Self-Propulsion by Directed Explosive Emulsification.

An active droplet system, programmed to repeatedly move autonomously at a specific velocity in a well-defined direction, is demonstrated. Coulombic energy is stored in oversaturated interfacial assemblies of charged nanoparticle-surfactants by an applied DC electric field and can be released on demand. Spontaneous emulsification is suppressed by an increase in the stiffness of the oversaturated assemblies. Rapidly removing the field releases the stored energy in an explosive event that propels the droplet, where thousands of charged microdroplets are ballistically ejected from the surface of the parent droplet. The ejection is made directional by a symmetry breaking of the interfacial assembly, and the combined interaction force of the microdroplet plume on one side of the droplet propels the droplet distances tens of times its size, making the droplet active. The propulsion is autonomous, repeatable, and agnostic to the chemical composition of the nanoparticles. The symmetry-breaking in the nanoparticle assembly controls the microdroplet velocity and direction of propulsion. This mechanism of droplet propulsion will advance soft micro-robotics, establishes a new type of active matter, and introduces new vehicles for compartmentalized delivery.

Magnetocapacitance at the Ni/BiInO3 Schottky Interface.

We report the observation of a magnetocapacitance effect at the interface between Ni and epitaxial nonpolar BiInO3 thin films at room temperature. A detailed surface study using X-ray photoelectron spectroscopy (XPS) reveals the formation of an intermetallic Ni-Bi alloy at the Ni/BiInO3 interface and a shift in the Bi 4f and In 3d core levels to higher binding energies with increasing Ni thickness. The latter infers band bending in BiInO3, corresponding to the formation of a p-type Schottky barrier. The current-voltage characteristics of the Ni/BiInO3/(Ba,Sr)RuO3/NdScO3(110) heterostructure show a significant dependence on the applied magnetic field and voltage cycling, which can be attributed to voltage-controlled band bending and spin-polarized charge accumulation in the vicinity of the Ni/BiInO3 interface. The magnetocapacitance effect can be realized at room temperature without involving multiferroic materials.

Angular dependence of the magnetization relaxation in Co/Pt multilayers.

We study the influence of defects in Co/Pt multilayers on the room-temperature magnetization reversal and relaxation mechanisms via angle-dependent magnetic viscosity and coercive field measurements. The data reveal a transition from pinning-dominated domain wall propagation to a sequence of pinning-dominated and uniform switching, with increasing tilt away from the normal direction. The leading role of the dendritic domain wall propagation in the nanogranular exchange-coupled films is corroborated by the scaling of relaxation times, the angular dependence of the coercive field, and Kerr microscopy.

Ferromagnetic resonators synthesized by metal-organic decomposition epitaxy.

Metal-organic decomposition epitaxy is an economical wet-chemical approach suitable to synthesize high-quality low-spin-damping films for resonator and oscillator applications. This work reports the temperature dependence of ferromagnetic resonances and associated structural and magnetic quantities of yttrium iron garnet nanofilms that coincide with single-crystal values. Despite imperfections originating from wet-chemical deposition and spin coating, the quality factor for out-of-plane and in-plane resonances approaches 600 and 1000, respectively, at room temperature and 40 GHz. These values increase with temperature and are 100 times larger than those offered by commercial devices based on complementary metal-oxide semiconductor voltage-controlled oscillators at comparable production costs.

Evidence of symmetry breaking in a Gd2 di-nuclear molecular polymer.

A chiral 3D coordination compound, [Gd2(L)2(ox)2(H2O)2], arranged around a dinuclear Gd unit has been characterized by X-ray photoemission and X-ray absorption measurements in the context of density functional theory studies. Core level photoemission of the Gd 5p multiplet splittings indicates that spin orbit coupling dominates over j-J coupling evident in the 5p core level spectra of Gd metal. Indications of spin-orbit coupling are consistent with the absence of inversion symmetry due to the ligand field. Density functional theory predicts antiferromagnet alignment of the Gd2 dimers and a band gap of the compound consistent with optical absorption.

Electronic structure of cobalt valence tautomeric molecules in different environments.

Future molecular microelectronics require the electronic conductivity of the device to be tunable without impairing the voltage control of the molecular electronic properties. This work reports the influence of an interface between a semiconducting polyaniline polymer or a polar poly-D-lysine molecular film and one of two valence tautomeric complexes, i.e., [CoIII(SQ)(Cat)(4-CN-py)2] ↔ [CoII(SQ)2(4-CN-py)2] and [CoIII(SQ)(Cat)(3-tpp)2] ↔ [CoII(SQ)2(3-tpp)2]. The electronic transitions and orbitals are identified using X-ray photoemission, X-ray absorption, inverse photoemission, and optical absorption spectroscopy measurements that are guided by density functional theory. Except for slightly modified binding energies and shifted orbital levels, the choice of the underlying substrate layer has little effect on the electronic structure. A prominent unoccupied ligand-to-metal charge transfer state exists in [CoIII(SQ)(Cat)(3-tpp)2] ↔ [CoII(SQ)2(3-tpp)2] that is virtually insensitive to the interface between the polymer and tautomeric complexes in the CoII high-spin state.

Evidence of dynamical effects and critical field in a cobalt spin crossover complex.

The [Co(SQ)2(4-CN-py)2] complex exhibits dynamical effects over a wide range of temperature. The orbital moment, determined by X-ray magnetic circular dichroism (XMCD) with decreasing applied magnetic field, indicates a nonzero critical field for net alignment of magnetic moments, an effect not seen with the spin moment of [Co(SQ)2(4-CN-py)2].

Ferromagnetic liquid droplets with adjustable magnetic properties.

The assembly and jamming of magnetic nanoparticles (NPs) at liquid-liquid interfaces is a versatile platform to endow structured liquid droplets with a magnetization, i.e., producing ferromagnetic liquid droplets (FMLDs). Here, we use hydrodynamics experiments to probe how the magnetization of FMLDs and their response to external stimuli can be tuned by chemical, structural, and magnetic means. The remanent magnetization stems from magnetic NPs jammed at the liquid-liquid interface and dispersed NPs magneto-statically coupled to the interface. FMLDs form even at low concentrations of magnetic NPs when mixing nonmagnetic and magnetic NPs, since the underlying magnetic dipole-driven clustering of magnetic NP-surfactants at the interface produces local magnetic properties, similar to those found with pure magnetic NP solutions. While the net magnetization is smaller, such a clustering of NPs may enable structured liquids with heterogeneous surfaces.

Chiral Spin Textures in Amorphous Iron-Germanium Thick Films.

Topological solitary fields, such as magnetic and polar skyrmions, are envisioned to revolutionize microelectronics. These configurations have been stabilized in solid-state materials with a global inversion symmetry breaking, which translates in magnetic materials into a vector spin exchange known as the Dzyaloshinskii-Moriya interaction (DMI), as well as spin chirality selection and isotropic solitons. This work reports experimental evidence of 3D chiral spin textures, such as helical spins and skyrmions with different chirality and topological charge, stabilized in amorphous Fe-Ge thick films. These results demonstrate that structurally and chemically disordered materials with a random DMI can resemble inversion symmetry broken systems with similar magnetic properties, moments, and states. Disordered systems are distinguished from systems with global inversion symmetry breaking by their degenerate spin chirality that allows for forming isotropic and anisotropic topological spin textures at remanence, while offering greater flexibility in materials synthesis, voltage, and strain manipulation.

The effect of Cu additions in FePt-BN-SiO2 heat-assisted magnetic recording media.

Structural and chemical order impact magnetic properties of solids, which are governed by spin-orbit coupling and exchange interaction. The ordered L10 phase of FePt is a key material to heat-assisted magnetic recording; to enable high storage density, a solid understanding is needed of structural and chemical disorder at small length scales, as well as associated modifications of the electronic band structure. Here, we investigate the effect of boron and copper additions (≲6 mol% Cu) on structural and magnetic properties of L10 FePt granular media. Two copper-driven mechanisms, although competing, can lead to improvements in both structural and magnetic properties. In particular, the Cu substitution on the Fe-site leads to a degradation of magnetic properties due to the delocalized electron orbitals originating from a larger Cu d-orbital occupancy. At the same time, Cu substitution leads to an enhanced crystallographic order and consequently magneto-crystalline anisotropy, which offsets the former effect to a large extent. Our study is based on magnetometry, x-ray absorption spectroscopy, ab-initio calculations and a phenomenological theory of disordered FePt granular media. We do not observe a sizable modification to Fe moments and electronic configuration; Cu reveals two different resonances associated with the presence and absence of Cu-B bonds that vary with total Cu concentration.

Perspective: Ferromagnetic Liquids.

Mechanical jamming of nanoparticles at liquid-liquid interfaces has evolved into a versatile approach to structure liquids with solid-state properties. Ferromagnetic liquids obtain their physical and magnetic properties, including a remanent magnetization that distinguishes them from ferrofluids, from the jamming of magnetic nanoparticles assembled at the interface between two distinct liquids to minimize surface tension. This perspective provides an overview of recent progress and discusses future directions, challenges and potential applications of jamming magnetic nanoparticles with regard to 3D nano-magnetism. We address the formation and characterization of curved magnetic geometries, and spin frustration between dipole-coupled nanostructures, and advance our understanding of particle jamming at liquid-liquid interfaces.

Reconfigurable ferromagnetic liquid droplets.

Solid ferromagnetic materials are rigid in shape and cannot be reconfigured. Ferrofluids, although reconfigurable, are paramagnetic at room temperature and lose their magnetization when the applied magnetic field is removed. Here, we show a reversible paramagnetic-to-ferromagnetic transformation of ferrofluid droplets by the jamming of a monolayer of magnetic nanoparticles assembled at the water-oil interface. These ferromagnetic liquid droplets exhibit a finite coercivity and remanent magnetization. They can be easily reconfigured into different shapes while preserving the magnetic properties of solid ferromagnets with classic north-south dipole interactions. Their translational and rotational motions can be actuated remotely and precisely by an external magnetic field, inspiring studies on active matter, energy-dissipative assemblies, and programmable liquid constructs.

Spatial and Temporal Correlations of XY Macro Spins.

We use nano disk arrays with square and honeycomb symmetry to investigate magnetic phases and spin correlations of XY dipolar systems at the micro scale. Utilizing magnetization sensitive X-ray photoemission electron microscopy, we probe magnetic ground states and the "order-by-disorder" phenomenon predicted 30 years ago. We observe the antiferromagnetic striped ground state in square lattices, and 6-fold symmetric structures, including trigonal vortex lattices and disordered floating vortices, in the honeycomb lattice. The spin frustration in the honeycomb lattice causes a phase transition from a long-range ordered locked phase over a floating phase with quasi long-range order and indications of a Berezinskii-Thouless-Kosterlitz-like character, to the thermally excited paramagnetic state. Absent spatial correlation and quasi periodic switching of isolated vortices in the quasi long-range ordered phase suggest a degeneracy of the vortex circulation.

Experimental Evidence of Chiral Ferrimagnetism in Amorphous GdCo Films.

Inversion symmetry breaking has become a vital research area in modern magnetism with phenomena including the Rashba effect, spin Hall effect, and the Dzyaloshinskii-Moriya interaction (DMI)-a vector spin exchange. The latter one may stabilize chiral spin textures with topologically nontrivial properties, such as Skyrmions. So far, chiral spin textures have mainly been studied in helimagnets and thin ferromagnets with heavy-element capping. Here, the concept of chirality driven by interfacial DMI is generalized to complex multicomponent systems and demonstrated on the example of chiral ferrimagnetism in amorphous GdCo films. Utilizing Lorentz microscopy and X-ray magnetic circular dichroism spectroscopy, and tailoring thickness, capping, and rare-earth composition, reveal that 2 nm thick GdCo films preserve ferrimagnetism and stabilize chiral domain walls. The type of chiral domain walls depends on the rare-earth composition/saturation magnetization, enabling a possible temperature control of the intrinsic properties of ferrimagnetic domain walls.

Magnetically Patterned Rolled-Up Exchange Bias Tubes: A Paternoster for Superparamagnetic Beads.

We realized a deterministic transport system for superparamagnetic microbeads through micrometer-sized tubes acting as channels. Beads are moved stepwise in a paternoster-like manner through the tube and back on top of it by weak magnetic field pulses without changing the field pulse polarity and taking advantage of the magnetic stray field emerging from the tubular structures. The microtubes are engineered by rolling up exchange bias layer systems, magnetically patterned into parallel stripe magnetic domains. In this way, the tubes possess distinct azimuthally aligned magnetic domain patterns. This transport mechanism features high step velocities and remote control of not only the direction and trajectory but also the velocity of the transport without the need of fuel or catalytic material. Therefore, this approach has the potential to impact several fields of 3D applications in biotechnology, including particle transport related phenomena in lab-on-a-chip and lab-in-a-tube devices.

Retrieving spin textures on curved magnetic thin films with full-field soft X-ray microscopies.

X-ray tomography is a well-established technique to characterize 3D structures in material sciences and biology; its magnetic analogue--magnetic X-ray tomography--is yet to be developed. Here we demonstrate the visualization and reconstruction of magnetic domain structures in a 3D curved magnetic thin films with tubular shape by means of full-field soft X-ray microscopies. The 3D arrangement of the magnetization is retrieved from a set of 2D projections by analysing the evolution of the magnetic contrast with varying projection angle. Using reconstruction algorithms to analyse the angular evolution of 2D projections provides quantitative information about domain patterns and magnetic coupling phenomena between windings of azimuthally and radially magnetized tubular objects. The present approach represents a first milestone towards visualizing magnetization textures of 3D curved thin films with virtually arbitrary shape.

Manipulating topological states by imprinting non-collinear spin textures.

Topological magnetic states, such as chiral skyrmions, are of great scientific interest and show huge potential for novel spintronics applications, provided their topological charges can be fully controlled. So far skyrmionic textures have been observed in noncentrosymmetric crystalline materials with low symmetry and at low temperatures. We propose theoretically and demonstrate experimentally the design of spin textures with topological charge densities that can be tailored at ambient temperatures. Tuning the interlayer coupling in vertically stacked nanopatterned magnetic heterostructures, such as a model system of a Co/Pd multilayer coupled to Permalloy, the in-plane non-collinear spin texture of one layer can be imprinted into the out-of-plane magnetised material. We observe distinct spin textures, e.g. vortices, magnetic swirls with tunable opening angle, donut states and skyrmion core configurations. We show that applying a small magnetic field, a reliable switching between topologically distinct textures can be achieved at remanence.

Imaging of buried 3D magnetic rolled-up nanomembranes.

Increasing performance and enabling novel functionalities of microelectronic devices, such as three-dimensional (3D) on-chip architectures in optics, electronics, and magnetics, calls for new approaches in both fabrication and characterization. Up to now, 3D magnetic architectures had mainly been studied by integral means without providing insight into local magnetic microstructures that determine the device performance. We prove a concept that allows for imaging magnetic domain patterns in buried 3D objects, for example, magnetic tubular architectures with multiple windings. The approach is based on utilizing the shadow contrast in transmission X-ray magnetic circular dichroism (XMCD) photoemission electron microscopy and correlating the observed 2D projection of the 3D magnetic domains with simulated XMCD patterns. That way, we are not only able to assess magnetic states but also monitor the field-driven evolution of the magnetic domain patterns in individual windings of buried magnetic rolled-up nanomembranes.

Magnetic microstructure of rolled-up single-layer ferromagnetic nanomembranes.

The magnetic microstructure of rolled-up magnetic nanomembranes is revealed both theoretically and experimentally. Two types of nanomembranes are considered, one with a non-magnetic spacer layer and the other without. Experimentally, by using different materials and tuning the dimensions of the rolled-up nanomembranes, domain patterns consisting of spiral-like and azimuthally magnetized domains are observed, which are in qualitative agreement with the theoretical predictions.