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Abstract Emerging non-volatile memristor-based devices with resistive switching (RS) materials are being widely researched as promising contenders for the next generation of data storage and neuromorphic technologies. Titanium nitride (TiN_x) is a common industry-friendly electrode system for RS; however, the precise TiN_xproperties required for optimum RS performance is still lacking. Herein, using ion-assisted DC magnetron sputtering, we demonstrate the key importance not only of engineering the TiN_xbottom electrodes to be dense, smooth, and conductive, but also understoichiometric in N. With these properties, RS in HfO₂-based memristive devices is shown to be optimised for TiN_0.96. These devices have switching voltages ≤ ±1 V with promising device-to-device uniformity, endurance, memory window of ~40, and multiple non-volatile intermediate conductance levels. This study highlights the importance of precise tuning of TiN_xbottom electrodes to achieve robust performance of oxide resistive switching materials. 

Abstract Kerr microcombs have drawn substantial interest as mass-manufacturable, compact alternatives to bulk frequency combs. This could enable the deployment of many comb-reliant applications previously confined to laboratories. Particularly enticing is the prospect of microcombs performing optical frequency division in compact optical atomic clocks. Unfortunately, it is difficult to meet the self-referencing requirement of microcombs in these systems owing to the approximately terahertz repetition rates typically required for octave-spanning comb generation. In addition, it is challenging to spectrally engineer a microcomb system to align a comb mode with an atomic clock transition with a sufficient signal-to-noise ratio. Here we adopt a Vernier dual-microcomb scheme for optical frequency division of a stabilized ultranarrow-linewidth continuous-wave laser at 871 nm to an ~235 MHz output frequency. This scheme enables shifting an ultrahigh-frequency (~100 GHz) carrier-envelope offset beat down to frequencies where detection is possible and simultaneously placing a comb line close to the 871 nm laser—tuned so that, if frequency doubled, it would fall close to the clock transition in¹⁷¹Yb⁺. Our dual-comb system can potentially combine with an integrated ion trap towards future chip-scale optical atomic clocks. 

Abstract Nanocomposite thin films, comprising two or more distinct materials at nanoscale, have attracted significant research interest considering their potential of integrating multiple functionalities for advanced applications in electronics, energy storage, photonics, photovoltaics, and sensing. Among various fabrication technologies, a one-step pulsed laser deposition process enables the self-assembly of materials into vertically aligned nanocomposites (VANs). The demonstrated VAN systems include oxide–oxide, oxide–metal, and nitride–metal VAN films and their growth mechanisms are vastly different. These complexities pose challenges in the designs, materials selection, and prediction of the resulted VAN morphologies and properties. The review examines the key roles that surface energy plays in the VAN growth and provides a generalized materials design guideline combining the two key factors of surface energy and lattice strain/mismatch, along with other factors related to growth kinetics that collectively influence the morphology of VAN films. This review aims to offer valuable guidelines for future material selection and microstructure design in the development of self-assembled VAN films. 

Abstract Complex oxide thin films cover a range of physical properties and multifunctionalities that are critical for logic, memory, and optical devices. Typically, the high‐quality epitaxial growth of these complex oxide thin films requires single crystalline oxide substrates such as SrTiO₃(STO), MgO, LaAlO₃, a‐Al₂O_3,and many others. Recent successes in transferring these complex oxides as free‐standing films not only offer great opportunities in integrating complex oxides on other devices, but also present enormous opportunities in recycling the deposited substrates after transfer for cost‐effective and sustainable processing of complex oxide thin films. In this work, the surface modification effects introduced on the recycled STO are investigated, and their impacts on the microstructure and properties of subsequently grown epitaxial oxide thin films are assessed and compared with those grown on the pristine substrates. Detailed analyses using high‐resolution scanning transmission electron microscopy and geometric phase analysis demonstrate distinct strain states on the surfaces of the recycled STO versus the pristine substrates, suggesting a pre‐strain state in the recycled STO substrates due to the previous deposition layer. These findings offer opportunities in growing highly mismatched oxide films on the recycled STO substrates with enhanced physical properties. Specifically, yttrium iron garnet (Y₃Fe₅O₁₂) films grown on recycled STO present different ferromagnetic responses compared to that on the pristine substrates, underscoring the effects of surface modification. The study demonstrates the feasibility of reuse and redeposition using recycled substrates. Via careful handling and preparation, high‐quality epitaxial thin films can be grown on recycled substrates with comparable or even better structural and physical properties toward sustainable process of complex oxide devices. 

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. 

Abstract Flexible and wearable sensors show enormous potential for personalized healthcare devices by real‐time monitoring of an individual's health. Typically, a single functional material is selected for one sensor to sense a particular physical signal while multiple materials will be selected for multi‐mode sensing. Vertically aligned nanocomposites (VANs) have recently demonstrated various material combinations and novel coupled multifunctionalities that are hard to achieve in any single‐phase material alone, including multiphase multiferroics, magneto‐optic coupling, and strong magnetic and optical anisotropy. Integrating these novel VANs into wearable sensors shows enormous potential in multi‐mode sensing owing to their multifunctional nature. In this work, the transfer of VANs onto polydimethylsiloxane as a novel flexible chemical and pressure sensor is demonstrated. For this demonstration, the classical BaTiO₃‐Au VAN with combined plasmonic and piezoelectric properties is used to demonstrate a multi‐sensing mechanism. A thin water‐soluble buffer of Sr₃Al₂O₆serves as a buffer layer for the epitaxial growth and transfer process. The electrical output based on the piezoelectric responses and identifying 4‐mercaptobenzoic acid by surface‐enhanced Raman spectroscopy reveal great potential for free‐standing VANs in a wearable multifunctional sensing platform. 

Abstract The demonstration of epitaxial thin film transfer has enormous potential for thin film devices free from the traditional substrate epitaxy limitations. However, large‐area continuous film transfer remains a challenge for the commonly reported polymer‐based transfer methods due to bending and cracking during transfer, especially for highly strained epitaxial thin films. In this work, a new epoxy‐based, rigid transfer method is used to transfer films from an SrTiO₃(STO) growth substrate onto various new substrates, including those that will typically pose significant problems for epitaxy. An epitaxial multiferroic Bi₃Fe₂Mn₂O_x(BFMO) layered supercell (LSC) material is selected as the thin film for this demonstration. The results of surface and structure studies show an order of magnitude increase in the continuous area of transferred films when compared to previous transfer methods. The magnetic properties of the BFMO LSC films are shown to be enhanced by the release of strain in this method, and ferromagnetic resonance is found with an exceptionally low Gilbert damping coefficient. The large‐area transfer of this highly strained complex oxide BFMO thin film presents enormous potential for the integration of many other multifunctional oxides onto new substrates for future magnetic sensors and memory devices. 

Tuning spin and charge degrees of freedom of complex oxide materials can enable significant advancements in future spintronics. In this study, by three dimensional strain engineering, we demonstrate room temperature ferroelectricity and magnetoelectricity in a vertically aligned nanocomposite thin film structure, composed of vertical nanopillars of SmFeO3 (SFO) embedded within the NiFeO4 (NFO) matrix. A three-dimensional tensile strain is induced in the SFO as a result of the unique film architecture. The tensile strain in SFO produces strong room temperature ferroelectric response instead of the normally very weak ferroelectricity of unstrained SFO, which is an improper ferroelectric. The induced ferroelectricity in SFO enables self-biased magnetoelectric coupling to be achieved between the two phases (magnetoelectric coupling coefficient ∼4 × 10−11 sm−1 at room temperature). The magnetoelectric coupling is facilitated by strain transfer across the vertical interfaces of the two phases. We additionally observe an exchange bias of ∼200 Oe (at 2 K) surviving up to the room temperature, indicating strongly coupled interfaces of SFO and NFO. These findings represent a step forward in future magnetoelectric RAM devices. 

The unique redox properties and high oxygen capacity of nanostructured CeO₂demonstrate a wide range of applications, such as electrolytes for solid oxide fuel cells, gas sensors, and catalysis for automotive exhaust gas. Most CeO₂nanomaterials are prepared by chemical synthesis or hard templating methods. An effective way to obtain highly textured, small‐radius dimensions with high specific surface area remains challenging. Here, highly textured CeO₂nanostructures with various shapes ranging from nanowires to nanoporous thin films are successfully synthesized. Vertically aligned nanocomposites (VANs) of Sr₃Al₂O₆(SAO) and CeO₂are synthesized first while varying concentration ratio between them. Once the SAO is dissolved in water, the remaining CeO₂forms distinct nanostructures. The thermal stability of the nanostructured CeO₂is evaluated byin situheating XRD and thermal annealing tests. This method provides an alternative approach to preparing nanostructured CeO₂without toxic chemical solutions or complex micro/nanofabrication techniques. These results present a novel approach to prepare nanostructured CeO₂for future sensing and energy device applications. 

An epitaxial NbN–Co VAN thin film was deposited on a MgO substrate with a cubic NbN phase, which presents ferromagnet properties with strong out-of-plane magnetic anisotropy. This hybrid metamaterial could find future applications in device design.