Coherent and transient states studied with extreme ultraviolet and X-ray free electron lasers: present and future prospects

The most recent light sources, extreme ultraviolet (EUV) and X-ray free electron lasers (FELs), have extended tabletop laser experiments to shorter wavelengths, adding element and chemical state specificity by exciting and probing electronic transitions from core levels. Through their unique properties, combining femtosecond X-ray pulses with coherence and enormous peak brightness, the FELs have enabled studies of a broad class of dynamic phenomena in matter that crosses many scientific disciplines and have led to major breakthroughs in the last few years. In this article, we review how the advances in the performance of the FELs, with respect to coherence, polarization and multi-color pulse production, have pushed the development of original experimental strategies to study non-equilibrium behavior of matter at the femtosecond–nanometer time–length scales. In this review, the emphasis is placed on the contribution of the EUV and soft X-ray FELs on three important subjects: (i) the new regime of X-ray matter interactions with ultrashort very intense X-ray pulses, (ii) the new potential of coherent imaging and scattering for answering questions about nano dynamics in complex materials and (iii) the unique possibility to stimulate and probe nonlinear phenomena that are at the heart of conversion of light into other forms of energy, relevant to photovoltaics, femtosecond magnetism and phase transitions in correlated materials.     

Undulators and generation of X-ray pulses in free-electron lasers with self-amplified spontaneous emission

The results of theoretical examination and comparative analysis of synchrotron radiation sources (specifically, undulators and X-ray free-electron lasers (FELs)) are presented. The problem of generation of shorter radiation pulses is prioritized; undulator systems and their corresponding FELs, which are considered to be the most promising in terms of generation of high-frequency ultrashort pulses of such radiation (in particular, in the X-ray range) are studied. The possibility of generation of higher harmonics is explored. The advantages and disadvantages of single-pass (with no reflecting elements) and multi-pass (with mirrors) FEL lasing schemes are revealed. The potential to reduce the duration of laser pulses produced by undulators and FELs and use them as sources of femtosecond pulses is investigated. The prospects for further development of X-ray free-electron lasers and the ways to improve the quality of their radiation with the given parameters are discussed.     

Multiwavelength anomalous diffraction at high x-ray intensity

The multiwavelength anomalous diffraction (MAD) method is used to determine phase information in x-ray crystallography by employing anomalous scattering from heavy atoms. X-ray free-electron lasers (FELs) show promise for revealing the structure of single molecules or nanocrystals, but the phase problem remains largely unsolved. Because of the ultrabrightness of x-ray FEL, samples experience severe electronic radiation damage, especially to heavy atoms, which hinders direct implementation of MAD with x-ray FELs. Here, we propose a generalized version of MAD phasing at high x-ray intensity. We demonstrate the existence of a Karle-Hendrickson-type equation in the high-intensity regime and calculate relevant coefficients with detailed electronic damage dynamics of heavy atoms. The present method offers a potential for ab initio structural determination in femtosecond x-ray nanocrystallography.     

On Harmonic Generation in X-Ray Free-Electron Lasers with Variable Undulator Deflection Parameter

Technical Physics - X-ray free-electron lasers (FELs) generate ultrashort bursts at wavelengths ~1 –100 Å. The possibility of harmonic generation in the X-ray range in FELs with a...     

Free‐electron laser multiplex driven by a superconducting linear accelerator

Free‐electron lasers (FELs) generate femtosecond XUV and X‐ray pulses at peak powers in the gigawatt range. The FEL user facility FLASH at DESY (Hamburg, Germany) is driven by a superconducting linear accelerator with up to 8000 pulses per second. Since 2014, two parallel undulator beamlines, FLASH1 and FLASH2, have been in operation. In addition to the main undulator, the FLASH1 beamline is equipped with an undulator section, sFLASH, dedicated to research and development of fully coherent extreme ultraviolet photon pulses using external seed lasers. In this contribution, the first simultaneous lasing of the three FELs at 13.4 nm, 20 nm and 38.8 nm is presented.     

Investigations of ultrafast phenomena in high-energy density physics using X-ray FEL radiation

The advent of highly intense and ultrashort pulses of short-wavelength radiation in the vacuum-ultraviolet to X-ray regime provides for the first time the possibility to study plasmas at the time scale of equilibration or even electron thermalization. The emerging radiation sources are free-electron lasers (FEL) based on high-energy electron accelerators. FELs provide a peak brilliance nine orders of magnitude higher than the best performing X-rays sources today. The FEL radiation parameters will enable the creation of high-energy density states of matter and the development of new diagnostics tools to investigate dense plasmas. As the first of the new sources the VUV-FEL at DESY, Hamburg becomes operational for high-energy density physics experiments during 2005.     

Harmonics Generation in Experiments with Free-Electron Lasers in the X-Ray Wavelength Range: a Theoretical Analysis

Technical Physics - The generation of undulator X-ray radiation harmonics in free-electron lasers (FELs), which has been observed in different experiments, has been given an analytical explanation....     

Numerical modeling of thermal loading of diamond crystal in X-ray FEL oscillators

Due to high reflectivity and high resolution of X-ray pulses, diamond is one of the most popular Bragg crystals serving as the reflecting mirror and mono-chromator in the next generation of free electron lasers(FELs).The energy deposition of X-rays will result in thermal heating, and thus lattice expansion of the diamond crystal,which may degrade the performance of X-ray FELs. In this paper, the thermal loading effect of diamond crystal for X-ray FEL oscillators has been systematically studied by combined simulation with Geant4 and ANSYS, and its dependence on the environmental temperature, crystal size, X-ray pulse repetition rate and pulse energy are presented. Our results show that taking the thermal loading effects into account, X-ray FEL oscillators are still robust and promising with an optimized design.     

Opportunities for resonant elastic X-ray scattering at X-ray free-electron lasers

X-ray Free-Electron Lasers (FELs) are beginning to deliver a revolution in X-ray experiments, thanks to their ultra-bright (peak brightness exceeding 10³³ photons/s/mm²/mrad²/0.1%BW), ultrashort (down to a few fs), spatially coherent X-ray pulses. Presently operational facilities cover wide spectral ranges, from the VUV and soft X-ray wavelengths of FLASH in Hamburg (down to 4.2 nm), to the hard X-rays delivered by the LCLS in Stanford (wavelengths of 0.15 nm or shorter). The basic properties of the new sources are briefly reviewed, and the impact on resonant scattering experiments is discussed. The perspective of investigating ultrafast magnetism, and, more generally, the time-dependent response of strongly correlated electron systems, in a pump-and-probe mode at the L edges of 3d transition metals, would be very attractive. In the hard X-ray range, the very recent proposal of self-seeded X-ray FELs, with 10⁻⁵ intrinsic bandwidth, tunable wavelength, 100 fs pulses and number of photons per pulse of order 10¹² also opens exciting possibilities for resonant scattering.     

Near-infrared storage ring free electron laser experiments at AIST

The development of free electron lasers (FELs) with a compact storage ring NIJI-IV in the near- and middle-infrared regions has been advanced at the National Institute of Advanced Industrial Science and Technology. The optical klystron ETLOK-III was installed in one of the long straight sections of the NIJI-IV, and spontaneous emission spectra were observed in the visible and near-infrared regions. Optical cavity chambers for infrared FELs were installed this February, and it was confirmed that the vibration amplitude of the optical cavity chambers was below 0.5 μm in an optical beam axis. FEL experiments in the near-infrared region will be performed this winter.     

Generation of femtosecond X-ray pulses via laser–electron beam interaction

The generation of femtosecond X-ray pulses will have important scientific applications by enabling the direct measurement of atomic motion and structural dynamics in condensed matter on the fundamental time scale of a vibrational period. Interaction of femtosecond laser pulses with relativistic electron beams is an effective approach to generating femtosecond pulses of X-rays. In this paper we present recent results from proof-of-principle experiments in which 300 fs pulses are generated from a synchrotron storage ring by using an ultrashort optical pulse to create femtosecond time structure on the stored electron bunch. A previously demonstrated approach for generating femtosecond X-rays via Thomson scattering between terawatt laser pulses and relativistic electrons is reviewed and compared with storage-ring based schemes.     

Femtosecond X-rays from relativistic electrons: new tools for probing structural dynamics

Femtosecond X-ray science is a new frontier in ultrafast research in which time-resolved measurement techniques are applied with X-ray pulses to investigate structural dynamics at the atomic scale on the fundamental time scale of an atomic vibrational period (∼100 fs). This new research area depends critically on the development of suitable femtosecond X-ray sources with the appropriate flux (ph/(s·0.1% BW)), brightness (ph/(s·mm²·mrad²·0.1% BW)), and tunability for demanding optical/X-ray pump probe experiments. In this paper we review recently demonstrated techniques for generating femtosecond X-rays via interaction between femtosecond laser pulses and relativistic electron beams. We give an overview of a novel femtosecond X-ray source that is proposed based on a linear accelerator combined with X-ray pulse compression.     

On the possibility of obtaining incoherent femtosecond X-ray pulses from a laser plasma

It is proposed to use a high rate of collisional ionization in a superdense laser plasma to generate incoherent femtosecond X-ray pulses. The calculations indicate that the use of picosecond laser pulses with a contrast of about 10¹⁰ will allow the generation of an X-ray pulse with a duration of about 10 fs. The adequacy of the proposed model of the excitation of linear X-ray radiation from the plasma has been tested in the experiments with a picosecond laser of a moderately high contrast.     

Single-molecule imaging with x-ray free-electron lasers: dream or reality?

X-ray free-electron lasers (XFEL) are revolutionary photon sources, whose ultrashort, brilliant pulses are expected to allow single-molecule diffraction experiments providing structural information on the atomic length scale of nonperiodic objects. This ultimate goal, however, is currently hampered by several challenging questions basically concerning sample damage, Coulomb explosion, and the role of nonlinearity. By employing an original ab?initio approach, we address these issues showing that XFEL-based single-molecule imaging will be only possible with a few-hundred long attosecond pulses, due to significant radiation damage and the formation of preferred multisoliton clusters which reshape the overall electronic density of the molecular system at the femtosecond scale.     

Electron beam brightness in linac drivers for free-electron-lasers

Linear accelerators delivering high brightness electron beams are essential for a number of current and proposed accelerator applications, such as free electron lasers (FELs). In this kind of facilities the charge density is high enough to drive collective effects (wakefields) that, notwithstanding the high beam rigidity at energies up to the GeV range, may increase the beam emittance relative to the injection level, eventually degrading the nominal beam brightness. New theoretical developments and experimental capabilities, driven by the recent construction of vacuum-ultra-violet and X-ray linac-driven FELs, have advanced the present knowledge. This article describes the progress in the field of ultra-relativistic electron beam manipulation to maximize the final beam brightness, with a focus on the most recent techniques including optics design, pulse shaping and brightness optimization strategies. The theoretical models are supported by a review of the experimental results in now-running FEL facilities.     

Generation of Soft X-Ray Radiation in a Compact Free-Electron Laser with Harmonic Multiplication

Technical Physics - Single-pass free-electron lasers (FELs) with harmonic multiplication in the X-ray range are studied theoretically with the objective of producing intense radiation with the...     

Indo‐French meeting on indus‐2 and soleil

With the availability of the first generation of X-ray free electron lasers, pump-probe measurements with femtosecond resolution and high brilliance are now possible. For condensed matter systems, a wealth of modes in the mid-infrared (MIR) and terahertz (THz) regime determine the physics such that targeted excitation with ultrashort pulses at long wavelength becomes an important tool. We will briefly discuss the methodology of pump-probe experiments at the Linac Coherent Light Source (LCLS) and then review methods of generation of intense THz and MIR pulses. This is followed with recent examples from atomic and condensed matter physics at LCLS, and we conclude with an outlook of future developments in this field.     

Theoretical Analysis of Radiation Properties of X-Ray Free-Electron Lasers

Radiophysics and Quantum Electronics - We perform a comparative analysis of the radiation of X-ray free-electron lasers (FELs) LCLS, PAL-XFEL, SwissFEL, SACLA, FLASH2, and European XFEL, as well as...     

在固体透明材料中利用级联四波混频方法获得宽带多色飞秒激光脉冲的研究

飞秒激光光谱学实验研究的深入与拓展对飞秒激光脉冲的要求也越来越高.比如多色抽运探测实验需要同时用到多个不同频率的超短飞秒激光脉冲.本文设计了一个更加简单紧凑的实验装置,对两束不同中心频率的入射光引入相反啁啾,在厚度为0.5 mm的CaF2晶体中利用级联四波混频获得了光谱半高全宽近100nm,支持傅里叶转换极限脉宽小于10 fs的多色飞秒激光脉冲.这一结果将为拓展飞秒激光光谱学研究和应用发挥重要作用.     

Fully coherent hard X-ray generation by two-stage phase-merging enhanced harmonic generation

Cascading stages of seeded free electron lasers (FELs) is a promising way to produce fully coherent X-ray radiation. We study a new approach to produce coherent hard X-rays by cascading the recently proposed phase-merging enhanced harmonic generation (PEHG) The scheme consists of one dogleg and two PEHG configurations, and may be one of the leading candidates for the extracted undulator branch in future X-ray FEL facilities. FEL physics studies show that such a scheme is feasible within the present technology and can provide high brightness X-ray radiation pulses with narrow bandwidth and full coherence The radiated peak power at 1 Å wavelength converted from an initial 200 nm seed laser is over 2 GW.