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Abstract Nanocomposite thin films, comprising two or more distinct materials at nanoscale, have attracted significant research interest considering their potential of integrating multiple functionalities for advanced applications in electronics, energy storage, photonics, photovoltaics, and sensing. Among various fabrication technologies, a one-step pulsed laser deposition process enables the self-assembly of materials into vertically aligned nanocomposites (VANs). The demonstrated VAN systems include oxide–oxide, oxide–metal, and nitride–metal VAN films and their growth mechanisms are vastly different. These complexities pose challenges in the designs, materials selection, and prediction of the resulted VAN morphologies and properties. The review examines the key roles that surface energy plays in the VAN growth and provides a generalized materials design guideline combining the two key factors of surface energy and lattice strain/mismatch, along with other factors related to growth kinetics that collectively influence the morphology of VAN films. This review aims to offer valuable guidelines for future material selection and microstructure design in the development of self-assembled VAN films. 

ZnO-Au nanocomposite thin films have been previously reported as hybrid metamaterials with unique optical properties such as plasmonic resonance properties and hyperbolic behaviors. In this study, Au composition in the ZnO-Au nanocomposites has been effectively tuned by target composition variation and thus resulted in microstructure and optical property tuning. Specifically, all the ZnO-Au nanocomposite thin films grown through the pulsed laser deposition (PLD) method show obvious vertically aligned nanocomposite (VAN) structure with the Au nanopillars embedded in the ZnO matrix. Moreover, the average diameter of Au nanopillars increases as Au concentration increases, which also leads to the redshifts in the surface plasmon resonance (SPR) wavelength and changes in the hyperbolic behaviors of the films. As a whole, this work discusses how strain-driven tuning of optical properties and microstructure resulted through a novel Au concentration variation approach which has not been previously attempted in the ZnO-Au thin film system. These highly ordered films present great promise in the areas of sensing, waveguides, and nanophotonics to name a few. 

Abstract Hybrid metamaterials (HMs) have attracted significant research interests owing to their unique optical properties and their ability to manipulate light‐matter interaction in a novel and controlled fashion beyond what any single material offers. Especially 3D HMs are of great interest due to their potential to provide advanced and precise control of such light‐matter interaction in nanoscale. In this study, a set of 3D HM nanocomposite films are designed by integrating three phases, i.e., vertically aligned CoFe₂nanosheets within the matrix of TiN/TaN multilayers. By increasing the number of TiN/TaN multilayers from 2 to 19, a high degree of tunability in optical property has been demonstrated, including well‐tailored optical permittivity, and tunable hyperbolic dispersion from Type‐II to Type‐I. Ferromagnetic CoFe₂nanosheets introduces novel magnetic responses, such as magnetic anisotropy and enhanced coercivity. Furthermore, in situ heating X‐ray diffraction (XRD) suggests good thermal stability of the 3D nanocomposite films up to the measured temperature of 600 °C. This three‐phase 3D nanocomposite design offers more flexibility in HM designs, multifunctionalities, and phase stability, compared with the typical two‐phase HMs toward future metamaterials by design. 

Abstract Flexible and wearable sensors show enormous potential for personalized healthcare devices by real‐time monitoring of an individual's health. Typically, a single functional material is selected for one sensor to sense a particular physical signal while multiple materials will be selected for multi‐mode sensing. Vertically aligned nanocomposites (VANs) have recently demonstrated various material combinations and novel coupled multifunctionalities that are hard to achieve in any single‐phase material alone, including multiphase multiferroics, magneto‐optic coupling, and strong magnetic and optical anisotropy. Integrating these novel VANs into wearable sensors shows enormous potential in multi‐mode sensing owing to their multifunctional nature. In this work, the transfer of VANs onto polydimethylsiloxane as a novel flexible chemical and pressure sensor is demonstrated. For this demonstration, the classical BaTiO₃‐Au VAN with combined plasmonic and piezoelectric properties is used to demonstrate a multi‐sensing mechanism. A thin water‐soluble buffer of Sr₃Al₂O₆serves as a buffer layer for the epitaxial growth and transfer process. The electrical output based on the piezoelectric responses and identifying 4‐mercaptobenzoic acid by surface‐enhanced Raman spectroscopy reveal great potential for free‐standing VANs in a wearable multifunctional sensing platform.