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Frédéric Bonell

Publications and source records attributed to Frédéric Bonell.

14 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↗

Rashba engineering at van der Waals interfaces

Two-dimensional transition metal dichalcogenide (TMD) interfaces offer a versatile platform for studying emergent quantum phenomena and enabling novel device functionalities. When distinct TMD monolayers are stacked vertically or laterally stitched, their interfaces can exhibit unique electronic band alignments, giving rise to long-lived interlayer excitons, charge transfer effects, and moiré superlattices with correlated states. Here, we demonstrate that the interface between a large variety of two different epitaxially grown TMD monolayers controls the intensity and sign of the Rashba spin splitting, which is probed using THz spintronic emission. Optimized TMD heterobilayers, such as HfSe$_2$/PtSe$_2$, show enhanced THz emission that surpass the spin-to-charge conversion efficiency of bulk TMDs, confirming the presence of Rashba states with large spin splitting at the interface. By combining spin- and angle-resolved photoemission spectroscopy with density functional theory, we reveal that the electronic hybridization between the two different TMD monolayers gives rise to extended in-gap states with strong Rashba spin-orbit coupling. The choice of TMD layers enables to engineer the sign and strength of spin-to-charge conversion in van der Waals heterobilayers opening up perspectives to build efficient and tunable THz spintronic emitters.

cond-mat.mes-hall↗

Room temperature magnetic vortices in the van der Waals magnet Fe$_5$GeTe$_2$

We investigate the effect of confinement on the magnetic state of a 12 nm-thick Fe$_5$GeTe$_2$ layer grown by molecular beam epitaxy. We use quantitative scanning NV magnetometry to locally extract the magnetization in rectangular uniformly in-plane magnetized microstructures, showing no enhancement of the Curie temperature compared to magnetization measurements performed before patterning the film, in contrast to previous results obtained on thick Fe$_3$GeTe$_2$ flakes. Under the application of a weak out-of-plane magnetic field, we observe the stabilization of magnetic vortices at room temperature in micrometric squares. Finally, we highlight the effect of the size of the patterned micro-discs and micro-squares on the stabilization of the vortices using experiments and micromagnetic simulations. Our work thus proposes and demonstrates a way to stabilize non-collinear textures at room temperature in a van der Waals magnets using confinement, although we also show that this approach alone is not successful to enhance the Curie temperature of Fe$_5$GeTe$_2$ significantly above 300 K.

cond-mat.mtrl-sci↗

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↗

Spin-orbit torque switching in 2D ferromagnet / topological insulator heterostructure grown by molecular beam epitaxy

Topological insulators (TIs) are a promising class of materials for manipulating the magnetization of an adjacent ferromagnet (FM) through the spin-orbit torque (SOT) mechanism. However, current studies combining TIs with conventional FMs present large device-to-device variations, resulting in a broad distribution of SOT magnitudes. It has been identified that the interfacial quality between the TI and the FM is of utmost importance in determining the nature and efficiency of the SOT. To optimize the SOT magnitude and enable ultra-low-power magnetization switching, an atomically smooth interface is necessary. To this end, we have developed the growth of a full van der Waals FM/TI heterostructure by molecular beam epitaxy. The compensated TI (Bi0.4Sb0.6)2Te3 and ferromagnetic Fe3GeTe2 (FGT) were chosen because of their exceptional crystalline quality, low carrier concentration in BST and relatively large Curie temperature and perpendicular magnetic anisotropy in FGT. We characterized the magnitude of the SOTs by using thorough harmonic magnetotransport measurements and showed that the magnetization of an ultrathin FGT film could be switched with a current density Jc < 10^10 A/m^2. In comparison to previous studies utilizing traditional FMs, our findings are highly reliable, displaying little to no variation between devices.

cond-mat.mes-hall↗

Visualizing giant ferroelectric gating effects in large-scale WSe$_2$/BiFeO$_3$ heterostructures

Multilayers based on quantum materials (complex oxides, topological insulators, transition-metal dichalcogenides, etc) have enabled the design of devices that could revolutionize microelectronics and optoelectronics. However, heterostructures incorporating quantum materials from different families remain scarce, while they would immensely broaden the range of possible applications. Here we demonstrate the large-scale integration of compounds from two highly-multifunctional families: perovskite oxides and transition-metal dichalcogenides (TMDs). We couple BiFeO$_3$, a room-temperature multiferroic oxide, and WSe$_2$, a semiconducting two-dimensional material with potential for photovoltaics and photonics. WSe$_2$ is grown by molecular beam epitaxy and transferred on a centimeter-scale onto BiFeO$_3$ films. Using angle-resolved photoemission spectroscopy, we visualize the electronic structure of 1 to 3 monolayers of WSe$_2$ and evidence a giant energy shift as large as 0.75 eV induced by the ferroelectric polarization direction in the underlying BiFeO$_3$. Such a strong shift opens new perspectives in the efficient manipulation of TMDs properties by proximity effects.

cond-mat.mtrl-sci↗

Phonon dynamics and thermal conductivity of PtSe2 thin films: Impact of crystallinity and film thickness on heat dissipation

We present a comparative investigation of the influence of crystallinity and film thickness on the acoustic and thermal properties of 2D layered PtSe2 thin films of varying thickness (0.6-24 nm) by combining a set of experimental techniques, namely, frequency domain thermo-reflectance, low-frequency Raman and pump-probe coherent phonon spectroscopy. We find a 35% reduction in the cross-plane thermal conductivity of polycrystalline films with thickness larger than 12 nm compared to the crystalline films of the same thickness due to phonon grain boundary scattering. Density functional theory calculations are in good agreement with the experiments and further reveal the ballistic nature of cross-plane heat transport in PtSe2 up to a certain thickness (~20 nm). In addition, our experiments revealed strong interlayer interactions in PtSe2, short acoustic phonon lifetimes in the range of picoseconds, out-of-plane elastic constant C33=31.8 GPa and layer-dependent group velocity ranging from 1340 m/s in bilayer PtSe2 to 1873 m/s in 8 layers of PtSe2. The potential of tuning the lattice cross-plane thermal conductivity of layered 2D materials with the level of crystallinity and the real-time observation of coherent phonon dynamics, which have direct implications on the cooling and transport of electrons, open a new playground for research in 2D thermoelectric devices and provide guidelines for thermal management in 2D electronics.

cond-mat.mtrl-sci↗

High carrier mobility in single-crystal PtSe2 grown by molecular beam epitaxy on ZnO(0001)

PtSe2 is attracting considerable attention as a high mobility two-dimensional material with envisionned applications in microelectronics, photodetection and spintronics. The growth of high quality PtSe2 on insulating substrates with wafer-scale uniformity is a prerequisite for electronic transport investigations and practical use in devices. Here, we report the growth of highly oriented few-layers PtSe2 on ZnO(0001) by molecular beam epitaxy. The crystalline structure of the films is characterized with electron and X-ray diffraction, atomic force microscopy and transmission electron microscopy. The comparison with PtSe2 layers grown on graphene, sapphire, mica, SiO2 and Pt(111) shows that among insulating substrates, ZnO(0001) yields films of superior structural quality. Hall measurements performed on epitaxial ZnO/PtSe2 with 5 monolayers of PtSe2 show a clear semiconducting behaviour and a high mobility in excess of 200 cm2V 1s-1 at room temperature and up to 447 cm2V-1s-1 at low temperature.

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↗

Control of spin-orbit torques by interface engineering in topological insulator heterostructures

(Bi$_{1-x}$Sb$_x$)$_2$Te$_3$ topological insulators (TIs) are gathering increasing attention owing to their large charge-to-spin conversion efficiency and the ensuing spin-orbit torques (SOTs) that can be used to manipulate the magnetization of a ferromagnet (FM). The origin of the torques, however, remains elusive, while the implications of hybridized states and the strong material intermixing at the TI/FM interface are essentially unexplored. By combining interface chemical analysis and spin-transfer ferromagnetic resonance (ST-FMR) measurements, we demonstrate that intermixing plays a critical role in the generation of SOTs. By inserting a suitable normal metal spacer, material intermixing is reduced and the TI properties at the interface are largely improved, resulting in strong variations in the nature of the SOTs. A dramatic enhancement of a field-like torque, opposing and surpassing the Oersted-field torque, is observed, which can be attributed to the non-equilibrium spin density in Rashba-split surface bands and to the suppression of spin memory loss.

cond-mat.mes-hall↗

A Molecular Approach for Engineering Interfacial Interactions in Magnetic-Topological Insulator Heterostructures

Controlling interfacial interactions in magnetic/topological insulator heterostructures is a major challenge for the emergence of novel spin-dependent electronic phenomena. As for any rational design of heterostructures that rely on proximity effects, one should ideally retain the overall properties of each component while tuning interactions at the interface. However, in most inorganic interfaces interactions are too strong, consequently perturbing, and even quenching, both the magnetic moment and the topological surface states at each side of the interface. Here we show that these properties can be preserved by using ligand chemistry to tune the interaction of magnetic ions with the surface states. By depositing Co-based porphyrin and phthalocyanine monolayers on the surface of Bi$_2$Te$_3$ thin films, robust interfaces are formed that preserve undoped topological surface states as well as the pristine magnetic moment of the divalent Co ions. The selected ligands allow us to tune the interfacial hybridization within this weak interaction regime. These results, which are in stark contrast with the observed suppression of the surface state at the first quintuple layer of Bi$_2$Se$_3$ induced by the interaction with Co phthalocyanines, demonstrate the capability of planar metal-organic molecules to span interactions from the strong to the weak limit.

cond-mat.mtrl-sci↗

Determination of the spin-lifetime anisotropy in graphene using oblique spin precession

We determine the spin-lifetime anisotropy of spin-polarized carriers in graphene. In contrast to prior approaches, our method does not require large out-of-plane magnetic fields and thus it is reliable for both low- and high-carrier densities. We first determine the in-plane spin lifetime by conventional spin precession measurements with magnetic fields perpendicular to the graphene plane. Then, to evaluate the out-of-plane spin lifetime, we implement spin precession measurements under oblique magnetic fields that generate an out-of-plane spin population. We find that the spin-lifetime anisotropy of graphene on silicon oxide is independent of carrier density and temperature down to 150 K, and much weaker than previously reported. Indeed, within the experimental uncertainty, the spin relaxation is isotropic. Altogether with the gate dependence of the spin lifetime, this indicates that the spin relaxation is driven by magnetic impurities or random spin-orbit or gauge fields.

cond-mat.mes-hall↗

Strongly anisotropic spin relaxation in graphene/transition metal dichalcogenide heterostructures at room temperature

Graphene has emerged as the foremost material for future two-dimensional spintronics due to its tuneable electronic properties. In graphene, spin information can be transported over long distances and, in principle, be manipulated by using magnetic correlations or large spin-orbit coupling (SOC) induced by proximity effects. In particular, a dramatic SOC enhancement has been predicted when interfacing graphene with a semiconducting transition metal dechalcogenide, such as tungsten disulphide (WS$_2$). Signatures of such an enhancement have recently been reported but the nature of the spin relaxation in these systems remains unknown. Here, we unambiguously demonstrate anisotropic spin dynamics in bilayer heterostructures comprising graphene and WS$_2$. By using out-of-plane spin precession, we show that the spin lifetime is largest when the spins point out of the graphene plane. Moreover, we observe that the spin lifetime varies over one order of magnitude depending on the spin orientation, indicating that the strong spin-valley coupling in WS$_2$ is imprinted in the bilayer and felt by the propagating spins. These findings provide a rich platform to explore coupled spin-valley phenomena and offer novel spin manipulation strategies based on spin relaxation anisotropy in two-dimensional materials.

cond-mat.mes-hall↗

Bias dependence of tunneling magnetoresistance in magnetic tunnel junctions with asymmetric barriers

The transport properties of magnetic tunnel junctions (MTJs) are very sensitive to interface modifications. In this work we investigate both experimentally and theoretically the effect of asymmetric barrier modifications on the bias dependence of tunneling magnetoresistance (TMR) in single crystal Fe/MgO-based MTJs with (i) one crystalline and one rough interface and (ii) with a monolayer of O deposited at the crystalline interface. In both cases we observe an asymmetric bias dependence of TMR and a reversal of its sign at large bias. We propose a general model to explain the bias dependence in these and similar systems reported earlier. The model predicts the existence of two distinct TMR regimes: (i) tunneling regime when the interface is modified with layers of a different insulator and (ii) resonant regime when thin metallic layers are inserted at the interface. We demonstrate that in the tunneling regime negative TMR is due to the high voltage which overcomes the exchange splitting in the electrodes, while the asymmetric bias dependence of TMR is due to the interface transmission probabilities. In the resonant regime inversion of TMR could happen at zero voltage depending on the alignment of the resonance levels with the Fermi surfaces of the electrodes. Moreover, the model predicts a regime in which TMR has different sign at positive and negative bias suggesting possibilities of combining memory with logic functions.

cond-mat.mtrl-sci↗