The first black-phosphorus synaptic device is demonstrated, which offers intrinsic anisotropy in its synaptic characteristics directly resulting from its low crystalline symmetry. Key features of biological synapses, such as long-term plasticity with heterogeneity, including long-term potentiation/depression and spike-timing-dependent plasticity, are mimicked. This demonstration represents an important step toward introducing intrinsic heterogeneity to artificial neuromorphic systems.

Recently rediscovered black phosphorus is a layered semiconductor with promising electronic and photonic properties. Dynamic control of its bandgap can allow for the exploration of new physical phenomena. However, theoretical investigations and photoemission spectroscopy experiments indicate that in its few-layer form, an exceedingly large electric field in the order of several volts per nanometre is required to effectively tune its bandgap, making the direct electrical control unfeasible. Here we reveal the unique thickness-dependent bandgap tuning properties in intrinsic black phosphorus, arising from the strong interlayer electronic-state coupling. Furthermore, leveraging a 10 nm-thick black phosphorus, we continuously tune its bandgap from ∼300 to below 50 meV, using a moderate displacement field up to 1.1 V nm−1. Such dynamic tuning of bandgap may not only extend the operational wavelength range of tunable black phosphorus photonic devices, but also pave the way for the investigation of electrically tunable topological insulators and semimetals.

Seeking earth-abundant electrocatalysts with high efficiency and durability has become the frontier of energy conversion research. Mixed-transition-metal (MTM)-based electrocatalysts, owing to the desirable electrical conductivity, synergistic effect of bimetal atoms, and structural stability, have recently emerged as new-generation hydrogen evolution reaction (HER) electrocatalysts. However, the correlation between anion species and their intrinsic electrocatalytic properties in MTM-based electrocatalysts is still not well understood. Here we present a novel approach to tuning the anion-dependent electrocatalytic characteristics in MTM-based catalyst for HER, using holey Ni/Co-based phosphides/selenides/oxides (Ni-Co-A, A = P, Se, O) as the model materials. The electrochemical results, combined with the electrical conductivity measurement and DFT calculation, reveal that P substitution could modulate the electron configuration, lower the hydrogen adsorption energy, and facilitate the desorption of hydrogen on the active sites in Ni-Co-A holey nanostructures, resulting in superior HER catalytic activity. Accordingly we fabricate the NCP holey nanosheet electrocatalyst for HER with an ultralow onset overpotential of nearly zero, an overpotential of 58 mV, and long-term durability, along with an applied potential of 1.56 V to boost overall water splitting at 10 mA cm, among the best electrocatalysts reported for non-noble-metal catalysts to date. This work not only presents a deeper understanding of the intrinsic HER electrocatalytic properties for MTM-based electrocatalyst with various anion species but also offers new insights to better design efficient and durable water-splitting electrocatalysts.

Transition metal dichalcogenides (TMDCs) are a promising class of two-dimensional (2D) materials for use in applications such as 2D electronics, optoelectronics, and catalysis. Due to the van der Waals (vdW) bonding between layers, vdW heterostructures can be constructed between two different species of TMDCs. Most studies employ exfoliation or co-vapor growth schemes, which are limited by the small size and uneven distribution of heterostructures on the growth substrate. In this work we demonstrate a one-step synthesis procedure for large-area vdW heterostructures between horizontal TMDCs MoS2 and WS2. The synthesis procedure is scalable and provides patterning ability, which is critical for electronic applications in integrated circuits. We demonstrate rectification characteristics of large-area MoS2/WS2 stacks. In addition, hydrogen evolution reaction performance was measured in these horizontal MoS2 and WS2 thin films, which indicate that, in addition to the catalytically active sulfur edge sites, defect sites may serve as catalyst sites.

Abstract