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Roberto Sant

Publications and source records attributed to Roberto Sant.

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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

Unveiling the Interplay of Charge and Magnetic Excitations in HgBa$_2$Ca$_2$Cu$_3$O$_{8+\delta}$

Unraveling the mechanism that binds electrons into Cooper pairs in cuprate high-temperature superconductors remains one of the most fundamental challenges in condensed-matter physics. While both magnetic interactions and lattice vibrations are known to govern key electronic properties, their possible cooperation has never been directly observed. We investigate HgBa$_2$Ca$_2$Cu$_3$O$_{8+\delta}$ (Hg1223) - the cuprate with the highest $T_{\mathrm{c}}$ at ambient pressure - as a magnifying glass to probe the possible entwining of the excitations at the core of the pairing. Using resonant inelastic X-ray scattering, we find that the charge response is dominated by dynamic charge density fluctuations (CDF) extending up to several hundred meV, where magnetic excitations reside. At the same momentum where CDF are most intense, the paramagnon energy exhibits a pronounced softening, revealing a strong interplay among charge, lattice, and spin excitations. Our results point to a cooperative mechanism in which dynamic charge fluctuations mediate the coupling between lattice, charge and spin degrees of freedom-shedding new light on the fundamental origin of high-$T_{\mathrm{c}}$ superconductivity.

cond-mat.supr-con

Ligand Mediated Magnetic Coupling Across Metamagnetic Transitions in CrPS4

Chromium thiophosphate (CrPS4) is a long-known material: a layered semiconducting antiferromagnet. Its recently discovered gate-tunable metamagnetic phase transitions, the remarkable positive and oscillating magnetoresistance as a tunnel barrier, and its Fano-resonance luminescence, elusive among the multitude of Cr3+ compounds, call for revisiting the understanding of its electronic structure, especially regarding how it relates to magnetic order. Here, we employ X-ray magnetic circular dichroism, implemented in both absorption and resonant inelastic X-ray spectroscopies, together with quantum many-body calculations, to unveil the role of metal-ligand covalency in mediating the metamagnetic transitions in CrPS4, using crystal-field and charge-transfer excitations as fingerprints of the evolving magnetic order. We reveal the role of extended superexchange paths involving P and S atoms, coupling interactions between the Cr spins across the different magnetic phases: antiferromagnetic, canted, and ferromagnetic. Our results elucidate the electronic states involved in these phases and provide prescriptions for engineering the metamagnetic phase diagram of CrPS4.

cond-mat.mtrl-sci

Magnetic behavior and phase diagram of epitaxial Er3Fe5O12 thin films across the compensation temperature

Rare-earth iron garnet (RE3Fe5O12) films are promising insulating ferrimagnets. They can show low magnetic damping, perpendicular magnetic anisotropy, and ultrafast spin dynamics, which makes them ideal for spin transport applications. In this work, we investigate the interaction between the magnetic sublattices in Er3Fe5O12 thin films grown by pulsed laser deposition on a Gd3Ga5O12 substrate. Structural and magnetic characterization reveals high-quality single-crystal growth, with compensation temperature close to the reported bulk value (~80 K). Magnetic phase diagrams based on element-specific measurements map out the regions where ferrimagnetic, canted, and aligned phases are stable across the compensation temperature. The micromagnetic dynamics resulting from perpendicular magnetic pulse perturbation of an in-plane magnetized layer was investigated at room temperature and reveals complex configurations. These results are a key feature for modulating magnetization dynamics through the compensation phenomenon, which is essential for spin-based devices operating in a low-temperature regime.

cond-mat.mtrl-sci

Orbital mixing and strong Hund's coupling stabilize spin order in van der Waals ferromagnet CrI3

Recent years have seen a vast increase in research into van der Waals magnetic materials. In many of these systems, magnetism is introduced via light 3d-transition metal elements, combined with chalcogenides or halogens. Despite the high technological promise in the field of spintronics, the connection between the d-orbital configuration and the occurrence of low-dimensional magnetic order is currently unclear. Here we address the prototypical two-dimensional ferromagnet CrI3, via complementary spectroscopies and density functional theory calculations. We reveal the electronic structure and orbital character of bulk CrI3 in the paramagnetic and ferromagnetic phases, describing the couplings underpinning its energy diagram, and providing a robust experimental demonstration that the stabilization of ferromagnetism is attributable to orbital mixing between I p and Cr eg states, and to the presence of strong Hund's coupling. These findings reveal the microscopic connection between orbital and spin degrees of freedom, providing fundamental insights into the behavior of low-dimensional magnetic materials.

cond-mat.mtrl-sci

In situ growth and magnetic characterization of Cr Chloride monolayers

Monolayer Chromium Dihalides and Trihalides materials can be grown on a variety of substrates by molecular beam epitaxy regardless of the lattice mismatch thanks to the van der Waals epitaxy. In this work, we studied the magnetic nature of Cr Chloride monolayers grown on Au(111), Ni(111) and graphene-passivated Ni(111) from the evaporation in ultra-high vacuum of the same halide precursor. Structural, morphological and magnetic characterizations were conducted in situ by low energy electron diffraction (LEED), scanning tunneling microscopy (STM) and X-ray magnetic circular dichroism (XMCD). Owing to opposite chemical behaviour, Au(111) and Ni(111) promote the formation of two different valence compounds, i.e. CrCl$_3$ and CrCl$_2$, showing distinct magnetic properties at 4 K. When graphene is used to passivate the Ni(111) surface, the formation of CrCl$_3$ becomes allowed also on this substrate. The coexistence of CrCl$_3$ and CrCl$_2$, both showing few nm lateral size and super-paramagnetic properties, is demonstrated by XMCD spectra displaying two dichroic peaks at the characteristic Cr$^{3+}$ and Cr$^{2+}$ energies. Site-selective magnetization measurements performed with the photon energy tuned on the two absorption edges show reversed magnetization of some of the CrCl$_2$ islands with respect to the CrCl3 domains, which is interpreted in terms of magnetic frustration.

cond-mat.mtrl-sci

Composite antiferromagnetic and orbital order with altermagnetic properties at a cuprate/manganite interface

Heterostructures from complex oxides allow one to combine various electronic and magnetic orders as to induce new quantum states. A prominent example is the coupling between superconducting and magnetic orders in multilayers from high-Tc cuprates and manganites. A key role is played here by the interfacial CuO2 layer whose distinct properties remain to be fully understood. Here, we study with resonant inelastic X-ray scattering (RIXS) the magnon excitations of this interfacial CuO2 layer. In particular, we show that the underlying antiferromagnetic exchange interaction at the interface is strongly suppressed to J ~ 70 meV, as compared to J ~ 130 meV for the CuO2 layers away from the interface. Moreover, we observe an anomalous momentum dependence of the intensity of the interfacial magnon mode and show that it suggests that the antiferromagnetic order is accompanied by a particular kind of orbital order that yields a so-called altermagnetic state. Such a two-dimensional altermagnet has recently been predicted to enable new spintronic applications and superconducting proximity effects.

cond-mat.str-el

A ferromagnetic Eu-Pt surface compound grown below hexagonal boron nitride

One of the fundamental applications for monolayer-thick 2D materials is their use as protective layers of metal surfaces and in-situ intercalated reactive materials in ambient conditions. Here we investigate the structural, electronic, and magnetic properties, as well as the chemical stability in air of a very reactive metal, Europium, after intercalation between a hexagonal boron nitride (hBN) layer and a Pt substrate. We demonstrate that Eu intercalation leads to a hBN-covered ferromagnetic EuPt$_2$ surface alloy with divalent Eu$^{2+}$ atoms at the interface. We expose the system to ambient conditions and find a partial conservation of the di-valent signal and hence the Eu-Pt interface. The use of a curved Pt substrate allows us to explore the changes in the Eu valence state and the ambient pressure protection at different substrate planes. The interfacial EuPt$_2$ surface alloy formation remains the same, but the resistance of the protecting hBN layer to ambient conditions is reduced, likely due to a rougher surface and a more discontinuous hBN coating.

cond-mat.mtrl-sci

Decoupling Molybdenum Disulfide from its Substrate by Cesium Intercalation

Intercalation of alkali atoms within the lamellar transition metal dichalcogenides is a possible route toward a new generation of batteries. It is also a way to induce structural phase transitions authorizing the realization of optical and electrical switches in this class of materials. The process of intercalation has been mostly studied in three-dimensional dichalcogenide films. Here, we address the case of a single-layer of molybdenum disulfide (MoS$_2$), deposited on a gold substrate, and intercalated with cesium (Cs) in ultra-clean conditions (ultrahigh vacuum). We show that intercalation decouples MoS$_2$ from its substrate. We reveal electron transfer from Cs to MoS$_2$, relative changes in the energy of the valence band maxima, and electronic disorder induced by structural disorder in the intercalated Cs layer. Besides, we find an abnormal lattice expansion of MoS$_2$, which we relate to immediate vicinity of Cs. Intercalation is thermally activated, and so is the reverse process of de-intercalation. Our work opens the route to a microscopic understanding of a process of relevance in several possible future technologies, and shows a way to manipulate the properties of two-dimensional dichalcogenides by "under-cover" functionalization.

cond-mat.mtrl-sci