Long-range magnetic order in hydroxide-layer-doped (Li[subscript 1;#8722;x;#8722;y]FexMn[subscript y]OD)FeSe
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CrMnFeCoNi, also called the Cantor alloy, is a well-known high-entropy alloy whose magnetic properties have recently become a focus of attention. Here, we present a detailed muon spin relaxation study of the influence of chemical composition and sample processing protocols on the magnetic phase transitions and spin dynamics of several different Cantor alloy samples. Specific samples studied include a pristine equiatomic sample, samples with deficient and excess Mn content, and equiatomic samples magnetized in a field of 9 T or plastically deformed in pressures up to 0.5 GPa. The results confirm the sensitive dependence of the transition temperature on composition and demonstrate that post-synthesis pressure treatments cause the transition to become significantly less homogeneous throughout the sample volume. In addition, we observe critical spin dynamics in the vicinity of the transition in all samples, reminiscent of canonical spin glasses and magnetic materials with ideal continuous phase transitions. Application of an external magnetic field suppresses the critical dynamics in the Mn-deficient sample, while the equiatomic and Mn-rich samples show more robust critical dynamics. The spin-flip thermal activation energy in the paramagnetic phase increases with Mn content, ranging from 3.1(3) × 10 -21 J for 0% Mn to 1.2(2) × 10 -20 J for 30% Mn content. These results shed light on critical magnetic behavior in environments of extreme chemical disorder and demonstrate the tunability of spin dynamics in the Cantor alloy via chemical composition and sample processing.
For this study, perovskite nickelate heterostructures consisting of single unit cells of EuNiO 3 and LaNiO 3 have been grown on a set of single crystalline substrates by pulsed laser interval deposition to investigate the effect of epitaxial strain on electronic and magnetic properties at the extreme interface limit. Despite the variation of substrate in-plane lattice constants and lattice symmetry, the structural response to heterostructuring is primarily controlled by the presence of the EuNiO 3 layer. In sharp contrast to bulk LaNiO 3 or EuNiO 3 , the superlattices grown under tensile strains exhibit metal-to-insulator transitions (MIT) below room temperature. The onset of magnetic and electronic transitions associated with the MIT can be further separated by application of large tensile strain. Furthermore, these transitions can be entirely suppressed by very small compressive strain. X-ray resonant absorption spectroscopy measurements reveal that such strain-controlled MIT is directly linked to a strain-induced self-doping effect without any chemical doping.
The hexagonal CaCu 5 –type structure (P6/mmm) is the prototype for more than 100 ternary borides, gallides, and silicides, with general stoichiometry of RTM 3 X 2 (R=lanthanide/alkaline earth; TM=transition metal; X=B, Ga, Si, Ge). Here we report the synthesis, crystal structure, and bulk magnetic properties of polycrystalline and single crystal samples of EuPd 3 Si 2 and its nonmagnetic analog SrPd 3 Si 2 . Both compounds crystallize in the orthorhombic space group symmetry Imma (no. 74, Z = 2, oI12) displaying pseudohexagonal symmetry. Ferromagnetic (FM) order of Eu 2+ at T C1 =78K and a spin-reorientation transition at T C2 =5K appear as distinctive features in bulk magnetization, specific heat, and resistivity/resistance measurements. Neutron powder diffraction measurements on EuPd 3 Si 2 confirm FM order of the Eu 2+ spins below T C1 , with the spins aligned along the a axis below T C2 . Electronic band structure calculations corroborate the crystal structure and the FM state for EuPd 3 Si 2 , with a Pd d–band polarization in the same direction as the Eu 4f polarization, enhancing the observed spin moment.
Abstract not provided.
In this paper, we present the fabrication of nano-magnet arrays, comprised of two sets of interleaving SmCo 5 and Co nano-magnets, and the subsequent development and implementation of a protocol to program the array to create a one-dimensional rotating magnetic field. We designed the array based on the microstructural and magnetic properties of SmCo 5 films annealed under different conditions, also presented here. Leveraging the extremely high contrast in coercivity between SmCo 5 and Co, we applied a sequence of external magnetic fields to program the nano-magnet arrays into a configuration with alternating polarization, which based on simulations creates a rotating magnetic field in the vicinity of nano-magnets. Our proof-of-concept demonstration shows that complex, nanoscale magnetic fields can be synthesized through coercivity contrast of constituent magnetic materials and carefully designed sequences of programming magnetic fields.
Spin-forbidden (Δ𝑆 ≠0) multiplet excitations and their coupling to magnetic properties are of increasing importance for magneto-optical studies of correlated materials. Nonetheless, the mechanisms for optically brightening these transitions and their generality remain poorly understood. Here, we report magnetic circular dichroism (MCD) spectroscopy on the van der Waals ferromagnet (FM) CrI 3 . Previously unreported spin-forbidden (Δ𝑆 =1) 4 𝐴 2g → 2 𝐸 g / 2 𝑇 1g Cr 3+ 𝑑𝑑 excitations are observed near the ligand-to-metal charge-transfer excitation threshold. The assignment of these excitations and their Cr 3+ multiplet character is established through complementary Cr 𝐿 3 -edge resonant inelastic x-ray scattering measurements along with charge-transfer multiplet calculations and chemical trends in the chromium trihalide series (Cr𝑋 3 , 𝑋 = Cl, Br, I). We utilize the high sensitivity of MCD spectroscopy to study the thickness-dependent optical response. The spin-forbidden excitations remain robust down to the monolayer limit, and we observe a significant magnetic-field dependence of the MCD spectrum across the antiferromagnetic-to-FM transition in few-layer samples. We preliminarily attribute this behavior to changes in the metal-ligand covalency with magnetic state. Our results clarify the magneto-optical response of CrI 3 and identify covalency as a central mechanism for the brightening and field tunability of spin-forbidden multiplet excitations.
We report that heterostructures made from topological and magnetic insulators promise to form excellent platforms for new electronic and spintronic functionalities mediated by interfacial effects. We report the results of a first-principles density functional theory study of the geometric, electronic structure, and magnetic properties of the EuS( 111 )/Bi 2 Se 3 interface, including van der Waals and relativistic spin-orbit effects. In contrast to previous theoretical studies, we find no appreciable magnetic anisotropy in such a heterostructure. We also do not see additional induced magnetization at the interface or the magnetic proximity effect on the topological states. This is due to the localized nature of Eu moments and because of a partial charge transfer of ~ 0.5 electron from Eu to Se. The formation of the surface dipole shifts the Dirac cone about 0.4 eV below the chemical potential, and the associated electrostatic screening moves the topological state from the first to the second quintuple layer of Bi 2 Se 3 .
Beyond its fascinating chemistry as the first element in the Periodic Table, hydrogen is of high societal importance in energy technologies and of growing importance in energy-efficient computing. In energy, hydrogen has reemerged as a potential solution to long-term energy storage and as a carbon-free input for materials manufacturing. Its utilization and production rely on the availability of proton-conducting electrolytes and mixed proton–electron conductors for the components in fuel cells and electrolyzers. In computing, proton mediation of electronic properties has garnered attention for electrochemically controlled energy-efficient neuromorphic computing. Incorporation of substitutional and interstitial hydride ions in oxides, though only recently established, enables tuning of electronic and magnetic properties, inviting a range of possible exotic applications. This article addresses common themes in the fundamental science of hydrogen incorporation and transport in oxides as relevant to pressing technological needs. The content covers (1) lattice (or bulk) mechanisms of hydrogen transport, primarily addressing proton transport, but also touching on hydride ion transport; (2) interfacial transport; (3) exploitation of extreme external drivers to achieve unusual response; and (4) advances in methods to probe the hydrogen environment and transport pathway. The snapshot of research activities in the field of hydrogen-laden materials described here underscores exciting recent breakthroughs, remaining open questions, and breathtaking experimental tools now available for unveiling the nature of hydrogen in solid-state matter.
Multifunctional iron oxide-gold hybrid nanostructures have been produced via solution chemistries and investigated for analyte detection. Gold nanoparticles of various shapes have been used for probing surface-enhanced Raman scattering (SERS) effects as they display unique optical properties in the visible-near IR region of the spectrum. When coupled with other nanoparticles, namely iron oxide nanoparticles, hybrid structures with increased functionality were produced. By exploiting their magnetic properties, nanogaps or “hot spots” were rationally created and evaluated for SERS enhancement studies. The “hot spots” were created by using a seeded reaction to increase the gold loading on the iron oxide support by 43% by weight. SERS Nanomaterials were evaluated for their ability to promote surface-enhanced Raman scattering of a model analyte, 4-mercaptophenol. The data shows an enhancement effect of the model analyte on gold decorated iron oxide nanoparticles.
Single-crystal iron oxide nanorings have been proposed as a promising candidate for magnetic hyperthermia application because of their unique shape-induced vortex-domain structure, which supports good colloidal stability and enhanced magnetic properties. However, the synthesis of single crystalline iron oxide has proven to be challenging. In this article, we showed that chemically synthesized multigrain magnetite nanorings disfavor a shape-induced magnetic vortex-domain structure. Our results indicate that the multigrain Fe 3 O 4 nanorings with an average outer diameter of ~110 nm and an inner to outer diameter ratio of ~0.5 do not show a shape-induced vortex-domain structure, which was observed in the single-crystal Fe 3 O 4 nanorings of similar dimensions. At 300 Ks, multigrain magnetite nanorings showed an effective anisotropy field of 440 Oe, which can be attributed to its high surface area and intraparticle interaction. Both calorimetric and AC loop measurements showed a moderate inductive heating efficiency of multigrain magnetite nanorings of ~300 W/g at 800 Oe. Our results shed light on the magnetic ground states of chemically synthesized multigrain Fe 3 O 4 nanorings.
The quantum Hall effect (QHE) is traditionally considered to be a purely two-dimensional (2D) phenomenon. Recently, however, a three-dimensional (3D) version of the QHE was reported in the Dirac semimetal ZrTe 5 . It was proposed to arise from a magnetic-field-driven Fermi surface instability, transforming the original 3D electron system into a stack of 2D sheets. Here, we report thermodynamic, spectroscopic, thermoelectric and charge transport measurements on such ZrTe 5 samples. The measured properties: magnetization, ultrasound propagation, scanning tunneling spectroscopy, and Raman spectroscopy, show no signatures of a Fermi surface instability, consistent with in-field single crystal X-ray diffraction. Instead, a direct comparison of the experimental data with linear response calculations based on an effective 3D Dirac Hamiltonian suggests that the quasi-quantization of the observed Hall response emerges from the interplay of the intrinsic properties of the ZrTe 5 electronic structure and its Dirac-type semi-metallic character.
For the integration with other parts of spintronic devices, it is desired to minimize the size of skyrmions to a nanometer scale. To provide a theoretical guidance for this endeavour, we established an extended NdJ relationship between the skyrmion size and fundamental magnetic properties of two-dimensional hexagonal ferromagnetic lattices, including multiple exchanges between different neighbors (J 1 -J 4 ), Dzyaloshinskii-Moriya interactions (d 1 and d 2 ) and on-site magnetic anisotropy energy. We demonstrated the applicability of this approach through density functional theory and spin spiral calculations for several interface, e.g., Co/Gra, Rh/Gra, Co/Pt 3 and MgO/Co/Pt 3 , and showed that the size of Néel skyrmions can be effectively reduced by either enhancing d or more conveniently reducing J through cancelation of J i s.
We report hybrid and all-inorganic, vacancy-ordered double perovskites of d 2 W 4+ with the formula A 2 WCl 6 (A = CH 3 NH 3 + , Rb + , and Cs + ). These compounds, which are reddish in color, can be distinguished from structurally similar compounds obtained by hydrothermal methods on the basis of structure, spectroscopic, and magnetic properties. The latter are green and incorporate oxygen, with the actual formula Cs 2 WO x Cl 6–x and distinct optical absorption and emission behavior. Furthermore, the local-moment magnetism of the pure-red d 2 compounds reported here does not correspond to the appropriate Kotani model, suggesting as-yet undiscovered physics in these systems.
The observation of inverted magnetic hysteresis loops and negative magnetic remanence (NRM) in a 7.6 nm thin film of La 0.7 Sr 0.3 MnO 3 grown on SrTiO 3 substrates is reported here. The film was grown employing pulsed laser deposition and characterized by reflection high-energy electron diffraction during growth and using x-ray reflectivity measurements post-growth. Magnetic properties of the film were measured from 5 K to 400 K under both the field-cooled (FC) and zero-field-cooled (ZFC) conditions. The observed results of inverted magnetic hysteresis loops and NRM are interpreted in terms of the co-existence of a magnetically inhomogeneous region consisting of superparamagnetic spin clusters with a blocking temperature $T_B$ = 240 K and the ferromagnetic state with an ordering temperature $T_C$ = 290 K. Hysteresis loop inversion is observed in the temperature region of $T_B < T < T_C$ whereas NRM appears in the mixed superparamagnetic and ferromagnetic states for $T < T_C$ down to 5 K. These observations of hysteresis loop inversion and NRM are related to the magneto-static interaction between the superparamagnetic and ferromagnetic phases leading to anti-alignment of spin of both magnetic phases with respect to each other.
Here, we report synthesis and magnetic properties of quasi-one-dimensional spin- 1 2 Heisenberg antiferromagnetic chain compound BaNa 2 Cu ( VO 4 ) 2 . This orthovanadate has a centrosymmetric crystal structure, C 2 / c , where the magnetic Cu 2 + ions form spin chains. These chains are arranged in layers, with the chain direction changing by 62 ° between the two successive layers. Alternatively, the spin lattice can be viewed as anisotropic triangular layers upon taking the interchain interactions into consideration. Despite this potential structural complexity, temperature-dependent magnetic susceptibility, heat capacity, electron spin resonance intensity, and nuclear magnetic resonance (NMR) shift agree well with the uniform spin- 1 / 2 Heisenberg chain model with an intrachain coupling of J / k B ≃ 5.6 K. The saturation field obtained from the magnetic isotherm measurement consistently reproduces the value of J / k B . Further, the V 51 NMR spin-lattice relaxation rate mimics the one-dimensional character in the intermediate temperature range, whereas magnetic long-range order sets in below T N ≃ 0.25 K. The effective interchain coupling is estimated to be J ⊥ / k B ≃ 0.1 K. The theoretical estimation of exchange couplings using band-structure calculations reciprocate our experimental findings and unambiguously establish the one-dimensional character of the compound. Finally, the spin lattice of BaNa 2 Cu ( VO 4 ) 2 is compared with the chemically similar but not isostructural compound BaAg 2 Cu ( VO 4 ) 2 .
Spintronics holds great potential for next-generation high-speed and low–power consumption information technology. Recently, lead halide perovskites (LHPs), which have gained great success in optoelectronics, also show interesting magnetic properties. However, the spin-related properties in LHPs originate from the spin-orbit coupling of Pb, limiting further development of these materials in spintronics. Here, we demonstrate a new generation of halide perovskites, by alloying magnetic elements into optoelectronic double perovskites, which provide rich chemical and structural diversities to host different magnetic elements. In our iron-alloyed double perovskite, Cs 2 Ag(Bi:Fe)Br 6 , Fe 3+ replaces Bi 3+ and forms FeBr 6 clusters that homogenously distribute throughout the double perovskite crystals. Furthermore, we observe a strong temperature-dependent magnetic response at temperatures below 30 K, which is tentatively attributed to a weak ferromagnetic or antiferromagnetic response from localized regions. We anticipate that this work will stimulate future efforts in exploring this simple yet efficient approach to develop new spintronic materials based on lead-free double perovskites.
The efficiency and stability of RuO 2 in electrocatalysis has made this material a subject of intense fundamental and industrial interest. The surface functionality is rooted in its electronic and magnetic properties, determined by a complex interplay of lattice-, spin-rotational, and time-reversal symmetries, as well as the competition between Coulomb and kinetic energies. This interplay was predicted to produce a network of Dirac nodal lines (DNLs), where the valence and conduction bands touch along continuous lines in momentum space. Here we uncover direct evidence for three DNLs in RuO 2 by angle-resolved photoemission spectroscopy. These DNLs give rise to a flat-band surface state that is readily tuned by the electrostatic environment, and that presents an intriguing platform for exotic correlation phenomena. Our findings support high spin-Hall conductivities and bulk magnetism in RuO 2 , and are likely related to its catalytic properties.