Edge.

The interaction of intense light with matter gives rise to competing nonlinear responses that can dynamically change material properties. Prominent examples are saturable absorption (SA) and two-photon absorption (TPA), which dynamically increase and decrease the transmission of a sample depending on pulse intensity, respectively. The availability of intense soft X-ray pulses from free-electron lasers (FELs) has led to observations of SA and TPA in separate experiments, leaving open questions about the possible interplay between and relative strength of the two phenomena. Here, we systematically study both phenomena in one experiment by exposing graphite films to soft X-ray FEL pulses of varying intensity. By applying real-time electronic structure calculations, we find that for lower intensities the nonlinear contribution to the absorption is dominated by SA attributed to ground-state depletion; our model suggests that TPA becomes more dominant for larger intensities (>1014 W/cm2). Our results demonstrate an approach of general utility for interpreting FEL spectroscopies.

Coherent and ultrashort soft x-ray pulses from echo-enabled harmonic cascade free-electron lasers

It is a long-standing challenge for laser technologies to generate intense fully coherent pulses in the x-ray regime. Here, we demonstrate an external seeding mechanism, termed echo-enabled harmonic cascade (EEHC) for generating coherent and ultrashort soft x-ray pulses. The mechanism uses echo-enabled harmonic generation as the first stage, producing intense extreme ultraviolet pulses that seed the second stage x-ray free-electron laser (FEL) with the high-gain harmonic generation setup. Benefiting from the low sensitivity to electron-beam imperfections of EEHC, we generated high-power nearly transform-limited soft x-ray pulses. We have also demonstrated a unique feature of EEHC in generating isolated few-femtosecond-long x-ray pulses. The supreme up-frequency conversion efficiency and flexible pulse length control of this EEHC mechanism allow us to exceed the current limitations of seeded FELs while preserving the coherence of the seed. Our results are a step towards fully coherent and ultrashort x-ray lasers and could enable the extension of nonlinear optical techniques to shorter wavelengths.

Atomistic investigation of cavitation and ablation in tantalum foils under irradiation with x-rays approaching 5 keV

The rapid irradiation and heating of matter can lead to material removal via a process known as ablation. While previous investigations have focused on ablation with optical and soft x-ray pulses, the process is not well understood for the high-energy x-rays delivered at current x-ray free electron laser facilities. In this paper, we use hybrid two-temperature model molecular dynamics simulations to determine the damage threshold and dynamics for tantalum foils under irradiation with x-rays in the range 1--5 keV. We report that damage occurs for foils with thickness $\ensuremath{\ge}300$ nm when heated to around 1.25 eV/atom. This damage results from the combined processes of melting and cavitation, finally resulting in the removal of material layers. The predictions of this study, in terms of the cavitation threshold and underlying dynamics, could guide interpretation of experiments as well as applications including development of beamline optics for free-electron lasers. We report consistency between cavitation and ablation behavior in isochoric heating experiments and spall processes in hydrodynamic compression and release experiments, confirming the primary modes of damage are mechanical in nature for the x-ray energies investigated.

Optimization and stability analysis of the cascaded EEHG-HGHG free-electron laser

X-ray free-electron lasers (XFELs) are powerful tools to explore and study nature for achieving remarkable advances. Generally, seeded FELs are ideal sources for supplying fully coherent soft x-ray pulses. Benefiting from the high-frequency up-conversion efficiency, the cascading configuration with echo-enabled harmonic generation (EEHG) and high-gain harmonic generation (HGHG) holds promising prospects for generating fully coherent radiation at 1 nm wavelength. In this paper, we design and optimize EEHG-HGHG configuration using parameters of Shanghai High-Repetition-Rate XFEL and Extreme Light Facility. In addition, we systematically analyze the effect of relative timing jitter on the output FEL performance based on various start-to-end electron beams. The intensive numerical simulations show that the cascaded EEHG-HGHG scheme can achieve 1 nm FEL pulses with peak power up to 15 GW. Further sensitivity analysis indicates that the relative timing jitter between the electron beam and seed laser has a significant impact on the FEL performance. The RMS timing jitter of 3 fs can lead to the final output pulse energy fluctuations of 29%.

Direct observation of ultrafast exciton localization in an organic semiconductor with soft X-ray transient absorption spectroscopy

The localization dynamics of excitons in organic semiconductors influence the efficiency of charge transfer and separation in these materials. Here we apply time-resolved X-ray absorption spectroscopy to track photoinduced dynamics of a paradigmatic crystalline conjugated polymer: poly(3-hexylthiophene) (P3HT) commonly used in solar cell devices. The π→π* transition, the first step of solar energy conversion, is pumped with a 15 fs optical pulse and the dynamics are probed by an attosecond soft X-ray pulse at the carbon K-edge. We observe X-ray spectroscopic signatures of the initially hot excitonic state, indicating that it is delocalized over multiple polymer chains. This undergoes a rapid evolution on a sub 50 fs timescale which can be directly associated with cooling and localization to form either a localized exciton or polaron pair.

Optimization of echo-enabled harmonic generation toward coherent EUV and soft X-ray free-electron laser at NSLS-II.

Prebunching via echo-enabled harmonic generation (EEHG) is an efficient way to reduce the radiator length and improve the longitudinal coherence as well as output stability in storage-ring-based free-electron lasers. We propose a conceptual design, which uses two straight sections to seed coherent extreme-ultraviolet (EUV) and soft X-ray emission with nearly MHz repetition rate. To take the large energy spread (10−3) of a storage ring into account and utilize the existing bending magnets between the two straight sections as the first chicane, we implement a special modeling tool, named EEHG optimizer. This tool has been successfully applied to maximize the prebunching with a reasonably low energy modulation, thereby generating intense coherent X-ray pulses within a short undulator length (a few meters) limited by the available space of a storage ring. Numerical simulations confirm that the optimized EEHG parameters can be directly applied to generate a 10 MW scale peak power with fully coherent ultrafast EUV to soft X-ray pulses based on the NSLS-II parameters. This method can be easily extended to other types of diffraction-limited storage rings.

An Easy Technique for Focus Characterization and Optimization of XUV and Soft X-ray Pulses

For many applications of extreme ultraviolet (XUV) and X-ray pulses, a small focus size is crucial to reach the required intensity or spatial resolution. In this article, we present a simple way to characterize an XUV focus with a resolution of 1.85 µm. Furthermore, this technique was applied for the measurement and optimization of the focus of an ellipsoidal mirror for photon energies ranging from 18 to 150 eV generated by high-order harmonics. We envisage a broad range of applications of this approach with sub-micrometer resolution from high-harmonic sources via synchrotrons to free-electron lasers.

The time-resolved atomic, molecular and optical science instrument at the Linac Coherent Light Source.

The newly constructed time-resolved atomic, molecular and optical science instrument (TMO) is configured to take full advantage of both linear accelerators at SLAC National Accelerator Laboratory, the copper accelerator operating at a repetition rate of 120 Hz providing high per-pulse energy as well as the superconducting accelerator operating at a repetition rate of about 1 MHz providing high average intensity. Both accelerators power a soft X-ray free-electron laser with the new variable-gap undulator section. With this flexible light source, TMO supports many experimental techniques not previously available at LCLS and will have two X-ray beam focus spots in line. Thereby, TMO supports atomic, molecular and optical, strong-field and nonlinear science and will also host a designated new dynamic reaction microscope with a sub-micrometer X-ray focus spot. The flexible instrument design is optimized for studying ultrafast electronic and molecular phenomena and can take full advantage of the sub-femtosecond soft X-ray pulse generation program.

Magnetic implosion of thin aluminum foil liners

Metal liner implosions driven by a pulsed current generator are used in research on inertial confinement fusion, generation of soft x-ray pulses and megagauss magnetic fields. The energy density in the plasma column formed during the liner stagnation is largely determined by the initial radius and the radial convergence of the liner. When the liner implosion time is close to the current rise time, the liner initial radius is proportional to the current rise time. The paper presents the results of experiments on the fast implosion of cylindrical liners on the MIG generator (2 MA, 80 ns) at the Institute of High Current Electronics, Tomsk, Russia. Liners 0.7–1.0 mm in diameter were made from a 1.8 to 2.5 μm thick aluminum foil. A low-density plasma was pre-injected into the liner area. As the Lorentz force sweeps away the pre-injected plasma, the current switches to the liner in 1–3 ns. Then the liner is imploded in 3–7 ns by a current close to the peak generator current. The stagnation radius measured via time-integrated pinhole camera images was found to be not more than 25 µm. Such a radius of the stagnated plasma assumes that the plasma mass density is several times higher than the solid aluminum density.

Physical Foundations of Subatomic Attosecond Quantum Technologies for Storing Energy in Materials

The article discusses the current development of physical principles of subatomic quantum technologies using ultrashort attosecond energy pulses within the ranges of deep-UV and soft X-ray radiation. It is necessary as a foundation of the process of nondestructive high-capacity reverse energy harvesting using accumulating nanoelectromechanical systems (NEMS) of supra-atomic scale with linear dimensions of 0.1 nm up to 10 nm and subatomic thickness of boundary interfaces up to 0.1 nm. The article compares the physical principles of up-to-date femtosecond quantum technologies and the prospective attosecond quantum technologies. The latter aims to improve the capacity, controllability, and performance efficiency of quantum energy storages by utilizing quantum electronic excitations of hybrid nature. Harder and shorter by one or two orders of magnitude UV and X-ray impulses are required for attosecond energy storages, unlike the femtosecond ones. Quantum femtochemistry describes the reactions caused by optical spectrum radiation pulses. In the case of attosecond pulses, highly excited quantum entangled subatomic electron pairs demonstrate nonlinear energy pulse accumulation effects. Goldstone condensates of bosonic electron pairs produce boundary shells of compact cavities of a quantum-size NEMS resonator. Hybrid electronic excitations of NEMS are a specific feature of the nonlinear quantum subatomic response of materials to attosecond deep-UV and soft X-ray pulses. The attosecond physics of the processes is the basis for the development of new subatomic attosecond quantum technologies for storing energy in materials.

Attosecond coherent electron motion in Auger-Meitner decay.

In quantum systems, coherent superpositions of electronic states evolve on ultrafast time scales (few femtoseconds to attoseconds; 1 attosecond = 0.001 femtoseconds = 10-18 seconds), leading to a time-dependent charge density. Here we performed time-resolved measurements using attosecond soft x-ray pulses produced by a free-electron laser, to track the evolution of a coherent core-hole excitation in nitric oxide. Using an additional circularly polarized infrared laser pulse, we created a clock to time-resolve the electron dynamics and demonstrated control of the coherent electron motion by tuning the photon energy of the x-ray pulse. Core-excited states offer a fundamental test bed for studying coherent electron dynamics in highly excited and strongly correlated matter.

Pulse Peak Migration during the Outburst Decay of the Magnetar SGR 1830-0645: Crustal Motion and Magnetospheric Untwisting

Abstract Magnetars, isolated neutron stars with magnetic-field strengths typically ≳1014 G, exhibit distinctive months-long outburst epochs during which strong evolution of soft X-ray pulse profiles, along with nonthermal magnetospheric emission components, is often observed. Using near-daily NICER observations of the magnetar SGR 1830-0645 during the first 37 days of a recent outburst decay, a pulse peak migration in phase is clearly observed, transforming the pulse shape from an initially triple-peaked to a single-peaked profile. Such peak merging has not been seen before for a magnetar. Our high-resolution phase-resolved spectroscopic analysis reveals no significant evolution of temperature despite the complex initial pulse shape, yet the inferred surface hot spots shrink during peak migration and outburst decay. We suggest two possible origins for this evolution. For internal heating of the surface, tectonic motion of the crust may be its underlying cause. The inferred speed of this crustal motion is ≲100 m day−1, constraining the density of the driving region to ρ ∼ 1010 g cm−3, at a depth of ∼200 m. Alternatively, the hot spots could be heated by particle bombardment from a twisted magnetosphere possessing flux tubes or ropes, somewhat resembling solar coronal loops, that untwist and dissipate on the 30–40 day timescale. The peak migration may then be due to a combination of field-line footpoint motion (necessarily driven by crustal motion) and evolving surface radiation beaming. This novel data set paints a vivid picture of the dynamics associated with magnetar outbursts, yet it also highlights the need for a more generic theoretical picture where magnetosphere and crust are considered in tandem.