arXiv subjects

Arnaud Magrez

Publications and source records attributed to Arnaud Magrez.

At least 37 records · Page 2Linked to original sources

arXiv2022

Observation of a new light-induced skyrmion phase in the Mott insulator Cu2OSeO3

We report the discovery of a novel skyrmion phase in the multiferroic insulator Cu2OSeO3 for magnetic fields below the equilibrium skyrmion pocket. This phase can be accessed by exciting the sample out of equilibrium with near-infrared (NIR) femtosecond laser pulses but can not be reached by any conventional field cooling protocol. From the strong wavelength dependence of the photocreation process and via spin dynamics simulations, we identify the magnetoelastic effect as the most likely photocreation mechanism. This effect results in a transient modification of the magnetic interaction extending the equilibrium skyrmion pocket to lower magnetic fields. Once created, the skyrmions rearrange and remain stable over a long time, reaching minutes. The presented results are relevant for designing high-efficiency non-volatile data storage based on magnetic skyrmions.

cond-mat.str-el↗

arXiv2022

Mixed Valence Pseudobrookite Al$_{1.75}$Ti$_{1.25}$O$_5$: High Temperature Phase Transitions, Magnetism and Resistivity

Dark blue single crystals of Al$_{1.75}^{3+}$ Ti$_{1.0}^{4+}$ Ti$_{0.25}^{3+}$O$_5$ were grown with a novel synthesis method based on the reaction of a Ti3+/Ti4+ containing langbeinite melt and Al$_2$O$_3$. The obtained needles crystallize in the pseudobrookite structure and undergo two reversible phase transitions from orthorhombic Cmcm to C2/m first and subsequently to C2 symmetry. Like the known aluminum titanate pseudobrookites, anistropic thermal expansion is observed. The temperature evolution of the crystal structure reveals some insights into the mechanism leading to the decomposition of the Al$_{1.75}$Ti$_{1.25}$O$_5$ above 725$^\circ$C. The magnetic and electrical properties are discussed and compared to other reported aluminum titanate pseudobrookites.

cond-mat.mtrl-sci↗

arXiv2022

Imaging the ultrafast coherent control of a skyrmion crystal

Exotic magnetic textures emerging from the subtle interplay between thermodynamic and topological fluctuation have attracted intense interest due to their potential applications in spintronic devices. Recent advances in electron microscopy have enabled the imaging of random photo-generated individual skyrmions. However, their deterministic and dynamical manipulation is hampered by the chaotic nature of such fluctuations and the intrinsically irreversible switching between different minima in the magnetic energy landscape. Here, we demonstrate a method to coherently control the rotation of a skyrmion crystal by discrete amounts at speeds which are much faster than previously observed. By employing circularly polarized femtosecond laser pulses with an energy below the bandgap of the Mott insulator Cu2OSeO3, we excite a collective magnon mode via the inverse Faraday effect. This triggers coherent magnetic oscillations that directly control the rotation of a skyrmion crystal imaged by cryo-Lorentz Transmission Electron Microscopy. The manipulation of topological order via ultrafast laser pulses shown here can be used to engineer fast spin-based logical devices.

cond-mat.str-el↗

arXiv2022

Tuning topological spin textures in size-tailored chiral magnet insulator particles

Topological spin textures such as skyrmions hold high potential for use as magnetically active elements in diverse near-future applications. While skyrmions in metallic multilayers attract great attention in this context, unleashing the myriad potential of skyrmions for various applications requires the discovery and customization of alternative host system paradigms. Here we developed and applied a chemical method to synthesize octahedral particles of the chiral insulating skyrmion host Cu2OSeO3 with both narrow size distribution, and tailored dimensions approaching the nanoscale. Combining magnetometry and neutron scattering experiments with micromagnetic simulations, we show that the bulk phase diagram of Cu2OSeO3 changes dramatically below octahedral heights of 400 nm. Further particle size-dependent regimes are identified where various topological spin textures such as skyrmions, merons and bobbers can stabilize, prior to a lower critical octahedral height of approx. 190 nm below which no topological spin texture is found stable. These findings suggest conditions under which sparse topological spin textures confined to chiral magnet nanoparticles can be stable, and provide fresh potential for insulator-based application paradigms.

cond-mat.mtrl-sci↗

arXiv2021

Magnetic field induced quantum spin liquid in the two coupled trillium lattices of K$_2$Ni$_2$(SO$_4$)$_3$

Quantum spin liquids are exotic states of matter which form when strongly frustrated magnetic interactions induce a highly entangled quantum paramagnet far below the energy scale of the magnetic interactions. Three-dimensional cases are especially challenging due to the significant reduction of the influence of quantum fluctuations. Here, we report the magnetic characterization of {\kni} forming a three dimensional network of Ni$^{2+}$ spins. Using density functional theory calculations we show that this network consists of two interconnected spin-1 trillium lattices. In the absence of a magnetic field, magnetization, specific heat, neutron scattering and muon spin relaxation experiments demonstrate a highly correlated and dynamic state, coexisting with a peculiar, very small static component exhibiting a strongly renormalized moment. A magnetic field $B \gtrsim 4$ T diminishes the ordered component and drives the system in a pure quantum spin liquid state. This shows that a system of interconnected $S=1$ trillium lattices exhibit a significantly elevated level of geometrical frustration.

cond-mat.str-el↗

arXiv2020

Ferrimagnetic 120$^\circ$ magnetic structure in Cu2OSO4

We report magnetic properties of a 3d$^9$ (Cu$^{2+}$) magnetic insulator Cu2OSO4 measured on both powder and single crystal. The magnetic atoms of this compound form layers, whose geometry can be described either as a system of chains coupled through dimers or as a Kagomé lattice where every 3rd spin is replaced by a dimer. Specific heat and DC-susceptibility show a magnetic transition at 20 K, which is also confirmed by neutron scattering. Magnetic entropy extracted from the specific heat data is consistent with a $S=1/2$ degree of freedom per Cu$^{2+}$, and so is the effective moment extracted from DC-susceptibility. The ground state has been identified by means of neutron diffraction on both powder and single crystal and corresponds to a $\sim120$ degree spin structure in which ferromagnetic intra-dimer alignment results in a net ferrimagnetic moment. No evidence is found for a change in lattice symmetry down to 2 K. Our results suggest that \sample \ represents a new type of model lattice with frustrated interactions where interplay between magnetic order, thermal and quantum fluctuations can be explored.

cond-mat.str-el↗

arXiv2020

Peculiar magnetic dynamics across the in-field transition in Ca3Co2O6

The discovery of multiple coexisting magnetic phases in a crystallographically homogeneous compound Ca$_3$Co$_2$O$_6$ has stimulated an ongoing research activity. In recent years the main focus has been on the zero field state properties, where exceedingly long time scales have been established. In this study we report a detailed investigation of static and dynamic properties of Ca$_3$Co$_2$O$_6$ across the magnetic field induced transition around 3.5 T. This region has so far been practically neglected while we argue that in some aspects it represents a simpler version of the transition across the $B = 0$ state. Investigating the frequency dependence of the ac susceptibility we reveal that on the high field side ($B > 3.5$ T) the response corresponds to a relatively narrow distribution of magnetic clusters. The distribution appears very weakly dependent on magnetic field, with an associated energy barrier of around 200 K. Below 3.5 T a second contribution arises, with much smaller characteristic frequencies and a strong temperature and magnetic field dependence. We discuss these findings in the context of intra-chain and inter-chain clustering of magnetic moments.

cond-mat.str-el↗

arXiv2019

The Dirac nodal line network in non-symmorphic rutile semimetal RuO$_2$

We employ angle resolved photoemission spectroscopy (ARPES) to investigate the Fermi surface of RuO$_2$. We find a network of two Dirac nodal lines (DNL) as previously predicted in theory, where the valence- and conduction bands touch along continuous lines in momentum space. In addition, we find evidence for a third DNL close to the Fermi level which appears robust despite the presence of significant spin orbit coupling. We demonstrate that the third DNL gives rise to a topologically trivial flat-band surface state (FBSS) at the (110) surface. This FBSS can be tuned by surface doping and presents an interesting playground for the study of surface chemistry and exotic correlation phenomena.

cond-mat.mes-hall↗

arXiv2019

Electrical transport in onion-like carbon - PMMA nanocomposites

We report electrical conductivity measurements of Polymethyl-methacrylate filled by onion-like carbon particles with primary particle size of $\approx 5$ nm. We shown that the conductivity $σ$ is exceptionally high even at very low loadings, and that its low-temperature dependence follows a Coulomb gap regime at atmospheric pressure and an activated behavior at a pressure of $2$ GPa. We interpret this finding in terms of the enhancement under the applied pressure of the effective dielectric permittivity within the aggregates of onion-like carbons, which improves the screening of the Coulomb interaction and reduces the optimal hopping distance of the electrons.

cond-mat.dis-nn↗

arXiv2018

Tuning of a skyrmion cluster in magnetoelectric Cu$_2$OSeO$_3$ by electric field

Chiral magnetic textures with non-trivial topology are known as skyrmions, and due to their unique properties they are promising in novel magnetic storage applications. While the electric manipulation of either isolated skyrmions or a whole skyrmion lattice have been intensively reported, the electric effects on skyrmion clusters remain scarce. In magnetoelectric compound Cu$_2$OSeO$_3$, a skyrmion cluster can be created near the helical-skyrmion phase boundary. Here, we report the in situ electric field writing/erasing of skyrmions in such a skyrmion cluster. Our real space/time image data obtained by Lorentz transmission electron microscopy and the quantitative analysis evidence the linear increase of the number of skyrmions in the cluster upon the application of a creating electric field. The energy needed to create a single skyrmion is estimated to be $\mathcal{E}=4.7 \times 10^{-24}$ J.

cond-mat.str-el↗

arXiv2018

Melting a skyrmion lattice topologically: through the hexatic phase to a skyrmion liquid

Skyrmions are twirling magnetic textures whose non-trivial topology leads to particle-like properties promising for information technology applications. Perhaps the most important aspect of interacting particles is their ability to form thermodynamically distinct phases from gases and liquids to crystalline solids. Dilute gases of skyrmions have been realized in artificial multilayers, and solid crystalline skyrmion lattices have been observed in bulk skyrmion hosting materials. Yet, to date melting of the skyrmion lattice into a skyrmion liquid has not been reported experimentally. Through direct imaging with cryo-Lorentz transmission electron microscopy, we demonstrate that the skyrmion lattice in the material Cu$_2$OSeO$_3$ can be dynamically melted. Remarkably, we discover this melting process to be a topological defects mediated two-step transition via a theoretically hypothesized hexatic phase to the liquid phase. The existence of hexatic and liquid phases instead of a simple fading of the local magnetic moments upon thermal excitations implies that even in bulk materials skyrmions possess considerable particle nature, which is a pre-requisite for application schemes.

cond-mat.str-el↗

arXiv2018

Spin-resolved electronic response to the phase transition in MoTe$_2$

The semimetal MoTe$_2$ is studied by spin- and angle- resolved photoemission spectroscopy to probe the detailed electronic structure underlying its broad range of response behavior. A novel spin-texture is uncovered in the bulk Fermi surface of the non-centrosymmetric structural phase that is consistent with first-principles calculations. The spin-texture is three-dimensional, both in terms of momentum dependence and spin-orientation, and is not completely suppressed above the centrosymmetry-breaking transition temperature. Two types of surface Fermi arc are found to persist well above the transition temperature. The appearance of a large Fermi arc depends strongly on thermal history, and the electron quasiparticle lifetimes are greatly enhanced in the initial cooling. The results indicate that polar instability with strong electron-lattice interactions exists near the surface when the bulk is largely in a centrosymmetric phase.

cond-mat.mtrl-sci↗

arXiv2018

Singlet state formation and its impact on magnetic structure in tetramer system SeCuO$_3$

We present an experimental investigation of the magnetic structure in a tetramer system SeCuO$_3$ using neutron diffraction and nuclear resonance techniques. We establish a non-collinear, commensurate antiferromagnetic ordering with a propagation vector $\textbf{k} = \left(0,0,1 \right)$. The order parameter follows a critical behavior near $T_N = 8$ K, with a critical exponent $β= 0.32$ in agreement with a 3D universality class. Evidence is presented that a singlet state starts to form on tetramers at temperatures as high as 200 K, and its signature is preserved within the ordered state through a strong renormalization of the ordered magnetic moment on two non-equivalent copper sites, $m_{Cu1} \approx 0.4 μ_B$ and $m_{Cu2} \approx 0.7 μ_B$ at 1.5 K.

cond-mat.str-el↗

arXiv2017

In situ Electric Field Skyrmion Creation in Magnetoelectric Cu$_2$OSeO$_3$

Magnetic skyrmions are localized nanometric spin textures with quantized winding numbers as the topological invariant. Rapidly increasing attention has been paid to the investigations of skyrmions since their experimental discovery in 2009, due both to the fundamental properties and the promising potential in spintronics based applications. However, controlled creation of skyrmions remains a pivotal challenge towards technological applications. Here, we report that skyrmions can be created locally by electric field in the magnetoelectric helimagnet Cu$\mathsf{_2}$OSeO$\mathsf{_3}$. Using Lorentz transmission electron microscopy, we successfully write skyrmions in situ from a helical spin background. Our discovery is highly coveted since it implies that skyrmionics can be integrated into contemporary field effect transistor based electronic technology, where very low energy dissipation can be achieved, and hence realizes a large step forward to its practical applications.

cond-mat.str-el↗

arXiv2017

Role of the particle size polydispersity in the electrical conductivity of carbon nanotube-epoxy composites

Carbon nanotubes (CTNs) with large aspect-ratios are extensively used to establish electrical connectedness in polymer melts at very low CNT loadings. However, the CNT size polydispersity and the quality of the dispersion are still not fully understood factors that can substantially alter the desired characteristics of CNT nanocomposites. Here we demonstrate that the electrical conductivity of polydisperse CNT-epoxy composites with purposely-tailored distributions of the nanotube length L is a quasiuniversal function of the first moment of L. This finding challenges the current understanding that the conductivity depends upon higher moments of the CNT length. We explain the observed quasiuniversality by a combined effect between the particle size polydispersity and clustering. This mechanism can be exploited to achieve controlled tuning of the electrical transport in general CNT nanocomposites.

cond-mat.mtrl-sci↗

arXiv2017

Strongly bound excitons in anatase TiO2 single crystals and nanoparticles

Anatase TiO$_2$ is among the most studied materials for light-energy conversion applications, but the nature of its fundamental charge excitations is still unknown. Yet it is crucial to establish whether light absorption creates uncorrelated electron-hole pairs or bound excitons and, in the latter case, to determine their character. Here, by combining steady-state angle-resolved photoemission spectroscopy and spectroscopic ellipsometry with state-of-the-art ab initio calculations, we demonstrate that the direct optical gap of single crystals is dominated by a strongly bound exciton rising over the continuum of indirect interband transitions. This exciton possesses an intermediate character between the Wannier-Mott and Frenkel regimes and displays a peculiar two-dimensional wavefunction in the three-dimensional lattice. The nature of the higher-energy excitations is also identified. The universal validity of our results is confirmed up to room temperature by observing the same elementary excitations in defect-rich samples (doped single crystals and nanoparticles) via ultrafast two-dimensional deep-ultraviolet spectroscopy.

cond-mat.mtrl-sci↗

arXiv2016

Probing the coupling between a doublon excitation and the charge-density wave in TaS2 by ultrafast optical spectroscopy

Recently, the switching between the different charge-ordered phases of 1T-TaS2 has been probed by ultrafast techniques, revealing unexpected phenomena such as "hidden" metastable states and peculiar photoexcited charge patterns. Here, we apply broadband pump-probe spectroscopy with varying excitation energy to study the ultrafast optical properties of 1T-TaS2 in the visible regime. By scanning the excitation energy in the near-IR region we unravel the coupling between different charge excitations and the low-lying charge-density wave state. We find that the amplitude mode of the charge-density wave exhibits strong coupling to a long-lived doublon state that is photoinduced in the center of the star-shaped charge-ordered Ta clusters by the near-IR optical excitation.

cond-mat.str-el↗

arXiv2015

The Role of Transport Agents in MoS2 Single Crystals

We report resistivity, thermoelectric power and thermal conductivity of MoS2 single crystals prepared by chemical vapour transport (CVT) method using I2, Br2 and TeCl4 as transport agents. The material presents low-lying donor and acceptor levels, which dominate the in-plane charge transport. Intercalates into the Van der Waals gap strongly influence the inter-plane resistivity. Thermoelectric power displays the characteristics of strong electron-phonon interaction. Detailed theoretical model of thermal conductivity reveals the presence of high number of defects in the MoS2 structure. We show that these defects are inherent to CVT growth method, coming mostly from the transport agent molecules inclusion as identified by Total Reflection X-ray Fluorescence analysis (TXRF) and in-beam activation analysis (IBAA).

cond-mat.mtrl-sci↗