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Abstract Mott insulator VO₂exhibits an ultrafast and reversible semiconductor‐to‐metal transition (SMT) near 340 K (67 °C). In order to fulfill the multifunctional device applications, effective transition temperature (T_c) tuning as well as integrated functionality in VO₂is desired. In this study, multifunctionalities including tailorable SMT characteristics, ferromagnetic (FM) integration, and magneto‐optical (MO) coupling, have been demonstrated via metal/VO₂nanocomposite designs with controlled morphology, i.e., a two‐phase Ni/VO₂pillar‐in‐matrix geometry and a three‐phase Au/Ni/VO₂particle‐in‐matrix geometry. EvidentT_creduction of 20.4 to 54.9 K has been achieved by morphology engineering. Interestingly, the Au/Ni/VO₂film achieves a record‐lowT_cof 295.2 K (22.2 °C), slightly below room temperature (25 °C). The change in film morphology is also correlated with unique property tuning. Highly anisotropic magnetic and optical properties have been demonstrated in Ni/VO₂film, whereas Au/Ni/VO₂film exhibits isotropic properties because of the uniform distribution of Au/Ni nanoparticles. Furthermore, a strong MO coupling with enhanced magnetic coercivity and anisotropy is demonstrated for both films, indicating great potential for optically active property tuning. This demonstration opens exciting opportunities for the VO₂‐based device implementation towards smart windows, next‐generation optical‐coupled switches, and spintronic devices. 

Abstract Interface‐type (IT) resistive switching (RS) memories are promising for next generation memory and computing technologies owing to the filament‐free switching, high on/off ratio, low power consumption, and low spatial variability. Although the switching mechanisms of memristors have been widely studied in filament‐type devices, they are largely unknown in IT memristors. In this work, using the simple Au/Nb:SrTiO₃(Nb:STO) as a model Schottky system, it is identified that protons from moisture are key element in determining the RS characteristics in IT memristors. The Au/Nb:STO devices show typical Schottky interface controlled current–voltage (I–V) curves with a large on/off ratio under ambient conditions. Surprisingly, in a controlled environment without protons/moisture, the largeI–Vhysteresis collapses with the disappearance of a high resistance state (HRS) and the Schottky barrier. Once the devices are re‐exposed to a humid environment, the typical largeI–Vhysteresis can be recovered within hours as the HRS and Schottky interface are restored. The RS mechanism in Au/Nb:STO is attributed to the Schottky barrier modulation by a proton assisted electron trapping and detrapping process. This work highlights the important role of protons/moisture in the RS properties of IT memristors and provides fundamental insight for switching mechanisms in metal oxides‐based memory devices. 

Abstract In this work, a scalable and rapid process is developed for creating a low‐cost humidity sensor for wireless monitoring of moisture levels within packaged goods. The sensor comprises a moisture‐sensitive interdigitated capacitor connected to a planar spiral coil, forming an LC circuit whose resonant frequency is a function of environmental humidity. The sensor is fabricated on a commercially available metallized parchment paper through selective laser ablation of the laminated aluminum (Al) film on the parchment paper substrate. The laser ablation process provides a unique one‐step patterning of the conductive Al layer on the paper while simultaneously creating high surface area Al₂O₃nanoparticles within the laser‐ablated regions. The intrinsic humidity‐responsive characteristics of the laser‐induced Al₂O₃nanostructures provide the wireless sensor with a tenfold higher sensitivity to humidity than a similar LC resonant sensor prepared by conventional photolithography‐based processes on FR‐4 substrates. The frequency change of the sensor is observed to be a linear function within the range of 0−85% RH, providing an average sensitivity of −87 kHz RH⁻¹with good repeatability and stable performance. Furthermore, the employment of scalable laser fabrication processes using commercially available inexpensive materials renders these technologies viable for roll‐to‐roll manufacturing of low‐cost wireless sensors for smart packaging applications. 

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. 

Abstract Ultrathin epitaxial films of ferromagnetic insulators (FMIs) with Curie temperatures near room temperature are critically needed for use in dissipationless quantum computation and spintronic devices. However, such materials are extremely rare. Here, a room‐temperature FMI is achieved in ultrathin La_0.9Ba_0.1MnO₃films grown on SrTiO₃substrates via an interface proximity effect. Detailed scanning transmission electron microscopy images clearly demonstrate that MnO₆octahedral rotations in La_0.9Ba_0.1MnO₃close to the interface are strongly suppressed. As determined from in situ X‐ray photoemission spectroscopy, OK‐edge X‐ray absorption spectroscopy, and density functional theory, the realization of the FMI state arises from a reduction of Mn e_gbandwidth caused by the quenched MnO₆octahedral rotations. The emerging FMI state in La_0.9Ba_0.1MnO₃together with necessary coherent interface achieved with the perovskite substrate gives very high potential for future high performance electronic devices. 

Abstract Vanadium dioxide (VO₂) is a well‐studied Mott‐insulator because of the very abrupt physical property switching during its semiconductor‐to‐metal transition (SMT) around 341 K (68 °C). In this work, through novel oxide‐metal nanocomposite designs (i.e., Au:VO₂and Pt:VO₂), a very broad range of SMT temperature tuning from≈323.5 to≈366.7 K has been achieved by varying the metallic secondary phase in the nanocomposites (i.e., Au:VO₂and Pt:VO₂thin films, respectively). More surprisingly, the SMTT_ccan be further lowered to≈301.8 K (near room temperature) by reducing the Au particle size from 11.7 to 1.7 nm. All the VO₂nanocomposite thin films maintain superior phase transition performance, i.e., large transition amplitude, very sharp transition, and narrow width of thermal hysteresis. Correspondingly, a twofold variation of the complex dielectric function has been demonstrated in these metal‐VO₂nanocomposites. The wide range physical property tuning is attributed to the band structure reconstruction at the metal‐VO₂phase boundaries. This demonstration paved a novel approach for tuning the phase transition property of Mott‐insulating materials to near room temperature transition, which is important for sensors, electrical switches, smart windows, and actuators. 

Abstract Key challenges limiting the adoption of metallic plasmonic nanostructures for practical devices include structural stability and the ease of large‐scale fabrication. Overcoming these issues may require novel metamaterial fabrication with potentials for improved durability under extreme conditions. Here, a self‐assembled growth of a hybrid plasmonic metamaterial in thin‐film form is reported, with epitaxial Ag nanopillars embedded in TiN, a mechanically strong and chemically inert matrix. One of the key achievements lies in the successful control of the tilt angle of the Ag nanopillars (from 0° to 50°), which is attributed to the interplay between the growth kinetics and thermodynamics during deposition. Such an anisotropic nature offered by the tilted Ag nanopillars in TiN matrix is crucial for achieving broadband, asymmetric optical selectivity. Optical spectra coupled with numerical simulations demonstrate strong plasmonic resonance, as well as angular selectivity in a broad UV–vis to near‐infrared regime. The nanostructured metamaterials in this work, which consist of highly conductive metallic nanopillars in a durable nitride matrix, have the potential to serve as a novel hybrid material platform for highly tailorable nanoscale metamaterial designs, suitable for high temperature optical applications. 

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. 

The integration of nanocomposite thin films with combined multifunctionalities on flexible substrates is desired for flexible device design and applications. For example, combined plasmonic and magnetic properties could lead to unique optical switchable magnetic devices and sensors. In this work, a multiphase TiN-Au-Ni nanocomposite system with core–shell-like Au-Ni nanopillars embedded in a TiN matrix has been demonstrated on flexible mica substrates. The three-phase nanocomposite film has been compared with its single metal nanocomposite counterparts, i.e., TiN-Au and TiN-Ni. Magnetic measurement results suggest that both TiN-Au-Ni/mica and TiN-Ni/mica present room-temperature ferromagnetic property. Tunable plasmonic property has been achieved by varying the metallic component of the nanocomposite films. The cyclic bending test was performed to verify the property reliability of the flexible nanocomposite thin films upon bending. This work opens a new path for integrating complex nitride-based nanocomposite designs on mica towards multifunctional flexible nanodevice applications. 

Magnetic and ferroelectric oxide thin films have long been studied for their applications in electronics, optics, and sensors. The properties of these oxide thin films are highly dependent on the film growth quality and conditions. To maximize the film quality, epitaxial oxide thin films are frequently grown on single‐crystal oxide substrates such as strontium titanate (SrTiO₃) and lanthanum aluminate (LaAlO₃) to satisfy lattice matching and minimize defect formation. However, these single‐crystal oxide substrates cannot readily be used in practical applications due to their high cost, limited availability, and small wafer sizes. One leading solution to this challenge is film transfer. In this demonstration, a material from a new class of multiferroic oxides is selected, namely bismuth‐based layered oxides, for the transfer. A water‐soluble sacrificial layer of Sr₃Al₂O₆is inserted between the oxide substrate and the film, enabling the release of the film from the original substrate onto a polymer support layer. The films are transferred onto new substrates of silicon and lithium niobate (LiNbO₃) and the polymer layer is removed. These substrates allow for the future design of electronic and optical devices as well as sensors using this new group of multiferroic layered oxide films.