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Abstract Two-dimensional (2D) ferroelectric materials have emerged as significant platforms for multi-functional three-dimensional (3D) integrated electronic devices. Among 2D ferroelectric materials, ferro-ionic CuInP2S6 has the potential to achieve the versatile advances in neuromorphic computing systems due to its phase tunability and ferro-ionic characteristics. As CuInP2S6 exhibits a ferroelectric phase with insulating properties at room temperature, the external temperature and electrical field should be required to activate the ferro-ionic conduction. Nevertheless, such external conditions inevitably facilitate stochastic ionic conduction, which completely limits the practical applications of 2D ferro-ionic materials. Herein, free-standing 2D ferroelectric heterostructure is mechanically manipulated for nano-confined conductive filaments growth in free-standing 2D ferro-ionic memristor. The ultra-high mechanical bending is selectively facilitated at the free-standing area to spatially activate the ferro-ionic conduction, which allows the deterministic local positioning of Cu+ ion transport. According to the local flexoelectric engineering, 5.76×102-fold increased maximum current is observed within vertical shear strain 720 nN, which is theoretically supported by the 3D flexoelectric simulation. In conclusion, we envision that our universal free-standing platform can provide the extendable geometric solution for ultra-efficient self-powered system and reliable neuromorphic device.

In the era of big data, negative differential resistance (NDR) devices have attracted significant attention as a means of handling massive amounts of information. While 2D materials have been used to achieve NDR behavior, their intrinsic material characteristics have produced limited performance improvements. In this article, a facile phase modification method is presented via a plasma‐assisted sulfidation process to synthesize multiphased WS2 thin films, including distorted 1 T (D‐1 T) phase and 2 H phases for photoreactive NDR devices with p‐Si. The D‐1 T phase offers a feasible route to achieve high‐performance NDR devices with excellent stability and semimetallic properties. A comprehensive investigation of experimental and computational analyses elucidates the phase transition mechanism with various temperatures and electrical properties of D‐1 T WS2. In addition, optimizing electron tunneling in the multiple‐phased tungsten disulfide (MP‐WS2)/p‐Si heterojunction at MP‐WS2 with 77.4% D‐1 T phase results in superior NDR performance with a peak‐to‐valley current ratio of 13.8 and reliable photoreactive random‐access memory. This unique phase engineering process via plasma‐assisted sulfidation provides a pioneering perspective in functionalization and reliability for next‐generation nanoelectronics.

Abstract Molecular electronics enables functional electronic behavior via single molecules or molecular self‐assembled monolayers, providing versatile opportunities for hybrid molecular‐scale electronic devices. Although various molecular junction structures are constructed to investigate charge transfer dynamics, significant challenges remain in terms of interfacial charging effects and far‐field background signals, which dominantly block the optoelectrical observation of interfacial charge transfer dynamics. Here, tip‐induced optoelectrical engineering is presented that synergistically correlates photo‐induced force microscopy and Kelvin probe force microscopy to remotely control and probe the interfacial charge transfer dynamics with sub‐10 nm spatial resolution. Based on this approach, the optoelectrical origin of metal–molecule interfaces is clearly revealed by the nanoscale heterogeneity of the tip‐sample interaction and optoelectrical reactivity, which theoretically aligned with density functional theory calculations. For a practical device‐scale demonstration of tip‐induced optoelectrical engineering, interfacial tunneling is remotely controlled at a 4‐inch wafer‐scale metal–insulator–metal capacitor, facilitating a 5.211‐fold current amplification with the tip‐induced electrical field. In conclusion, tip‐induced optoelectrical engineering provides a novel strategy to comprehensively understand interfacial charge transfer dynamics and a non‐destructive tunneling control platform that enables real‐time and real‐space investigation of ultrathin hybrid molecular systems.

In the past decades, toxic gas emissions have increased significantly owing to the rapid growth of industry and road transportation. Therefore, monitoring major pollutants, such as NO2, is crucial to protecting human health. The 2D materials that contain numerous adsorption sites and exhibit ultrahigh chemical reactivity can be used as sensor materials to detect these toxic gases. Herein, highly uniform, large‐area carbon‐incorporating hierarchical MoS2 nanobranches are synthesized by metal–organic chemical vapor deposition (MOCVD). An in situ carbon‐incorporation method that uses the carbon impurity present in the precursor as the seed during the MOCVD process is employed to form a hierarchical structure containing abundant adsorption sites. A gas sensor based on the resulting C‐MoS2 nanobranches contains many edge sites exhibits high adsorption energy, and consequently, has high NO2 gas sensitivity. Hence, this hierarchical C‐MoS2 gas sensor shows excellent sensing properties, exhibiting a device response of 1.67 at an extremely low NO2 concentration (≈5 ppb). The limit of detection of the gas sensor for NO2 is calculated to be low (≈1.58 ppt), further confirming its exceptional performance. Thus, the hierarchical C‐MoS2 nanobranches deposited herein provide novel insights regarding the properties of 2D materials and are highly suited for fabricating high‐performance NO2 sensors.

Abstract Among the transition metal dichalcogenides (TMD), tungsten disulfide (WS2) and molybdenum disulfide (MoS2) are promising sulfides for replacing noble metals in the hydrogen evolution reaction (HER) owing to their abundance and good catalytic activity. However, the catalytic activity is derived from the edge sites of WS2 and MoS2, while their basal planes are inert. We propose a novel process for N-doped TMD synthesis for advanced HER using N2 + Ar + H2S plasma. The high ionization energy of Ar gas enabled nitrogen species activation results in efficient N-doping of TMD (named In situ-MoS2 and In situ-WS2). In situ-MoS2 and WS2 were characterized by various techniques (Raman spectroscopy, XPS, HR-TEM, TOF–SIMS, and OES), confirming nanocrystalline and N-doping. The N-doped TMD were used as electrocatalysts for the HER, with overpotentials of 294 mV (In situ-MoS2) and 298 mV (In situ-WS2) at a current density of 10 mA cm−2, which are lower than those of pristine MoS2 and WS2, respectively. Density functional theory (DFT) calculations were conducted for the hydrogen Gibbs energy (∆GH) to investigate the effect of N doping on the HER activity. Mixed gas plasma proposes a facile and novel fabrication process for direct N doping on TMD as a suitable HER electrocatalyst.

This study identified time-varying harmonic characteristics in a high-density plasma (HDP) chemical vapor deposition (CVD) chamber by depositing low-k oxide (SiOF). The characteristics of harmonics are caused by the nonlinear Lorentz force and the nonlinear nature of the sheath. In this study, a noninvasive directional coupler was used to collect harmonic power in the forward and reverse directions, which were low frequency (LF) and high bias radio frequency (RF). The intensity of the 2nd and 3rd harmonics responded to the LF power, pressure, and gas flow rate introduced for plasma generation. Meanwhile, the intensity of the 6th harmonic responded to the oxygen fraction in the transition step. The intensity of the 7th (forward) and 10th (in reverse) harmonic of the bias RF power depended on the underlying layers (silicon rich oxide (SRO) and undoped silicate glass (USG)) and the deposition of the SiOF layer. In particular, the 10th (reverse) harmonic of the bias RF power was identified using electrodynamics in a double capacitor model of the plasma sheath and the deposited dielectric material. The plasma-induced electronic charging effect on the deposited film resulted in the time-varying characteristic of the 10th harmonic (in reverse) of the bias RF power. The wafer-to-wafer consistency and stability of the time-varying characteristic were investigated. The findings of this study can be applied to in situ diagnosis of SiOF thin film deposition and optimization of the deposition process.

The bifunctionality of chromism-integrated sensors and devices has been highlighted because of their reversibility, fast response, and visual indication. For example, one of the representative chromism electrochromic materials exhibits optical modulation under ion insertion/extraction by applying a potential. This operation mechanism can be integrated with various sensors (pressure, strain, biomolecules, gas, etc.) and devices (energy conversion/storage systems) as visual indicators for user-friendly operation. In this review, recent advances in the field of chromism-integrated systems for visual indicators are categorized for various chromism-integrated sensors and devices. This review can provide insights for researchers working on chromism, sensors, or devices. The integrated chromic devices are evaluated in terms of coloration-bleach operation, cycling stability, and coloration efficiency. In addition, the existing challenges and prospects for chromism-integrated sensors and devices are summarized for further research.