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Here, we propose phase and interfacial engineering by inserting a functional WO 3 layer and selenized it to achieve a 2D-layered WSe 2 /WO 3 heterolayer structure by a plasma-assisted selenization process. The 2D-layered WSe 2 /WO 3 heterolayer was coupled with an Al 2 O 3 film as a resistive switching (RS) layer to form a hybrid structure, with which Pt and W films were used as the top and bottom electrodes, respectively. The device with good uniformity in SET/RESET voltage and high low-/high-resistance window can be obtained by controlling a conversion ratio from a WO 3 film to a 2D-layered WSe 2 thin film. The Pt/Al 2 O 3 /(2D-layered WSe 2 /WO 3 )/W structure shows remarkable improvement to the pristine Pt/Al 2 O 3 /W and Pt/Al 2 O 3 /2D-layered WO 3 /W in terms of low SET/RESET voltage variability (-20/20)%, multilevel characteristics (uniform LRS/HRS distribution), high on/off ratio (10 4 -10 5 ), and retention (∼10 5 s). The thickness of the obtained WSe 2 was tuned at different gas ratios to optimize different 2D-layered WSe 2 /WO 3 (%) ratios, showing a distinctive trend of reduced and uniform SET/RESET voltage variability as 2D-layered WSe 2 /WO 3 (%) changes from 90/10 (%) to 45/55 (%), respectively. The electrical measurements confirm the superior ability of the metallic 1T phase of the 2D-layered WSe 2 over the semiconducting 2H phase. Through systemic studies of RS behaviors on the effect of 1T/2H phases and 2D-layered WSe 2 /WO 3 ratios, the low-temperature plasma-assisted selenization offers compatibility with the temperature-limited 3D integration process and also provides much better thickness control over a large area.

In this work, a low-power memristor based on vertically stacked two-dimensional (2D) layered materials, achieved by plasma-assisted vapor reaction, as the switching material, with which the copper and gold metals as electrodes featured by reversible polymorphous phase changes from a conducting 1T-phase to a semiconducting 2H-one once copper cations interacted between vertical lamellar layers and vice versa, was demonstrated. Here, molybdenum diselenide was chosen as the switching material, and the reversible polymorphous phase changes activated by the intercalation of Cu cations were confirmed by pseudo-operando Raman scattering, transmission electron microscopy, and scanning photoelectron microscopy under high and low resistance states, respectively. The switching can be activated at about ±1 V with critical currents less than 10 μA with an on/off ratio approaching 100 after 100 cycles and low power consumption of ∼0.1 microwatt as well as linear weight updates controlled by the amount of intercalation. The work provides alternative feasibility of reversible and all-solid-state metal interactions, which benefits monolithic integrations of 2D materials into operative electronic circuits.

Objective: Stromal barriers, such as the abundant desmoplastic stroma that is characteristic of pancreatic ductal adenocarcinoma (PDAC), can block the delivery and decrease the tumour-penetrating ability of therapeutics such as tumour necrosis factor-related apoptosis-inducing ligand (TRAIL), which can selectively induce cancer cell apoptosis. This study aimed to develop a TRAIL-based nanotherapy that not only eliminated the extracellular matrix barrier to increase TRAIL delivery into tumours but also blocked antiapoptotic mechanisms to overcome TRAIL resistance in PDAC., Design: Nitric oxide (NO) plays a role in preventing tissue desmoplasia and could thus be delivered to disrupt the stromal barrier and improve TRAIL delivery in PDAC. We applied an in vitro-in vivo combinatorial phage display technique to identify novel peptide ligands to target the desmoplastic stroma in both murine and human orthotopic PDAC. We then constructed a stroma-targeted nanogel modified with phage display-identified tumour stroma-targeting peptides to co-deliver NO and TRAIL to PDAC and examined the anticancer effect in three-dimensional spheroid cultures in vitro and in orthotopic PDAC models in vivo ., Results: The delivery of NO to the PDAC tumour stroma resulted in reprogramming of activated pancreatic stellate cells, alleviation of tumour desmoplasia and downregulation of antiapoptotic BCL-2 protein expression, thereby facilitating tumour penetration by TRAIL and substantially enhancing the antitumour efficacy of TRAIL therapy., Conclusion: The co-delivery of TRAIL and NO by a stroma-targeted nanogel that remodels the fibrotic tumour microenvironment and suppresses tumour growth has the potential to be translated into a safe and promising treatment for PDAC., Competing Interests: Competing interests: None declared., (© Author(s) (or their employer(s)) 2022. Re-use permitted under CC BY-NC. No commercial re-use. See rights and permissions. Published by BMJ.)

A conductive-bridge random access memory (CBRAM) has been considered a promising candidate for the next-generation nonvolatile memory technology because of its excellent performance, for which the resistive switching behavior depends on the formation/dissolution of conducting filaments in an electrolyte layer originated by the cation injection from the active electrode with electrochemical reactions. Typically, the controllability of cations into the electrolyte layer is a main issue, leading to stable switching reliability. In this work, an architecture combining spike-shaped Ag electrodes created by Al 2 O 3 nanopillar arrays as a physical diffusion barrier by glancing angle deposition technology was proposed to localize Ag cation injection for the formation of controllable filaments inside TiO x as the switching layer. Interestingly, the dimension of the Ag plugs defined by the topography of Al 2 O 3 nanopillar arrays can control Ag cation injection to influence the dimensionality of conductive filaments. Compared to the typical planar-Ag/TiO x /Pt device, the spiked-Ag/Al 2 O 3 nanopillar arrays/TiO x /Pt device shows improvement of endurance and voltage disturbance. With enhanced multilevel characteristics, the spiked active-metal-based CBRAM device can be expected to serve as an analogue synapse for neuromorphic applications.

Here, a current-accelerated phase cycling by an in situ current-induced oxidation process was demonstrated to reversibly switch the local metallic Cu and semiconducting Cu 2 O phases of patterned polycrystalline copper nanobelts. Once the Cu nanobelts were applied by a direct-current bias of ∼0.5 to 1 V in air with opposite polarities, the resistance between several hundred ohms and more than MΩ can be manipulated. In practice, the thickness of 60 nm with a moderate grain size inhibiting both electromigration and permanent oxidation is the optimized condition for reversible switching when the oxygen supply is sufficient. More than 40% of the copper localized beneath the positively biased electrode was oxidized assisted by the Joule heating, blocking the current flow. On the contrary, the reduction reaction of Cu 2 O was activated by the thermally assisted electromigration of Cu atoms penetrating the interlayer at the reverse bias. Finally, based on a high on/off ratio, the fast switching and the scalable production, reusable feasibility based on copper nanobelts such as the memristor array was demonstrated.

Antiangiogenic therapy is widely administered in many cancers, and the antiangiogenic drug sorafenib offers moderate benefits in advanced hepatocellular carcinoma (HCC). However, antiangiogenic therapy can also lead to hypoxia-driven angiogenesis and immunosuppression in the tumor microenvironment (TME) and metastasis. Here, we report the synthesis and evaluation of NanoMnSor, a tumor-targeted, nanoparticle drug carrier that efficiently codelivers oxygen-generating MnO 2 and sorafenib into HCC. We found that MnO 2 not only alleviates hypoxia by catalyzing the decomposition of H 2 O 2 to oxygen but also enhances pH/redox-responsive T1-weighted magnetic resonance imaging and drug-release properties upon decomposition into Mn 2+ ions in the TME. Moreover, macrophages exposed to MnO 2 displayed increased mRNA associated with the immunostimulatory M1 phenotype. We further show that NanoMnSor treatment leads to sorafenib-induced decrease in tumor vascularization and significantly suppresses primary tumor growth and distal metastasis, resulting in improved overall survival in a mouse orthotopic HCC model. Furthermore, NanoMnSor reprograms the immunosuppressive TME by reducing the hypoxia-induced tumor infiltration of tumor-associated macrophages, promoting macrophage polarization toward the immunostimulatory M1 phenotype, and increasing the number of CD8 + cytotoxic T cells in tumors, thereby augmenting the efficacy of anti-PD-1 antibody and whole-cell cancer vaccine immunotherapies. Our study demonstrates the potential of oxygen-generating nanoparticles to deliver antiangiogenic agents, efficiently modulate the hypoxic TME, and overcome hypoxia-driven drug resistance, thereby providing therapeutic benefit in cancer.

Aluminum-sulfur batteries (ASBs) have attracted substantial interest due to their high theoretical specific energy density, low cost, and environmental friendliness, while the traditional sulfur cathode and ionic liquid have very fast capacity decay, limiting cycling performance because of the sluggishly electrochemical reaction and side reactions with the electrolyte. Herein, we demonstrate, for the first time, excellent rechargeable aluminum-selenium batteries (ASeBs) using a new deep eutectic solvent, thiourea-AlCl 3 , as an electrolyte and Se nanowires grown directly on a flexible carbon cloth substrate (Se NWs@CC) by a low-temperature selenization process as a cathode. Selenium (Se) is a chemical analogue of sulfur with higher electronic conductivity and lower ionization potential that can improve the battery kinetics on the sluggishly electrochemical reaction and the reduction of the polarization where the thiourea-AlCl 3 electrolyte can stabilize the side reaction during the reversible conversion reaction of Al-Se alloying processes during the charge-discharge process, yielding a high specific capacity of 260 mAh g -1 at 50 mA g -1 and a long cycling life of 100 times with a high Coulombic efficiency of nearly 93% at 100 mA g -1 . The working mechanism based on the reversible conversion reaction of the Al-Se alloying processes, confirmed by the ex situ Raman, XRD, and XPS measurements, was proposed. This work provides new insights into the development of rechargeable aluminum-chalcogenide (S, Se, and Te) batteries.

While immunotherapy holds great promise for combating cancer, the limited efficacy due to an immunosuppressive tumor microenvironment and systemic toxicity hinder the broader application of cancer immunotherapy. Here, we report a combinatorial immunotherapy approach that uses a highly efficient and tumor-selective gene carrier to improve anticancer efficacy and circumvent the systemic toxicity. In this study, we engineered tumor-targeted lipid-dendrimer-calcium-phosphate (TT-LDCP) nanoparticles (NPs) with thymine-functionalized dendrimers that exhibit not only enhanced gene delivery capacity but also immune adjuvant properties by activating the stimulator of interferon genes (STING)-cGAS pathway. TT-LDCP NPs delivered siRNA against immune checkpoint ligand PD-L1 and immunostimulatory IL-2-encoding plasmid DNA to hepatocellular carcinoma (HCC), increased tumoral infiltration and activation of CD8 + T cells, augmented the efficacy of cancer vaccine immunotherapy, and suppressed HCC progression. Our work presents nanotechnology-enabled dual delivery of siRNA and plasmid DNA that selectively targets and reprograms the immunosuppressive tumor microenvironment to improve cancer immunotherapy., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).)

Selenium (Se) is one of the potential candidates as photodetector because of its outstanding properties such as high photoconductivity (∼8 × 10 4 S cm -1 ), piezoelectricity, thermoelectricity, and nonlinear optical responses. Solution phase synthesis becomes an efficient way to produce Se, but a contamination issue that could deteriorate the electric characteristic of Se should be taken into account. In this work, a facile, controllable approach of synthesizing Se nanowires (NWs)/films via a plasma-assisted growth process was demonstrated at the low substrate temperature of 100 °C. The detailed formation mechanisms of nanowires arrays to thin films at different plasma powers were investigated. Moreover, indium (In) layer was used to enhance the adhesive strength with 50% improvement on a SiO 2 /Si substrate by mechanical interlocking and surface alloying between Se and In layers, indicating great tolerance for mechanical stress for future wearable devices applications. Furthermore, the direct growth of Se NWs/films on a poly(ethylene terephthalate) substrate was demonstrated, exhibiting a visible to broad infrared detection ranges from 405 to 1555 nm with a high on/off ratio of ∼700 as well as the fast response time less than 25 ms. In addition, the devices exhibited fascinating stability in the atmosphere over one month.

In this work, polymethylmethacrylate (PMMA) as a superior mediate for the pressure welding of silver nanowires (Ag NWs) networks as transparent electrodes without any thermal treatment is demonstrated. After a pressing of 200 kg cm -2 , not only the sheet resistance but also the surface roughness of the PMMA-mediated Ag NWs networks decreases from 2.6 kΩ sq -1 to 34.3 Ω sq -1 and from 76.1 to 12.6 nm, respectively. On the other hand, high transparency of an average transmittance in the visible wavelengths of 93.5% together with a low haze value of 2.58% can be achieved. In terms of optoelectronic applications, the promising potential of the PMMA-mediated pressure-welded Ag NWs networks used as a transparent electrode in a green organic light-emitting diode (OLED) device is also demonstrated. In comparison with the OLED based on commercial tin-doped indium oxide electrode, the increments of power efficiency and external quantum efficiency (EQE) from 80.1 to 85.9 lm w -1 and 19.2% to 19.9% are demonstrated. In addition, the PMMA-mediated pressure welding succeeds in transferring Ag NWs networks to flexible polyethylene naphthalate and polyimide substrates with the sheet resistance of 42 and 91 Ω sq -1 after 10 000 times of bending, respectively., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The formation of PtSe 2 -layered films is reported in a large area by the direct plasma-assisted selenization of Pt films at a low temperature, where temperatures, as low as 100 °C at the applied plasma power of 400 W can be achieved. As the thickness of the Pt film exceeds 5 nm, the PtSe 2 -layered film (five monolayers) exhibits a metallic behavior. A clear p-type semiconducting behavior of the PtSe 2 -layered film (≈trilayers) is observed with the average field effective mobility of 0.7 cm 2 V -1 s -1 from back-gated transistor measurements as the thickness of the Pt film reaches below 2.5 nm. A full PtSe 2 field effect transistor is demonstrated where the thinner PtSe 2 , exhibiting a semiconducting behavior, is used as the channel material, and the thicker PtSe 2 , exhibiting a metallic behavior, is used as an electrode, yielding an ohmic contact. Furthermore, photodetectors using a few PtSe 2 -layered films as an adsorption layer synthesized at the low temperature on a flexible substrate exhibit a wide range of absorption and photoresponse with the highest photocurrent of 9 µA under the laser wavelength of 408 nm. In addition, the device can maintain a high photoresponse under a large bending stress and 1000 bending cycles., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Direct reduction of metal oxides into a few transition metal dichalcogenide (TMDCs) monolayers has been recently explored as an alternative method for large area and uniform deposition. However, not many studies have addressed the characteristics and requirement of the metal oxides into TMDCs by the selenization/sulfurization processes, yielding a wide range of outstanding properties to poor electrical characteristics with nonuniform films. The large difference implies that the process is yet not fully understood. In particular, the selenization/sulfurization at low temperature leads to poor crystallinity films with poor electrical performance, hindering its practical development. A common approach to improve the quality of the selenized/sulfurized films is by further increasing the process temperature, thus requiring additional transfer in order to explore the electrical properties. Here, we show that by finely tuning the quality of the predeposited oxide the selenization/sulfurization temperature can be largely decreased, avoiding major substrate damage and allowing direct device fabrication. The direct relationship between the role of selecting different metal oxides prepared by e-beam evaporation and reactive sputtering and their oxygen deficiency/vacancy leading to quality influence of TMDCs was investigated in detail. Because of its outstanding physical properties, the formation of tungsten diselenide (WSe 2 ) from the reduction of tungsten oxide (WO x ) was chosen as a model for proof of concept. By optimizing the process parameters and the selection of metal oxides, layered WSe 2 films with controlled atomic thickness can be demonstrated. Interestingly, the domain size and electrical properties of the layered WSe 2 films are highly affected by the quality of the metal oxides, for which the layered WSe 2 film with small domains exhibits a metallic behavior and the layered WSe 2 films with larger domains provides clear semiconducting behavior. Finally, an 8'' wafer scale-layered WSe 2 film was demonstrated, giving a step forward in the development of 2D TMDC electronics in the industry.

The necessity for new sources for greener and cleaner energy production to replace the existing ones has been increasingly growing in recent years. Of those new sources, the hydrogen evolution reaction has a large potential. In this work, for the first time, MoSe 2 /Mo core-shell 3D-hierarchical nanostructures are created, which are derived from the Mo 3D-hierarchical nanostructures through a low-temperature plasma-assisted selenization process with controlled shapes grown by a glancing angle deposition system., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Graphene, a two-dimensional material with honeycomb arrays of carbon atoms, has shown outstanding physical properties that make it a promising candidate material for a variety of electronic applications. To date, several issues related to the material synthesis and device fabrication need to be overcome. Despite the fact that large-area graphene films synthesised by chemical vapour deposition (CVD) can be grown with relatively few defects, the required transfer process creates wrinkles and polymer residues that greatly reduce its performance in device applications. Graphene synthesised on silicon carbide (SiC) has shown outstanding mobility and has been successfully used to develop ultra-high frequency transistors; however, this fabrication method is limited due to the use of costly ultra-high vacuum (UHV) equipment that can reach temperatures over 1500 °C. Here, we show a simple and novel approach to synthesise graphene on SiC substrates that greatly reduces the temperature and vacuum requirements and allows the use of equipment commonly used in the semiconductor processing industry. In this work, we used plasma treatment followed by annealing in order to obtain large-scale graphene films from bulk SiC. After exposure to N2 plasma, the annealing process promotes the reaction of nitrogen ions with Si and the simultaneous condensation of C on the surface of SiC. Eventually, a uniform, large-scale, n-type graphene film with remarkable transport behaviour on the SiC wafer is achieved. Furthermore, graphene field effect transistors (FETs) with high carrier mobilities on SiC were also demonstrated in this study.

Tunable multilevel storage of complementary resistive switching (CRS) on single-step formation of ZnO/ZnWOx bilayer structure via interfacial engineering was demonstrated for the first time. In addition, the performance of the ZnO/ZnWOx-based CRS device with the voltage- and current-sweep modes was demonstrated and investigated in detail. The resistance switching behaviors of the ZnO/ZnWOx bilayer ReRAM with adjustable RESET-stop voltages was explained using an electrochemical redox reaction model whose electron-hopping activation energies of 28, 40, and 133 meV can be obtained from Arrhenius equation at RESET-stop voltages of 1.0, 1.3, and 1.5 V, respectively. In the case of the voltage-sweep operation on the ZnO-based CRS device, the maximum array numbers (N) of 9, 15, and 31 at RESET-stop voltages of 1.4, 1.5, and 1.6 V were estimated, while the maximum array numbers increase into 47, 63, and 105 at RESET-stop voltages of 2.0, 2.2, and 2.4 V, operated by the current-sweep mode, respectively. In addition, the endurance tests show a very stable multilevel operation at each RESET-stop voltage under the current-sweep mode.

CuOx nanowires were synthesized by a low-cost and large-scale electrochemical process with AAO membranes at room temperature and its resistive switching has been demonstrated. The switching characteristic exhibits forming-free and low electric-field switching operation due to coexistence of significant amount of defects and Cu nanocrystals in the partially oxidized nanowires. The detailed resistive switching characteristics of CuOx nanowire systems have been investigated and possible switching mechanisms are systematically proposed based on the microstructural and chemical analysis via transmission electron microscopy.

An optical polymeric biochip system based on the complementary metal oxide semiconductor (CMOS) photo array sensor and polymeric enzyme biochip for rapidly quantitating uric acid in a one-step procedure was developed. The CMOS sensor was designed with N(+)/P-well structure and manufactured using a standard 0.5 microm CMOS process. The polymeric enzyme biochip was immobilized with uricase-peroxidase and used to fill the reacting medium with the sample. This study encompasses the cloning of the Bacillus subtilis uricase gene and expression in Escherichia coli, as well as the purification of uricase and measurement of its activity. The cloned uricase gene included an open reading frame of 1491 nucleotides that encodes a protein of approximately 55 kDa. The expression of the putative MBP-fusion protein involved approximately 98 kDa of the protein. The CMOS sensor response was stronger at a higher temperature range of 20-40 degrees C, with optimal pH at 8.5. The calibration curve of purified uric acid was linear in the concentration range from 2.5 to 12.5 mg/dL. The results obtained for serum uric acid correlated quite closely with those obtained using the Beckman Synchron method.

We designed a complementary metal oxide semiconductor (CMOS) chip with accompanied accessories as a system for the detections and quantifications of biochemical luminescence. This is the first of such instruments that has been reported. The semiconductor chip was manufactured through a 0.25 microm CMOS standard process. A current mirror was designed in integrated circuit (IC) to amplify the signal current that was induced by chemiluminescence. Horseradish peroxidase (HRP)-luminol-H2O2 system was used as an example to constitute a useful platform for coupling to chemiluminescence reactions which produce H2O2. Glucose-glucose oxidase (GOD) reaction was coupled with HRP-luminol-H2O2 reaction to demonstrate the ability of the novel CMOS base instrument for quantifying the biological luminescence of a variety of valuable clinical assays. Our results illustrated that the combination of the specifically designed CMOS IC and commercially available electronic devices established a simple and useful bioanalytical tool.