Lorenzo Raimondi

Two-colour pump–probe experiments with a twin-pulse-seed extreme ultraviolet free-electron laser

Exploring the dynamics of matter driven to extreme non-equilibrium states by an intense ultrashort X-ray pulse is becoming reality, thanks to the advent of free-electron laser technology that allows development of different schemes for probing the response at variable time delay with a second pulse. Here we report the generation of two-colour extreme ultraviolet pulses of controlled wavelengths, intensity and timing by seeding of high-gain harmonic generation free-electron laser with multiple independent laser pulses. The potential of this new scheme is demonstrated by the time evolution of a titanium-grating diffraction pattern, tuning the two coherent pulses to the titanium M-resonance and varying their intensities. This reveals that an intense pulse induces abrupt pattern changes on a time scale shorter than hydrodynamic expansion and ablation. This result exemplifies the essential capabilities of the jitter-free multiple-colour free-electron laser pulse sequences to study evolving states of matter with element sensitivity.

Tunability experiments at the FERMI@Elettra free-electron laser

FERMI@Elettra is a free electron-laser (FEL)-based user facility that, after two years of commissioning, started preliminary users dedicated runs in 2011. At variance with other FEL user facilities, FERMI@Elettra has been designed to deliver improved spectral stability and longitudinal coherence. The adopted scheme, which uses an external laser to initiate the FEL process, has been demonstrated to be capable of generating FEL pulses close to the Fourier transform limit. We report on the first instance of FEL wavelength tuning, both in a narrow and in a large spectral range (fine- and coarse-tuning). We also report on two different experiments that have been performed exploiting such FEL tuning. We used fine-tuning to scan across the 1s–4p resonance in He atoms, at ≈23.74xa0eV (52.2xa0nm), detecting both UV–visible fluorescence (4p–2s, 400xa0nm) and EUV fluorescence (4p–1s, 52.2xa0nm). We used coarse-tuning to scan the M4,5 absorption edge of Ge (∼29.5xa0eV) in the wavelength region 30–60xa0nm, measured in transmission geometry with a thermopile positioned on the rear side of a Ge thin foil.

Coherent control with a short-wavelength free-electron laser

Researchers demonstrate correlation of two colours (63.0 and 31.5 nm wavelengths) in a free-electron laser and control photoelectron angular distribution by adjusting phase with 3 attosecond resolution.

Invited Article: Coherent imaging using seeded free-electron laser pulses with variable polarization: First results and research opportunities

FERMI@Elettra, the first vacuum ultraviolet and soft X-ray free-electron laser (FEL) using by default a seeded scheme, became operational in 2011 and has been opened to users since December 2012. The parameters of the seeded FERMI FEL pulses and, in particular, the superior control of emitted radiation in terms of spectral purity and stability meet the stringent requirements for single-shot and resonant coherent diffraction imaging (CDI) experiments. The advantages of the intense seeded FERMI pulses with variable polarization have been demonstrated with the first experiments performed using the multipurpose experimental station operated at the diffraction and projection imaging (DiProI) beamline. The results reported here were obtained with fixed non-periodic targets during the commissioning period in 2012 using 20-32 nm wavelength range. They demonstrate that the performance of the FERMI FEL source and the experimental station meets the requirements of CDI, holography, and resonant magnetic scattering in both multi- and single-shot modes. Moreover, we present the first magnetic scattering experiments employing the fully circularly polarized FERMI pulses. The ongoing developments aim at pushing the lateral resolution by using shorter wavelengths provided by double-stage cascaded FERMI FEL-2 and probing ultrafast dynamic processes using different pump-probe schemes, including jitter-free seed laser pump or FEL-pump∕FEL-probe with two color FEL pulses generated by the same electron bunch.

The FERMI free-electron lasers

FERMI is a seeded free-electron laser (FEL) facility located at the Elettra laboratory in Trieste, Italy, and is now in user operation with its first FEL line, FEL-1, covering the wavelength range between 100 and 20u2005nm. The second FEL line, FEL-2, a high-gain harmonic generation double-stage cascade covering the wavelength range 20-4u2005nm, has also completed commissioning and the first user call has been recently opened. An overview of the typical operating modes of the facility is presented.

Widely tunable two-colour seeded free-electron laser source for resonant-pump resonant-probe magnetic scattering

The advent of free-electron laser (FEL) sources delivering two synchronized pulses of different wavelengths (or colours) has made available a whole range of novel pump–probe experiments. This communication describes a major step forward using a new configuration of the FERMI FEL-seeded source to deliver two pulses with different wavelengths, each tunable independently over a broad spectral range with adjustable time delay. The FEL scheme makes use of two seed laser beams of different wavelengths and of a split radiator section to generate two extreme ultraviolet pulses from distinct portions of the same electron bunch. The tunability range of this new two-colour source meets the requirements of double-resonant FEL pump/FEL probe time-resolved studies. We demonstrate its performance in a proof-of-principle magnetic scattering experiment in Fe–Ni compounds, by tuning the FEL wavelengths to the Fe and Ni 3p resonances.

Mirrors for X-ray telescopes: Fresnel diffraction-based computation of point spread functions from metrology

The imaging sharpness of an X-ray telescope is chiefly determined by the optical quality of its focusing optics, which in turn mostly depends on the shape accuracy and the surface finishing of the grazing-incidence X-ray mirrors that compose the optical modules. To ensure the imaging performance during the mirror manufacturing, a fundamental step is predicting the mirror point spread function (PSF) from the metrology of its surface. Traditionally, the PSF computation in X-rays is assumed to be different depending on whether the surface defects are classified as figure errors or roughness. [...] The aim of this work is to overcome this limit by providing analytical formulae that are valid at any light wavelength, for computing the PSF of an X-ray mirror shell from the measured longitudinal profiles and the roughness power spectral density (PSD), without distinguishing spectral ranges with different treatments. The method we adopted is based on the Huygens-Fresnel principle for computing the diffracted intensity from measured or modeled profiles. In particular, we have simplified the computation of the surface integral to only one dimension, owing to the grazing incidence that reduces the influence of the azimuthal errors by orders of magnitude. The method can be extended to optical systems with an arbitrary number of reflections - in particular the Wolter-I, which is frequently used in X-ray astronomy - and can be used in both near- and far-field approximation. Finally, it accounts simultaneously for profile, roughness, and aperture diffraction. We describe the formalism with which one can self-consistently compute the PSF of grazing-incidence mirrors, [...] Finally, we validate this by comparing the simulated PSF of a real Wolter-I mirror shell with the measured PSF in hard X-rays.

Nanoscale dynamics by short-wavelength four wave mixing experiments

Multi-dimensional spectroscopies with vacuum ultraviolet (VUV)/x-ray free-electron laser (FEL) sources would open up unique capabilities for dynamic studies of matter at the femtosecond?nanometer time?length scales. Using sequences of ultrafast VUV/x-ray pulses tuned to electron transitions enables element-specific studies of charge and energy flow between constituent atoms, which embody the very essence of chemistry and condensed matter physics. A remarkable step forward towards this goal would be achieved by extending the four wave mixing (FWM) approach at VUV/soft x-ray wavelengths, thanks to the use of fully coherent sources, such as seeded FELs. Here, we demonstrate the feasibility of VUV/soft x-ray FWM at Fermi@Elettra and we discuss its applicability to probe ultrafast intramolecular dynamics, charge injection processes involving metal oxides and electron correlation and magnetism in solid materials. The main advantage in using VUV/soft x-ray wavelengths is in adding element-sensitivity to FWM methods by exploiting the core resonances of selected atoms in the sample.

Determining the polarization state of an extreme ultraviolet free-electron laser beam using atomic circular dichroism

Ultrafast extreme ultraviolet and X-ray free-electron lasers are set to revolutionize many domains such as bio-photonics and materials science, in a manner similar to optical lasers over the past two decades. Although their number will grow steadily over the coming decade, their complete characterization remains an elusive goal. This represents a significant barrier to their wider adoption and hence to the full realization of their potential in modern photon sciences. Although a great deal of progress has been made on temporal characterization and wavefront measurements at ultrahigh extreme ultraviolet and X-ray intensities, only few, if any progress on accurately measuring other key parameters such as the state of polarization has emerged. Here we show that by combining ultra-short extreme ultraviolet free electron laser pulses from FERMI with near-infrared laser pulses, we can accurately measure the polarization state of a free electron laser beam in an elegant, non-invasive and straightforward manner using circular dichroism.

Two-colour generation in a chirped seeded free-electron laser: a close look

We present the experimental demonstration of a method for generating two spectrally and temporally separated pulses by an externally seeded, single-pass free-electron laser operating in the extreme-ultraviolet spectral range. Our results, collected on the FERMI@Elettra facility and confirmed by numerical simulations, demonstrate the possibility of controlling both the spectral and temporal features of the generated pulses. A free-electron laser operated in this mode becomes a suitable light source for jitter-free, two-colour pump-probe experiments.