Role of Interlayer in 3D Vertically Aligned Nanocomposite Frameworks with Tunable Magnetotransport Properties

Abstract To investigate the role of interlayers on the growth, microstructure, and physical properties of 3D nanocomposite frameworks, a set of novel 3D vertically aligned nanocomposite (VAN) frameworks are assembled by a relatively thin interlayer (M) sandwiched by two consecutively grown La_0.7Sr_0.3MnO₃ (LSMO)‐ZnO VANs layers. ZnO nanopillars from the two VAN layers and the interlayer (M) create a heterogeneous 3D frame embedded in the LSMO matrix. The interlayer (M) includes yttria‐stabilized zirconia (YSZ), CeO₂, SrTiO₃, BaTiO₃, and MgO with in‐plane matching distances increasing from ≈3.63 to ≈4.21 Å, and expected in‐plane strains ranging from tensile (≈8.81% on YSZ interlayer) to compressive (≈–6.23% on MgO interlayer). The metal‐insulator transition temperature increases from ≈133 K (M = YSZ) to ≈252 K (M = MgO), and the low‐field magnetoresistance peak value is tuned from ≈36.7% to ≈20.8%. The 3D heterogeneous frames empower excellent tunable magnetotransport properties and promising potentials for microstructure‐enabled applications.