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The phenomenon of granular magnetoresistance offers the promise of rapid functional materials discovery and high-sensitivity, low-cost sensing technology. Since its discovery over 25 years ago, a major challenge has been the preparation of solids composed of well-characterized, uniform, nanoscale magnetic domains. Rapid advances in colloidal nanochemistry now facilitate the study of more complex and finely controlled materials, enabling the rigorous exploration of the fundamental nature and maximal capabilities of this intriguing class of spintronic materials. We present the first study of size-dependence in granular magnetoresistance using colloidal nanoparticles. These data demonstrate a strongly nonlinear size-dependent magnetoresistance with smaller particles having strong ΔR/R ∼ 18% at 300 K and larger particles showing a 3-fold decline. Importantly, this indicates that CoFe2O4 can act as an effective room temperature granular magnetoresistor and that neither a high superparamagnetic blocking temperature nor a low overall resistance are determining factors in viable magnetoresistance values for sensing applications. These results demonstrate the promise of wider exploration of nontraditional granular structures composed of nanomaterials, molecule-based magnets, and metal-organic frameworks.

Magnetoresistance provides a high-precision, versatile sensing mechanism that has continuously advanced in tandem with methods for top-down engineering of high-precision multilayer devices. Materials composed of solution-prepared nanocrystals can replicate some of the behavior of traditional magnetoresistive stacks but are limited by their intrinsic response mechanism: a gradual shift from low to high resistance with field. To fundamentally alter this behavior, we demonstrate the first instance of any form of spin valve behavior arising from a nanoparticle composite magnetoresistor. Single-layer films of varying CoFe2O4 to Fe3O4 nanoparticle ratios are used to show how the low-field sensitivity can be tuned to values exceeding those of either single-component material. Additionally, the sensitivity is shown to be a simple function of the magnetization of the individual component materials.

The synthesis of iron oxide nanoparticles with control over size and shape has long been an area of research, with iron oleate being arguably the most successful precursor. Issues with reproducibility and versatility in iron oleate-based syntheses remain, however, in large part due to the mutable nature of its structure and stoichiometry. In this work, we characterize two new forms of iron oleate precursor that can be isolated in large quantities, show long-term stability, and have well-defined stoichiometry, leading to reproducible and predictable reactivity. Synthesis with these precursors is shown to produce iron oxide nanoparticles in a tunable size range of 4–16 nm with low size dispersity and properties consistent with magnetite in the superparamagnetic size regime.

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