Electrochemical metallization (ECM) threshold switches are in great demand for various applications such as next-generation logic technology, future memory, and neuromorphic computing. However, the instability of operation due to inherent filamentary randomness is a severe problem that is yet to be solved. Here, we propose a specially treated hafnium oxide (HfO x :N)-based ECM threshold switch with high reliability, low-voltage operation (0.2 V), high ON/ OFF ratio (5 × 10 8 ), great endurance (10 6 ), and fast switching speed (1.5 μs at 2 V). The nitrogen ions in the HfO x :N layer assist confining the path of the metallic filament, which significantly suppresses filament randomness as well as reduces power consumption and alternating current response time. The feasibility of ECM threshold switches to logic applications, AND and OR, is first introduced. The ECM threshold switch has great potential to be utilized in complementary logic circuits because of its ultralow operation power consumption, high integrability using an array structure (4F 2 ), and fast switching characteristics. Furthermore, we have successfully verified its applicability to flexible electronics on polyethylene naphthalate films that can retain stable operation under considerable mechanical stress. We believe that this research paves the way to fabricate highly reliable ECM threshold switches for flexible complementary logic circuits with ultralow power consumption.

A metal-interlayer-semiconductor (M-I-S) structure with excellent thermal stability and electrical performance for a nonalloyed contact scheme is developed, and considerations for designing thermally stable M-I-S structure are demonstrated on the basis of n-type germanium (Ge). A thermal annealing process makes M-I-S structures lose their Fermi-level unpinning and electron Schottky barrier height reduction effect in two mechanisms: (1) oxygen (O) diffusion from the interlayer to the contact metal due to high reactivity of a pure metal contact with O and (2) interdiffusion between the contact metal and semiconductor through grain boundaries of the interlayer. A pure metal contact such as titanium (Ti) provides very poor thermal stability due to its high reactivity with O. A structure with a tantalum nitride (TaN) metal contact and a titanium dioxide (TiO) interlayer exhibits moderate thermal stability up to 400 °C because TaN has much lower reactivity with O than with Ti. However, the TiO interlayer cannot prevent the interdiffusion process because it is easily crystallized during thermal annealing and its grain boundaries act as diffusion path. A zinc oxide (ZnO) interlayer doped with group-III elements, such as an aluminum-doped ZnO (AZO) interlayer, acts as a good diffusion barrier due to its high crystallization temperature. A TaN/AZO/n-Ge structure provides excellent thermal stability above 500 °C as it can prevent both O diffusion and interdiffusion processes; hence, it exhibits Ohmic contact properties for all thermal annealing temperatures. This work shows that, to fabricate a thermally stable and low resistive M-I-S contact structure, the metal contact should have low reactivity with O and a low work-function, and the interlayer should have a high crystallization temperature and a low conduction band offset to Ge. Furthermore, new insights are provided for designing thermally stable M-I-S contact schemes for any semiconductor material that suffers from the Fermi-level pinning problem.

Energy barrier formed at a metal/semiconductor interface is a critical factor determining the performance of nanoelectronic devices. Although diverse methods for reducing the Schottky barrier height (SBH) via interface engineering have been developed, it is still difficult to achieve both an ultralow SBH and a low dependence on the contact metals. In this study, a novel structure, namely, a metal/transition-metal dichalcogenide (TMD) interlayer (IL)/dielectric IL/semiconductor (MTDS) structure, was developed to overcome these issues. Molybdenum disulfide (MoS2) is a promising TMD IL material owing to its interface characteristics, which yields a low SBH and reduces the reliance on contact metals. Moreover, an ultralow SBH is achieved via the insertion of an ultrathin ZnO layer between MoS2 and a semiconductor, thereby inducing an n-type doping effect on the MoS2 IL and forming an interface dipole in the favorable direction at the ZnO IL/semiconductor interfaces. Consequently, the lowest SBH (0.07 eV) and a remarkable improvement in the reverse current density (by a factor of approximately 5400) are achieved, with a wide room for contact-metal dependence. This study experimentally and theoretically validates the effect of the proposed MTDS structure, which can be a key technique for next-generation nanoelectronics.