Hyperbolic metamaterials (HMM) possess significant anisotropic physical properties and tunability and thus find many applications in integrated photonic devices. HMMs consisting of metal and dielectric phases in either multilayer or vertically aligned nanocomposites (VAN) form are demonstrated with different hyperbolic properties. Herein, self‐assembled HfO2‐Au/TiN‐Au multilayer thin films, combining both the multilayer and VAN designs, are demonstrated. Specifically, Au nanopillars embedded in HfO2and TiN layers forming the alternative layers of HfO2‐Au VAN and TiN‐Au VAN. The HfO2and TiN layer thickness is carefully controlled by varying laser pulses during pulsed laser deposition (PLD). Interestingly, tunable anisotropic physical properties can be achieved by adjusting the bi‐layer thickness and the number of the bi‐layers. Type II optical hyperbolic dispersion can be obtained from high layer thickness structure (e.g., 20 nm), while it can be transformed into Type I optical hyperbolic dispersion by reducing the thickness to a proper value (e.g., 4 nm). This new nanoscale hybrid metamaterial structure with the three‐phase VAN design shows great potential for tailorable optical components in future integrated devices.
Single-Step Fabrication of Au-Fe-BaTiO3 Nanocomposite Thin Films Embedded with Non-Equilibrium Au-Fe Alloyed Nanostructures
Nanocomposite thin film materials present great opportunities in coupling materials and functionalities in unique nanostructures including nanoparticles-in-matrix, vertically aligned nanocomposites (VANs), and nanolayers. Interestingly the nanocomposites processed through a non-equilibrium processing method, e.g., pulsed laser deposition (PLD), often possess unique metastable phases and microstructures that could not achieve using equilibrium techniques, and thus lead to novel physical properties. In this work, a unique three-phase system composed of BaTiO3 (BTO), with two immiscible metals, Au and Fe, is demonstrated. By adjusting the deposition laser frequency from 2 Hz to 10 Hz, the phase and morphology of Au and Fe nanoparticles in BTO matrix vary from separated Au and Fe nanoparticles to well-mixed Au-Fe alloy pillars. This is attributed to the non-equilibrium process of PLD and the limited diffusion under high laser frequency (e.g., 10 Hz). The magnetic and optical properties are effectively tuned based on the morphology variation. This work demonstrates the stabilization of non-equilibrium alloy structures in the VAN form and allows for the exploration of new non-equilibrium materials systems and their properties that could not be easily achieved through traditional equilibrium methods.
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- NSF-PAR ID:
- 10415789
- Date Published:
- Journal Name:
- Nanomaterials
- Volume:
- 12
- Issue:
- 19
- ISSN:
- 2079-4991
- Page Range / eLocation ID:
- 3460
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract -
null (Ed.)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.more » « less
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Bacterial cellulose nanocrystals (BCNCs) are biocompatible cellulose nanomaterials that can host guest nanoparticles to form hybrid nanocomposites with a wide range of applications. Herein, we report the synthesis of a hybrid nanocomposite that consists of plasmonic gold nanoparticles (AuNPs) and superparamagnetic iron oxide (Fe 3 O 4 ) nanoparticles supported on BCNCs. As a proof of concept, the hybrid nanocomposites were employed to isolate and detect malachite green isothiocyanate (MGITC) via magnetic separation and surface-enhanced Raman scattering (SERS). Different initial gold precursor (Au 3+ ) concentrations altered the size and morphology of the AuNPs formed on the nanocomposites. The use of 5 and 10 mM Au 3+ led to a heterogenous mix of spherical and nanoplate AuNPs with increased SERS enhancements, as compared to the more uniform AuNPs formed using 1 mM Au 3+ . Rapid and sensitive detection of MGITC at concentrations as low as 10 −10 M was achieved. The SERS intensity of the normalized Raman peak at 1175 cm −1 exhibited a log-linear relationship for MGITC concentrations between 2 × 10 −10 and 2 × 10 −5 M for Au@Fe 3 O 4 @BCNCs. These results suggest the potential of these hybrid nanocomposites for application in a broad range of analyte detection strategies.more » « less
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Metamaterials present great potential in the applications of solar cells and nanophotonics, such as super lenses and other meta devices, owing to their superior optical properties. In particular, hyperbolic metamaterials (HMMs) with exceptional optical anisotropy offer improved manipulation of light–matter interactions as well as a divergence in the density of states and thus show enhanced performances in related fields. Recently, the emerging field of oxide–metal vertically aligned nanocomposites (VANs) suggests a new approach to realize HMMs with flexible microstructural modulations. In this work, a new oxide–metal metamaterial system, CeO 2 –Au, has been demonstrated with variable Au phase morphologies from nanoparticle-in-matrix (PIM), nanoantenna-in-matrix, to VAN. The effective morphology tuning through deposition background pressure, and the corresponding highly tunable optical performance of three distinctive morphologies, were systematically explored and analyzed. A hyperbolic dispersion at high wavelength has been confirmed in the nano-antenna CeO 2 –Au thin film, proving this system as a promising candidate for HMM applications. More interestingly, a new and abnormal in-plane epitaxy of Au nanopillars following the large mismatched CeO 2 matrix instead of the well-matched SrTiO 3 substrate, was discovered. Additionally, the tilting angle of Au nanopillars, α , has been found to be a quantitative measure of the balance between kinetics and thermodynamics during the depositions of VANs. All these findings provide valuable information in the understanding of the VAN formation mechanisms and related morphology tuning.more » « less
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.3390/nano12193460
