Free-electron Laser Pulse Duration Research Articles

Nanoscale Transient Magnetization Gratings Created and Probed by Femtosecond Extreme Ultraviolet Pulses.

We utilize coherent femtosecond extreme ultraviolet (EUV) pulses from a free electron laser (FEL) to generate transient periodic magnetization patterns with periods as short as 44 nm. Combining spatially periodic excitation with resonant probing at the M-edge of cobalt allows us to create and probe transient gratings of electronic and magnetic excitations in a CoGd alloy. In a demagnetized sample, we observe an electronic excitation with a rise time close to the FEL pulse duration and ∼0.5 ps decay time indicative of electron-phonon relaxation. When the sample is magnetized to saturation in an external field, we observe a magnetization grating, which appears on a subpicosecond time scale as the sample is demagnetized at the maxima of the EUV intensity and then decays on the time scale of tens of picoseconds via thermal diffusion. The described approach opens multiple avenues for studying dynamics of ultrafast magnetic phenomena on nanometer length scales.

Pulse length effects on autoionizing states under the influence of intense SASE XUV fields

The Fano absorption line shape of an autoionizing state encodes information on its internal atomic structure and dynamics. When driven near-resonantly with intense extreme ultraviolet (XUV) electric fields, the absorption profile can be deliberately modified, including observable changes of both the line-shape asymmetry and strength of the resonance, revealing information on the underlying dynamics of the system in response to such external driving. We report on the influence of the XUV pulse parameters at high intensity that can be achieved with a free-electron laser (FEL) with statistically broadened spectra based on self-amplified spontaneous emission (SASE). More specifically, the impact of the FEL pulse duration is studied for the example of the doubly excited 2s2p resonance in helium, where line-shape modifications have been measured with XUV transient absorption spectroscopy in Fraunhofer-type transmission geometry. A computational few-level-model provides insight into the impact of different average pulse durations of the stochastic FEL pulses. These findings are supported by measurements performed at the Free-Electron Laser in Hamburg (FLASH) and provide further insight into XUV strong-coupling dynamics of resonant transitions driven by intense high-frequency FEL sources.

Parallel Broadband Femtosecond Reflection Spectroscopy at a Soft X-Ray Free-Electron Laser

X-ray absorption spectroscopy (XAS) and the directly linked X-ray reflectivity near absorption edges yield a wealth of specific information on the electronic structure around the resonantly addressed element. Observing the dynamic response of complex materials to optical excitations in pump–probe experiments requires high sensitivity to small changes in the spectra which in turn necessitates the brilliance of free electron laser (FEL) pulses. However, due to the fluctuating spectral content of pulses generated by self-amplified spontaneous emission (SASE), FEL experiments often struggle to reach the full sensitivity and time-resolution that FELs can in principle enable. Here, we implement a setup which solves two common challenges in this type of spectroscopy using FELs: First, we achieve a high spectral resolution by using a spectrometer downstream of the sample instead of a monochromator upstream of the sample. Thus, the full FEL bandwidth contributes to the measurement at the same time, and the FEL pulse duration is not elongated by a monochromator. Second, the FEL beam is divided into identical copies by a transmission grating beam splitter so that two spectra from separate spots on the sample (or from the sample and known reference) can be recorded in-parallel with the same spectrometer, enabling a spectrally resolved intensity normalization of pulse fluctuations in pump–probe scenarios. We analyze the capabilities of this setup around the oxygen K- and nickel L-edges recorded with third harmonic radiation of the free electron laser in Hamburg (FLASH), demonstrating the capability for pump–probe measurements with sensitivity to reflectivity changes on the per mill level.

Characterization of soft X-ray FEL pulse duration with two-color photoelectron spectroscopy.

The pulse duration of soft X-ray free-electron laser (FEL) pulses of SACLA BL1 (0.2-0.3 nC per bunch, 0.5-0.8 MeV) were characterized by photoelectron sideband measurements. The intensity of the He 1 s-1 photoelectron sidebands generated by a near-infrared femtosecond laser was measured as a function of the time delay between the two pulses using an arrival time monitor. From the width of the cross-correlation trace thus derived, the FEL pulse duration was evaluated to be 28 ± 5 fs full width at half-maximum in the photon energy range between 40 eV and 120 eV.

Multielectron-Ion Coincidence Spectroscopy of Xe in Extreme Ultraviolet Laser Fields: Nonlinear Multiple Ionization via Double Core-Hole States.

Ultrafast multiphoton ionization of Xe in strong extreme ultraviolet free-electron laser (FEL) fields (91eV, 30fs, 1.6×10^{12} W/cm^{2}) has been investigated by multielectron-ion coincidence spectroscopy. The electron spectra recorded in coincidence with Xe^{4+} show characteristic features associated with two-photon absorption to the 4d^{-2} double core-hole (DCH) states and subsequent Auger decay. It is found that the pathway via the DCH states, which has eluded clear identification in previous studies, makes a large contribution to the multiple ionization, despite the long FEL pulse duration compared with the lifetime of the 4d core-hole states.

Coherence time characterization method for hard X-ray free-electron lasers.

Coherence time is one of the fundamental characteristics of light sources. Methods based on autocorrelation have been widely applied from optical domain to soft X-rays to characterize the radiation coherence time. However, for the hard X-ray regime, due to the lack of proper mirrors, it is extremely difficult to implement such autocorrelation scheme. In this paper, a novel approach for characterizing the coherence time of a hard X-ray free-electron laser (FEL) is proposed and validated numerically. A phase shifter is adopted to control the correlation between X-ray and microbunched electrons. The coherence time of the FEL pulse can be extracted from the cross-correlation. Semi-analytical analysis and three-dimensional time-dependent numerical simulations are presented to elaborate the details. A coherence time of 218.2 attoseconds for 6.92 keV X-ray FEL pulses is obtained in our simulation based on the configuration of Linac Coherent Light Source. This approach provides critical temporal coherence diagnostics for X-ray FELs, and is decoupled from machine parameters, applicable for any photon energy, radiation brightness, repetition rate and FEL pulse duration.

Mapping ultrafast ionization of atoms and clusters with terahertz-streaking delay

We apply THz-field streaking to temporally resolve the ultrafast ionization of neutral cluster vs atomic targets exposed to intense ultrashort soft x-ray pulses from a free-electron laser (FEL). In the experiment pristine Xe and mixed Xe/Ar clusters as well as Xe atoms are ionized in the vicinity of the $4d\ensuremath{\rightarrow}\ensuremath{\varepsilon}f$ giant resonance of Xe. We compare the relative streaking delay between the center-of-mass oscillations of electrons that have final kinetic energies in the spectral region of the Xe($4d$) photoline. Our results show that clusters are ionized at the beginning of the 100 fs FEL pulse as supported by calculations of target frustration in the focal volume. We have identified a significantly larger 40 fs relative streaking delay between mixed Xe-Ar clusters vs Xe atoms compared to a 15 fs relative delay found for pristine Xe clusters. This is attributed to the high sensitivity of our spectroscopic measurement to the degree of condensation of the cluster target. Our results show that THz streaking is a powerful technique to temporally study electron emission from extended targets under intense FEL radiation on time scales that are significantly shorter than the FEL pulse duration.

FLASH free-electron laser single-shot temporal diagnostic: terahertz-field-driven streaking.

The commissioning of a terahertz-field-driven streak camera installed at the free-electron laser (FEL) FLASH at DESY in Hamburg, being able to deliver photon pulse duration as well as arrival time information with ∼10 fs resolution for each single XUV FEL pulse, is reported. Pulse durations between 300 fs and <15 fs have been measured for different FLASH FEL settings. A comparison between the XUV pulse arrival time and the FEL electron bunch arrival time measured at the FLASH linac section exhibits a correlation width of 20 fs r.m.s., thus demonstrating the excellent operation stability of FLASH. In addition, the terahertz-streaking setup was operated simultaneously to an alternative method to determine the FEL pulse duration based on spectral analysis. FLASH pulse duration derived from simple spectral analysis is in good agreement with that from terahertz-streaking measurement.

Plasma switch as a temporal overlap tool for pump-probe experiments at FEL facilities

We have developed an easy-to-use and reliable timing tool to determine the arrival time of an optical laser and a free electron laser (FEL) pulses within the jitter limitation. This timing tool can be used from XUV to X-rays and exploits high FELs intensities. It uses a shadowgraph technique where we optically (at 800 nm) image a plasma created by an intense XUV or X-ray FEL pulse on a transparent sample (glass slide) directly placed at the pump - probe sample position. It is based on the physical principle that the optical properties of the material are drastically changed when its free electron density reaches the critical density. At this point the excited glass sample becomes opaque to the optical laser pulse. The ultra-short and intense XUV or X-ray FEL pulse ensures that a critical electron density can be reached via photoionization and subsequent collisional ionization within the XUV or X-ray FEL pulse duration or even faster. This technique allows to determine the relative arrival time between the optical laser and the FEL pulses in only few single shots with an accuracy mainly limited by the optical laser pulse duration and the jitter between the FEL and the optical laser. Considering the major interest in pump-probe experiments at FEL facilities in general, such a femtosecond resolution timing tool is of utmost importance.

Femtosecond x-ray free electron laser pulse duration measurement from spectral correlation function

We present a novel method for measuring the duration of femtosecond x-ray pulses from self-amplified spontaneous emission free electron lasers by performing statistical analysis in the spectral domain. Analytical expressions of the spectral correlation function were derived in the linear regime to extract both the pulse duration and the spectrometer resolution. Numerical simulations confirmed that the method can be also used in the nonlinear regime. The method was demonstrated experimentally at the Linac Coherent Light Source by measuring pulse durations down to 13 fs FWHM.

Evolution of photoionization two-stream instability in collisional plasma

A kinetic model which takes into account gas jet photoionization by an ultrashort linearly polarized EUV/X-ray free electron laser (FEL) pulse, a self-generated low frequency electric field, and elastic electron scattering on atoms is introduced to study the photoionization two-stream (PITS) instability. The evolution of PITS instability is described in terms of an integral equation for electron density perturbations. This paper presents a generalization of previous theories of the PITS instability in collisionless plasmas. The instability is produced by the anisotropy of photoionized electrons and is strongly affected by electron–atom collisions. Relaxation of the PITS instability is studied for different relations between the FEL pulse duration, the instability growth time, and the electron collision time.

Experimental Characterization of Superradiance in a Single-Pass High-Gain Laser-Seeded Free-Electron Laser Amplifier

In this Letter we report the first experimental characterization of superradiance in a single-pass high-gain free-electron laser (FEL) seeded by a 150 femtosecond (FWHM) Ti:sapphire laser. The nonlinear energy gain after an exponential gain regime was observed. We also measured the evolution of the longitudinal phase space in both the exponential and superradiant regimes. The output FEL pulse duration was measured to be as short as 81 fs, a roughly 50% reduction compared to the input seed laser. The temporal distribution of the FEL radiation as predicted by a numerical simulation was experimentally verified for the first time.