Searcharxiv⌕ Search

arXiv subjects

Bence G. Márkus

Publications and source records attributed to Bence G. Márkus.

14 recordsLinked to original sources

Disorder-driven symmetry suppression by van der Waals planar defects in a magnetic topological insulator

Magnetic topological insulators offer a platform to control electronic topology through magnetic order, yet reliable routes to tune their properties remain limited. Here, we show that ion irradiation allows to modify the magnetic properties and the anomalous Hall response of the van der Waals magnetic topological insulator MnBi$_2$Te$_4$. Using noble gas ion beams, intrinsic defects are introduced via collision cascades without chemical doping. We identify two distinct regimes. At low fluence, cation antisite disorder leads to a near-complete redistribution of Bi over cation sites while preserving long-range crystallographic order, accompanied by a transition from $p$-type to $n$-type transport. At high fluence, cation-anion intermixing drives the formation of a previously unreported layer-disordered phase characterized by a high density of van der Waals-specific planar defects, including swapped bilayers. Despite significant structural disorder, the system retains partial periodic order up to high displacement levels. Magnetometry and X-ray spectroscopy show that the Mn high-spin state and intralayer antiferromagnetic interactions likely persist, while macroscopic magnetic anisotropy is strongly reduced. At the same time, the magnitude of the anomalous Hall conductivity is reduced by an order of magnitude, far exceeding the change in magnetization, and its sign is modified. The observations are consistent with a suppression of the Berry curvature of the occupied states. These results establish ion irradiation as a means to tune anomalous Hall conductivity in topological insulators through defect engineering and reveal a disorder-driven approach to control symmetry and electronic structure in van der Waals magnetic materials.

cond-mat.mtrl-sci↗

Mn--Cr dopant association in dilute co-doped $\mathrm{ZnAl_2O_4}$ revealed by combined EPR and optical spectroscopy

Efficient and durable phosphors made from abundant elements underpin energy-saving solid-state lighting, near-infrared light sources for sensing, and X-ray and biomedical imaging. Co-doping is a standard route to brighter phosphors, yet the fate of the co-dopants is rarely established. We combine quantitative electron paramagnetic resonance (EPR) spin counting with photoluminescence, photoluminescence excitation, and X-ray-excited spectroscopy across two dilute Mn/Cr co-doping series of hydrothermally grown $\mathrm{ZnAl_2O_4}$ nanoparticles and show that the two ions can form an exchange-coupled, edge-sharing Cr--Mn defect complex, with $\mathrm{Mn^{2+/4+}}$ entering an octahedral site next to $\mathrm{Cr^{3+}}$. The octahedral Mn lifts the inversion symmetry of the $\mathrm{Cr^{3+}}$ site and strengthens its parity-forbidden absorption, enhancing the $\mathrm{Cr^{3+}}$ emission without energy transfer. The population of the defect complex follows the law of mass action, and above a threshold Mn concentration, Mn re-partitions into EPR-silent octahedral configurations that quench both emissions. Concentration optima in co-doped phosphors can thus reflect defect speciation, not only energy-transfer efficiency, which opens a structural design handle for brighter emitters.

cond-mat.mtrl-sci↗

Highly Efficient Functionalization of hBN with Lithium Oxalate: A Multifunctional Platform for Composites, Ion Transport, and Spin Labeling

Multifunctional solid-state materials are crucial for enabling safer and simpler lithium battery architectures. Here we report a scalable, solvent-free mechanochemical strategy to overcome the chemical inertness of hexagonal boron nitride and produce Li$_2$(BN)$_6$C$_2$O$_4$ (LBNCO), a lithium-rich boron nitride nanostructure. High-energy milling simultaneously exfoliates hBN and induces robust covalent oxalate functionalization, yielding a nanocrystalline lamellar compound with intrinsically incorporated lithium. LBNCO exhibits Li$^+$ ionic conductivity, electronic insulation, and thermal stability exceeding $350~^{\circ}$C. Additional mechanochemical processing enables further lithium enrichment without compromising chemical stability, allowing tunable ionic conductivity. By integrating ion transport, mechanical robustness, and thermal stability within a single material, LBNCO establishes a new platform for solid-state lithium batteries and related technologies.

cond-mat.mtrl-sci↗

Conductivity scaling of the anomalous Hall effect in the altermagnetic semiconductor α-MnTe

α-MnTe is a prototypical altermagnet exhibiting a strong anomalous Hall effect (AHE), despite having a nearly vanishing magnetization. Lately, sample-to-sample variations of the amplitude of the AHE have raised concerns of a possible defect related origin, especially in thin films. Here, we study the AHE in α-MnTe films grown on SrF2 that have the crystal structure and m'm'm magnetic point group symmetry expected for bulk. By studying the scaling of the AHE with conductivity for those films and previously reported measurements in the literature, we find that sample-to-sample variations are well explained by a scaling law consistent with a hopping origin. Importantly, a comparison with other magnetic semiconductors reveals the colossal amplitude of the AHE of α-MnTe compared to its measured spontaneous magnetization from magnetometry and polarized neutron reflectivity. Our findings address the important fundamental question of the origin of the AHE of α-MnTe and further demonstrate the potential of altermagnets as promising spintronic materials.

cond-mat.str-el↗

Transient Plastic Spin Labeling with Chlorine Dioxide

Plastic waste, being one of the most important problems for humankind, poses severe threats to ecosystems, wildlife, and human health. Tracing, quantifying, and identifying types of plastic waste is of crucial importance to understand its environmental pathways and develop targeted strategies for reduction, recycling, and remediation. To contribute to addressing this global issue, we investigated the spin-labeling capabilities of aqueous chlorine dioxide (ClO$_2$) radicals upon introduction into poly(ethylene terephthalate) and utilized electron spin resonance spectroscopy for detection. The technique is capable of identifying plastic species as the unpaired electron of the radical molecule is strongly sensitive to its local environment through its coupling parameters. Temperature-dependent measurements revealed that the molecules are immobilized at low temperatures and exhibit well-resolved anisotropic and hyperfine spectra that are quantitatively described by a model spin Hamiltonian. Even above the melting point of water, some degrees of freedom remain blocked as a result of the polymer matrix. Furthermore, employing a time-series measurement at room temperature enabled us to determine the diffusion coefficient of the molecule in the polymer.

cond-mat.other↗

Anisotropy, frustration and saddle point in the twisted Kagome antiferromagnet ErPdPb

The kagome lattice, with its inherent geometric frustration, provides a rich platform for exploring intriguing magnetic phenomena and topological electronic structures. In reduced-symmetry structures, such as twisted kagome systems involving rare earth elements, additional anisotropy can arise, enabling intriguing properties including spin-ice states, magnetocaloric effects, noncollinear magnetic ordering, and anomalous Hall effect. Here, we report the synthesis of single crystals of ErPdPb, which features a twisted kagome lattice net of Er atoms within the hexagonal ZrNiAl-type structure, and we investigate its magnetic, electronic, and thermal properties. The material exhibits antiferromagnetic ordering below 2.2 K, consistently observed in magnetic, transport, and heat capacity measurements. Magnetization measurements reveal 1/3 metamagnetic steps along the c-axis below the Néel temperature, suggesting an Ising-spin-like state on the twisted kagome lattice. A pronounced anisotropy between in-plane and out-of-plane resistivity is observed throughout the temperature range of 1.8-300 K, and the compound exhibits a significant frustration index of 13.6 (12.7) along the c-axis (ab-plane). Heat capacity measurements show a broad hump at 2.2 K, with an additional increase below 0.5 K. The anisotropic magnetic properties are further explored through density functional theory (DFT) calculations, which suggest strong easy-axis anisotropy, consistent with experimental magnetic measurements and crystal-field model expectations, and quasi-one-dimensional bands and a spin-split saddle point at the zone center.

cond-mat.str-el↗

Crystal Growth and Physical Properties of Orthorhombic Kagome Lattice Magnets $R$Fe$_6$Ge$_6$ ($R$=Y, Tb, Dy)

Kagome magnets represent a promising class of materials that exhibit intriguing electronic and magnetic properties, and they have recently garnered significant attention. While most kagome-lattice compounds are hexagonal, we report here single-crystal growth and physical property measurements of $R$Fe$_6$Ge$_6$ ($R$ = Y, Dy, Tb) compounds, which crystallize in an orthorhombic structure. The structure can be derived from a hexagonal prototype $R$Fe$_3$Ge$_2$ by replacing every other $R$ atom with a covalent Ge$_2$ dimer. Ordering of these dimers renders the structure orthorhombic, slightly distorts the kagome net, and makes the three Fe sites formally inequivalent. The iron and rare-earth sublattices order independently. Fe moments order above 400 K, forming ferromagnetic kagome planes stacked antiferromagnetically, while rare-earth moments order below 9 K. TbFe$_6$Ge$_6$ exhibits a single magnetic ordering transition associated with the Tb atoms, whereas DyFe$_6$Ge$_6$ shows two distinct magnetic phase transitions, strongly influenced by crystal electric field effects on the Dy$^{3+}$ ions. Density functional theory (DFT) calculations indicate that the ferromagnetic ordering of the Fe planes is driven by a high density of states at the Fermi energy. They also reveal three dramatically different structural energy scales: $R$ and Ge$_2$ form alternating 1D chains perpendicular to the kagome planes, and violating this alternation incurs a large energy cost. Aligning these chains is less costly, and achieving a two-dimensional order of anti-aligned chains requires very little energy. These compounds represent a unique class of materials, offering new opportunities to investigate the interplay between the distinct crystal lattice geometry and the underlying electronic and magnetic properties.

cond-mat.mtrl-sci↗

Unprecedented Spin-Lifetime of Itinerant Electrons in Natural Graphite Crystals

A long spin-lifetime of electrons is the holy grail of spintronics, a field exploiting the electron angular momentum as information carrier and storage unit. Previous reports indicated a spin lifetime, $τ_{\text{s}}$ near $10$ ns at best in graphene-based devices at low temperatures. We detail the observation of $τ_{\text{s}}$ approaching the ultralong $1{,}000$~ns at room temperature in natural graphite crystals using magnetic resonance spectroscopy. The relaxation time shows a giant anisotropy: the lifetime of spins, polarized perpendicular to the graphite plane, is more than $50$ times longer than for the in-plane polarization. The temperature dependence of $τ_{\text{s}}$ proves that diffusion of spins to the crystallite edges, where relaxation occurs, limits the lifetime. This suggests that graphite is an excellent candidate for spintronic applications, seamlessly integrating with emerging 2D van der Waals technologies.

cond-mat.mes-hall↗

Surface Chemistry-Driven Oxidation Mechanisms in Ti$_{\text{3}}$C$_{\text{2}}$T$_{\textit{x}}$ MXenes

Ti$_3$C$_2$T$_x$ is a leading compound within the MXenes family and can find host in widespread applications. It is synthesized by selectively etching layers from the Ti$_3$AlC$_2$ precursor, and this process typically introduces surface terminations, T$_x$, such as $-$OH, $=$O, or $-$F. However, the aggressive chemical conditions required for its preparation, as well as exposure to air, humidity, and heat, can lead to impurity phases that potentially compromise its desirable properties. We reveal a two-step oxidation process during heat treatment, where initial oxidation occurs between layers without altering the integrity of the Ti$_3$C$_2$ layered structure, followed by the formation of anatase TiO$_2$ at elevated temperatures. The process was carefully monitored using \emph{in situ} Raman spectroscopy and \emph{in situ} microwave conductivity measurements, employed to Ti$_3$C$_2$T$_x$ prepared using various etching techniques involving concentrated HF, LiF + HCl, and HF + HCl mixtures. The oxidation process is heavily influenced by the synthesis route and surface chemistry of Ti$_3$C$_2$T$_x$, with fluoride and oxyfluoride groups playing a pivotal role in stabilizing the anatase phase. The absence of these groups, in contrast, can lead to the formation of rutile TiO$_2$.

cond-mat.mtrl-sci↗

Unexpected Tuning of the Anomalous Hall Effect in Altermagnetic MnTe Thin Films

The discovery of an anomalous Hall effect (AHE) sensitive to the magnetic state of antiferromagnets can trigger a new era of spintronics, if materials that host a tunable and strong AHE are identified. Altermagnets are a new class of materials that can under certain conditions manifest a strong AHE, without having a net magnetization. But the ability to control their AHE is still lacking. In this study, we demonstrate that the AHE in altermagnetic α-MnTe grown on GaAs(111) substrates can be "written on-demand" by cooling the material under an in-plane magnetic field. The magnetic field controls the strength and the coercivity of the AHE. Remarkably, this control is unique to α-MnTe grown on GaAs and is absent in α-MnTe grown on SrF2. The tunability that we reveal challenges our current understanding of the symmetry-allowed AHE in this material and opens new possibilities for the design of altermagnetic spintronic devices.

cond-mat.mtrl-sci↗

Anomalous specific heat peak of BaVS$_3$ at 69 K explained by enhanced electron scattering upon ion relocation

The present study deals with the anomalous heat capacity peak and thermal conductivity of BaVS$_3$ near the metal-insulator transition present at $69$ K. The transition is related to a structural transition from an orthorhombic to monoclinic phase. Heat capacity measurements at this temperature exhibit a significant and relatively broad peak, which is also sample dependent. The present study calculates the entropy increase during the structural transition and we show that the additional entropy is caused by enhanced electron scattering as a result of the structural reorientation of the nuclei. Within the model it is possible to explain quantitatively the observed peak alike structure in the heat capacity and in heat conductivity.

cond-mat.str-el↗

Electronic and magnetic properties of black phosphorus

Black phosphorus has emerged as the next member in the graphene inspired two-dimensional materials family. Its electronic and magnetic properties are studied herein using electron and nuclear magnetic resonance techniques (ESR and NMR) and microwave conductivity measurement. The latter is a unique technique to study conductivity on air sensitive samples. The ESR study indicates the absence of free charge carriers and no sign of paramagnetic defects are found. $^{31}$P NMR shows the presence of a characteristic Pake doublet structure due to the interaction between $I = 1/2$ nuclei. Microwave conductivity shows, in accordance with the ESR results, that black phosphorus behaves as a semiconductor and we identify extrinsic and intrinsic charge carrier contributions to the conductivity and extracted the sizes of the gaps. ESR measurement also yields that bP might find applications as a microwave absorbent.

cond-mat.str-el↗

Anisotropic Elliott-Yafet Theory and Application to KC$_8$ Potassium Intercalated Graphite

We report Electron Spin Resonance (ESR) measurements on stage-I potassium intercalated graphite (KC$_8$). Angular dependent measurements show that the spin-lattice relaxation time is longer when the magnetic field is perpendicular to the graphene layer as compared to when the magnetic field is in the plane. This anisotropy is analyzed in the framework of the Elliott-Yafet theory of spin-relaxation in metals. The analysis considers an anisotropic spin-orbit Hamiltonian and the first order perturbative treatment of Elliott is reproduced for this model Hamiltonian. The result provides an experimental input for the first-principles theories of spin-orbit interaction in layered carbon and thus to a better understanding of spin-relaxation phenomena in graphene and in other layered materials as well.

cond-mat.str-el↗

Transport, Magnetic and Vibrational Properties of Chemically Exfoliated Few Layer Graphene

We study the vibrational, magnetic and transport properties of Few Layer Graphene (FLG) using Raman and electron spin resonance spectroscopy and microwave conductivity measurements. FLG samples were produced using wet chemical exfoliation with different post-processing, namely ultrasound treatment, shear mixing, and magnetic stirring. Raman spectroscopy shows a low intensity D mode which attests a high sample quality. The G mode is present at $1580$ cm$^{-1}$ as expected for graphene. The 2D mode consists of 2 components with varying intensities among the different samples. This is assigned to the presence of single and few layer graphene in the samples. ESR spectroscopy shows a main line in all types of materials with a width of about $1$ mT and and a $g$-factor in the range of $2.005-2.010$. Paramagnetic defect centers with a uniaxial $g$-factor anisotropy are identified, which shows that these are related to the local sp$^2$ bonds of the material. All kinds of investigated FLGs have a temperature dependent resistance which is compatible with a small gap semiconductor. The difference in resistance is related to the different grain size of the samples.

cond-mat.mtrl-sci↗