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Register a new userAssembly-mediated Interplay of Dipolar Interactions and Surface Spin Disorder in Colloidal Maghemite Nanoclusters
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Controlled assembly of single-crystal, colloidal maghemite nanoparticles is facilitated via a high-temperature polyol-based pathway. Structural characterization shows that size-tunable nanoclusters of 50 and 86 nm diameters (D), with high dispersibility in aqueous media, are composed of $sim$ 13 nm (d) crystallographically oriented nanoparticles. The interaction effects are examined against the increasing volume fraction, $phi$, of the inorganic magnetic phase that goes from individual colloidal nanoparticles ($phi$= 0.47) to clusters ($phi$= 0.72). The frozen-liquid dispersions of the latter exhibit weak ferrimagnetic behavior at 300 K. Comparative Mossbauer spectroscopic studies imply that intra-cluster interactions come into play. A new insight emerges from the clusters temperature-dependent ac susceptibility that displays two maxima in $chi$(T), with strong frequency dispersion. Scaling-law analysis, together with the observed memory effects suggest that a superspin glass state settles-in at T$_{B}$ $sim$ 160-200 K, while at lower-temperatures, surface spin-glass freezing is established at T$_{f}$ $sim$40- 70 K. In such nanoparticle-assembled systems, with increased $phi$, Monte Carlo simulations corroborate the role of the inter-particle dipolar interactions and that of the constituent nanoparticles surface spin disorder in the emerging spin-glass dynamics.
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We study the interplay between the effects of surface anisotropy and dipolar interactions in monodisperse assemblies of nanomagnets with oriented anisotropy. We derive asymptotic formulas for the assembly magnetization taking account of temperature, applied field, core and surface anisotropy, and dipolar inter-particle interactions. We find that the interplay between surface anisotropy and dipolar interactions is well described by the analytical expression of the assembly magnetization derived here: the overall sign of the product of the two parameters governing the surface and the dipolar contributions determines whether intrinsic and collective terms compete or have synergistic effects on the magnetization. This is illustrated by the magnetization curves of $gamma-Fe_{2}O_{3}$ nanoparticles assemblies in the low concentration limit.
Elevated-temperature polyol-based colloidal-chemistry approach allows for the development of size-tunable (50 and 86 nm) assemblies of maghemite iso-oriented nanocrystals, with enhanced magnetization. 1H-Nuclear Magnetic Resonance (NMR) relaxometric experiments show that the ferrimagnetic cluster-like colloidal entities exhibit a remarkable enhancement (4 to 5 times) in the transverse relaxivity, if compared to that of the superparamagnetic contrast agent Endorem, over an extended frequency range (1-60 MHz). The marked increase of the transverse relaxivity r2 at a clinical magnetic field strength (1.41 T), which is 405.1 and 508.3 mM-1 s-1 for small and large assemblies respectively, allows to relate the observed response to the raised intra-aggregate magnetic material volume fraction. Furthermore, cell tests with murine fibroblast culture medium confirmed the cell viability in presence of the clusters. We discuss the NMR dispersion profiles on the basis of relaxivity models to highlight the magneto-structural characteristics of the materials for improved T2-weighted magnetic resonance images.
We report the observation of a spin-orbit torque (SOT) originating from the surface Rashba-Edelstein effect. We found that the SOT in a prototypical spin-orbitronic system, a Pt/Co bilayer, can be manipulated by molecular self-assembly on the Pt surface. This evidences that the Rashba spin-orbit coupling at the Pt surface generates a sizable SOT, which has been hidden by the strong bulk and interface spin-orbit coupling. We show that the molecular tuning of the surface Rashba-Edelstein SOT is consistent with density functional theory calculations. These results illustrate the crucial role of the surface spin-orbit coupling in the SOT generation, which alters the landscape of metallic spin-orbitronic devices.
We investigate the effective interaction between two randomly charged but otherwise net-neutral, planar dielectric slabs immersed in an asymmetric Coulomb fluid containing a mixture of mobile monovalent and multivalent ions. The presence of charge disorder on the apposed bounding surfaces of the slabs leads to substantial qualitative changes in the way they interact, as compared with the standard picture provided by the van der Waals and image-induced, ion-depletion interactions. While, the latter predict purely attractive interactions between strictly neutral slabs, we show that the combined effects from surface charge disorder, image depletion, Debye (or salt) screening and also, in particular, their coupling with multivalent ions, give rise to a more diverse behavior for the effective interaction between net-neutral slabs. Disorder effects show large variation depending on the properly quantified strength of disorder, leading either to non-monotonic effective interaction with both repulsive and attractive branches when the surface charges are weakly disordered (small disorder variance) or to a dominating attractive interaction that is larger both in its range and magnitude than what is predicted from the van der Waals and image-induced, ion-depletion interactions, when the surfaces are strongly disordered (large disorder variance).
In the present work, we investigate the magnetic properties of ferrimagnetic and noninteracting maghemite (g-Fe2O3) hollow nanoparticles obtained by the Kirkendall effect. From the experimental characterization of their magnetic behavior, we find that polycrystalline hollow maghemite nanoparticles are characterized by low superparamagnetic-to-ferromagnetic transition temperatures, small magnetic moments, significant coercivities and irreversibility fields, and no magnetic saturation on external magnetic fields up to 5 T. These results are interpreted in terms of the microstructural parameters characterizing the maghemite shells by means of an atomistic Monte Carlo simulation of an individual spherical shell model. The model comprises strongly interacting crystallographic domains arranged in a spherical shell with random orientations and anisotropy axis. The Monte Carlo simulation allows discernment between the influence of the structure polycrystalline and its hollow geometry, while revealing the magnetic domain arrangement in the different temperature regimes.
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