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P. Gargiani

Publications and source records attributed to P. Gargiani.

At least 19 recordsLinked to original sources

Revealing magnetism in the distorted kagome $R$Ti$_3$Bi$_4$ ($R$ = Nd, Sm, Gd) via ARPES and XMCD

Kagome materials are known for hosting emergent quantum phenomena driven by the interaction between different lattice, charge and spin orders. Here, we present a detailed angle resolved photoemission (ARPES), density functional theory (DFT) and x-ray magnetic circular dichroism (XMCD) study of the electronic and magnetic structure of $R$Ti$_3$Bi$_4$ ($R$ = Nd, Sm, Gd). ARPES and DFT demonstrate that the bulk electronic band structure is dominated by the hybridization of the Ti bands, and the weak electron-like pocket at $\Gamma$ is identified as a surface state. The isotropic XAS profile of the $M_{4,5}$-edge of the rare earth is consistent with the presence of $R^{3+}$ oxidation state. Using the XMCD sum rules, backed by the atomic multiplet theory calculations, we obtain the spin and orbital magnetic moments. The Ti $L_{2,3}$-edge XMCD reveals the presence of a small magnetic moment in GdTi$_3$Bi$_4$, presumably driven by the proximity of the {Ti} kagome layers to the $zigzag$ chains of Gd, while the total magnetic moment of Gd is shared by the $f$ and $d$ electrons. Our combined XMCD, ARPES and DFT study brings an important piece of information to understand the spin flip transitions and anomalous Hall effect observed in the $R$Ti$_3$Bi$_4$ kagome metals.

cond-mat.mtrl-sci

Trigonal distortion in the Kitaev candidate honeycomb magnet BaCo2(AsO4)2

We conducted x-ray absorption (XAS) and magnetic circular dichroism (XMCD) measurements at the Co $L_{2,3}$ edges on single crystals of the Kitaev candidate honeycomb lattice compound BaCo$_2$(AsO$_4$)$_2$. The measurements employed the inverse partial fluorescence yield technique, which is ideal for acquiring reliable x-ray absorption spectra from highly insulating samples, enabling precise quantitative analysis. Our experimental results revealed a significant linear dichroic signal, indicating strong trigonal distortion in the CoO$_{6}$ octahedra in BaCo$_2$(AsO$_4$)$_2$. We performed a detailed analysis of the experimental XAS and XMCD spectra using a full-multiplet configuration-interaction cluster model. This analysis unveiled that the $t_{2g}$ hole density is predominantly localized in the $a_{1g}$ orbital. Through XMCD sum rules and theoretical calculations, we quantified both the spin and orbital magnetic moments. Our study demonstrates that the local electronic structure of the CoO$_{6}$ octahedra displays an effective trigonal distortion of approximately $-0.114$ eV. This distortion is larger than the Co $3d$ spin-orbit coupling constant, emphasizing the crucial impact of local structural distortions on the electronic and magnetic properties of BaCo$_2$(AsO$_4$)$_2$.

cond-mat.str-el

Magnetoelastic coupling in intercalated transition metal dichalcogenides

The large van der Waals gap in transition metal dichalcogenides (TMDs) offers an avenue to host external metal atoms that modify the ground state of these 2D materials. Here, we experimentally and theoretically address the charge correlations in a family of intercalated TMDs. While short-range charge fluctuations develop in Co$_{1/3}$TaS$_{2}$ and Fe$_{1/3}$TaS$_{2}$, long-range charge order switches-on in Fe$_{1/3}$NbS$_{2}$ driven by the interplay of magnetic order and lattice degrees of freedom. The magnetoelastic coupling is demonstrated in Fe$_{1/3}$NbS$_{2}$ by the enhancement of the charge modulations upon magnetic field below T$_\mathrm{N}$, although Density Functional Perturbation Theory (DFPT) calculations predict negligible electron(spin)-phonon coupling. Furthermore, we show that Co-intercalated TaS$_2$ displays a kagome-like Fermi surface, hence opening the path to engineer electronic band structures and study the entanglement of spin, charge, and spin-phonon mechanisms in the large family of intercalated TMDs.

cond-mat.str-el

Flat band driven itinerant magnetism in the Co-pnictides CaCo$_2$As$_2$ and LaCo$_2$P$_2$

Flat bands can induce strong electron correlation effects that help stabilize both magnetic and superconducting states. Here, we carry out angle-resolved photoemission spectroscopy and density functional theory calculations to study the electronic structure of the Co-pnictides CaCo$_2$As$_2$ and LaCo$_2$P$_2$. We find that, while the $k_z$ Fermi topology of ferromagnetic LaCo$_2$P$_2$ is markedly 2-dimensional, antiferromagnetic CaCo$_2$As$_2$ develops a 3D Fermi surface described by a $zig-zag$-like band dispersion perpendicular to the Co-As plane. Furthermore, the magnetism is driven by the electronic correlations of the flat bands with $d_{xy}$ and $d_{z^2}$ orbital character at the Fermi level. Our results link the electronic dimensionality and the magnetic order, and emphasize the critical role of the As-As and P-P bond strength along the $c$-direction to understand the electronic band structure and the rich phase diagram of transition metal pnictides.

cond-mat.str-el

Self-intercalation as origin of high-temperature ferromagnetism in epitaxially grown Fe5GeTe2 thin films

The role of self-intercalation in 2D van der Waals materials is key to the understanding of many of their properties. Here we show that the magnetic ordering temperature of thin films of the 2D ferromagnet Fe5GeTe2 is substantially increased by self-intercalated Fe that resides in the van der Waals gaps. The epitaxial films were prepared by molecular beam epitaxy and their magnetic properties explored by element-specific x-ray magnetic circular dichroism that showed ferromagnetic ordering up to 375 K. Both surface and bulk sensitive x-ray absorption modes were used to confirm that the magnetic signal is of an intrinsic nature. Fe occupation within the van der Waals gap was determined by x-ray diffraction which showed a notably higher occupation with respect to bulk crystals. We thus infer, supported by first-principles calculations, that the higher magnetic ordering temperature results from an increased exchange interaction between the individual Fe5GeTe2 layers mediated by Fe atoms residing within the van der Waals gaps. Our findings establish self-intercalation during epitaxial growth as an efficient mechanism to achieve high-temperature magnetism in a broad class of van der Waals materials.

cond-mat.mtrl-sci

Epitaxial monolayers of magnetic 2D semiconductor FeBr$_{2}$ grown on Au(111)

Magnetic two-dimensional (2D) semiconductors have attracted a lot of attention because modern preparation techniques are capable of providing single crystal films of these materials with precise control of thickness down to the single-layer limit. It opens up a way to study rich variety of electronic and magnetic phenomena with promising routes towards potential applications. We have investigated the initial stages of epitaxial growth of the magnetic van der Waals semiconductor FeBr\textsubscript{2} on a single-crystal Au(111) substrate by means of low-temperature scanning tunneling microscopy, low-energy electron diffraction, x-ray photoemission spectroscopy, low-energy electron emission microscopy and x-ray photoemission electron microscopy. Magnetic properties of the one- and two-layer thick films were measured via x-ray absorption spectroscopy/x-ray magnetic circular dichroism. Our findings show a striking difference in the magnetic behaviour of the single layer of FeBr\textsubscript{2} and its bulk counterpart, which can be attributed to the modifications in the crystal structure due to the interaction with the substrate.

cond-mat.mtrl-sci

Two-dimensional ferromagnetic extension of a topological insulator

Inducing a magnetic gap at the Dirac point of the topological surface state (TSS) in a 3D topological insulator (TI) is a route to dissipationless charge and spin currents. Ideally, magnetic order is present only at the surface and not in the bulk, e.g. through proximity of a ferromagnetic (FM) layer. However, such a proximity-induced Dirac mass gap has not been observed, likely due to insufficient overlap of TSS and the FM subsystem. Here, we take a different approach, namely FM extension, using a thin film of the 3D TI Bi$_2$Te$_3$, interfaced with a monolayer of the lattice-matched van der Waals ferromagnet MnBi$_2$Te$_4$. Robust 2D ferromagnetism with out-of-plane anisotropy and a critical temperature of $\text{T}_\text{c}\approx$~15 K is demonstrated by X-ray magnetic dichroism and electrical transport measurements. Using angle-resolved photoelectron spectroscopy, we observe the opening of a sizable magnetic gap in the 2D FM phase, while the surface remains gapless in the paramagnetic phase above T$_c$. This sizable gap indicates a relocation of the TSS to the FM ordered Mn moments near the surface, which leads to a large mutual overlap.

cond-mat.mtrl-sci

Hybrid Bloch-N\'eel spiral states in Mn$_{1.4}$PtSn probed by resonant soft x-ray scattering

Multiple intriguing phenomena have recently been discovered in tetragonal Heusler compounds, where $D_{2d}$ symmetry sets a unique interplay between Dzyaloshinskii-Moriya (DM) and magnetic dipolar interactions. In the prototype $D_{2d}$ compound Mn$_{1.4}$PtSn, this has allowed the stabilization of exotic spin textures such as first-reported anti-skyrmions or elliptic Bloch-type skyrmions. While less attention has so far been given to the low-field spiral state, this remains extremely interesting as a simplest phase scenario on which to investigate the complex hierarchy of magnetic interactions in this materials family. Here, via resonant small-angle soft x-ray scattering experiments on high-quality single crystals of Mn$_{1.4}$PtSn at low temperatures, we evidence how the underlying $D_{2d}$ symmetry of the DMI in this material is reflected in its magnetic texture. Our studies reveal the existence of a novel and complex metastable phase, which possibly has a mixed character of both the N\'{e}el-type cycloid and the Bloch-type helix, that forms at low temperature in zero fields upon the in-plane field training. This hybrid spin-spiral structure has a remarkable tunability, allowing to tilt its orientation beyond high-symmetry crystallographic directions and control its spiral period. These results broaden the reachness of Heusler $D_{2d}$ materials exotic magnetic phase diagram and extend its tunability, thus enhancing a relevant playground for further fundamental explorations and potential applications in energy saving technologies.

cond-mat.str-el

Valence state determines the band magnetocrystalline anisotropy in 2D rare-earth/noble-metal compounds

In intermetallic compounds with zero-orbital momentum ($L=0$) the magnetic anisotropy and the electronic band structure are interconnected. Here, we investigate this connection on divalent Eu and trivalent Gd intermetallic compounds. We find by X-ray magnetic circular dichroism an out-of-plane easy magetization axis in 2D atom-thick EuAu$_2$. Angle-resolved photoemission and density-functional theory prove that this is due to strong $f-d$ band hybridization and Eu$^{2+}$ valence. In contrast, the easy in-plane magnetization of the structurally-equivalent GdAu$_2$ is ruled by spin-orbit-split $d$-bands, notably Weyl nodal lines, occupied in the Gd$^{3+}$ state. Regardless of the $L$ value, we predict a similar itinerant electron contribution to the anisotropy of analogous compounds.

cond-mat.mtrl-sci

Absence of magnetic-proximity effect at the interface of Bi$_2$Se$_3$ and (Bi,Sb)$_2$Te$_3$ with EuS

We performed x-ray magnetic circular dichroism (XMCD) measurements on heterostructures comprising topological insulators (TIs) of the (Bi,Sb)$_2$(Se,Te)$_3$ family and the magnetic insulator EuS. XMCD measurements allow us to investigate element-selective magnetic proximity effects at the very TI/EuS interface. A systematic analysis reveals that there is neither significant induced magnetism within the TI nor an enhancement of the Eu magnetic moment at such interface. The induced magnetic moments in Bi, Sb, Te, and Se sites are lower than the estimated detection limit of the XMCD measurements of $\sim\!10^{-3}$ $μ_\mathrm{B}$/at.

cond-mat.mes-hall

Absence of ferromagnetism in VSe$_2$ caused by its charge density wave phase

How magnetism emerges in low-dimensional materials such as transition metal dichalcogenides at the monolayer limit is still an open question. Herein, we present a comprehensive study of the magnetic properties of single crystal and monolayer VSe$_{2}$, both experimentally and \emph{ab initio}. Magnetometry, X-ray magnetic circular dichrosim (XMCD) and \emph{ab initio} calculations demonstrate that the charge density wave in bulk stoichiometric VSe$_{2.0}$ causes a structural distortion with a strong reduction in the density of sates at the Fermi level, prompting the system towards a non-magnetic state but on the verge of a ferromagnetic instability. In the monolayer limit, the structural rearrangement induces a Peierls distortion with the opening of an energy gap at the Fermi level and the absence of magnetic order. Control experiments on defect-induced VSe$_{2-δ}$ single crystals show a breakdown of magnetism, discarding vacancies as a possible origin of magnetic order in VSe$_{2}$.

cond-mat.mes-hall

Growth-sequence-dependent interface magnetism of SrIrO$_3$ - La$_{0.7}$Sr$_{0.3}$MnO$_3$ bilayers

Bilayers of the oxide 3d ferromagnet La$_{0.7}$Sr$_{0.3}$MnO$_{3}$ (LSMO) and the 5d paramagnet SrIrO$_{3}$ (SIO) with large spin-orbit coupling (SOC) have been investigated regarding the impact of interfacial SOC on magnetic order. For the growth sequence of LSMO on SIO, ferromagnetism is strongly altered and large out-of-plane-canted anisotropy associated with lacking magnetic saturation up to 4 T has been observed. Thin bilayer films have been grown coherently in both growth sequences on SrTiO$_3$ (001) by pulsed laser deposition and structurally characterized by scanning transmission electron microscopy (STEM) and x-ray diffraction (XRD). Measurements of magnetization and field-dependent Mn L$_{2,3}$ edge x-ray magnetic circular dichroism (XMCD) reveal changes of LSMO magnetic order which are strong in LSMO on SIO and weak in LSMO underneath of SIO. We attribute the impact of the growth sequence to the interfacial lattice structure/symmetry which is known to influence the interfacial magnetic coupling.

cond-mat.mtrl-sci

Coherent charge and magnetic ordering in Ho/Y superlattice revealed by element-selective x-ray scattering

Magnetic rare-earth / non-magnetic metal superlattices are well-known to display chiral spin helices in the rare-earth layers that propagate coherently across the non-magnetic layers. However, the underlying mechanism that preserves the magnetic phase and chirality coherence across the non-magnetic layers has remained elusive. In this Letter, we use resonant and element-specific x-ray scattering to evidence directly the formation of two fundamentally different long-range modulations in a Holmium/Yttrium (Ho/Y) multilayer: the known Ho chiral spin helix with periodicity 25 Å, and a newly observed charge density wave with periodicity 16 Å that propagates through both the Ho and non-magnetic Y layer. With x-ray circular magnetic dichroism measurements ruling out the existence of a magnetic proximity effect induced moment in the non-magnetic Y layers, we propose that the charge density wave is also chiral, thus providing the means for the transmittance of magnetic chirality coherence between Ho layers.

cond-mat.mes-hall

Chiral asymmetry detected in a 2D array of permalloy square nanomagnets using circularly polarized X ray Resonant Magnetic Scattering

The sensitivity of Circularly polarized X ray Resonant Magnetic Scattering (CXRMS) to chiral asymmetry has been demonstrated. The study was performed on a 2D array of Permalloy (Py) square nanomagnets of 700 nm lateral size arranged in a chess lattice of 1000 nm lattice parameter. Previous X ray Magnetic Circular Dichroism Photoemission Electron microscopy (XMCD-PEEM) images on this sample showed the formation of vortices at remanence and a preference in their chiral state. The magnetic hysteresis loops of the array along the diagonal axis of the squares indicate a non-negligible and anisotropic interaction between vortices. The intensity of the magnetic scattering using circularly polarized light along one of the diagonal axes of the square magnets becomes asymmetric in intensity in the direction transversal to the incident plane at fields where the vortex states are formed. The asymmetry sign is inverted when the direction of the applied magnetic field is inverted. The result is the expected in the presence of an unbalanced chiral distribution. The effect is observed by CXRMS due to the interference between the charge scattering and the magnetic scattering.

cond-mat.mes-hall

Systematics of electronic and magnetic properties in the transition metal doped Sb$_2$Te$_3$ quantum anomalous Hall platform

The quantum anomalous Hall effect (QAHE) has recently been reported to emerge in magnetically-doped topological insulators. Although its general phenomenology is well established, the microscopic origin is far from being properly understood and controlled. Here we report on a detailed and systematic investigation of transition-metal (TM)-doped Sb$_2$Te$_3$. By combining density functional theory (DFT) calculations with complementary experimental techniques, i.e., scanning tunneling microscopy (STM), resonant photoemission (resPES), and x-ray magnetic circular dichroism (XMCD), we provide a complete spectroscopic characterization of both electronic and magnetic properties. Our results reveal that the TM dopants not only affect the magnetic state of the host material, but also significantly alter the electronic structure by generating impurity-derived energy bands. Our findings demonstrate the existence of a delicate interplay between electronic and magnetic properties in TM-doped TIs. In particular, we find that the fate of the topological surface states critically depends on the specific character of the TM impurity: while V- and Fe-doped Sb$_2$Te$_3$ display resonant impurity states in the vicinity of the Dirac point, Cr and Mn impurities leave the energy gap unaffected. The single-ion magnetic anisotropy energy and easy axis, which control the magnetic gap opening and its stability, are also found to be strongly TM impurity-dependent and can vary from in-plane to out-of-plane depending on the impurity and its distance from the surface. Overall, our results provide general guidelines for the realization of a robust QAHE in TM-doped Sb$_2$Te$_3$ in the ferromagnetic state.

cond-mat.mes-hall

Graphene-based synthetic antiferromagnets and ferrimagnets

Hybrid Graphene/magnetic structures offer a unique playground for fundamental research, and opportunities for emerging technologies. Graphene-spaced ultrathin structures with antiferromagnetic exchange-coupling (AFC) seem a relevant scenario, analogous to that of conventional metallic multilayer devices. Unfortunately, the AFC found so far between bulk magnetic single crystals and Graphene-spaced adatoms, clusters or molecules either requires low temperatures, is too weak, or of complex nature, for realistic exploitation. Here we show theoretically and experimentally that a strong perpendicular AFC can be established in ultrahin-film structures such as Fe/Gr/Co on Ir(111), first-time enabling Graphene-based synthetic antiferromagnet and ferrimagnet materials with unprecedented magnetic properties and appearing suitable for applications. Remarkably, the established AFC is robust on structure thicknesses, thermally stable up to room temperature, very strong but field-controllable, and occurs in perpendicular orientation with opposite high remanent layer magnetizations. Our atomistic first-principle simulations provide further ground for the feasibility of Graphene-mediated AFC ultra-thin film structures, revealing that Graphene acts not only as mere spacer but has a direct role in sustaining antiferromagnetic superexchange-coupling between the magnetic layers. These results provide a path for the design of unique and ultimately-thin synthetic antiferromagnetic structures, which seem exciting for fundamental nanoscience studies or for potential use in Graphene-spintronics applications.

cond-mat.mtrl-sci

Absence of magnetic proximity effects in magnetoresistive Pt/CoFe2O4 hybrid interfaces

Ultra-thin Pt films grown on insulating ferrimagnetic CoFe2O4 (111) epitaxial films display a magnetoresistance upon rotating the magnetization of the magnetic layer. We report here X-ray magnetic circular dichroism (XMCD) recorded at Pt-L2,3 and Pt-M3 edges. The results indicate that the Pt magnetic moment, if any, is below the detection limit (< 0.001 μ$_B$/Pt), thus strongly favoring the view that the presence of CoFe2O4 does not induce the formation of magnetic moments in Pt. Therefore, the observed magnetoresistance cannot be attributed to some sort of proximity-induced magnetic moments at Pt ions and subsequent magnetic-field dependent scattering. It thus follows that either bulk (spin Hall and Inverse spin Hall Effects) or interface (Rashba) spin-orbit related effects dominate the observed magnetoresistance. Furthermore, comparison of bulk magnetization and XMCD data at (Fe,Co)-L2,3 edges suggests the presence of some spin disorder in the CoFe2O4 layer which may be relevant for the observed anomalous non-saturating field-dependence of spin Hall magnetoresistance.

cond-mat.mtrl-sci

Mesoscopic electron focusing in topological insulators

The particle wave duality sets a fundamental correspondence between optics and quantum mechanics. Within this framework, the propagation of quasiparticles can give rise to superposition phenomena which, like for electromagnetic waves, can be described by the Huygens principle. However, the utilization of this principle by means of propagation and manipulation of quantum information is limited by the required coherence in time and space. Here we show that in topological insulators, which in their pristine form are characterized by opposite propagation directions for the two quasiparticles spin channels, mesoscopic focusing of coherent charge density oscillations can be obtained at large nested segments of constant energy contours by magnetic surface doping. Our findings provide evidence of strongly anisotropic Dirac fermion-mediated interactions. Even more remarkably, the validity of our findings goes beyond topological insulators but applies for systems with spin orbit lifted degeneracy in general. It demonstrates how spin information can be transmitted over long distances, allowing the design of experiments and devices based on coherent quantum effects in this fascinating class of materials.

cond-mat.mes-hall