A long spin‐lifetime of electrons is the holy grail of spintronics, a field exploiting the electron angular momentum as an information carrier and storage unit. Previous reports indicated a spin lifetime, τ s near 10 ns at best in graphene‐based devices at low temperatures. The observation of τ s approaching the ultralong 1,000 ns at room temperature in natural graphite crystals is detailed 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 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.
Time-resolved photoconductivity is widely used to characterize non-equilibrium charge-carrier lifetime, impurity content, and solar cell efficiency in a broad range of semiconductors. Most measurements are limited to the detection of reflection of electromagnetic radiation at a single frequency and a single photoexciting light wavelength. We present a time-resolved photoconductivity instrument that enables broadband frequency detection (essentially from DC to 100 GHz), temperature-dependent measurements, and multiple excitation photon energy. The measurement is realized with the help of a coplanar waveguide, which acts as an efficient antenna and whose performance was tested over 10 MHz-10 GHz. The instrument enables the study of surface and bulk charge-recombination specific processes.
The synthesis of silicon carbide has been widely explored to tailor its material properties for specific needs, particularly particle size, polytype distribution, and defect density. While many applications require defect-free material, the intrinsic defect states in SiC make it an attractive candidate for quantum technologies. However, the controlled introduction of such defects remains a major challenge. In this work, we investigate the influence of aluminium concentration and high-energy ball milling duration on defect formation and polytype distribution in silicon carbide synthesized through controlled thermal reactions. Our findings highlight the critical role of Al in altering the reaction between Si and C, stabilizing specific polytypes, and promoting the formation of optically and magnetically active point defects. Multivariate analysis using machine learning-assisted partial least squares regression revealed strong correlations between structural parameters and defect concentrations. These results demonstrate that optimizing Al concentration and milling conditions enables controlled synthesis of SiC with tailored polytypism and targeted defect configurations, presenting a scalable route for quantum technological applications.
Plastic waste, one of the most critical problems for humankind, poses severe threats to ecosystems, wildlife, and human health. Tracing, quantifying, and identifying types of plastic waste are crucial to understanding its environmental pathways and developing targeted strategies for reduction, recycling, and remediation. To contribute to addressing this global issue, we investigated the spin-labeling capabilities of chlorine dioxide (ClO2) radicals introduced 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, certain degrees of freedom remain restricted 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
MXenes combine widely tunable electronic properties with promising chemical agility, yet Ti3C2Tx, the most studied member of this family, exhibits puzzling electronic and magnetic anomalies near room temperature. Here, we show that these effects arise from self-formed titanium suboxide domains, predominantly Ti3O5, stabilized within the MXene galleries. Employing comprehensive in situ structural, spectroscopic, thermodynamic, and transport analyses, we identify subtle but reproducible transitions at K and K. Raman microscopy and X-ray diffraction were used to track Ti3O5 polymorphism, while thermodynamic and transport signatures coincide with known transformations. Electron paramagnetic resonance reveals a marked anomaly in the Dysonian diffusion parameter without a considerable change in spin susceptibility, indicating reconfigured electronic pathways rather than carrier loss. These results reframe Ti3C2Tx as an inherently composite MXene-oxide system whose functional response is governed by minority suboxide phases. Beyond resolving a field-wide controversy, controlled oxidation emerges as a design lever to engineer phase-change behavior for thermal latching, opto-thermal switching, and robust, near-room-temperature MXene devices.
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_2C_2O_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 ^∘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.
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.
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$_2$.
Ti3C2Tx is a leading compound within the MXenes family and can find host in widespread applications. It is synthesized by selectively etching layers from the Ti3AlC2 precursor, and this process typically introduces surface terminations, Tx, 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. Herein, a two‐step oxidation process is revealed during heat treatment, where initial oxidation occurs between layers without altering the integrity of the Ti3C2‐layered structure, followed by the formation of anatase TiO2 at elevated temperatures. The process is carefully monitored using in situ Raman spectroscopy and in situ microwave conductivity measurements, applied to Ti3C2Tx prepared using various etching techniques involving concentrated hydrofluoric acid, LiF + HCl, and HF + HCl mixtures. The oxidation process is heavily influenced by the synthesis route and surface chemistry of Ti3C2Tx, 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 TiO2.
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.
The measurement and description of the charge-carrier lifetime (τc) is crucial for the wide-ranging applications of lead-halide perovskites. We present time-resolved microwave-detected photoconductivity decay (TRMCD) measurements and a detailed analysis of the possible recombination mechanisms including trap-assisted, radiative, and Auger recombination. We prove that performing injection-dependent measurement is crucial in identifying the recombination mechanism. We present temperature and injection level dependent measurements in CsPbBr3, which is the most common inorganic lead-halide perovskite. In this material, we observe the dominance of charge-carrier trapping, which results in ultra-long charge-carrier lifetimes. Although charge trapping can limit the effectiveness of materials in photovoltaic applications, it also offers significant advantages for various alternative uses, including delayed and persistent photodetection, charge-trap memory, afterglow light-emitting diodes, quantum information storage, and photocatalytic activity.
Coherent light sources emitting in the terahertz range are highly sought after for fundamental research and applications. Terahertz lasers rely on achieving population inversion. We demonstrate the generation of terahertz radiation using nitrogen-vacancy centers in a diamond single crystal. Population inversion is achieved through the Zeeman splitting of the S = 1 state in 15 tesla, resulting in a splitting of 0.42 terahertz, where the middle Sz = 0 sublevel is selectively pumped by visible light. To detect the terahertz radiation, we use a phase-sensitive terahertz setup, optimized for electron spin resonance (ESR) measurements. We determine the spin-lattice relaxation time up to 15 tesla using the light-induced ESR measurement, which shows the dominance of phonon-mediated relaxation and the high efficacy of the population inversion. The terahertz radiation is tunable by the magnetic field, thus these findings may lead to the next generation of tunable coherent terahertz sources.
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 Néel 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 and 13.5 nm diameter magnetite nanoparticles suspended in water. We identify clear fingerprints of Brownian relaxation for the sample of 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 Brownian relaxation. This peak vanishes below 273 K.
Understanding the recombination lifetime of charge carriers () is essential for the diverse applications of photovoltaic materials, such as perovskites. The study on the inorganic perovskite, CsPbBr 3 , reveals recombination dynamics exceeding 1 ms below 200 K and approaching 100 μs at room temperature. Utilizing time‐resolved microwave‐detected photoconductivity decay in conjunction with injection dependence, it is found that is dominated by impurity charge trapping. The observed injection dependence is well corroborated by modeling of the trap mechanism. The ultralong decay time is also consistent with photoconductivity measurements with a continuous‐wave excitation at powers corresponding to around 1 Sun irradiation. While charge‐carrier trapping may, in theory, impose limitations on the photovoltaic efficiency of single‐cell devices, it can also contribute to increased efficiency in tandem cells and find applications in photodetection, photocatalysis, and quantum information storage.
Knowledge of the charge-carrier recombination lifetime, tau, is crucial for the various applications of photovoltaic perovskites. We studied the novel inorganic perovskite, CsPbBr3 and we observe recombination dynamics beyond 1 ms below 200 K and tau approaching 100 us at room temperature. Time-resolved microwave-detected photoconductivity decay (TRMCD), used in combination with injection dependence, evidence that tau is dominated by impurity charge trapping. The observed injection dependence is well corroborated by modeling of the trap mechanism. The ultra-long decay time is also consistent with photoconductivity measurements with a continuous-wave excitation at powers corresponding to around one Sun irradiation. While in principle charge-carrier trapping may limit the photovoltaic efficiency in single-cell photovoltaic devices, it could also lead to enhanced efficiency in tandem cells as well as for alternative applications including photodetection and quantum information storage.
Graphite has been intensively studied, yet its electron spins dynamics remains an unresolved problem even 70 years after the first experiments. The central quantities, the longitudinal ( T 1 ) and transverse ( T 2 ) relaxation times were postulated to be equal, mirroring standard metals, but T 1 has never been measured for graphite. Here, based on a detailed band structure calculation including spin-orbit coupling, we predict an unexpected behavior of the relaxation times. We find, based on saturation ESR measurements, that T 1 is markedly different from T 2 . Spins injected with perpendicular polarization with respect to the graphene plane have an extraordinarily long lifetime of 100 ns at room temperature. This is ten times more than in the best graphene samples. The spin diffusion length across graphite planes is thus expected to be ultralong, on the scale of ~ 70 μ m, suggesting that thin films of graphite — or multilayer AB graphene stacks — can be excellent platforms for spintronics applications compatible with 2D van der Waals technologies. Finally, we provide a qualitative account of the observed spin relaxation based on the anisotropic spin admixture of the Bloch states in graphite obtained from density functional theory calculations.
Abstract DNA mismatch repair (MMR) corrects mismatched DNA bases arising from multiple sources including polymerase errors and base damage. By detecting spontaneous mutagenesis using whole genome sequencing of cultured MMR deficient human cell lines, we show that a primary role of MMR is the repair of oxygen-induced mismatches. We found an approximately twofold higher mutation rate in MSH6 deficient DLD-1 cells or MHL1 deficient HCT116 cells exposed to atmospheric conditions as opposed to mild hypoxia, which correlated with oxidant levels measured using electron paramagnetic resonance spectroscopy. The oxygen-induced mutations were dominated by T to C base substitutions and single T deletions found primarily on the lagging strand. A broad sequence context preference, dependence on replication timing and a lack of transcriptional strand bias further suggested that oxygen-induced mutations arise from polymerase errors rather than oxidative base damage. We defined separate low and high oxygen–specific MMR deficiency mutation signatures common to the two cell lines and showed that the effect of oxygen is observable in MMR deficient cancer genomes, where it best correlates with the contribution of mutation signature SBS21. Our results imply that MMR corrects oxygen-induced genomic mismatches introduced by a replicative process in proliferating cells.
Silicon carbide (SiC) is a very promising platform for quantum information processing, as it can host room temperature solid state defect quantum bits. These room temperature quantum bits are realized by paramagnetic silicon vacancy and divacancy defects in SiC that are typically introduced by irradiation techniques. However, irradiation techniques often introduce unwanted defects near the target quantum bit defects that can be detrimental for the operation of quantum bits. Here, we demonstrate that by adding aluminum precursor to the silicon and carbon sources, quantum bit defects are created in the synthesis of SiC without any post treatments. We optimized the synthesis parameters to maximize the paramagnetic defect concentrations—including already established defect quantum bits—monitored by electron spin resonance spectroscopy.
Raw data for MS entitled "Ultralong 100 ns Spin Relaxation Time in Graphite at Room Temperature" in Origin files.