Phase-transforming metamaterial with magnetic interactions.

Solid-solid phase transformations can affect energy transduction and change material properties (e.g., superelasticity in shape memory alloys and soft elasticity in liquid crystal elastomers). Traditionally, phase-transforming materials are based on atomic- or molecular-level thermodynamic and kinetic mechanisms. Here, we develop elasto-magnetic metamaterials that display phase transformation behaviors due to nonlinear interactions between internal elastic structures and embedded, macroscale magnetic domains. These phase transitions, similar to those in shape memory alloys and liquid crystal elastomers, have beneficial changes in strain state and mechanical properties that can drive actuations and manage overall energy transduction. The constitutive response of the elasto-magnetic metamaterial changes as the phase transitions occur, resulting in a nonmonotonic stress-strain relation that can be harnessed to enhance or mitigate energy storage and release under high-strain-rate events, such as impulsive recoil and impact. Using a Landau free energy-based predictive model, we develop a quantitative phase map that relates the geometry and magnetic interactions to the phase transformation. Our work demonstrates how controllable phase transitions in metamaterials offer performance capabilities in energy management and programmable material properties for high-rate applications.

Stacking-dependent interlayer magnetic interactions in CrSe2.

Recently, CrSe2, a new ferromagnetic van der Waals two-dimensional material, was discovered to be highly stable under ambient conditions, making it an attractive candidate for fundamental research and potential device applications. Here, we study the interlayer interactions of bilayer CrSe2using first-principles calculations. We demonstrate that the interlayer interaction depends on the stacking structure. The AA and AB stackings exhibit antiferromagnetic (AFM) interlayer interactions, while the AC stacking exhibits ferromagnetic (FM) interlayer interaction. Furthermore, the interlayer interaction can be further tuned by tensile strain and charge doping. Specifically, under large tensile strain, most stacking structures exhibit FM interlayer interactions. Conversely, under heavy electron doping, all stacking structures exhibit AFM interlayer interactions. These findings are useful for designing spintronic devices based on CrSe2.

The Physical Mechanism of Linear and Nonlinear Optical Properties of Nanographene-Induced Chiral Inversion.

Based on density functional theory (DFT) and wave function analysis, the ultraviolet and visible spectrophotometry (UV-Vis) spectra and Raman spectra of 1-meso and 1-rac obtained by the chiral separation of chiral nanographenes are theoretically investigated. The electron excitation properties of 1-meso and 1-rac are studied by means of transition density matrix (TDM) and charge density difference (CDD) diagrams. The intermolecular interaction is discussed based on an independent gradient model based on Hirshfeld partition (IGMH). The interaction of 1-meso and 1-rac with the external environment is studied using the electrostatic potential (ESP), and the electron delocalization degree of 1-meso and 1-rac is studied based on the magnetically induced current under the external magnetic field. Through the chiral separation of 1-rac, two enantiomers, 1-(P, P) and 1-(M, M), were obtained. The electrical-magnetic interaction of the molecule is revealed by analyzing the electron circular dichroism (ECD) spectra of 1-meso, 1-(P, P) and 1-(M, M), the transition electric dipole moment (TEDM) and the transition magnetic dipole moment (TMDM). It is found that 1-(P, P) and 1-(M, M) have opposite chiral properties due to the inversion of the structure.

Development of a Non-Linear Bi-Directional Vortex-Induced Piezoelectric Energy Harvester with Magnetic Interaction.

In this study, magnetic force is introduced to the design of a bi-directional U-shaped piezoelectric energy harvester for vortex-induced vibrations. The theoretical model of the beam structure is derived based on the Euler-Bernoulli beam theory. The vortex-induced vibration and the non-linear magnetic force are modeled according to the Rayleigh oscillator and the charge model, respectively. A prototype is fabricated and tested in two orthogonal directions under vortex-induced vibrations in a wind tunnel. Up and down wind-speed sweeps are carried out to investigate the non-linear responses of the harvester. The distance between the magnets and the length of the side beams are adjusted to examine the influence of the magnetic force on the lock-in region and voltage output of the harvester. Overall, the harvester shows strong non-linearity in the horizontal excitations. After adding magnets to the system, significant improvement of the lock-in region and the peak voltage is noticed in the horizontal mode under both up and down sweeps.

Opening Magnetic Hysteresis by Axial Ferromagnetic Coupling: From Mono-Decker to Double-Decker Metallacrown.

Combining Ising-type magnetic anisotropy with collinear magnetic interactions in single-molecule magnets (SMMs) is a significant synthetic challenge. Herein we report a Dy[15-MCCu -5] (1-Dy) SMM, where a DyIII ion is held in a central pseudo-D5h pocket of a rigid and planar Cu5 metallacrown (MC). Linking two Dy[15-MCCu -5] units with a single hydroxide bridge yields the double-decker {Dy[15-MCCu -5]}2 (2-Dy) SMM where the anisotropy axes of the two DyIII ions are nearly collinear, resulting in magnetic relaxation times for 2-Dy that are approximately 200 000 times slower at 2 K than for 1-Dy in zero external field. Whereas 1-Dy and the YIII -diluted Dy@2-Y analogue do not show remanence in magnetic hysteresis experiments, the hysteresis data for 2-Dy remain open up to 6 K without a sudden drop at zero field. In conjunction with theoretical calculations, these results demonstrate that the axial ferromagnetic Dy-Dy coupling suppresses fast quantum tunneling of magnetization (QTM). The relaxation profiles of both complexes curiously exhibit three distinct exponential regimes, and hold the largest effective energy barriers for any reported d-f SMMs up to 625 cm-1 .

UNO DMRG CAS CI calculations of binuclear manganese complex Mn(IV)2 O2 (NHCHCO2 )4 : Scope and applicability of Heisenberg model.

Both direct exchange and super-exchange interactions cooperate to realize inter-spin magnetic interaction in binuclear manganese complex Mn(IV)2 O2 (NHCHCO2 )4 with a di-µ-oxo path. We revisited this spin system using DMRG CAS methods and CAS selection procedures. Our results indicate that our previous "dynamically extended spin polarization" (DE-SP) procedure for organic polyradicals and so forth does not work well. Thus, we have examined another selection procedure, the "dynamically extended super-exchange" (DE-SE) procedure. DMRG CASCI [18,18] by UB3LYP(HS)-UNO(DE-SE) can realize antiferromagnetic J values similar to experimental ones (-87 cm-1 ). In addition, all J values between all spin states (HS[septet],IS[quintet],IS[triplet],LS[singlet])were also shown to be correct under sufficiently large M values. © 2018 Wiley Periodicals, Inc.

Design Procedure and Experimental Verification of a Broadband Quad-Stable 2-DOF Vibration Energy Harvester.

Vibration-based energy harvesters brought the idea of self-powered sensors to reality in the past few years. Many strategies to improve the performance of linear vibration energy harvesters that collect energy over a limited bandwidth have been proposed. In this paper, a bi-stable two degrees of freedom (2-DOF) cut-out vibration energy harvester employing a pair of permanent magnets is designed through a proposed design methodology. Based on this methodology, the nonlinear harvesters can be optimally designed such that the bandwidth can be widened for a targeted output voltage. The proper selection of the harvester parameters as well as the gap distances between the tip and the fixed magnets are the bases of this methodology. The mathematical modeling of the proposed harvester and the formula for the potential energy between the tip and the fixed magnets are presented. Additionally, to enhance the performance of the bi-stable energy harvester (BEH), a quad-stable energy harvester (QEH) was configured by adding more fixed magnets. Experiments were performed to validate the numerical simulations and the results showed that, the simulation and experimental results are consistent. The results indicate that, the QEH covers a wider bandwidth than the BEH and based on a figure of merit the QEH shows the best performance among many harvesters presented in the literature.

Magnetic Interaction Observed in Hetero Biradical Derivatives Containing a 2,2,5,5-Tetramethylpyrrolin-1-yloxyl Unit as a Localized Spin Center.

The magneto-structural correlation of hetero biradical derivatives containing a 2,2,5,5-tetramethylpyrrolin-1-yloxyl unit as a localized spin center and a verdazyl or nitronyl nitroxide radical is reported. The magnetic susceptibility measurement revealed that the verdazyl attached biradical 1 exhibits ferromagnetic interaction, whereas antiferromagnetic interaction is observed for nitronyl nitroxide attached biradical 2. An EPR study in toluene glass matrix suggests that both 1 and 2 have a ground triplet state. DFT calculations predict that there is intramolecular ferromagnetic interaction for both biradicals. The computation also suggests that the intramolecular magnetic interaction is weaker with larger dihedral angle between pyrroline ring and verdazyl ring/O-N-C-N-O plane of nitronyl nitroxide. The computations of model compounds 3 and 4 suggest that spin polarization on vinylic moiety without distribution of SOMO might be an essential condition for the intramolecular ferromagnetic interaction.

Spin Orientation of Two-Dimensional Electrons Driven by Temperature-Tunable Competition of Spin-Orbit and Exchange-Magnetic Interactions.

Finding ways to create and control the spin-dependent properties of two-dimensional electron states (2DESs) is a major challenge for the elaboration of novel spin-based devices. Spin-orbit and exchange-magnetic interactions (SOI and EMI) are two fundamental mechanisms that enable access to the tunability of spin-dependent properties of carriers. The silicon surface of HoRh2Si2 appears to be a unique model system, where concurrent SOI and EMI can be visualized and controlled by varying the temperature. The beauty and simplicity of this system lie in the 4f moments, which act as a multiple tuning instrument on the 2DESs, as the 4f projections parallel and perpendicular to the surface order at essentially different temperatures. Here we show that the SOI locks the spins of the 2DESs exclusively in the surface plane when the 4f moments are disordered: the Rashba-Bychkov effect. When the temperature is gradually lowered and the system experiences magnetic order, the rising EMI progressively competes with the SOI leading to a fundamental change in the spin-dependent properties of the 2DESs. The spins rotate and reorient toward the out-of-plane Ho 4f moments. Our findings show that the direction of the spins and the spin-splitting of the two-dimensional electrons at the surface can be manipulated in a controlled way by using only one parameter: the temperature.

Fermionic behavior of ideal anyons.

We prove upper and lower bounds on the ground-state energy of the ideal two-dimensional anyon gas. Our bounds are extensive in the particle number, as for fermions, and linear in the statistics parameter α . The lower bounds extend to Lieb-Thirring inequalities for all anyons except bosons.

Role of Dy 4felectrons on magnetic coupling and reorientation in DyFeO3.

Spin reorientation transition is an ubiquitous phenomenon observed in magnetic rare earth orthferrites RFeO3, which has garnered significant attention in recent years due to its potential applications in spintronics or magnetoelectric devices. Although a plenty of experimental works suggest that the magnetic interaction between R3+and Fe3+spins is at the heart of the spin reorientation, but a direct and conclusive theoretical support has been lacking thus far, primarily due to the challenging nature of handling R 4felectrons. In this paper, we explored DyFeO3as an example by means of comprehensive first principles calculations, and compared two different approaches, where the Dy 4felectrons were treated separately as core or valence states, aiming to elucidate the role of Dy 4felectrons, particularly in the context of the spin reorientation transition. The comparison provides a solid piece of evidence for the experimental argument that the Dy3+-Fe3+magnetic interactions play a vital role in triggering spin reorientation of Fe3+moments at low temperatures. The findings revealed here not only extend our understanding on the underlying mechanism for spin reorientation transition in RFeO3, but also highlight the importance of explicit description of R 4felectrons in rationally reproducing their structural, electronic and magnetic properties.

Visualizing Nanoscale Interlayer Magnetic Interactions and Unconventional Low-Frequency Behaviors in Ferromagnetic Multishelled Structures.

Precise manipulation of van der Waals forces within 2D atomic layers allows for exact control over electron-phonon coupling, leading to the exceptional quantum properties. However, applying this technique to diverse structures such as 3D materials is challenging. Therefore, investigating new hierarchical structures and different interlayer forces is crucial for overcoming these limitations and discovering novel physical properties. In this work, a multishelled ferromagnetic material with controllable shell numbers is developed. By strategically regulating the magnetic interactions between these shells, the magnetic properties of each shell are fine-tuned. This approach reveals distinctive magnetic characteristics including regulated magnetic domain configurations and enhanced effective fields. The nanoscale magnetic interactions between the shells are observed and analyzed, which shed light on the modified magnetic properties of each shell, enhancing the understanding and control of ferromagnetic materials. The distinctive magnetic interaction significantly boosts electromagnetic absorption at low-frequency frequencies used by fifth-generation wireless devices, outperforming ferromagnetic materials without multilayer structures by several folds. The application of magnetic interactions in materials science reveals thrilling prospects for technological and electronic innovation.

Biomimetic Multi-Interface Design of Raspberry-like Absorbent: Gd-doped FeNi3@Covalent Organic Framework Derivatives for Efficient Electromagnetic Attenuation.

Structural design and interface regulation are useful strategies for achieving strong electromagnetic wave absorption (EMWA) and broad effective absorption bandwidth (EAB). Herein, a monomer-mediated strategy is employed to control the growth of covalent organic framework (COF) wrapping flower-shaped Gd-doped FeNi3 (GFN), and a novel raspberry-like absorbent based on biomimetic design is fabricated by thermal catalysis. Further, a unique dielectric-magnetic synergistic system is constructed by utilizing the COF-derived nitrogen-doped porous carbon (NPC) as the shell and anisotropic GFN as the core. The electromagnetic parameters of the GFN@NPC composites can be tuned by adjusting the proportions of GFN and NPC. Off-axis electron holography results further clarify the interface polarization and microscale magnetic interactions affecting the EMW loss mechanism. As a result, the GFN@NPC samples exhibit broad EMWA performance. The EAB values of all GFN@NPC composites reach up to 6.0 GHz, with the GFN@NPC-2 sample showing a minimum reflection loss (RLmin) of -69.6 dB at 1.68 mm. In addition, GFN@NPC-2 achieves a maximum radar cross-section (RCS) reduction of 29.75 dB·m2. A multi-layer gradient structure is also constructed using metamaterial simulation to achieve an ultra-wide EAB of 12.24 GHz. Overall, this work provides a novel bio-inspired design strategy to develop high-performance EMWA materials.

Programmable Modular Acoustic Microrobots.

Microrobots have emerged as promising tools for biomedical and in vivo applications, leveraging their untethered actuation capabilities and miniature size. Despite extensive research on diversifying multi-actuation modes for single types of robots, these tiny machines tend to have limited versatility while navigating different environments or performing specific tasks. To overcome such limitations, self-assembly microstructures with on-demand reconfiguration capabilities have gained recent attention as the future of biocompatible microrobotics, as they can address drug delivery, microsurgery, and organoid development processes. Reversible modular reconfiguration structures require specific arrangements of particles that can assume several shapes when external fields are applied. We show how magnetic interaction can be used to assemble cylindrical microrobots into modular microstructures with different shapes. The motion actuation of the formed microstructure happens due to an external acoustic field, which generates responsive forces in the air bubbles trapped in the inner cavity of the robots. An external magnetic field can also steer these structures. We illustrate these capabilities by assembling the robots into different shapes that can swim and be steered, showing the potential to perform biomedical applications. Furthermore, we confirm the biocompatibility of the cylindrical microrobot used as the building blocks of our microstructure. Exposing Chinese Hamster Ovary cells to our microrobots for 24 hours demonstrates cell viability when in contact with the microrobot.

Local Manipulation of Skyrmion Nucleation in Microscale Areas of a Thin Film with Nitrogen-Ion Implantation.

Precise manipulation of skyrmion nucleation in microscale or nanoscale areas of thin films is a critical issue in developing high-efficient skyrmionic memories and logic devices. Presently, the mainstream controlling strategies focus on the application of external stimuli to tailor the intrinsic attributes of charge, spin, and lattice. This work reports effective skyrmion manipulation by controllably modifying the lattice defect through ion implantation, which is potentially compatible with large-scale integrated circuit technology. By implanting an appropriate dose of nitrogen ions into a Pt/Co/Ta multilayer film, the defect density was effectively enhanced to induce an apparent modulation of magnetic anisotropy, consequently boosting the skyrmion nucleation. Furthermore, the local control of skyrmions in microscale areas of the macroscopic film was realized by combining the ion implantation with micromachining technology, demonstrating a potential application in both binary storage and multistate storage. These findings provide a new approach to advancing the functionalization and application of skyrmionic devices.

A Self-Assembly of Single Layer of Co Nanorods to Reveal the Magnetostatic Interaction Mechanism.

In this work, we report a self-assembly method to fabricate a single layer of Co nanorods to study their magnetostatic interaction behavior. The Co nanorods with cambered and flat tips were synthesized by using a solvothermal route and an alcohol-thermal method, respectively. Both of them represent hard magnetic features. Co nanorods with cambered tips have an average diameter of 10 nm and length of 100 nm with coercivity of 6.4 kOe, and flat-tip nanorods with a 30 nm diameter and 100 nm length exhibit a coercivity of 4.9 kOe. They are further assembled on the surface of water in assistance of surfactants. The results demonstrate that the assembly type is dependent on the magnetic induction lines direction. For Co nanorods with flat tips, most of magnetic induction lines are parallel to the length direction, leading to an assembly that is tip to tip. For Co nanorods with cambered tips, they are prone to holding together side by side for their random magnetic induction lines. Under an applied field, the Co nanorods with flat tips can be further aligned into a single layer of Co nanorods. Our work gives a possible mechanism for the magnetic interaction of Co nanorods and provides a method to study their magnetic behavior.

Iron Oxide Nanorings and Nanotubes for Magnetic Hyperthermia: The Problem of Intraparticle Interactions.

Magnetic interactions can play an important role in the heating efficiency of magnetic nanoparticles. Although most of the time interparticle magnetic interactions are a dominant source, in specific cases such as multigranular nanostructures intraparticle interactions are also relevant and their effect is significant. In this work, we have prepared two different multigranular magnetic nanostructures of iron oxide, nanorings (NRs) and nanotubes (NTs), with a similar thickness but different lengths (55 nm for NRs and 470 nm for NTs). In this way, we find that the NTs present stronger intraparticle interactions than the NRs. Magnetometry and transverse susceptibility measurements show that the NTs possess a higher effective anisotropy and saturation magnetization. Despite this, the AC hysteresis loops obtained for the NRs (0-400 Oe, 300 kHz) are more squared, therefore giving rise to a higher heating efficiency (maximum specific absorption rate, SARmax = 110 W/g for the NRs and 80 W/g for the NTs at 400 Oe and 300 kHz). These results indicate that the weaker intraparticle interactions in the case of the NRs are in favor of magnetic hyperthermia in comparison with the NTs.

Magnetic Actuation of Hollow Swarming Spheres for Dynamic Catalysis.

Untethered robots with smart human-machine interactions can execute complex activities such as target cargo delivery or assembly of functional scaffolds. However, it remains challenging for fabricating microscale hollow hydrogel robots that can go with autonomous transformation of their geometric formations to adapt to unstructured environments. We herein report hydrogel-based microscopic hollow swarming spheres (HSSs) with anisotropic/isotropic alignments of Fe3O4 particles in the porous wall that can navigate under complex topography conditions by altering their geometric formation, including passing around or jumping over obstacles, assembling into various formation patterns, and swimming in a high-viscosity system. We introduce HSSs into a catalytic reaction model, in which HSSs as a catalyst can shift between water and oil phases to initiate or terminate the decomposition reaction of H2O2. This dynamic catalysis is expected to construct free-radical "living" polymerization for controlling the reaction rate and polymer dispersity index in the future.

Excellent Thermoelectric Performance from In Situ Reaction between Co Nanoparticles and BiSbTe Flexible Films.

Low-cost flexible thermoelectric (TE) films with excellent cooling performance are critical for the in-plane heat dissipation application based on the TE film refrigeration technology. In this work, a flexible film epoxy/Bi0.5Sb1.5Te3 is developed by the incorporation of ferromagnetic Co nanoparticles to improve the electrical transport and cooling performance. The magnetic properties and microstructures clearly indicate that part of Co nanoparticles in situ reacts with Te from Bi0.5Sb1.5Te3 to form CoTe2, as well as BiTe' antisite defects. The electric conductivity is greatly enhanced because of the increased carrier density, while a large Seebeck coefficient is well maintained because of the extra magnetic scattering. The power factor of the flexible film with 0.2 wt % Co nanoparticles reached 2.28 mW·m-1·K-2 at 300 K, increased by 34% compared to the epoxy/Bi0.5Sb1.5Te3 film. The maximum cooling temperature difference is 1.5 times higher compared with the epoxy/Bi0.5Sb1.5Te3 film. This work provides a general method to improve the electrothermal conversion performance of BiSbTe-based flexible films through in situ reaction.

Optical physics on chiral brominated azapirones: Bromophilone A and B.

In this work, we use the visualization method to study their intramolecular electric-magnetic interactions and reveal the physical mechanism of their electronic transition to explain the cause of the opposite ECD spectrum orientations. Azaphilone A and B are two chiral molecules, due to their differing chirality, the electronic circular dichroism (ECD) spectra of bromophilone A and B are very different at 431 nm. Based on the two-step transition process, the charge-transfer characteristics of the corresponding two-photon excited states of the two chiral molecules are analysed in detail by calculating the photoinduced charge transfer and electron-hole coherence in the two-photon absorption (TPA) process.