Femtosecond Polarization Shaping of Free-Electron Laser Pulses.

We demonstrate the generation of extreme-ultraviolet (XUV) free-electron laser (FEL) pulses with time-dependent polarization. To achieve polarization modulation on a femtosecond timescale, we combine two mutually delayed counterrotating circularly polarized subpulses from two cross-polarized undulators. The polarization profile of the pulses is probed by angle-resolved photoemission and above-threshold ionization of helium; the results agree with solutions of the time-dependent Schrödinger equation. The stability limit of the scheme is mainly set by electron-beam energy fluctuations, however, at a level that will not compromise experiments in the XUV. Our results demonstrate the potential to improve the resolution and element selectivity of methods based on polarization shaping and may lead to the development of new coherent control schemes for probing and manipulating core electrons in matter.

Observation of Magnetic Helicoidal Dichroism with Extreme Ultraviolet Light Vortices.

We report on the experimental evidence of magnetic helicoidal dichroism, observed in the interaction of an extreme ultraviolet vortex beam carrying orbital angular momentum with a magnetic vortex. Numerical simulations based on classical electromagnetic theory show that this dichroism is based on the interference of light modes with different orbital angular momenta, which are populated after the interaction between light and the magnetic topology. This observation gives insight into the interplay between orbital angular momentum and magnetism and sets the framework for the development of new analytical tools to investigate ultrafast magnetization dynamics.

Time-resolved photoelectron imaging of complex resonances in molecular nitrogen.

We have used the FERMI free-electron laser to perform time-resolved photoelectron imaging experiments on a complex group of resonances near 15.38 eV in the absorption spectrum of molecular nitrogen, N2, under jet-cooled conditions. The new data complement and extend the earlier work of Fushitani et al. [Opt. Express 27, 19702-19711 (2019)], who recorded time-resolved photoelectron spectra for this same group of resonances. Time-dependent oscillations are observed in both the photoelectron yields and the photoelectron angular distributions, providing insight into the interactions among the resonant intermediate states. In addition, for most states, we observe an exponential decay of the photoelectron yield that depends on the ionic final state. This observation can be rationalized by the different lifetimes for the intermediate states contributing to a particular ionization channel. Although there are nine resonances within the group, we show that by detecting individual photoelectron final states and their angular dependence, we can identify and differentiate quantum pathways within this complex system.

Tracking attosecond electronic coherences using phase-manipulated extreme ultraviolet pulses.

The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within an XUV pulse sequence opens exciting possibilities for coherent control and multidimensional spectroscopy, but has not been accomplished. Here, we overcome these constraints in a highly time-stabilized and phase-modulated XUV-pump, XUV-probe experiment, which directly probes the evolution and dephasing of an inner subshell electronic coherence. This approach, avoiding any XUV optics for direct pulse manipulation, opens up extensive applications of advanced nonlinear optics and spectroscopy at XUV wavelengths.

Complete Characterization of Phase and Amplitude of Bichromatic Extreme Ultraviolet Light.

Intense, mutually coherent beams of multiharmonic extreme ultraviolet light can now be created using seeded free-electron lasers, and the phase difference between harmonics can be tuned with attosecond accuracy. However, the absolute value of the phase is generally not determined. We present a method for determining precisely the absolute phase relationship of a fundamental wavelength and its second harmonic, as well as the amplitude ratio. Only a few easily calculated theoretical parameters are required in addition to the experimental data.

Chirped pulse amplification in an extreme-ultraviolet free-electron laser.

Chirped pulse amplification in optical lasers is a revolutionary technique, which allows the generation of extremely powerful femtosecond pulses in the infrared and visible spectral ranges. Such pulses are nowadays an indispensable tool for a myriad of applications, both in fundamental and applied research. In recent years, a strong need emerged for light sources producing ultra-short and intense laser-like X-ray pulses, to be used for experiments in a variety of disciplines, ranging from physics and chemistry to biology and material sciences. This demand was satisfied by the advent of short-wavelength free-electron lasers. However, for any given free-electron laser setup, a limit presently exists in the generation of ultra-short pulses carrying substantial energy. Here we present the experimental implementation of chirped pulse amplification on a seeded free-electron laser in the extreme-ultraviolet, paving the way to the generation of fully coherent sub-femtosecond gigawatt pulses in the water window (2.3-4.4 nm).

Generation of Phase-Locked Pulses from a Seeded Free-Electron Laser.

In a coherent control experiment, light pulses are used to guide the real-time evolution of a quantum system. This requires the coherence and the control of the pulses' electric-field carrier waves. In this work, we use frequency-domain interferometry to demonstrate the mutual coherence of time-delayed pulses generated by an extreme ultraviolet seeded free-electron laser. Furthermore, we use the driving seed laser to lock and precisely control the relative phase between the two free-electron laser pulses. This new capability opens the way to a multitude of coherent control experiments, which will take advantage of the high intensity, short wavelength, and short duration of the pulses generated by seeded free-electron lasers.

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.

Spectrotemporal shaping of seeded free-electron laser pulses.

We demonstrate the ability to control and shape the spectrotemporal content of extreme-ultraviolet (XUV) pulses produced by a seeded free-electron laser (FEL). The control over the spectrotemporal properties of XUV light was achieved by precisely manipulating the linear frequency chirp of the seed laser. Our results agree with existing theory, which allows us to retrieve the temporal properties (amplitude and phase) of the FEL pulse from measurements of the spectra as a function of the FEL operating parameters. Furthermore, we show the first direct evidence of the full temporal coherence of FEL light and generate Fourier limited pulses by fine-tuning the FEL temporal phase. The possibility of tailoring the spectrotemporal content of intense short-wavelength pulses represents the first step towards efficient nonlinear optics in the XUV to x-ray spectral region and will enable precise manipulation of core-electron excitations using the methods of coherent quantum control.

Single-shot spectro-temporal characterization of XUV pulses from a seeded free-electron laser.

Intense ultrashort X-ray pulses produced by modern free-electron lasers (FELs) allow one to probe biological systems, inorganic materials and molecular reaction dynamics with nanoscale spatial and femtoscale temporal resolution. These experiments require the knowledge, and possibly the control, of the spectro-temporal content of individual pulses. FELs relying on seeding have the potential to produce spatially and temporally fully coherent pulses. Here we propose and implement an interferometric method, which allows us to carry out the first complete single-shot spectro-temporal characterization of the pulses, generated by an FEL in the extreme ultraviolet spectral range. Moreover, we provide the first direct evidence of the temporal coherence of a seeded FEL working in the extreme ultraviolet spectral range and show the way to control the light generation process to produce Fourier-limited pulses. Experiments are carried out at the FERMI FEL in Trieste.

Can a metal surface repel electric charges?

We show that the interaction between a surface and a charge packet moving parallel to it can become repulsive above a critical relativistic energy. We find that this is true for a lossless dielectric surface and also for a Drude metallic surface--in apparent contrast with such common notions as image charge. This counterintuitive phenomenon occurs for packets larger in the transverse than in the longitudinal (parallel to the motion) direction. The repulsion does not occur for a point charge that is instead attracted at all energies. In addition to the above attractive or repulsive transverse force, there is a longitudinal decelerating force, which for a dielectric corresponds to the Cerenkov effect. Once again, the behavior of a line packet differs from that of a point charge: for a packet with infinite transverse size, the decelerating field decreases to zero as the relativistic factor γ → ∞, whereas, for a point charge, the asymptotic value is finite. These findings have a potential impact not only on fundamental electrodynamics but also on accelerator physics and electron spectroscopy.

Striking influence of the catalyst support and its acid-base properties: new insight into the growth mechanism of carbon nanotubes.

In the accepted mechanisms of carbon nanotube (CNT) growth by catalytic chemical vapor deposition (CCVD), the catalyst support is falsely considered as a passive material whose only role is to prevent catalytic particles from coarsening. The chemical changes that occur to the carbon source molecules on the surface are mainly overlooked. Here, we demonstrate the strong influence of the support on the growth of CNTs and show that it can be tuned by controlling the acid-base character of the support surface. This finding largely clarifies the CCVD growth mechanism. The CNTs' growth stems from the support where the presence of basic sites catalyzes the aromatization and reduces the complexity of CNT precursor molecules. On basic supports, the growth is activated and CNTs are more than 1000 times longer than those produced on acidic supports. These results could be the bedrock of future development of more efficient growth of CNTs on surfaces of functional materials. Finally, the modification of the aciditiy of the catalyst support during the super growth process is also discussed.