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At least 1,747 records · Page 97

Structural insights into Lewis acid- and F4TCNQ-doped conjugated polymers by solid-state magnetic resonance spectroscopy

Molecular doping strategies facilitate orders of magnitude enhancement in the charge carrier mobility of organic semiconductors (OSCs). Understanding the different doping mechanisms and molecular-level constraints on doping efficiency related to the material energy levels is crucial to develop versatile dopants for OSCs. Given the compositional and structural heterogeneities associated with OSC thin films, insight into dopant–polymer interactions by long-range techniques such as X-ray scattering and electron microscopy is exceedingly challenging to obtain. This study employs short-range probes, solid-state (ss)NMR and EPR spectroscopy, to resolve local structures and intermolecular interactions between dopants such as F4TCNQ (2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane), Lewis acid BCF (tris[pentafluorophenyl] borane) and Lewis base conjugated polymer, PCPDTBT (P4) (poly[2,6-(4,4-bis(2-hexadecyl)-4H-cyclopenta[2,1-b;3,4-b']dithiophene)-alt-4,7(2,1,3-benzothiadiazole)]). Analysis of 1 H and 13 C ssNMR spectra of P4, P4 : F4TCNQ and P4 : BCF blends indicates that the addition of dopants induces local structural changes in the P4 polymer, and causes paramagnetism-induced signal broadening and intensity losses. The hyperfine interactions in P4 : BCF and P4 : F4TCNQ are characterized by two-dimensional pulsed EPR spectroscopy. For P4 : F4TCNQ, 19 F ssNMR analysis indicates that the F4TCNQ molecules are distributed and aggregated into different local chemical environments. By comparison, BCF molecules are intermixed with the P4 polymer and interact with traces of water molecules to form BCF–water complexes that serve as Brønsted acid sites, as revealed by 11 B ssNMR spectroscopy. These results indicate that the P4–dopant blends exhibit complex morphology with different distributions of dopants, whereby the combined use of ssNMR and EPR provides essential insights into how higher doping efficiency is observed with BCF and a mediocre efficiency is associated with F4TCNQ molecules.

36 MATERIALS SCIENCE↗

Tunable Magnetic Resonance in Microwave Spintronics Devices

Magnetic resonance is one of the key properties of magnetic materials for the application of microwave spintronics devices. The conventional method for tuning magnetic resonance is to use an electromagnet, which provides very limited tuning range. Hence, the quest for enhancing the magnetic resonance tuning range without using an electromagnet has attracted tremendous attention. In this paper, we exploit the huge exchange coupling field between magnetic interlayers, which is on the order of 4000 Oe and also the high frequency modes of coupled oscillators to enhance the tuning range. Furthermore, we demonstrate a new scheme to control the magnetic resonance frequency. Moreover, we report a shift in the magnetic resonance frequency as high as 20 GHz in CoFe-based tunable microwave spintronics devices, which is 10X higher than conventional methods.

Microwave Detectors↗

Tunable Magnetic Resonance in Microwave Spintronics Devices

Magnetic resonance is one of the key properties of magnetic materials for the application of microwave spintronics devices. The conventional method for tuning magnetic resonance is to use an electromagnet, which provides very limited tuning range. Hence, the quest for enhancing the magnetic resonance tuning range without using an electromagnet has attracted tremendous attention. In this paper, we exploit the huge exchange coupling field between magnetic interlayers, which is on the order of 4000 Oe and also the high frequency modes of coupled oscillators to enhance the tuning range. Furthermore, we demonstrate a new scheme to control the magnetic resonance frequency. Moreover, we report a shift in the magnetic resonance frequency as high as 20 GHz in CoFe based tunable microwave spintronics devices, which is 10X higher than conventional methods.

Microwave Detectors↗

Cr silicate as a prototype for engineering magnetic phases in air-stable two-dimensional transition-metal silicates

Abstract Identifying environmentally inert, ferromagnetic two-dimensional (2D) materials with high Curie temperatures ( T c ) down to the single layer limit has been an obstacle to fundamental studies of 2D magnetism and application of 2D heterostructures to spin-polarized devices. To address this challenge, the growth, structure and magnetic properties of a 2D Cr-silicate single layer on Pt(111) was investigated experimentally and theoretically. The layer was grown by sequentially depositing SiO and Cr followed by annealing in O 2 . Scanning tunneling microscopy (STM), low-energy electron diffraction (LEED), and low energy electron microscopy all indicated a well-ordered layer that uniformly covered the surface, with STM and LEED indicating that the silicate relaxed to its favored lattice constant. Further experimental characterizations demonstrated that the Cr was nominally 3+ but with a lower electron density than typical trivalent Cr compounds. Comparison with theory identified a Cr 2 Si 2 O 9 structure that resembles a single layer of a dehydrogenated dioctahedral silicate. Magnetic circular dichroism in x-ray absorption spectroscopy revealed a ferromagnetically ordered state up to at least 80 K. Theoretical analysis revealed that the Cr in a dehydrogenated Cr-silicate/Pt(111) is more oxidized than Cr in freestanding Cr 2 Si 2 O 9 H 4 layers. This greater oxidation was found to enhance ferromagnetic coupling and suggests that the magnetism may be tuned by doping. The 2D Cr-silicate is the first member of a broad series of possible layered first-row transition metal silicates with magnetic order; thus, this paper introduces a new platform for investigating 2D ferromagnetism and the development of magnetoelectronic and spintronic devices by stacking 2D atomic layers.

2D materials↗

Study of structural, transport and magneto-crystalline anisotropy in La 1-x Sr x MnO 3 (0.30 ≤ x ≤ 0.40) perovskite manganites

In this paper we present structural, transport, magnetic and magneto-crystalline anisotropy of La 1–x Sr x MnO 3 (х = 0.30, 0.33, 0.36, and 0.40) synthesized using the solid-state reaction method. The X-ray diffraction pattern of the samples is well indexed to the rhombohedral structure with R 3 - c space group. Lattice parameters and unit cell volume are found to decrease monotonically upon increasing Sr 2+ concentration at La 3+ site. X-ray photoelectron spectroscopy confirms the presence of Mn 4+ and Mn 3+ , the ratio of which (Mn 4+ /Mn 3+ ) increases from 0.44 to 0.64 with increasing Sr 2+ concentration. From the ρ(T) and M(T) data analysis, we find that T MI and M S are larger for x = 0.33 composition, suggesting a weakening of the double-exchange interaction due to competing super-exchange interactions in x = 0.30, 0.36 and 0.40 samples. We calculated MCA constant (K 1 ) by fitting the saturation magnetisation data at a higher magnetic field using the law of approach model, M = M S [1-a/H-b/H 2 ]-χH with K 1 2 = (105/8)bMs 2 and is in the order of 10 5 erg/cm 3 .

36 MATERIALS SCIENCE↗

Hidden frustration in the triangular-lattice antiferromagnet NdCd 3 ⁢P 3

We report a study of the magnetic ground state and crystal electric field (CEF) scheme in the triangular-lattice antiferromagnet NdCd 3 ⁢P 3 . Combined neutron scattering, magnetization, and heat capacity measurements demonstrate that the Nd 3+ moments occupying the triangular lattice in this material harbor hidden signs of frustration not detected in typical Curie-Weiss-based parametrization of the frustration index (𝑓 = Θ 𝐶⁢𝑊 /𝑇 𝑁 ). This is evidenced by a zero-field splitting of the Kramers' ground state and first excited state doublets at temperatures far in excess of 𝑇 𝑁 as well as signatures of low-energy fluctuations for 𝑇 ≫ 𝑇 𝑁 . As a result, a suppression of the zero-field ordered moment relative to its field saturation value is observed, and the impacts of this magnetic frustration as well as the coexisting bond frustration in the CdP honeycomb network on the physical properties of NdCd 3 ⁢P3 are discussed.

Frustrated magnetism↗

Structural, magnetic and electrical transport properties of YMnAl

The intermetallic compound YMnAl, crystallizing in the cubic C-15 (MgCu 2 -type) structure, was prepared using arc-melting and annealing. Rietveld refinement of the XRD pattern yields a lattice parameter of a = 7.816(1) Å⁠. The system exhibits antiferromagnetic order with a transition temperature of approximately 38 K, along with indications of a spin-glass–like phase. The effective magnetic moment, estimated from Curie–Weiss fitting of the susceptibility versus temperature curve, is 6.06 μ B /f.u. and the Curie–Weiss temperature of −79 K confirming the antiferromagnetic nature. Isothermal magnetization measurements below and above the Néel temperature show no saturation, with a maximum magnetization of 0.09 μ B /f.u observed at an applied field of 9 T. The temperature dependence of resistivity exhibits a negative temperature coefficient, characteristic of dirty metals. Hall effect measurements indicate the absence of an anomalous Hall contribution. The Hall coefficient RH, carrier concentration n, and mobility μ estimated from R XY (H) are -1.05×10 -8 m 3 /C, 5.92×10 26 m -3 and 1.05×10 -3 m 2 /V.s, respectively. Our first-principles calculations indicate that YMnAl in the orthorhombic (Imma) structure has the lowest energy; however, the substitutional disorder occurring during experimental synthesis may favor the formation of the cubic Laves phase.

Crystallography↗

Magnetic field induced antiferromagnetic cone structure in multiferroic BiFeO 3

Neutron diffraction measurements were performed under high magnetic fields up to 17 T in a multiferroic BiFeO 3 single crystal, in which an intermediate magnetic (IM) phase has been found between the cycloid and canted antiferromagnetic phases [S. Kawachi et al., Phys. Rev. Mater. 1, 024408 (2017)]. We clearly found that the incommensurate magnetic peaks, which split perpendicular to the magnetic field in the cycloid phase, rotate by 90 deg to align parallel to the field in the IM phase. The magnetic structure in the IM phase can be best described by an antiferromagnetic cone (AF cone) structure. The transition from the cycloid to AF cone is of first order and the direction of the magnetic wave vector and the easy plane of the cycloidal component are rotated by 90 deg without changing the cycloidal modulation period, whereas the transition from the AF cone to canted antiferromagnetic phase is gradual and the cone angle becomes smaller gradually without changing the modulation period. Interestingly, the cycloidal component as well as the cone angle in the IM phase shows a large hysteresis between the field increasing and decreasing processes. Finally, this result, combined with the magnetostriction with a large hysteresis previously reported in the IM phase, suggests a strong magnetoelastic coupling.

36 MATERIALS SCIENCE↗

Spin–Phonon Coupling in Ferromagnetic Monolayer Chromium Tribromide

Novel 2D magnets exhibit intrinsic electrically tunable magnetism down to the monolayer limit, which has significant value for nonvolatile memory and emerging computing device applications. In these compounds, spin–phonon coupling (SPC) typically plays a crucial role in magnetic fluctuations, magnon dissipation, and ultimately establishing long-range ferromagnetic order. However, a systematic understanding of SPC in 2D magnets that combines theory and experiment is still lacking. Here in this work, monolayer chromium tribromide is studied to investigate SPC in 2D magnets via Raman spectroscopy and first principle calculations. The experimental Curie temperature and phonon shifts are found to be in good agreement with the numerical simulations. Specifically, it is demonstrated how magnetic exchange interactions affect phonon vibrations, which helps establish design fundamentals for 2D magnetic materials and other related devices.

36 MATERIALS SCIENCE↗

Imaging the Breakdown and Restoration of Topological Protection in Magnetic Topological Insulator MnBi 2 Te 4

Quantum anomalous Hall (QAH) insulators transport charge without resistance along topologically protected chiral 1D edge states. Yet, in magnetic topological insulators to date, topological protection is far from robust, with zero-magnetic field QAH effect only realized at temperatures an order of magnitude below the Néel temperature T N , though small magnetic fields can stabilize QAH effect. Understanding why topological protection breaks down is therefore essential to realizing QAH effect at higher temperatures. Here a scanning tunneling microscope is used to directly map the size of exchange gap (E g,ex ) and its spatial fluctuation in the QAH insulator 5-layer MnBi 2 Te 4 . Long-range fluctuations of E g,ex are observed, with values ranging between 0 (gapless) and 70 meV, appearing to be uncorrelated to individual surface point defects. The breakdown of topological protection is directly imaged, showing that the gapless edge state, the hallmark signature of a QAH insulator, hybridizes with extended gapless regions in the bulk. Finally, it is unambiguously demonstrated that the gapless regions originate from magnetic disorder, by demonstrating that a small magnetic field restores E g,ex in these regions, explaining the recovery of topological protection in magnetic fields. The results indicate that overcoming magnetic disorder is the key to exploiting the unique properties of QAH insulators.

36 MATERIALS SCIENCE↗

Phenomenology of magnetic black holes with electroweak-symmetric coronas

Magnetically charged black holes (MBHs) are interesting solutions of the Standard Model and general relativity. They may possess a “hairy” electroweak-symmetric corona outside the event horizon, which speeds up their Hawking radiation and leads them to become nearly extremal on short timescales. Their masses could range from the Planck scale up to the Earth mass. We study various methods to search for primordially produced MBHs and estimate the upper limits on their abundance. We revisit the Parker bound on magnetic monopoles and show that it can be extended by several orders of magnitude using the large-scale coherent magnetic fields in Andromeda. This sets a mass-independent constraint that MBHs have an abundance less than 4 × 10 -4 times that of dark matter. MBHs can also be captured in astrophysical systems like the Sun, the Earth, or neutron stars. There, they can become non-extremal either from merging with an oppositely charged MBH or absorbing nucleons. The resulting Hawking radiation can be detected as neutrinos, photons, or heat. High-energy neutrino searches in particular can set a stronger bound than the Parker bound for some MBH masses, down to an abundance 10 -7 of dark matter.

79 ASTRONOMY AND ASTROPHYSICS↗

Effect of atom substitutions on the magnetic properties in Ce 2 Fe 17 : Toward permanent magnet applications

Due to the rapidly developing technologies and huge market demand, there has been increasing interest internationally in exploring permanent magnet formulations in addition to the well-known Nd 2 Fe 14 B and SmCo 5 /Sm 2 Co 17 . Given Fe's low materials cost and generally high magnetization, Fe-rich rare earth binaries such as Ce 2 Fe 17 comprise a rich “hunting ground” for such new materials. While this compound suffers from a low ordering point and is a heli magnet, these difficulties are easily remedied by the substitution of appropriate amounts of cobalt for Fe, with room-temperature saturation magnetization as high as 1.5 T. In this work, we try to switch the all-important magnetic anisotropy from planar to uniaxial behavior in Ce 2 Fe 17 via 18 h - and 6 c -type atom substitutions with Si, Ir, and numerous other atoms. The uniaxial magnetocrystalline anisotropy is successfully achieved in the 6 c -site-substituted Ce 2 Fe 15 Ir 2 systems, along with large magnetization. We find that iridium substitution, in particular, induces a substantial uniaxial anisotropy of 11.25 MJ/m 3 , which is comparable to most of the current rare earth permanent magnets. Although the iridium substitution is costly, the finding of Ir-triggered uniaxial magnetic anisotropy indicates the potential of Ce–Fe-based alloys for permanent magnets.

36 MATERIALS SCIENCE↗

Viscous damping of Alfven normal modes in non-uniform plasmas

The Alfven normal mode in a nonuniform, viscous plasma is investigated. Because the ideal hydromagnetic equation is singular in a nonuniform magnetic field, viscosity is included in order to regularize the equation, analogous to the removal of the singular point by resistivity (Mok and Einaudi, 1985). The eigenvalue equation is then solved numerically for a particular magnetic configuration. The real part of the frequency of this viscous normal mode is found to be similar to the one in the resistive case, while the damping is shown to be comparable, and sometimes to exceed, the resistive effect under certain conditions in which the Lundquist number is sufficiently large. The damping rate is evaluated for various plasma conditions corresponding to different parts of the solar atmosphere. The effects of viscosity are found to dominate resistivity in the quiet sun corona and solar wind.

Mok, Y.↗

Inferring the scrape-off layer heat flux width in a divertor with a low degree of axisymmetry

Plasma facing components (PFCs) in the next generation of tokamak devices will operate in challenging environments, with heat loads predicted to exceed 10 MWm -2 . The magnitude of these heat loads is set by the width of the channel, the ‘scrape-off layer’ (SOL), into which heat is exhausted, and can be characterised by an e-folding length scale for the decay of heat flux across the channel. It is expected this channel will narrow as tokamaks move towards reactor relevant conditions. Understanding the processes involved in setting the SOL heat flux width is imperative to be able to predict the heat loads PFCs must handle in future devices. Measurements of the SOL width are performed on the high-field spherical tokamak, ST40, using a newly commissioned infrared thermography system. With its high on-axis toroidal magnetic field (≥1.5 T) ST40 is uniquely positioned to investigate the influence of toroidal field on the heat flux width in spherical tokamaks, whilst also extending measurements of the SOL width in spherical tokamaks to increased poloidal field (≥0.3 T). Due to the divertor on ST40 having a low degree of axisymmetry, it is necessary for a set of radial measurements of the heat flux to be taken across the divertor, made possible using an automated toolchain that fully incorporates its 3D geometry. These radial profiles are combined with the magnetic geometry of the plasma to infer the width of the SOL, with both Eich and double exponential profiles of heat flux observed. A reduction in the heat flux is observed toroidally across part of the divertor, along with increased heat loads observed locally around the edges of the tiles. Future work in characterising the impact of tile misalignment and uncertainties in the reconstructed divertor magnetic geometry is required in order to further understand the observed heat flux patterns, as are additional investigations into the role potentially being played by an inhomogeneous sheath electric field.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Probing atomic-scale symmetry breaking by rotationally invariant machine learning of multidimensional electron scattering

Abstract The 4D scanning transmission electron microscopy (STEM) method maps the structure and functionality of solids on the atomic scale, yielding information-rich data sets describing the interatomic electric and magnetic fields, structural and electronic order parameters, and other symmetry breaking distortions. A critical bottleneck is the dearth of analytical tools that can reduce complex 4D-STEM data to physically relevant descriptors. We propose an approach for the systematic exploration of 4D-STEM data using rotationally invariant variational autoencoders (rrVAE), which disentangle the general rotation of the object from other latent representations. The implementation of purely rotational rrVAE is discussed as are applications to simulated data for graphene and zincblende structures. The rrVAE analysis of experimental 4D-STEM data of defects in graphene is illustrated and compared to the classical center-of-mass analysis. This approach is universal for probing symmetry-breaking phenomena in complex systems and can be implemented for a broad range of diffraction methods.

36 MATERIALS SCIENCE↗

Rapid solidified ductile Cu-Al-Mn ribbon and its elastocaloric potential

Abstract Cu-Al-Mn alloys display martensitic transformation over a wide range of temperatures. In addition to low cost, this alloy is known for its low transformation stress with reasonable latent heat favoring elastocaloric applications. However, the ductility of Cu-Al-Mn can be limited owing to ordering and intergranular fracture. Through rapid solidification by melt spinning, we show that Cu-Al-Mn ribbon can be made highly ductile (greater than 8% tensile strain in the as-spun state and 10% tensile strain after heat treatment). The ductility of the melt-spun ribbon is related to the suppression of L2 1 ordering that is characterized through magnetic property measurement. Heat treatment of the ribbon promotes bamboo grain formation, and the latent heat is increased to 6.4 J g −1 . Under tensile conditions, we show that the ribbon exhibited about 4 °C temperature change (4.4 °C on heating and 4.2 °C on cooling from 6.3% strain).

36 MATERIALS SCIENCE↗

Hund's metal physics: From SrNiO 2 to LaNiO 2

We study the normal state electronic structure of the recently discovered infinite-layer nickelate superconductor, Nd 1-x Sr x NiO 2 , using density functional theory plus dynamical mean-field theory calculations. Starting with the multiorbital compound SrNiO 2 , our calculations show that despite large charge-carrier doping from SrNiO 2 to LaNiO 2 , the Ni-3d total occupancy is barely changed due to the decreased hybridization with the occupied oxygen-2p states and increased hybridization with the unoccupied La-5d states. Thus, using SrNiO 2 as a reference, La 1-x Sr x NiO 2 is naturally and conclusively found to be a multiorbital electronic system with characteristic Hund's metal behaviors, such as metallicity, the importance of high-spin configurations, tendency towards orbital differentiation, and the absence of magnetism in regimes which are ordered according to static mean-field theories. Finally, our results are in good agreement with the existing spectroscopic studies and make an essential step towards an understanding of the electronic structures of Nd 1-x Sr x NiO 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Current-enabled optical conductivity of superconductors

In most superconductors, optical excitations require impurity scattering or the presence of multiple bands. This is because in clean single-band superconductors, the combination of particle-hole and inversion symmetries prevents momentum-conserving transitions. In this Letter we show how the flow of supercurrent can lead to new contributions to optical conductivity. As the supercurrent breaks inversion symmetry, transitions across the superconducting gap become allowed even in clean superconductors and dominate over impurity-induced contributions for energies comparable to the gap width. Further, the response is dependent on the nature of the underlying normal state as well as on the type of superconducting order. Use of an external magnetic field to produce a screening supercurrent with controllable magnitude and direction, enables a detailed investigation of the superconducting state, allowing determination of the gap symmetry in unconventional superconductors for which other techniques have not been practicable.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗