Atom-thin transition metal dichalcogenides (TMDs) have emerged as fascinating materials and key structures for electrocatalysis. So far, their edges, dopant heteroatoms and defects have been intensively explored as active sites for the hydrogen evolution reaction (HER) to split water. However, grain boundaries (GBs), a key type of defects in TMDs, have been overlooked due to their low density and large structural variations. Here, we demonstrate the synthesis of wafer-size atom-thin TMD films with an ultra-high-density of GBs, up to ~10¹² cm⁻². We propose a climb and drive 0D/2D interaction to explain the underlying growth mechanism. The electrocatalytic activity of the nanograin film is comprehensively examined by micro-electrochemical measurements, showing an excellent hydrogen-evolution performance (onset potential: −25 mV and Tafel slope: 54 mV dec⁻¹), thus indicating an intrinsically high activation of the TMD GBs.

In 2D van der Waals heterostructures, interactions between atomic layers dramatically change the vibrational properties of the hybrid system and demonstrate several interesting phenomena that are absent in individual materials. In this paper, we have investigated the vibrational properties of the heterostructure between transition metal dichalcogenide (TMD) and hexagonal boron nitride (hBN) on gold film at low- and high-frequency ranges by Raman spectroscopy. Nineteen Raman modes have been observed from the sample, including a new interlayer coupling mode at 28.8 cm⁻¹. Compared to reported experimental results of tungsten disulfide (WS₂) on SiO₂/Si substrates, the Raman spectrum for WS₂ on hBN/Au emerges a blue shift of about 8 cm⁻¹. Furthermore, a remarkable enhancement of Raman intensity can be obtained when tuning hBN thickness in the heterostructure. Through systematic first-principles calculations, numerical simulations, and analytical calculations, we find that the 28.8 cm⁻¹ mode originates from the shearing motion between monolayer TMD and hBN layers. In addition, the gold substrate and hBN layers form an optical cavity and the cavity interference effects enhance the obtained Raman intensity. This paper demonstrates the novel vibrational modes of 2D van der Waals heterostructure as an effective tool to characterize a variety of such heterostructures and reveals a new method to enhance the Raman response of 2D materials.

Nonlinear optical processing of ambient natural light is highly desired for computational imaging and sensing. Strong optical nonlinear response under weak broadband incoherent light is essential for this purpose. By merging 2D transparent phototransistors (TPTs) with liquid crystal (LC) modulators, we create an optoelectronic neuron array that allows self-amplitude modulation of spatially incoherent light, achieving a large nonlinear contrast over a broad spectrum at orders-of-magnitude lower intensity than achievable in most optical nonlinear materials. We fabricated a 10,000-pixel array of optoelectronic neurons, and experimentally demonstrated an intelligent imaging system that instantly attenuates intense glares while retaining the weaker-intensity objects captured by a cellphone camera. This intelligent glare-reduction is important for various imaging applications, including autonomous driving, machine vision, and security cameras. The rapid nonlinear processing of incoherent broadband light might also find applications in optical computing, where nonlinear activation functions for ambient light conditions are highly sought.