Unlike the metal-oxide-semiconductor field-effect transistors (MOSFET), whose working mechanism relies on a large number of electrons and holes, memristor, in contrast, realizes its resistive switching and information storage only via a limited number of ions within the switching medium
33. Fabrication inhomogeneity (e.g. the poly-grain nature of the graphene electrodes, the polymer-assisted transfer/lithography processes, and the subsequently nonuniformity deposition), and the initial formation of conduction filaments as well as its intrinsic stochastic switching mechanism, lead to the memristive device-to-device variability (DDV). Note that the device structure in the current study can be seen in the
Fig. 1a and the fabrication details can be found in the Experiments section and Fig. S2 in the Supplementary Materials. A typical resistive switching curve of graphene-based CBRAM have been shown in
Fig. 1b. For the Set process, the active electrode (silver in this study) gets oxidized into Ag
+ and dissolved into the electrolyte, which is then reduced at the inert electrode surface and piled up as a metallic filament to bridge the active electrode during the Set bias voltage, during which the device is switched to the low resistance state (LRS). When an opposite polarity Reset voltage is applied, the conductive filament starts to be ruptured and the device is switched back to the high resistance state (HRS), which is the Reset process. Considering the differences of fabrications, initial filament formation and variation of repeated cycles and current fluctuation over time, the filament revolution (from Ag to Ag+ and from Ag+ to Ag) can be in highly stochastic, as shows in
Fig. 1c. Since the silver cations transport more easily in a defect-rich region with lowest electrochemical potentials, the variability of the CF shape will be formed due to the inhomogeneous nature of the AlO
x34. Briefly, the AlO
x amorphous electrolyte plays at least 3 roles for the variability during forming process and subsequent multiple cycles
35⇓-37: 1. noise source for current fluctuation: the electrolyte may include redox reactions of the Ag atoms or ions at the filament surface, or resulting atomic reversible rearrangements at the metastable positions or the defects sites, which may cause current fluctuation over time; 2. solubility: the CF and sub-filaments (if existed) will be dissolved at various degrees during the gradual Reset operation, which determined the HRS in the following cycle; 3. thermal conductivity: during repeated bias sweeping back and forth, a large amount of Joule heat is generated and accumulated within the electrolyte; Ag nanoparticles will merge into larger clusters to minimize the interfacial energy. As a result, not only the shape of the CF, but also the device performance will be influenced, because both the drift and diffusion current of the Set and Reset processes are thermally accelerated; in other words, whether the heat can be promptly dissipated with the electrolyte is also a stochastic factor to the device switching characterizations. Moreover, considering the weak thermal conductivity of the van der Waals interface of graphene electrode, the memristive variation will be further complicated. To analysis the CCV statistically, conventionally, a large number of IV curves could be analysis via Weibull distribution, time series analysis (TSA) or multivariate strategy to forecast the Set and Reset jointly
38. However, they neglect the physical correlation between the cycles. To consider the correlation between cycles, an iterative recurrent neural network based Long Short-Term Memory (LSTM) has been utilized to analyse the CCV of oxide-based memristor successfully. In this work, we extracted the physical parameters from memristive measurements and utilized principal component analysis (PCA) to analyse the DDV and LSTM to analyse the CCV. Moreover, the TTV is also analysed based on physical models, where the TTV under different voltage biases are shown in
Fig. 1d1-d3. The device array and the device architecture have been shown in
Fig. 1e-g via scanning electron microscope (SEM) observation. To inspect the device vertical structure and the thickness of the electrolyte layer, the transmission electron microscopy (TEM) image is shown in
Fig. 1f. Moreover, elemental distribution of the TEM image with energy dispersive X-ray spectroscopy (EDX) including Ag, Al, C, O and Si has been exhibited in Fig. S3a-g in Supplementary Materials. Raman spectrum detecting has been also carried out to verify the high crystallinity and low defect density of the graphene electrode, as shown in Fig. S3h in Supplementary Materials.