arXiv subjects

Nicolas Rougemaille

Publications and source records attributed to Nicolas Rougemaille.

At least 19 recordsLinked to original sources

arXiv2026

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↗

arXiv2025

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↗

arXiv2025

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↗

arXiv2024

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↗

arXiv2024

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↗

arXiv2023

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↗

arXiv2023

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↗

arXiv2023

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↗

arXiv2022

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↗

arXiv2021

Tunable stochasticity in an artificial spin network

Metamaterials present the possibility of artificially generating advanced functionalities through engineering of their internal structure. Artificial spin networks, in which a large number of nanoscale magnetic elements are coupled together, are promising metamaterial candidates that enable the control of collective magnetic behavior through tuning of the local interaction between elements. In this work, the motion of magnetic domain-walls in an artificial spin network leads to a tunable stochastic response of the metamaterial, which can be tailored through an external magnetic field and local lattice modifications. This type of tunable stochastic network produces a controllable random response exploiting intrinsic stochasticity within magnetic domain-wall motion at the nanoscale. An iconic demonstration used to illustrate the control of randomness is the Galton board. In this system, multiple balls fall into an array of pegs to generate a bell-shaped curve that can be modified via the array spacing or the tilt of the board. A nanoscale recreation of this experiment using an artificial spin network is employed to demonstrate tunable stochasticity. This type of tunable stochastic network opens new paths towards post-Von Neumann computing architectures such as Bayesian sensing or random neural networks, in which stochasticity is harnessed to efficiently perform complex computational tasks.

cond-mat.mes-hall↗

arXiv2020

In-plane magnetic domains and Néel-like domain walls in thin flakes of the room temperature CrTe$_2$ van der Waals ferromagnet

The recent discovery of magnetic van der Waals materials has triggered a wealth of investigations in materials science, and now offers genuinely new prospects for both fundamental and applied research. Although the catalogue of van der Waals ferromagnets is rapidly expanding, most of them have a Curie temperature below 300 K, a notable disadvantage for potential applications. Combining element-selective x-ray magnetic imaging and magnetic force microscopy, we resolve at room temperature the magnetic domains and domains walls in micron-sized flakes of the CrTe$_2$ van der Waals ferromagnet. Flux-closure magnetic patterns suggesting in-plane six-fold symmetry are observed. Upon annealing the material above its Curie point (315 K), the magnetic domains disappear. By cooling back down the sample, a different magnetic domain distribution is obtained, indicating material stability and lack of magnetic memory upon thermal cycling. The domain walls presumably have Néel texture, are preferentially oriented along directions separated by 120 degrees, and have a width of several tens of nanometers. Besides microscopic mapping of magnetic domains and domain walls, the coercivity of the material is found to be of a few mT only, showing that the CrTe$_2$ compound is magnetically soft. The coercivity is found to increase as the volume of the material decreases.

cond-mat.mtrl-sci↗

arXiv2019

Room temperature 2D ferromagnetism in few-layered 1$T$-CrTe$_{2}$

Spin-related electronics using two dimensional (2D) van der Waals (vdW) materials as a platform are believed to hold great promise for revolutionizing the next generation spintronics. Although many emerging new phenomena have been unravelled in 2D electronic systems with spin long-range orderings, the scarcely reported room temperature magnetic vdW material has thus far hindered the related applications. Here, we show that intrinsic ferromagnetically aligned spin polarization can hold up to 316 K in a metallic phase of 1$T$-CrTe$_{2}$ in the few-layer limit. This room temperature 2D long range spin interaction may be beneficial from an itinerant enhancement. Spin transport measurements indicate an in-plane room temperature negative anisotropic magnetoresistance (AMR) in few-layered CrTe$_{2}$, but a sign change in the AMR at lower temperature, with -0.6$\%$ at 300 K and +5$\%$ at 10 K, respectively. This behavior may originate from the specific spin polarized band structure of CrTe$_{2}$. Our findings provide insights into magnetism in few-layered CrTe$_{2}$, suggesting potential for future room temperature spintronic applications of such 2D vdW magnets.

cond-mat.mes-hall↗

arXiv2019

Confined step-flow growth of Cu intercalated between graphene and a Ru(0001) surface

By comparing the growth of Cu thin films on bare and graphene-covered Ru(0001) surfaces, we demonstrate the role of graphene as a surfactant allowing the formation of flat Cu films. Low-energy electron microscopy, X-ray photoemission electron microscopy and X-ray absorption spectroscopy reveal that depositing Cu at 580 K leads to distinct behaviors on both types of surfaces. On bare Ru, a Stranski-Krastanov growth is observed, with first the formation of an atomically flat and monolayer-thick wetting layer, followed by the nucleation of three-dimensional islands. In sharp contrast, when Cu is deposited on a graphene-covered Ru surface under the very same conditions, Cu intercalates below graphene and grows in a step-flow manner: atomically-high growth fronts of intercalated Cu form at the graphene edges, and extend towards the center of the flakes. Our findings suggest potential routes in metal heteroepitaxy for the control of thin film morphology.

cond-mat.mtrl-sci↗

arXiv2019

Proposal to recover an extensive ground state degeneracy in a two-dimensional square array of nanomagnets

We investigate numerically the micromagnetic properties and the low-energy physics of an artificial square spin system in which the nanomagnets are physically connected at the lattice vertices. Micromagnetic simulations reveal that the energy stored at the vertex sites strongly depends on the type of magnetic domain wall formed by the four connected nanomagnets. As a consequence, the energy gap between the vertex types can be partially modified by varying the geometrical parameters of the nanomagnets, such as their width and thickness. Based on the energy levels given by the micromagnetic simulations, we compute the thermodynamic properties of the corresponding spin models using Monte Carlo simulations. We found two regimes, both being characterized by an extensive ground state manifold, in sharp contrast with similar lattices with disconnected nanomagnets. For narrow and thin nanomagnets, low-energy spin configurations consist of independent ferromagnetic straight lines crossing the whole lattice. The ground state manifold is thus highly degenerate, although this degeneracy is subdominant. In the limit of thick and wide nanomagnets, our findings suggest that the celebrated square ice model may be fabricated experimentally from a simple square lattice of connected elements. These results show that the micromagnetic nature of artificial spin systems involves another degree of freedom that can be finely tuned to explore strongly correlated disordered magnetic states of matter.

cond-mat.mes-hall↗

arXiv2018

Graphene as a Mechanically Active, Deformable Two-Dimensional Surfactant

In crystal growth, surfactants are additive molecules used in dilute amount or as dense, permeable layers to control surface morphologies. Here, we investigate the properties of a strikingly different surfactant: a two-dimensional and covalent layer with close atomic packing, graphene. Using in situ, real time electron microscopy, scanning tunneling microscopy, kinetic Monte Carlo simulations, and continuum mechanics calculations, we reveal why metallic atomic layers can grow in a two-dimensional manner below an impermeable graphene membrane. Upon metal growth, graphene dynamically opens nanochannels called wrinkles, facilitating mass transport, while at the same time storing and releasing elastic energy via lattice distortions. Graphene thus behaves as a mechanically active, deformable surfactant. The wrinkle-driven mass transport of the metallic layer intercalated between graphene and the substrate is observed for two graphene-based systems, characterized by different physico-chemical interactions, between graphene and the substrate, and between the intercalated material and graphene. The deformable surfactant character of graphene that we unveil should then apply to a broad variety of species, opening new avenues for using graphene as a two-dimensional surfactant forcing the growth of flat films, nanostructures and unconventional crystalline phases.

cond-mat.mtrl-sci↗

arXiv2018

Micromagnetics of anti-skyrmions in ultrathin films

We present a combined analytical and numerical micromagnetic study of the equilibrium energy, size and shape of anti-skyrmionic magnetic configurations. Anti-skyrmions can be stabilized when the Dzyaloshinskii-Moriya interaction has opposite signs along two orthogonal in-plane directions, breaking the magnetic circular symmetry. We compare the equilibrium energy, size and shape of anti-skyrmions and skyrmions that are stabilized respectively in environments with anisotropic and isotropic Dzyaloshinskii-Moriya interaction, but with the same strength of the magnetic interactions.When the dipolar interactions are neglected the skyrmion and the anti-skyrmion have the same energy, shape and size in their respective environment. However, when dipolar interactions are considered, the energy of the anti-skyrmion is strongly reduced and its equilibrium size increased with respect to the skyrmion. While the skyrmion configuration shows homochiral Néel magnetization rotations, anti-skyrmions show partly Néel and partly Bloch rotations. The latter do not produce magnetic charges and thus cost less dipolar energy. Both magnetic configurations are stable when the magnetic energies almost cancel each other, which means that a small variation of one parameter can drastically change their configuration, size and energy.

cond-mat.mtrl-sci↗

arXiv2018

The skyrmion-bubble transition in a ferromagnetic thin film

Magnetic skyrmions and bubbles, observed in ferromagnetic thin films with perpendicular magnetic anisotropy, are topological solitons which differ by their characteristic size and the balance in the energies at the origin of their stabilisation. However, these two spin textures have the same topology and a continuous transformation between them is allowed. In the present work, we derive an analytical model to explore the skyrmion-bubble transition. We evidence a region in the parameter space where both topological soliton solutions coexist and close to which transformations between skyrmion and bubbles are observed as a function of the magnetic field. Above a critical point, at which the energy barrier separating both solutions vanishes, only one topological soliton solution remains, which size can be continuously tuned from micrometer to nanometer with applied magnetic field.

cond-mat.mtrl-sci↗

arXiv2017

Intercalating cobalt between graphene and iridium (111): a spatially-dependent kinetics from the edges

Using low-energy electron microscopy, we image in real time the intercalation of a cobalt monolayer between graphene and the (111) surface of iridium. Our measurements reveal that the edges of a graphene flake represent an energy barrier to intercalation. Based on a simple description of the growth kinetics, we estimate this energy barrier and find small, but substantial, local variations. These local variations suggest a possible influence of the graphene orientation with respect to its substrate and of the graphene edge termination on the energy value of the barrier height. Besides, our measurements show that intercalated cobalt is energetically more favorable than cobalt on bare iridium, indicating a surfactant role of graphene.

cond-mat.mtrl-sci↗