Short-wavelength Free-electron Lasers Research Articles

Probing Laser‐Driven Structure Formation at Extreme Scales in Space and Time

AbstractIrradiation of solid surfaces with high intensity, ultrashort laser pulses triggers a variety of secondary processes that can lead to the formation of transient and permanent structures over a large range of length scales from mm down to the nano‐range. One of the most prominent examples are LIPSS – Laser‐Induced Periodic Surface Structures. While LIPSS have been a scientific evergreen for of almost 60 years, experimental methods that combine ultrafast temporal with the required nm spatial resolution have become available only recently with the advent of short pulse, short wavelength free electron lasers. Here, the current status and future perspectives in this field are discussed by exploiting the unique possibilities of these 4th‐generation light sources to address by time‐domain experimental techniques the fundamental LIPSS‐question, namely why and how laser irradiation can initiate the transition of a “chaotic” (rough) surface from an aperiodic into a periodic structure.

Controlling Fragmentation of the Acetylene Cation in the Vacuum Ultraviolet via Transient Molecular Alignment.

An open-loop control scheme of molecular fragmentation based on transient molecular alignment combined with single-photon ionization induced by a short-wavelength free electron laser (FEL) is demonstrated for the acetylene cation. Photoelectron spectra are recorded, complementing the ion yield measurements, to demonstrate that such control is the consequence of changes in the electronic response with molecular orientation relative to the ionizing field. We show that stable C2H2+ cations are mainly produced when the molecules are parallel or nearly parallel to the FEL polarization, while the hydrogen fragmentation channel (C2H2+ → C2H+ + H) predominates when the molecule is perpendicular to that direction, thus allowing one to distinguish between the two photochemical processes. The experimental findings are supported by state-of-the art theoretical calculations.

Observation of Rabi dynamics with a short-wavelength free-electron laser

Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field1. They are ubiquitous in physics with applications in different areas such as photonics2, nano-electronics3, electron microscopy4 and quantum information5. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light–matter interactions within the rotating-wave approximation6. Although intense nanometre-wavelength light sources have been available for more than a decade7–9, Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser10 can drive Rabi dynamics between the ground state and an excited state in helium atoms. The measured photoelectron signal reveals an Autler–Townes doublet and an avoided crossing, phenomena that are both fundamental to coherent atom–field interactions11. Using an analytical model derived from perturbation theory on top of the Rabi model, we find that the ultrafast build-up of the doublet structure carries the signature of a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond12 and few-femtosecond13 extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

Longitudinal phase space improvement of a continuous-wave photoinjector toward X-ray free-electron laser application

The electron source still remains a major challenge for continuous-wave (CW) X-ray free-electron lasers (FELs). In this paper, we study the feasibility of an injection line based on a DC and superconducting radio-frequency (SRF) combined photocathode injector. We present a detailed investigation on the longitudinal phase space evolution of the electron beam along the injection line. We also analyze the main issues determining the high-order energy spread and current skewness. Based on the analysis, we propose to use a harmonic cavity as the buncher for the injection line. Simulation shows that an extracted electron beam with a normalized RMS emittance of 0.37 μm, an RMS bunch length of 1.0 mm, a high-order RMS energy spread of 2.75 keV, and a current skewness of 0 can be obtained at the bunch charge of 100 pC. This study is meaningful to the design of the injection lines for short-wavelength CW FELs, including those based on normal-conducting very-high-frequency (VHF) guns or DC guns.

Multi-resolution electron spectrometer array for future free-electron laser experiments.

The design of an angular array of electron time-of-flight (eToF) spectrometers is reported, intended for non-invasive spectral, temporal, and polarization characterization of single shots of high-repetition rate, quasi-continuous, short-wavelength free-electron lasers (FELs) such as the LCLS II at SLAC. This array also enables angle-resolved, high-resolution eToF spectroscopy to address a variety of scientific questions on ultrafast and nonlinear light-matter interactions at FELs. The presented device is specifically designed for the time-resolved atomic, molecular and optical science endstation (TMO) at LCLS II. In its final version, the spectrometer comprises up to 20 eToF spectrometers aligned to collect electrons from the interaction point, which is defined by the intersection of the incoming FEL radiation and a gaseous target. The full composition involves 16 spectrometers forming a circular equiangular array in the plane normal to the X-ray propagation and four spectrometers at 54.7° angle relative to the principle linear X-ray polarization axis with orientations in the forward and backward direction of the light propagation. The spectrometers are capable of independent and minimally chromatic electrostatic lensing and retardation, in order to enable simultaneous angle-resolved photo- and Auger-Meitner electron spectroscopy with high energy resolution. They are designed to ensure an energy resolution of 0.25 eV across an energy window of up to 75 eV, which can be individually centered via the adjustable retardation to cover the full range of electron kinetic energies relevant to soft X-ray methods, 0-2 keV. The full spectrometer array will enable non-invasive and online spectral-polarimetry measurements, polarization-sensitive attoclock spectroscopy for characterizing the full time-energy structure of SASE or seeded LCLS II pulses, and support emerging trends in molecular-frame spectroscopy measurements.

Site-specific interrogation of an ionic chiral fragment during photolysis using an X-ray free-electron laser

Short-wavelength free-electron lasers with their ultrashort pulses at high intensities have originated new approaches for tracking molecular dynamics from the vista of specific sites. X-ray pump X-ray probe schemes even allow to address individual atomic constituents with a ‘trigger’-event that preludes the subsequent molecular dynamics while being able to selectively probe the evolving structure with a time-delayed second X-ray pulse. Here, we use a linearly polarized X-ray photon to trigger the photolysis of a prototypical chiral molecule, namely trifluoromethyloxirane (C3H3F3O), at the fluorine K-edge at around 700 eV. The created fluorine-containing fragments are then probed by a second, circularly polarized X-ray pulse of higher photon energy in order to investigate the chemically shifted inner-shell electrons of the ionic mother-fragment for their stereochemical sensitivity. We experimentally demonstrate and theoretically support how two-color X-ray pump X-ray probe experiments with polarization control enable XFELs as tools for chiral recognition.

Attosecond polarization modulation of x-ray radiation in a free-electron laser

A new method to generate short wavelength Free Electron Laser output with modulated polarisation at attosecond timescales is presented. Simulations demonstrate polarisation switching timescales that are four orders of magnitude faster than the current state of the art and, at X-Ray wavelengths, approaching the atomic unit of time of approximately $24$~attoseconds. Such polarisation control has significant potential in the study of ultra-fast atomic and molecular processes. The output alternates between either orthogonal linear or circularly polarised light without the need for any polarising optical elements. This facilitates operation at the high brightness X-ray wavelengths associated with FELs. As the method uses an afterburner configuration it would be relatively easy to install at exciting FEL facilities, greatly expanding their research capability.

Semi-analytical analysis of high-brightness microbunched beam dynamics with collective and intrabeam scattering effects

The studies of incoherent single-particle and collective multi-particle effects are, in general, separated in accelerator beam dynamics in that the two dynamical phenomena involve quite different time scales. Recent experimental measurements indicate that in some parameter regime, the small-angle, multiple scattering effects within a high-brightness electron beam can have a strong influence on microbunched beam dynamics. In this paper, we apply our recently developed semi-analytical kinetic analysis to investigate the collective phase space microbunched dynamics in the presence of incoherent single-particle effects. Particular emphasis will be placed on evaluation of the intrinsic or slice energy spread. An example of two linear beam transport lines, followed by two identical, interleaving bunch compressor chicanes, is then presented. The semi-analytical calculations are consistent with particle tracking simulations. Moreover, the threshold condition is derived, indicating the relation among relevant physical quantities. At threshold, the incoherent effect can be beneficial for effective suppression of the collective microbunching instability. We expect that this work could shed light on high-brightness electron transport beamline design to improve short-wavelength free-electron laser performance.

Novel method for the generation of stable radiation from free-electron lasers at high repetition rates

For more than a decade free-electron lasers (FELs) have been in operation, providing scientists from many disciplines with the benefits of ultrashort, nearly transversely coherent radiation pulses with wavelengths down to the \AA{}ngstrom range. If no further techniques are applied, the FEL will only amplify radiation from the stochastic distributed electron density in the electron bunch. Contemporary developments aim at producing stable and single-mode radiation by preparing an electron bunch with favorable longitudinal electron density distributions using magnets and conventional laser pulses (seed), hence the name ``seeding.'' In recent years, short wavelength FELs at high electron beam energies and high repetition rates were proposed and built. At those repetition rates, an external seed with sufficient power to manipulate the electron beam cannot be provided by present state-of-the-art laser systems, thus no external seeding scheme could be applied yet. In this paper, we present ways to seed FELs to generate short wavelength radiation at high repetition rates, making use of tested electron beam manipulation schemes. For our parameter study, we used the parameters of FLASH, the free-electron laser in Hamburg. First simulations are presented, showing the feasibility of the method proposed.

The regime of multi-stage trapping in free-electron lasers operating in the super-radiant and SASE regimes

The use of electron–wave interaction systems consisting of several tapered sections is considered as a method of efficiency enhancement of free-electron lasers (FELs) operating in different regimes of emission of a short wave pulse from a short electron bunch. These regimes are the principally multi-frequency self-amplified spontaneous emission regime traditionally used in short-wavelength FELs and the regime of electron–wave group synchronism, in which super-radiation of a quasi-monochromatic wave packet propagating together with the electron bunch occurs. In both the cases, the use of multi-stage trapping of electrons in the bunch by the radiated wave provides a significant (at least by an order of magnitude) increase in efficiency as compared to the saturated-stage efficiency in regular systems.

Design, specifications, and first beam measurements of the compact linear accelerator for research and applications front end

The compact linear accelerator for research and applications (CLARA) is an ultrabright electron beam test facility being developed at STFC Daresbury Laboratory. The ultimate aim of CLARA is to test advanced free electron laser (FEL) schemes that can later be implemented on existing and future short-wavelength FELs. In addition, CLARA is a unique facility to provide a high-quality electron beam to test novel concepts and ideas in a wide range of disciplines and to function as a technology demonstrator for a future United Kingdom x-ray FEL facility. CLARA is being built in three phases; the first phase, or front end (FE), comprises an S-band rf photoinjector, a linac, and an S-bend merging with the existing versatile electron linear accelerator beam line; the second phase will complete the acceleration to full beam energy of 250 MeV and also incorporate a separate beam line for use of electrons at 250 MeV; and the third phase will include the FEL section. The CLARA FE was commissioned during 2018, and the facility was later made available for user experiments. Significant advancements have been made in developing high-level software and a simulation framework for start-to-end simulations. The high-level software has been successfully used for unmanned rf conditioning and for characterization of the electron beam. This paper describes the design of the CLARA FE, performance of technical systems, high-level software developments, preliminary results of measured beam parameters, and plans for improvements and upgrades. © 2020 authors. Published by the American Physical Society.

Study of a free-electron laser driven by a laser-plasma accelerated beam at Peking University

The percent level energy spread and large divergence of laser-plasma beam are the main challenges of realizing compact short-wavelength free-electron lasers based on laser-plasma accelerators. These issues can be solved with proposed transverse gradient undulator method or bunch decompression method along with proper transport design. We present a study of using an expected 500 MeV laser-plasma beam with 0.3 mm⋅mrad normalized emittance and 0.3 mrad divergence at Peking University to drive compact free-electron laser at 30 nm. We employ the bunch decompression method with a chromatic matching beamline as well as the transverse gradient undulator method with assumed matched beam. Simulation shows that 700 MW power, 9.7 fs pulse duration and 0.85% relative bandwidth FEL output can be obtained using chromatic matched bunch decompression method. FEL with similar performance can be obtained using the transverse gradient undulator scheme.

Wakefield benchmarking at a single-pass high brightness electron linac

Collective effects such as wakefields affect the dynamics of high brightness electron beams in linear accelerators (linacs) and can degrade the performance of short wavelength free-electron lasers (FELs). If a reliable model of wakefields is made available, the accelerator can be designed and configured with parameters that minimize their disrupting effect. In this paper, the simulated effect of geometric (diffractive) wakefields and of coherent synchrotron radiation on the electron beam energy distribution at the FERMI FEL is benchmarked with measurements, so quantifying the accuracy of the model. Wakefield modeling is then extended to the undulator line, where particle tracking confirms the limited impact of the resistive wall wakefield on the lasing process. The study reveals an overall good understanding of collective effects in the facility.

Systematic study of a corrugated waveguide as a microwave undulator.

Microwave undulators have great potential to be used in short-wavelength free-electron lasers. In this paper, the properties of a corrugated waveguide and its performance as an undulator cavity for a UK X-ray free-electron laser were systematically studied. The equations presented in this paper allow a fast estimation of the dimensions of the corrugated waveguide. An undulator cavity operating at 36 GHz designed for the HE11 and HE12 modes was investigated and the performance of both modes compared.

Effects of field fluctuations on driven autoionizing resonances

The excitation of an autoionizing resonance by intense radiation requires a theoretical description beyond the transition probability per unit time. This implies a time-dependent formulation incorporating all features of the radiation source, such as pulse temporal shape and duration, as well as stochastic properties, for pulses other than Fourier limited. The radiation from short wavelength free electron lasers is a case in point, as it is the only source that can provide the necessary intensity. In view of ongoing experiments with such sources, we present a systematic study for an isolated autoionizing resonance. We find that intensity, pulse duration and field fluctuations conspire in producing unexpected excitation profiles, not amenable to a description in terms of the usual Fano profile. In particular, the role of intensity fluctuations turns out to pose challenging theoretical problems part of which have been addressed herein.

A Free Electron Laser Based on a Sectional System of RF Undulators

An efficient mode of the multistage capture and deceleration of particles in a sectioned undulator system for use in free electron lasers. This scheme is based on using a series of RF undulators with profiled resonant parameters that are powered by the independent powerful pulsed RF oscillators. The proposed mode allows efficiency to be obtained at a level of several percent in short-wavelength free electron lasers based on using dense bunches of electrons with relatively high energy spreads, formed in state-of-the-art laser plasma accelerators.

Symmetry breakdown of electron emission in extreme ultraviolet photoionization of argon

Short wavelength free-electron lasers (FELs), providing pulses of ultrahigh photon intensity, have revolutionized spectroscopy on ionic targets. Their exceptional photon flux enables multiple photon absorptions within a single femtosecond pulse, which in turn allows for deep insights into the photoionization process itself as well as into evolving ionic states of a target. Here we employ ultraintense pulses from the FEL FERMI to spectroscopically investigate the sequential emission of electrons from gaseous, atomic argon in the neutral as well as the ionic ground state. A pronounced forward-backward symmetry breaking of the angularly resolved emission patterns with respect to the light propagation direction is experimentally observed and theoretically explained for the region of the Cooper minimum, where the asymmetry of electron emission is strongly enhanced. These findings aim to originate a better understanding of the fundamentals of photon momentum transfer in ionic matter.

Seeded X-ray free-electron laser generating radiation with laser statistical properties

The invention of optical lasers led to a revolution in the field of optics and to the creation of such fields of research as quantum optics. The reason was their unique statistical and coherence properties. The emerging, short-wavelength free-electron lasers (FELs) are sources of very bright coherent extreme-ultraviolet and X-ray radiation with pulse durations on the order of femtoseconds, and are presently considered to be laser sources at these energies. FELs are highly spatially coherent to the first-order but in spite of their name, behave statistically as chaotic sources. Here, we demonstrate experimentally, by combining Hanbury Brown and Twiss interferometry with spectral measurements that the seeded XUV FERMI FEL-2 source does indeed behave statistically as a laser. The results may be useful for quantum optics experiments and for the design and operation of next generation FEL sources.

Revisiting photon-statistics effects on multiphoton ionization

We present a detailed analysis of the effects of photon statistics on multi-photon ionization. Through a detailed study of the role of intermediate states, we evaluate the conditions under which the premise of non-resonant processes is valid. The limitations of its validity are manifested in the dependence of the process on the stochastic properties of the radiation and found to be quite sensitive to the intensity. The results are quantified through detailed calculations for coherent, chaotic and squeezed vacuum radiation. Their significance in the context of recent developments in radiation sources such as the short wavelength Free Electron Laser and squeezed vacuum radiation are also discussed.

Dispersion effects on performance of free-electron laser based on laser wakefield accelerator

In this study, we investigate a new simple scheme using a planar undulator (PU) together with a properly dispersed electron beam ($e$ beam) with a large energy spread (${\sim}1\%$) to enhance the free-electron laser (FEL) gain. For a dispersed $e$ beam in a PU, the resonant condition is satisfied for the center electrons, while the frequency detuning increases for the off-center electrons, inhibiting the growth of the radiation. The PU can act as a filter for selecting the electrons near the beam center to achieve the radiation. Although only the center electrons contribute, the radiation can be enhanced significantly owing to the high-peak current of the beam. Theoretical analysis and simulation results indicate that this method can be used for the improvement of the radiation performance, which has great significance for short-wavelength FEL applications.