arXiv subjects

Emanuele Pedersoli

Publications and source records attributed to Emanuele Pedersoli.

At least 19 recordsLinked to original sources

arXiv2026

Ultrafast internal dynamics of chiral domain walls probed by time-resolved XRMS

We measure picosecond dynamics of labyrinthine stripe domains with chiral Néel-type domain walls using time-resolved x-ray resonant magnetic scattering (XRMS). At the stripe-domain wavevector, the helicity-summed signal shows ultrafast demagnetization, recovery, and a weak oscillatory contribution that we identify as a signature of laser-launched coherent surface phonons. In contrast, the dichroic signal, which is sensitive to the in-plane magnetization inside the Néel walls, shows a strong oscillatory response whose frequency decreases with increasing pump fluence. We attribute this softening to pump-induced changes in the effective anisotropy and saturation magnetization, which modify the restoring field of an internal domain-wall mode. Time-resolved XRMS thus isolates wall-specific dynamics and provides access to internal domain-wall motion in disordered stripe textures on picosecond time scales.

physics.optics↗

arXiv2026

Ultrafast excitation of Bloch plasmon polaritons in hyperbolic metamaterials with an extreme ultra-violet transient grating

Manipulating materials properties with light drives advances in materials science and photonics. Hyperbolic metamaterials are promising candidates as next-generation quantum optical media. They support Bloch plasmon polaritons, which are characterized by potentially infinite wave-vectors and long lifetimes, but cannot be excited through direct light illumination due to momentum mismatch. Here, we experimentally show that a transient grating, formed via interference of fully coherent seeded free-electron laser pulses in a thin insulator film, enables the excitation of Bloch plasmon polaritons in an underlying hyperbolic metamaterial. Finite element simulations confirm the role of the transient grating in facilitating phase-matching and mode excitation. Our findings demonstrate a route to spatiotemporally excite Bloch plasmon polaritons modes, offering an alternative to permanently nanostructured gratings and potentially enabling ultrafast control of optical modes excitation.

physics.optics↗

arXiv2026

Single-shot imaging with randomized structured illumination at a free electron laser

Stroboscopic nanoscale imaging with free electron laser light is revolutionizing our understanding of fast dynamics in heterogeneous systems. The short wavelength of X-ray and extreme ultraviolet radiation makes it possible to achieve nanoscale resolution, while resonance with atomic transitions gives access to electronic and magnetic degrees of freedom. Here, we report on our implementation of a recently developed imaging method, randomized probe imaging, at a free electron laser. The advantage of randomized probe imaging over existing methods is its compatibility both with extended and strongly scattering samples. Our implementation delivers robust single-shot reconstructions at up to a full-pitch resolution of 400 nm over a field of view with a 40 μm diameter. We also demonstrate single-shot imaging of magnetic domain structures using circular dichroism at resonance, paving the way to future time-resolved studies of magnetic dynamics, shock physics, and the dynamics of collective electronic phases.

physics.optics↗

arXiv2025

Distinct element-specific nanoscale magnetization dynamics following ultrafast laser excitation

Time-resolved ultrafast extreme ultraviolet (EUV) magnetic scattering is used to study laser-driven ultrafast magnetization dynamics of labyrinthine domains in a [Co/Ni/Pt] multilayer. Our measurements at the Co and Ni M-edges reveal distinct ultrafast distortions of the scattering pattern position and width for Ni compared to Co. Ni shows a strong modification of the scattering pattern, approximately 10 to 40 times stronger than Co. As distortions of the labyrinthine pattern in reciprocal space relate to the modification of domain textures in real space, significant differences in Co and Ni highlight a 3D distortion of the domain pattern in the far-from-equilibrium regime.

cond-mat.mtrl-sci↗

arXiv2024

Ultrafast Opto-magnetic Effects in the Extreme Ultraviolet Spectral Range

Coherent light-matter interactions mediated by opto-magnetic phenomena like the inverse Faraday effect (IFE) are expected to provide a non-thermal pathway for ultrafast manipulation of magnetism on timescales as short as the excitation pulse itself. As the IFE scales with the spin-orbit coupling strength of the involved electronic states, photo-exciting the strongly spin-orbit coupled core-level electrons in magnetic materials appears as an appealing method to transiently generate large opto-magnetic moments. Here, we investigate this scenario in a ferrimagnetic GdFeCo alloy by using intense and circularly polarized pulses of extreme ultraviolet radiation. Our results reveal ultrafast and strong helicity-dependent magnetic effects which are in line with the characteristic fingerprints of an IFE, corroborated by ab initio opto-magnetic IFE theory and atomistic spin dynamics simulations.

cond-mat.mtrl-sci↗

arXiv2023

FEL stochastic spectroscopy revealing silicon bond softening dynamics

Time-resolved X-ray Emission/Absorption Spectroscopy (Tr-XES/XAS) is an informative experimental tool sensitive to electronic dynamics in materials, widely exploited in diverse research fields. Typically, Tr-XES/XAS requires X-ray pulses with both a narrow bandwidth and sub-picosecond pulse duration, a combination that in principle finds its optimum with Fourier transform-limited pulses. In this work, we explore an alternative xperimental approach, capable of simultaneously retrieving information about unoccupied (XAS) and occupied (XES) states from the stochastic fluctuations of broadband extreme ultraviolet pulses of a free-electron laser. We used this method, in combination with singular value decomposition and Tikhonov regularization procedures, to determine the XAS/XES response from a crystalline silicon sample at the L2,3-edge, with an energy resolution of a few tens of meV. Finally, we combined this spectroscopic method with a pump-probe approach to measure structural and electronic dynamics of a silicon membrane. Tr-XAS/XES data obtained after photoexcitation with an optical laser pulse at 390 nm allowed us to observe perturbations of the band structure, which are compatible with the formation of the predicted precursor state of a non-thermal solid-liquid phase transition associated with a bond softening phenomenon.

cond-mat.mtrl-sci↗

arXiv2023

Evidence of extreme domain wall speeds under ultrafast optical excitation

Time-resolved ultrafast EUV magnetic scattering was used to test a recent prediction of >10 km/s domain wall speeds by optically exciting a magnetic sample with a nanoscale labyrinthine domain pattern. Ultrafast distortion of the diffraction pattern was observed at markedly different timescales compared to the magnetization quenching. The diffraction pattern distortion shows a threshold-dependence with laser fluence, not seen for magnetization quenching, consistent with a picture of domain wall motion with pinning sites. Supported by simulations, we show that a speed of $\approx$ 66 km/s for highly curved domain walls can explain the experimental data. While our data agree with the prediction of extreme, non-equilibrium wall speeds locally, it differs from the details of the theory, suggesting that additional mechanisms are required to fully understand these effects.

cond-mat.mes-hall↗

arXiv2023

Three-dimensional coherent diffraction snapshot imaging using extreme ultraviolet radiation from a free electron laser

The possibility to obtain a three-dimensional representation of a single object with sub-$μ$m resolution is crucial in many fields, from material science to clinical diagnostics. This is typically achieved through tomography, which combines multiple two-dimensional images of the same object captured at different orientations. However, this serial imaging method prevents single-shot acquisition in imaging experiments at free electron lasers. In the present experiment, we report on a new approach to 3D imaging using extreme-ultraviolet radiation. In this method, two EUV pulses hit simultaneously an isolated 3D object from different sides, generating independent coherent diffraction patterns, resulting in two distinct bidimensional views obtained via phase retrieval. These views are then used to obtain a 3D reconstruction using a ray tracing algorithm. This EUV stereoscopic imaging approach, similar to the natural process of binocular vision, provides sub-$μ$m spatial resolution and single shot capability. Moreover, ultrafast time resolution and spectroscopy can be readily implemented, a further extension to X-ray wavelengths can be envisioned as well.

physics.optics↗

arXiv2022

Robust scenario for the generation of non-equilibrium topological fluctuation states

The recently discovered topological fluctuation state provides a fascinating new perspective on the ultrafast emergence of topology in condensed matter systems. However, rather little is known about the physics of this state and the origin of the topological fluctuations. Using time-resolved small-angle x-ray scattering, we observe that topological fluctuation states appear after laser excitation even if the final state does not host stable skyrmions. Simulations support these findings and reveal that the fluctuations originate from the competition between spontaneous nucleation and decay of skyrmions, consistent with Arrhenius-like activation over a potential barrier. Stable skyrmions can freeze out of such fluctuations when the effective temperature of the system relaxes faster than the decay time of the skyrmions. Our results reveal a robust scenario for the generation of topological fluctuation states, potentially enabling their study in a wide variety of magnetic systems.

cond-mat.mtrl-sci↗

arXiv2022

Atom-Specific Probing of Electron Dynamics in an Atomic Adsorbate by Time-Resolved X-ray Spectroscopy

The electronic excitation occurring on adsorbates at ultrafast time scales from optical lasers that initiate surface chemical reactions is still an open question. Here, we report the ultrafast temporal evolution of X-ray absorption spectroscopy (XAS) and X-ray emission spectroscopy (XES) of a simple well known adsorbate prototype system, namely carbon (C) atoms adsorbed on a nickel (Ni(100)) surface, following intense laser optical pumping at 400 nm. We observe ultrafast (~100 fs) changes in both XAS and XES showing clear signatures of the formation of a hot electron-hole pair distribution on the adsorbate. This is followed by slower changes on a few ps time scale, shown to be consistent with thermalization of the complete C/Ni system. Density functional theory spectrum simulations support this interpretation.

physics.chem-ph↗

arXiv2022

High energy-resolution transient ghost absorption spectroscopy

We demonstrate the measurement of ultrafast dynamics using ghost spectroscopy and a pump-probe approach with an optical pump and a short-wavelength radiation probe. The ghost spectroscopy approach is used to overcome the challenge of the strong intensity and spectrum fluctuations at free-electron lasers and to provide high -spectral resolution, which enables the measurement of small energy shifts in the absorption spectrum. We exploit the high resolution to explore the dynamics of the charge carrier excitations and relaxations and their impact on the photoinduced structural changes in silicon by measuring the variation of the absorption spectrum of a Si(100) membrane near the silicon L2,3 edge and the accompanying edge shifts in response to the optical illumination.

physics.optics↗

arXiv2022

All-optical switching on the nanometer scale excited and probed with femtosecond extreme ultraviolet pulses

Ultrafast control of magnetization on the nanometer length scale, in particular all-optical switching, is key to putting ultrafast magnetism on the path towards future technological application in data storage technology. However, magnetization manipulation with light on this length scale is challenging due to the wavelength limitations of optical radiation. Here, we excite transient magnetic gratings in a GdFe alloy with a periodicity of 87 nm by interference of two coherent femtosecond light pulses in the extreme ultraviolet spectral range at the free electron laser facility FERMI. The subsequent ultrafast evolution of the magnetization pattern is probed by diffraction of a third, time-delayed pulse tuned to the Gd N-edge at a wavelength of 8.3 nm. By examining the simultaneously recorded first and second diffraction orders and by performing reference real-space measurements with a wide-field magneto-optical microscope with femtosecond time resolution, we can conclusively demonstrate the ultrafast emergence of all-optical switching on the nanometer length scale.

cond-mat.mtrl-sci↗

arXiv2022

High-resolution absorption measurements with free-electron lasers using ghost spectroscopy

We demonstrate a simple and robust high-resolution ghost spectroscopy approach for x-ray and extreme ultraviolet absorption spectroscopy at free-electron laser sources. Our approach requires an on-line spectrometer before the sample and a downstream bucket detector. We use this method to measure the absorption spectrum of silicon, silicon carbide and silicon nitride membranes in the vicinity of the silicon L2,3-edge. We show that ghost spectroscopy allows the high-resolution reconstruction of the sample spectral response using a coarse energy scan with self-amplified spontaneous emission radiation. For the conditions of our experiment the energy resolution of the ghost-spectroscopy reconstruction is higher than the energy resolution reached by scanning the energy range by narrow spectral bandwidth radiation produced by the seeded free-electron laser. When we set the photon energy resolution of the ghost spectroscopy to be equal to the resolution of the measurement with the seeded radiation, the measurement time with the ghost spectroscopy method is shorter than scanning the photon energy with seeded radiation. The exact conditions for which ghost spectroscopy can provide higher resolution at shorter times than measurement with narrow band scans depend on the details of the measurements and on the properties of the samples and should be addressed in future studies.

physics.ins-det↗

arXiv2021

Ultrafast adsorbate excitation probed with sub-ps resolution XAS

We use a pump-probe scheme to measure the time evolution of the C K-edge X-ray absorption spectrum (XAS) from CO/Ru(0001) after excitation by an ultrashort high-intensity optical laser pulse. Due to the short duration of the X-ray probe pulse and precise control of the pulse delay, the excitation-induced dynamics during the first ps after the pump can be resolved with unprecedented time resolution. By comparing with theoretical (DFT) spectrum calculations we find high excitation of the internal stretch and frustrated rotation modes occurring within 200 fs of laser excitation, as well as thermalization of the system in the ps regime. The ~100 fs initial excitation of these CO vibrational modes is not readily rationalized by traditional theories of nonadiabatic coupling of adsorbates to metal surfaces, e. g. electronic frictions based on first order electron-phonon coupling or transient population of adsorbate resonances. We suggest that coupling of the adsorbate to non-thermalized electron-hole pairs is responsible for the ultrafast initial excitation of the modes.

physics.chem-ph↗

arXiv2021

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 the light phase chirality 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.

physics.optics↗

arXiv2021

Faster chiral versus collinear magnetic order recovery after optical excitation revealed by femtosecond XUV scattering

While chiral spin structures stabilized by Dzyaloshinskii-Moriya interaction (DMI) are candidates as novel information carriers, their dynamics on the fs-ps timescale is little known. Since with the bulk Heisenberg exchange and the interfacial DMI two distinct exchange mechanisms are at play, the ultra-fast dynamics of the chiral order needs to be ascertained and compared to the dynamics of the conventional collinear order. Using an XUV free-electron laser we determine the fs-ps temporal evolution of the chiral order in domain walls in a magnetic thin film sample by an IR pump - X-ray magnetic scattering probe experiment. Upon demagnetisation we observe that the dichroic (CL-CR) signal connected with the chiral order correlator $m_z m_x$ in the domain walls recovers significantly faster than the (CL+CR) sum signal representing the average collinear domain magnetisation $m_z^2 + m_x^2$. We explore possible explanations based on spin structure dynamics and reduced transversal magnetisation fluctuations inside the domain walls and find that the latter can explain the experimental data leading to different dynamics for collinear magnetic order and chiral magnetic order.

cond-mat.mtrl-sci↗

arXiv2021

Ultrafast time-evolution of chiral Néel magnetic domain walls probed by circular dichroism in x-ray resonant magnetic scattering

Non-collinear spin textures in ferromagnetic ultrathin films are attracting a renewed interest fueled by possible fine engineering of several magnetic interactions, notably the interfacial Dzyaloshinskii-Moriya interaction. This allows the stabilization of complex chiral spin textures such as chiral magnetic domain walls (DWs), spin spirals, and magnetic skyrmions. We report here on the ultrafast behavior of chiral DWs after optical pumping in perpendicularly magnetized asymmetric multilayers, probed using time-resolved circular dichroism in x-ray resonant magnetic scattering (CD-XRMS). We observe a picosecond transient reduction of the CD-XRMS, which is attributed to the spin current-induced coherent and incoherent torques within the continuously dependent spin texture of the DWs. We argue that a specific demagnetization of the inner structure of the DW induces a flow of hot spins from the interior of the neighboring magnetic domains. We identify this time-varying change of the DW textures shortly after the laser pulse as a distortion of the homochiral N'eel shape toward a transient mixed Bloch-Néel-Bloch textures along a direction transverse to the DW. Our study highlights how time-resolved CD-XRMS can be a unique tool for studying the time evolution in other systems showing a non-collinear electric/magnetic ordering such as skyrmion lattices, conical/helical phases, as well as the recently observed antiskyrmion lattices, in metallic or insulating materials.

cond-mat.mtrl-sci↗

arXiv2020

Time-Resolved XUV absorption spectroscopy and magnetic circular dichroism at the Ni $M_{2,3}$-edges

Ultrashort optical pulses can trigger a variety of non-equilibrium processes in magnetic thin films affecting electrons and spins on femtosecond timescales. In order to probe the charge and magnetic degrees of freedom simultaneously, we developed an x-ray streaking technique that has the advantage of providing a jitter-free picture of absorption cross section changes. In this paper, we present an experiment based on this approach which we performed using five photon probing energies at the Ni $M_{2,3}$-edges. This allowed us to retrieve the absorption and magnetic circular dichroism time traces, yielding detailed information on transient modifications of electron and spin populations close to the Fermi level. Our findings suggest that the observed charge and magnetic dynamics both depend on the XUV probing wavelength, and can be described, at least qualitatively, by assuming ultrafast energy shifts of the electronic and magnetic elemental absorption resonances, as reported in recent work. However, our analysis also hints at more complex changes, highlighting the need for further experimental and theoretical analysis in order to gain a thorough understanding of the interplay of electronic and spin degrees of freedom in optically excited magnetic thin films.

cond-mat.mtrl-sci↗