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Memristive technology has been rapidly emerging as a potential alternative to traditional CMOS technology, which is facing fundamental limitations in its development. Since oxide-based resistive switches were demonstrated as memristors in 2008, memristive devices have garnered significant attention due to their biomimetic memory properties, which promise to significantly improve power consumption in computing applications. Here, we provide a comprehensive overview of recent advances in memristive technology, including memristive devices, theory, algorithms, architectures, and systems. In addition, we discuss research directions for various applications of memristive technology including hardware accelerators for artificial intelligence, in-sensor computing, and probabilistic computing. Finally, we provide a forward-looking perspective on the future of memristive technology, outlining the challenges and opportunities for further research and innovation in this field. By providing an up-to-date overview of the state-of-the-art in memristive technology, this review aims to inform and inspire further research in this field.

Two-dimensional (2D) photodetectors based on photovoltaic effect or photogating effect can hardly achieve both high photoresponsivity and large linear dynamic range at the same time, which greatly limits many practical applications such as imaging sensors. Here, the conductive-sensitizer strategy, a general design for improving photoresponsivity and linear dynamic range in 2D photodetectors is provided and experimentally demonstrated on vertically stacked bilayer WS 2 /GaS 0.87 under a parallel circuit mode. Owing to successful band alignment engineering, the isotype type-II heterojunction enables efficient charge carrier transfer from WS 2 , the high-mobility sensitizer, to GaS 0.87 , the low-mobility channel, under illumination from a broad visible spectrum. The transferred electron charges introduce a reverse electric field which efficiently lowers the band offset between the two materials, facilitating a transition from low-mobility photocarrier transport to high-mobility photocarrier transport with increasing illumination power. We achieved a large linear dynamic range of 73 dB as well as a high and constant photoresponsivity of 13 A/W under green light. X-ray photoelectron spectroscopy, cathodoluminescence, and Kelvin probe force microscopy further identify the key role of defects in monolayer GaS 0.87 in engineering the band alignment with monolayer WS 2 . This work proposes a design route based on band and interface modulation for improving performance of 2D photodetectors and provides deep insights into the important role of strong interlayer coupling in offering heterostructures with desired properties and functions.

Confining electric fields to a nanoscale region is challenging yet crucial for applications such as high-resolution probing of electrical properties of materials and electric-field manipulation of nanoparticles. State-of-the-art techniques involving atomic force microscopy typically have a lateral resolution limit of tens of nanometers due to limitations in the probe geometry and stray electric fields that extend over space. Engineering the probes is the most direct approach to improving this resolution limit. However, current methods to fabricate high-resolution probes, which can effectively confine the electric fields laterally, involve expensive and sophisticated probe manipulation, which has limited the use of this approach. Here, we demonstrate that nanoscale phase switching of configurable thin films on probes can result in high-resolution electrical probes. These configurable coatings can be both germanium-antimony-tellurium (GST) as well as amorphous-carbon, materials known to undergo electric field-induced nonvolatile, yet reversible switching. By forming a localized conductive filament through phase transition, we demonstrate a spatial resolution of electrical field beyond the geometrical limitations of commercial platinum probes (i.e., an improvement of ∼48%). We then utilize these confined electric fields to manipulate nanoparticles with single nanoparticle precision via dielectrophoresis. Our results advance the field of nanomanufacturing and metrology with direct applications for pick and place assembly at the nanoscale.

Heterophase homojunction formation in atomically thin 2D layers is of great importance for next-generation nanoelectronics and optoelectronics applications. Technologically challenging, controllable transformation between the semiconducting and metallic phases of transition metal chalcogenides is of particular importance. Here, we demonstrate that controlled laser irradiation can be used to directly ablate PdSe 2 thin films using high power or trigger the local transformation of PdSe 2 into a metallic phase PdSe 2- x using lower laser power. Such transformations are possible due to the low decomposition temperature of PdSe 2 and a variety of stable phases compared to other 2D transition metal dichalcogenides. Scanning transmission electron microscopy is used to reveal the laser-induced Se-deficient phases of PdSe 2 material. The process sensitivity to the laser power allows patterning flexibility for resist-free device fabrication. The laser-patterned devices demonstrate that a laser-induced metallic phase PdSe 2- x is stable with increased conductivity by a factor of about 20 compared to PdSe 2 . These findings contribute to the development of nanoscale devices with homojunctions and scalable methods to achieve structural transformations in 2D materials.

Chalcogenide glasses as nanoscale thin films have become leading candidates for several optical and photonic technologies, ranging from reflective displays and filters to photonic memories. Current material systems, however, show strong optical absorption which limits their performance efficiencies and complicates device level integration. Herein, we report sputter deposited thin films of GeSe 3 , which are low loss and in which the flexible nature of the atomic structure results in thermally activated tunability in the refractive index as well as in the film's physical volume. Such changes, which occur beyond a threshold temperature are observed to be accumulative and directed toward a more equilibrium amorphous state of the film, instead of crystallization. Our results provide insight into a new type of configurability that is based on strong coupling in the material's opto-structural properties. The low optical losses in this material system combined with the tunability in the optical properties in the visible and near-infrared have direct application in higher performing optical coatings and in corrective optics.

Doping of two-dimensional materials provides them tunable physical properties and widens their applications. Here, we demonstrate the postgrowth doping strategy in monolayer and bilayer tungsten disulfide (WS 2 ) crystals, which utilizes a metal exchange mechanism, whereby Sn atoms become substitutional dopants in the W sites by energetically favorable replacement. We achieve this using chemical vapor deposition techniques, where high-quality grown WS 2 single crystals are first grown and then subsequently reacted with a SnS precursor. Thermal control of the exchange doping mechanism is revealed, indicating that a sufficiently high enough temperature is required to create the S vacancies that are the initial binding sites for the SnS precursor and metal exchange occurrence. This results in a better control of dopant distribution compared to the tradition all-in-one approach, where dopants are added during the growth phase. The Sn dopants exhibit an n-type doping behavior in the WS 2 layers based on the decreased threshold voltage obtained from transistor device measurements. Annular dark-field scanning transmission electron microscopy shows that in bilayer WS 2 the Sn doping occurs only in the top layer, creating vertical heterostructures with atomic layer doping precision. This postgrowth modification opens up ways to selectively dope one layer at a time and construct mixed stoichiometry vertical heterojunctions in bilayer crystals.

We show that grain boundaries (GBs) in polycrystalline monolayer WS 2 can act as conduction channels with a lower gate onset potential for field-effect transistors made parallel, compared to devices made in pristine areas and perpendicular to GBs. Localized doping at the GB causes photoluminescence quenching and a reduced Schottky barrier with the metal electrodes, resulting in higher conductivity at lower applied bias values. Samples are grown by chemical vapor deposition with large domains of ∼100 μm, enabling numerous devices to be made within single domains, across GBs and at many similar sites across the substrate to reveal similar behaviors. We corroborate our electrical measurements with Kelvin probe microscopy, highlighting the nature of the doping-type in the material to change at the grain boundaries. Molecular dynamics simulations of the GB are used to predict the atomic structure of the dislocations and meandering tilt GB behavior on the nanoscale. These results show that GBs can be used to provide conduction pathways that are different to transport across GBs and in pristine area for potential electronic applications.

Phase-change materials are increasingly being explored for photonics applications, ranging from high-resolution displays to artificial retinas. Surprisingly, our understanding of the underlying mechanism of light-matter interaction in these materials has been limited to photothermal crystallization because of its relevance in applications such as rewritable optical discs. Here, we report a photoconductivity study of nanoscale thin films of phase-change materials. We identify strong photoconductive behavior in phase-change materials, which we show to be a complex interplay of three independent mechanisms: photoconductive, photoinduced crystallization, and photoinduced thermoelectric effects. We find that these effects also congruously contribute to a substantial photovoltaic effect, even in notionally symmetric devices. Notably, we show that device engineering plays a decisive role in determining the dominant mechanism; the contribution of the photothermal effects to the extractable photocurrent can be reduced to <0.4% by varying the electrodes and device geometry. We then show that the contribution of these individual effects to the photoresponse is phase-dependent with the amorphous state being more photoactive than the crystalline state and that a reversible change occurs in the charge transport from thermionic to tunnelling during phase transformation. Finally, we demonstrate photodetectors with an order of magnitude tunability in photodetection responsivity and bandwidth using these materials. Our results provide insights to the photophysics of phase-change materials and highlight their potential in future optoelectronics.

Two-dimensional (2D) materials hold great promise in flexible electronics, but the weak van der Waals interlayer bonding may pose a problem during bending, where easy interlayer sliding can occur. Furthermore, thin films of rigid materials are often observed to delaminate from soft substrates during straining. Here, we study the influence of substrate strain on some of the heterostructure configurations we expect to find in devices, composed of three common 2D materials: graphene, tungsten disulfide, and boron nitride. We used photoluminescence (PL) spectroscopy to measure changes in the heterostructures with strain applied in situ. All heterostructures were fabricated directly on polymer substrates, using materials synthesized by chemical vapor deposition. We observed an inhomogeneous release of strain in all structures, leading to a nonrecoverable broadening of the PL peak and shift of the bandgap. This suggests the need for preconditioning devices before service to ensure stable behavior. A gradual time-dependent relaxation of strain between strain cycles was characterized using time-dependent measurements-an effect which could lead to drift of device behavior during operation. Furthermore, possible degradation was assessed by performing the strain and relax the cycle up to 200 times, where we found little further change after the initial shifts had stabilized. These results have important ramifications for devices fabricated from these and other 2D materials, as they suggest extra processing steps and considerations that must be taken to achieve consistent and stable properties.

Two-dimensional gallium sulfide (GaS) crystals are synthesized by a simple and efficient ambient pressure chemical vapor deposition (CVD) method using a single-source precursor of Ga 2 S 3 . The synthesized GaS structures involve triangular monolayer domains and multilayer flakes with thickness of 1 and 15 nm, respectively. Regions of continuous films of GaS are also achieved with about 0.7 cm 2 uniform coverage. This is achieved by using hydrogen carrier gas and the horizontally placed SiO 2 /Si substrates. Electron microscopy and spectroscopic measurements are used to characteristic the CVD-grown materials. This provides important insights into novel approaches for enlarging the domain size of GaS crystals and understanding of the growth mechanism using this precursor system., Competing Interests: The authors declare no competing financial interest.

Tin disulfide crystals with layered two-dimensional (2D) sheets are grown by chemical vapor deposition using a novel precursor approach and integrated into all 2D transistors with graphene (Gr) electrodes. The Gr:SnS 2 :Gr transistors exhibit excellent photodetector response with high detectivity and photoresponsivity. We show that the response of the all 2D photodetectors depends upon charge trapping at the interface and the Schottky barrier modulation. The thickness-dependent SnS 2 measurements in devices reveal a transition from the interface-dominated response for thin crystals to bulklike response for the thicker SnS 2 crystals, showing the sensitivity of devices fabricated using layered materials on the number of layers. These results show that SnS 2 has photosensing performance when combined with Gr electrodes that is comparable to other 2D transition metal dichalcogenides of MoS 2 and WS 2 .

The edge sites of MoS 2 are catalytically active for the hydrogen evolution reaction (HER), and growing monolayer structures that are edge-rich is desirable. Here, we show the production of large-area highly branched MoS 2 dendrites on amorphous SiO 2 /Si substrates using an atmospheric pressure chemical vapor deposition and explore their use in electrocatalysis. By tailoring the substrate construction, the monolayer MoS 2 evolves from triangular to dendritic morphology because of the change of growth conditions. The rough edges endow dendritic MoS 2 with a fractal dimension down to 1.54. The highly crystalline basal plane and the edge of the dendrites are visualized at atomic resolution using an annular dark field scanning transmission electron microscope. The monolayer dendrites exhibit strong photoluminescence, which is indicative of the direct band gap emission, which is preserved after being transferred. Post-transfer sulfur annealing restores the structural defects and decreases the n-type doping in MoS 2 monolayers. The annealed MoS 2 dendrites show good and highly durable HER performance on the glassy carbon with a large exchange current density of 32 μA cm geo -2 , demonstrating its viability as an efficient HER catalyst.

We show that hexagonal domains of monolayer tungsten disulfide (WS 2 ) grown by chemical vapor deposition (CVD) with powder precursors can have discrete segmentation in their photoluminescence (PL) emission intensity, forming symmetric patterns with alternating bright and dark regions. Two-dimensional maps of the PL reveal significant reduction within the segments associated with the longest sides of the hexagonal domains. Analysis of the PL spectra shows differences in the exciton to trion ratio, indicating variations in the exciton recombination dynamics. Monolayers of WS 2 hexagonal islands transferred to new substrates still exhibit this PL segmentation, ruling out local strain in the regions as the dominant cause. High-power laser irradiation causes preferential degradation of the bright segments by sulfur removal, indicating the presence of a more defective region that is higher in oxidative reactivity. Atomic force microscopy (AFM) images of topography and amplitude modes show uniform thickness of the WS 2 domains and no signs of segmentation. However, AFM phase maps do show the same segmentation of the domain as the PL maps and indicate that it is caused by some kind of structural difference that we could not clearly identify. These results provide important insights into the spatially varying properties of these CVD-grown transition metal dichalcogenide materials, which may be important for their effective implementation in fast photo sensors and optical switches.

We study the interactions in graphene/WS2 two-dimensional (2D) layered vertical heterostructures with variations in the areal coverage of graphene by the WS2. All 2D materials were grown by chemical vapor deposition and transferred layer by layer. Photoluminescence (PL) spectroscopy of WS2 on graphene showed PL quenching along with an increase in the ratio of exciton/trion emission, relative to WS2 on SiO2 surface, indicating a reduction in the n-type doping levels of WS2 as well as reduced radiative recombination quantum yield. Electrical measurements of a total of 220 graphene field effect transistors with different WS2 coverage showed double-Dirac points in the field effect measurements, where one is shifted closer toward the 0 V gate neutrality position due to the WS2 coverage. Photoirradiation of the WS2 on graphene region caused further Dirac point shifts, indicative of a reduction in the p-type doping levels of graphene, revealing that the photogenerated excitons in WS2 are split across the heterostructure by electron transfer from WS2 to graphene. Kelvin probe microscopy showed that regions of graphene covered with WS2 had a smaller work function and supports the model of electron transfer from WS2 to graphene. Our results demonstrate the formation of junctions within a graphene transistor through the spatial tuning of the work function of graphene using these 2D vertical heterostructures.

We study how grain boundaries (GB) in chemical vapor deposition (CVD) grown monolayer WS2 influence the electroluminescence (EL) behavior in lateral source-drain devices under bias. Real time imaging of the WS2 EL shows arcing between the electrodes when probing across a GB, which then localizes at the GB region as it erodes under high bias conditions. In contrast, single crystal WS2 domains showed no signs of arcing or localized EL. Analysis of the eroded GB region shows the formation of micro- and nanoribbons across the monolayer WS2 domains. Comparison of the EL spectrum with the photoluminescence spectrum from the monolayer WS2 shows close agreement, indicating the EL emission comes from direct band gap excitonic recombination. These results provide important insights into EL devices that utilize CVD grown monolayer transition metal dichalcogenides when GBs are present in the active device region.

Synthetic 2D crystal films grown by chemical vapor deposition are typically polycrystalline, and determining grain size within domains and continuous films is crucial for determining their structure. Here we show that grain boundaries in the 2D transition metal dichalcogenide WS2, grown by CVD, can be preferentially oxidized by controlled heating in air. Under our developed conditions, preferential degradation at the grain boundaries causes an increase in their physical size due to oxidation. This increase in size enables their clear and rapid identification using a standard optical microscope. We demonstrate that similar treatments in an Ar environment do no show this effect, confirming that oxidation is the main role in the structural change. Statistical analysis of grain boundary (GB) angles shows dominant mirror formation. Electrical biasing across the GB is shown to lead to changes at the GB and their observation under an optical microscope. Our approach enables high-throughput screening of as-synthesized WS2 domains and continuous films to determine their crystallinity and should enable improvements in future CVD growth of these materials.

The low mass and high quality factors that nanomechanical resonators exhibit lead to exceptional sensitivity in the frequency domain. This is especially appealing for the design of ultrasensitive force and mass sensors. The sensitivity of a nanomechanical mass and force sensor depends on its mass and quality factor; a low resonator mass and a higher quality factor reduce both the minimum resolvable mass and force. Graphene, a single atomic layer thick membrane is an ideal candidate for nanoelectromechanical resonators due to its extremely low mass and high stiffness. Here, we show that by employing the intrinsic piezoresistivity of graphene to transduce its motion in nanoelectromechanical systems, we approach a force resolution of 16.3 ± 0.8 aN/Hz(1/2) and a minimum detectable mass of 1.41 ± 0.02 zeptograms (10(-21) g) at ambient temperature. Quality factors of the driven response of the order of 10(3) at pressures ∼10(-6) Torr on several devices are also observed. Moreover, we demonstrate this at ambient temperature on chemical-vapor-deposition-grown graphene to allow for scale-up, thus demonstrating its potential for applications requiring exquisite force and mass resolution such as mass spectroscopy and magnetic resonance force microscopy.