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  1. Two-dimensional (2D) materials with robust ferromagnetic behavior have attracted great interest because of their potential applications in next-generation nanoelectronic devices. Aside from graphene and transition metal dichalcogenides, Bi-based layered oxide materials are a group of prospective candidates due to their superior room-temperature multiferroic response. Here, an ultrathin Bi 3 Fe 2 Mn 2 O 10+ δ layered supercell (BFMO322 LS) structure was deposited on an LaAlO 3 (LAO) (001) substrate using pulsed laser deposition. Microstructural analysis suggests that a layered supercell (LS) structure consisting of two-layer-thick Bi–O slabs and two-layer-thick Mn/Fe–O octahedra slabs was formed on top of the pseudo-perovskite interlayer (IL). A robust saturation magnetization value of 129 and 96 emu cm −3 is achieved in a 12.3 nm thick film in the in-plane (IP) and out-of-plane (OP) directions, respectively. The ferromagnetism, dielectric permittivity, and optical bandgap of the ultrathin BFMO films can be effectively tuned by thickness and morphology variation. In addition, the anisotropy of all ultrathin BFMO films switches from OP dominating to IP dominating as the thickness increases. This study demonstrates the ultrathin BFMO film with tunable multifunctionalities as a promising candidate for novel integrated spintronic devices. 
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    Integration of highly anisotropic multiferroic thin films on silicon substrates is a critical step towards low-cost devices, especially high-speed and low-power consumption memories. In this work, an oxide–metal vertically aligned nanocomposite (VAN) platform has been used to successfully demonstrate self-assembled multiferroic BaTiO 3 –Fe (BTO–Fe) nanocomposite films with high structural anisotropy on Si substrates. The effects of various buffer layers on the crystallinity, microstructure, and physical properties of the BTO–Fe films have been explored. With an appropriate buffer layer design, e.g. SrTiO 3 /TiN bilayer buffer, the epitaxial quality of the BTO matrix and the anisotropy of the Fe nanopillars can be improved greatly, which in turn enhances the physical properties, including the ferromagnetic, ferroelectric, and optical response of the BTO–Fe thin films. This unique combination of properties integrated on Si offers a promising approach in the design of multifunctional nanocomposites for Si-based memories and optical devices. 
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    A new two-phase BaTiO 3  : La 0.7 Sr 0.3 MnO 3 nanocomposite system with a molar ratio of 8 : 2 has been grown on single crystal SrTiO 3 (001) substrates using a one-step pulsed laser deposition technique. Vertically aligned nanocomposite thin films with ultra-thin La 0.7 Sr 0.3 MnO 3 pillars embedded in the BaTiO 3 matrix have been obtained and the geometry of the pillars varies with deposition frequency. The room temperature multiferroic properties, including ferromagnetism and ferroelectricity, have been demonstrated. Anisotropic ferromagnetism and dielectric constants have been observed, which can be tuned by deposition frequencies. The tunable anisotropic optical properties originated from the conducting pillars in the dielectric matrix structure, which cause different electron transport paths. In addition, tunable band gaps have been discovered in the nanocomposites. This multiferroic and anisotropic system has shown its great potentials towards multiferroics and non-linear optics. 
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