Tunable Release of Ions from Graphene Oxide Laminates for Sustained Antibacterial Activity in a Biomimetic Environment.

Silver has long been recognized for its potent antimicrobial properties, but achieving a slow and longer-term delivery of silver ions presents significant challenges. Previous efforts to control silver ion dosages have struggled to sustain release for extended periods in biomimetic environments, especially in the presence of complex proteins. This challenge is underscored by the absence of technology for sustaining antimicrobial activity, especially in the context of orthopedic implants where long-term efficacy, extending beyond 7 days, is essential. In this study, the tunable, slow, and longer-term release of silver ions from the two-dimensional (2D) nanocapillaries of graphene oxide (GO) laminates incorporated with silver ions (Ag-GO) for antimicrobial applications are successfully demonstrated. To closely mimic a physiologically relevant serum-based environment, a novel in vitro study model using 100% fetal bovine serum (FBS) is introduced as the test medium for microbiology, biocompatibility, and bioactivity studies. To emulate fluid circulation in a physiological environment, the in vitro studies are challenged with serum exchange protocols on different days. The findings show that the Ag-GO coating can sustainably release silver ions at a minimum dosage of 10 µg cm-2 day-1, providing an effective and sustained antimicrobial barrier for over ten days.

Alternating Superconducting and Charge Density Wave Monolayers within Bulk 6R-TaS2.

Van der Waals (vdW) heterostructures continue to attract intense interest as a route of designing materials with novel properties that cannot be found in nature. Unfortunately, this approach is currently limited to only a few layers that can be stacked on top of each other. Here, we report a bulk vdW material consisting of superconducting 1H TaS2 monolayers interlayered with 1T TaS2 monolayers displaying charge density waves (CDW). This bulk vdW heterostructure is created by phase transition of 1T-TaS2 to 6R at 800 °C in an inert atmosphere. Its superconducting transition (Tc) is found at 2.6 K, exceeding the Tc of the bulk 2H phase. Using first-principles calculations, we argue that the coexistence of superconductivity and CDW within 6R-TaS2 stems from amalgamation of the properties of adjacent 1H and 1T monolayers, where the former dominates the superconducting state and the latter the CDW behavior.

Diffusion-Controlled Faradaic Charge Storage in High-Performance Solid Electrolyte-Gated Zinc Oxide Thin-Film Transistors.

An electrochemical device capable of manifesting reversible charge storage at the interface of an active layer offers formidable advantages, such as low switching energy and long retention time, in realizing synaptic behavior for ultralow power neuromorphic systems. Contrary to a supercapacitor-based field-effect device that is prone to low memory retention due to fast discharge, a solid electrolyte-gated ZnO thin-film device exhibiting a battery-controlled charge storage mechanism via mobile charges at its interface with tantalum oxide is demonstrated. Analysis via cyclic voltammetry and chronoamperometry uniquely distinguishes the battery behavior of these devices, with an electromotive force generated due to polarization of charges strongly dependent on the scan rate of the applied voltage. The Faradaic-type diffusion-controlled charge storage mechanism exhibited by these devices is capable of delivering robust enhancement in the channel conductance and leads to a superior ON-OFF ratio of 108-109. The nonvolatile behavior of the interface charge storage and slow diffusion of ions is utilized in efficiently emulating spike timing-dependent plasticity (STDP) at similar time scales of biological synapses and unveils the possibility of STDP behavior using multiple in-plane gates that alleviate additional requirement of waveform-shaping circuits.

Negative Capacitance beyond Ferroelectric Switches.

Negative capacitance transistors are a unique class of switches capable of operation beyond the Boltzmann limit to realize subthermionic switching. To date, the negative capacitance effect has been predominantly attributed to devices employing an unstable insulator with ferroelectric properties, exhibiting a two-well energy landscape, in accordance with the Landau theory. The theory and operation of a solid electrolyte field effect transistor (SE-FET) of subthreshold swing less than 60 mV/dec in the absence of a ferroelectric gate dielectric are demonstrated in this work. Unlike ferroelectric FETs that rely on a sudden switching of dipoles to achieve negative capacitance, we demonstrate a distinctive mechanism that relies on the accumulation and dispersion of ions at the interfaces of the oxide, leading to a subthreshold slope (SS) as low as 26 mV/dec in these samples. The frequency of operation of these unscaled devices lies in a few millihertz because at higher or lower frequencies, the ions in the insulator are either too fast or too slow to produce voltage amplification. This is unlike Landau switches, where the SS remains below 60 mV/dec even under quasi-static sweep of the gate bias. The proposed FETs show a higher on-current with a thicker oxide in the entire range of gate voltage, clearly distinguishing their scaling laws from those of ferroelectric FETs. Our theory, validated with experiment, demonstrates a new class of devices capable of negative capacitance that opens up alternate methods of steep switching beyond the traditional approach of ferroelectric or memristive FETs.

Nanoionics-Based Three-Terminal Synaptic Device Using Zinc Oxide.

Artificial synaptic thin film transistors (TFTs) capable of simultaneously manifesting signal transmission and self-learning are demonstrated using transparent zinc oxide (ZnO) in combination with high κ tantalum oxide as gate insulator. The devices exhibit pronounced memory retention with a memory window in excess of 4 V realized using an operating voltage less than 6 V. Gate polarity induced motion of oxygen vacancies in the gate insulator is proposed to play a vital role in emulating synaptic behavior, directly measured as the transmission of a signal between the source and drain (S/D) terminals, but with the added benefit of independent control of synaptic weight. Unlike in two terminal memristor/resistive switching devices, multistate memory levels are demonstrated using the gate terminal without hampering the signal transmission across the S/D electrodes. Synaptic functions in the devices can be emulated using a low programming voltage of 200 mV, an order of magnitude smaller than in conventional resistive random access memory and other field effect transistor based synaptic technologies. Robust synaptic properties demonstrated using fully transparent, ecofriendly inorganic materials chosen here show greater promise in realizing scalable synaptic devices compared to organic synaptic and other liquid electrolyte gated device technologies. Most importantly, the strong coupling between the in-plane gate and semiconductor channel through ionic charge in the gate insulator shown by these devices, can lead to an artificial neural network with multiple presynaptic terminals for complex synaptic learning processes. This provides opportunities to alleviate the extreme requirements of component and interconnect density in realizing brainlike systems.