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Johann Coraux

Publications and source records attributed to Johann Coraux.

At least 19 recordsLinked to original sources

Probing magnetic correlations in space and time within predefined topological sectors of a macroscopic spin liquid

The triangular Ising antiferromagnet, with its residual entropy density and critical correlations at absolute zero, is the archetype of a two-dimensional spin liquid. Its ground state is partitioned into topological sectors connected by global spin flip events that wrap the lattice boundaries, and become statistically irrelevant in the thermodynamic limit where magnetic fluctuations are restricted to the dominant sector. Thus far, these properties have been mainly investigated from a theoretical perspective, and one might wonder to what extent they can be transposed to real materials. Here, we present experimental observations obtained in an artificial, macroscopic realisation of the seminal triangular Ising antiferromagnet that consists of a lattice of millimeter-sized NdFeB cylinders put into motion by a mechanical shaker. Specifically, we demonstrate that the very-low-energy physics and the true ground state of this model can be reached experimentally. Besides, we are able to probe, in space and time, the magnetic properties within manually preselected pockets of the ground-state manifold that emulate, to a good approximation, the behaviour in distinct topological sectors. Our approach opens new avenues for naked-eye visualisation and hand manipulation of many-body phenomena associated to frustrated magnetism and models of statistical physics.

cond-mat.stat-mech

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

Surface reconstruction-driven band folding and spin-orbit enhancement at the $α$-antimonene/Au(111) interface

The electronic properties of the two-dimensional (2D) $α$ phase of antimonene are unique, featuring unpinned Dirac cones that can be moved with strain. Here we investigate the structural and electronic properties of an epitaxial 2D $α$-antimonene, grown on Au(111). Using angle-resolved photoemission spectroscopy and density-functional theory, we reveal a strong hybridization at the Sb/Au interface, which imprints a rectangular reconstruction in the Au states, producing a band folding and hybrid bands exhibiting trigonal pockets. Additionally, hybridization displaces part of the Au wavefunction in regions of large electrostatic potential gradient, thereby enhancing spin-orbit splitting. Our work underscores that the pristine electronic properties of $α$-antimonene may be deeply modified by its substrate, and even overwhelmed by the bands of the latter, and also shows that spin-orbit interaction in a heavy metal (Au) can be substantially enhanced by a lighter element (Sb).

cond-mat.mtrl-sci

Colloquium: A critique on van der Waals and two-dimensional magnets

Magnetic two-dimensional (2D) crystals were isolated about a decade ago, triggering a tremendous research activity worldwide. This colloquium raises a stiff question: what is really new about them? At first sight, they seem to be purer implementations of 2D spin models than traditional systems such as ultra-thin films. Yet, they partly realized their promises so far, and whether they give fresh perspectives on long-standing predictions in statistical physics is still an open question. Undoubtedly, they are uniquely amenable to electric-field effect, susceptible to mechanical deformation, and sensitive to moirés, for example. They represent interesting platforms for exploring, challenging, or simply revisiting a wide range of phenomena in condensed matter magnetism. This colloquium intends to offer a critical, yet not necessarily skeptical, overview of the field, clarifying what we believe could be unique with 2D magnets, related quasi-2D van der Waals magnets, and their heterostructures.

cond-mat.mtrl-sci

Gate-tunable spectrum and charge dispersion mitigation in a graphene superconducting qubit

Controlling the energy spectrum of quantum-coherent superconducting circuits, i.e. the energies of excited states, the circuit anharmonicity and the states' charge dispersion, is essential for designing performant qubits. This control is usually achieved by adjusting the circuit's geometry. In-situ control is traditionally obtained via an external magnetic field, in the case of tunnel Josephson junctions. More recently, semiconductor-weak-links-based Josephson junctions have emerged as an alternative building block with the advantage of tunability via the electric-field effect. Gate-tunable Josephson junctions have been succesfully integrated in superconducting circuits using for instance semiconducting nanowires or two-dimensional electron gases. In this work we demonstrate, in a graphene superconducting circuit, a large gate-tunability of qubit properties: frequency, anharmonicity and charge dispersion. We rationalize these features using a model considering the transmission of Cooper pairs through Andreev bound states. Noticeably, we show that the high transmission of Cooper pairs in such weak link strongly suppresses the charge dispersion. Our work illustrates the potential for graphene-based qubits as versatile building-blocks in advanced quantum circuits.

cond-mat.mes-hall

Laser patterning of the room temperature van der Waals ferromagnet 1$T$-CrTe$_2$

Lamellar crystalline materials, whose layers are bond by van der Waals forces, can be stacked to form ultrathin artificial heterostructures, and in particular vertical magnetic junctions when some of the stacked materials are (ferro)magnetic. Here, using the room temperature van der Waals ferromagnet 1$T$-CrTe$_2$, we report a method for patterning lateral magnetic junctions. Exploiting the heat-induced phase transformation of the material into Cr$_x$Te$_y$ compounds ($x/y>1/2$), we use local laser heating to imprint patterns at the micron-scale. Optimizing laser heat dissipation, we further demonstrate the crucial role of the substrate to control the phase transformation. If plain, unstructured poorly heat-conducting substrates allow for direct writing of magnetic patterns, structured $h$-BN layers can serve as heat stencils to draw potentially thinner patterns. Besides, $h$-BN encapsulation turns out to be heat-protective (in addition from protecting against oxidation as it is generally used for), allowing the demonstration of room temperature ferromagnetism in $<$7~nm-thick 1$T$-CrTe$_2$.

cond-mat.mtrl-sci

Three-dimensional deformations in single-layer $α$ antimonene and interaction with a Au(111) surface from first principles

Using density functional theory, we investigate the electronic structure of the alpha phase of an antimony monolayer in its isolated form and in contact to the (111) surface of gold. We demonstrate that the isolated single-layer actually displays a slightly modulated puckering that stabilizes the monolayer, not a uniform one as often assumed. Moreover, it has dramatic consequences on the electronic band structure: the material is a semiconductor with low-dispersing bands near the Brillouin zone center. By further application of about 12% strain on the armchair direction, a double-cone features develops wherein an electronic bandgap of about 21~meV is found. When in contact with a Au(111) surface, a strong interaction with gold arises, as it appears clearly from (i) substantial atomic displacements compared to the isolated form, and (ii) hybridization of Sb and Au orbitals. The latter profoundly modifies the electronic band structure by strengthening the spin-orbit splitting of hybridized bands and spoiling the double-cone feature whose manipulation through substrate-induced strain appears therefore questionable, at least in the simulated epitaxial implementation.

cond-mat.mtrl-sci

Square ice Coulomb phase as a percolated vertex lattice

The square ice is a canonical example of a Coulomb phase in two dimensions: Its ground state is extensively degenerate and satisfies a local constraint on the spin arrangement (the so-called ice rule). In this paper, we use a loop flip algorithm to explore the properties of this ground state that we analyze not in terms of a spin texture, but rather in terms of a spatial distribution of ice-rule satisfying vertices. More specifically, we determine for various lattice sizes the average vertex populations characterizing the ice manifold, the pairwise vertex correlations, and the size distribution of vertex clusters. Comparing these results to those obtained from random, constraint-free vertex tilings, the square ice manifold is found to resemble an almost ideal vertex gas, and the cluster size distribution of ice-rule satisfying vertices is well approximated by percolation theory. Remarkably, this description remains reasonably accurate when monopoles are present in a dilute amount, allowing a direct comparison with experiments. Revising former experimental results on two artificial square ice systems, we illustrate the interest of our approach to spot the presence of a Coulomb phase from a vertex analysis.

cond-mat.str-el

Unusual Coulomb phase physics in the arctic square ice

The square ice is a two-dimensional spin liquid hosting a Coulomb phase physics. When constrained under specific boundary conditions, the so-called domain-wall boundary conditions, a phase separation occurs that leads to the formation of a spin liquid confined within a disk surrounded by magnetically ordered regions. Here, we numerically characterize the ground-state properties of this spin liquid, coined the arctic square ice in reference to a phenomenon known in statistical mechanics. Our results reveal that both the vertex distributions and the magnetic correlations are inhomogeneous within the liquid region, and they exhibit a radial dependence. If these properties resemble those of the conventional square ice close to the center of the disk, they evolve continuously as the disk perimeter is approached. There, the spin liquid orders. As a result, pinch points, signaling the presence of algebraic spin correlations, coexist with magnetic Bragg peaks in the magnetic structure factor computed within the disk. The arctic square ice thus appears as an unconventional Coulomb phase sharing common features with a fragmented spin liquid, albeit on a charge-neutral vacuum.

cond-mat.str-el

Direct measurement of a $\sin(2φ)$ current phase relation in a graphene superconducting quantum interference device

In a Josephson junction, the current phase relation relates the phase variation of the superconducting order parameter, $φ$, between the two superconducting leads connected through a weak link, to the dissipationless current . This relation is the fingerprint of the junction. It is usually dominated by a $\sin(φ)$ harmonic, however its precise knowledge is necessary to design superconducting quantum circuits with tailored properties. Here, we directly measure the current phase relation of a superconducting quantum interference device made with gate-tunable graphene Josephson junctions and we show that it can behave as a $\sin(2φ)$ Josephson element, free of the traditionally dominant $\sin(φ)$ harmonic. Such element will be instrumental for the development of superconducting quantum bits protected from decoherence.

cond-mat.mes-hall

Epitaxial two-dimensional membranes under intrinsic and extrinsic strains

Two-dimensional (2D) materials naturally form moiré patterns with other crystalline layers, such as other 2D material or the surface of a substrate. These patterns add a nanoscale characteristic length in the form of a superlattice: the moiré wavelength. Understanding the origin and characteristics of these patterns is crucial to design/interpret moiré-induced physical properties. Here, we use a mixed continuum mechanics + atomistic modeling to study two experimentally relevant epitaxial 2D materials -- graphene on Ir(111) and MoS$_2$ on Au(111) -- under extrinsic and intrinsic strain. We consider three different scenarios affecting substantially the lattice constant of the 2D materials, the wavelength and corrugation of the moiré pattern. (i) Under the influence of the interaction with the substrate, bending energy produces non trivial variations of the moiré properties, even when the strain is small; (ii) When locked on a progressively strained substrate via the valleys of the moiré, the membranes' nanorippling amplitude goes through several jumps related to relatively smaller jumps in the interatomic distance of the 2D materials; (iii) Finally, increasing the zero-deformation value of this interatomic distance (possibly controlable with temperature or illumination in experiments) the moiré wavelength can either increase or decrease.

cond-mat.mes-hall

Stability of the In-Plane Room Temperature van der Waals Ferromagnet Chromium Ditelluride and Its Conversion to Chromium-Interleaved CrTe$_2$ Compounds

Van der Waals magnetic materials are building blocks for novel kinds of spintronic devices and playgrounds for exploring collective magnetic phenomena down to the two-dimensional limit. Chromium-tellurium compounds are relevant in this perspective. In particular, the 1$T$ phase of CrTe$_2$ has been argued to have a Curie temperature above 300~K, a rare and desirable property in the class of lamellar materials, making it a candidate for practical applications. However, recent literature reveals a strong variability in the reported properties, including magnetic ones. Using electron microscopy, diffraction and spectroscopy techniques, together with local and macroscopic magnetometry approaches, our work sheds new light on the structural, chemical and magnetic properties of bulk 1$T$-CrTe$_2$ exfoliated in the form of flakes having a thickness ranging from few to several tens of nanometers. We unambiguously establish that 1$T$-CrTe$_2$ flakes are ferromagnetic above room temperature, have an in-plane easy axis of magnetization, low coercivity, and we confirm that their Raman spectroscopy signatures are two modes, $E_{2\text{g}}$ (103.5~cm$^{-1}$) and $A_{1\text{g}}$ (136.5~cm$^{-1}$). We also prove that thermal annealing causes a phase transformation to monoclinic Cr$_5$Te$_8$ and, to a lesser extent, to trigonal Cr$_5$Te$_8$. In sharp contrast with 1$T$-CrTe$_2$, none of these compounds have a Curie temperature above room temperature, and they both have perpendicular magnetic anisotropy. Our findings reconcile the apparently conflicting reports in the literature and open opportunities for phase-engineered magnetic properties.

cond-mat.mtrl-sci

Positional and Rotational Molecular Degrees of Freedom in a Metal-Organic Surface Alloy: the Copper-Fullerene System and its Multiple Structural Phases

Mixing two chemical elements at the surface of a substrate is known to produce rich phase diagrams of surface alloys. Here, we extend the concept of surface alloying to the case where the two constituent elements are not both atoms, but rather one atom (copper) and one molecule (fullerene). When deposited at room temperature on a Cu(111) surface, fullerenes intermix with the metal substrate. Surprisingly, 10 distinct copper-fullerene surface alloys are found to coexist. The structure of these alloys, i.e. their composition and commensurability relationship with the substrate, is resolved using scanning tunneling microscopy and density functional theory calculations. This diversity in the alloying process is associated to the multiple possibilities a fullerene can bind to the Cu surface. The molecules are indeed found to have in-plane and out-of-plane positional degree of freedom: the molecular alloys have elastic in-plane properties and can buckle. In addition, the molecules can rotate on their binding sites, conferring extra degrees of freedom to the system. We introduce a competing-interaction energy model, parametrized against the results of the \textit{ab initio} calculations, that describes well all the phases we observe experimentally.

cond-mat.mtrl-sci

Elastic properties of moiré lattices in epitaxial two-dimensional materials

Unlike conventional two-dimensional (2D) semiconductor superlattices, moiré patterns in 2D materials are flexible and their electronic, magnetic, optical, and mechanical properties depend on their topography. Within a continuous+atomistic theory treating 2D materials as crystalline elastic membranes, we abandon the flat-membrane scenario usually assumed for these materials and address out-of-plane deformations. We confront our predictions to experimental analyses on model systems, epitaxial graphene, and MoS$_2$ on metals and reveal that compression/expansion and bending energies stored in the membrane can compete with adhesion energy, leading to a subtle moiré wavelength selection and the formation of wrinkles.

cond-mat.mes-hall

Two-way twisting of a confined monolayer: orientational ordering within the van der Waals gap between graphene and its crystalline substrate

Two-dimensional confinement of lattices produces a variety of order and disorder phenomena. When the confining walls have atomic granularity, unique structural phases are expected, of relevance in nanotribology, porous materials or intercalation compounds where \textit{e.g.} electronic states can emerge accordingly. The interlayer's own order is frustrated by the competing interactions exerted by the two confining surfaces. We revisit the concept of orientational ordering, introduced by Novaco and McTague to describe the twist of incommensurate monolayers on crystalline surfaces. We predict a two-way twist of the monolayer as its density increases. We discover such a behavior in alkali atom monolayers (sodium, cesium) confined between graphene and an iridium surface, using scanning tunneling microscopy and electron diffraction.

cond-mat.mes-hall

Nano-sheets of two-dimensional polymers with dinuclear (arene)ruthenium nodes, synthesised at a liquid/liquid interface

We developed a new class of mono- or few-layered two-dimensional polymers based on dinuclear (arene)ruthenium nodes, obtained by combining the imine condensation with an interfacial chemistry process, and use a modified Langmuir-Schaefer method to transfer them onto solid surfaces. Robust nano-sheets of 2D polymers including dinuclear complexes of heavy ruthenium atoms as nodes were synthesised. These nano-sheets, whose thickness is of a few tens of nanometers, were suspended onto solid porous membranes. Then, they were thoroughly characterised with a combination of local probes, including Raman scattering, Fourier transform infrared spectroscopy and transmission electron microscopy in imaging and diffraction mode.

cond-mat.mtrl-sci

Fermi resonance in the Raman spectrum of graphene

We report the observation of an intense anomalous peak at 1608 cm$^{-1}$ in the Raman spectrum of graphene associated to the presence of chromium nanoparticles in contact with graphene. Bombardment with an electron beam demonstrates that this peak is distinct from the well studied D$'$ peak appearing as defects are created in graphene; the new peak is found non dispersive. We argue that the bonding of chromium atoms with carbon atoms softens the out-of-plane optical (ZO) phonon mode, in such a way that the frequency of its overtone decreases to $2ω_{\rm ZO}\simω_{\rm G}$, where $ω_{\rm G}$=1585~cm$^{-1}$ is the frequency of the Raman-active E$_{\rm 2g}$ mode. Thus, the observed new peak is attributed to the 2ZO mode which becomes Raman-active following a mechanism known as Fermi resonance. First-principles calculations on vibrational and anharmonic properties of the graphene/Cr interface support this scenario.

cond-mat.mes-hall

Structure of graphene and a surface carbide grown on the (0001) surface of rhenium

Transition metal surfaces catalyse a broad range of thermally-activated reactions involving carbon-containing-species -- from atomic carbon to small hydrocarbons or organic molecules, and polymers. These reactions yield well-separated phases, for instance graphene and the metal surface, or, on the contrary, alloyed phases, such as metal carbides. Here, we investigate carbon phases on a rhenium (0001) surface, where the former kind of phase can transform into the latter. We find that this transformation occurs with increasing annealing time, which is hence not suitable to increase the quality of graphene. Our scanning tunneling spectroscopy and reflection high-energy electron diffraction analysis reveal that repeated short annealing cycles are best suited to increase the lateral extension of the structurally coherent graphene domains. Using the same techniques and with the support of density functional theory calculations, we next unveil, in real space, the symmetry of the many variants (two six-fold families) of a rhenium surface carbide observed with diffraction since the 1970s, and finally propose models of the atomic details. One of these models, which nicely matches the microscopy observations, consists of parallel rows of eight aligned carbon trimers with a so-called $(7\times\sqrt{\mathrm{19}})$ unit cell with respect to Re(0001).

cond-mat.mtrl-sci