Ag Ion Migration Research Articles

Halide Perovskites-Based Diffusive Memristors for Artificial Mechano-Nociceptive System.

Numerous efforts for emulating organ systems comprised of multiple functional units have driven substantial advancements in bio-realistic electronics and systems. The resistance change behavior observed in diffusive memristors shares similarities with the potential change in biological neurons. Here, the diffusive threshold switching phenomenon in Ag-incorporated organometallic halide perovskites is utilized to demonstrate the functions of afferent neurons. Halide perovskites-based diffusive memristors show a low threshold voltage of ≈0.2V with little variation, attributed to the facile migration of Ag ions uniformly dispersed within the halide matrix. Based on the reversible and reliable volatile threshold switching, the memristors successfully demonstrate fundamental nociceptive functions including threshold firing, relaxation, and sensitization. Furthermore, to replicate the biological mechano-nociceptive phenomenon at a system level, an artificial mechano-nociceptive system is built by integrating a diffusive memristor with a force-sensing resistor. The presented system is capable of detecting and discerning the detrimental impact caused by a heavy steel ball, effectively exhibiting the corresponding sensitization response. By further extending the single nociceptive system into a 5 × 5 array, successful stereoscopic nociception of uneven impulses is achieved in the artificial skin system through array-scale sensitization. These results represent significant progress in the field of bio-inspired electronics and systems.

High-performance Ta2O5-based resistive random-access memory with embedded graphene quantum dots and Pt–Ag composite active layer

Resistive random-access memory (RRAM) has garnered significant interest in developing nonvolatile memory systems due to its ability to provide external field tunable resistive states with fast speed and low power consumption. This tunable resistive state primarily results from the formation and breakage of conductive pathways triggered by active ion migration. However, due to the stochastic nature of ion migration, the stability of the switching process is a long-standing bottleneck. Here, we investigate the impact of device kinetic parameters on the stability of resistive switching behavior and propose a high-performance RRAM with a Pt–Ag/Ta2O5/GQDs/Pt structure. Incorporating quantum dots can regulate the direction of Ag ion migration, while the Pt–Ag composite electrode can manipulate the oxidation rate of Ag atoms. Compared to the Ag/Ta2O5/GQDs/Pt device, the Pt–Ag/Ta2O5/GQDs/Pt device exhibited a 15-fold reduction in operating voltage, a 10-fold increase in on/off ratio, and superior endurance and uniformity. These findings demonstrate that tuning kinetic parameters has the potential to enhance resistive switching performance, which offers an effective pathway for designing high-performance memory systems.

Topological Data analysis of Ion Migration Mechanism.

Topological data analysis based on persistent homology has been applied to the molecular dynamics simulation for the fast ion-conducting phase (α-phase) of AgI to show its effectiveness on the ion migration mechanism analysis. Time-averaged persistence diagrams of α-AgI, which quantitatively record the shape and size of the ring structures in the given atomic configurations, clearly showed the emergence of the four-membered rings formed by two Ag and two I ions at high temperatures. They were identified as common structures during the Ag ion migration. The averaged potential energy change due to the deformation of the four-membered ring during Ag migration agrees well with the activation energy calculated from the conductivity Arrhenius plot. The concerted motion of two Ag ions via the four-membered ring was also successfully extracted from molecular dynamics simulations by our approach, providing new insight into the specific mechanism of the concerted motion.

Amyloid–Gold Nanoparticle Hybrids for Biocompatible Memristive Devices

Biomolecular materials offer tremendous potential for the development of memristive devices due to their low cost of production, environmental friendliness, and, most notably, biocompatibility. Herein, biocompatible memristive devices based on amyloid-gold nanoparticle hybrids have been investigated. These memristors demonstrate excellent electrical performance, featuring an ultrahigh Roff/Ron ratio (>107), a low switching voltage (<0.8 V), and reliable reproducibility. Additionally, the reversible transition from threshold switching to resistive switching mode was achieved in this work. The arrangement of peptides in amyloid fibrils endows the surface polarity and phenylalanine packing, which provides channels for the migration of Ag ions in the memristors. By modulating voltage pulse signals, the study successfully imitates the synaptic behavior of excitatory postsynaptic current (EPSC), paired-pulse facilitation (PPF), and the transition from short-term plasticity (STP) to long-term plasticity (LTP). More interestingly, Boolean logic standard cells were designed and simulated using the memristive devices. The fundamental and experimental results of this study thus offer insights into the utilization of biomolecular materials for advanced memristive devices.

Improvement of forming-free threshold switching reliability of CeO2-based selector device by controlling volatile filament formation behaviors

Diffusive memristor-based threshold switching devices are promising candidates for selectors in the crossbar memory architecture. However, the reliability and uniformity of the devices are primary concerns due to uncontrolled diffusion of metal ions in the solid electrolyte of diffusive memristors. In this study, CeO2-based selectors with Ag electrodes were demonstrated to have forming-free threshold switching characteristics. In particular, by inserting an amorphous SiO2 layer in a CeO2-based selector device, we have effectively controlled volatile filament formation that is essential for uniform and reliable switching operations. The inserted SiO2 layer acts as a barrier that could retard the migration of Ag ions and prevents the formation of strong filaments in the solid electrolyte. This enables the bilayer device to have improved uniformity and cyclic endurance. The proposed selector device, Ag/CeO2/SiO2/Pt, showed excellent DC I–V switching cycles (103), high selectivity of 104, good endurance (&amp;gt;104), and narrow distribution of switching voltages. These results would be helpful to implement CeO2-based threshold switching devices as selectors for high-density storage crossbar memory architectures.

Exploring Low Power and Ultrafast Memristor on p-Type van der Waals SnS.

Memristor devices that exhibit high integration density, fast speed, and low power consumption are candidates for neuromorphic devices. Here, we demonstrate a filament-based memristor using p-type SnS as the resistive switching material, exhibiting superlative metrics such as a switching voltage ∼0.2 V, a switching speed faster than 1.5 ns, high endurance switching cycles, and an ultralarge on/off ratio of 108. The device exhibits a power consumption as low as ∼100 fJ per switch. Chip-level simulations of the memristor based on 32 × 32 high-density crossbar arrays with 50 nm feature size reveal on-chip learning accuracy of 87.76% (close to the ideal software accuracy 90%) for CIFAR-10 image classifications. The ultrafast and low energy switching of p-type SnS compared to n-type transition metal dichalcogenides is attributed to the presence of cation vacancies and van der Waals gap that lower the activation barrier for Ag ion migration.

Oxide Passivation of Halide Perovskite Resistive Memory Device: A Strategy for Overcoming Endurance Problem.

Owing to a low operation voltage, high on/off ratio, and tunable band gap, halide perovskites (HPs) are being conceived as an alternative to oxide or chalcogenide materials in resistive-switching (RS) memory devices. However, the HP-based RS memory devices face problems such as short endurance, low retention, and device stability. Herein, the oxide-passivated HP devices were fabricated by hybridizing the oxide sol-gel and halide adduct methods. The silicon oxide (SiO2)-passivation enhanced the device properties with an endurance of 6000 cycles and retention of 1.8 × 104 s. The study of activation energy using ionic conductivity and time-of-flight secondary-ion mass spectroscopy demonstrated that the migration path of the Ag ions is well-controlled by the SiO2 passivation layer. Various oxides were used as passivation materials. Especially, the zirconium oxide-passivated devices exhibit excellent properties with an endurance of 57 000 cycles and retention of 7.8 × 104 s. The high cohesive energy of oxides effectively increased the formation voltage by retarding the Ag-ion migration, leading to the improved endurance properties of the devices. This paper proposes a strategy for significantly improving the low endurance property of HP-based RS memory devices using the oxide passivation technology.

Effects of electron beam irradiation on a Ag/AsS2 bilayer using conductive atomic force microscopy

Metal-chalcogenide systems are used in a variety of fields, including microelectromechanical systems, plasmonics, photonics and the fabrication of X-ray masks. The development of fabrication methods for micro- and nanostructures in metal-chalcogenide bilayers is of significant interest for these fields. This study investigates the effects of electron beam irradiation in an Ag/AsS2 bilayer using conductive atomic force microscopy. An unusual distribution of conductivity is observed, which suggests the presence of at least two competing mechanisms of Ag-ion migration within the amorphous chalcogenide during electron beam irradiation. The surface relief of the Ag/AsS2 bilayer is modified by an electric field from the conductive atomic force microscopy probe.

Self-assembling crystalline peptide microrod for neuromorphic function implementation

Self-assembling crystalline peptide microrod for neuromorphic function implementation

Zeolite‐Based Memristive Synapse with Ultralow Sub‐10‐fJ Energy Consumption for Neuromorphic Computation

The development of neuromorphic computation faces the appreciable challenge of implementing hardware with energy consumption on the level of a femtojoule per synaptic event to be comparable with the energy consumption of human brain. Controllable ultrathin conductive filaments are needed to achieve such extremely low energy consumption in memristive synapses but their formation is difficult to control owing to their stochastic morphology and unexpected overgrowth. Herein, a zeolite-based memristive synapse is demonstrated for the first time, in which Ag exchange in the sub-nanometer pore closely resembles synaptic Ca2+ dynamics across biomembrane channel. Particularly, the confined ultrasmall pore and low Ag ion migration barrier give the zeolite-based memristive synapse ultralow energy consumption below 10 fJ per synaptic spike, on par with the biological counterpart. Experimental results reveal that the gradual memristive effect is attributed to the dimension modulation of Ag clusters. In addition to emulating inherent cognitive functions through electrical stimulations, the experience-dependent transition of short-term plasticity to long-term plasticity using a chemical modulation method is achieved by treating the initial Ag quantity as a learning experience. The proposed memristors can be used to develop highly efficient memristive neural networks and are considered as a candidate for application in neuromorphic computation.

Suppressed Stochastic Switching Behavior and Improved Synaptic Functions in an Atomic Switch Embedded with a 2D NbSe2 Material.

We investigated chemical vapor-deposited (CVD) two-dimensional (2D) niobium diselenide (NbSe2) material for the resistive switching and synaptic characteristics. Three different atomic switch devices with Ag/HfO2/Pt, Ag/Ti/HfO2/Pt, and Ag/NbSe2/HfO2/Pt were studied as both memory and neuromorphic devices. Both the inserted Ti and NbSe2 buffer layers effectively control the stochastic Ag-ion diffusion, leading to suppressed variation of switching characteristics, which is a critical issue in an atomic switch device. Especially, the device with the 2D NbSe2 buffer layer strikingly enhanced the device reliability in both endurance and retention. In conjunction with scanning transmission electron microscopy (STEM) and energy-dispersive spectrometry (EDS) analysis of the control of the Ag-ion migration, it was understood that filament connection is interrelated with the SET and RESET processes. Besides resistive behaviors in the memory device, various synapse functions such as spike-rate-dependent plasticity (SRDP), forgetting curve, potentiation, and depression were demonstrated with an atomic switch with the 2D NbSe2 buffer layer. Furthermore, the emulated long-term synaptic property was simulated using the MNIST 28 × 28 pixel database. Using adopting a CVD 2D NbSe2 blocking layer, the stochastic Ag-ion diffusion behavior is well-controlled and therefore stable switching and synapse functions are attained.

Understanding interfacial chemistry of positive bias high-voltage degradation in photovoltaic modules

Photovoltaic module degradation from a high system voltage is a prevalent degradation mode in the field, where the enabling degradation mechanisms are inherently dependent on the voltage bias polarity of the installed system. Here, the effects of positive bias on module performance are confirmed and the underlying chemical degradation processes are more thoroughly investigated to reveal different degradation pathways from those previously reported in negative bias studies. When cells are under +1000 V stress, crystalline silicon mini-modules with poly(ethylene-co-vinyl acetate) (EVA) encapsulant demonstrated a significant photocurrent loss due to EVA discoloration and delamination from increased chemical reactivity at the front-side EVA/cell metallization interface. Brown discoloration of the EVA encapsulant near the cell gridlines is linked to an electrochemical reaction at the Ag gridlines under hot and humid conditions (85 °C, 85% relative humidity). Chemical compositional analysis using X-ray photoelectron spectroscopy (XPS) confirmed that the discoloration is attributed to the formation of silver sulfide (Ag2S) and/or silver oxide (Ag2O) species at the EVA/Ag gridline interface. The subsequent migration of Ag ions from the cell gridlines into the bulk of the EVA was evident from XPS depth profiling and optical microscopy. However, the Ag signal was not detected at the EVA/glass interface, inferring limited ionic transport through the nominally 0.45 mm thick encapsulant. For the samples studied herein, the sulfur is believed by the process of elimination to come from the ambient air, diffusing into the module through the permeable polymer backsheet.

Abruptly-Switching MoS₂-Channel Atomic-Threshold-Switching Field-Effect Transistor With AgTi/HfO₂-Based Threshold Switching Device

A two-dimension (2D) atomic-threshold-switching field-effect transistor (ATS-FET) was implemented, by connecting an AgTi/HfO2-based threshold-switching (TS) device in series to the drain electrode of the 2D baseline-FET with molybdenum disulfide (MoS2) channel material. We optimized/developed the Ag/HfO2-based TS device because its characteristic is associated to the way how to achieve high performance of the 2D ATS-FET. By reducing the effective device area of the Ag/HfO2-based TS device down to $4~\mu \text{m}^{2}$ , low threshold voltage ( $\text{V}_{\mathrm {T}} \sim 0.42$ V), low threshold current (IT, drain current at the threshold voltage, $\sim 3.79 \times 10^{-11}$ A), and low VT variation (~0.09 V) were achieved. This is because the randomly formed filaments and electric field are better controlled with the scaled effective area. Next, the titanium (Ti)-injection barrier layer was inserted between the top electrode and the switching layer, while maintaining the optimized area in the TS device. The inserted Ti-injection barrier layer prevents the migration of Ag ions into the switching layer, enabling the stable TS operation even under the compliance current of $100~\mu \text{A}$ . Additionally, it locally restricts the region where the filaments are created inside the switching layer, resulting in a 17% lower VT variation and stable IT to approximately $\sim 1.5 \times 10^{-11}$ A in 100 cycles. Due to the low off-state leakage current and low variation characteristic of the optimized AgTi/HfO2-based TS device, the 2D ATS-FET (vs. 2D baseline-FET) shows the reduction of off-state leakage current (by $\sim 10^{2}$ in sub-threshold region) and the stable switching characteristic. The proposed 2D ATS-FET shows stably steep switching characteristics, e.g., sub-threshold swing under forward bias (~19 mV/decade) and reverse bias (~26 mV/decade), because of its abruptly switching characteristics of the TS device.

Understanding filamentary growth and rupture by Ag ion migration through single-crystalline 2D layered CrPS4

Memristive electrochemical metallization (ECM) devices based on cation migration and electrochemical metallization in solid electrolytes are considered promising for neuromorphic computing systems. Two-dimensional (2D) layered materials are emerging as potential candidates for electrolytes in reliable ECM devices due to their two-dimensionally confined material properties. However, electrochemical metallization within a single-crystalline 2D layered material has not yet been verified. Here, we use transmission electron microscopy and energy-dispersive X-ray spectroscopy to investigate the resistive switching mechanism of an ECM device containing a single-crystalline 2D layered CrPS4 electrolyte. We observe the various conductive filament (CF) configurations induced by an applied voltage in an Ag/CrPS4/Au device in the initial/low-resistance/high-resistance/breakdown states. These observations provide concrete experimental evidence that CFs consisting of Ag metal can be formed inside single-crystalline 2D layered CrPS4 and that their configuration can be changed by an applied voltage. Density functional theory calculations confirm that the sulfur vacancies in single-crystalline CrPS4 can facilitate Ag ion migration from the active electrode layer. The electrically induced changes in Ag CFs inside single-crystalline 2D layered CrPS4 raise the possibility of a reliable ECM device that exploits the properties of two-dimensionally confined materials.

An Optimized Ag–5Pd–3.5Au Bonding Wire for the Resistance of Ag Ion Migration in LED Packages

The bondability and reliability of Ag–5Pd–3.5Au alloy wire was verified previously for application in light-emitting diode (LED) packages. This Ag-alloy bonding wire has an electrical resistivity of 4.6 $\mu \Omega \cdot $ cm, lower than those of the ternary Ag–3Pd–20Au (8.6 $\mu \Omega \cdot $ cm) and Ag–3Pd–8Au wires (5.0 $\mu \Omega \cdot $ cm). Further evaluation of the resistance of ion migration in Ag-alloy bonding wires using water drop tests indicated that a declining tendency of ion migration rates existed for various binary Ag–Pd and ternary Ag–Pd–Au alloy wires with increases in Pd and Au contents. Among the all Ag-alloy bonding wires in this study, the Ag–5Pd–3.5Au wire exhibited the lowest ion migration rate of 4.87 $\mu \text{m}$ /s. The measurements of anodic dissolution rates were consistent with the tendency of ion migration rates, which were dependent on Pd and Au contents, resulting in the low value of Ag–5Pd–3.5Au alloy wire (0.017 $\mu \text{m}$ /s).

Oxide-Electrolyte Thickness Dependence Diode-Like Threshold Switching and High on/off Ratio Characteristics by Using Al2O3 Based CBRAM

Diode-like threshold switching and high on/off ratio characteristics by using an Al/Ag/Al2O3/TiN conductive bridge resistive random access memories (CBRAM) have been obtained. The 5 nm-thick Al2O3 device shows superior memory parameters such as low forming voltage and higher switching uniformity as compared to the 20 nm-thick switching layer, owing to higher electric field across the material. Capacitance-voltage (CV) characteristics are observed for the Ag/Al2O3/TiN devices, suggesting the unipolar/bipolar resistive switching phenomena. Negative capacitance (NC) at low frequency proves inductive behavior of the CBRAM devices due to Ag ion migration into the Al2O3 oxide-electrolyte. Thicker Al2O3 film shows diode-like threshold switching behavior with long consecutive 10,000 cycles. It has been found that a thinner Al2O3 device has a larger on/off ratio of &gt;108 as compared to a thicker one. Program/erase (P/E) cycles, read endurance, and data retention of the thinner Al2O3 oxide-electrolyte shows superior phenomena than the thicker electrolyte. The switching mechanism is also explored.

Tailored 2D/3D Halide Perovskite Heterointerface for Substantially Enhanced Endurance in Conducting Bridge Resistive Switching Memory.

Hybrid organic-inorganic halide perovskites (HPs) have garnered significant attention for use in resistive switching (RS) memory devices due to their low cost, low operation voltage, high on/off ratio, and excellent mechanical properties. However, the HP-based RS memory devices continue to face several challenges owing to the short endurance and stability of the HP film. Herein, two-dimensional/three-dimensional (2D/3D) perovskite heterojunction films were prepared via a low-temperature all-solution process and their RS behavior was investigated for the first time. The 2D/3D perovskite RS devices exhibited excellent performance with an endurance of 2700 cycles, a high on/off ratio of 106, and an operation speed of 640 μs. The calculated thermally assisted ion hopping activation energy and the results of the time-of-flight secondary ion mass spectroscopy demonstrated that the 2D perovskite layer could efficiently prevent the Ag ion migration into the 3D perovskite film. Moreover, we found that owing to its high thermal conductivity, the 2D perovskite can control the rupture of the Ag conductive filament. Thus, the 2D perovskite layer enhances endurance by controlling both Ag migration and filament rupture. Hence, this study provides an alternate strategy for improving endurance of HP-based RS memory devices.

Preparation of Nano-Silver-Containing Polyethylene Composite Film and Ag Ion Migration into Food-Simulants.

Nano-composite films were developed between silver nanoparticles (Ag NPs) and a low-density polyethylene (LDPE) using master batches by melt extruding and melt compounding. The Ag/PE composite film showed decreased gas permeability, moisture permeability coefficient, the tear strength, the longitudinal and transverse elongation to that of commercial LDPE. Although stiffness increased at high Ag (40 ppm) concentration, but the longitudinal and transverse tensile strength enhance comparing with commercial PE. Light transmittance and haze were comparable. Both Nano-silver and composite films are effective against Escherichia coli (E. coli). Antibacterial activity of nano-silver for E. coli was determined by diameter of the inhibition zone and the minimum inhibitory concentration of nano-silver is detected by tube double dilution method reaching 15.63 ppm. The composite films are effective inhibition of E. coli at concentrations of 40 ppm Ag nanoparticles. Moreover, Nano-silver migration occurs in composite film. One-side migration was conducted to detect under three food simulants (3% acetic acid, 50% ethanol and distilled water) at three degree of temperature (25 °C, 40 °C and 70 °C) on different period of time (2, 4, 6, 8, 10 and 12 hours). These results indicated that the highest migration amount was obtained with 3% acetic acid following distilled water and finally 50% ethanol under same conditions. The migration level is dependent upon time and temperature and high migration time and temperature can enhance migration level. These findings demonstrate that nano-silver-containing polyethylene composite film may have a great potential for developing antibacterial and acid food packaging system.

Resistive Switching in Nonperovskite-Phase CsPbI3 Film-Based Memory Devices.

Because of their attractive photoelectrical properties, perovskite-phase, CsPbX3 (X = I, Br, or Cl) materials have recently gained attention for their applications in resistive switching (RS) memories. However, phase transition of the CsPbI3 from perovskite (cubic phase) to nonperovskite (orthorhombic phase) at room temperature is problematic; it remains a challenge to apply nonperovskite CsPbI3 in RS memories. In the present work, a polymethylmethacrylate (PMMA)-assisted deposition method for nonperovskite CsPbI3 is introduced to fabricate a composite film of CsPbI3 with PMMA (PMMA@CsPbI3) with a smooth surface morphology on fluorine-doped tin oxide (FTO) substrates. Devices with a Ag/PMMA@CsPbI3/FTO architecture show nonvolatile RS characteristics with an ON/OFF ratio around 102, endurance over 500 cycles, and a retention time of 103 s. Analyses suggested that a Schottky barrier at the Ag/PMMA@CsPbI3 interface and a bias-induced migration of Ag ions within the composite films are responsible for the RS operation. This is the first record for RS devices based on nonperovskite CsPbI3, and it may bring the future research on nonperovskite CsPbI3 applied in RS memory devices some new inspiration..

Self-rectifying resistive switching behavior observed in sodium copper chlorophyllin-polyvinyl alcohol composites on a flexible and transparent substrate

Sodium copper chlorophyllin (SCC)- polyvinyl alcohol (PVA) composites thin films have been prepared on flexible and transparent ITO/PET substrates using Ag as the top electrode. FE-SEM shows that the prepared SCC-PVA thin films are smooth and dense, SCC particles have embedded in PVA and formed nano-islands, which are distributed irregularly in the thin film. The optical transmittance spectrum demonstrates that Ag/SCC-PVA/ITO/PET can be used as a transparent electronic device. I–V characteristics of the Ag/SCC-PVA/ITO/PET show that the device exhibits self-rectifying resistive switching performance, which could be related to the forming/rapture of Ag conductive filaments induced by the migration of Ag ions. This study demonstrates the potential uses of SCC-PVA in low-cost, flexible and transparent resistive switching memory.