The ability to tune material properties using gating by electric fields is at the heart of modern electronic technology. It is also a driving force behind recent advances in two-dimensional systems, such as the observation of gate electric-field-induced superconductivity and metal-insulator transitions. Here, we describe an ionic field-effect transistor (termed an iFET), in which gate-controlled Li ion intercalation modulates the material properties of layered crystals of 1T-TaS2. The strong charge doping induced by the tunable ion intercalation alters the energetics of various charge-ordered states in 1T-TaS2 and produces a series of phase transitions in thin-flake samples with reduced dimensionality. We find that the charge-density wave states in 1T-TaS2 collapse in the two-dimensional limit at critical thicknesses. Meanwhile, at low temperatures, the ionic gating induces multiple phase transitions from Mott-insulator to metal in 1T-TaS2 thin flakes, with five orders of magnitude modulation in resistance, and superconductivity emerges in a textured charge-density wave state induced by ionic gating. Our method of gate-controlled intercalation opens up possibilities in searching for novel states of matter in the extreme charge-carrier-concentration limit.

Electron–electron and electron–phonon interactions are two major driving forces that stabilize various charge-ordered phases of matter. In layered compound 1T-TaS2, the intricate interplay between the two generates a Mott-insulating ground state with a peculiar charge-density-wave (CDW) order. The delicate balance also makes it possible to use external perturbations to create and manipulate novel phases in this material. Here, we study a mosaic CDW phase induced by voltage pulses, and find that the new phase exhibits electronic structures entirely different from that of the original Mott ground state. The mosaic phase consists of nanometre-sized domains characterized by well-defined phase shifts of the CDW order parameter in the topmost layer, and by altered stacking relative to the layers underneath. We discover that the nature of the new phase is dictated by the stacking order, and our results shed fresh light on the origin of the Mott phase in 1T-TaS2.

Although polymers have been studied for well over a century, there are few examples of covalently linked polymer crystals synthesised directly from solution. One-dimensional (1D) covalent polymers that are packed into a framework structure can be viewed as a 1D covalent organic framework (COF), but making a single crystal of this has been elusive. Herein, by combining labile metal coordination and dynamic covalent chemistry, we discover a strategy to synthesise single-crystal metallo-COFs under solvothermal conditions. The single-crystal structure is rigorously solved using single-crystal electron diffraction technique. The noncentrosymmetric metallo-COF allows second harmonic generation. Due to the presence of syntactic pendant amine groups along the polymer chains, the metallopolymer crystal can be further cross-linked into a crystalline woven network.

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 10 8 . 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.

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