Extreme Ultraviolet Free-electron Laser Pulses Research Articles

Generation and measurement of intense few-femtosecond superradiant extreme-ultraviolet free-electron laser pulses

Free-electron lasers producing ultrashort pulses with high peak power promise to extend ultrafast non-linear spectroscopic techniques into the extreme-ultraviolet–X-ray regime. Key aspects are the synchronization between pump and probe, and the control of the pulse properties (duration, intensity and coherence). Externally seeded free-electron lasers produce coherent pulses that can be synchronized with femtosecond accuracy. An important goal is to shorten the pulse duration, but the simple approach of shortening the seed is not sufficient because of the finite-gain bandwidth of the conversion process. An alternative is the amplification of a soliton in a multistage, superradiant cascade: here, we demonstrate the generation of few-femtosecond extreme-ultraviolet pulses, whose duration we measure by autocorrelation. We achieve pulses four times shorter, and with a higher peak power, than in the standard high-gain harmonic generation mode and we prove that the pulse duration matches the Fourier transform limit of the spectral intensity distribution. By amplifying a soliton in a multistage cascade, few-femtosecond extreme-ultraviolet free-electron laser pulses are achieved.

Measuring the frequency chirp of extreme-ultraviolet free-electron laser pulses by transient absorption spectroscopy

High-intensity ultrashort pulses at extreme ultraviolet (XUV) and x-ray photon energies, delivered by state-of-the-art free-electron lasers (FELs), are revolutionizing the field of ultrafast spectroscopy. For crossing the next frontiers of research, precise, reliable and practical photonic tools for the spectro-temporal characterization of the pulses are becoming steadily more important. Here, we experimentally demonstrate a technique for the direct measurement of the frequency chirp of extreme-ultraviolet free-electron laser pulses based on fundamental nonlinear optics. It is implemented in XUV-only pump-probe transient-absorption geometry and provides in-situ information on the time-energy structure of FEL pulses. Using a rate-equation model for the time-dependent absorbance changes of an ionized neon target, we show how the frequency chirp can be directly extracted and quantified from measured data. Since the method does not rely on an additional external field, we expect a widespread implementation at FELs benefiting multiple science fields by in-situ on-target measurement and optimization of FEL-pulse properties.

EUV stimulated emission from MgO pumped by FEL pulses.

Stimulated emission is a fundamental process in nature that deserves to be investigated and understood in the extreme ultra-violet (EUV) and x-ray regimes. Today, this is definitely possible through high energy density free electron laser (FEL) beams. In this context, we give evidence for soft-x-ray stimulated emission from a magnesium oxide solid target pumped by EUV FEL pulses formed in the regime of travelling-wave amplified spontaneous emission in backward geometry. Our results combine two effects separately reported in previous works: emission in a privileged direction and existence of a material-dependent threshold for the stimulated emission. We develop a novel theoretical framework, based on coupled rate and transport equations taking into account the solid-density plasma state of the target. Our model accounts for both observed mechanisms that are the privileged direction for the stimulated emission of the Mg L2,3 characteristic emission and the pumping threshold.

Photoelectron angular distributions in infrared one-photon and two-photon ionization of FEL-pumped Rydberg states of helium

The photoelectron angular distributions (PADs) have been investigated for infrared (IR) ionization of He atoms excited to Rydberg states by extreme ultraviolet free-electron laser pulses. The experiment was carried out with two pulses which do not overlap in time. Depending on the intensity of the IR pulses, one IR photon ionization or additionally two-photon above-threshold ionization is observed. For low IR intensity, the PAD is well described by a contribution of s and d partial waves in accordance with early experiments. At high IR intensity, the PAD for two IR photon ionization clearly shows the contribution of higher partial waves. The experimental data are compared with the results of theoretical calculations based on solving the time-dependent Schrödinger equation.

Photoelectron angular distributions for the two-photon sequential double ionization of xenon by ultrashort extreme ultraviolet free electron laser pulses

Xenon atoms are double-ionized by sequential two-photon absorption by ultrashort extreme ultraviolet free-electron laser pulses with a photon energy of 23.0 and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The angular distributions of photoelectrons generated by two-photon double ionization are obtained using velocity map imaging. The results are reproduced reasonably well by the present theoretical calculations within the multi-configurational Dirac–Fock approach.

Photoelectron angular distributions for the two-photon ionization of helium by ultrashort extreme ultraviolet free-electron laser pulses

The two-photon ionization of helium atoms by ultrashort extreme-ultraviolet free-electron laser pulses, produced by the SPring-8 Compact SASE Source test accelerator, was investigated at photon energies of 20.3, 21.3, 23.0 and 24.3 eV. The angular distribution of photoelectrons generated by two-photon ionization is obtained using a velocity map imaging spectrometer. The phase-shift differences and amplitude ratios of the outgoing s and d continuum wave packets are extracted from the photoelectron angular distributions. The obtained values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to a resonance with an excited level or Rydberg manifold. The difference stems from the co-presence of resonant and non-resonant path contributions in the two-photon ionization by femtosecond pulses. Since the relative contribution of both paths can be controlled in principle by the pulse shape, these results illustrate a new way to tailor the continuum wave packet.

Doubly resonant three-photon double ionization of Ar atoms induced by an EUV free-electron laser

A mechanism for three-photon double ionization of atoms by extreme-ultraviolet free-electron laser pulses is revealed, where in a sequential process the second ionization step, proceeding via resonant two-photon ionization of ions, is strongly enhanced by the excitation of ionic autoionizing states. In contrast to the conventional model, the mechanism explains the observed relative intensities of photoelectron peaks and their angular dependence in three-photon double ionization of argon.

Ion-ion coincidence studies on multiple ionizations of N2 and O2 molecules irradiated by extreme ultraviolet free-electron laser pulses

We have investigated multiple ionization of N(2) and O(2) molecules by 52 nm extreme-ultraviolet light pulses at the free-electron laser facility SCSS in Japan. Coulomb break-up of parent ions with charge states up to 5+ is found by the ion-ion coincidence technique. The charge-state dependence of kinetic energy release distributions suggests that the electrons are emitted sequentially in competition with the elongation of the bond length.

Frustration of direct photoionizations of rare gas clusters in intense extreme ultraviolet free-electron laser pulses

We performed a momentum imaging measurements of Ar clusters irradiated by extreme ultraviolet free electron laser pulses (61nm 1.3×1011W/cm2) for various cluster sizes. Dominant fragment ions were Ar+ and Ar2+ ions with significant kinetic energy (up to 40eV). This indicates that Ar clusters absorbed many photons, become highly ionized and finally dissociated into many fragments through Coulomb explosion. The size dependence of the ion kinetic energy distribution indicates that larger clusters significantly suffer from the frustration of direct photoelectron emissions and multiple ionizations.

Frustration of direct photoionizations of argon clusters irradiated with intense EUV-FEL pulses

We have measured the kinetic energies of fragment ions from Ar clusters (average cluster size <N> ∼ 10 to 600) exposed to intense extreme ultraviolet free-electron laser pulses (λ ∼ 61nm, I ∼ 1.3×1011 [W/cm2]). We found that the average kinetic energy of fragment ions was saturated for <N> ≳ 200.

Single-shot timing measurement of extreme-ultraviolet free-electron laser pulses

Arrival time fluctuations of extreme-ultraviolet (EUV) pulses from the free-electron laser in Hamburg (FLASH) are measured single-pulse resolved at the experimental end-station. To this end, they are non-collinearly superimposed in space and time with visible femtosecond laser pulses on a GaAs substrate. The EUV irradiation induces changes of the reflectivity for the visible pulse. The temporal delay between the two light pulses is directly encoded in the spatial position of the reflectivity change which is captured with a CCD camera. For each single shot, the relative EUV/visible arrival-time can be measured with about 40 fs rms accuracy. The method constitutes a novel route for an improvement of future pump–probe experiments at short-wavelength free-electron lasers (FELs) by a pulse-wise correction with simultaneously measured arrival times of individual EUV pulses.