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Nanomaterials have unique properties, functionalities, and excellent performance, and as a result have gained significant interest across disciplines and industries. However, currently, there is a lack of techniques that can assemble as-synthesized nanomaterials in a scalable manner. Electrophoretic deposition (EPD) is a promising method for the scalable assembly of colloidally stable nanomaterials into thick films and arrays. In EPD, an electric field is used to assemble charged colloidal particles onto an oppositely charged substrate. However, in constant voltage EPD the deposition rate decreases with increasing deposition time, which has been attributed in part to the fact that the electric field in the suspension decreases with time. This decreasing electric field has been attributed to two probable causes, (i) increased resistance of the particle film and/or (ii) the growth of an ion-depletion region at the substrate. Here, to increase EPD yield and scalability we sought to distinguish between these two effects and found that the growth of the ion-depletion region plays the most significant role in the increase of the deposit resistance. Here, we also demonstrate a method to maintain constant deposit resistance in EPD by periodic replenishing of suspension, thereby improving EPD’s scalability. 

Incorporating nanoparticles into devices for a wide range of applications often requires the formation of thick films, which is particularly necessary for improving magnetic power storage, microwave properties, and sensor performance. One approach to assembling nanoparticles into films is the use of electrophoretic deposition (EPD). This work seeks to develop methods to increase film thickness and stability in EPD by increasing film-substrate interactions via functionalizing conductive substrates with various chelating agents. Here, we deposited iron oxide nanoparticles onto conductive substrates functionalized with three chelating agents with different functional moieties and differing chelating strengths. We show that increasing chelating strength can increase film-substrate interactions, resulting in thicker films when compared to traditional EPD. Results will also be presented on how the chelating strength relates to film formation as a function of deposition conditions. Yield for EPD is influenced by deposition conditions including applied electric field, particle concentration, and deposition time. This work shows that the functionalization of substrates with chelating agents that coordinate strongly with nanoparticles (phosphonic acid and dopamine) overcome parameters that traditionally hinder the deposition of thicker and more stable films, such as applied electric field and high particle concentration. We show that functionalizing substrates with chelating agents is a promising method to fabricate thick, stable films of nanoparticles deposited via EPD over a larger processing space by increasing film-substrate interactions. 

For modern switching power supplies, current bulk magnetic materials, such as ferrites or magnetic metal alloys, cannot provide both low loss and high magnetic saturation to function with both high power density and high efficiency at high frequencies (10-100 MHz). Magnetic nanocomposites comprised of a ferrite and magnetic metal alloy provide the opportunity to achieve these desired magnetic properties, but previously investigated thin-film fabrication techniques have difficulty achieving multi-micrometer film thicknesses which are necessary to provide practical magnetic energy storage and power handling. Here, we present a versatile technique to fabricate thick magnetic nanocomposites via a two-step process, consisting of the electrophoretic deposition of an iron oxide nanoparticle phase into a mold on a substrate, followed by electro-infiltration of a nickel matrix. The deposited films are imaged via scanning electron microscopy and energy dispersive X-ray spectroscopy to identify the presence of iron and nickel, confirming the infiltration of the nickel between the iron oxide nanoparticles. A film thickness of ∼7 μm was measured via stylus profilometry. Further confirmation of successful composite formation is obtained with vibrating sample magnetometry, showing the saturation magnetization value of the composite (473 kA/m) falls between that of the iron oxide nanoparticles (280 kA/m) and the nickel matrix (555 kA/m). These results demonstrate the potential of electrophoretic deposition coupled with electro-infiltration to fabricate magnetic nanocomposite films. 

Magnetic nanocomposites with 0-3 connectivity, whereby a 0D magnetic nanoparticle phase is embedded into a 3D magnetic metal matrix phase, have gained increased interest for use in applications ranging from integrated power inductor cores to exchange-spring magnets. The electro-infiltration process, in which a metal phase is electroplated through a nanoparticle film phase, is an inexpensive approach compatible with semiconductor fabrication methods for the formation of these nanocomposites. Past demonstrations of electro-infiltrated nanocomposites have relied on scanning electron microscopy and energy dispersive x-ray spectroscopy to evaluate the 0-3 composite structure. However, a detailed investigation of the boundary between the particle and metal matrix phases cannot be performed with these tools, and it is unknown whether the particle/matrix interfaces are dense and void-free. This detail is critical, as the presence of even nanoscale voids would affect any potential magnetic exchange coupling and hence the overall electromagnetic properties of the material. This work seeks to explore the phase boundary of 0-3 magnetic nanocomposite fabricated by electro-infiltration by using scanning transmission electron microscopy and energy-dispersive x-ray spectroscopy to analyze the nanostructure of two different composites—a nickel/iron-oxide composite and a permalloy/iron-oxide composite. High-resolution imaging indicates that the interface between the particle phase and matrix phase is dense and void-free. These results will help guide future studies on the design and implementation of these magnetic nanocomposites for end applications.