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Philippe Ohresser

Publications and source records attributed to Philippe Ohresser.

18 recordsLinked to original sources

High temperature ferromagnetism in epitaxial monolayers of Co-doped Fe5GeTe2

Magnetic van der Waals materials have mainly been investigated in their bulk form or as few-layers flakes. Due to the challenges in producing atomically thin films, only a few have been isolated as monolayers, which typically exhibit long-range magnetic order below 150 K. In this work, we use molecular beam epitaxy to synthesize Co-doped Fe5GeTe2, achieving precise control over both thickness and composition. We demonstrate ferromagnetism well above room temperature in multilayer samples and present clear evidence of ferromagnetic ordering in monolayers up to $\sim$200 K. The changes in Curie temperature and magnetic anisotropy with composition exhibit similar trends in both monolayers and thicker films, indicating that the magnetic properties are primarily governed by intralayer magnetic interactions. Through element-specific X-ray magnetic circular dichroism and density functional theory, we identify the substitution site of Co dopants and reveal the mechanism behind the Curie temperature enhancement induced by Co doping. Our findings suggest that, despite their weak magnetic moment, Co dopants strengthen the magnetic moments on neighboring Fe atoms and enhance the intralayer ferromagnetic exchange interactions.

cond-mat.mtrl-sci

Disorder-driven symmetry suppression by van der Waals planar defects in a magnetic topological insulator

Magnetic topological insulators offer a platform to control electronic topology through magnetic order, yet reliable routes to tune their properties remain limited. Here, we show that ion irradiation allows to modify the magnetic and the topological properties of the van der Waals magnetic topological insulator MnBi$_2$Te$_4$. Using inert ion beams, intrinsic defects are introduced via collision cascades without chemical doping. We identify two distinct regimes. At low fluence, cation antisite disorder leads to a near-complete redistribution of Bi over cation sites while preserving long-range crystallographic order, accompanied by a transition from $p$-type to $n$-type transport. At high fluence, cation-anion intermixing drives the formation of a previously unreported layer-disordered phase characterized by a high density of van der Waals-specific planar defects, including swapped bilayers. Despite significant structural disorder, the system retains partial periodic order up to high displacement levels. Magnetometry and X-ray spectroscopy show that the Mn high-spin state and antiferromagnetic interactions persist, while magnetic anisotropy is strongly reduced. At the same time, the anomalous Hall conductivity is suppressed fivefold, far exceeding the change in magnetization, indicating a direct modification of Berry curvature. These results establish ion irradiation as a means to tune topology through defect engineering and reveal a disorder-driven approach to control symmetry and electronic structure in van der Waals magnetic materials.

cond-mat.mtrl-sci

Electronic and magnetic properties of light rare-earth cubic Laves compounds derived from XMCD experiments

This work presents electronic and magnetic properties of selected members in the cubic Laves phase series Nd1-xPrxCoNi and Ce0.25Pr0.75CoNi, together with the corresponding binary compositions (NdCo2, NdNi2, PrCo2, PrNi2, CeCo2, CeNi2), using soft x-ray absorption spectroscopy, x-ray magnetic circular dichroism (XMCD), density-functional theory, and crystal field multiplet calculations. All transition-metal moments saturate below 1 T, while the rare-earth moments do not saturate even at 5 T, consistent with van Vleck paramagnetic contributions and crystal field suppression. While the sum rules are widely used to extract element-specific magnetic moments from XMCD, we show that for 3d transition metals, their application requires accurate estimates of the number of unoccupied 3d states. We observe a finite magnetic moment on Ni, challenging the common assumption of its nonmagnetic character in Laves phases. The orbital magnetic moments were determined using the spin rules, while the spin moments were estimated from single-ion values from multiplet calculations, due to the invalidity of the spin sum rule for light rare-earth elements. The magnetic moments of Nd and Pr are found to be suppressed relative to their free-ion values, with multiplet theory indicating that this is due to crystal field effects. Our results confirm that Nd and Pr maintain localized 4f3 and 4f2 configurations, respectively, and that their element-specific magnetic moments are robust to rare-earth substitution. Ce, on the other hand, exhibits a tunable mixed-valent ground state with both magnetic 4f1 and nonmagnetic 4f0 components. The relative fraction of these states varies with the electronegativity of the surrounding 3d transition metals, revealing a pathway to tune Ce magnetism via composition. This work establishes a framework for accurately interpreting XMCD in light rare-earth-based intermetallics.

cond-mat.mtrl-sci

Inducing ferromagnetism by structural engineering in a strongly spin-orbit coupled oxide

Magnetic materials with strong spin-orbit coupling (SOC) are essential for the advancement of spin-orbitronic devices, as they enable efficient spin-charge conversion, complex magnetic structures, spin-valley physics, topological phases and other exotic phenomena. 5d transition-metal oxides such as SrIrO3 feature large SOC, but usually show paramagnetic behavior due to broad bands and a low density of states at the Fermi level, accompanied by a relatively low Coulomb repulsion. Here, we unveil ferromagnetism in 5d SrIrO3 thin films grown on SrTiO3 (111). Through substrate-induced structural engineering, a zigzag stacking of three-unit-cell thick layers along the [111] direction is achieved, stabilizing a ferromagnetic state at the interfaces. Magnetotransport measurements reveal an anomalous Hall effect below ~30 K and hysteresis in the Hall conductivity below 7 K, indicating ferromagnetic ordering. X-ray magnetic circular dichroism further supports these results. Theoretical analysis suggests that the structural engineering of the IrO6 octahedral network enhances the density of states at the Fermi level and thus stabilizes Stoner ferromagnetism. This work highlights the potential of structurally engineered 5d oxides for spin-orbitronic devices, where efficient control of SOC-induced magnetic phases by electric currents can lead to lower energy consumption and improved performance in next-generation device technologies.

cond-mat.mtrl-sci

Effects of antiferromagnetic coupling and pinning on domain wall dynamics in synthetic ferrimagnets

Domain wall (DW) dynamics in antiferromagnetic (AFM) systems offer the advantages over their ferromagnetic counterparts of having faster and more energy efficient manipulation due to the absence of net magnetization, leading to reduced magnetic crosstalk and improved performance in spintronic devices. A comprehensive analysis of DW dynamics across regimes such as creep, depinning, and flow is well established in ferromagnetic systems but remains lacking in AFM-coupled systems. In this study, we explore the nature of DW dynamics in synthetic ferrimagnetic multilayers composed of Pt|Co|Tb|Al for different Tb thickness, focusing on the underlying pinning parameters, and on the different regimes of DW dynamics driven by spin-orbit torques (SOTs). We find that due to the AFM coupling between Co and Tb, the magnetic moment of Tb increases with Tb thickness resulting in a reduced saturation magnetization and an enhanced depinning field. The DW disorder interaction is found to vary weakly with the AFM coupling between Co and Tb, while the complete withdrawal of the Tb layer strongly increases the anisotropy and the DW pinning. Furthermore, we propose a novel approach to measure effective SOTs by comparing depinning transitions in current and field-induced DW motion. This research reveals new insights into DW dynamics in coupled AFM systems, highlighting enhancements in mobility through optimized SOTs and pinning landscapes.

cond-mat.other

Interfacial spin-orbitronic effects controlled with different oxidation levels at the Co|Al interface

Perpendicular magnetic anisotropy (PMA) and Dzyaloshinskii-Moriya interactions are key interactions in modern spintronics. These interactions are thought to be dominated by the oxidation of the Co|Al interface in the archetypal Platinum-Cobalt-Aluminum oxide system. Here, we observe a double sign change in the anisotropy and about threefold variation in interfacial chiral interaction, influenced not only by the oxidation, but also by the metallic Al thickness. Contrary to previous assumptions about negligible spin-orbit effects at light metal interfaces, we not only observe strong PMA with fully oxidized Al, decreasing and turning negative (in-plane) with less oxygen at the Co|Al interface, we also observe that the magnetic anisotropy reverts to positive (out-of-plane) values at fully metallic Co|Al interface. These findings suggest modification in Co d band via Co|Al orbital hybridization, an effect supported by X-ray absorption spectroscopy and ab initio theory calculations, highlighting the key impact of strain on interfacial mechanisms at fully metallic Co|Al interface.

cond-mat.mtrl-sci

Multi-Orbital Interactions and Spin Polarization in Single Rare-Earth Adatoms

Surface-adsorbed rare-earth nanostructures are ideal platforms to investigate the interplay between intra-atomic interactions and multi-orbital spin configurations. However, addressing these properties has posed severe experimental and theoretical challenges. Here, we use the orbital selectivity offered by X-ray absorption spectroscopy to quantify the Coulomb integrals of Nd atoms on conductive surfaces, as well as the variation of individual orbital occupation upon cluster nucleation. Using X-ray magnetic circular dichroism we identify magnetic moments of the order of \MK{few tens of}~$μ_{\rm{B}}$ at the $5d$ orbitals and their magnetic coupling with the $4f$ spins. Our results validate orbital-resolved X-ray spectroscopy as a reliable method for quantifying complex multi-orbital interactions in surface-adsorbed lanthanides.

cond-mat.mes-hall

Magnetic evolution of Cr$_2$Te$_3$ epitaxially grown on graphene with post-growth annealing

Two-dimensional and van der Waals ferromagnets are ideal platform to study low dimensional magnetism and proximity effects in van der Waals heterostructures. Their ultimate two dimensional character offers also the opportunity to easily adjust their magnetic properties using strain or electric fields. Among 2D ferromagnets, the Cr$_{1+x}$Te$_2$ compounds with $x$=0-1 are very promising because their magnetic properties depend on the amount of self-intercalated Cr atoms between pure CrTe$_2$ layers and the Curie temperature (T$_C$) can reach room temperature for certain compositions. Here, we investigate the evolution of the composition, structural and magnetic properties of thin Cr$_{1.33}$Te$_2$ (Cr$_2$Te$_3$) films epitaxially grown on graphene upon annealing. We observe a transition above 450°C from the Cr$_{1.33}$Te$_2$ phase with perpendicular magnetic anisotropy and a T$_C$ of 180 K to a composition close to Cr$_{1.39}$Te$_2$ with in-plane magnetic anisotropy and a T$_C$ of 240-250 K. This phase remains stable up to 650°C above which a pure Cr film starts to form. This work demonstrates the complex interplay between intercalated Cr, lattice parameters and magnetic properties in Cr$_{1+x}$Te$_2$ compounds.

cond-mat.mtrl-sci

Epitaxial van der Waals heterostructures of Cr2Te3 on 2D materials

Achieving large-scale growth of two-dimensional (2D) ferromagnetic materials with high Curie temperature (TC) and perpendicular magnetic anisotropy (PMA) is highly desirable for the development of ultra-compact magnetic sensors and magnetic memories. In this context, van der Waals (vdW) Cr2Te3 appears as a promising candidate. Bulk Cr2Te3 exhibits strong PMA and a TC of 180 K. Moreover, both PMA and TC might be adjusted in ultrathin films by engineering composition, strain, or applying an electric field. In this work, we demonstrate the molecular beam epitaxy (MBE) growth of vdW heterostructures of five-monolayer quasi-freestanding Cr2Te3 on three classes of 2D materials: graphene (semimetal), WSe2 (semiconductor) and Bi2Te3 (topological insulator). By combining structural and chemical analysis down to the atomic level with ab initio calculations, we confirm the single crystalline character of Cr2Te3 films on the 2D materials with sharp vdW interfaces. They all exhibit PMA and TC close to the bulk Cr2Te3 value of 180 K. Ab initio calculations confirm this PMA and show how its strength depends on strain. Finally, Hall measurements reveal a strong anomalous Hall effect, which changes sign at a given temperature. We theoretically explain this effect by a sign change of the Berry phase close to the Fermi level. This transition temperature depends on the 2D material in proximity, notably as a consequence of charge transfer. MBE-grown Cr2Te3/2D material bilayers constitute model systems for the further development of spintronic devices combining PMA, large spin-orbit coupling and sharp vdW interface.

cond-mat.mtrl-sci

Quantum advantage in a molecular spintronic engine that harvests thermal fluctuation energy

Recent theory and experiments have showcased how to harness quantum mechanics to assemble heat/information engines with efficiencies that surpass the classical Carnot limit. So far, this has required atomic engines that are driven by cumbersome external electromagnetic sources. Here, using molecular spintronics, we propose an implementation that is both electronic and autonomous. Our spintronic quantum engine heuristically deploys several known quantum assets by having a chain of spin qubits formed by the paramagnetic Co centers of phthalocyanine (Pc) molecules electronically interact with electron-spin selecting Fe/C60 interfaces. Density functional calculations reveal that transport fluctuations across the interface can stabilize spin coherence on the Co paramagnetic centers, which host spin flip processes. Across vertical molecular nanodevices, we measure enduring dc current generation, output power above room temperature, two quantum thermodynamical signatures of the engine's processes, and a record 89% spin polarization of current across the Fe/C60 interface. It is crucially this electron spin selection that forces, through demonic feedback and control, charge current to flow against the built-in potential barrier. Further research into spintronic quantum engines, insight into the quantum information processes within spintronic technologies, and retooling the spintronic-based information technology chain, could help accelerate the transition to clean energy.

cond-mat.mes-hall

Strain engineering of the magnetic anisotropy and magnetic moment in NdFeO3 epitaxial thin films

Strain engineering is a powerful mean for tuning the various functionalities of ABO3 perovskite oxide thin films. Rare-earth orthoferrite RFeO3 materials such as NdFeO3 (NFO) are of prime interest because of their intriguing magnetic properties as well as their technological potential applications especially as thin films. Here, using a large set of complementary and advanced techniques, we show that NFO epitaxial thin films, successfully grown by pulsed laser deposition on (001)-SrTiO3, show a strong magnetic anisotropy below a critical thickness tc of 54 nm, associated with the occurrence of structural modifications related to symmetry and domain pattern changes. By varying the tensile misfit strain through the decrease of film thickness below tc, the amplitudes of in and out-of-plane magnetization can be continuously tuned while their ratio stays constant. Furthermore, different low-temperature magnetic behaviors are evidenced for strained and relaxed films, suggesting that the strain-induced structural state impacts the magnetic phase stability.

cond-mat.mtrl-sci

Large-scale epitaxy of two-dimensional van der Waals room-temperature ferromagnet Fe5GeTe2

In recent years, two-dimensional van der Waals materials have emerged as an important platform for the observation of long-range ferromagnetic order in atomically thin layers. Although heterostructures of such materials can be conceived to harness and couple a wide range of magneto-optical and magneto-electrical properties, technologically relevant applications require Curie temperatures at or above room-temperature and the ability to grow films over large areas. Here we demonstrate the large-area growth of single-crystal ultrathin films of stoichiometric Fe5GeTe2 on an insulating substrate using molecular beam epitaxy. Magnetic measurements show the persistence of soft ferromagnetism up to room temperature, with a Curie temperature of 293 K, and a weak out-of-plane magnetocrystalline anisotropy. Surface, chemical, and structural characterizations confirm the layer-by-layer growth, 5:1:2 Fe:Ge:Te stoichiometric elementary composition, and single crystalline character of the films.

cond-mat.mtrl-sci

Possible multi-orbital ground state in CeCu$_2$Si$_2$

The crystal-field ground state wave function of CeCu$_2$Si$_2$ has been investigated with linear polarized $M$-edge x-ray absorption spectroscopy from 250mK to 250K, thus covering the superconducting ($T_{\text{c}}$=0.6K), the Kondo ($T_{\text{K}}$$\approx$20K) as well as the Curie-Weiss regime. The comparison with full-multiplet calculations shows that the temperature dependence of the experimental linear dichroism is well explained with a $Γ_7^{(1)}$ crystal-field ground-state and the thermal population of excited states at around 30meV. The crystal-field scheme does not change throughout the entire temperature range thus making the scenario of orbital switching unlikely. Spectroscopic evidence for the presence of the Ce 4$f^0$ configuration in the ground state is consistent with the possibility for a multi-orbital character of the ground state. We estimate from the Kondo temperature and crystal-field splitting energies that several percents of the higher lying $Γ_6$ state and $Γ_7^{(2)}$ crystal-field states are mixed into the primarily $Γ_7^{(1)}$ ground state. This estimate is also supported by re-normalized band-structure calculations that uses the experimentally determined crystal-field scheme.

cond-mat.str-el

Linking electronic transport through a spin crossover thin film to the molecular spin state using X-ray absorption spectroscopy operando techniques

One promising route toward encoding information is to utilize the two stable electronic states of a spin crossover molecule. However, while this property is clearly manifested in transport across single molecule junctions, evidence linking charge transport across a solid-state device to the molecular film's spin state has thus far remained indirect. To establish this link, we deploy materials-centric and device-centric operando experiments involving X-ray absorption spectroscopy. We find a correlation between the temperature dependencies of the junction resistance and the Fe spin state within the device's Fe(bpz)2(phen) molecular film. We also factually observe that the Fe molecular site mediates charge transport. Our dual operando studies reveal that transport involves a subset of molecules within an electronically heterogeneous spin crossover film. Our work confers an insight that substantially improves the state-of-the-art regarding spin crossover-based devices, thanks to a methodology that can benefit device studies of other next-generation molecular compounds.

physics.app-ph

Nanoscale distribution of magnetic anisotropies in bimagnetic soft core-hard shell MnFe$_2$O$_4$@CoFe$_2$O$_4$ nanoparticles

The nanoscale distribution of magnetic anisotropies was measured in core@shell MnFe$_2$O$_4$@CoFe$_2$O$_4$ 7.0 nm particles using a combination of element selective magnetic spectroscopies with different probing depths. As this picture is not accessible by any other technique, emergent magnetic properties were revealed. The coercive field is not constant in a whole nanospinel. The very thin (0.5 nm) CoFe$_2$O$_4$ hard shell imposes a strong magnetic anisotropy to the otherwise very soft MnFe$_2$O$_4$ core: a large gradient in coercivity was measured inside the MnFe$_2$O$_4$ core with lower values close to the interface region, while the inner core presents a substantial coercive field (0.54 T) and a very high remnant magnetization (90% of the magnetization at saturation).

cond-mat.mtrl-sci

Europium Underneath Graphene on Ir(111): Intercalation Mechanism, Magnetism, and Band Structure

The intercalation of Eu underneath Gr on Ir(111) is comprehensively investigated by microscopic, magnetic, and spectroscopic measurements, as well as by density functional theory. Depending on the coverage, the intercalated Eu atoms form either a $(2 \times 2)$ or a $(\sqrt{3} \times \sqrt{3})$R$30^{\circ}$ superstructure with respect to Gr. We investigate the mechanisms of Eu penetration through a nominally closed Gr sheet and measure the electronic structures and magnetic properties of the two intercalation systems. Their electronic structures are rather similar. Compared to Gr on Ir(111), the Gr bands in both systems are essentially rigidly shifted to larger binding energies resulting in n-doping. The hybridization of the Ir surface state $S_1$ with Gr states is lifted, and the moire superperiodic potential is strongly reduced. In contrast, the magnetic behavior of the two intercalation systems differs substantially as found by X-ray magnetic circular dichroism. The $(2 \times 2)$ Eu structure displays plain paramagnetic behavior, whereas for the $(\sqrt{3} \times \sqrt{3})$R$30^{\circ}$ structure the large zero-field susceptibility indicates ferromagnetic coupling, despite the absence of hysteresis at 10 K. For the latter structure, a considerable easy-plane magnetic anisotropy is observed and interpreted as shape anisotropy.

cond-mat.mes-hall

Magnetism of cobalt nanoclusters on graphene on iridium

The structure and magnetic properties of Co clusters, comprising from 26 to 2700 atoms, self-organized or not on the graphene/Ir(111) moiré, were studied in situ with the help of scanning tunneling microscopy and X-ray magnetic circular dichroism. Surprisingly the small clusters have almost no magnetic anisotropy. We find indication for a magnetic coupling between the clusters. Experiments have to be performed carefully so as to avoid cluster damage by the soft X-rays.

cond-mat.mtrl-sci

Origin and tailoring of the antiferromagnetic domain structure in $α$-Fe$_2$O$_3$ thin films unraveled by statistical analysis of dichroic spectro-microscopy (X-PEEM) images

The magnetic microstructure and domain wall distribution of antiferromagnetic $α$-Fe$_2$O$_3$ epitaxial layers is determined by statistical image analyses. Using dichroic spectro-microscopy images, we demonstrate that the domain structure is statistically invariant with thickness and that the antiferromagnetic domain structure of the thin films is inherited from the ferrimagnetic precursor layer one, even after complete transformation into antiferromagnetic $α$-Fe$_2$O$_3$. We show that modifying the magnetic domain structure of the precursor layer is a genuine way to tune the magnetic domain structure and domain walls of the antiferromagnetic layers.

cond-mat.mtrl-sci