Synapse 3 Compatible Devices
Teena Ruiter
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Physical neural networks made of analog resistive switching processors are promising platforms for analog computing. State-of-the-art resistive switches rely on either conductive filament formation or phase change. These processes suffer from poor reproducibility or high energy consumption, respectively. Herein, we demonstrate the behavior of an alternative synapse design that relies on a deterministic charge-controlled mechanism, modulated electrochemically in solid-state. The device operates by shuffling the smallest cation, the proton, in a three-terminal configuration. It has a channel of active material, WO3. A solid proton reservoir layer, PdHx, also serves as the gate terminal. A proton conducting solid electrolyte separates the channel and the reservoir. By protonation/deprotonation, we modulate the electronic conductivity of the channel over seven orders of magnitude, obtaining a continuum of resistance states. Proton intercalation increases the electronic conductivity of WO3 by increasing both the carrier density and mobility. This switching mechanism offers low energy dissipation, good reversibility, and high symmetry in programming.
There are two main types of resistive switching mechanisms discussed and used in literature to change the conductance, both of them relying on two-terminal configurations20. The conductive-filament (CF) mechanism is based on the formation of a narrowly confined conducting path (made of metal atoms or oxygen vacancies) inside an insulating matrix, typically an insulating oxide21,22,23,24. The phase-change mechanism (PCM) is realized by changing the material between its conducting and insulating phases, such as the Ge-Sb-Te chalcogenides, controlled by Joule heating25,26. Both resistive switching mechanisms have been demonstrated in artificial intelligence applications, but the CF mechanism suffers from lack of reproducibility, while the PCM suffers from high energy dissipation and drift10,27,28. As a result, the performance of such two-terminal devices in a memory matrix environment is still far from the desired specifications for reliable, fast and energy-efficient training of neural networks29. A fundamentally new working mechanism is desirable for enabling new opportunities to address these challenges.
In this work, we demonstrate proton intercalation in inorganic materials as a basis for emulating synapse behavior with low energy cost, long retention, and good symmetry. This system offers a deterministic, charged-controlled mechanism that uniformly switches the channel conductance. Thus, it should not pose issues related to lack of reproducibility that heavily depends on the microstructural and chemical heterogeneities in the high-k dielectric materials used in two-terminal CF devices. In addition, if the intercalating ion and the chosen materials are suitable, the energy consumption of the switching process can be very small, as demonstrated in this work. We quantify the protonation-conductance relationship of this artificial electrochemical synapse, providing insights into the proper selection of operating window for the chosen material, WO3. We adopt the constant current gating, and propose that it is more suitable than the constant voltage gating for such three-terminal electrochemical resistive switches because it offers better controllability, reproducibility, and symmetry. X-ray absorption and photoelectron spectroscopy, together with first-principles calculations, reveal that the electronic carrier density and mobility contribute to the conductivity change as a function of protonation in WO3.
The proton as a small cation could reside in the interconnected channels of the WO3 lattice and bond with the oxygen ion to form OHO defect in these channel sites (Fig. 1c). There is a main difference here with respect to the conductive filament (CF) or phase change mechanism (PCM) approach. That is, the intercalation of the protons involves a high degree of spatial homogeneity within the channel material. This means that the active material (HxWO3) can stay single-phase during the intercalation due to the high equilibrium solubility limit of H in the solid solution phase.
As discussed above, and unlike the previous protonation of oxides which rely on the electrolysis of water to generate the protons47, our device is a closed system with proton shuffling between the solid-state gate and the channel material. This not only reduces the energy consumption by avoiding the water hydrolysis reaction, but also improves the controllability. In a practical device, this electrochemical synapse should be encapsulated by insulating layers that are also proton barriers in order to prevent the long-term loss of protons or ingress of oxygen into the system, essential for device endurance. (See Supplementary Figs. 6 and 14 for demonstration of the encapsulated device).
Two features of this protonic electrochemical synapse discussed here enable this low operating energy. First, the cation employed here to modulate the conductivity is the smallest and lightest cation, the proton, needing low energy to migrate and transfer at interfaces. Second, the electrochemical potentials of the gate and channel materials are close, resulting in a small open-circuit potential, as shown in Fig. 2a. This means that the device is operated only within a small voltage window. The first feature minimizes the kinetic contribution to the energy consumption, while the second one minimizes the thermodynamic contribution. In addition, the small but non-zero open-circuit potential change after gating indicates that a selector component may be needed to program individual synapses in an array, as demonstrated in ref. 19, and to avoid cross-talk of individual synapses when not gating.
From the analysis of the valence band and the W 4f photoelectron peak, we can conclude that, upon intercalation of protons, new in-gap states form, gradually lowering the effective bandgap of WO3 to 0. This process is accompanied by the injection of electrons, which pushes the Fermi level toward the conduction band. When the quantity of injected electrons is significant enough, the Fermi level completely shifts into the conduction band. Consistent with electron injection and n-type doping, the oxidation state of W is reduced. As a result, we expect a continuous increase of electronic conductivity with increasing protonation level in HxWO3, as shown in Fig. 2a.
As a result of this in situ XRD analysis, we can conclude that, with the insertion of protons into the channel sites, the WO6 octahedra become more ordered and the crystal structure becomes more symmetrical, as seen from the monoclinic to tetragonal transition in Fig. 4d. The increased symmetry can arise from increased concentration of electronic charge in WO3, namely W5+/W6+ polarons. We have also found that the interaxial angles approach 90 upon proton insertion in WO3 (see Supplementary Fig. 11 in Supplementary Information.) The increased symmetry of the structure can also contribute to a change of the band structure60 and eventually the conductive behavior39,57.
Gating through the application of a voltage is widely adopted in the literature to induce resistive switching (also demonstrated in Supplementary Fig. 12 on our device)61. Typical reported gating voltage values range from several volts to tens of volts. Very often, the gating voltage is used as a descriptor to indicate the final state of the sample49,62. Here we emphasize that, in such an electrochemical synapse (or ionic gating) devices, there can be a significant difference between the gating voltage applied and the change in the open-circuit potential of the device due to polarization. That is, the equilibrium chemical potential of the active material does not necessarily follow the applied gating voltage precisely63. Such difference could be a major reason for the lack of consistency of the gating voltages reported in the literature17,40,49,64.
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