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Giorgio Rossi

Publications and source records attributed to Giorgio Rossi.

18 recordsLinked to original sources

Tracking the local order parameter through the Hubbard exciton decoherence time in the Mott-Hubbard insulator LaVO3

The prototypical Mott-Hubbard insulator LaVO3 undergoes a structural phase transition accompanied by the onset of spin and orbital ordering below 140 K. By combining ultrafast optical pump-probe spectroscopy and two-dimensional electronic spectroscopy, we investigate the interplay between fluctuations of the local spin and orbital order parameter and the lifetime of high-energy electron-hole excitations. Specifically, we demonstrate that the pump-induced perturbation of the order parameter leads to a change of the Hubbard exciton decoherence time and, consequently, of its homogeneous linewidth. Dynamical mean-field theory calculations confirm that the exciton scattering rate is crucially affected by the degree of order of the spin and orbital lattices in LaVO3. Our results demonstrate that multi-dimensional ultrafast optical spectroscopy can be used to track the dynamics of the order parameter, thus opening new routes in the study of correlated quantum materials characterized by intertwined orders.

cond-mat.str-el

Spin waves excited by hard x-ray transient gratings

Recent progress in ultrafast x-ray sources helped establish x-rays as an important tool for probing lattice and magnetic dynamics initiated by femtosecond optical pulses. Here, we explore the potential of ultrashort hard x-ray pulses for driving magnetic dynamics. We use a transient grating technique in which a spatially periodic x-ray excitation pattern gives rise to material excitations at a well-defined wave vector, whose dynamics are monitored via diffraction of an optical probe pulse. The excitation of a ferrimagnetic gadolinium bismuth iron garnet film placed in an external tilted magnetic field by x-rays at the Gd L3 edge results in both magnetic and non-magnetic transient gratings whose contributions to the diffracted signal are separated by polarization analysis. We observe the magnetization precession at both longitudinal acoustic and spin wave frequencies. An analysis with the Landau-Lifshitz-Gilbert equation indicates that the magnetization precession is driven by strain resulting from thermal expansion induced by absorbed x-rays. The results establish x-ray transient gratings as a tool for driving coherent phonons and magnons, with the potential of accessing wave vectors across the entire Brillouin zone.

physics.optics

Thermal treatment effects on PMN-0.4PT/Fe multiferroic heterostructures

Multiferroic heterostructures have gained in recent years a renewed role in spintronic applications due to their possibility in controlling the magnetic properties via interfacial coupling by exploiting the ferroelectric response to various external stimuli. Whereas the main mechanisms ruling the converse magnetoelectric coupling are considered as established, the research on how to optimize the ferroelectric properties is an active field. In particular the complex phase diagram of [Pb(Mg1/3Nb2/3)O3]-x[PbTiO3] (PMN-xPT) single crystals, that present relaxor ferroelectric and photovoltaic properties, deserves further investigation. For instance, crystalline quality and thermal stability of the ferroelectric domains in heterostructures need assessment. Here we show how, by thermal annealing over the ferroelectric Curie temperature and then cooling PMN-0.4PT/Fe heterostructures in inert atmosphere the domain population is significantly modified, evolving from a highly disordered, mostly out-of-plane domain population, to improved crystallinity and prevalent in-plane oriented domains. Upon further annealing, the domain population switches back to prevalent out-of-plane orientation suggesting that intermediate annealing steps can freeze PMN-0.4PT domain population in a metastable configuration. The structural analysis was carried out by combining micro-Raman and X-ray diffraction (XRD) measurements. In the three states the magnetic properties of interfacial Fe thin film are affected by the ferroelectric configurations as a consequence of changing interfacial strain, evolving from an isotropic behavior to an anisotropic one and back.

cond-mat.mtrl-sci

Uncovering the lowest thickness limit for room-temperature ferromagnetism of Cr$_{1.6}$Te$_{2}$

Metallic ferromagnetic transition metal dichalcogenides have emerged as important building blocks for scalable magnonics and memory applications. Downscaling such systems to the ultra-thin limit is critical to integrate them into technology. Here, we achieved layer-by-layer control over the transition metal dichalcogenide Cr$_{1.6}$Te$_{2}$ by using pulsed laser deposition, and we uncovered the minimum critical thickness above which room temperature magnetic order is maintained. The electronic and magnetic structure is explored experimentally and theoretically and it is shown that the films exhibit strong in-plane magnetic anisotropy as a consequence of large spin-orbit effects. Our study elucidates both magnetic and electronic properties of Cr$_{1.6}$Te$_{2}$, and corroborates the importance of intercalation to tune the magnetic properties of nanoscale materials architectures.

cond-mat.mtrl-sci

Signatures of a surface spin-orbital chiral metal

The relation between crystal symmetries, electron correlations, and electronic structure steers the formation of a large array of unconventional phases of matter, including magneto-electric loop currents and chiral magnetism. Detection of such hidden orders is a major goal in condensed matter physics. However, to date, nonstandard forms of magnetism with chiral electronic ordering have been experimentally elusive. Here, we develop a theory for symmetry-broken chiral ground states and propose a methodology based on circularly polarized spin-selective angular-resolved photoelectron spectroscopy to probe them. We exploit the archetypal quantum material Sr2RuO4 and reveal spectroscopic signatures which, even though subtle, may be reconciled with the formation of spin-orbital chiral currents at the material surface. As we shed light on these chiral regimes, our findings pave the way for a deeper understanding of ordering phenomena and unconventional magnetism.

cond-mat.str-el

Observation of termination-dependent topological connectivity in a magnetic Weyl kagome-lattice

Engineering surfaces and interfaces of materials promises great potential in the field of heterostructures and quantum matter designer, with the opportunity of driving new many-body phases that are absent in the bulk compounds. Here, we focus on the magnetic Weyl kagome system Co$_3$Sn$_2$S$_2$ and show how for different sample's terminations the Weyl-points connect also differently, still preserving the bulk-boundary correspondence. Scanning-tunnelling microscopy has suggested such a scenario indirectly. Here, we demonstrate this directly for the fermiology of Co$_3$Sn$_2$S$_2$, by linking it to the system real space surfaces distribution. By a combination of micro-ARPES and first-principles calculations, we measure the energy-momentum spectra and the Fermi surfaces of Co$_3$Sn$_2$S$_2$ for different surface terminations and show the existence of topological features directly depending on the top-layer electronic environment. Our work helps to define a route to control bulk-derived topological properties by means of surface electrostatic potentials, creating a realistic and reliable methodology to use Weyl kagome metals in responsive magnetic spintronics.

cond-mat.str-el

The electronic structure of intertwined kagome, honeycomb, and triangular sublattices of the intermetallics MCo$_2$Al$_9$

Intermetallics are an important playground to stabilize a large variety of physical phenomena, arising from their complex crystal structure. The ease of their chemical tuneabilty makes them suitable platforms to realize targeted electronic properties starting from the symmetries hidden in their unit cell. Here, we investigate the family of the recently discovered intermetallics MCo$_2$Al$_9$ (M: Sr, Ba) and we unveil their electronic structure for the first time. By using angle-resolved photoelectron spectroscopy and density functional theory calculations, we discover the existence of Dirac-like dispersions as ubiquitous features in this family, coming from the hidden kagome and honeycomb symmetries embedded in the unit cell. Finally, from calculations, we expect that the spin-orbit coupling is responsible for opening energy gaps in the electronic structure spectrum, which also affects the majority of the observed Dirac-like states. Our study constitutes the first experimental observation of the electronic structure of MCo$_2$Al$_9$ and proposes these systems as hosts of Dirac-like physics with intrinsic spin-orbit coupling. The latter effect suggests MCo$_2$Al$_9$ as a future platform for investigating the emergence of non-trivial topology.

cond-mat.str-el

Flat band separation and robust spin-Berry curvature in bilayer kagome metals

Kagome materials have emerged as a setting for emergent electronic phenomena that encompass different aspects of symmetry and topology. It is debated whether the XV$_6$Sn$_6$ kagome family (where X is a rare earth element), a recently discovered family of bilayer kagome metals, hosts a topologically non-trivial ground state resulting from the opening of spin-orbit coupling gaps. These states would carry a finite spin-Berry curvature, and topological surface states. Here, we investigate the spin and electronic structure of the XV$_6$Sn$_6$ kagome family. We obtain evidence for a finite spin-Berry curvature contribution at the center of the Brillouin zone, where the nearly flat band detaches from the dispersing Dirac band because of spin-orbit coupling. In addition, the spin-Berry curvature is further investigated in the charge density wave regime of ScV$_6$Sn$_6$, and it is found to be robust against the onset of the temperature-driven ordered phase. Utilizing the sensitivity of angle resolved photoemission spectroscopy to the spin and orbital angular momentum, our work unveils the spin-Berry curvature of topological kagome metals, and helps to define its spectroscopic fingerprint.

cond-mat.str-el

Dynamics and Resilience of the Charge Density Wave in a bilayer kagome metal

Long-range electronic order descending from a metallic parent state constitutes a rich playground to study the intricate interplay of structural and electronic degrees of freedom. With dispersive and correlation features as multifold as topological Dirac-like itinerant states, van-Hove singularities, correlated flat bands, and magnetic transitions at low temperature, kagome metals are located in the most interesting regime where both phonon and electronically mediated couplings are significant. Several of these systems undergo a charge density wave (CDW) transition, and the van-Hove singularities, which are intrinsic to the kagome tiling, have been conjectured to play a key role in mediating such an instability. However, to date, the origin and the main driving force behind this charge order is elusive. Here, we use the topological bilayer kagome metal ScV6Sn6 as a platform to investigate this puzzling problem, since it features both kagome-derived nested Fermi surface and van-Hove singularities near the Fermi level, and a CDW phase that affects the susceptibility, the neutron scattering, and the specific heat, similarly to the siblings AV3Sb5 (A = K, Rb, Cs) and FeGe. We report on our findings from high-resolution angle-resolved photoemission, density functional theory, and time-resolved optical spectroscopy to unveil the dynamics of its CDW phase. We identify the structural degrees of freedom to play a fundamental role in the stabilization of charge order. Along with a comprehensive analysis of the subdominant impact from electronic correlations, we find ScV6Sn6 to feature an instance of charge density wave order that predominantly originates from phonons. As we shed light on the emergent phonon profile in the low-temperature ordered regime, our findings pave the way for a deeper understanding of ordering phenomena in all CDW kagome metals.

cond-mat.str-el

Discovery of a magnetic Dirac system with large intrinsic non-linear Hall effect

Magnetic materials exhibiting topological Dirac fermions are attracting significant attention for their promising technological potential in spintronics. In these systems, the combined effect of the spin-orbit coupling and magnetic order enables the realization of novel topological phases with exotic transport properties, including the anomalous Hall effect and magneto-chiral phenomena. Herein, we report experimental signature of topological Dirac antiferromagnetism in TaCoTe2 via angle-resolved photoelectron spectroscopy (ARPES) and first-principles density functional theory (DFT) calculations. In particular, we find the existence of spin-orbit coupling-induced gaps at the Fermi level, consistent with the manifestation of a large intrinsic non-linear Hall conductivity. Remarkably, we find that the latter is extremely sensitive to the orientation of the Néel vector, suggesting TaCoTe2 a suitable candidate for the realization of non-volatile spintronic devices with an unprecedented level of intrinsic tunability.

cond-mat.str-el

Disentangling structural and electronic properties in V$_{2}$O$_{3}$ thin films: a genuine non-symmetry breaking Mott transition

Phase transitions are key in determining and controlling the quantum properties of correlated materials. Here, by using the powerful combination of precise material synthesis and angle resolved photoelectron spectroscopy, we show evidence for a genuine Mott transition undressed of any symmetry breaking side effects in the thin-films of V$_{2}$O$_{3}$. In particular, and in sharp contrast with the bulk V$_{2}$O$_{3}$ crystals, we unveil the purely electronic dynamics approaching the metal-insulator transition, disentangled from the structural transformation that is prevented by the residual substrate-induced strain. On approaching the transition, the spectral signal evolves surprisingly slowly over a wide temperature range, the Fermi wave-vector does not change, and the critical temperature appears to be much lower than the one reported for the bulk. Our findings are on one side fundamental in demonstrating the universal benchmarks of a genuine non-symmetry breaking Mott transition, extendable to a large array of correlated quantum systems and, on the other, given that the fatal structural breakdown is avoided, they hold promise of exploiting the metal-insulator transition by implementing V$_{2}$O$_{3}$ thin films in devices.

cond-mat.str-el

Strain-induced magnetization control in an oxide multiferroic heterostructure

Controlling magnetism by using electric fields is a goal of research towards novel spintronic devices and future nano-electronics. For this reason, multiferroic heterostructures attract much interest. Here we provide experimental evidence, and supporting DFT analysis, of a transition in La0.65Sr0.35MnO3 (LSMO) thin film to a stable ferromagnetic phase, that is induced by the structural and strain properties of the ferroelectric BaTiO3 (BTO) substrate, which can be modified by applying external electric fields. X-ray Magnetic Circular Dichroism (XMCD) measurements on Mn L edges with a synchrotron radiation show, in fact two magnetic transitions as a function of temperature that correspond to structural changes of the BTO substrate. We also show that ferromagnetism, absent in the pristine condition at room temperature, can be established by electrically switching the BTO ferroelectric domains in the out-of-plane direction. The present results confirm that electrically induced strain can be exploited to control magnetism in multiferroic oxide heterostructures.

cond-mat.mtrl-sci

Space Charge Free Ultrafast Photoelectron Spectroscopy on Solids by a Narrowband Tunable Extreme Ultraviolet Light Source

Here we report on a novel High Harmonic Generation (HHG) light source designed for space charge free ultrafast photoelectron spectroscopy (PES) on solids. The ultimate overall energy resolution achieved on a polycrystalline Au sample is ~22 meV at 40 K. These results have been obtained at a photon energy of 16.9 eV with a pulse bandwidth of ~19 meV, by varying, up to 200 kHz, the photon pulses repetition rate and the photon fluence on the sample. These features set a new benchmark for tunable narrowband HHG sources. By comparing the PES energy resolution and the photon pulse bandwidth with a pulse duration of ~105 fs, as retrieved from time-resolved (TR) angle resolved (AR) PES experiments on Bi$_2$Se$_3$, we validate a way for a space charge free photoelectric process close to Fourier transform limit conditions for ultrafast TR-PES experiments on solids.

physics.optics

Selective control of localised vs. delocalised carriers in anatase TiO2 through reaction with O2

Two-dimensional (2D) metallic states induced by oxygen vacancies at oxide surfaces and interfaces provide new opportunities for the development of advanced applications, but the ability to control the behavior of these states is still limited. We used Angle Resolved Photoelectron Spectroscopy combined with density functional theory to study the reactivity of states induced by the oxygen vacancies at the (001)-(1x4) surface of anatase TiO2, where both 2D metallic and deeper lying in-gap states (IGs) are observed. Remarkably, the two states exhibit very different evolution when the surface is exposed to molecular O2: while IGs are almost completely quenched, the metallic states are only weakly affected. The energy scale analysis for the vacancy migration and recombination resulting from the DFT calculations confirms indeed that only the IGs originate from and remain localized at the surface, whereas the metallic states originate from subsurface vacancies, whose migration and recombination at the surface is energetically less favorable rendering them therefore insensitive to oxygen dosing.

cond-mat.mtrl-sci

Transient quantum isolation and critical behavior in the magnetization dynamics of half-metallic manganites

We combine time resolved pump-probe Magneto-Optical Kerr Effect and Photoelectron Spectroscopy experiments supported by theoretical analysis to determine the relaxation dynamics of delocalized electrons in half-metallic ferromagnetic manganite $La_{1-x}Sr_{x}MnO_{3}$. We observe that the half-metallic character of $La_{1-x}Sr_{x}MnO_{3}$ determines the timescale of both the electronic phase transition and the quenching of magnetization, revealing a quantum isolation of the spin system in double exchange ferromagnets extending up to hundreds of picoseconds. We demonstrate the use of time-resolved hard X-ray photoelectron spectroscopy (TR-HAXPES) as a unique tool to single out the evolution of strongly correlated electronic states across a second-order phase transition in a complex material.

cond-mat.str-el

Tailoring ferromagnetism through electrically controlled morphology

Converse magnetoelectric coupling in artificial multiferroics is generally modelled through three possible mechanisms: charge transfer, strain mediated or ion migration. Here we demonstrate a novel and highly reliable approach, where electrically controlled morphological modifications control the ferromagnetic response of a magnetoelectric heterostructure, specifically FexMn1-x ferromagnetic films on ferroelectric PMN-PT (001) substrates. The ferroelectric PMN-PT substrates present, in correspondence to electrical switching, fully reversible morphological changes at the surface, to which correspond reproducible modifications of the ferromagnetic response of the FexMn1-x films. Topographic analysis by atomic force microscopy shows the formation of surface cracks after application of a positive electric field up to 6 kV/cm, which disappear after application of negative voltage of the same amplitude. In-operando x-ray magnetic circular dichroic spectroscopy at Fe edge in FexMn1-x layers shows local variations of dichroic signal up to a factor 2.5 as a function of the electrically-driven morphological state. These findings highlight the role of morphology and surface topography as a key aspect in magnetoelectric coupling, whose proof of electrically reversible modification of the magnetic response adds a new possibility in the design of multiferroic heterostructures with electrically controlled functionalities.

cond-mat.mtrl-sci

The role of spin-orbit coupling in the electronic structure of IrO$_2$

The delicate interplay of electronic charge, spin, and orbital degrees of freedom is in the heart of many novel phenomena across the transition metal oxide family. Here, by combining high- resolution angle resolved photoemission spectroscopy and first principles calculations (with and without spin-orbit coupling), the electronic structure of the rutile binary iridate, IrO$_2$ is investigated. The detailed study of electronic bands measured on a high-quality single crystalline sample, and use of a wide range of photon energy provide a huge improvement over the previous studies. The excellent agreement between theory and experimental results shows that the single-particle DFT description of IrO$_2$ band structure is adequate, without the need of invoking any treatment of correlation effects. Although many observed features point to a 3D nature of the electronic structure, clear surface effects are revealed. The discussion of the orbital character of the relevant bands crossing the Fermi level sheds light on spin orbit coupling-driven phenomena in this material, unveiling a spin-orbit induced avoided crossing, a property likely to play key role in its large spin Hall effect.

cond-mat.mtrl-sci

Very Efficient Spin Polarization Analysis (VESPA): New Exchange Scattering-based Setup for Spin-resolved ARPES at APE-NFFA Beamline at Elettra

Complete Photoemission Experiments, enabling to measure the full quantum set of the photoelectron final state, are in high demand for the study of materials and nanostructures whose properties are determined by strong electron and spin correlations. We report here on the implementation of the new spin polarimeter VESPA (Very Efficient Spin Polarization Analysis) at the APE-NFFA Beamline at Elettra that is based on the exchange coupling between the photoelectron spin and a ferromagnetic surface in a reflectometry setup. The system was designed to be integrated with a dedicated Scienta-Omicron DA30 electron energy analyzer allowing for two simultaneous reflectometry measurements, along perpendicular axes, that, after magnetization switching of the two targets allow to perform the 3D vectorial reconstruction of the spin polarization while operating the DA30 in high resolution mode. VESPA represents the very first installation for spin resolved ARPES (SPARPES) at the Elettra synchrotron in Trieste, and is being heavily exploited by SPARPES users since fall 2015.

physics.ins-det