Phase control plays an important role in the precise synthesis of inorganic materials, as the phase structure has a profound influence on properties such as conductivity and chemical stability. Phase-controlled preparation has been challenging for the metallic-phase group-VI transition metal dichalcogenides (the transition metals are Mo and W, and the chalcogens are S, Se and Te), which show better performance in electrocatalysis than their semiconducting counterparts. Here, we report the large-scale preparation of micrometre-sized metallic-phase 1T'-MoX (X = S, Se)-layered bulk crystals in high purity. We reveal that 1T'-MoS crystals feature a distorted octahedral coordination structure and are convertible to 2H-MoS following thermal annealing or laser irradiation. Electrochemical measurements show that the basal plane of 1T'-MoS is much more active than that of 2H-MoS for the electrocatalytic hydrogen evolution reaction in an acidic medium.

Interfacial coupling between neighboring layers of van der Waals heterostructures (vdWHs), formed by vertically stacking more than two types of two-dimensional materials (2DMs), greatly affects their physical properties and device performance. Although high-resolution cross-sectional scanning tunneling electron microscopy can directly image the atomically sharp interfaces in the vdWHs, the interfacial coupling and lattice dynamics of vdWHs formed by two different types of 2DMs, such as semimetal and semiconductor, are not clear so far. Here, we report the ultralow-frequency Raman spectroscopy investigation on interfacial couplings in the vdWHs formed by graphene and MoS flakes. Because of the significant interfacial layer-breathing couplings between MoS and graphene flakes, a series of layer-breathing modes with frequencies dependent on their layer numbers are observed in the vdWHs, which can be described by the linear chain model. It is found that the interfacial layer-breathing force constant between MoS and graphene, α(I) = 60 × 10 N/m, is comparable with the layer-breathing force constant of multilayer MoS and graphene. The results suggest that the interfacial layer-breathing couplings in the vdWHs formed by MoS and graphene flakes are not sensitive to their stacking order and twist angle between the two constituents. Our results demonstrate that the interfacial interlayer coupling in vdWHs formed by two-dimensional semimetals and semiconductors can lead to new lattice vibration modes, which not only can be used to measure the interfacial interactions in vdWHs but also is beneficial to fundamentally understand the properties of vdWHs for further engineering the vdWHs-based electronic and photonic devices.

Transparent and flexible devices based on two-dimensional (2D) materials hold great potential for many electronic/optoelectronic applications. The direct and fast thickness identification of 2D materials on transparent substrates is therefore an essential step in such applications, but remains challenging. Here, we present a simple, rapid and reliable optical method to identify the thickness of 2D nanosheets on transparent substrates, such as polydimethylsiloxane, glass, and coverslip. Under reflection and transmission light, 1-20L MoS and 1-14L WSe nanosheets can be reliably identified by measuring the optical contrast difference between the 2D nanosheets and substrates in color, red, green or blue channels. Meanwhile, the values of all the measured contrast differences as a function of layer number can be well fitted with the Boltzmann function, indicating the generalizability and reliability of our optical method. Our method will not only facilitate the fundamental study of the thickness-dependent properties of 2D nanosheets, but will also expand their potential applications in the field of flexible/transparent electronics and optoelectronics.

rGO–Ag scroll meshes shows 3 orders of magnitude higher humidity response compared to that of rGO scroll meshes.