arXiv subjects

S. Bonetti

Publications and source records attributed to S. Bonetti.

At least 19 recordsLinked to original sources

arXiv2026

THz-induced phonomagnetism in diamagnetic quantum paraelectric KTaO$_3$

The current efforts striving to develop new ways of data manipulation are aimed at ultrafast control of magnetization in magnetic materials, as well as at inducing magnetic moments in diamagnetics. We demonstrate that in the diamagnetic quantum paraelectric KTaO$_3$, the electric field of circularly polarized THz pulses with an amplitude of $\sim 300\,$kV/cm induces a transient magnetic-like response by resonantly exciting its degenerate soft polar phonon. This phonon-mediated response was measured using the THz pump---optical probe technique via the time-resolved magneto-optic Faraday effect. Our detection scheme was set up to cancel out the major part of the electro-optic Kerr effect which also usually significantly contributes to the transient response. The Kerr-effect-related signal was further suppressed by subtracting the experimental data related to oppositely circularly polarized THz radiation. Thus, we were able to unambiguously identify a temperature-dependent magnetic-like behavior of the KTaO$_3$ crystal manifested by the extracted Faraday rotation. We developed a theoretical model describing well quantitatively the measured curves of the transient Faraday effect signal. However, their amplitudes exhibit an unexpected temperature dependence, which might be a key to a deeper understanding of the observed phonomagnetic effect.

cond-mat.mtrl-sci↗

arXiv2026

Extreme-ultraviolet optical response of atomically-thin molybdenum disulfide

We report multi-angle reflectivity measurements in the extreme-ultraviolet (XUV) range for mono- and bilayer MoS$_2$ on a Si$_3$N$_4$ substrate. Using a single-sheet 2D conductivity model, we extract the complex optical response of the MoS$_2$ bilayer between 25 and 90 eV and derive an effective refractive index by introducing a thickness equal to the interlayer spacing. The MoS$_2$ monolayer response is consistently reproduced either by halving the 2D conductivity or the effective thickness, indicating a robust scaling with layer number. The resulting optical constants display a broad resonance at the Mo N$_{2,3}$ edge with no signatures of sharp core-exciton features despite the reduced dimensionality. First-principles calculations reproduce the experimental results and show that local-field (Hartree) effects dominate the XUV response, while screened-exchange (SEX) contributions remain weak and mainly induce spectral shifts. Our analysis demonstrates that excitonic effects play a minor role in the XUV optical response of atomically thin MoS$_2$, highlighting key differences with respect to the visible and infrared regimes, and calling for a reassessment of the use of Mo-based transition metal dichalcogenides in attosecond spectroscopy and XUV excitonics.

physics.optics↗

arXiv2025

Time-domain extreme ultraviolet diffuse scattering spectroscopy of nanoscale surface phonons

We report the observation of dynamic fringe patterns in the diffuse scattering of extreme ultraviolet light from surfaces, following femtosecond optical excitation. At each point on the detector, the diffuse scattering intensity exhibits oscillations at well-defined frequencies that correspond to surface phonons with wave vectors determined by the scattering geometry, indicating that the optical excitation generates coherent surface phonons propagating in all directions and spanning a wavelength range from 60 to 300 nm. This phenomenon is observed on a variety of samples, including single-layer and multilayer metal films, as well as bulk semiconductors. The measured surface phonon dispersions show good agreement with theoretical calculations. By comparing signal amplitudes from samples with different surface morphologies, we find that the excitation mechanism is linked to the natural surface roughness of the samples. However, the signal is still detectable on extremely smooth surfaces with sub-nanometer roughness. Our findings demonstrate a simple and effective method for optically exciting coherent surface phonons with nanoscale wavelengths on a wide range of solid samples and establish a foundation for surface phonon spectroscopy in a wave vector range well beyond the limit of conventional surface Brillouin scattering.

cond-mat.mtrl-sci↗

arXiv2024

Terahertz-driven parametric excitation of Raman-active phonons in LaAlO$_{3}$

Achieving parametric excitation in an oscillating physical system involves periodically adjusting one of its parameters to modulate the oscillator's natural frequency. This phenomenon has been observed in numerous systems within physics and engineering, profoundly transforming modern science and technology. Despite rapid progress, the parametric control of collective excitations, such as phonons, remains a challenge while promising to generate novel and intriguing effects in a largely unexplored field. Here, we investigate the terahertz (THz) field-induced dynamics of Raman-active phonons in the perovskite structure of LaAlO$_3$ (LAO). Utilizing intense THz pulses, we demonstrate a novel mechanism of parametric phonon excitation marked by substantial subharmonic components. Theoretical analysis can successfully capture the hallmarks of the observed phenomena in a physical scenario with the THz field inducing a parametric coupling between the Raman mode and pairs of acoustic phonon excitations.

cond-mat.mtrl-sci↗

arXiv2024

Ultrafast terahertz field control of the emergent magnetic and electronic interactions at oxide interfaces

Ultrafast electric-field control of emergent electronic and magnetic states at oxide interfaces offers exciting prospects for the development of new generations of energy-efficient devices. Here, we demonstrate that the electronic structure and emergent ferromagnetic interfacial state in epitaxial LaNiO3/CaMnO3 superlattices can be effectively controlled using intense single-cycle THz electric-field pulses. We employ a combination of polarization-dependent X-ray absorption spectroscopy with magnetic circular dichroism and X-ray resonant magnetic reflectivity to measure a detailed magneto-optical profile and thickness of the ferromagnetic interfacial layer. Then, we use time-resolved and temperature-dependent magneto-optical Kerr effect, along with transient optical reflectivity and transmissivity measurements, to disentangle multiple correlated electronic and magnetic processes driven by ultrafast high-field (~1 MV/cm) THz pulses. These processes include an initial sub-picosecond electronic response, consistent with non-equilibrium Joule heating; a rapid (~270 fs) demagnetization of the ferromagnetic interfacial layer, driven by THz-field-induced nonequilibrium spin-polarized currents; and subsequent multi-picosecond dynamics, possibly indicative of a change in the magnetic state of the superlattice due to the transfer of spin angular momentum to the lattice. Our findings shed light on the intricate interplay of electronic and magnetic phenomena in this strongly correlated material system, suggesting a promising avenue for efficient control of two-dimensional ferromagnetic states at oxide interfaces using ultrafast electric-field pulses.

cond-mat.mtrl-sci↗

arXiv2023

Terahertz metamaterials for light-driven magnetism

We describe the design of two types of metamaterials aimed at enhancing terahertz field pulses that can be used to control the magnetic state in condensed matter systems. The first structure is a so-called "dragonfly" antenna, able to realize a five-fold enhancement of the impinging terahertz magnetic field, while preserving its broadband features. For currently available state-of-the-art table top sources, this leads to peak magnetic fields exceeding 1 T. The second structure is an octopole antenna aimed at enhancing a circularly-polarized terahertz electric field, while preserving its polarization state. We obtain a five-fold enhancement of the electric field, hence expected to exceed the 1 MV/cm peak amplitude. Both our structures can be readily fabricated on top of virtually any material.

cond-mat.mes-hall↗

arXiv2023

High-resolution ptychographic imaging at a seeded free-electron laser source using OAM beams

Electromagnetic waves possessing orbital angular momentum (OAM) are powerful tools for applications in optical communications, new quantum technologies and optical tweezers. Recently, they have attracted growing interest since they can be harnessed to detect peculiar helical dichroic effects in chiral molecular media and in magnetic nanostructures. In this work, we perform single-shot per position ptychography on a nanostructured object at a seeded free-electron laser, using extreme ultraviolet OAM beams of different topological charge order $\ell$ generated with spiral zone plates. By controlling $\ell$, we demonstrate how the structural features of OAM beam profile determine an improvement of about 30% in image resolution with respect to conventional Gaussian beam illumination. This result extends the capabilities of coherent diffraction imaging techniques, and paves the way for achieving time-resolved high-resolution (below 100 nm) microscopy on large area samples.

physics.optics↗

arXiv2022

Terahertz electric-field driven dynamical multiferroicity in SrTiO$_3$

The emergence of collective order in matter is among the most fundamental and intriguing phenomena in physics. In recent years, the ultrafast dynamical control and creation of novel ordered states of matter not accessible in thermodynamic equilibrium is receiving much attention. Among those, the theoretical concept of dynamical multiferroicity has been introduced to describe the emergence of magnetization by means of a time-dependent electric polarization in non-ferromagnetic materials. In simple terms, a large amplitude coherent rotating motion of the ions in a crystal induces a magnetic moment along the axis of rotation. However, the experimental verification of this effect is still lacking. Here, we provide evidence of room temperature magnetization in the archetypal paraelectric perovskite SrTiO$_3$ due to this mechanism. To achieve it, we resonantly drive the infrared-active soft phonon mode with intense circularly polarized terahertz electric field, and detect a large magneto-optical Kerr effect. A simple model, which includes two coupled nonlinear oscillators whose forces and couplings are derived with ab-initio calculations using self-consistent phonon theory at a finite temperature, reproduces qualitatively our experimental observations on the temporal and frequency domains. A quantitatively correct magnitude of the effect is obtained when one also considers the phonon analogue of the reciprocal of the Einsten - de Haas effect, also called the Barnett effect, where the total angular momentum from the phonon order is transferred to the electronic one. Our findings show a new path for designing ultrafast magnetic switches by means of coherent control of lattice vibrations with light.

cond-mat.str-el↗

arXiv2021

Non-equilibrium self-assembly of spin-wave solitons in FePt nanoparticles

Magnetic nanoparticles such as FePt in the L10-phase are the bedrock of our current data storage technology. As the grains become smaller to keep up with technological demands, the superparamagnetic limit calls for materials with higher magneto-crystalline anisotropy. This in turn reduces the magnetic exchange length to just a few nanometers enabling magnetic structures to be induced within the nanoparticles. Here we describe the existence of spin-wave solitons, dynamic localized bound states of spin-wave excitations, in FePt nanoparticles. We show with time-resolved X-ray diffraction and micromagnetic modeling that spin-wave solitons of sub-10 nm sizes form out of the demagnetized state following femtosecond laser excitation. The measured soliton spin-precession frequency of 0.1 THz positions this system as a platform to develop miniature devices capable of filling the THz gap.

cond-mat.mtrl-sci↗

arXiv2021

Ultrafast amplification and non-linear magneto-elastic coupling of coherent magnon modes in an antiferromagnet

We investigate the role of domain walls in the ultrafast magnon dynamics of an antiferromagnetic NiO single crystal in a pump-probe experiment with variable pump photon energy. Analysing the amplitude of the energy-dependent photo-induced ultrafast spin dynamics, we detect a yet unreported coupling between the material's characteristic THz- and a GHz-magnon modes. We explain this unexpected coupling between two orthogonal eigenstates of the corresponding Hamiltonian by modelling the magneto-elastic interaction between spins in different domains. We find that such interaction, in the non-linear regime, couples the two different magnon modes via the domain walls and it can be optically exploited via the exciton-magnon resonance.

cond-mat.other↗

arXiv2020

Nanoscale transient magnetization gratings excited and probed by femtosecond extreme ultraviolet pulses

We utilize coherent femtosecond extreme ultraviolet (EUV) pulses derived from a free electron laser (FEL) to generate transient periodic magnetization patterns with periods as short as 44 nm. Combining spatially periodic excitation with resonant probing at the dichroic M-edge of cobalt allows us to create and probe transient gratings of electronic and magnetic excitations in a CoGd alloy. In a demagnetized sample, we observe an electronic excitation with 50 fs rise time close to the FEL pulse duration and ~0.5 ps decay time within the range for the electron-phonon relaxation in metals. When the experiment is performed on a sample magnetized to saturation in an external field, we observe a magnetization grating, which appears on a sub-picosecond time scale as the sample is demagnetized at the maxima of the EUV intensity and then decays on the time scale of tens of picoseconds via thermal diffusion. The described approach opens prospects for studying dynamics of ultrafast magnetic phenomena on nanometer length scales.

cond-mat.mes-hall↗

arXiv2018

Spin-current-mediated rapid magnon localisation and coalescence after ultrafast optical pumping of ferrimagnetic alloys

Sub-picosecond magnetisation manipulation via femtosecond optical pumping has attracted wide attention ever since its original discovery in 1996. However, the spatial evolution of the magnetisation is not yet well understood, in part due to the difficulty in experimentally probing such rapid dynamics. Here, we find evidence of rapid magnetic order recovery in materials with perpendicular magnetic anisotropy via nonlinear magnon processes. We identify both localisation and coalescence regimes, whereby localised magnetic textures nucleate and subsequently evolve in accordance with a power law formalism. Coalescence is observed for optical excitations both above and below the switching threshold. Simulations indicate that the ultrafast generation of noncollinear magnetisation via optical pumping establishes exchange-mediated spin currents with an equivalent 100% spin polarised charge current density of $10^8$ A/cm$^2$. Such large spin currents precipitate rapid recovery of magnetic order after optical pumping. These processes suggest an ultrafast optical route for the stabilization of desired meta-stable states, e.g., isolated skyrmions.

cond-mat.mes-hall↗

arXiv2017

Anti-reflection coating design for metallic terahertz meta-materials

We demonstrate a silicon-based, single-layer anti-reflection coating that suppresses the reflectivity of metals at near-infrared frequencies, enabling optical probing of nano-scale structures embedded in highly reflective surroundings. Our design does not affect the interaction of terahertz radiation with metallic structures that can be used to achieve terahertz near-field enhancement. We have verified the functionality of the design by calculating and measuring the reflectivity of both infrared and terahertz radiation from a silicon/gold double layer as a function of the silicon thickness. We have also fabricated the unit cell of a terahertz meta-material, a dipole antenna comprising two 20-nm thick extended gold plates separated by a 2 $\mu$m gap, where the terahertz field is locally enhanced. We used the time-domain finite element method to demonstrate that such near-field enhancement is preserved in the presence of the anti-reflection coating. Finally, we performed magneto-optical Kerr effect measurements on a single 3-nm thick, 1-$\mu$m wide magnetic wire placed in the gap of such a dipole antenna. The wire only occupies 2\% of the area probed by the laser beam, but its magneto-optical response can be clearly detected. Our design paves the way for ultrafast time-resolved studies, using table-top femtosecond near-infrared lasers, of dynamics in nano-structures driven by strong terahertz radiation.

physics.app-ph↗

arXiv2017

Free-standing magnetic nano-membranes for electron spin-filtering applications

Free-standing ferromagnetic nano-membranes with thicknesses below 10 nm could effectively be used for spin selective filtering of electrons. Such membranes can work both as spin detectors in electron-spectroscopy, -microscopy and -diffraction as well as a source of spin polarized electrons. Theoretical studies and previous work has indicated that ferromagnetic membranes of a few nm have Sherman functions in the 30-60 % range and would provide an effective alternative to current spin detection technology. Here we demonstrate the fabrication of gold capped Co nano-membranes with a 2.6 nm Co layer and a total thickness below 10 nm. The membranes have a Sherman function $S\approx 0.41$ and a transmission of $3.7\times 10^{-2}$ for electron energies of 2 eV. The integration of such spin-filtering membranes in a hemispherical electron analyzer is shown to provide massively parallel detection capabilities and a "2-dimensional" figure of merit $FOM_\mathrm{2D}$ = 67.2, the highest reported to date.

cond-mat.mes-hall↗

arXiv2016

Ultrafast THz Field Control of Electronic and Structural Interactions in Vanadium Dioxide

Vanadium dioxide, an archetypal correlated-electron material, undergoes an insulator-metal transition near room temperature that exhibits electron-correlation-driven and structurally-driven physics. Using ultrafast optical spectroscopy and x-ray scattering we show that these processes can be disentangled in the time domain. Specifically, following intense sub-picosecond electric-field excitation, a partial collapse of the insulating gap occurs within the first ps. Subsequently, this electronic reconfiguration initiates a change in lattice symmetry taking place on a slower timescale. We identify the kinetic energy increase of electrons tunneling in the strong electric field as the driving force, illustrating a novel method to control electronic interactions in correlated materials on an ultrafast timescale.

cond-mat.str-el↗

arXiv2016

THz-driven ultrafast spin-lattice scattering in amorphous metallic ferromagnets

We use single-cycle THz fields and the femtosecond magneto-optical Kerr effect to respectively excite and probe the magnetization dynamics in two thin-film ferromagnets with different lattice structure: crystalline Fe and amorphous CoFeB. We observe Landau-Lifshitz-torque magnetization dynamics of comparable magnitude in both systems, but only the amorphous sample shows ultrafast demagnetization caused by the spin-lattice depolarization of the THz-induced ultrafast spin current. Quantitative modelling shows that such spin-lattice scattering events occur on similar time scales than the conventional spin conserving electronic scattering ($\sim30$ fs). This is significantly faster that optical laser-induced demagnetization. THz conductivity measurements point towards the influence of lattice disorder in amorphous CoFeB as the driving force for enhanced spin-lattice scattering.

cond-mat.mtrl-sci↗

arXiv2015

Generation of high-frequency strain waves during femtosecond demagnetization of Fe/MgO films

We use femtosecond time-resolved hard x-ray scattering to detect coherent acoustic phonons excited during ultrafast laser demagnetization of bcc Fe films. We determine the lattice strain propagating through the film through analysis of the oscillations in the x-ray scattering signal as a function of momentum transfer. The width of the strain wavefront is ~100 fs, similar to demagnetization timescales. First-principles calculations show that the high-frequency Fourier components of the strain, which give rise to the sharp wavefront, could in part originate from non-thermal dynamics of the lattice not considered in the two-temperature model.

cond-mat.mtrl-sci↗

arXiv2015

X-Ray Detection of Transient Magnetic Moments Induced by a Spin Current in Cu

We have used a MHz lock-in x-ray spectro-microscopy technique to directly detect changes of magnetic moments in Cu due to spin injection from an adjacent Co layer. The elemental and chemical specificity of x-rays allows us to distinguish two spin current induced effects. We detect the creation of transient magnetic moments of $3\times 10^{-5}$ $μ_\mathrm{B}$ on Cu atoms within the bulk of the 28 nm thick Cu film due to spin-accumulation. The moment value is compared to predictions by Mott's two current model. We also observe that the hybridization induced existing magnetic moments on Cu interface atoms are transiently increased by about 10% or $4\times 10^{-3}$ $μ_\mathrm{B}$. This reveals the dominance of spin-torque alignment over Joule heat induced disorder of the interfacial Cu moments during current flow.

cond-mat.mtrl-sci↗