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Ferenc Simon

Publications and source records attributed to Ferenc Simon.

At least 19 recordsLinked to original sources

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

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

The development of multifunctional solid-state materials is key to advancing lithium-ion batteries with enhanced safety and simplified architectures. Here, we report a scalable, highly efficient (near $100\%$), solvent-free mechanochemical synthesis of hexagonal boron nitride (hBN) functionalized with lithium oxalate (Li$_2$C$_2$O$_4$), yielding a novel lamellar composite that functions both as a lithium-ion conductor and separator. The high-energy milling process promotes exfoliation of hBN and covalent attachment of oxalate groups at edge and defect sites, forming a brown, nanocrystalline material with uniform lithium distribution. The composite exhibits room-temperature ionic and negligible electronic conductivity, thermal stability at least up to $350~^{\circ}$C, and hosts stable free radicals enabling its use as a spin label. The synthesis produces no byproducts and can be extended towards lithium doping via secondary mechanochemical steps, creating highly doped, chemically stable phases that host additional Li for ionic conduction. These results introduce a new class of lithium-rich, boron nitride-based solids for solid-state batteries, combining ion conduction, mechanical robustness, and thermal resilience in a single material platform.

cond-mat.mtrl-sci

Magnetic Dissipation in Ferrofluids

Ferrofluids, composed of magnetic nanoparticles suspended in a non-magnetic carrier liquid, have attracted considerable attention since their discovery in the 1960s. Their combination of liquid and magnetic properties gives rise to complex behaviors and unique functionalities, enabling a wide range of technological applications. Among these is the ability of the magnetic material to be moved by and to absorb heat when exposed to an external magnetic field -- a process that can occur through various dissipation mechanisms depending on the system. A detailed understanding of these mechanisms is crucial for tailoring materials to specific applications. We provide a comprehensive overview of the theoretical principles underlying different energy dissipation processes and propose a coherent framework for their interpretation. Particular attention is devoted to describing the frequency-dependent susceptibility, which is the key parameter to describe dissipation. We demonstrate that dissipation, predicted from magnetometry-based studies, matches well with direct, frequency-dependent calorimetric results, expanding the available frequency range of the characterization. The demonstrating measurements were carried out with a dilute ferrofluid containing magnetite nanoparticles of a mean diameter of 10.6 nm.

cond-mat.mtrl-sci

Physical Modeling of Saturated Common Mode Choke

Common mode chokes (CMCs) are conventional circuit elements performing several tasks, including noise suppression, hindering electromagnetic interference, providing signal integrity, and circuit protection. Much as they are widely used, their fundamental construction and description are often qualitative and lack an understanding of the underlying physical principles. We discuss the behavior of a commercial CMC based on the physical description of the superparamagnetic core and parasitic circuit elements. The results are validated using a DC bias current and an external magnetic field, which affect the magnetic properties. The behavior of the CMCs in the strongly non-linear regime is also described.

physics.app-ph

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, $\tau_{\text{s}}$ near $10$ ns at best in graphene-based devices at low temperatures. We detail the observation of $\tau_{\text{s}}$ 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 $\tau_{\text{s}}$ 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

Terahertz Emission From Diamond Nitrogen-Vacancy Centers

Coherent light sources emitting in the terahertz range are highly sought after for fundamental research and applications. THz lasers rely on achieving population inversion. We demonstrate the generation of THz radiation using nitrogen-vacancy (NV) centers in a diamond single crystal. Population inversion is achieved through the Zeeman splitting of the $S=1$ state in $15\ \text{T}$, resulting in a splitting of $0.42\ \text{THz}$, where the middle $S_z=0$ sublevel is selectively pumped by visible light. To detect the THz radiation, we utilize a phase-sensitive THz setup, optimized for electron spin resonance measurements (ESR). We determine the spin-lattice relaxation time up to $15\ \text{T}$ using the light-induced ESR measurement, which shows the dominance of phonon-mediated relaxation and the high efficacy of the population inversion. The THz radiation is tunable by the magnetic field, thus these findings may lead to the next generation of tunable coherent THz sources.

physics.optics

Incidence of the Brownian relaxation process on the magnetic properties of ferrofluids

Ferrofluids containing magnetic nanoparticles represent a special class of magnetic materials due to the added freedom of particle tumbling in the fluids. We studied this process, known as Brownian relaxation, and its effect on the magnetic properties of ferrofluids with controlled magnetite nanoparticle sizes. For small nanoparticles (below 10 nm diameter) the N\'eel process is expected to dominate the magnetic response, whereas for larger particles, Brownian relaxation becomes important. Temperature- and magnetic field-dependent magnetization studies, differential scanning calorimetry, and AC susceptibility measurements were carried out for 6, 8, 10.6, and 13.5 nm diameter magnetite nanoparticles suspended in water. We identify clear fingerprints of the Brownian relaxation for the sample of the large diameter nanoparticles as both magnetic and thermal hysteresis develop at the water freezing temperature, whereas the samples of small diameter nanoparticles remain hysteresis-free down to the magnetic blocking temperature. This is supported by the temperature-dependent AC susceptibility measurements: above 273 K, the data show a low-frequency Debye peak, which is characteristic of the Brownian relaxation. This peak vanishes below 273 K.

cond-mat.mtrl-sci

Ultra-clean isotope engineered double-walled carbon nanotubes as tailored hosts to trace the growth of carbyne

Increasing attention is currently given to carbyne, the sp1 hybridized one-dimensional carbon allotrope, because of its predicted outstanding mechanical, optical, and electrical properties. Although recently substantial progress has been reported on confined carbyne synthesized inside double-walled carbon nanotubes (DWCNTs), its formation mechanism and precursors for growth remain elusive. Here, we show a rational design of isotope engineered ultra-clean DWCNTs as tailored hosts to trace the growth of carbyne, which allows to identify the precursor and unravel the formation mechanism of carbyne during high-vacuum annealing at high-temperatures. Using this approach, ultra-clean DWCNTs with 80.4% 13C-enriched inner walls and outer tubes of naturally abundant served to unambiguously prove that only the carbonaceous materials inside the DWCNTs can act as precursors. The exchange of C atoms between inner and outer tubes happens without any growth of carbyne. After applying a secondary oxidation step, it is possible to produce the carbonaceous precursors from the partially oxidized DWCNTs. In this manner, not only carbyne with a record of ~28.8% 13C enrichment is grown, but concomitant healing, reorganization and regrowth of the DWCNTs occurs. This work enables to identify the precursor and trace the growth mechanism of confined carbyne with engineered properties. This is a crucial step, towards accessing the full application potential of confined carbyne hybrids by tailoring not only the isotopic fillers, but also the inner and outer tubes of the DWCNT hosts.

cond-mat.mtrl-sci

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

Spin-relaxation time in materials with broken inversion symmetry and large spin-orbit coupling

We study the spin-relaxation time in materials where a large spin-orbit coupling (SOC) is present which breaks the spatial inversion symmetry. Such a spin-orbit coupling is realized in zincblende structures and heterostructures with a transversal electric field and the spin relaxation is usually described by the so-called D'yakonov-Perel' (DP) mechanism. We combine a Monte Carlo method and diagrammatic calculation based approaches in our study; the former tracks the time evolution of electron spins in a quasiparticle dynamics simulation in the presence of the built-in spin-orbit magnetic fields and the latter builds on the spin-diffusion propagator by Burkov and Balents [Burkov and Balents Phys. Rev. B. 69, 245312 (2004).]. Remarkably, we find a parameter free quantitative agreement between the two approaches and it also returns the conventional result of the DP mechanism in the appropriate limit. We discuss the full phase space of spin relaxation as a function of SOC strength, its distribution, and the magnitude of the momentum relaxation rate. This allows us to identify two novel spin-relaxation regimes; where spin relaxation is strongly non-exponential and the spin relaxation equals the momentum relaxation. A compelling analogy between the spin-relaxation theory and the NMR motional narrowing is highlighted.

cond-mat.str-el

Controlled isotope arrangement in 13C enriched carbon nanotubes

We report the synthesis of a novel isotope engineered $^{13}{\rm C}$--$^{12}{\rm C}$ heteronuclear nanostructure: single-wall carbon nanotubes made of $^{13}{\rm C}$ enriched clusters which are embedded in natural carbon regions. The material is synthesized with a high temperature annealing from $^{13}{\rm C}$ enriched benzene and natural ${\rm C}_{60}$, which are co-encapsulated inside host SWCNTs in an alternating fashion. The Raman 2D line indicates that the $^{13}{\rm C}$ isotopes are not distributed uniformly in the inner tubes. A semi-empirical method based modeling of the Raman modes under $^{13}{\rm C}$ isotope enrichment shows that experimental data is compatible with the presence of $^{13}{\rm C}$ rich clusters which are embedded in a natural carbon containing matrix. This material may find applications in quantum information processing and storage using nuclear spins as qubits.

cond-mat.mtrl-sci

Anomalous hyperfine coupling and nuclear magnetic relaxation in Weyl semimetals

The electron-nuclear hyperfine interaction shows up in a variety of phenomena including e.g. NMR studies of correlated states and spin decoherence effects in quantum dots. Here we focus on the hyperfine coupling and the NMR spin relaxation time, $T_1$ in Weyl semimetals. Since the density of states in Weyl semimetals varies with the square of the energy around the Weyl point, a naive power counting predicts a $1/T_1T\sim E^4$ scaling with $E$ the maximum of temperature ($T$) and chemical potential. By carefully investigating the hyperfine interaction between nuclear spins and Weyl fermions, we find that while its spin part behaves conventionally, its orbital part diverges unusually with the inverse of energy around the Weyl point. Consequently, the nuclear spin relaxation rate scales in a graphene like manner as $1/T_1T\sim E^2\ln(E/ω_0)$ with $ω_0$ the nuclear Larmor frequency. This allows us to identify an effective hyperfine coupling constant, which is tunable by gating or doping, which is relevant for decoherence effect in spintronics devices and double quantum dots where hyperfine coupling is the dominant source of spin-blockade lifting.

cond-mat.mes-hall

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

The Elliott-Yafet theory of spin relaxation generalized for large spin-orbit coupling

We generalize the Elliott-Yafet (EY) theory of spin relaxation in metals with inversion symmetry for the case of large spin-orbit coupling (SOC). The EY theory treats the SOC to the lowest order but this approach breaks down for metals of heavy elements (such as e.g. caesium or gold), where the SOC energy is comparable to the relevant band-band separation energies. The generalized theory is presented for a four-band model system without band dispersion, where analytic formulae are attainable for arbitrary SOC for the relation between the momentum- and spin-relaxation rates. As an extended description, we also consider an empirical pseudopotential approximation where SOC is deduced from the band potential (apart from an empirical scaling constant) and the spin-relaxation rate can be obtained numerically. Both approaches recover the usual EY theory for weak SOC and give that the spin-relaxation rate approaches the momentum-relaxation rate in the limit of strong SOC. We argue that this limit is realized in gold by analyzing spin relaxation data. A calculation of the $g$-factor shows that the empirical Elliott-relation, which links the $g$-factor and spin-relaxation rate, is retained even for strong SOC.

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

Unusual spin dynamics in topological insulators

The dynamic spin susceptibility (DSS) has a ubiquitous Lorentzian form in conventional materials with weak spin orbit coupling, whose spectral width characterizes the spin relaxation rate. We show that DSS has an unusual non-Lorentzian form in topological insulators, which are characterized by strong SOC. At zero temperature, the high frequency part of DSS is universal and increases in certain directions as $ω^{d-1}$ with $d=2$ and 3 for surface states and Weyl semimetals, respectively, while for helical edge states, the interactions renormalize the exponent as $d=2K-1$ with $K$ the Luttinger-liquid parameter. As a result, spin relaxation rate cannot be deduced from the DSS in contrast to the case of usual metals, which follows from the strongly entangled spin and charge degrees of freedom in these systems. These parallel with the optical conductivity of neutral graphene.

cond-mat.str-el

The empirical Monod-Beuneu relation of spin-relaxation revisited for elemental metals

Monod and Beuneu [Monod and Beuneu, Phys. Rev. B 19, 911 (1979)] established the validity of the Elliott-Yafet theory for elemental metals through correlating the experimental electron spin resonance line-width with the so-called spin-orbit admixture coefficients and the momentum-relaxation theory. The spin-orbit admixture coefficients data were based on atomic spin-orbit splitting. We highlight two shortcomings of the previous description: i) the momentum-relaxation involves the Debye temperature and the electron-phonon coupling whose variation among the elemental metals was neglected, ii) the Elliott-Yafet theory involves matrix elements of the spin-orbit coupling (SOC), which are however not identical to the SOC induced energy splitting of the atomic levels, even though the two have similar magnitudes. We obtain the empirical spin-orbit admixture parameters for the alkali metals by considering the proper description of the momentum relaxation theory. In addition, we present a model calculation which highlights the difference between the SOC matrix element and energy splitting.

cond-mat.mes-hall