Leigang Li

Strain relaxation and enhanced perpendicular magnetic anisotropy in BiFeO3:CoFe2O4 vertically aligned nanocomposite thin films

Self-assembled BiFeO3:CoFe2O4 (BFO:CFO) vertically aligned nanocomposite thin films have been fabricated on SrTiO3 (001) substrates using pulsed laser deposition. The strain relaxation mechanism between BFO and CFO with a large lattice mismatch has been studied by X-ray diffraction and transmission electron microscopy. The as-prepared nanocomposite films exhibit enhanced perpendicular magnetic anisotropy as the BFO composition increases. Different anisotropy sources have been investigated, suggesting that spin-flop coupling between antiferromagnetic BFO and ferrimagnetic CFO plays a dominant role in enhancing the uniaxial magnetic anisotropy.

Role of scaffold network in controlling strain and functionalities of nanocomposite films

The tuning of functional properties in thick oxide films via nanoscaffolds induced large vertical lattice strain. Strain is a novel approach to manipulating functionalities in correlated complex oxides. However, significant epitaxial strain can only be achieved in ultrathin layers. We show that, under direct lattice matching framework, large and uniform vertical strain up to 2% can be achieved to significantly modify the magnetic anisotropy, magnetism, and magnetotransport properties in heteroepitaxial nanoscaffold films, over a few hundred nanometers in thickness. Comprehensive designing principles of large vertical strain have been proposed. Phase-field simulations not only reveal the strain distribution but also suggest that the ultimate strain is related to the vertical interfacial area and interfacial dislocation density. By changing the nanoscaffold density and dimension, the strain and the magnetic properties can be tuned. The established correlation among the vertical interface—strain—properties in nanoscaffold films can consequently be used to tune other functionalities in a broad range of complex oxide films far beyond critical thickness.

Self-Assembled Epitaxial Au–Oxide Vertically Aligned Nanocomposites for Nanoscale Metamaterials

Metamaterials made of nanoscale inclusions or artificial unit cells exhibit exotic optical properties that do not exist in natural materials. Promising applications, such as super-resolution imaging, cloaking, hyperbolic propagation, and ultrafast phase velocities have been demonstrated based on mostly micrometer-scale metamaterials and few nanoscale metamaterials. To date, most metamaterials are created using costly and tedious fabrication techniques with limited paths toward reliable large-scale fabrication. In this work, we demonstrate the one-step direct growth of self-assembled epitaxial metal-oxide nanocomposites as a drastically different approach to fabricating large-area nanostructured metamaterials. Using pulsed laser deposition, we fabricated nanocomposite films with vertically aligned gold (Au) nanopillars (∼20 nm in diameter) embedded in various oxide matrices with high epitaxial quality. Strong, broad absorption features in the measured absorbance spectrum are clear signatures of plasmon resonances of Au nanopillars. By tuning their densities on selected substrates, anisotropic optical properties are demonstrated via angular dependent and polarization resolved reflectivity measurements and reproduced by full-wave simulations and effective medium theory. Our model predicts exotic properties, such as zero permittivity responses and topological transitions. Our studies suggest that these self-assembled metal-oxide nanostructures provide an exciting new material platform to control and enhance optical response at nanometer scales.

Continuous Tuning of Phase Transition Temperature in VO2 Thin Films on c-Cut Sapphire Substrates via Strain Variation

Vanadium dioxide (VO2) thin films with controlled thicknesses are deposited on c-cut sapphire substrates with Al-doped ZnO (AZO) buffer layers by pulsed laser deposition. The surface roughness of AZO buffer layers is varied by controlling oxygen pressure during growth. The strain in the VO2 lattice is found to be dependent on the VO2 thickness and the VO2/AZO interface roughness. The semiconductor-to-metal transition (SMT) properties of VO2 thin films are characterized and the transition temperature (Tc) is successfully tuned by the VO2 thickness as well as the VO2/AZO interface roughness. It shows that the Tc of VO2 decreases with the decrease of film thickness or VO2/AZO interface roughness. Other SMT properties of the VO2 films are maintained during the Tc tuning. The results suggest that the strain tuning induced by AZO buffer provides an effective approach for tuning Tc of VO2 continuously.

Enhanced tunable magnetoresistance properties over a wide temperature range in epitaxial (La0.7Sr0.3MnO3)1−x:(CeO2)x nanocomposites

Vertically aligned nanocomposite (VAN) (La0.7Sr0.3MnO3)1−x:(CeO2)x (LSMO:CeO2) thin films have been grown on SrTiO3 (001) substrates by pulsed laser deposition. Tunable magnetoresistance properties as well as microstructures are demonstrated in these VAN films by modulating the film composition (x = 0, 0.3, 0.4, 0.45, 0.5, and 0.55). The sample of x = 0.3 shows a large low-field magnetoresistance (LFMR) in a high temperature range, i.e., over 10% at the range of 280 K to 320 K under 1 T and with a peak value of ∼13.5% at 310 K. In addition, a vast enhancement of LFMR in a low temperature range of 20–150 K with peak of ≈34.3% at 45 K for 1 T could be achieved with x = 0.5. The enhanced LFMR properties can be attributed to both the phase boundary induced spin fluctuation and the magnetic tunneling effect through vertical ferromagnetic/insulator/ferromagnetic structures. The observed enhanced LFMR performance, especially at high temperatures, as well as its simple growth method, offers a great potential for ...

Self-Assembled Heteroepitaxial Oxide Nanocomposite for Photoelectrochemical Solar Water Oxidation

We report on spontaneously phase ordered heteroepitaxial SrTiO3 (STO):ZnFe2O4 (ZFO) nanocomposite films that give rise to strongly enhanced photoelectrochemical solar water oxidation, consistent with enhanced photoinduced charge separation. The STO:ZFO nanocomposite yielded an enhanced photocurrent density of 0.188 mA/cm2 at 1.23 V vs a reversible hydrogen electrode, which was 7.9- and 2.6-fold higher than that of the plain STO film and ZFO film cases under 1-sun illumination, respectively. The photoelectrode also produced stable photocurrent and Faradaic efficiencies of H2 and O2 formation that were more than 90%. Incident-photon-to-current-conversion efficiency measurements, Tauc plots, Mott–Schottky plots, and electrochemical impedance spectroscopy measurements proved that the strongly enhanced photogenerated charge separation resulted from vertically aligned pseudosingle crystalline components, epitaxial heterojunctions, and a staggered band alignment of the components of the nanocomposite films. This study presents a completely new avenue for efficient solar energy conversion applications.

Heterointerface design and strain tuning in epitaxial BiFeO3:CoFe2O4 nanocomposite films

The ability to control the morphology of heterointerfaces with coupled functionalities is fascinating from both fundamental and technological perspectives. Here, using BiFeO3:CoFe2O4 vertically aligned nanocomposite (VAN) films as a model system, we demonstrate a simple and effective method to modulate the heterointerface and its morphology in nanocomposite films with pulsed laser deposition. By tuning the deposition frequency through thickness during film growth, both vertically straight and gradient heterointerfaces have been achieved. The modulated heterointerface is strongly correlated with strain tuning and interface coupling, and thus modifies the magnetic anisotropy, coercive fields, and ferroelectric switching behavior. This study provides a viable approach for tailoring the interface strain and coupling in VAN and achieving tunable physical properties.

Perpendicular Exchange-Biased Magnetotransport at the Vertical Heterointerfaces in La(0.7)Sr(0.3)MnO3:NiO Nanocomposites.

Heterointerfaces in manganite-based heterostructures in either layered or vertical geometry control their magnetotransport properties. Instead of using spin-polarized tunneling across the interface, a unique approach based on the magnetic exchange coupling along the vertical interface to control the magnetotransport properties has been demonstrated. By coupling ferromagnetic La0.7Sr0.3MnO3 and antiferromagnetic NiO in an epitaxial vertically aligned nanocomposite (VAN) architecture, a dynamic and reversible switch of the resistivity between two distinct exchange biased states has been achieved. This study explores the use of vertical interfacial exchange coupling to tailor magnetotransport properties, and demonstrates their viability for spintronic applications.

Self-Assembled Magnetic Metallic Nanopillars in Ceramic Matrix with Anisotropic Magnetic and Electrical Transport Properties.

Ordered arrays of metallic nanopillars embedded in a ceramic matrix have recently attracted considerable interest for their multifunctionality in advanced devices. A number of hurdles need to be overcome for achieving practical devices, including selections of metal-ceramic combination, creation of tunable and ordered structure, and control of strain state. In this article, we demonstrate major advances to create such a fine nanoscale structure, i.e., epitaxial self-assembled vertically aligned metal-ceramic composite, in one-step growth using pulsed laser deposition. Tunable diameter and spacing of the nanopillars can be achieved by controlling the growth parameters such as deposition temperature. The magnetic metal-ceramic composite thin films demonstrate uniaxial anisotropic magnetic properties and enhanced coercivity compared to that of bulk metal. The system also presents unique anisotropic electrical transport properties under in-plane and out-of-plane directions. This work paves a new avenue to fabricate epitaxial metal-ceramic nanocomposites, which can simulate broader future explorations in nanocomposites with novel magnetic, optical, electrical, and catalytical properties.

Strain and Interface Effects in a Novel Bismuth-Based Self-Assembled Supercell Structure

Bi2FeMnO6 (BFMO) thin films with both conventional pseudocubic structure and novel supercell structure have been grown on SrTiO3 (001) substrates with different thicknesses of CeO2 buffer layers (ranging from 6.7 to 50.0 nm) using pulsed laser deposition. The correlation between the thickness of the CeO2 buffer layer and the structure of the BFMO films shows that the CeO2 buffer layer, as thin as 6.7 nm, is sufficient in triggering the novel BFMO supercell structure. This may be ascribed to the interfacial strain between the BFMO supercell structure and the CeO2 buffer layer which also serves as a seed layer. The buffer layer thickness is found to be critical to control the microstructure and magnetism of the formed BFMO supercell structures. Thin seed layers can produce a smoother interface between the BFMO film and the CeO2 buffer layer, and therefore better ferrimagnetic properties. Our results have demonstrated that strain and interface could be utilized to generate novel thin film structures and to tune the functionalities of thin films.