Free-electron Laser Pulses Research Articles

X-ray pulse compressors in Laue diffraction geometry

We theoretically investigate the impact of nonlinear dispersion of crystals and multilayers used in Laue-type pulse compressors (LPCs) on chirped x-ray pulse compression, as well as the optimization method for the configuration of LPCs. We also study the application of LPCs to compress chirped x-ray free-electron laser pulses based on the parameters of LCLS-II-HE. The results show that the optimal thickness is half of the Pendellosung period, yielding the best compressor performance with minimal impact from the nonlinear dispersion. This work also provides a new idea for generating ultra-short two-color or multi-color x-ray pulses by considering deviations from the optimized thickness.

Synthesis of microbunching rotation for generating isolated attosecond soft x-ray free-electron laser pulses

Synthesis of microbunching rotation for generating isolated attosecond soft x-ray free-electron laser pulses

Experimental Demonstration of Mode-Coupled and High-Brightness Self-Amplified Spontaneous Emission in an X-Ray Free-Electron Laser.

X-ray free-electron lasers (FELs) are modern research tools with applications in multiple scientific fields. Standard x-ray FEL pulses are produced by the self-amplified spontaneous emission (SASE) mechanism. SASE-FEL pulses have high power, short duration, and excellent transverse coherence but exhibit poor temporal coherence with power and spectral profiles consisting of multiple randomly distributed spikes. Here, we present the demonstration of two modes that enhance the temporal coherence of SASE-FEL radiation: mode-coupled and high-brightness SASE. Both schemes are based on delaying the electron beam with magnetic chicanes placed between the undulator modules of the FEL facility. First, we show the generation of frequency combs with tunable peak separation via the mode-coupled SASE scheme. Second, we present a proof-of-principle demonstration of the high-brightness SASE mechanism, producing FEL pulses with a bandwidth reduction up to a factor of 3 with respect to standard SASE pulses. The demonstration was done at Athos, the soft x-ray beamline of SwissFEL, for photon energies between 500 and 600eV. Our work will benefit current applications and may open up new research areas requiring frequency combs or narrow bandwidths.

Electron-cloud alignment dynamics induced by an intense X-ray free-electron laser pulse: a case study on atomic argon

In an intense X-ray free-electron laser (XFEL) pulse, atoms are sequentially ionised by multiple X-ray photons. Photoionisation generally induces an alignment of the electron cloud of the produced atomic ion regarding its orbital-angular-momentum projections. However, how the alignment evolves during sequential X-ray multi-photon ionisation accompanied by decay processes has been unexplored. Here we present a theoretical prediction of the time evolution of the electron-cloud alignment of argon ions induced by XFEL pulses. To this end, we calculate state-resolved ionisation dynamics of atomic argon interacting with an intense linearly polarised X-ray pulse, which generates ions in a wide range of charge states with non-zero orbital- and spin-angular momenta. Employing time-resolved alignment parameters, we predict the existence of non-trivial alignment dynamics during intense XFEL pulses. This implies that even if initially the atomic electron cloud is perfectly spherically symmetric, X-ray multi-photon ionisation can lead to noticeable reshaping of the electron cloud.

Reduction of arrival time jitter or energy spread with arclike variable bunch compressors

Synchronizing free-electron laser pulses for time-resolved experiments is necessary as an unsynchronized system reduces the effective repetition rate of the experiment. Additionally, free-electron laser longitudinal coherence and spectral brightness are limited by electron beam energy spread. In this paper, a variable bunch compressor design and compression schemes were developed to: reduce klystron-induced arrival time jitter by 85% while preserving peak current and transverse emittance and to minimize electron beam correlated energy spread for potential self-seeding or HB-SASE modes. Published by the American Physical Society 2024

“Beam à la carte”: Laser heater shaping for attosecond pulses in a multiplexed x-ray free-electron laser

Electron beam shaping allows the control of the temporal properties of x-ray free-electron laser pulses from femtosecond to attosecond timescales. Here, we demonstrate the use of a laser heater to shape electron bunches and enable the generation of attosecond x-ray pulses. We demonstrate that this method can be applied in a selective way, shaping a targeted subset of bunches while leaving the remaining bunches unchanged. This experiment enables the delivery of shaped x-ray pulses to multiple undulator beamlines, with pulse properties tailored to specialized scientific applications.

Measurement of temporal evolution of antiferromagnetic domain change in nickel oxide driven by 2TO phonon mode excitation via pump-probe experiment

The temporal evolution of antiferromagnetic domain pattern changes under resonant excitation of the second-order transverse optical phonon mode in nickel oxide was investigated using mid-infrared free electron laser (MIR-FEL) pulses and visible nanosecond probe laser pulses at room temperature. We visualized the domain patterns through magneto-optical polarized microscopy in transmission and observed their temporal variation after the phonon excitation via MIR-FEL. We evaluated the differences throughout the timeline using the structural similarity index measure technique from domain images with and without MIR-FEL irradiation. We found that the MIR-FEL irradiation induces significant structural changes in the domain patterns. The maximum difference was observed at the timing of the MIR-FEL irradiation and exponentially recovered with the time constant of 1.4 ± 0.2 ms. This rather long-time constant could be owing to the spin relaxation, whilst further investigation is needed to confirm the underlying mechanism.

Resonant Raman Auger spectroscopy on transient core-excited Ne ions

Abstract Short-lived core-ionized neon atoms were investigated by measuring under resonant Raman conditions the Auger decay following the excitation of a second core electron into a Rydberg state. Making use of intense and narrow bandwidth x-ray free-electron laser pulses, the photoexcitation spectrum of the femtosecond-lived Ne+1s02s22p6np series was characterized. Energy position and lifetimes of the lower-lying Rydberg states were determined and the final state configurations following the decay of the Ne+1s02s22p63p double-core hole resonance were partially resolved.

Transient absorption of warm dense matter created by an X-ray free-electron laser

Warm dense matter is at the boundary between a plasma and a condensed phase and plays a role in astrophysics, planetary science and inertial confinement fusion research. However, its electronic structure and ionic structure upon irradiation with strong laser pulses remain poorly understood. Here, we use an intense and ultrafast X-ray free-electron laser pulse to simultaneously create and characterize warm dense copper using L-edge X-ray absorption spectroscopy over a large irradiation intensity range. Below a pulse intensity of 1015 W cm−2, an absorption peak below the L edge appears, originating from transient depletion of the 3d band. This peak shifts to lower energy with increasing intensity, indicating the movement of the 3d band upon strong X-ray excitation. At higher intensities, substantial ionization and collisions lead to the transition from reverse saturable absorption to saturable absorption of the X-ray free-electron laser pulse, two nonlinear effects that hold promise for X-ray pulse-shaping. We employ theoretical calculations that combine a model based on kinetic Boltzmann equations with finite-temperature real-space density-functional theory to interpret these observations. The results can be used to benchmark non-equilibrium models of electronic structure in warm dense matter.

Evolution of level population in Ar interacting with XFEL pulses: impact of resonant absorptions

Theoretical exploration of the population dynamics at fine-structure levels of Ar atoms interacting with ultrafast ultraintense x-ray free electron laser (XFEL) pulses is conducted. A time-dependent rate equation based on a detailed-level accounting approach is applied for tracking population levels, encompassing microscopic atomic processes such as photoexcitation, radiative decay, photoionization and Auger decay. A Monte Carlo algorithm is implemented to solve large-scale rate equations efficiently. The primary investigation centers on generating Ar17+ through resonant absorption by the second-harmonic radiation of the x-ray pulse. The calculated population ratios of Ar17+ to Ar16+ align well with the experimental measurements (LaForge et al 2021 Phys. Rev. Lett. 127 213202). In comparison to the transition energy of the strongest line, (1s2)0→(1s1/22p3/2)1 of Ar16+, there is a distinct ∼25 eV red shift in the peak ratio, which is attributed to the presence of intricate resonant channels in the lower ionization stages. The results demonstrate the sensitivity of the population ratio Ar17+/Ar16+ to the laser pulse parameters such as x-ray pulse duration, bandwidth and the contribution of second-harmonic radiation, indicating their potential as diagnostic tools in future experiments.

Design of an aperiodic Cr/C reflective multilayer quarter-wave plate at the carbon K-edge

An aperiodic Cr/C reflective multilayer quarter-wave plate is designed and optimized at the carbon K-edge, by implementing both the genetic algorithm (GA) and the non-dominated sorting genetic algorithm II (NSGA-II). The performance is demonstrated using test free electron laser (FEL) pulses simulated by GENESIS to convert the imperfect linearly polarized light to circular polarization; the characteristics are verified by a numerical analysis of the Stokes parameter of the FEL pulses before and after penetration through the multilayer.

Transmissions of an x-ray free electron laser pulse through Al: Influence of nonequilibrium electron kinetics.

A theoretical model for investigating the radiative transfer of an x-ray free electron laser (XFEL) pulse is developed based on a one-dimensional radiative transfer equation. The population dynamics of energy levels is obtained by rate equationapproximation coupling with the Fokker-Planck equation, in which the electron energy distribution function (EEDF) is self-consistently determined. As an illustrative example, XFEL pulse propagation through a solid-density aluminum (Al) is investigated. The characteristics of the temporal evolution of the x-ray pulse shape, level population, and EEDF are demonstrated. The EEDF usually has two parts in XFEL-Al interactions: the near equilibrium part in the lower energy regions and the nonequilibrium part in the higher energy region. The deep gap between the two parts is quickly filled in the solid-density Al plasma. The pulse shape is distorted and the duration shortens as the x-ray pulse propagates through the Al sample. The x-ray transmission spectra were compared with experimental and other theoretical results, and good agreement was found. There are slight discrepancies between the transmission obtained by solving the Fokker-Planck equationand Maxwellian assumptions because nonequilibrium electrons in the higher energy region account for only a small fraction of the total electrons.

Impact of MoS2 Monolayers on the Thermoelastic Response of Silicon Heterostructures.

Understanding the thermoelastic response of a nanostructure is crucial for the choice of materials and interfaces in electronic devices with improved and tailored transport properties at the nanoscale. Here, we show how the deposition of a MoS2 monolayer can strongly modify the nanoscale thermoelastic dynamics of silicon substrates close to their interface. We demonstrate this by creating a transient grating with extreme ultraviolet light, using ultrashort free-electron laser pulses, whose ≈84 nm period is comparable to the size of elements typically used in nanodevices, such as electric contacts and nanowires. The thermoelastic response, featuring coherent acoustic waves and incoherent relaxation, is tangibly modified by the presence of monolayer MoS2. Namely, we observed a major reduction of the amplitude of the surface mode, which is almost suppressed, while the longitudinal mode is basically unperturbed, aside from a faster decay of the acoustic modulations. We interpret this behavior as a selective modification of the surface elasticity, and we discuss the conditions to observe such effect, which may be of immediate relevance for the design of Si-based nanoscale devices.

Sub-photon accuracy noise reduction of a single shot coherent diffraction pattern with an atomic model trained autoencoder

Single-shot imaging with femtosecond X-ray lasers is a powerful measurement technique that can achieve both high spatial and temporal resolution. However, its accuracy has been severely limited by the difficulty of applying conventional noise-reduction processing. This study uses deep learning to validate noise reduction techniques, with autoencoders serving as the learning model. Focusing on the diffraction patterns of nanoparticles, we simulated a large dataset treating the nanoparticles as composed of many independent atoms. Three neural network architectures are investigated: neural network, convolutional neural network and U-net, with U-net showing superior performance in noise reduction and subphoton reproduction. We also extended our models to apply to diffraction patterns of particle shapes different from those in the simulated data. We then applied the U-net model to a coherent diffractive imaging study, wherein a nanoparticle in a microfluidic device is exposed to a single X-ray free-electron laser pulse. After noise reduction, the reconstructed nanoparticle image improved significantly even though the nanoparticle shape was different from the training data, highlighting the importance of transfer learning.

Ultra-high harmonic conversion of a seeded free-electron laser via harmonic optical klystron

External seeded free-electron lasers (FELs) are compelling tools for generating fully coherent EUV and soft x-ray radiations. Echo-enabled harmonic generation (EEHG), the most typical representative of external seeded FELs, has witnessed a remarkable growth of fully coherent FELs in the last decade, continuously evolving towards higher harmonic conversions and shorter wavelengths. Ultra-high harmonic generation is imperative in the field of FELs. This paper presents a novel method for generating FEL radiation with ultra-high harmonic conversion, utilizing harmonic optical klystron in combination with EEHG. This method can effectively increase the harmonic conversion order to about 90. Theoretical analysis and numerical simulations show that intense and almost fully coherent FEL pulses can be generated with a wavelength of 3 nm. At the same time, the seed laser intensity required by this scheme is lower compared to nominal EEHG, thus facilitating the generation of high-repetition-rate seeded FELs.

Extreme focusing of hard X-ray free-electron laser pulses enables 7 nm focus width and 1022 W cm−2 intensity

Extreme focusing of hard X-ray free-electron laser pulses enables 7 nm focus width and 1022 W cm−2 intensity

Wave packet dynamics and control in excited states of molecular nitrogen.

Wave packet interferometry with vacuum ultraviolet light has been used to probe a complex region of the electronic spectrum of molecular nitrogen, N2. Wave packets of Rydberg and valence states were excited by using double pulses of vacuum ultraviolet (VUV), free-electron-laser (FEL) light. These wave packets were composed of contributions from multiple electronic states with a moderate principal quantum number (n ∼ 4-9) and a range of vibrational and rotational quantum numbers. The phase relationship of the two FEL pulses varied in time, but as demonstrated previously, a shot-by-shot analysis allows the spectra to be sorted according to the phase between the two pulses. The wave packets were probed by angle-resolved photoionization using an infrared pulse with a variable delay after the pair of excitation pulses. The photoelectron branching fractions and angular distributions display oscillations that depend on both the time delays and the relative phases of the VUV pulses. The combination of frequency, time delay, and phase selection provides significant control over the ionization process and ultimately improves the ability to analyze and assign complex molecular spectra.

X-ray-induced atomic transitions via machine learning: A computational investigation

Intense x-ray free-electron laser pulses can induce multiple sequences of one-photon ionization and accompanying decay processes in atoms, producing highly charged atomic ions. Considering individual quantum states during these processes provides more precise information about the x-ray multiphoton ionization dynamics than the common configuration-based approach. However, in such a state-resolved approach, extremely huge-sized rate-equation calculations are inevitable. Here we present a strategy that embeds machine-learning models into a framework for atomic state-resolved ionization dynamics calculations. Machine learning is employed for the required atomic transition parameters, whose calculations possess the computationally most expensive steps. We find for argon that both feedforward neural networks and random forest regressors can predict these parameters with acceptable, but limited accuracy. State-resolved ionization dynamics of argon, in terms of charge-state distributions and electron and photon spectra, are also presented. Comparing fully calculated and machine-learning-based results, we demonstrate that the proposed machine-learning strategy works in principle and that the performance, in terms of charge-state distributions and electron and photon spectra, is good. Our work establishes a first step toward accelerating the calculation of atomic state-resolved ionization dynamics induced by high-intensity x rays. Published by the American Physical Society 2024

Transient X-Ray Absorption Near Edge Structure Spectroscopy Using Broadband Free-Electron Laser Pulses.

A new method for time-resolved X-ray absorption near edge structure (XANES) spectroscopy that enables faster data acquisition and requires smaller sample quantities for high-quality data, thus allowing the analysis of more samples in a shorter time is introduced. The method uses large bandwidth free electron laser pulses to measure laser-excited XANES spectra in transmission mode. A beam-splitting grating configuration allows simultaneous measurements of the spectra of the incoming X-ray Free Electron Laser (XFEL) pulses and transmission XANES, which is crucial for compensating the pulse-dependent intensity and spectrum fluctuations due to the self-amplified spontaneous emission operation. The implementation of this new methodology is applied on a liquid solution of ammonium iron(III) oxalate jet and is compared to previous results, showing great improvements in the speed of acquisition and spectral resolution, and the ability to measure a large 2-D spectral-time map quickly.

The collapse of a sonoluminescent cavitation bubble imaged with X-ray free-electron laser pulses

Single bubble sonoluminescence (SBSL) is the phenomenon of synchronous light emission due to the violent collapse of a single spherical bubble in a liquid, driven by an ultrasonic field. During the bubble collapse, matter inside the bubble reaches extreme conditions of several gigapascals and temperatures on the order of 10000 K, leading to picosecond flashes of visible light. To this day, details regarding the energy focusing mechanism rely on simulations due to the fast dynamics of the bubble collapse and spatial scales below the optical resolution limit. In this work we present phase-contrast holographic imaging with single x-ray free-electron laser (XFEL) pulses of a SBSL cavitation bubble in water. X-rays probe the electron density structure and by that provide a uniquely new view on the bubble interior and its collapse dynamics. The involved fast time-scales are accessed by sub-100 fs XFEL pulses and a custom synchronization scheme for the bubble oscillator. We find that during the whole oscillation cycle the bubble’s density profile can be well described by a simple step-like structure, with the radius R following the dynamics of the Gilmore model. The quantitatively measured internal density and width of the boundary layer exhibit a large variance. Smallest reconstructed bubble sizes reach down to R≃0.8μm , and are consistent with spherical symmetry. While we here achieved a spatial resolution of a few 100 nm, the visibility of the bubble and its internal structure is limited by the total x-ray phase shift which can be scaled with experimental parameters.