Understanding the ultrafast demagnetization of transition metals requires pump-probe experiments sensitive to the time evolution of the electronic, spin, and lattice thermodynamic baths. By means of time-resolved photoelectron energy and spin-polarization measurements in the low-pump-fluence regime on iron, we disentangle the different dynamics of hot electrons and demagnetization in the subpicosecond and picosecond time range. We observe a broadening of the Fermi-Dirac distribution, following the excitation of nonthermal electrons at specific region of the iron valence band. The corresponding reduction of the spin polarization is remarkably delayed with respect to the dynamics of electronic temperature. The experimental results are corroborated with a microscopic 3-temperature model highlighting the role of thermal disorder in the quenching of the average spin magnetic moment, and indicating Elliot-Yafet type spin-flip scattering as the main mediation mechanism, with a spin-flip probability of 0.1 and a rate of energy exchange between electrons and lattice of 2.5Kfs−1.
van der Waals materials provide a versatile toolbox for the emergence of new quantum phenomena and fabrication of functional heterostructures. Among them, the trihalide VI3 stands out for its unique magnetic and structural landscape. Here we investigate the spin and orbital magnetic degrees of freedom in the layered ferromagnet VI3 by means of temperature-dependent X-ray absorption spectroscopy and X-ray magnetic circular and linear dichroism. We detect localized electronic states and reduced magnetic dimensionality, due to electronic correlations. We furthermore provide experimental evidence of (a) an unquenched orbital magnetic moment (up to 0.66(7) μB/V atom) in the ferromagnetic state and (b) an instability of the orbital moment in the proximity of the spin reorientation transition. Our results support a coherent picture where electronic correlations give rise to a strong magnetic anisotropy and a large orbital moment and establish VI3 as a prime candidate for the study of orbital quantum effects.
Polarization dependent x-ray absorption spectroscopy was used to study the magnetic ground state and the orbital occupation in bulk-phase VI3 van der Waals crystals below and above the ferromagnetic and structural transitions. X-ray natural linear dichroism and x-ray magnetic circular dichroism spectra acquired at the V $L_{2,3}$ edges are compared against multiplet cluster calculations within the frame of the ligand field theory to quantify the intra-atomic electronic interactions at play and evaluate the effects of symmetry reduction occurring in a trigonally distorted VI6 unit. We observed a non zero linear dichroism proving the presence of an anisotropic charge density distribution around the V3+ ion due to the unbalanced hybridization between the vanadium and the ligand states. Such hybridization acts as an effective trigonal crystal field, slightly lifting the degeneracy of the $t_{2g}^2$ ground state. However, the energy splitting associated to the distortion underestimates the experimental band gap, suggesting that the insulating ground state is stabilized by Mott correlation effects rather than via a Jahn–Teller mechanism. Our results clarify the role of the distortion in VI3 and establish a benchmark for the study of the spectroscopic properties of other van der Waals halides, including emerging 2D materials with mono and few-layers thickness, whose fundamental properties might be altered by reduced dimensions and interface proximity.
This thesis completes my work as doctoral student of the Scuola di Dottorato in Fisica, Astrofisica e Fisica Applicata at the Universit`a degli Studi di Milano, that has been carried out since November 2019 at the Istituto Officina dei Materiali of the Consiglio Nazionale delle Ricerche (IOM-CNR) in the premises of the Elettra - Sincrotrone Trieste and FERMI@Elettra infrastructures and in the framework of the NFFA facility.
My experimental activity employed complementary spectroscopy and polarimetry techniques oriented to address the characterisation of electronic and spin properties of systems with decreasing dimensionality. This programme has been conducted by exploiting state-of-the-art infrastructures to generate visible, UV and EUV ultrashort pulses (tabletop lasers and HHG at NFFA-SPRINT laboratory) and soft X-ray synchrotron light (at Elettra, Diamond and ESRF synchrotron light sources).
I used photoemission as the main tool in my investigation, supplementing my results with absorption spectroscopy. I focused on three materials, Fe(001)-p(1x1)O/MgO, EuSn2P2 and VI3, of high interest in modern and next-generation magnetic devices.
In the three systems I studied the electronic band structure to identify key features hinting at the bound electrons behaviour. I investigated the properties of the magnetically ordered phases and found evidence of the reduced dimensionality in the emergence of atypical spin ordering and the increasingly manifest electron correlation phenomena.
The information retained by band electrons is critical to access the spin polarisation of the bands and to give insight into the effects of spatial confinement on the spin degree of freedom.
The possibility of modifying the ferromagnetic response of a multiferroic heterostructure via fully optical means exploiting the photovoltaic/photostrictive properties of the ferroelectric component is an effective method for tuning the interfacial properties. In this study, the effects of 405 nm visible-light illumination on the ferroelectric and ferromagnetic responses of (001) Pb(Mg1/3Nb2/3)O3-0.4PbTiO3 (PMN-PT)/Ni heterostructures are presented. By combining electrical, structural, magnetic, and spectroscopic measurements, how light illumination above the ferroelectric bandgap energy induces a photovoltaic current and the photostrictive effect reduces the coercive field of the interfacial magnetostrictive Ni layer are shown. Firstly, a light-induced variation in the Ni orbital moment as a result of sum-rule analysis of x-ray magnetic circular dichroic measurements is reported. The reduction of orbital moment reveals a photogenerated strain field. The observed effect is strongly reduced when polarizing out-of-plane the PMN-PT substrate, showing a highly anisotropic photostrictive contribution from the in-plane ferroelectric domains. These results shed light on the delicate energy balance that leads to sizeable light-induced effects in multiferroic heterostructures, while confirming the need of spectroscopy for identifying the physical origin of interface behavior.
The generation and control of surface acoustic waves (SAWs) in a magnetic material are objects of an intense research effort focused on magnetoelastic properties, with fruitful ramifications in spin-wave-based quantum logic and magnonics. We implement a transient grating setup to optically generate SAWs also seeding coherent spin waves via magnetoelastic coupling in ferromagnetic media. In this work we report on SAW-driven ferromagnetic resonance (FMR) experiments performed on polycrystalline Ni thin films in combination with time-resolved Faraday polarimetry, which allows extraction of the value of the effective magnetization and of the Gilbert damping. The results are in full agreement with measurements on the very same samples from standard FMR. Higher-order effects due to parametric modulation of the magnetization dynamics, such as down-conversion, up-conversion, and frequency mixing, are observed, testifying the high sensitivity of this technique.
Space and mirror charge effects in time-resolved photoemission spectroscopy can be modeled to obtain relevant information on the recombination dynamics of charge carriers. We successfully extracted from these phenomena the reneutralization characteristic time of positive charges generated by photoexcitation in CeO2-based films. For the above-band-gap excitation, a large fraction of positive carriers with a lifetime that exceeds 100 ps are generated. Otherwise, the sub-band-gap excitation induces the formation of a significantly smaller fraction of charges with lifetimes of tens of picoseconds, ascribed to the excitation of defect sites or to multiphoton absorption. When the oxide is combined with Ag nanoparticles, the sub-band-gap excitation of localized surface plasmon resonances leads to reneutralization times longer than 300 ps. This was interpreted by considering the electronic unbalance at the surface of the nanoparticles generated by the injection of electrons, via localized surface plasmon resonance (LSPR) decay, into CeO2. This study represents an example of how to exploit the space charge effect in gaining access to the surface carrier dynamics in CeO2 within the picosecond range of time, which is fundamental to describe the photocatalytic processes.
Phase transitions are key in determining and controlling the quantum properties of correlated materials. Here, by using the combination of material synthesis and photoelectron spectroscopy, we demonstrate a genuine Mott transition undressed of any symmetry breaking side effects in the thin films of V2O3. In particular and in contrast with the bulk V2O3, 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 slowly over a wide temperature range, the Fermi wave-vector does not change, and the critical temperature is lower than the one reported for the bulk. Our findings are fundamental in demonstrating the universal benchmarks of a genuine nonsymmetry breaking Mott transition, extendable to a large array of correlated quantum systems, and hold promise of exploiting the metal–insulator transition by implementing V2O3 thin films in devices.
Machine-learning techniques are revolutionizing the way to perform efficient materials modeling. We here propose a combinatorial machine-learning approach to obtain physical formulas based on simple and easily accessible ingredients, such as atomic properties. The latter are used to build materials features that are finally employed, through linear regression, to predict the energetic stability of semiconducting binary compounds with respect to zinc blende and rocksalt crystal structures. The adopted models are trained using a dataset built from first-principles calculations. Our results show that already one-dimensional (1D) formulas well describe the energetics; a simple grid-search optimization of the automatically obtained 1D-formulas enhances the prediction performance at a very small computational cost. In addition, our approach allows one to highlight the role of the different atomic properties involved in the formulas. The computed formulas clearly indicate that “spatial” atomic properties (i.e., radii indicating maximum probability densities for 𝑠,𝑝,𝑑 electronic shells) drive the stabilization of one crystal structure with respect to the other, suggesting the major relevance of the radius associated with the 𝑝-shell of the cation species.
Curved magnets attract considerable interest for their unusually rich phase diagram, often encompassing exotic (e.g., topological or chiral) spin states. Micromagnetic simulations are playing a central role in the theoretical understanding of such phenomena; their predictive power, however, rests on the availability of reliable model parameters to describe a given material or nanostructure. Here we demonstrate how noncollinear-spin polarized density-functional theory can be used to determine the flexomagnetic coupling coefficients in real systems. By focusing on monolayer CrI3, we find a crossover as a function of curvature between a magnetization normal to the surface to a cycloidal state, which we rationalize in terms of effective anisotropy and Dzyaloshinskii-Moriya contributions to the magnetic energy. Our results reveal an unexpectedly large impact of spin-orbit interactions on the curvature-induced anisotropy, which we discuss in the context of existing phenomenological models
We unravel the interplay of topological properties and the layered (anti)ferromagnetic ordering in EuSn2P2, using spin and chemical selective electron and X-ray spectroscopies supported by first-principle calculations. We reveal the presence of in-plane long-range ferromagnetic order triggering topological invariants and resulting in the multiple protection of topological Dirac states. We provide clear evidence that layer-dependent spin-momentum locking coexists with ferromagnetism in this material, a cohabitation that promotes EuSn2P2 as a prime candidate axion insulator for topological antiferromagnetic spintronics applications.
Two-dimensional (2D) van der Waals (vdW) magnets provide an ideal platform for exploring, on the fundamental side, new microscopic mechanisms and for developing, on the technological side, ultracompact spintronic applications. So far, bilinear spin Hamiltonians have been commonly adopted to investigate the magnetic properties of 2D magnets, neglecting higher order magnetic interactions. However, we here provide quantitative evidence of giant biquadratic exchange interactions in monolayer NiX2 (X=Cl, Br and I), by combining first-principles calculations and the newly developed machine learning method for constructing Hamiltonian. Interestingly, we show that the ferromagnetic ground state within NiCl2 single layers cannot be explained by means of the bilinear Heisenberg Hamiltonian; rather, the nearest-neighbor biquadratic interaction is found to be crucial. Furthermore, using a three-orbitals Hubbard model, we propose that the giant biquadratic exchange interaction originates from large hopping between unoccupied and occupied orbitals on neighboring magnetic ions. On a general framework, our work suggests biquadratic exchange interactions to be important in 2D magnets with edge-shared octahedra.
Topological materials are a promising platform for a wide range of next-generation technologies. In article number 2100063, Antonio Politano, Salvador Barraza-Lopez, Jin Hu and co-workers report a new topological material, SmSbTe, displaying a coexistence of magnetism, enhanced electronic correlations, and Dirac fermions, as illustrated in the cover image. This discovery suggests that SmSbTe represents an ideal platform for exotic quantum phenomena arising from the interplay between degrees of freedom. The manipulation of these phenomena would further pave a path for quantum material-based functional devices.
The emergence of Dirac semimetals has stimulated growing attention, owing to the considerable technological potential arising from their peculiar exotic quantum transport related to their nontrivial topological states. Especially, materials showing type-II Dirac fermions afford novel device functionalities enabled by anisotropic optical and magnetotransport properties. Nevertheless, real technological implementation has remained elusive so far. Definitely, in most Dirac semimetals, the Dirac point lies deep below the Fermi level, limiting technological exploitation. Here, it is shown that kitkaite (NiTeSe) represents an ideal platform for type-II Dirac fermiology based on spin-resolved angle-resolved photoemission spectroscopy and density functional theory. Precisely, the existence of type-II bulk Dirac fermions is discovered in NiTeSe around the Fermi level and the presence of topological surface states with strong (≈50%) spin polarization. By means of surface-science experiments in near-ambient pressure conditions, chemical inertness towards ambient gases (oxygen and water) is also demonstrated. Correspondingly, NiTeSe-based devices without encapsulation afford long-term efficiency, as demonstrated by the direct implementation of a NiTeSe-based microwave receiver with a room-temperature photocurrent of 2.8 µA at 28 GHz and more than two orders of magnitude linear dynamic range. The findings are essential to bringing to fruition type-II Dirac fermions in photonics, spintronics, and optoelectronics.
Due to their peculiar quasiparticle excitations, topological metals have high potential for applications in the fields of spintronics, catalysis, and superconductivity. Here, by combining spin- and angle-resolved photoemission spectroscopy, scanning tunneling microscopy/spectroscopy, and density functional theory, we discover surface-termination-dependent topological electronic states in the recently discovered mitrofanovite Pt3Te4. Mitrofanovite crystal is formed by alternating, van der Waals bound layers of Pt2Te2 and PtTe2. Our results demonstrate that mitrofanovite is a topological metal with termination-dependent (i) electronic band structure and (ii) spin texture. Despite their distinct electronic character, both surface terminations are characterized by electronic states exhibiting strong spin polarization with a node at the Γ point and sign reversal across the Γ point, indicating their topological nature and the possibility of realizing two distinct electronic configurations (both of them with topological features) on the surface of the same material.
The effects of competing magnetic interactions in stabilizing different spin configurations are drawing renewed attention in order to unveil emerging topological spin textures and to highlight microscopic mechanisms leading to their stabilization. The possible key role of the two-site exchange anisotropy in selecting specific helicity and vorticity of skyrmionic lattices has only recently been proposed. In this work, we explore the phase diagram of a frustrated localized magnet characterized by a two-dimensional centrosymmetric triangular lattice, focusing on the interplay between the two-ion anisotropy and the single-ion anisotropy. The effects of an external magnetic field applied perpendicularly to the magnetic layer, are also investigated. By means of Monte Carlo simulations, we find an abundance of different spin configurations, going from trivial to high-order Q skyrmionic and meronic lattices. In closer detail, we find that a dominant role is played by the two-ion over the single-ion anisotropy in determining the planar spin texture; the strength and the sign of single ion anisotropy, together with the magnitude of the magnetic field, tune the perpendicular spin components, mostly affecting the polarity (and, in turn, the topology) of the spin texture. Our analysis confirms the crucial role of the anisotropic symmetric exchange in systems with dominant short-range interactions; at the same time, we predict a rich variety of complex magnetic textures, which may arise from a fine tuning of competing anisotropic mechanisms.
The magnetic properties of the two-dimensional VI3 bilayer are the focus of our first-principles analysis, highlighting the role of t2g orbital splitting and carried out in comparison with the CrI3 prototypical case, where the splitting is negligible. In VI3 bilayers, the empty a1g state is found to play a crucial role in both stabilizing the insulating state and in determining the interlayer magnetic interaction. Indeed, an analysis based on maximally localized Wannier functions allows one to evaluate the interlayer exchange interactions in two different VI3 stackings (labeled AB and AB′), to interpret the results in terms of the virtual-hopping mechanism, and to highlight the strongest hopping channels underlying the magnetic interlayer coupling. Upon application of electric fields perpendicular to the slab, we find that the magnetic ground state in the AB′ stacking can be switched from antiferromagnetic to ferromagnetic, suggesting the VI3 bilayer as an appealing candidate for electric-field-driven miniaturized spintronic devices.
We investigated the relationship between ferromagnetism and metallicity in strained La0.67Ca0.33MnO3 films grown on lattice-mismatched NdGaO3 (001) by means of spectroscopic techniques directly sensitive to the ferromagnetic state, to the band structure, and to the chemical state of the atoms. In this system, the ferromagnetic metallic (FMM) phase spatially coexists with an insulating one in most of the phase diagram. First, the observation of an almost 100% spin polarization of the photoelectrons at the Fermi level in the fundamental state provides direct evidence of the half-metallicity of the FMM phase, a result that has been previously observed through direct probing of the valence band only on unstrained, phase-homogeneous La0.67Sr0.33MnO3. Second, the spin polarization results to be correlated with the occupancy at the Fermi level for all the investigated temperature regimes. These outcomes show that the half-metallic behavior predicted by a double-exchange model persists even in phase-separated manganites. Moreover, the correlation between metallicity and ferromagnetic alignment is confirmed by X-ray magnetic circular dichroism, a more bulk-sensitive technique, allowing one to explain transport properties in terms of the conduction through aligned FMM domains.
The femtosecond evolution of the electronic temperature of laser-excited gold nanoparticles is measured, by means of ultrafast time-resolved photoemission spectroscopy induced by extreme-ultraviolet radiation pulses. The temperature of the electron gas is deduced by recording and fitting high-resolution photo emission spectra around the Fermi edge of gold nanoparticles providing a direct, unambiguous picture of the ultrafast electron-gas dynamics. These results will be instrumental to the refinement of existing models of femtosecond processes in laterally-confined and bulk condensed-matter systems, and for understanding more deeply the role of hot electrons in technological applications.
Quantum materials are central for the development of novel functional systems that are often based on interface specific phenomena. Fabricating controlled interfaces between quantum materials requires adopting a flexible growth technique capable to synthesize different materials within a single-run deposition process with high control of structure, stoichiometry, and termination. Among the various available thin film growth technologies, pulsed laser deposition (PLD) allows controlling the growth of diverse materials at the level of single atomic layers. In PLD the atomic species are supplied through an ablation process of a stoichiometric target either in form of polycrystalline powders or of a single crystal. No carrier gases are needed in the deposition process. The ablation process is compatible with a wide range of background pressure. We present results of thin-film growth by PLD obtained by using an Nd:YAG infrared pulsed laser source operating at its first harmonics. With respect to the traditional PLD systems—based on excimer KrF UV-lasers—optimal conditions for the growth of thin films and heterostructures are reached at large target-to-substrate distance. Merits and limitations of this approach for growing oxide and non-oxide thin films are discussed. The merits of an Nd:YAG laser to grow very high-quality thin films suggest the possibility of implementing compact in-situ setups e.g. integrated with analytical instrumentation under ultra-high vacuum conditions.
The advent of topological semimetals enables the exploitation of symmetry-protected
topological phenomena and quantized transport. Here, we present homogeneous rectifiers,
converting high-frequency electromagnetic energy into direct current, based on low-energy
Dirac fermions of topological semimetal-NiTe2, with state-of-the-art efficiency already in the
first implementation. Explicitly, these devices display room-temperature photosensitivity as
high as 251 mA W−1 at 0.3 THz in an unbiased mode, with a photocurrent anisotropy ratio of
22, originating from the interplay between the spin-polarized surface and bulk states. Device
performances in terms of broadband operation, high dynamic range, as well as their high
sensitivity, validate the immense potential and unique advantages associated to the control of
nonequilibrium gapless topological states via built-in electric field, electromagnetic polar-
ization and symmetry breaking in topological semimetals. These findings pave the way for the
exploitation of topological phase of matter for high-frequency operations in polarization-
sensitive sensing, communications and imaging.
Research on ultrathin quantum materials requires full control of the growth and surface quality of the specimens in order to perform experiments on their atomic structure and electron states leading to ultimate analysis of their intrinsic properties. We report results on epitaxial FeSe thin films grown by pulsed laser deposition (PLD) on CaF2 (001) substrates as obtained by exploiting the advantages of an all-in-situ ultra-high vacuum (UHV) laboratory allowing for direct high-resolution surface analysis by scanning tunnelling microscopy (STM), synchrotron radiation X-ray photoelectron spectroscopy (XPS) and angle-resolved photoemission spectroscopy (ARPES) on fresh surfaces. FeSe PLD growth protocols were fine-tuned by optimizing target-to-substrate distance d and ablation frequency, atomically flat terraces with unit-cell step heights are obtained, overcoming the spiral morphology often observed by others. In-situ ARPES with linearly polarized horizontal and vertical radiation shows hole-like and electron-like pockets at the Γ and M points of the Fermi surface, consistent with previous observations on cleaved single crystal surfaces. The control achieved in growing quantum materials with volatile elements such as Se by in-situ PLD makes it possible to address the fine analysis of the surfaces by in-situ ARPES and XPS. The study opens wide avenues for the PLD based heterostructures as work-bench for the understanding of proximity-driven effects and for the development of prospective devices based on combinations of quantum materials.
Topological spin structures, such as magnetic skyrmions, hold great promises for data storage applications, thanks to their inherent stability. In most cases, skyrmions are stabilized by magnetic fields in non-centrosymmetric systems displaying the chiral Dzyaloshinskii-Moriya exchange interaction, while spontaneous skyrmion lattices have been reported in centrosymmetric itinerant magnets with long-range interactions. Here, a spontaneous anti-biskyrmion lattice with unique topology and chirality is predicted in the monolayer of a semiconducting and centrosymmetric metal halide, NiI2. Our first-principles and Monte Carlo simulations reveal that the anisotropies of the short-range symmetric exchange, when combined with magnetic frustration, can lead to an emergent chiral interaction that is responsible for the predicted topological spin structures. The proposed mechanism finds a prototypical manifestation in two-dimensional magnets, thus broadening the class of materials that can host spontaneous skyrmionic states. Skyrmions, topological spin textures, are typically stabilized by the Dzyaloshinskii-Moriya interaction and an applied magnetic field. In this theoretical study, by analysing monolayer NiI2, the authors suggest that two-site anisotropy with magnetic frustration can stabilize a skyrmion lattice.
Chiral crystal YbNi3Ga9 is known as an intermediate valence compound in which a strong hybridization between the 4f orbitals and the conduction band is present. The Co-substitution to YbNi3Ga9 works as a hole doping that reduces the Kondo temperature and enhances the effective mass of itinerant charge carriers. Using angle-resolved photoelectron spectroscopy, the complex band structure of Yb(Ni1−xCox)3Ga9 (x=0,0.1) is revealed. A Yb2+ 4f7/2 band and evidences of hybridization to valence bands are found near the Fermi level. Both YbNi3Ga9 and the Co-substituted compound exhibit double hexagonal Fermi surfaces centered at the Γ¯-point, surrounded by a large snowflake-like surface, and a triangular electron-like surface along the Γ¯M¯ direction. By changing the incident photon energy, the band dispersion along the c-axis and the barrel-shaped Fermi surface is observed.
We present the results of a photon energy and polarization dependent angle-resolved photoemission spectroscopy (ARPES) study on high quality, epitaxial SrNbO3 thin films prepared in situ by pulsed laser deposition (PLD). We show that the Fermi surface is composed of three bands mainly due to t(2g) orbitals of Nb 4d, in analogy with the 3d-based perovskite systems. The bulk band dispersion for the conduction and valence states obtained by density functional theory (DFT) is generally consistent with the ARPES data. The small discrepancy in the bandwidth close to the Fermi level seems to result from the interplay of correlation effects and the presence of vacancies. The ARPES results are complemented by soft x-ray photoemission spectroscopy measurements in order to provide indications on the chemical states and the stoichiometry of the material.
Here, we report on a novel narrowband High Harmonic Generation (HHG) light source designed for ultrafast photoelectron spectroscopy (PES) on solids. Notably, at 16.9 eV photon energy, the harmonics bandwidth equals 19 meV. This result has been obtained by seeding the HHG process with 230 fs pulses at 515 nm. The ultimate energy resolution achieved on a polycrystalline Au sample at 40 K is ∼22 meV at 16.9 eV. These parameters set a new benchmark for narrowband HHG sources and have been obtained by varying the repetition rate up to 200 kHz and, consequently, mitigating the space charge, operating with ≈3×107 electrons/s and ≈5×108 photons/s. By comparing the harmonics bandwidth and the ultimate energy resolution with a pulse duration of ∼105 fs (as retrieved from time-resolved experiments on bismuth selenide), we demonstrate a new route for ultrafast space-charge-free PES experiments on solids close to transform-limit conditions.
We predict NiTe2 to be a type-II Dirac semimetal based on ab initio calculations and explore its bulk and spin-polarized surface states using spin- and angle-resolved photoemission spectroscopy (spin-ARPES). Our results show that, unlike PtTe2, PtSe2, and PdTe2, the Dirac node in NiTe2 is located in close vicinity to the Fermi energy. Additionally, NiTe2 also hosts a pair of band inversions below the Fermi level along the Γ−A high-symmetry direction, with one of them leading to a Dirac cone in the surface states. The bulk Dirac nodes and the ladder of band inversions in NiTe2 support unique topological surface states with chiral spin texture over a wide range of energies. Our work paves the way for the exploitation of the low-energy type-II Dirac fermions in NiTe2 in the fields of spintronics, infrared plasmonics, and ultrafast optoelectronics.
The layered van der Waals antiferromagnet MnBi2Te4 has been predicted to combine the band ordering of archetypical topological insulators such as Bi2Te3 with the magnetism of Mn, making this material a viable candidate for the realization of various magnetic topological states. We have systematically investigated the surface electronic structure of MnBi2Te4(0001) single crystals by use of spin- and angle-resolved photoelectron spectroscopy experiments. In line with theoretical predictions, the results reveal a surface state in the bulk band gap and they provide evidence for the influence of exchange interaction and spin-orbit coupling on the surface electronic structure.
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 La1−xSrxMnO3. We observe that the half-metallic character of La1−xSrxMnO3 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 as a unique tool to single out the evolution of strongly correlated electronic states across a second-order phase transition in a complex material.
By performing density functional theory and Green's functions calculations, complemented by x-ray photoemission spectroscopy, we investigate the electronic structure of Fe/GeTe(111), a prototypical ferromagnetic/Rashba-ferroelectric interface. We reveal that such a system exhibits several intriguing properties resulting from the complex interplay of exchange interaction, electric polarization, and spin-orbit coupling. Despite a rather strong interfacial hybridization between Fe and GeTe bands, resulting in a complete suppression of the surface states of the latter, the bulk Rashba bands are hardly altered by the ferromagnetic overlayer. This could have a deep impact on spin-dependent phenomena observed at this interface, such as spin-to-charge interconversion, which are likely to involve bulk rather than surface Rashba states.
La misura della polarizzazione in spin di un fascio di elettroni fotoemessi da una superficie ferromagnetica permette di studiare in modo diretto la struttura elettronica determinata dall’interazione di scambio e quindi il momento magnetico di spin del sistema, caratterizzandone il comportamento magnetico. Da una parte lo sviluppo del campo della spintronica, dall’altra la richiesta sempre crescente di strumenti e dispositivi di immagazzinamento e trattamento dati ad alte prestazioni, marcano la necessità di esplorare le configurazioni degli stati elettronici e le loro eccitazioni.
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,
IrO2, 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 IrO2 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 a key role in its large spin Hall effect.
The design and characterization of a HHG source conceived for Time and Angle Resolved PhotoElectron Spectroscopy (TR-ARPES) experiments are presented. The harmonics are selected through a grating monochromator with an innovative design able to provide XUV radiation for two distinct TR-ARPES setups.
The electric and nonvolatile control of the spin texture in semiconductors would represent a fundamental step toward novel electronic devices combining memory and computing functionalities. Recently, GeTe has been theoretically proposed as the father compound of a new class of materials, namely ferroelectric Rashba semiconductors. They display bulk bands with giant Rashba-like splitting due to the inversion symmetry breaking arising from the ferroelectric polarization, thus allowing for the ferroelectric control of the spin. Here, we provide the experimental demonstration of the correlation between ferroelectricity and spin texture. A surface-engineering strategy is used to set two opposite predefined uniform ferroelectric polarizations, inward and outward, as monitored by piezoresponse force microscopy. Spin and angular resolved photoemission experiments show that these GeTe(111) surfaces display opposite sense of circulation of spin in bulk Rashba bands. Furthermore, we demonstrate the crafting of nonvolatile ferroelectric patterns in GeTe films at the nanoscale by using the conductive tip of an atomic force microscope. Based on the intimate link between ferroelectric polarization and spin in GeTe, ferroelectric patterning paves the way to the investigation of devices with engineered spin configurations.
The recent discovery of hidden spin polarization emerging in bulk electronic states of specific nonmagnetic crystals is a fascinating phenomenon, though hardly explored yet. Here, we study from a theoretical perspective nonmagnetic
BaNiS2, recently suggested to exhibit a giant Rashba-like spin-orbit splitting of the bulk bands, despite the absence of heavy elements. We employ density functional theory and Green's functions calculations to reveal the exact spin textures of both bulk and surface. We predict unambiguous signatures of spin-polarized electronic states at the surface, which reflect the bulk Rashba splitting and which could be experimentally measured with sufficient resolution: this would constitute a clear report of a bulk-Rashba-induced spin splitting at the surface of centrosymmetric crystals.