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Bettina Lotsch

Publications and source records attributed to Bettina Lotsch.

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Harnessing van der Waals CrPS4 and Surface Oxides for non-monotonic pre-set field induced Exchange Bias in Fe3GeTe2

Two-dimensional van der Waals (vdW) heterostructures are an attractive platform for studying exchange bias due to their defect free and atomically flat interfaces. Chromium thiophosphate (CrPS4), an antiferromagnetic material, possesses uncompensated magnetic spins in a single layer, rendering it a promising candidate for exploring exchange bias phenomena. Recent findings have highlighted that naturally oxidized vdW ferromagnetic Fe3GeTe2 exhibits exchange bias, attributed to the antiferromagnetic coupling of its ultrathin surface oxide layer (O-FGT) with the underlying unoxidized Fe3GeTe2. Anomalous Hall measurements are employed to scrutinize the exchange bias within the CrPS4/(O-FGT)/Fe3GeTe2 heterostructure. This analysis takes into account the contributions from both the perfectly uncompensated interfacial CrPS4 layer and the interfacial oxide layer. Intriguingly, a distinct and non-monotonic exchange bias trend is observed as a function of temperature below 140 K. The occurrence of exchange bias induced by a 'pre-set field' implies that the prevailing phase in the polycrystalline surface oxide is ferrimagnetic Fe3O4. Moreover, the exchange bias induced by the ferrimagnetic Fe3O4 is significantly modulated by the presence of the van der Waals antiferromagnetic CrPS4 layer, forming a heterostructure, along with additional iron oxide phases within the oxide layer. These findings underscore the intricate and complex nature of exchange bias in van der Waals heterostructures, highlighting their potential for tailored manipulation and control.

cond-mat.mtrl-sci

Skyrmionic Spin Structures in Layered Fe5GeTe2 Up To Room Temperature

The role of the crystal lattice, temperature and magnetic field for the spin structure formation in the 2D van der Waals magnet Fe5GeTe2 is a key open question. Using Lorentz transmission electron microscopy, we experimentally observe topological spin structures up to room temperature in the metastable pre-cooling and stable post-cooling phase of Fe5GeTe2. Over wide temperature and field ranges, skyrmionic magnetic bubbles form without preferred chirality, which is indicative of a centrosymmetric crystal structure. In the pre-cooling phase, these bubbles are observable even without the application of an external field, while in the post-cooling phase, a transformation from bubble domains to stripe domains is seen. To understand the magnetic order in Fe5GeTe2 we compare macroscopic magnetometry characterization results with microscopic density functional theory calculation. Our results show that even up to room temperature, topological spin structures can be stabilized in centrosymmetric van der Waals magnets.

cond-mat.mes-hall

Influence of Layer Slipping on Adsorption of Light Gases in Covalent Organic Frameworks: A Combined Experimental and Computational Study

Sorption of gases in micro- and mesoporous materials is typically interpreted on the basis of idealized structural models where real structure effects such as defects and disorder are absent. For covalent organic frameworks (COFs) significant discrepancies between measured and simulated adsorption isotherms are often reported but rarely traced back to their origins. This is because little is known about the real structure of COFs and its effect on the sorption properties of these materials. In the present work molecular simulations are used to obtain adsorption isotherms of argon, nitrogen, and carbon dioxide in the COF-LZU1 at various temperatures. The (perfect) model COF has a BET surface that is higher than the experimental BET surface by a factor of approximately 1.33, suggesting defects or inclusions are present in the real structure. We find that the saturation adsorption loading of small gaseous species in COF-LZU1, as determined from grand canonical Monte Carlo simulations, is also higher by approximately the same factor compared to the experimental saturation loading. The influence of interlayer slipping on the shape of the adsorption isotherm and the adsorption capacity is studied. Comparison between simulation and experiment at lower loadings suggests the layers to be shifted instead of perfectly eclipsed. The sensitivity of the adsorption isotherms in this regime towards the underlying framework topology shows that real structure effects have significant influence on the gas uptake. Accounting for layer slipping is important to applications such as catalysis, gas storage and separation.

physics.chem-ph

Strong bulk spin-orbit torques quantified in the van der Waals ferromagnet Fe3GeTe2

The recent emergence of magnetic van der Waals materials allows for the investigation of current induced magnetization manipulation in two dimensional materials. Uniquely, Fe3GeTe2 has a crystalline structure that allows for the presence of bulk spin-orbit torques (SOTs), that we quantify in a Fe3GeTe2 flake. From the symmetry of the measured torques, we identify the current induced effective fields using harmonic analysis and find dominant bulk SOTs, which arise from the symmetry in the crystal structure. Our results show that Fe3GeTe2 uniquely can exhibit bulk SOTs in addition to the conventional interfacial SOTs enabling magnetization manipulation even in thick single layers without the need for complex multilayer engineering.

cond-mat.mtrl-sci

Spin-split band hybridization in graphene proximitized with $α$-RuCl$_3$ nanosheets

Proximity effects induced in the 2D Dirac material graphene potentially open access to novel and intriguing physical phenomena. Thus far, the coupling between graphene and ferromagnetic insulators has been experimentally established. However, only very little is known about graphene's interaction with antiferromagnetic insulators. Here, we report a low temperature study of the electronic properties of high quality van der Waals heterostructures composed of a single graphene layer proximitized with $α$-RuCl$_3$. The latter is known to become antiferromagnetically ordered below 10 K. Shubnikov de Haas oscillations in the longitudinal resistance together with Hall resistance measurements provide clear evidence for a band realignment that is accompanied by a transfer of electrons originally occupying the graphene's spin degenerate Dirac cones into $α$-RuCl$_3$ band states with in-plane spin polarization. Left behind are holes in two separate Fermi pockets, only the dispersion of one of which is distorted near the Fermi energy due to spin selective hybridization with these spin polarized $α$-RuCl$_3$ band states. This interpretation is supported by our DFT calculations. An unexpected damping of the quantum oscillations as well as a zero field resistance upturn close to the N$é$el temperature of $α$-RuCl$_3$ suggests the onset of additional spin scattering due to spin fluctuations in the $α$-RuCl$_3$.

cond-mat.mtrl-sci

Chemical Principles of Topological Semimetals

Initiated by the discovery of topological insulators, topologically non-trivial materials have attracted immense interest in the physics community in the past decade. One of the latest additions to the field, the material class of topological semimetals, has grown at an extremely fast rate . While the prototype of a topological semimetal, graphene, has been known for a while, the first 3D analogues of graphene have only been discovered recently. This review, written from a chemistry perspective, intends to make the growing field of topological semimetals accessible to the wider community of materials scientists and scholars from related disciplines. To this end, we describe key features of topological semimetals, embedded in their electronic structure, and how they can be achieved based on chemical principles. We introduce the different classes of topological semimetals and review their salient representatives. Finally, selected properties and potential applications of these materials are discussed.

cond-mat.mtrl-sci

Similar ultrafast dynamics of several dissimilar Dirac and Weyl semimetals

Recent years have seen the rapid discovery of solids whose low-energy electrons have a massless, linear dispersion, such as Weyl, line-node, and Dirac semimetals. The remarkable optical properties predicted in these materials show their versatile potential for optoelectronic uses. However, little is known of their response in the picoseconds after absorbing a photon. Here we measure the ultrafast dynamics of four materials that share non-trivial band structure topology but that differ chemically, structurally, and in their low-energy band structures: ZrSiS, which hosts a Dirac line node and Dirac points; TaAs and NbP, which are Weyl semimetals; and Sr$_{1-y}$Mn$_{1-z}$Sb$_2$, in which Dirac fermions coexist with broken time-reversal symmetry. After photoexcitation by a short pulse, all four relax in two stages, first sub-picosecond, and then few-picosecond. Their rapid relaxation suggests that these and related materials may be suited for optical switches and fast infrared detectors. The complex change of refractive index shows that photoexcited carrier populations persist for a few picoseconds.

cond-mat.mtrl-sci

Butterfly Magnetoresistance, Quasi-2D Dirac Fermi Surfaces, and a Topological Phase Transition in ZrSiS

Magnetoresistance (MR), the change of a material's electrical resistance in response to an applied magnetic field, is a technologically important property that has been the topic of intense study for more than a quarter century. Here we report the observation of an unusual "butterfly" shaped titanic angular magnetoresistance (AMR) in the non-magnetic, Dirac material, ZrSiS. The MR is large and positive, reaching nearly 1.8 x 10^5 percent at 9 T and 2 K at an angle of 45o between the applied current (along the a-axis) and the applied field (90o is H parallel to the c-axis). Approaching 90o, a "dip" is seen in the AMR which can be traced to an angle dependent deviation from the H^2 law. By analyzing the SdH oscillations at different angles, we find that ZrSiS has a combination of 2D and 3D Dirac pockets comprising its Fermi surface and that the anomalous transport behavior coincides with a topological phase transition whose robust signature is evident despite transport contributions from other parts of the Fermi surface. We also find that as a function of angle, the temperature dependent resistivity in high field displays a broad peak-like behavior, unlike any known Dirac/Weyl material. The combination of very high mobility carriers and multiple Fermi surfaces in ZrSiS allow for large bulk property changes to occur as a function of angle between applied fields makes it a promising platform to study the physics stemming from the coexistence of 2D and 3D Dirac electrons.

cond-mat.mtrl-sci