skip to main content

Title: Self-assembled HfO 2 -Au nanocomposites with ultra-fine vertically aligned Au nanopillars
Oxide-metal-based hybrid materials have gained great research interest in recent years owing to their potential for multifunctionality, property coupling, and tunability. Specifically, oxide-metal hybrid materials in a vertically aligned nanocomposite (VAN) form could produce pronounced anisotropic physical properties, e.g. , hyperbolic optical properties. Herein, self-assembled HfO 2 -Au nanocomposites with ultra-fine vertically aligned Au nanopillars (as fine as 3 nm in diameter) embedded in a HfO 2 matrix were fabricated using a one-step self-assembly process. The film crystallinity and pillar uniformity can be obviously improved by adding an ultra-thin TiN-Au buffer layer during the growth. The HfO 2 -Au hybrid VAN films show an obvious plasmonic resonance at 480 nm, which is much lower than the typical plasmonic resonance wavelength of Au nanostructures, and is attributed to the well-aligned ultra-fine Au nanopillars. Coupled with the broad hyperbolic dispersion ranging from 1050 nm to 1800 nm in wavelength, and unique dielectric HfO 2 , this nanoscale hybrid plasmonic metamaterial presents strong potential for the design of future integrated optical and electronic switching devices.  more » « less
Award ID(s):
2016453 1565822 1809520
Author(s) / Creator(s):
; ; ; ; ; ; ; ;
Date Published:
Journal Name:
Page Range / eLocation ID:
11979 to 11987
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    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.

    more » « less
  2. null (Ed.)
    Self-assembled oxide–metallic alloy nanopillars as hybrid plasmonic metamaterials ( e.g. , ZnO–Ag x Au 1−x ) in a thin film form have been grown using a pulsed laser deposition method. The hybrid films were demonstrated to be highly tunable via systematic tuning of the oxygen background pressure during deposition. The pressure effects on morphology and optical properties have been investigated and found to be critical to the overall properties of the hybrid films. Specifically, low background pressure results in the vertically aligned nanocomposite (VAN) form while the high-pressure results in more lateral growth of the nanoalloys. Strong surface plasmon resonance was observed in the UV-vis region and a hyperbolic dielectric function was achieved due to the anisotropic morphology. The oxide–nanoalloy hybrid material grown in this work presents a highly effective approach for tuning the binary nanoalloy morphology and properties through systematic parametric changes, important for their potential applications in integrated photonics and plasmonics such as sensors, energy harvesting devices, and beyond. 
    more » « less
  3. 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
  4. Abstract

    Photonic integrated circuits require various optical materials with versatile optical properties and easy on‐chip device integration. To address such needs, a well‐designed nanoscale metal‐oxide metamaterial, that is, plasmonic Au nanoparticles embedded in nonlinear LiNbO3(LNO) matrix, is demonstrated with tailorable optical response. Specifically, epitaxial and single‐domain LNO thin films with tailored Au nanoparticle morphologies (i.e., various nanoparticle sizes and densities), are grown by a pulsed laser deposition method. The optical measurement presents obvious surface plasmon resonance and dramatically varied complex dielectric function because of the embedded Au nanoparticles, and its response can be well tailored by varying the size and density of Au nanoparticles. An optical waveguide structure based on the thin film stacks of a‐Si on SiO2/Au‐LNO is fabricated and exhibits low optical dispersion with an optimized evanescent field staying in the LNO‐Au active layer. The hybrid Au‐LNO metamaterial thin films provide a novel platform for tunable optical materials and their future on‐chip integrations in photonic‐based integrated circuits.

    more » « less
  5. Abstract

    Integration of nanoscale photonic and plasmonic components on Si substrates is a critical step toward Si‐based integrated nanophotonic devices. In this work, a set of unique complex 3D metamaterials with intercalated nanolayered and nanopillar structures with tunable plasmonic and optical properties on Si substrates is designed. More specifically, the 3D metamaterials combine metal (Au) nanopillars and alternating metal‐nitride (Au‐TiN and Au‐TaN) nanolayers, epitaxially grown on Si substrates. The ultrafine Au nanopillars (d≈ 3 nm) continuously grow throughout all the nanolayers with high epitaxial quality. Novel optical properties, such as highly anisotropic optical property, high absorbance covering the entire visible spectrum regime, and hyperbolic property in the visible regime, are demonstrated. Furthermore, a waveguide based on a silicon nitride (Si3N4) ridge with a multilayer structure is successfully fabricated. The demonstration of 3D nanoscale metamaterial design integrated on Si opens up a new route toward tunable metamaterials nanostructure designs with versatile material selection for various optical components in Si integrated photonics.

    more » « less