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Abstract 1D multiferroic fibers are known to exhibit attractive characteristics, including enhanced magnetoelectric (ME) coupling compared to thin film and bulk architectures. A comprehensive understanding of composite fibers, however, has been hindered by the complexity of their structure, leading to limited reports. Here, clear and strong ME coupling is experimentally detected in a composite Janus nanofiber aggregate using second harmonic generation (SHG) polarimetry under different magnetic field orientations. The observation of such a pronounced effect using an all‐optical method has not been previously reported in multiferroic fibers. A series of global fits is performed to the SHG polarimetry results to investigate the behavior of nanofibers within an aggregate. We find the magnetically assembled fibers exhibit semi‐cylindrical alignment as well as the expected lengthwise alignment despite variations in size and composition from fiber to fiber. The ME coupling and the semi‐cylindrical alignment seen in SHG are further corroborated via X‐ray diffraction under similar magnetic field conditions. These findings contribute to the development of complex composite and multifunctional devices using multiferroic nanostructures as building blocks, even those with inhomogeneous shapes and geometries. 

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.