Paramagnetic State Research Articles

Origin of correlated diffuse scattering in the hexagonal manganites

We use a combination of first-principles density-functional calculations and spin-dynamics simulations to explain the unusual diffuse inelastic neutron scattering in the hexagonal multiferroic yttrium manganite, YMnO3. Using symmetry considerations, we construct a model spin Hamiltonian with parameters derived from our density-functional calculations and show that it captures the measured behavior. We then show that the observed directionality in the structured diffuse scattering in momentum space is a hallmark of the triangular geometry, and that its persistence across a wide range of temperatures, both above and below the Néel temperature TN, is a result of the strong magnetic frustration. We predict that this diffuse scattering exists in a yet-to-be-observed modulated continuum of energies, that its associated spin excitations have distinct in-plane and out-of-plane character, and that vestiges of the magnetic frustration persist into the sub−TN state. Finally, we show that visualizing the magnetic order in terms of composite trimer magnetoelectric monopoles and toroidal moments, rather than individual spins, provides insight into the real-space fluctuations, revealing clusters of emerging order in the paramagnetic state, as well as collective short-range excitations in the ordered antiferromagnetic phase. Our understanding of this directional diffuse scattering in such a wide temperature range, both below and above TN, provides new insight into the magnetic phase transitions in classical frustrated systems. Published by the American Physical Society 2024

Reentrant multiple-q magnetic order and a “spin meta-cholesteric” phase in Sr3Fe2O7

Topologically nontrivial magnetic structures such as skyrmion lattices are well known in materials lacking lattice inversion symmetry, where antisymmetric exchange interactions are allowed. Only recently, topological multi-q magnetic textures that spontaneously break the chiral symmetry, for example, three-dimensional hedgehog lattices, were discovered in centrosymmetric compounds, where they are instead driven by frustrated interactions. Here we show that the bilayer perovskite Sr3Fe2O7, previously believed to adopt a simple single-q spin-helical order, hosts two distinct types of multi-q spin textures. Its ground state represents a novel multi-q spin texture with unequally intense spin modulations at the two ordering vectors. This is followed in temperature by a new “spin meta-cholesteric” phase, in which the chiral symmetry is spontaneously broken along one of the crystal directions, but the weaker orthogonal modulation melts, giving rise to intense short-range dynamical fluctuations. Shortly before the transition to the paramagnetic state, vortex-crystal order spanned by two equivalent q vectors emerges. This renders Sr3Fe2O7 an ideal material to study transitions among multiple-q spin textures in a centrosymmetric host.

Thermal transport and spin–phonon interaction in magnetic Janus Cr2X3S3 (X = Br, I) monolayers

Comprehending the relationship between spin and phonons is essential to regulate the lattice thermal conductivity in 2D magnetic materials. Lattice thermal conductivity is a relevant part to consider in magnetic data storage and the working of spin-based devices. In this article, we examined the origin and effect of spin–phonon coupling (SPC) on the lattice thermal conductivity of pristine CrI3 monolayer-based Janus monolayers Cr2X3S3 (X=Br,I). We find a high SPC in these Janus monolayers due to in-plane Cr–S atomic vibrations. We observe a reduction in the lattice thermal conductivity at Janus monolayer magnetic states (∼52.3% in Cr2Br3S3 and ∼63.9% in Cr2I3S3) compared to its paramagnetic states. The analysis is also conducted to determine which magnetic state has more anharmonicity using potential energy wells. A wide range of 2D magnetic materials can benefit from our results in the future development of spin-based thermal devices.

Re-examination of the intumescence mechanism of fire retarded PP with APP/pentaerythritol/zeolite-4A using advanced spectroscopic techniques

The mixture of ammonium polyphosphate (APP) and pentaerythritol (PER) is a very efficient flame retardant (FR) intumescent system suitable for polyolefins such as polypropylene (PP). The mechanisms of intumescence of this FR system in this polymer was investigated using different spectroscopic techniques including continuous wave (CW) electron paramagnetic resonance (EPR) spectroscopy and solid state nuclear magnetic resonance (NMR) technique. In this work, the intumescence mechanism of PP/APP/PER formulations with and without 4A is revisited. The intumescent system was in-depth investigated using NMR, CW EPR and pulsed EPR. The CW EPR technique confirmed that free radicals are mainly generated during the intumescence of the system between 250 and 350 °C. Thanks to the pulsed EPR and solid state NMR, it was evidenced that a key structural shift from a predominantly carbonaceous residue to a predominantly phosphorated residue. Besides, it was also evidenced that zeolite 4A totally collapses during extrusion of PP/APP/PER formulations reacting with APP to generate aluminophosphates. Then, silicophosphates are generated between 350 and 400 °C. Both alumino- and silicophosphates contribute to protect aromatic structures in the residue at high temperatures.

Temperature dependence of spin transport behavior in Heusler alloy CPP-GMR

In this study, we investigate the effect of temperature on the performance of a read sensor by utilizing an atomistic model coupled with a spin transport model. Specifically, we study the temperature dependence of spin transport behavior and MR outputs in a Co2FeAl0.5Si0.5\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\ ext {Co}_2\ ext {FeAl}_{0.5}\ ext {Si}_{0.5}$$\\end{document} (CFAS)(5nm)/Cu(5nm)/CFAS(5nm) trilayer with diffusive interfaces. Initially, the two-channel model of spin-dependent resistivity is used to calculate the temperature dependence of spin transport parameters which serves as essential input for the spin accumulation model. Our findings demonstrate that as the temperature increases, the spin transport parameters and magnetic properties decrease due to the influence of thermal fluctuation. At a critical temperature, where the ferromagnet transitions to a paramagnetic state, we observe zero spin polarization. Furthermore, at elevated temperatures, the spin accumulation deviates from the equilibrium value, leading to a reduction in the magnitude of spin current and spin transport parameters due to thermal effects. As a consequence, the MR ratio decreases from 65% to 20% with increasing temperature from 0 to 400 K. Our results are consistent with previous experimental measurements. This study allows to deeply understand the physical mechanism in the reader stack which can significantly benefit reader design.

Transition-Metal-Related Quantum Emitters in Wurtzite AlN and GaN.

Transition-metal centers exhibit a paramagnetic ground state in wide-bandgap semiconductors and are promising for nanophotonics and quantum information processing. Specifically, there is a growing interest in discovering prominent paramagnetic spin defects that can be manipulated using optical methods. Here, we investigate the electronic structure and magneto-optical properties of Cr and Mn substitutional centers in wurtzite AlN and GaN. We use state-of-the-art hybrid density functional theory calculations to determine level structure, stability, optical signatures, and magnetic properties of these centers. The excitation energies are calculated using the constrained occupation approach and rigorously verified with the complete active space configuration interaction approach. Our simulations of the photoluminescence spectra indicate that in AlN and in GaN are responsible for the observed narrow quantum emission near 1.2 eV. We compute the zero-field splitting (ZFS) parameters and outline an optical spin polarization protocol for and . Our results demonstrate that these centers are promising candidates for spin qubits.

Manganese diluted TlInS2 layered semiconductor: Optical, electronic and magnetic properties

Manganese–doped TlInS2 (TlInS2+Mn) layered semiconductors with different doping concentrations of about 0.1 and 0.3 at. percent were investigated. Photo–induced current transient spectroscopy (PICTS) measurements in the temperature range of 80 and 300 K have been made for identifying energy levels related to Mn dopant within the electronic bandgap of TlInS2+Mn crystal. Optical absorption spectra in the photon energy range of ∼1.8–3.1 eV have been extracted by fitting the transmittance spectra of TlInS2+Mn recorded at the temperatures varied from ∼40–300 K. A redshift trend of the absorption edge with increasing of temperature was observed. On the other hand, a blue shift in the absorption edge with Mn doping was observed in the absorption spectra. The Mn dopant induced photoluminescence (PL) was also investigated in the visible region ranging from 320 to 960 nm. Seven peaks were observed in the PL spectra of Mn doped TlInS2 crystal in the regions both ∼960–620 nm (∼1.3–2 eV) and ∼620–320 nm (∼2–3.8 eV) due to the electronic states of Mn ions. Laser–induced breakdown spectroscopy (LIBS) technique was applied to establish of the elemental chemical composition and to confirm presence of each constituent element in TlInS2:Mn. The dc magnetization measurements of TlInS2+Mn performed in a wide temperature range of ∼5 and ∼300 K revealed different (diamagnetic and paramagnetic states) magnetic phases inside the studied temperature range. The X–band electron paramagnetic resonance (ESR) experiments were carried out in the low–temperature phase of TlInS2+Mn to probe the structure of Mn centers in TlInS2. The measurements revealed that the ESR spectrum changes drastically in the low–temperature phase of TlInS2+Mn bulk sample. Finally, a detailed density functional theory (DFT) based computational investigation of electronic band structures, density of states and optical properties of TlInS2+Mn compound has been performed. The results of ab–initio calculations are discussed for three possible states when the manganese atom was doped by replacing either the Tl, In or S atoms in the unit cell of TlInS2. Additionally, the effect of interstitial Mn dopant on the electronic structure and optical properties of TlInS2 material has been simulated.

Magneto-chemical effects in the elastic properties of Co3Al-based compounds

The thermodynamic and mechanical properties of the L12Co3Al type of compounds are fundamental for understanding and designing Co-based superalloys. In these systems, both compositional and magnetic changes can occur upon service due to the elevated temperature. Here, using first-principle calculations, we study the bulk properties of three families of Co3Al-based compounds: (Co1−xNix)3Al (0⩽x⩽0.5), Co3(Al1−yWy) (0⩽y⩽1), and (Co0.5Ni0.5)3(Al0.5TizTa0.5−z) (0⩽z⩽0.5). The calculated lattice constants, Curie temperatures, and formation energies show good agreement with the limited available theoretical and experimental data. Our results reveal the impact of chemistry and magnetism on the elastic parameters. We find that both chemical composition and magnetic state alter the elastic parameters and the elastic anisotropy, which in turn makes the predictions based on common ductile–brittle criteria challenging. We separate the volume and chemical effects for both ferromagnetic and paramagnetic states and show that in most cases, the chemical effect gives the dominant contribution to the alloying trends in the elastic parameters. The present findings reveal the complex relationship between alloying elements and elastic parameters in the Co3Al-based precipitates, providing insights into their mechanical properties for engineering applications.

Compact Electron Paramagnetic Resonance on a Chip Spectrometer Using a Single Sided Permanent Magnet.

Electron paramagnetic resonance (EPR) spectroscopy provides information about the physical and chemical properties of materials by detecting paramagnetic states. Conventional EPR measurements are performed in high Q resonator using large electromagnets which limits the available space for operando experiments. Here we present a solution toward a portable EPR sensor based on the combination of the EPR-on-a-Chip (EPRoC) and a single-sided permanent magnet. This device can be placed directly into the sample environment (i.e., catalytic reaction vessels, ultrahigh vacuum deposition chambers, aqueous environments, etc.) to conduct in situ and operando measurements. The EPRoC reported herein is comprised of an array of 14 voltage-controlled oscillator (VCO) coils oscillating at 7 GHz. By using a single grain of crystalline BDPA, EPR measurements at different positions of the magnet with respect to the VCO array were performed. It was possible to create a 2D spatial map of a 1.5 mm × 5 mm region of the magnetic field with 50 μm resolution. This allowed for the determination of the magnetic field intensity and homogeneity, which are found to be 254.69 mT and 700 ppm, respectively. The magnetic field was mapped also along the vertical direction using a thin film a-Si layer. The EPRoC and permanent magnet were combined to form a miniaturized EPR spectrometer to perform experiments on tempol (4-hydroxy-2,2,6,6-teramethylpiperidin-1-oxyl) dissolved in an 80% glycerol and 20% water solution. It was possible to determine the molecular tumbling correlation time and to establish a calibration procedure to quantify the number of spins within the sample.

Transition from ferromagnetic to noncollinear to paramagnetic state with increasing Ru concentration in FeRu films

Transition from ferromagnetic to noncollinear to paramagnetic state with increasing Ru concentration in FeRu films

Weak-coupling theory of magic-angle twisted bilayer graphene

Strong correlations occur in magic-angle twisted bilayer graphene (MATBG) when the octet of flat moiré minibands centered on charge neutrality (CN) is partially occupied. The octet consists of a single valence band and a single conduction band for each of four degenerate spin-valley flavors. Motivated by the importance of Hartree electrostatic interactions in determining the filling-factor-dependent band structure, we use a time-dependent Hartree approximation to gain insight into electronic correlations. We find that the electronic compressibility is dominated by Hartree interactions, that paramagnetic states are stable over a range of density near CN, and that the dependence of energy on flavor polarization is strongly overestimated by mean-field theory. Published by the American Physical Society 2024

Magnetic excitation in the hyperkagome antiferromagnet Mn3RhSi

In a paramagnetic state of a hyperkagome lattice antiferromagnet Mn3RhSi, magnetic diffuse scattering by magnetic short-range order is observed over a wide temperature range of approximately 500 K above the Néel temperature of 190 K. We have studied the magnetic excitation with a single crystal in a wide energy range from 0.3 to 140 meV by inelastic neutron scattering, where the prominent inelastic neutron-scattering signal is observed at Q=(2,0,0). The inelastic scattering intensity integrated for two of twelve magnon modes leads to a localized magnetic moment of about 5 μB per Mn site, although the long-range ordered magnetic moment is only 2.61 μB at 4 K. The result suggests that a large part of the magnetic moment does not order in Mn3RhSi, possibly due to the geometrical spin frustration of the hyperkagome lattice. Published by the American Physical Society 2024

The impact of cobalt oxide additions and heat treatment on wollastonite for magnetic applications

Magnetic nanocomposite was prepared using the wet chemical precipitation approach with varying amounts of cobaltous oxide (CoO). The concentrations of CoO were 0.5, 3.5, 6.5, and 9.5 g per 100 % wollastonite composition. Samples were sintered separately at 1000 and 1200 °C. X-ray diffraction analysis (XRD) of the sintered parent sample revealed the formation of wollastonite CaSiO3 and larnite Ca2SiO4, as well as a minor silicon oxide SiO2 phase. In CoO-doped samples, Co-åkermanite Ca2CoSi2O7 and other phases were formed. The XRD and scanning electron microscope SEM confirm the samples' submicron and nanocrystalline microstructure. The Fourier transform infrared spectroscopy (FTIR) and Raman spectra (RS) of investigated samples sintered at 1000 and 1200 °C revealed their bond structure. Both analyses confirmed that incorporating CoO into CaSiO3 significantly improved its vibrational modes, reflecting structural modifications. By increasing the cobalt oxide content from 3.5 to 9.5 wt%, the samples attain the ideal paramagnetic state, as demonstrated by the magnetic hysteresis (M − H) curve, which is linearly reversible. Formation of the Ca2CoSi2O7 significantly alters the magnetic characteristics of the samples, whether through increasing the cobalt oxide concentration up to 9.5 wt% or modifying the sintering temperature. This enables the prepared nonocomposites to be suitable for novel magnetic applications.

Finite Temperature Magnetism in the Triangular Lattice Antiferromagnet KErTe2

Abstract After the discovery of the ARECh2 (A = alkali or monovalent ions, RE = rare-earth, Ch = chalcogen) triangular lattice quantum spin liquid (QSL) family, a series of its oxide, sulfide, and selenide counterparts has been consistently reported and extensively investigated. While KErTe2 represents the initial synthesized telluride member, preserving its triangular spin lattice, it was anticipated that the substantial tellurium ions could impart more pronounced magnetic attributes and electronic structures to this material class. This study delves into the magnetism of KErTe2 at finite temperatures through magnetization and electron spin resonance (ESR) measurements. Based on the angular momentum J ^ after spin-orbit coupling (SOC) and symmetry analysis, we obtain the magnetic effective Hamiltonian to describe the magnetism of Er3+ in R 3 ¯ m space group. Applying the mean-field approximation to the Hamiltonian, we can simulate the magnetization and magnetic heat capacity of KErTe2 in paramagnetic state and determine the crystalline electric field (CEF) parameters and partial exchange interactions. The relatively narrow energy gaps between the CEF ground state and excited states exert a significant influence on the magnetism. For example, small CEF excitations can result in a significant broadening of the ESR linewidth at 2 K. For the fitted exchange interactions, although the values are small, given a large angular momentum J = 15/2 after SOC, they still have a noticeable effect at finite temperatures. Notably, the heat capacity data under different magnetic fields along the c axis direction also roughly match our calculated results, further validating the reliability of our analytical approach. These derived parameters serve as crucial tools for future investigations into the ground state magnetism of KErTe2. The findings presented herein lay a foundation for exploration of the intricate magnetism within the triangular-lattice delafossite family.

Data-driven design of high-curie temperature full-heusler alloys for spintronic applications

In this study, we employ density functional theory (DFT) and subgroup discovery (SGD) to explore the structural and magnetic properties of full cubic Heusler compounds, with a particular emphasis on their Curie temperatures (Tc) and magnetic stability. Our comprehensive examination of 2903 structures across both L21 and Xa phases identifies configurations that exhibit both structural stability and superior magnetic properties. Notable among these, compounds such as Co2MnSi, Co2CrGe, and Cr2VGe exhibit remarkable magnetic stability, maintaining their ferromagnetic properties well above room temperature. Co2MnSi displays a substantial magnetic moment of 5.00 μB and maintains its ferromagnetic properties up to a Curie temperature of 937 K, underscoring its suitability for high-temperature applications. Similarly, Co2CrGe, with a magnetic moment of 4.00 μB, transitions to a paramagnetic state at a higher temperature of 952 K, demonstrating enhanced thermal durability. Moreover, Cr2VGe, notable for its robust magnetic moment of 2.81 μB, retains its ferromagnetic characteristics until an exceptional 2412 K, making it extremely valuable for thermally intensive environments. These findings underscore the potential of these materials in developing durable and efficient spintronic devices that operate under extreme thermal conditions. By mapping the interplay between electronic structure and magnetic properties, our study provides a predictive framework for optimizing the performance of spintronic materials.

Contrasting Magnetic Characteristics of Disordered Nd0.5Ba0.5Mn0.5Fe0.5O3-δ/2 and 112-Type Ordered NdBaMnFeO6-δ Perovskites.

The magnetic properties of disordered Nd0.5Ba0.5Mn0.5Fe0.5O3-δ/2 and ordered NdBaMnFeO6-δ perovskites were investigated through temperature- and field-dependent DC-magnetization measurements. The temperature dependence of magnetic susceptibilities revealed that antiferromagnetic ordering occurs at temperatures below 185 K for the disordered Nd0.5Ba0.5Mn0.5Fe0.5O3-δ/2 sample, whereas the ordered NdBaMnFeO6-δ perovskite exhibited a paramagnetic state throughout the entire temperature range examined. Notably, the disordered sample exhibited a glassy state, even at room temperature, which transformed into an antiferromagnetic state under higher applied magnetic fields. The magnetic ordering in the disordered Nd0.5Ba0.5Mn0.5Fe0.5O3-δ/2 perovskite and the magnetic-disordering state in the structurally ordered NdBaMnFeO6-δ perovskite could be attributed to the alteration of the oxidation state of Mn.

Correlated normal state fermiology and topological superconductivity in UTe2

UTe2 is a promising candidate for spin-triplet superconductors, in which a paramagnetic normal state becomes superconducting due to spin fluctuations. Here, we theoretically show that electron correlation induces a dramatic change in the normal state fermiology with an emergent correlated Fermi surface (FS) driven by Kondo resonance at low temperatures. This emergent correlated FS can account for various unconventional superconducting properties in a unified way. In particular, the geometry of the correlated FS can naturally host topological superconductivity in the presence of odd-parity pairings, which become the leading instability due to strong ferromagnetic spin fluctuations. Moreover, two pairs of odd-parity channels appear as nearly degenerate solutions which may lead to time-reversal breaking multicomponent superconductivity. The resulting time-reversal-breaking superconducting state is a Weyl superconductor in which Weyl points migrate along the correlated FS as the relative magnitude of nearly degenerate pairing solutions varies.

Conductive single-phase SrMoO3 epitaxial films synthesized in pure Ar ambience via plasma-assisted radio frequency sputtering

ABSTRACT The cubic perovskite SrMoO3 with a paramagnetic ground state and remarkably low room-temperature resistivity has been considered as a suitable candidate for the new-era oxide-based technology. However, the difficulty of preparing single-phase SrMoO3 thin films by hydrogen-free sputtering has hindered their practical use, especially due to the formation of thermodynamically favorable SrMoO4 impurity. In this work, we developed a radio frequency sputtering technology enabling the reduction reaction and achieved conductive epitaxial SrMoO3 films with pure phase from a SrMoO4 target in a hydrogen-free, pure argon environment. We demonstrated the significance of controlling the target-to-substrate distance (TSD) on the synthesis of SrMoO3; the film resistivity drastically changes from 1.46 × 105 μΩ·cm to 250 μΩ·cm by adjusting the TSD. Cross-sectional microstructural analyses demonstrated that films with the lowest resistivity, deposited for TSD = 2.5 cm, possess a single-phase SrMoO3 with an epitaxial perovskite structure. The formation mechanism of the conductive single-phase SrMoO3 films can be attributed to the plasma-assisted growth process by tuning the TSD. Temperature-dependent resistivity and Hall effect studies revealed metal-like conducting properties for low-resistive SrMoO3 films, while the high-resistive ones displayed semiconductor-like behavior. Our approach makes hydrogen-free, reliable and cost-efficient scalable deposition of SrMoO3 films possible, which may open up promising prospects for a wide range of future applications of oxide materials.

Magnetic instability in the spin susceptibility of chiral carbon-based structures

Chiral carbon nanostructures have been found to display unexpected magnetic behaviors. Several theoretical calculations performed in the macroscopic limit q=0 have addressed or predicted some of these findings. To gain more insight into the magnetism of these systems at finite q, here we use linear response theory to calculate the wave-vector-dependent spin susceptibility χ(q,0) in a half-filling tight-binding model of a helix of carbon atoms with intrinsic spin-orbit coupling (SOC). We find that at the nesting wave number q=2kF the paramagnetic state of the system is unstable with respect to the formation of a spin-density-wave type state. Chirality has a small effect on the paramagnetic phase but has no impact on the spin-density-wave type state. Published by the American Physical Society 2024

Cryogenic temperature magnetocaloric effect and critical behavior of GdDyErAlM (M=Fe, Co, Ni) high entropy amorphous alloys

High entropy amorphous alloys (HE AMs) have attracted extensive interest lately due to their superior magnetocaloric properties. However, the critical behavior and mechanical properties have received less research, which restricts their applications. This work presented a comprehensive investigation of the magnetocaloric effect (MCE), critical behavior, and mechanical performance of quinary Gd20Dy20Er20Al20M20 (M = Fe, Co, Ni) HE AMs. All samples exhibited distinct spin glass-like behavior below TC and competitive MCE around hydrogen liquefaction temperature range. Excellent MCE was achieved by the HE AMs through a second-order phase transition from paramagnetic state to ferromagnetic state at 79 K for Fe, 41 K for Co, and 36 K for Ni. Among them, the maximum magnetic entropy change (-ΔSM)max of Gd20Dy20Er20Al20Co20 amorphous alloys was 9.59 J kg−1 K−1 under 0–5 T. Furthermore, RC and RCP of Gd20Dy20Er20Al20Fe20 amorphous alloys were respectively 519 J kg−1 and 613 J kg−1, larger than that of most RE-based amorphous alloys. For all samples, the critical behavior of the phase transition approached the mean field model, and this responded to the long-range ordering of the magnetic interaction. The bending plasticity of Gd20Dy20Er20Al20M20 (M = Fe, Co, Ni) HE AMs were 0.78, 1.03, 0.89, respectively. The adjustable Tc, large (-ΔSM), high RCP, and outstanding mechanical properties suggested Gd20Dy20Er20Al20M20 (M = Fe, Co, Ni) HE AMs may find utility as magnetic refrigerants in low-temperature applications.