arXiv subjects

Federico Pressacco

Publications and source records attributed to Federico Pressacco.

16 recordsLinked to original sources

arXiv2026

Femtosecond concerted rotation of molecules on a 2D material interface

Interfaces between molecules and 2D materials exhibit energy-driven functionalities, wherein charge transfer directs molecular motion. Unlike equilibrium systems, where molecular assemblies settle into static configurations, continuous energy input can drive transient, collective molecular rearrangements. Here, we reveal ultrafast spectroscopic fingerprints of a collective rotational response of molecules on a 2D material following photoexcitation. Our results suggest that photoinduced charge transfer reshapes the interfacial energy potential, giving rise to macroscopic, unidirectional molecular rotation and the formation of a homochiral molecular arrangement. Using a multiplexed ultrafast photoemission spectroscopy approach, we simultaneously track, electronic states, atomic positions, and orbital wavefunctions with femtosecond and sub-ångström resolution. Multimodal valence and core electron emission analysis disentangles the intertwined electronic-structural dynamics of the molecule and the 2D material, revealing the dynamic modulation of charge distribution and intermolecular forces that drive collective molecular motion. Our findings open a pathway for designing energy-driven molecular systems with tunable interfacial dynamics, with potential applications in chiral engineering and active matter systems.

cond-mat.mtrl-sci↗

arXiv2024

Laser induced ultrafast Gd 4f spin dynamics at the surface of amorphous CoxGd100-x ferrimagnetic alloys

We have investigated the laser induced ultrafast dynamics of Gd 4f spins at the surface of CoxGd100-x alloys by means of surface-sensitive and time-resolved dichroic resonant Auger spectroscopy. We have observed that the laser induced quenching of Gd 4f magnetic order at the surface of the CoxGd100-x alloys occur on a much longer time scale than that previously reported in bulk sensitive time-resolved experiments. In parallel, we have characterized the static structural and magnetic properties at the surface and in the bulk of these alloys by combining Physical Property Measurement System (PPMS) magnetometry with X-ray Magnetic Circular Dichroism in absorption spectroscopy (XMCD) and X-Ray Photoelectron spectroscopy (XPS). The PPMS and XMCD measurements give information regarding the composition in the bulk of the alloys. The XPS measurements show non-homogeneous composition at the surface of the alloys with a strongly increased Gd content within the first layers compared to the nominal bulk values. Such larger Gd concentration results in a reduced indirect Gd 4f spin-lattice coupling. It explains the slower Gd 4f demagnetization we have observed in our surface-sensitive and time-resolved measurements compared to that previously reported by bulk-sensitive measurements.

cond-mat.mtrl-sci↗

arXiv2023

Real-time observation of phonon-electron energy and angular momentum flow in laser-heated nickel

Identifying the microscopic nature of non-equilibrium energy transfer mechanisms among electronic, spin and lattice degrees of freedom is central for understanding ultrafast phenomena such as manipulating magnetism on the femtosecond timescale. Here we use time and angle-resolved photoemission spectroscopy to go beyond the often-employed ensemble-averaged view of non-equilibrium dynamics in terms of quasiparticle temperature evolutions. We show for ferromagnetic Ni that the non-equilibrium electron and spin dynamics display pronounced variations with electron momentum whereas the magnetic exchange interaction remains isotropic. This highlights the influence of lattice-mediated scattering processes and opens a pathway towards unraveling the still elusive microscopic mechanism of spin-lattice angular momentum transfer.

cond-mat.mtrl-sci↗

arXiv2023

New insights into the laser-assisted photoelectric effect from solid-state surfaces

Photoemission from a solid surface provides a wealth of information about the electronic structure of the surface and its dynamic evolution. Ultrafast pump-probe experiments are particularly useful to study the dynamic interactions of photons with surfaces as well as the ensuing electron dynamics induced by these interactions. Time-resolved laser-assisted photoemission (tr-LAPE) from surfaces is a novel technique to gain deeper understanding of the fundamentals underlying the photoemission process. Here, we present the results of a femtosecond time-resolved soft X-ray photoelectron spectroscopy experiment on two different metal surfaces conducted at the X-ray Free-Electron Laser FLASH in Hamburg. We study photoemission from the W 4f and Pt 4f core levels using ultrashort soft X-ray pulses in combination with synchronized infrared (IR) laser pulses. When both pulses overlap in time and space, laser-assisted photoemission results in the formation of a series of sidebands that reflect the dynamics of the laser-surface interaction. We demonstrate a qualitatively new level of sideband generation up to the sixth order and a surprising material dependence of the number of sidebands that has so far not been predicted by theory. We provide a semi-quantitative explanation of this phenomenon based on the different dynamic dielectric responses of the two materials. Our results advance the understanding of the LAPE process and reveal new details of the IR field present in the surface region, which is determined by the dynamic interplay between the IR laser field and the dielectric response of the metal surfaces.

cond-mat.mtrl-sci↗

arXiv2023

Out-of-equilibrium charge redistribution in a copper-oxide based superconductor by time-resolved X-ray photoelectron spectroscopy

Charge-transfer excitations are of paramount importance for understanding the electronic structure of copper-oxide based high-temperature superconductors. In this study, we investigate the response of a Bi$_2$Sr$_2$CaCu$_2$O$_{\mathrm{8}+ δ}$ crystal to the charge redistribution induced by an infrared ultrashort pulse. Element-selective time-resolved core-level photoelectron spectroscopy with a high energy resolution allows disentangling the dynamics of oxygen ions with different coordination and bonds thanks to their different chemical shifts. Our experiment shows that the O\,$1s$ component arising from the Cu-O planes is significantly perturbed by the infrared light pulse. Conversely, the apical oxygen, also coordinated with Sr ions in the Sr-O planes, remains unaffected. This result highlights the peculiar behavior of the electronic structure of the Cu-O planes. It also unlocks the way to study the out-of-equilibrium electronic structure of copper-oxide-based high-temperature superconductors by identifying the O\,$1s$ core-level emission originating from the oxygen ions in the Cu-O planes. This ability could be critical to gain information about the strongly-correlated electron ultrafast dynamical mechanisms in the Cu-O plane in the normal and superconducting phases.

cond-mat.str-el↗

arXiv2022

Multispectral time-resolved energy-momentum microscopy using high-harmonic extreme ultraviolet radiation

A 790-nm-driven high-harmonic generation source with a repetition rate of 6 kHz is combined with a toroidal-grating monochromator and a high-detection-efficiency photoelectron time-of-flight momentum microscope to enable time- and momentum-resolved photoemission spectroscopy over a spectral range of $23.6$-$45.5$ eV with sub-100-fs time resolution. Three-dimensional (3D) Fermi surface mapping is demonstrated on graphene-covered Ir(111) with energy and momentum resolutions of $\lesssim$$100$ meV and $\lesssim$$0.1$ $Å^{-1}$, respectively. The table-top experiment sets the stage for measuring the $k_z$-dependent ultrafast dynamics of 3D electronic structure, including band structure, Fermi surface, and carrier dynamics in 3D materials as well as 3D orbital dynamics in molecular layers.

cond-mat.mtrl-sci↗

arXiv2022

Tracking the surface atomic motion in a coherent phonon oscillation

X-ray photoelectron diffraction is a powerful tool for determining the structure of clean and adsorbate-covered surfaces. Extending the technique into the ultrafast time domain will open the door to studies as diverse as the direct determination of the electron-phonon coupling strength in solids and the mapping of atomic motion in surface chemical reactions. Here we demonstrate time-resolved photoelectron diffraction using ultrashort soft X-ray pulses from the free electron laser FLASH. We collect Se 3d photoelectron diffraction patterns over a wide angular range from optically excited Bi$_2$Se$_3$ with a time resolution of 140 fs. Combining these with multiple scattering simulations allows us to track the motion of near-surface atoms within the first 3 ps after triggering a coherent vibration of the A$_{1g}$ optical phonons. Using a fluence of 4.2 mJ/cm$^2$ from a 1.55 eV pump laser, we find the resulting coherent vibrational amplitude in the first two interlayer spacings to be on the order of 1 pm.

cond-mat.mtrl-sci↗

arXiv2022

Melting of magnetic order in ${\mathrm{NaOsO}}_{3}$ by fs laser pulses

NaOsO$_3$ has recently attracted significant attention for the strong coupling between its electronic band structure and magnetic ordering. Here, we used time-resolved magnetic X-ray diffraction to determine the timescale of the photoinduced \afm dynamics in NaOsO$_3$. Our measurements are consistent with a sub-100~fs melting of the \afm long-range order, that occurs significantly faster than the lattice dynamics as monitored by the transient change in intensity of selected Bragg structural reflections, which instead show a decrease of intensity on a timescale of several ps.

cond-mat.str-el↗

arXiv2021

Ultrafast electronic line width broadening in the C 1s core level of graphene

Core level binding energies and absorption edges are at the heart of many experimental techniques concerned with element-specific structure, electronic structure, chemical reactivity, elementary excitations and magnetism. X-ray photoemission spectroscopy (XPS) in particular, can provide information about the electronic and vibrational many-body interactions in a solid as these are reflected in the detailed energy distribution of the photoelectrons. Ultrafast pump-probe techniques add a new dimension to such studies, introducing the ability to probe a transient state of the many-body system. Here we use a free electron laser to investigate the effect of a transiently excited electron gas on the core level spectrum of graphene, showing that it leads to a large broadening of the C 1s peak. Confirming a decade-old prediction, the broadening is found to be caused by an exchange of energy and momentum between the photoemitted core electron and the hot electron system, rather than by vibrational excitations. This interpretation is supported by a line shape analysis that accounts for the presence of the excited electrons. Fitting the spectra to this model directly yields the electronic temperature of the system, in agreement with electronic temperature values obtained from valence band data. Furthermore, making use of time- and momentum-resolved C 1s spectra, we illustrate how the momentum change of the outgoing core electrons leads to a small but detectable change in the time-resolved photoelectron diffraction pattern and to a nearly complete elimination of the core level binding energy variation associated with the narrow $σ$-band in the C 1s state. The results demonstrate that the XPS line shape can be used as an element-specific and local probe of the excited electron system and that X-ray photoelectron diffraction investigations remain feasible at very high electronic temperatures.

cond-mat.str-el↗

arXiv2021

Ultrafast MHz-rate burst-mode pump-probe laser for the FLASH FEL facility based on nonlinear compression of ps-level pulses from an Yb-amplifier chain

The Free-Electron Laser (FEL) FLASH offers the worldwide still unique capability to study ultrafast processes with high-flux, high-repetition rate XUV and soft X-ray pulses. The vast majority of experiments at FLASH are of pump-probe type. Many of them rely on optical ultrafast lasers. Here, a novel FEL facility laser is reported which combines high average power output from Yb:YAG amplifiers with spectral broadening in a Herriott-type multi-pass cell and subsequent pulse compression to sub-100 fs durations. Compared to other facility lasers employing optical parametric amplification, the new system comes with significantly improved noise figures, compactness, simplicity and power efficiency. Like FLASH, the optical laser operates with 10 Hz burst repetition rate. The bursts consist of 800 $μ$s long trains of up to 800 ultrashort pulses being synchronized to the FEL with femtosecond precision. In the experimental chamber, pulses with up to 50 $μ$J energy, 60 fs FWHM duration and 1 MHz rate at 1.03 $μ$m wavelength are available and can be adjusted by computer-control. Moreover, nonlinear polarization rotation is implemented to improve laser pulse contrast. First cross-correlation measurements with the FEL at the plane-grating monochromator photon beamline are demonstrated, exhibiting the suitability of the laser for user experiments at FLASH.

physics.optics↗

arXiv2021

Subpicosecond metamagnetic phase transition driven by non-equilibrium electron dynamics

Femtosecond light-induced phase transitions between different macroscopic orders provide the possibility to tune the functional properties of condensed matter on ultrafast timescales. In first-order phase transitions, transient non-equilibrium phases and inherent phase coexistence often preclude non-ambiguous detection of transition precursors and their temporal onset. Here, we present a study combining time-resolved photoelectron spectroscopy and ab-initio electron dynamics calculations elucidating the transient subpicosecond processes governing the photoinduced generation of ferromagnetic order in antiferromagnetic FeRh. The transient photoemission spectra are accounted for by assuming that not only the occupation of electronic states is modified during the photoexcitation process. Instead, the photo-generated non-thermal distribution of electrons modifies the electronic band structure. The ferromagnetic phase of FeRh, characterized by a minority band near the Fermi energy, is established 350+- 30 fs after the laser excitation. Ab-initio calculations indicate that the phase transition is initiated by a photoinduced Rh-to-Fe charge transfer.

cond-mat.str-el↗

arXiv2020

Observation of an excitonic Mott transition through ultrafast core-$\textit{cum}$-conduction photoemission spectroscopy

Time-resolved soft-X-ray photoemission spectroscopy is used to simultaneously measure the ultrafast dynamics of core-level spectral functions and excited states upon excitation of excitons in WSe$_2$. We present a many-body approximation for the Green's function, which excellently describes the transient core-hole spectral function. The relative dynamics of excited-state signal and core levels reveals a delayed core-hole renormalization due to screening by excited quasi-free carriers, revealing an excitonic Mott transition. These findings establish time-resolved core-level photoelectron spectroscopy as a sensitive probe of subtle electronic many-body interactions and an ultrafast electronic phase transition.

cond-mat.mes-hall↗

arXiv2020

Single-layer graphene on epitaxial FeRh thin films

Graphene is a 2D material that displays excellent electronic transport properties with prospective applications in many fields. Inducing and controlling magnetism in the graphene layer, for instance by proximity of magnetic materials, may enable its utilization in spintronic devices. This paper presents fabrication and detailed characterization of single-layer graphene formed on the surface of epitaxial FeRh thin films. The magnetic state of the FeRh surface can be controlled by temperature, magnetic field or strain due to interconnected order parameters. Characterization of graphene layers by X-ray Photoemission and X-ray Absorption Spectroscopy, Low-Energy Ion Scattering, Scanning Tunneling Microscopy, and Low-Energy Electron Microscopy shows that graphene is single-layer, polycrystalline and covers more than 97% of the substrate. Graphene displays several preferential orientations on the FeRh(001) surface with unit vectors of graphene rotated by 30°, 15°, 11°, and 19° with respect to FeRh substrate unit vectors. In addition, the graphene layer is capable to protect the films from oxidation when exposed to air for several months. Therefore, it can be also used as a protective layer during fabrication of magnetic elements or as an atomically thin spacer, which enables incorporation of switchable magnetic layers within stacks of 2D materials in advanced devices.

cond-mat.mtrl-sci↗

arXiv2019

Time- and momentum-resolved photoemission studies using time-of-flight momentum microscopy at a free-electron laser

Time-resolved photoemission with ultrafast pump and probe pulses is an emerging technique with wide application potential. Real-time recording of non-equilibrium electronic processes, transient states in chemical reactions or the interplay of electronic and structural dynamics offers fascinating opportunities for future research. Combining valence-band and core-level spectroscopy with photoelectron diffraction for electronic, chemical and structural analysis requires few 10 fs soft X-ray pulses with some 10 meV spectral resolution, which are currently available at high repetition rate free-electron lasers. The PG2 beamline at FLASH (DESY, Hamburg) provides a high pulse rate of 5000 pulses/s, 60 fs pulse duration and 40 meV bandwidth in an energy range of 25-830 eV with a photon beam size down to 50 microns in diameter. We have constructed and optimized a versatile setup commissioned at FLASH/PG2 that combines FEL capabilities together with a multidimensional recording scheme for photoemission studies. We use a full-field imaging momentum microscope with time-of-flight energy recording as the detector for mapping of 3D band structures in ($k_x$, $k_y$, $E$) parameter space with unprecedented efficiency. Our instrument can image full surface Brillouin zones with up to 7 Å $^{-1}$ diameter in a binding-energy range of several eV, resolving about $2.5\times10^5$ data voxels. As an example, we present results for the ultrafast excited state dynamics in the model van der Waals semiconductor WSe$_2$.

cond-mat.mtrl-sci↗

arXiv2018

Laser induced phase transition in epitaxial FeRh layers studied by pump-probe valence band photoemission

We use time-resolved X-ray photoelectron spectroscopy to probe the electronic and magnetization dynamics in FeRh films after ultrafast laser excitations. We present experimental and theoretical results which investigate the electronic structure of the FeRh during the first-order phase transition identifying a clear signature of the magnetic phase. We find that a spin polarized feature at the Fermi edge is a fingerprint of the magnetic status of the system that is independent of the long-range ferromagnetic alignment of the magnetic domains. We use this feature to follow the phase transition induced by a laser pulse in a pump-probe experiment and find that the magnetic transition occurs in less than 50 ps, and reaches its maximum in 100 ps.

cond-mat.str-el↗

arXiv2015

Stable room-temperature ferromagnetic phase at the FeRh(100) surface

Interfaces and low dimensionality are sources of strong modifications of electronic, structural, and magnetic properties of materials. FeRh alloys are an excellent example because of the first-order phase transition taking place at $\sim$400 K from an antiferromagnetic phase at room temperature to a high temperature ferromagnetic one. It is accompanied by a resistance change and volume expansion of about 1\%. We have investigated the electronic and magnetic properties of FeRh(100) epitaxially grown on MgO by combining spectroscopies characterized by different probing depths, namely X-ray magnetic circular dichroism and photoelectron spectroscopy. We thus reveal that the symmetry breaking induced at the Rh-terminated surface stabilizes a surface ferromagnetic layer involving five planes of Fe and Rh atoms in the nominally antiferromagnetic phase at room temperature. First-principles calculations provide a microscopic description of the structural relaxation and the electron spin-density distribution that fully support the experimental findings.

cond-mat.mtrl-sci↗