arXiv subjects

Emanuele Pedersoli

Publications and source records attributed to Emanuele Pedersoli.

25 records · Page 2Linked to original sources

arXiv2020

Element- and enantiomer-selective visualization of ibuprofen dimer vibrations

In chemistry, biology and materials science, the ability to access interatomic interactions and their dynamical evolution has become possible with the advent of femtosecond lasers. In particular, the observation of vibrational wave packets via optical (UV-visible-IR) spectroscopies has been a major achievement as it can track the motion of nuclei within the system. However, optical spectroscopies only detect the effect of the interatomic vibrations on the global electronic surfaces. New tuneable, pulsed and polarized sources of short-wavelength radiation, such as X-Ray Free electron lasers, can overcome this limitation, allowing for chemical and, of primary importance in biochemistry, enantiomeric selectivity. This selectivity may be complemented by taking into account the chemical shifts of atoms belonging to different molecular moieties

cond-mat.soft↗

arXiv2020

Simultaneous two-color snapshot view on ultrafast charge and spin dynamics in a Fe-Cu-Ni tri-layer

Ultrafast phenomena on a femtosecond timescale are commonly examined by pump-probe experiments. This implies multiple measurements where the sample under investigation is pumped with a short light pulse and then probed with a second pulse at various time delays to follow its dynamics. Recently, the principle of streaking extreme ultraviolet (XUV) pulses in the temporal domain has enabled recording the dynamics of a system within a single pulse. However, separate pump-probe experiments at different absorption edges still lack a unified timing, when comparing the dynamics in complex systems. Here we report on an experiment using a dedicated optical element and the two-color emission of the FERMI XUV free-electron laser to follow the charge and spin dynamics in composite materials at two distinct absorption edges, simultaneously. The sample, consisting of ferromagnetic Fe and Ni layers, separated by a Cu layer, is pumped by an infrared laser and probed by a two-color XUV pulse with photon energies tuned to the M edges of these two transition metals. The experimental geometry intrinsically avoids any timing uncertainty between the two elements and unambiguously reveals an approximately 100 fs delay of the magnetic response with respect to the electronic excitation for both Fe and Ni. This delay shows that the electronic and spin degrees of freedom are decoupled during the demagnetization process. These observations underline the importance of simultaneous investigation of the temporal response of both charge and spin in multi-component materials. In a more general scenario, the experimental approach can be extended to continuous energy ranges, promising the development of jitter-free transient absorption spectroscopy in the XUV and soft X-ray regimes.

cond-mat.mtrl-sci↗

arXiv2019

Pulse-to-pulse wavefront sensing at free-electron lasers using ptychography

The pressing need for the detailed wavefront properties of ultra-bright and ultra-short pulses produced by free-electron lasers (FELs) has spurred the development of several complementary characterization approaches. Here we present a method based on ptychography that can retrieve full high-resolution complex-valued wave functions of individual pulses. Our technique is demonstrated within experimental conditions suited for diffraction experiments in their native imaging state. This lensless technique, applicable to many other short-pulse instruments, can achieve diffraction-limited resolution.

eess.IV↗

arXiv2018

Single shot time-resolved magnetic x-ray absorption at a Free Electron Laser

Ultrafast dynamics are generally investigated using stroboscopic pump-probe measurements, which characterize the sample properties for a single, specific time delay. These measurements are then repeated for a series of discrete time delays to reconstruct the overall time trace of the process. As a consequence, this approach is limited to the investigation of fully reversible phenomena. We recently introduced an off-axis zone plate based X-ray streaking technique, which overcomes this limitation by sampling the relaxation dynamics with a single femtosecond X-ray pulse streaked over a picosecond long time window. In this article we show that the X-ray absorption cross section can be employed as the contrast mechanism in this novel technique. We show that changes of the absorption cross section on the percent level can be resolved with this method. To this end we measure the ultrafast magnetization dynamics in CoDy alloy films. Investigating different chemical compositions and infrared pump fluences, we demonstrate the routine applicability of this technique. Probing in transmission the average magnetization dynamics of the entire film, our experimental findings indicate that the demagnetization time is independent of the specific infrared laser pump fluence. These results pave the way for the investigation of irreversible phenomena in a wide variety of scientific areas.

cond-mat.mtrl-sci↗

arXiv2017

In-situ single-shot diffractive fluence mapping for X-ray free-electron laser pulses

Free-electron lasers (FEL) in the extreme ultraviolet (XUV) and X-ray regime opened up the possibility for experiments at high power densities, in particular allowing for fluence-dependent absorption and scattering experiments to reveal non-linear light-matter interactions at ever shorter wavelengths. Findings of such non-linear effects in the XUV and X-ray regime are met with tremendous interest, but prove difficult to understand and model due to the inherent shot-to-shot fluctuations in photon intensity and the often structured, non-Gaussian spatial intensity profile of a focused FEL beam. Presently, the focused beam spot is characterized and optimized separately from the actual experiment. Here, we present the first simultaneous measurement of diffraction signals from solid samples in tandem with the corresponding single-shot spatial fluence distribution on the actual sample. This new in-situ characterization scheme enables fast and direct monitoring and thus control of the sample illumination which ultimately is necessary for a quantitative understanding of non-linear light-matter interaction in X-ray and XUV FEL experiments.

physics.ins-det↗

arXiv2016

Soft x-rays induce femtosecond solid-to-solid phase transition

Soft x-rays were applied to induce graphitization of diamond through a non-thermal solid-to-solid phase transition. This process was observed within poly-crystalline diamond with a time-resolved experiment using ultrashort soft x-ray pulses of duration 52.5 fs and cross correlated by an optical pulse of duration 32.8 fs. This scheme enabled for the first time the measurement of a phase transition on a timescale of ~150 fs. Excellent agreement between experiment and theoretical predictions was found, using a dedicated code that followed the non-equilibrium evolution of the irradiated diamond including all transient electronic and structural changes. These observations confirm that soft x-rays can induce a non-thermal ultrafast solid-to-solid phase transition on a hundred femtosecond timescale.

physics.atom-ph↗

arXiv2012

Evidence of vectorial photoelectric effect on Copper

Quantum Efficiency (QE) measurements of single photon photoemission from a Cu(111) single crystal and a Cu polycrystal photocathodes, irradiated by 150 fs-6.28 eV laser pulses, are reported over a broad range of incidence angle, both in s and p polarizations. The maximum QE (\simeq 4\times10^{-4}) for polycrystalline Cu is obtained in p polarization at an angle of incidence θ = 65deg. We observe a QE enhancement in p polarization which can not be explained in terms of optical absorption, a phenomenon known as vectorial photoelectric effect. Issues concerning surface roughness and symmetry considerations are addressed. An explanation in terms of non local conductivity tensor is proposed.

cond-mat.mtrl-sci↗