Nonlinear effects in two-dimensional (2D) atomic layered materials have recently attracted increasing interest. Phenomena such as nonlinear optical edge response, chiral electroluminescence, and valley and spin currents beyond linear orders have opened up a great opportunity to expand the functionalities and potential applications of 2D materials. Here we report the first observation of strong optical second-harmonic generation (SHG) in monolayer GaSe under nonresonant excitation and emission condition. Our experiments show that the nonresonant SHG intensity of GaSe is the strongest among all the 2D atomic crystals measured up to day. At the excitation wavelength of 1600 nm, the SHG signal from monolayer GaSe is around 1-2 orders of magnitude larger than that from monolayer MoS2 under the same excitation power. Such a strong nonlinear signal facilitates the use of polarization-dependent SHG intensity and SHG mapping to investigate the symmetry properties of this material: the monolayer GaSe shows 3-fold lattice symmetry with an intrinsic correspondence to its geometric triangular shape in our growth condition; whereas the bilayer GaSe exhibits two dominant stacking orders: AA and AB stacking. The correlation between the stacking orders and the interlayer twist angles in GaSe bilayer indicates that different triangular GaSe atomic layers have the same dominant edge configuration. Our results provide a route toward exploring the structural information and the possibility to observe other nonlinear effects in GaSe atomic layers.

2D Molybdenum disulfide (MoS2 ) is a promising candidate material for high-speed and flexible optoelectronic devices, but only with low photoresponsivity. Here, a large enhancement of photocurrent response is obtained by coupling few-layer MoS2 with Au plasmonic nanostructure arrays. Au nanoparticles or nanoplates placed onto few-layer MoS2 surface can enhance the local optical field in the MoS2 layer, due to the localized surface plasmon (LSP) resonance. After depositing 4 nm thick Au nanoparticles sparsely onto few-layer MoS2 phototransistors, a doubled increase in the photocurrent response is observed. The photocurrent of few-layer MoS2 phototransistors exhibits a threefold enhancement with periodic Au nanoarrays. The simulated optical field distribution confirms that light can be trapped and enhanced near the Au nanoplates. These findings offer an avenue for practical applications of high performance MoS2 -based optoelectronic devices or systems in the future.

Grain boundaries in as-grown polycrystalline MoS2 monolayers are revealed by second-harmonic-generation microscopy. Through the anisotropic polarization pattern and phase interference at the grain boundary, grain edge termination and boundary types are identified. Statistical analysis on hundreds of grains shows that grain-boundary formation is driven by kinetics and can be nicely described by the edge attachment growth model.