Tuning the dimensional order in self-assembled magnetic nanostructures: theory, simulations, and experiments.

A major obstacle to building nanoscale magnetic devices or even experimentally studying novel nanomagnetic spin textures is the present lack of a simple and robust method to fabricate various nano-structured alloys. Here, theoretical and experimental investigations were conducted to understand the underlying physical mechanisms of magnetic particle self-assembly in zero applied magnetic field. By changing the amount of NaOH added during the synthesis, we demonstrate that the resulting morphology of the assembled FeCo structure can be tuned from zero-dimensional (0D) nanoparticles to one-dimensional (1D) chains, and even three-dimensional (3D) networks. Two numerical simulations were developed to predict aspects of nanostructure formation by accounting for the magnetic interactions between individual magnetic nanoparticles. The first utilized the Boltzmann distribution to determine the equilibrium structure of a nanochain, iteratively predicting the local deviation angle θ of each particle as it attaches to a forming chain. The second simulation illustrates the differences in nanostructure arrangement and dimensionality (0D, 1D, or 3D) that arise from random interactions at various nanoparticle densities. The simulation results closely match the experimental findings, as seen from SEM images, demonstrating their ability to capture the system's structural properties. In addition, magnetic hysteresis measurements of the samples were performed along two orthogonal directions to show the influence of dimensional order on the magnetic behavior. The normalized remanence (MR/MS||) of the FeCo alloys increases as the dimensions of nanostructures are increased. Of the three cases, the FeCo 3D network structures exhibit the highest normalized nanostructure remanence of 0.33 and an increased coercivity to above 200 Oe at 300 K. This combined numerical and experimental investigation aims to shed light on the preparation of FeCo nanostructures with tailorable dimensional order and it opens new avenues for exploring the complex spin textures and coercive behavior of these multi-dimensional nanomagnetic structures.

Self-Assembly of Magnetic Nanochains in an Intrinsic Magnetic Dipole Force-Dominated Regime.

Magnetic nanoparticle chains offer the anisotropic magnetic properties that are often desirable for micro- and nanoscale systems; however, to date, large-scale fabrication of these nanochains is limited by the need for an external magnetic field during the synthesis. In this work, the unique self-assembly of nanoparticles into chains as a result of their intrinsic dipolar interactions only is examined. In particular, it is shown that in a high concentration reaction regime, the dipole-dipole coupling between two neighboring magnetic iron cobalt (FeCo) nanocubes, was significantly strengthened due to small separation between particles and their high magnetic moments. This dipole-dipole interaction enables the independent alignment and synthesis of magnetic FeCo nanochains without the assistance of any templates, surfactants, or even external magnetic field. Furthermore, the precursor concentration ([M] = 0.016, 0.021, 0.032, 0.048, 0.064, and 0.096 m) that dictates the degree of dipole interaction is examined-a property dependent on particle size and inter-particle distance. By varying the spinner speed, it is demonstrated that the balance between magnetic dipole coupling and fluid dynamics can be used to understand the self-assembly process and control the final structural topology from that of dimers to linear chains (with aspect ratio >10:1) and even to branched networks. Simulations unveil the magnetic and fluid force landscapes that determine the individual nanoparticle interactions and provide a general insight into predicting the resulting nanochain morphology. This work uncovers the enormous potential of an intrinsic magnetic dipole-induced assembly, which is expected to open new doors for efficient fabrication of 1D magnetic materials, and the potential for more complex assemblies with further studies.

Nanoparticle-Based Magnetorheological Elastomers with Enhanced Mechanical Deflection for Haptic Displays.

Haptics allows tactile interactions between humans and digital interfaces. Magnetorheological elastomers (MREs) constitute a promising candidate material for creating the tactile interface of the future─one able to recreate 3D shapes that can be sensed with touch. Furthermore, an MRE formed by using nanoparticles, as opposed to previously used microparticles, is necessary to generate a variety of shapes involving sharp curvatures over small, micrometer-scale horizontal distances to pave the way for haptic displays with microtexture resolution. Here we fabricated both isotropic and anisotropic MREs with different concentrations (2-8 vol % nanoparticles) of soft, low-remanence ferromagnetic nanoparticles. When placed in a magnetic field gradient, isotropic MREs, nonintuitively, show higher deflection than anisotropic MREs, with the former achieving displacement on the order of a millimeter at just 100 mT. This enhanced performance in the isotropic case is explained based on the soft magnetic nature of the nanoparticles. We show that performance improves with magnetic content up to a composition of 6 vol %, where it plateaus. This behavior is attributed to the stiffness of the composite material increasing at a faster rate than the magnetization as the rigid magnetic nanoparticles are added to the elastomeric matrix. Moreover, 6 vol % microparticle-based isotropic and anisotropic MREs were fabricated and compared with the nanoparticle-based MREs. Anisotropic nanoparticle-based films show higher deflection when compared with their microparticle-based counterparts. The latter is only able to match the nanoparticle film deflection at higher applied fields of almost 300 mT. This performance difference between nanoparticle and microparticle-based films is attributed to the increased anisotropic film stiffness resulting from the larger micrometer-size particles. Finally, the optimally designed nanoparticle-based isotropic film was utilized to create a programmable and real-time reconfigurable braille-inspired interface.

Influence of Nonuniform Micron-Scale Strain Distributions on the Electrical Reorientation of Magnetic Microstructures in a Composite Multiferroic Heterostructure.

Composite multiferroic systems, consisting of a piezoelectric substrate coupled with a ferromagnetic thin film, are of great interest from a technological point of view because they offer a path toward the development of ultralow power magnetoelectric devices. The key aspect of those systems is the possibility to control magnetization via an electric field, relying on the magneto-elastic coupling at the interface between the piezoelectric and the ferromagnetic components. Accordingly, a direct measurement of both the electrically induced magnetic behavior and of the piezo-strain driving such behavior is crucial for better understanding and further developing these materials systems. In this work, we measure and characterize the micron-scale strain and magnetic response, as a function of an applied electric field, in a composite multiferroic system composed of 1 and 2 µm squares of Ni fabricated on a prepoled [Pb(Mg1/3Nb2/3)O3]0.69-[PbTiO3]0.31 (PMN-PT) single crystal substrate by X-ray microdiffraction and X-ray photoemission electron microscopy, respectively. These two complementary measurements of the same area on the sample indicate the presence of a nonuniform strain which strongly influences the reorientation of the magnetic state within identical Ni microstructures along the surface of the sample. Micromagnetic simulations confirm these experimental observations. This study emphasizes the critical importance of surface and interface engineering on the micron-scale in composite multiferroic structures and introduces a robust method to characterize future devices on these length scales.