Noise Tailoring in Memristive Filaments.

In this study, the possibilities of noise tailoring in filamentary resistive switching memory devices are investigated. To this end, the resistance and frequency scaling of the low-frequency 1/f-type noise properties are studied in representative mainstream material systems. It is shown that the overall noise floor is tailorable by the proper material choice, as demonstrated by the order-of-magnitude smaller noise levels in Ta2O5 and Nb2O5 transition-metal oxide memristors compared to Ag-based devices. Furthermore, the variation of the resistance states allows orders-of-magnitude tuning of the relative noise level in all of these material systems. This behavior is analyzed in the framework of a point-contact noise model highlighting the possibility for the disorder-induced suppression of the noise contribution arising from remote fluctuators. These findings promote the design of multipurpose resistive switching units, which can simultaneously serve as analog-tunable memory elements and tunable noise sources in probabilistic computing machines.

A Rational Fabrication Method for Low Switching-Temperature VO2.

Due to its remarkable switching effect in electrical and optical properties, VO2 is a promising material for several applications. However, the stoichiometry control of multivalent vanadium oxides, especially with a rational deposition technique, is still challenging. Here, we propose and optimize a simple fabrication method for VO2 rich layers by the oxidation of metallic vanadium in atmospheric air. It was shown that a sufficiently broad annealing time window of 3.0-3.5 h can be obtained at an optimal oxidation temperature of 400 °C. The presence of VO2 was detected by selected area diffraction in a transmission electron microscope. According to the temperature dependent electrical measurements, the resistance contrast (R30 °C/R100 °C) varied between 44 and 68, whereas the optical switching was confirmed using in situ spectroscopic ellipsometric measurement by monitoring the complex refractive indices. The obtained phase transition temperature, both for the electrical resistance and for the ellipsometric angles, was found to be 49 ± 7 °C, i.e., significantly lower than that of the bulk VO2 of 68 ± 6 °C.

A non-oxidizing fabrication method for lithographic break junctions of sensitive metals.

Electrochemically active metals offer advanced functionalities with respect to the well-established gold electrode arrangements in various electronic transport experiments on atomic scale objects. Such functionalities can arise from stronger interactions with the leads which provide better coupling to specific molecules and may also facilitate metallic filament formation in atomic switches. However, the higher reactivity of the electrode metal also imposes challenges in the fabrication and reliability of nanometer scale platforms, limiting the number of reported applications. Here we present a high-yield lithographic fabrication procedure suitable to extend the experimental toolkit with mechanically controllable break junctions of oxygen sensitive metallic electrodes. We fabricate and characterize silver break junctions exhibiting single-atomic conductance and superior mechanical and electrical stability at room temperature. As a proof-of-principle application, we demonstrate resistive switching between metastable few-atom configurations at finite voltage bias.

Universal 1/f type current noise of Ag filaments in redox-based memristive nanojunctions.

The microscopic origins and technological impact of 1/f type current fluctuations in Ag based, filamentary type resistive switching devices have been investigated upon downscaling toward the ultimate single atomic limit. The analysis of the low-frequency current noise spectra revealed that the main electronic noise contribution arises from the resistance fluctuations due to internal dynamical defects of Ag nanofilaments. The resulting 0.01-1% current noise ratio, i.e. the total noise level with respect to the mean value of the current, is found to be universal: its magnitude only depends on the total resistance of the device, irrespective of the materials aspects of the surrounding solid electrolyte and of the specific filament formation procedure. Moreover, the resistance dependence of the current noise ratio also displays the diffusive to ballistic crossover, confirming that stable resistive switching operation utilizing Ag nanofilaments is not compromised even in truly atomic scale junctions by technologically impeding noise levels.

From electroburning to sublimation: substrate and environmental effects in the electrical breakdown process of monolayer graphene.

We report on the characterization of the electrical breakdown (EB) process for the formation of tunneling nanogaps in single-layer graphene. In particular, we investigated the role of oxygen in the breakdown process by varying the environmental conditions (vacuum and ambient conditions). We show that the density of oxygen molecules in the chamber is a crucial parameter that defines the physical breakdown process: at low density, the graphene lattice is sublimating, whereas at high density, the process involved is oxidation, independent of the substrate material. To estimate the activation energies of the two processes, we use a scheme which consists of applying voltage pulses across the junction during the breakdown. By systematically varying the voltage pulse length, and estimating the junction temperature from a 1D thermal model, we extract activation energies which are consistent with the sublimation of graphene under high vacuum and the electroburning process under air. Our study demonstrates that, in our system, a better control of the gap formation is achieved in the sublimation regime.

Multiple Physical Time Scales and Dead Time Rule in Few-Nanometers Sized Graphene-SiOx-Graphene Memristors.

The resistive switching behavior in SiOx-based phase change memory devices confined by few nanometer wide graphene nanogaps is investigated. Our experiments and analysis reveal that the switching dynamics is not only determined by the commonly observed bias voltage dependent set and reset times. We demonstrate that an internal time scale, the dead time, plays a fundamental role in the system's response to various driving signals. We associate the switching behavior with the formation of microscopically distinct SiOx amorphous and crystalline phases between the graphene electrodes. The reset transition is attributed to an amorphization process due to a voltage driven self-heating; it can be triggered at any time by appropriate voltage levels. In contrast, the formation of the crystalline ON state is conditional and only occurs after the completion of a thermally assisted structural rearrangement of the as-quenched OFF state which takes place within the dead time after a reset operation. Our results demonstrate the technological relevance of the dead time rule which enables a zero bias access of both the low and high resistance states of a phase change memory device by unipolar voltage pulses.

Asymmetry-induced resistive switching in Ag-Ag2S-Ag memristors enabling a simplified atomic-scale memory design.

Prevailing models of resistive switching arising from electrochemical formation of conducting filaments across solid state ionic conductors commonly attribute the observed polarity of the voltage-biased switching to the sequence of the active and inert electrodes confining the resistive switching memory cell. Here we demonstrate stable switching behaviour in metallic Ag-Ag2S-Ag nanojunctions at room temperature exhibiting similar characteristics. Our experimental results and numerical simulations reveal that the polarity of the switchings is solely determined by the geometrical asymmetry of the electrode surfaces. By the lithographical design of a proof of principle device we demonstrate the merits of simplified fabrication of atomic-scale, robust planar Ag2S memory cells.

Precursor configurations and post-rupture evolution of Ag-CO-Ag single-molecule junctions.

Experimental correlation analysis and first-principles theory are used to probe the structure and evolution of Ag-CO-Ag single-molecule junctions both before the formation and after the rupture of the junctions. Two dimensional correlation histograms and conditional histograms demonstrate that prior to the single-molecule bridge configuration the CO molecule is already bound parallel to the Ag single-atom contact. This molecular precursor configuration is accompanied by the opening of additional conductance channels compared to the single-channel transport in pure Ag monoatomic junctions. To investigate the post-rupture evolution of the junction we introduce a cross-correlation analysis between the opening and the subsequent closing conductance traces. This analysis implies that the molecule is bound rigidly to the apex of one electrode, and so the same single-molecule configuration is re-established as the junction is closed. The experimental results are confirmed by ab initio simulations of the evolution of contact geometries, transmission eigenvalues and scattering wavefunctions.

High-yield fabrication of nm-size gaps in monolayer CVD graphene.

Herein we demonstrate the controlled and reproducible fabrication of sub-5 nm wide gaps in single-layer graphene electrodes. The process is implemented for graphene grown via chemical vapor deposition using an electroburning process at room temperature and in vacuum. A yield of over 95% for the gap formation is obtained. This approach allows producing single-layer graphene electrodes for molecular electronics at a large scale. Additionally, from Raman spectroscopy and electroburning carried out simultaneously, we can follow the heating process and infer the temperature at which the gap formation happens.