Dustin A. Gilbert

Rapid Size-Controlled Synthesis of Dextran-Coated, 64Cu-Doped Iron Oxide Nanoparticles

Research into developing dual modality probes enabled for magnetic resonance imaging (MRI) and positron emission tomography (PET) has been on the rise recently due to the potential to combine the high resolution of MRI and the high sensitivity of PET. Current synthesis techniques for developing multimodal probes is largely hindered in part by prolonged reaction times during radioisotope incorporation--leading to a weakening of the radioactivity. Along with a time-efficient synthesis, the resulting products must fit within a critical size range (between 20 and 100 nm) to increase blood retention time. In this work, we describe a novel, rapid, microwave-based synthesis technique to grow dextran-coated iron oxide nanoparticles doped with copper (DIO/Cu). Traditional methods for coprecipitation of dextran-coated iron oxide nanoparticles require refluxing for 2 h and result in approximately 50 nm diameter particles. We demonstrate that microwave synthesis can produce 50 nm nanoparticles with 5 min of heating. We discuss the various parameters used in the microwave synthesis protocol to vary the size distribution of DIO/Cu and demonstrate the successful incorporation of (64)Cu into these particles with the aim of future use for dual-mode MR/PET imaging.

Quantitative Decoding of Interactions in Tunable Nanomagnet Arrays Using First Order Reversal Curves

To develop a full understanding of interactions in nanomagnet arrays is a persistent challenge, critically impacting their technological acceptance. This paper reports the experimental, numerical and analytical investigation of interactions in arrays of Co nanoellipses using the first-order reversal curve (FORC) technique. A mean-field analysis has revealed the physical mechanisms giving rise to all of the observed features: a shift of the non-interacting FORC-ridge at the low-HC end off the local coercivity HC axis; a stretch of the FORC-ridge at the high-HC end without shifting it off the HC axis; and a formation of a tilted edge connected to the ridge at the low-HC end. Changing from flat to Gaussian coercivity distribution produces a negative feature, bends the ridge, and broadens the edge. Finally, nearest neighbor interactions segment the FORC-ridge. These results demonstrate that the FORC approach provides a comprehensive framework to qualitatively and quantitatively decode interactions in nanomagnet arrays.

Rapid microwave-assisted synthesis of dextran-coated iron oxide nanoparticles for magnetic resonance imaging

Currently, magnetic iron oxide nanoparticles are the only nanosized magnetic resonance imaging (MRI) contrast agents approved for clinical use, yet commercial manufacturing of these agents has been limited or discontinued. Though there is still widespread demand for these particles both for clinical use and research, they are difficult to obtain commercially, and complicated syntheses make in-house preparation unfeasible for most biological research labs or clinics. To make commercial production viable and increase accessibility of these products, it is crucial to develop simple, rapid and reproducible preparations of biocompatible iron oxide nanoparticles. Here, we report a rapid, straightforward microwave-assisted synthesis of superparamagnetic dextran-coated iron oxide nanoparticles. The nanoparticles were produced in two hydrodynamic sizes with differing core morphologies by varying the synthetic method as either a two-step or single-step process. A striking benefit of these methods is the ability to obtain swift and consistent results without the necessity for air-, pH- or temperature-sensitive techniques; therefore, reaction times and complex manufacturing processes are greatly reduced as compared to conventional synthetic methods. This is a great benefit for cost-effective translation to commercial production. The nanoparticles are found to be superparamagnetic and exhibit properties consistent for use in MRI. In addition, the dextran coating imparts the water solubility and biocompatibility necessary for in vivo utilization.

Realization of Ground-State Artificial Skyrmion Lattices at Room Temperature

Magnetic Skyrmions exhibit topologically protected quantum states, not only offering exciting new mechanisms for ultrahigh density and low dissipation information storage, but also providing an ideal platform for explorations of unique topological phenomena. Prerequisite are systems exhibiting skyrmion lattices at ambient conditions. Here, we demonstrate the realization of artificial Bloch skyrmion lattices over extended areas in their ground state at room temperature by patterning asymmetric magnetic nanodots with controlled circularity on an underlayer film with perpendicular magnetic anisotropy (PMA) [1], shown in Fig. 1.

Tuning magnetic anisotropy in (001) oriented L10 (Fe1−xCux)55Pt45 films

We have achieved (001) oriented L10 (Fe1−xCux)55Pt45 thin films, with magnetic anisotropy up to 3.6 × 107 erg/cm3, using atomic-scale multilayer sputtering and post annealing at 400 °C for 10 s. By fixing the Pt concentration, structure and magnetic properties are systematically tuned by the Cu addition. Increasing Cu content results in an increase in the tetragonal distortion of the L10 phase, significant changes to the film microstructure, and lowering of the saturation magnetization and anisotropy. The relatively convenient synthesis conditions, along with the tunable magnetic properties, make such materials highly desirable for future magnetic recording technologies.

Structural and magnetic depth profiles of magneto-ionic heterostructures beyond the interface limit

Electric field control of magnetism provides a promising route towards ultralow power information storage and sensor technologies. The effects of magneto-ionic motion have been prominently featured in the modification of interface characteristics. Here, we demonstrate magnetoelectric coupling moderated by voltage-driven oxygen migration beyond the interface in relatively thick AlOx/GdOx/Co(15 nm) films. Oxygen migration and Co magnetization are quantitatively mapped with polarized neutron reflectometry under electro-thermal conditioning. The depth-resolved profiles uniquely identify interfacial and bulk behaviours and a semi-reversible control of the magnetization. Magnetometry measurements suggest changes in the microstructure which disrupt long-range ferromagnetic ordering, resulting in an additional magnetically soft phase. X-ray spectroscopy confirms changes in the Co oxidation state, but not in the Gd, suggesting that the GdOx transmits oxygen but does not source or sink it. These results together provide crucial insight into controlling magnetism via magneto-ionic motion, both at interfaces and throughout the bulk of the films. Mechanisms allowing electrical manipulation of magnetic material possess potential applications in low power memory and sensor technologies. Here, the authors demonstrate the control of magnetic characteristics via voltage-driven migration of oxygen across a GdOx/Co interface, well into the bulk of the cobalt.Electric-field control of magnetism provides a promising route towards ultralow power information storage and sensor technologies. The effects of magneto-ionic motion have so far been prominently featured in the direct modification of interface chemical and physical characteristics. Here we demonstrate magnetoelectric coupling moderated by voltage-driven oxygen migration beyond the interface limit in relatively thick AlOx/GdOx/Co (15 nm) films. Oxygen migration and its ramifications on the Co magnetization are quantitatively mapped with polarized neutron reflectometry under thermal and electro-thermal conditionings. The depth-resolved profiles uniquely identify interfacial and bulk behaviors and a semi-reversible suppression and recovery of the magnetization. Magnetometry measurements show that the conditioning changes the microstructure so as to disrupt long-range ferromagnetic ordering, resulting in an additional magnetically soft phase. X-ray spectroscopy confirms electric field induced changes in the Co oxidation state but not in the Gd, suggesting that the GdOx transmits oxygen but does not source or sink it. These results together provide crucial insight into controlling magnetic heterostructures via magneto-ionic motion, not only at the interface, but also throughout the bulk of the films.

Controllable Positive Exchange Bias via Redox-Driven Oxygen Migration

Ionic transport in metal/oxide heterostructures offers a highly effective means to tailor material properties via modification of the interfacial characteristics. However, direct observation of ionic motion under buried interfaces and demonstration of its correlation with physical properties has been challenging. Using the strong oxygen affinity of gadolinium, we design a model system of GdxFe1−x/NiCoO bilayer films, where the oxygen migration is observed and manifested in a controlled positive exchange bias over a relatively small cooling field range. The exchange bias characteristics are shown to be the result of an interfacial layer of elemental nickel and cobalt, a few nanometres in thickness, whose moments are larger than expected from uncompensated NiCoO moments. This interface layer is attributed to a redox-driven oxygen migration from NiCoO to the gadolinium, during growth or soon after. These results demonstrate an effective path to tailoring the interfacial characteristics and interlayer exchange coupling in metal/oxide heterostructures.

Chirality control via double vortices in asymmetric Co dots

Reproducible control of the magnetic vortex state in nanomagnets is of critical importance. We report onchirality control by manipulating the size and/or thickness of asymmetric Co dots. Below a critical diameterand/or thickness, chirality control is achieved by the nucleation of a single vortex. Interestingly, above thesecritical dimensions, chirality control is realized by the nucleation and subsequent coalescence of two vortices,resulting in a single vortex with the opposite chirality as found in smaller dots. Micromagnetic simulations andmagnetic force microscopy highlight the role of edge-bound half vortices in facilitating the coalescence process.

Probing the A1 to L10 transformation in FeCuPt using the first order reversal curve method

The A1-L10 phase transformation has been investigated in (001) FeCuPt thin films prepared by atomic-scale multilayer sputtering and rapid thermal annealing (RTA). Traditional x-ray diffraction is not always applicable in generating a true order parameter, due to non-ideal crystallinity of the A1 phase. Using the first-order reversal curve (FORC) method, the A1 and L10 phases are deconvoluted into two distinct features in the FORC distribution, whose relative intensities change with the RTA temperature. The L10 ordering takes place via a nucleation-and-growth mode. A magnetization-based phase fraction is extracted, providing a quantitative measure of the L10 phase homogeneity.

Microwave enhanced silica encapsulation of magnetic nanoparticles

The surface modification of various nanoparticles with silica has been exploited to increase their utility for bioapplications. However, silica encapsulation through conventional methods requires long reaction times (hours to days). Herein, we demonstrated that uniform and spherical silica encapsulation of magnetic nanoparticles can be achieved within 10 min via microwave irradiation after phase transferring monodisperse magnetic nanoparticles from organic to water phase. In addition, we showed that silica shell addition through microwave synthesis is more effective than conventional heating methods, such as a hot plate. The approach that we propose may be useful in preparing multifunctional nano-probes, particularly for radiolabeling, which requires fast preparation times.