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The possibility of using a parabolic refractive lens with initial X-ray free-electron laser (XFEL) pulses, i.e. without a monochromator, is analysed. It is assumed that the measurement time is longer than 0.3 fs, which is the time duration of a coherent pulse (spike). In this case one has to calculate the propagation of a monochromatic wave and then perform an integration of the intensity over the radiation spectrum. Here a general algorithm for calculating the propagation of time-dependent radiation in free space and through various objects is presented. Analytical formulae are derived describing the properties of the monochromatic beam focused by a system of one and two lenses. Computer simulations show that the European XFEL pulses can be focused with maximal efficiency, i.e. as for a monochromatic wave. This occurs even for nanofocusing lenses.

DNA-Origami-Assisted Flow-Aligned Single-Particle Diffractive Imaging using XFEL Pulses

Start-End Simulations for the LCLS X-Ray Free-Electron Laser

Short wavelength FELs using the SLAC linac

The X-ray free-electron laser (XFEL) based on self amplified spontaneous emission (SASE) is an unprecedented coherent hard X-ray source [1,2]. However, due to its huge size and construction cost, it would not be easy to have this magnificent scientific facility in your neighborhood. Therefore, there have been studies on why it must be so big (why its electron beam energy must be so high and why its undulator is so long) and how its size can be reduced (how its electron energy can be lowered) without degrading radiation quality [3, 4]. Size reduction of a XFEL machine is basically reduced to how a lower energy electron beam can generate a XFEL without degrading the radiation quality. The reason a high energy electron beam is needed is that a very small electron beam emittance is needed for lasing as the relation = n/γ indicates. Here, is the electron beam emittance, n is the gun emittance, and γ is the relativistic factor. Hence, if n is low enough, a lower electron energy can make the same . A compact XFEL without its quality being degraded obviously means a XFEL with high FEL efficiency. A FEL’s efficiency can be roughly estimated by using the FEL parameter ρ. We can make ρ high enough, even at a low electron beam energy, by using a low emittance gun as explained above. Therefore, the issue is reduced to developing an electron gun with improved gun emittance. The emittance performance of the photo-cathode gun was widely known to be around 1−1.2 μrad, and the design of Linac Coherent Light Source (LCLS) was based on this number [5]. However, in the recent LCLS com-

The Stanford Linear Accelerator Center (SLAC), in collaboration with Los Alamos National Laboratory, Lawrence Livermore National Laboratory, and the University of California at Los Angeles, is proposing to build a Free-Electron-Laser (FEL) R and D facility operating in the self-amplified spontaneous emission (SASE) mode in the wavelength range 1.5--15 {angstrom}. This FEL, called Linac Coherent Light Source (LCLS), utilizes the SLAC linac and produces sub-picosecond pulses of short wavelength x-rays with very high peak brightness and full transverse coherence. In this report, the Design Team has established performance parameters for all the major components of the LCLS and developed a layout of the entire system. Chapter 1 is the Executive Summary. Chapter 2 (Overview) provides a brief description of each of the major sections of the LCLS, from the rf photocathode gun, through the experimental stations and electron beam dump. Chapter 3 describes the scientific case for the LCLS. Chapter 4 provides a review of the principles of the FEL physics that the LCLS is based on, and Chapter 5 discusses the choice of the system's physical parameters. Chapters 6 through 10 describe in detail each major element of the system. Chapters 11 through 13 respectively cover undulator controls, mechanical alignment, and radiation issues.

A compact and robust diagnostic to determine spatial and temporal overlap between X-ray free-electron laser and optical laser pulses was developed and evaluated using monochromatic X-rays from the Linac Coherent Light Source. It was used to determine temporal overlap with a resolution of ∼10 fs, despite the large pulse energy fluctuations of the monochromatic X-ray pulses, and covers a wide optical wavelength range from ultraviolet to near-infrared with a single configuration.

Harmonic lasing in a free electron laser with a planar undulator (under the condition that the fundamental frequency is suppressed) might be a cheap and efficient way of extension of wavelength ranges of existing and planned x-ray free electron laser (FEL) facilities. Contrary to nonlinear harmonic generation, harmonic lasing can provide much more intense, stable, and narrow-band FEL beam which is easier to handle due to the suppressed fundamental frequency. In this paper we perform a parametrization of the solution of the eigenvalue equation for lasing at odd harmonics, and present an explicit expression for FEL gain length, taking into account all essential effects. We propose and discuss methods for suppression of the fundamental harmonic. We also suggest a combined use of harmonic lasing and lasing at the retuned fundamental wavelength in order to reduce bandwidth and to increase brilliance of x-ray beam at saturation. Considering 3rd harmonic lasing as a practical example, we come to the conclusion that it is much more robust than usually thought, and can be widely used in the existing or planned x-ray FEL (XFEL) facilities. In particular, Linac Coherent Light Source (LCLS) after a minor modification can lase to saturation at the 3rd harmonic up to the photon energy of 25--30 keV providing multigigawatt power level and narrow bandwidth. As for the European XFEL, harmonic lasing would allow one to extend operating range (ultimately up to 100 keV), to reduce FEL bandwidth and to increase brilliance, to enable two-color operation for pump-probe experiments, and to provide more flexible operation at different electron energies. Similar improvements can be realized in other x-ray FEL facilities with gap-tunable undulators like FLASH II, SACLA, LCLS II, etc. Harmonic lasing can be an attractive option for compact x-ray FELs (driven by electron beams with a relatively low energy), allowing the use of the standard undulator technology instead of small-gap in-vacuum devices. Finally, in this paper we discover that in a part of the parameter space, corresponding to the operating range of soft x-ray beam lines of x-ray FEL facilities (like SASE3 beam line of the European XFEL), harmonics can grow faster than the fundamental wavelength. This feature can be used in some experiments, but might also be an unwanted phenomenon, and we discuss possible measures to diminish it.

Atomic adsorption of Au and Pt on the rutile (1 1 0) surface was investigated by atomic-resolution aberration-corrected scanning transmission electron microscopy (STEM) measurements combined with density functional theory calculations. Au single atoms were deposited on the surface in a vacuum condition, and the observed results were compared with Pt single atoms on the same surface prepared by the same experimental manner. It was found that Au single atoms are stably adsorbed only at the bridging oxygen vacancy sites, which is quite different from Pt single atoms exhibiting the most frequently observed adsorption at the basal oxygen vacancy sites. Such a difference in oxygen-vacancy effect between Au and Pt can be explained by electronic structures of the surface vacancies as well as characters of outermost atomic orbitals of Au and Pt.

We present an extended MonteCarlo rate equation approach to examine the inner-shell ionization dynamics of atoms in an intense x-ray free-electron laser (XFEL) pulse. In addition to photoionization, Auger decay, and fluorescence processes, we include bound-to-bound transitions in the rate equation calculations. Using an efficient computational scheme, we account for "hidden resonances" unveiled during the course of an XFEL pulse. For Ar, the number of possible electron configurations is increased ten-billion-fold over that required under nonresonant conditions. We investigated the complex ionization dynamics of Ar atoms exposed to an 480-eV XFEL pulse, where production of ions above charge state 10+ is not allowed via direct one-photon ionization. We found that resonance-enhanced x-ray multiple ionization pathways play a dominant role in producing these nominally inaccessible charge states. Our calculated results agree with the measured Ar ion yield and pulse-duration dependence. We also predict the surprising ion yields reported earlier for Kr and Xe. The Monte Carlo rate equation method enables theoretical exploration of the complex dynamics of resonant high-intensity x-ray processes.

We present the implementation of an electronic-structure approach dedicated to ionization dynamics of molecules interacting with x-ray free-electron laser (XFEL) pulses. In our scheme, molecular orbitals for molecular core-hole states are represented by linear combination of numerical atomic orbitals that are solutions of corresponding atomic core-hole states. We demonstrate that our scheme efficiently calculates all possible multiple-hole configurations of molecules formed during XFEL pulses. The present method is suitable to investigate x-ray multiphoton multiple ionization dynamics and accompanying nuclear dynamics, providing essential information on the chemical dynamics relevant for high-intensity x-ray imaging.

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.

X-ray analysis is one of the most robust approaches to extract quantitative information from various materials and is widely used in various fields ever since Raimond Castaing established procedures to analyze electron-induced X-ray signals for materials characterization '70 years ago'. The recent development of aberration-correction technology in a (scanning) transmission electron microscopes (S/TEMs) offers refined electron probes below the Å level, making atomic-resolution X-ray analysis possible. In addition, the latest silicon drift detectors allow complex detector arrangements and new configurational designs to maximize the collection efficiency of X-ray signals, which make it feasible to acquire X-ray signals from single atoms. In this review paper, recent progress and advantages related to S/TEM-based X-ray analysis will be discussed: (i) progress in quantification for materials characterization including the recent applications to light element analysis, (ii) progress in analytical spatial resolution for atomic-resolution analysis and (iii) progress in analytical sensitivity toward single-atom detection and analysis in materials. Both atomic-resolution analysis and single-atom analysis are evaluated theoretically through multislice-based calculation for electron propagation in oriented crystalline specimen in combination with X-ray spectrum simulation.

X-ray free electron laser (FEL) machines like the Linac Coherent Light Source (LCLS) at SLAC require high-quality electron beams to generate X-ray lasers for various experiments. Digital low-level RF (LLRF) systems are widely used to control the high-power RF klystrons to provide a highly stable RF field in accelerator structures for beam acceleration. Feedback and feedforward controllers are implemented in LLRF systems to stabilize or adjust the phase and amplitude of the RF field. To achieve the RF stability and the accuracy of the phase and amplitude adjustment, low-noise and highly linear RF actuators are required. Aiming for the upgrade of the $S$ -band Linac at SLAC, an RF actuator is designed with an ${\hbox{I/Q}}$ modulator driven by two digital-to-analog converters (DAC) for the digital LLRF systems. A direct upconversion scheme is selected for RF actuation, and an on-line calibration algorithm is developed to compensate the RF reference leakage and the imbalance errors in the ${\hbox{I/Q}}$ modulator, which may cause significant phase and amplitude actuation errors. This paper presents the requirements on the RF actuator, the design of the hardware, the calibration algorithm, and the implementation in firmware and software and the test results at LCLS.

X-ray free-electron lasers (XFELs) deliver ultrashort coherent laser pulses in the X-ray spectral regime, enabling novel investigations into the structure of individual nanoscale samples. In this work, we demonstrate how single-shot small-angle X-ray scattering (SAXS) measurements combined with fluorescence and ion time-of-flight (TOF) spectroscopy can be used to obtain size- and structure-selective evaluation of the light-matter interaction processes on the nanoscale. We recorded the SAXS images of single xenon clusters using XFEL pulses provided by the SPring-8 Angstrom compact free-electron laser (SACLA). The XFEL fluences and the radii of the clusters at the reaction point were evaluated and the ion TOF spectra and fluorescence spectra were sorted accordingly. We found that the XFEL fluence and cluster size extracted from the diffraction patterns showed a clear correlation with the fluorescence and ion TOF spectra. Our results demonstrate the effectiveness of the multispectroscopic approach for exploring laser–matter interaction in the X-ray regime without the influence of the size distribution of samples and the fluence distribution of the incident XFEL pulses.