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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.

 

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.

 

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.

 

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.

 

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.

 

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.

 

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.

 

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. 

Interface‐type (IT) metal/oxide Schottky memristive devices have attracted considerable attention over filament‐type (FT) devices for neuromorphic computing because of their uniform, filament‐free, and analog resistive switching (RS) characteristics. The most recent IT devices are based on oxygen ions and vacancies movement to alter interfacial Schottky barrier parameters and thereby control RS properties. However, the reliability and stability of these devices have been significantly affected by the undesired diffusion of ionic species. Herein, a reliable interface‐dominated memristive device is demonstrated using a simple Au/Nb‐doped SrTiO₃(Nb:STO) Schottky structure. The Au/Nb:STO Schottky barrier modulation by charge trapping and detrapping is responsible for the analog resistive switching characteristics. Because of its interface‐controlled RS, the proposed device shows low device‐to‐device, cell‐to‐cell, and cycle‐to‐cycle variability while maintaining high repeatability and stability during endurance and retention tests. Furthermore, the Au/Nb:STO IT memristive device exhibits versatile synaptic functions with an excellent uniformity, programmability, and reliability. A simulated artificial neural network with Au/Nb:STO synapses achieves a high recognition accuracy of 94.72% for large digit recognition from MNIST database. These results suggest that IT resistive switching can be potentially used for artificial synapses to build next‐generation neuromorphic computing.