Free-electron Laser Radiation Research Articles

Soft X-ray multiphoton excitation of small iodine methane derivatives

The fragmentation pattern of the iodine-containing molecules and following a strong multiphoton excitation in the vicinity of the iodine 4d giant resonance regime is studied using soft X-ray free electron laser radiation. A strong difference of the charge distribution and the kinetic energy release (KER) for the two molecules is found. The effects can be attributed to charge rearrangement processes induced by the photoexcitation. The difference in the observed distribution for higher charge states of iodine and carbon fragments is consistent with an over-the-barrier model for the charge rearrangement in the dissociating molecules. The KER for singly ionised carbon fragments indicates an ultrafast charge rearrangement before the dissociation starts.

Real-time investigation of dynamic protein crystallization in living cells.

X-ray crystallography requires sufficiently large crystals to obtain structural insights at atomic resolution, routinely obtained in vitro by time-consuming screening. Recently, successful data collection was reported from protein microcrystals grown within living cells using highly brilliant free-electron laser and third-generation synchrotron radiation. Here, we analyzed in vivo crystal growth of firefly luciferase and Green Fluorescent Protein-tagged reovirus μNS by live-cell imaging, showing that dimensions of living cells did not limit crystal size. The crystallization process is highly dynamic and occurs in different cellular compartments. In vivo protein crystallization offers exciting new possibilities for proteins that do not form crystals in vitro.

Atomic kinetics for isochoric heating of solid aluminum under short intense XUV free electron laser irradiation

An atomic configuration kinetics model that links the cold solid state, the heated solid state and the dilute plasma state is presented. It is based on a coherent implementation of the Fermi-Dirac statistics for the free electrons and a link between the cold solid elementary processes and the plasma elementary processes. This model allows us to follow the bound electron kinetics continuously from the cold solid state to the plasma state. The good agreement of the obtained spectra for the isochoric heating of solid aluminum under XUV free electron laser (XUVFEL) irradiation show the validity of this approach. The kinetics model has also been included in a 1D Lagrangian hydrodynamics code. This code is an essential tool for the design and the interpretation of warm/hot dense matter experiments.

On the Importance of Electron Beam Brightness in High Gain Free Electron Lasers

Linear accelerators delivering high brightness electron beams are essential for driving short wavelength, high gain free-electron lasers (FELs). The FEL radiation output efficiency is often parametrized through the power gain length that relates FEL performance to electron beam quality at the undulator. In this review article we illustrate some approaches to the preliminary design of FEL linac-drivers, and analyze the relationship between the output FEL wavelength, exponential gain length and electron beam brightness. We extend the discussion to include FEL three-dimensional effects and electron beam projected emittances. Although mostly concentrating on FELs based upon self-amplified spontaneous emission (SASE), our findings are in some cases highly relevant to externally seeded FELs.

Transient charge dynamics in argon-cluster nanoplasmas created by intense extreme-ultraviolet free-electron-laser irradiation

We present extreme-ultraviolet (EUV) fluorescence spectra of Ar clusters irradiated by intense EUV free-electron-laser (FEL) pulses focused to intensities of up to $3\ifmmode\times\else\texttimes\fi{}{10}^{13}\phantom{\rule{0.16em}{0ex}}\mathrm{W}/{\mathrm{cm}}^{2}$ at a wavelength of 51 nm. The spectra reveal fluorescence at wavelengths shorter than that of the incident radiation, which can be assigned to EUV fluorescence lines from excited multiply charged ions $\mathrm{A}{\mathrm{r}}^{z+*}$ with $z$ as high as 6. This demonstrates that charge states as high as 7+ are produced by the FEL irradiation. The dependence of the spectra on cluster size shows that the highly charged ions are generated at the cluster surface, indicating inhomogeneous charging. The FEL power dependencies of the spectral features suggest that the inhomogeneous distribution of charge within the clusters reduces ionization thresholds at the cluster surface.

Broadband multilayer optics for ultrafast EUV absorption spectroscopy with free electron laser radiation

A new experimental approach for near–edge ultrafast absorption spectroscopy in the extreme ultraviolet (EUV) spectral region at the FERMI@Elettra EIS-TIMEX end-station is presented. An innovative multilayer mirror is proposed as the key element of the set-up. The multilayer structure is a tailor-made Mo/Y periodic stack tuned at the 12.2–12.6 nm wavelength range, designed and realized to probe matter under extreme conditions by focusing the tunable free electron laser radiation, without affecting the temporal beam properties. The performance of such coated mirrors has been investigated at FERMI@Elettra EIS-TIMEX and the results have been compared with those obtained using synchrotron light. Further, the focusing system has been tested by performing sub-100 fs absorption spectroscopy experiments at the L(2, 3)-edge of silicon.

Toward the Extreme Ultra Violet Four Wave Mixing Experiments: From Table Top Lasers to Fourth Generation Light Sources

Three different Transient Grating setups are presented, with pulsed and continuous wave probe at different wavelengths, ranging from infrared to the extreme ultra violet region. Both heterodyne and homodyne detections are considered. Each scheme introduces variations with respect to the previous one, allowing moving from classical table top laser experiments towards a new four wave mixing scheme based on free electron laser radiation. A comparison between the various setups and the first results from extreme ultra violet transient grating experiments is also discussed.

Cumulative HOM Excitation and Transition Effects in LCLS-II

LCLS-II is a proposed upgrade of the most powerful X-ray laser in the world built at SLAC National Accelerator Laboratory. When complete, multiple free electron laser (FEL) sections will be powered by a continuous wave superconducting radio frequency (SRF) electron linac. The vital parameters for FEL radiation quality are beam emittance and beam transverse position stability. Excitation of high order modes (HOM) in SRF niobium cavities leads to additional beam power dissipation through incoherent and coherent losses. Energy stored in HOM may cause cumulative effects — transverse and longitudinal position displacement of the center of bunches, which leads to transverse and longitudinal emittance dilution. Cumulative effects due to dipole HOM excitation in LCLS-II are analyzed. Transition HOM effects are caused by sudden changes (periodic or single case) in the beam bunch structure. Bunch center position disturbance due to transition HOM effects is estimated.

Binary doe with elongated focal depth to focus terahertz free electron laser radiation (novofel)

A binary silicon diffractive optical element (DOE) focusing laser radiation onto an axial segment (or a DOE with elongated focal depth) for the terahertz spectral range has been designed and characterized using terahertz radiation of the Novosibirsk Free Electron Laser (NovoFEL).

X-band rf driven free electron laser driver with optics linearization

In this paper, a compact hard X-ray free electron lasers (FEL) design is proposed with all X-band rf acceleration and two stage bunch compression. It eliminates the need of a harmonic rf linearization section by employing optics linearization in its first stage bunch compression. Quadrupoles and sextupoles are employed in a bunch compressor one (BC1) design, in such a way that second order longitudinal dispersion of BC1 cancels the second order energy correlation in the electron beam. Start-to-end 6-D simulations are performed with all the collective effects included. Emittance growth in the horizontal plane due to coherent synchrotron radiation is investigated and minimized, to be on a similar level with the successfully operating Linac coherent light source (LCLS). At a FEL radiation wavelength of 0.15 nm, a saturation length of 40 meters can be achieved by employing an undulator with a period of 1.5 cm. Without tapering, a FEL radiation power above 10 GW is achieved with a photon pulse length of 50 fs, which is LCLS-like performance. The overall length of the accelerator plus undulator is around 250 meters which is much shorter than the LCLS length of 1230 meters. That makes it possible to build hard X-ray FEL in a laboratory with limited size.

Radiation detectors based on microchannel plates for free-electron lasers

Detectors based on microchannel plates are used to detect the radiation of free-electron lasers operating in short-wavelength ranges. We present descriptions of radiation detectors for the FLASH free-electron laser (DESY, Hamburg) that operates in vacuum ultraviolet and soft X-ray wavelength ranges (4–100 nm) and detectors for the European X-ray free electron laser that is being constructed in Hamburg and is designed to operate in the X-ray wavelength range from 0.05 to 4.3 nm.

Spatio-Temporal Dynamical Systems in Inner-Shell Photoionization in Free Molecules, Clusters, and Solids

Dynamic spatial hole localization and symmetry breaking phenomena are examined. Absorption of X-ray synchrotron and free-electron–laser radiation in matter is accompanied by strong dynamic corehole localization and temporary trap of the electron ejected from a deep level within the finite size potential barrier. As a result the symmetry of core excited states is reduced in comparison with ground state as the inversion symmetry is being broken. This is a very general property of coreexcited polyatomic compounds with equivalent atoms as their equivalence implies their equal probability of excitation averaged over large timescale but not simultaneous core excitation. Different approaches to rationalizing the symmetry breaking phenomena are presented and discussed with the emphasis on the quasiatomic dynamic corehole localization model. By examining the experimental ultrafast probe of photoabsorption processes we demonstrate an important role of spatio-temporal (nanometric-femtosecond) dynamically localized coreexcited moieties in molecule, clusters and solids. The photoelectron angular distributions from N and O 1s levels in fixed-in-space N2 and CO2 molecules, the photoelectron induced rotational heating of N2, the Auger decay spectra of N2 and the near S 1s edge X-ray absorption fine structure of free SF6 molecules are discussed in more detail.

Spatio-temporal coherence of free-electron laser radiation in the extreme ultraviolet determined by a Michelson interferometer

A key feature of extreme ultraviolet (XUV) radiation from free-electron lasers (FELs) is its spatial and temporal coherence. We measured the spatio-temporal coherence properties of monochromatized FEL pulses at 13.5 nm using a Michelson interferometer. A temporal coherence time of (59±8) fs has been determined, which is in good agreement with the spectral bandwidth given by the monochromator. Moreover, the spatial coherence in vertical direction amounts to about 15% of the beam diameter and about 12% in horizontal direction. The feasibility of measuring spatio-temporal coherence properties of XUV FEL radiation using interferometric techniques advances machine operation and experimental studies significantly.

Longitudinal space charge assisted echo seeding of a free-electron laser with laser-spoiler noise suppression

Seed lasers are employed to improve the temporal coherence of free-electron laser (FEL) light. However, when these seed pulses are short relative to the particle bunch, the noisy, temporally incoherent radiation from the unseeded electrons can overwhelm the coherent, seeded radiation. In this paper, a technique to seed a particle bunch with an external laser is presented in which a new mechanism to improve the contrast between coherent and incoherent free electron laser radiation is employed together with a novel, simplified echo-seeding method. The concept relies on a combination of longitudinal space charge wakes and an echo-seeding technique to make a short, coherent pulse of FEL light together with noise background suppression. Several different simulation codes are used to illustrate the concept with conditions at the soft x-ray free-electron laser in Hamburg, FLASH.

Saturation phenomena for ultra short Free Electron Laser pulses

Saturable absorption was recently observed in transmission measurements above the LII,III edge of pure Al thin films using ultra short x-ray pulses at a free-electron-laser (FEL) facility . [1] The high fluence reachable by FEL pulses, the shortness of the pulse duration, and the typical lifetime of the excited state, are all important factors enabling observation of the phenomenon. We devised a simplified theoretical model describing the saturation phenomenon using a three- channel model containing ground, excited and relaxed states. This phenomenological model explicitly includes the interaction between the solid and photon field in semi classical way, and the resulting non-linear coupled equation is solved numerically. We successfully applied this model to recent experimental results obtained using FEL radiation. [2,3]

Quantized form factor shift in the presence of free electron laser radiation

In electron scattering, the target form factors contribute significantly to the diffraction pattern and carry information on the target electromagnetic charge distribution. Here we show that the presence of electromagnetic radiation, as intense as currently available in free electron lasers, shifts the dependence of the target form factors by a quantity that depends on the number of photons absorbed or emitted by the electron as well as on the parameters of the electromagnetic radiation. As example, we show the impact of intense ultraviolet and soft X-ray radiation on elastic electron scattering by the Ne-like argon ion and by the xenon atom. We find that the shift brought by the radiation to the form factor is of the order of some percent. Our results may open up a new avenue to explore matter with the assistance of laser.

Mid-infrared free-electron laser tuned to the amide I band for converting insoluble amyloid-like protein fibrils into the soluble monomeric form.

A mid-infrared free-electron laser (FEL) is operated as a pulsed and linearly polarized laser with tunable wavelengths within infrared region. Although the FEL can ablate soft tissues with minimum collateral damage in surgery, the potential of FEL for dissecting protein aggregates is not fully understood. Protein aggregates such as amyloid fibrils are in some cases involved in serious diseases. In our previous study, we showed that amyloid-like lysozyme fibrils could be disaggregated into the native form with FEL irradiation specifically tuned to the amide I band (1,620 cm−1). Here, we show further evidence for the FEL-mediated disaggregation of amyloid-like fibrils using insulin fibrils. Insulin fibrils were prepared in acidic solution and irradiated by the FEL, which was tuned to either 1,620 or 2,000 cm−1 prior to the experiment. The Fourier transform infrared spectroscopy (FT-IR) spectrum after irradiation with the FEL at 1,620 cm−1 indicated that the broad peak (1,630–1,660 cm−1) became almost a single peak (1,652 cm−1), and the β-sheet content was reduced to 25 from 40 % in the fibrils, while that following the irradiation at 2,000 cm−1 remained at 38 %. The Congo Red assay as well as transmission electron microscopy observation confirmed that the number of fibrils was reduced by FEL irradiation at the amide I band. Size-exclusion chromatography analysis indicated that the disaggregated form of fibrils was the monomeric form. These results confirm that FEL irradiation at the amide I band can dissect amyloid-like protein fibrils into the monomeric form in vitro.

Ab initio simulations for the ion-ion structure factor of warm dense aluminum.

We perform abinitio simulations based on finite-temperature density functional theory in order to determine the static and dynamic ion-ion structure factor in aluminum. We calculate the dynamic structure factor via the intermediate scattering function and extract the dispersion relation for the collective excitations. The results are compared with available experimental x-ray scattering data. Very good agreement is obtained for the liquid metal domain. In addition we perform simulations for warm dense aluminum in order to obtain the ion dynamics in this strongly correlated quantum regime. We determine the sound velocity for both liquid and warm dense aluminum which can be checked experimentally using narrow-bandwidth free electron laser radiation.

The role of space charge in spin-resolved photoemission experiments

Spin-resolved photoemission is one of the most direct ways of measuring the magnetization of a ferromagnet. If all valence band electrons contribute, the measured average spin polarization is proportional to the magnetization. This is even the case if electronic excitations are present, and thus is of particular interest for studying the response of the magnetization to a pump laser pulse. Here, we demonstrate the feasibility of ultrafast spin-resolved photoemission using free electron laser (FEL) radiation and investigate the effect of space charge on the detected spin polarization. The sample is exposed to the radiation of the FEL FLASH in Hamburg. Surprisingly, the measured spin polarization depends on the fluence of the FEL radiation: a higher FEL fluence reduces the measured spin polarization. Space-charge simulations can explain this effect. These findings have consequences for future spin-polarized photoemission experiments using pulsed photon sources.

Modeling saturable absorption for ultra short X-ray pulses

Saturable absorption was recently observed in transmission measurements above the LII,III edge of pure Al thin films using ultra short X-ray pulses at a free-electron-laser (FEL) facility. The high fluence reachable by FEL pulses, the shortness of the pulse duration, and the typical lifetime of the excited state are all important factors enabling observation of the phenomenon. We devised a simplified theoretical approach describing the saturation phenomenon using a three-channel model containing ground, excited and relaxed states. This phenomenological model explicitly includes the interaction between the solid and photon field in a semi-classical way, and the resulting non-linear coupled equation is solved numerically. We successfully applied this model to recent experimental results obtained using FEL radiation.