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Pierluigi Gargiani

Publications and source records attributed to Pierluigi Gargiani.

At least 19 recordsLinked to original sources

Revealing the origin of XMCD in an altermagnet via three-dimensional control of spins

Altermagnets are an emerging class of collinear antiferromagnets that exhibit unconventional spin-polarised electronic bands, potentially unlocking new functionalities that do not rely on spin-orbit coupling (SOC). Experimental signatures traditionally associated with spin polarisation, like X-ray magnetic circular dichroism (XMCD), are thus being used as a validation of altermagnetism. However, unlike altermagnetic spin-splitting, these responses require SOC and are not invariant under spin-space rotations. This brings into question the extent to which they can be considered direct signatures of altermagnetism. Here, we exploit the g-wave altermagnet $α$-Fe$_{2}$O$_{3}$ to demonstrate that XMCD is governed precisely by the spin-direction-induced symmetry breaking that altermagnetic spin groups are designed to ignore. Strikingly, the XMCD is highly anisotropic and is decoupled from the weak magnetic canting. We show that this anomalous XMCD can be described by on-site Faraday tensors capturing the locally uncompensated spin-orbital anisotropies - a scenario that can be applied to other altermagnets. Leveraging this, we reconstruct complete vectorial maps of nanoscale textures in $α$-Fe$_{2}$O$_{3}$ thin films, including domain walls and topological solitons, which are promising for building future spintronics and magnonics devices.

cond-mat.mtrl-sci

A Surface-confined Spiral State With the Double Period in the Cubic Chiral Helimagnet Cu$_2$OSeO$_3$

The chiral magnetoelectric insulator Cu$_2$OSeO$_3$ hosts a rich and anisotropic magnetic phase diagram that includes helical, conical, field-polarised, tilted conical, and skyrmion lattice phases. Using resonant elastic x-ray scattering (REXS), we uncover a new spiral state confined to the surface of Cu$_2$OSeO$_3$. This surface-confined spiral state (SSS) displays a real-space pitch of $\sim$120 nm, which remarkably is twice the length of the incommensurate structures observed to-date in Cu$_2$OSeO$_3$. The SSS phase emerges at temperatures below 30~K when the magnetic field is applied between $3^\circ$ to $18^\circ$ away from the $\langle\text{110}\rangle$ crystallographic axes. Its surface localisation is demonstrated through a combination of REXS in reflection and transmission geometries, with complementary small-angle neutron scattering measurements suggesting its absence from the bulk. We attribute the stabilisation of the SSS to competing anisotropic interactions at the crystal surface. The discovery of a robust, surface-confined spiral paves the way for engineering energy-efficient, nanoscale spin-texture platforms for next-generation devices.

cond-mat.str-el

Atomic-Scale Detection of Néel Vector Switching in the Single-Layer A-type Antiferromagnet Cr2S3-2D

The detection of Néel vector switching in a single-layer A-type antiferromagnet marks an important step toward functional two-dimensional spintronics. Here, Cr$_2$S$_3$-2D, grown on graphene on Ir(110), is established as a first single-layer A-type antiferromagnet. Spin-polarized scanning tunneling microscopy reveals hysteresis loops with a large switching field and a pronounced dependence on island size. X-ray magnetic circular dichroism at the Cr L$_{2,3}$ edges exhibits a tiny signal with a linear magnetic field dependence, consistent with a nearly compensated antiferromagnetic ground state and a Néel temperature of about 160 K. Quantitative analysis of the island-size dependence of the switching field, together with first principles calculations, indicates a slight imbalance between the magnetic moments of the two Cr planes of Cr$_2$S$_3$-2D when supported on a substrate. This imbalance results in a net magnetization for the A-type antiferromagnet, which enables the 180$^\circ$ rotation of the Néel vector. Moreover, Cr$_2$S$_3$-2D retains its magnetic properties after several days of exposure to air.

cond-mat.mes-hall

Noncollinear spin structure in Dy-doped classical ferrimagnet

Noncollinear spin structures have attracted tremendous attention because they offer a versatile platform for spin control and manipulation, essential in spintronics. Realizing noncollinearity in ferrimagnetic insulators is of particular interest as they can be potentially utilized in low-damping spintronics with tunable magnetic order. Within the spinel-ferrite family, Zn and Al-substituted nickel ferrite (NiZAF) has emerged as an excellent choice for low-damping spintronics. However, realizing noncollinearity in such systems remains challenging. Here, we present evidence of noncollinear spin structure in the NiZAF thin films induced by the rare earth Dy-doping, utilizing the soft x-ray spectroscopy methods such as magnetic circular dichroism and x-ray resonant magnetic reflectivity (XRMR). In particular, XRMR reveals a spiral-type spin structure, which is attributed to the Dzyaloshinskii-Moriya interaction, arising due to broken inversion symmetry by the Dy-induced local strain field as confirmed by our theoretical calculations. The realization of noncollinearity in the spinel-ferrite opens pathway to explore the possibility of chiral magnetic domains and topological spin textures exhibiting promise for oxide-based spintronics

cond-mat.mtrl-sci

Tunable magnetism in 2D organic-ion-intercalated MnPS3 via molecule-dependent vacancy generation

The magnetic properties of van der Waals materials are profoundly influenced by structural defects. The layered antiferromagnet MnPS3 offers a unique opportunity to explore defect-related magnetism, as Mn2+ vacancies can be generated by the intercalation of specific guest molecules. However, the effectiveness of this process in atomically thin flakes and the extent of the magnetic tunability remain unclear. Here, we show that the magnetic properties of MnPS3 can be tailored through the intercalation of different guest molecules. Notably, the insertion of four alkylammonium ions introduces different populations of Mn2+ vacancies, leading to a transition from the pristine antiferromagnetic state to more complex magnetic textures, including a ferrimagnetic state displaying a magnetic saturation of 1 uB/atom. Moreover, we show that the intercalation of few-nm-thick flakes also leads to the emergence of a ferrimagnetic response. This in-flake intercalation, which can be monitored in real time using optical microscopy, can be interrupted before completion, generating lateral heterostructures between pristine and intercalated areas. This approach opens the way to the use of partial intercalation to define regions with distinct magnetic properties within a single flake.

cond-mat.mtrl-sci

Sensing a magnetic rare-earth surface alloy by proximity effect with an open-shell nanographene

Open-shell nanographenes have attracted significant attention due to their structurally tunable spin ground state. While most characterization has been conducted on weakly-interacting substrates such as noble metals, the influence of magnetic surfaces remains largely unexplored. In this study, we investigate how TbAu2, a rare-earth-element-based surface alloy, affects the magnetic properties of phenalenyl (or [2]triangulene (2T)), the smallest spin-1/2 nanographene. Scanning tunneling spectroscopy (STS) measurements reveal a striking contrast: while 2T on Au(111) exhibits a zero-bias Kondo resonance - a hallmark of a spin-1/2 impurity screened by the conduction electrons of the underlying metal - deposition on TbAu2 induces a symmetric splitting of this feature by approximately 20 mV. We attribute this splitting to a strong proximity-induced interaction with the ferromagnetic out-of-plane magnetization of TbAu2. Moreover, our combined experimental and first-principles analysis demonstrates that this interaction is spatially modulated, following the periodicity of the TbAu2 surface superstructure. These findings highlight that TbAu2 serves as a viable platform for stabilizing and probing the magnetic properties of spin-1/2 nanographenes, opening new avenues for the integration of π-magnetic materials with magnetic substrates.

cond-mat.mtrl-sci

Emergent Magnetic Structures at the 2D Limit of the Altermagnet MnTe

MnTe has recently emerged as a canonical altermagnet, a newly identified class of magnetism characterized by compensated antiferromagnetic order coexisting with spin-split electronic bands, traditionally considered exclusive to ferromagnets. However, the extent to which altermagnetism persists as altermagnets are thinned to the two-dimensional (2D) limit remains unexplored. Here, we investigate the magnetic behaviour of 2D MnTe, specifically atomically-thin monolayers (MLs) and bilayers (BLs) grown on graphene/Ir(111) substrate, by combining experimental scanning tunneling microscopy, x-ray photoelectron spectroscopy, x-ray absorption spectroscopy and x-ray magnetic circular dichroism with density functional theory calculations. We find that while ML and BL MnTe adopt atomic structures with symmetries incompatible with altermagnetism, they exhibit intriguing magnetic phases: the BL forms a highly-robust layered antiferromagnet with in-plane spin anisotropy, whereas the ML exhibits a spin-glass-like behavior below its freezing temperature, a phenomenon not previously observed in an atomically thin material. These findings highlight how reduced dimensionality can promote the emergence of unusual magnetic structures distinct from those of their three-dimensional counterparts, providing new insights into low-dimensional magnetism.

cond-mat.mtrl-sci

Magnetic single wall CrI3 nanotubes encapsulated within multiwall Carbon Nanotubes

CrI3 is a layered ferromagnetic insulator that has recently attracted enormous interest as it was the first example of a stand-alone monolayer ferromagnet, paving the way towards the study of two-dimensional magnetic materials and their use as building blocks of hybrid van der Waals layered heterostructures. Here we go one step down in the dimensionality ladder and report the synthesis and characterization of a tubular one-dimensional van der Waals heterostructure where CrI3 nanotubes are encapsulated within multiwall carbon nanotubes, integrating a magnetic insulator and a conductor. By means of the capillary filling of multi-wall carbon nanotubes (MWCNT), we obtained single-wall CrI3 nanotubes with diameters ranging between 2 nm and 10 nm, with an average of 5.3 nm. Using aberration corrected electron microscopy in combination with spectroscopic techniques we confirm the structure and chemical composition of the nanotubes. SQUID measurements, combined with element-specific X-ray magnetic circular dichroism (XMCD) indicate unequivocally that the Cr atoms in encapsulated CrI3 nanotubes are magnetic with a collective state compatible with a radial magnetization state predicted both by first-principles calculations and a model Hamiltonian. Our results represent a step forward in establishing 1D van der Waals heterostructures as a playground for the exploration of non-collinear magnetic states arising from the interplay between magnetic anisotropy and curvature in tubular geometries.

cond-mat.mtrl-sci

Room Temperature Strong Orbital Moments in Perpendicularly Magnetized Magnetic Insulator

The balance between the orbital and spin magnetic moments in a magnetic system is the heart of many intriguing phenomena. Here, we show experimental evidence of a large orbital moment, which competes with its spin counterpart in a ferrimagnetic insulator thulium iron garnet, Tm3Fe5O12. Leveraging element-specific X-ray magnetic circular dichroism (XMCD), we establish that the dominant contribution to the orbital moment originates from 4f orbitals of Tm. Besides the large Tm orbital moment, intriguingly, our results also reveal a smaller but evident non-zero XMCD signal in the O K edge, suggesting additional spin-orbit coupling and exchange interactions with the nearest neighbour Fe atoms. The unquenched orbital moment is primarily responsible for a significant reduction in g-factor, typically 2 in transition metals, as determined independently using ferromagnetic resonance spectroscopy. Our findings reveal a non-linear reduction in the g-factor from 1.7 at 300 K to 1.56 at 200 K in Tm3Fe5O12 thin films. These results provide critical insights into the role of the f orbitals in long-range magnetic order and stimulate further exploration in orbitronics.

cond-mat.mtrl-sci

The role of rare-earth atoms in the anisotropy and antiferromagnetic exchange coupling at a hybrid metal-organic interface

Magnetic anisotropy and magnetic exchange interactions are crucial parameters that characterize the hybrid metal-organic interface, key component of an organic spintronic device. We show that the incorporation of 4$f$ RE atoms to hybrid metal-organic interfaces of CuPc/REAu$_2$ type (RE= Gd, Ho) constitutes a feasible approach towards on-demand magnetic properties and functionalities. The GdAu$_2$ and HoAu$_2$ substrates differ in their magnetic anisotropy behavior. Remarkably, the HoAu$_2$ surface boosts the inherent out-of-plane anisotropy of CuPc, owing to the match between the anisotropy axis of substrate and molecule. Furthermore, the presence of RE atoms leads to a spontaneous antiferromagnetic (AFM) exchange coupling at the interface, induced by the 3$d$-4$f$ superexchange interaction between the unpaired 3$d$ electron of CuPc and the 4$f$ electrons of the RE atoms. We show that 4$f$ RE atoms with unquenched quantum orbital momentum ($L$), as it is the case of Ho, induce an anisotropic interfacial exchange coupling.

cond-mat.mtrl-sci

Spin re-orientation induced anisotropic magnetoresistance switching in LaCo$_{0.5}$Ni$_{0.5}$O$_{3-δ}$ thin films

Realization of novel functionalities by tuning magnetic interactions in rare earth perovskite oxide thin films opens up exciting technological prospects. Strain-induced tuning of magnetic interactions in rare earth cobaltates and nickelates is of central importance due to their versatility in electronic transport properties. Here we reported the spin re-orientation induced switching of anisotropic magnetoresistance (AMR) and its tunability with strain in epitaxial LaCo$_{0.5}$Ni$_{0.5}$O$_{3-δ}$ thin films across the ferromagnetic transition. Moreover, with strain tuning, we could observe a two-fold to four-fold symmetry crossover in AMR across the magnetic transition temperature. The magnetization measurements revealed an onset of ferromagnetic transition around 50 K, and a further reduction in temperature showed a subtle change in the magnetization dynamics, which reduced the ferromagnetic long-range ordering and introduced glassiness in the system. X-ray absorption and X-ray magnetic circular dichroism spectroscopy measurements over Co and Ni L edges revealed the Co spin state transition below the magnetic transition temperature leading to the AMR switching and also the presence of Ni$^{2+}$ and Co$^{4+}$ ions evidencing the charge transfer from Ni to Co ions. Our work demonstrated the tunability of magnetic interactions mediated electronic transport in cobaltate-nickelate thin films, which is relevant in understanding Ni-Co interactions in oxides for their technological applications such as in AMR sensors.

cond-mat.mtrl-sci

Intermixing-driven surface and bulk ferromagnetism in the quantum anomalous Hall candidate MnBi$_6$Te$_{10}$

The recent realizations of the quantum anomalous Hall effect (QAHE) in MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$ benchmark the (MnBi$_2$Te$_4$)(Bi$_2$Te$_3$)$_n$ family as a promising hotbed for further QAHE improvements. The family owes its potential to its ferromagnetically (FM) ordered MnBi$_2$Te$_4$ septuple layers (SL). However, the QAHE realization is complicated in MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$ due to the substantial antiferromagnetic (AFM) coupling between the SL. An FM state, advantageous for the QAHE, can be stabilized by interlacing the SL with an increasing number $n$ of Bi$_2$Te$_3$ layers. However, the mechanisms driving the FM state and the number of necessary QLs are not understood, and the surface magnetism remains obscure. Here, we demonstrate robust FM properties in MnBi$_6$Te$_{10}$ ($n = 2$) with $T_C \approx 12$ K and establish their origin in the Mn/Bi intermixing phenomenon by a combined experimental and theoretical study. Our measurements reveal a magnetically intact surface with a large magnetic moment, and with FM properties similar to the bulk. Our investigation thus consolidates the MnBi$_6$Te$_{10}$ system as perspective for the QAHE at elevated temperatures.

cond-mat.mtrl-sci

Ferromagnetism on an atom-thick and extended 2D-metal-organic framework

Ferromagnetism (FM) is the cornerstone of permanent magnets, data storage and other technologies that directly impact our everyday life by their implementation in standard applications and devices. When downscaling bulk materials into their two-dimensional (2D) magnetic isotropic form, the Mermin-Wagner theorem precludes this collective state mediated by short-range exchange interactions at finite temperatures. Interestingly, this prediction fails when significant magnetic anisotropy is present in the material, as recently demonstrated in single layered van der Waals crystals. Before the latter, single layer metal-organic frameworks (MOFs) grown on metallic supports were one of the earliest candidates for achieving 2D-FM. Such high expectations were based on the chemical and spacing control of the 2D-MOF magnetic centers, the tunability of the organic linkers and the rich self-assembled architectures displayed. However, despite many attempts, extended FM in 2D-MOFs has been experimentally elusive. In this work, we demonstrate that extended, cooperative FM takes place in an atom thick 2D-MOF consisting of 9,10-dicyanoanthracene (DCA) molecules and Fe adatoms grown on Au(111). We show this by means of an experimental multitechnique approach that is endorsed by state-of-the art first-principles calculations. Particularly, this 2D ferromagnet follows a first order transition with TC ~ 35 K, which is driven by exchange interactions mainly through the molecular linkers (J=2 meV) and exhibits an out-of-plane square-like hysteresis loop. The strict periodicity of our 2D-MOF allows us to envision the fabrication of ultra-dense single atom magnetic memories and opens the way to explore periodic magnetic 2D-models that could considerably increase the fundamental superparamagnetic limit.

cond-mat.mtrl-sci

Ultrafast X-ray imaging of the light-induced phase transition in VO2

Using light to control transient phases in quantum materials is an emerging route to engineer new properties and functionality, with both thermal and non-thermal phases observed out of equilibrium. Transient phases are expected to be heterogeneous, either through photo-generated domain growth or by generating topological defects, and this impacts the dynamics of the system. However, this nanoscale heterogeneity has not been directly observed. Here we use time- and spectrally resolved coherent X-ray imaging to track the prototypical light induced insulator-to-metal phase transition in vanadium dioxide on the nanoscale with femtosecond time resolution. We show that the early-time dynamics are independent of the initial spatial heterogeneity and observe a 200 fs switch to the metallic phase. A heterogeneous response emerges only after hundreds of picoseconds. Through spectroscopic imaging, we reveal that the transient metallic phase is a highly orthorhombically strained rutile metallic phase, an interpretation that is in contrast to those based on spatially averaged probes. Our results demonstrate the critical importance of spatially and spectrally resolved measurements for understanding and interpreting the transient phases of quantum materials.

cond-mat.str-el

Orbital Occupancy and Hybridization in Strained SrVO$_3$ Epitaxial Films

Oxygen packaging in transition metal oxides determines the metal-oxygen hybridization and electronic occupation at metal orbitals. Strontium vanadate (SrVO$_3$), having a single electron in a $3d$ orbital, is thought to be the simplest example of strongly correlated metallic oxides. Here, we determine the effects of epitaxial strain on the electronic properties of SrVO$_3$ thin films, where the metal-oxide sublattice is corner-connected. Using x-ray absorption and x-ray linear dichroism at the V $L_{2,3}$ and O $K$-edges, it is observed that tensile or compressive epitaxial strain change the hierarchy of orbitals within the $t_{2g}$ and $e_g$ manifolds. Data show a remarkable $2p-3d$ hybridization, as well as a strain-induced reordering of the V $3d$($t_{2g}$, $e_g$) orbitals. The latter is itself accompanied by a consequent change of hybridization that modulates the hybrid $π^*$ and $σ^*$ orbitals and the carrier population at the metal ions, challenging a rigid band picture.

cond-mat.str-el

Intrinsic 2D-XY ferromagnetism in a van der Waals monolayer

Long before the recent fascination with two-dimensional materials, the critical behaviour and universality scaling of phase transitions in low-dimensional systems has been a topic of great interest. Particularly intriguing is the case of long-range magnetic order in two dimensions, once considered to be excluded in systems with continuous symmetry by the Hohenberg-Mermin-Wagner theorem. While an out-of-plane anisotropy has been shown to stabilize 2D magnetic order, this proof has remained elusive for a 2D magnet with in-plane rotational symmetry. Here, we construct a nearly ideal easy-plane system, a CrCl3 monolayer grown on Graphene/6H-SiC (0001), and unambiguously demonstrate robust in-plane ferromagnetic ordering with a critical scaling behaviour characteristic of a 2D-XY system. These observations suggest the first realization of a finite-size Berezinskii-Kosterlitz-Thouless (BKT) phase transition in a large-area, quasi-freestanding, van der Waals monolayer magnet with a XY universality class; and further constitute an ideal platform to study exotic phenomena like superfluid spin transport or 2D topological in-plane spin textures -- such as merons.

cond-mat.mes-hall

Magnetic response and electronic states of well defined Graphene/Fe/Ir(111) heterostructure

We investigate a well defined heterostructure constituted by magnetic Fe layers sandwiched between graphene (Gr) and Ir(111). The challenging task to avoid Fe-C solubility and Fe-Ir intermixing has been achieved with atomic controlled Fe intercalation at moderate temperature below 500 K. Upon intercalation of a single ordered Fe layer in registry with the Ir substrate, an intermixing of the Gr bands and Fe d states breaks the symmetry of the Dirac cone, with a downshift in energy of the apex by about 3 eV, and well-localized Fe intermixed states induced in the energy region just below the Fermi level. First principles electronic structure calculations show a large spin splitting of the Fe states, resulting in a majority spin channel almost fully occupied and strongly hybridized with Gr π states. X-ray magnetic circular dichroism on the Gr/Fe/Ir heterostructure reveals an ordered spin configuration with a ferromagnetic response of Fe layer(s), with enhanced spin and orbital configurations with respect to the bcc-Fe bulk values. The magnetization switches from a perpendicular easy magnetization axis when the Fe single layer is lattice matched with the Ir(111) surface to a parallel one when the Fe thin film is almost commensurate with graphene.

cond-mat.mtrl-sci

Orbital-resolved single atom magnetism measured with X-ray absorption spectroscopy

Lanthanide atoms and molecules are promising candidates for atomic data storage and quantum logic due to the long magnetic lifetime of their electron quantum states. Accessing these states through electrical transport requires the engineering of their electronic configuration down to the level of individual atomic orbitals. Here, we address the magnetism of surface-supported lanthanide atoms, clusters, and films with orbital selectivity using X-ray absorption spectroscopy and magnetic circular dichroism. We exploit the selection rules of electric dipole transitions to reveal the occupation and magnetism of the valence electrons of Gd and Ho deposited on MgO/Ag(100). Comparing our results with multiplet calculations and density functional theory, we identify a charge transfer mechanism that leaves the lanthanide species in an unconventional singly ionized configuration. Our approach allows determining the role of valence electrons on the quantum level structure of lanthanide-based nanostructures.

cond-mat.mes-hall