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   
                    
                            
                            Complex Oxide‐metal Hybrid Metamaterials with Integrated Magnetic and Plasmonic Non‐noble Metal Nanostructures
                        
                    
    
            Abstract Vertically aligned nanocomposite (VAN) thin films offer exceptional physical properties through diverse material combinations, providing a robust platform for designing complex nanocomposites with tailored performance. Considering materials compatibility issues, most of oxide‐metal VANs have focused on noble metals as the secondary phase in the oxide matrix. Here, an oxide‐metal hybrid metamaterials in the VAN form has been designed which combines ferroelectric BaTiO3(BTO) with two immiscible non‐noble metal elements of Co and Cu, resulting in a three‐phase BTO‐Co‐Cu (BTO‐CC) VAN film. This film exhibits a characteristic nanopillar‐in‐matrix nanostructure with three distinct types of nanopillar morphologies, i.e., Co‐rich cylindrical nanopillars, Cu‐Co‐nanolaminated Co rectangular nanopillars and Co‐Cu‐core–shell cylindrical nanopillars. Phase field modeling indicates the constructed structure is resulted from the interplay between thermochemical, chemomechanical, and interfacial energy driving forces. The strong structural anisotropy leads to anisotropic optical and magnetic properties, presenting potential as hyperbolic metamaterial (HMM) with transverse‐positive dispersion in the near‐infrared region. The inclusion of non‐noble Cu nanostructure induces surface plasmon resonance (SPR) in the visible region. Additionally, ferroelectric properties have been demonstrated in a BTO/BTO‐CC bilayer, confirming room‐temperature multiferroicity in the film. The complex three‐phase VANs offer a novel platform for exploring electro‐magneto‐optical coupling along vertical interfaces toward future integrated devices. 
        more » 
        « less   
        
    
    
                            - PAR ID:
- 10576392
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Functional Materials
- Volume:
- 35
- Issue:
- 30
- ISSN:
- 1616-301X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
- 
            
- 
            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
- 
            null (Ed.)Inducing new phases in thick films via vertical lattice strain is one of the critical advantages of vertically aligned nanocomposites (VANs). In SrTiO 3 (STO), the ground state is ferroelastic, and the ferroelectricity in STO is suppressed by the orthorhombic transition. Here, we explore whether vertical lattice strain in three-dimensional VANs can be used to induce new ferroelectric phases in SrTiO 3 :MgO (STO:MgO) VAN thin films. The STO:MgO system incorporates ordered, vertically aligned MgO nanopillars into a STO film matrix. Strong lattice coupling between STO and MgO imposes a large lattice strain in the STO film. We have investigated ferroelectricity in the STO phase, existing up to room temperature, using piezoresponse force microscopy, phase field simulation and second harmonic generation. We also serendipitously discovered the formation of metastable TiO nanocores in MgO nanopillars embedded in the STO film matrix. Our results emphasize the design of new phases via vertical epitaxial strain in VAN thin films.more » « less
- 
            Abstract Magneto‐optical (MO) coupling incorporates photon‐induced change of magnetic polarization that can be adopted in ultrafast switching, optical isolators, mode convertors, and optical data storage components for advanced optical integrated circuits. However, integrating plasmonic, magnetic, and dielectric properties in one single material system poses challenges since one natural material can hardly possess all these functionalities. Here, co‐deposition of a three‐phase heterostructure composed of a durable conductive nitride matrix with embedded core–shell vertically aligned nanopillars, is demonstrated. The unique coupling between ferromagnetic NiO core and atomically sharp plasmonic Au shell enables strong MO activity out‐of‐plane at room temperature. Further, a template growth process is applied, which significantly enhances the ordering of the nanopillar array. The ordered nanostructure offers two schemes of spin polarization which result in stronger antisymmetry of Kerr rotation. The presented complex hybrid metamaterial platform with strong magnetic and optical anisotropies is promising for tunable and modulated all‐optical‐based nanodevices.more » « less
- 
            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.more » « less
 An official website of the United States government
An official website of the United States government 
				
			 
					 
					
