Monolayer transition metal dichalcogenides have intrinsic spin-valley degrees of freedom, making it appealing to exploit valleytronic and optoelectronic applications at the nanoscale. Here, we demonstrate that a chiral plasmonic antenna consisting of two stacked gold nanorods can modulate strongly valley-polarized photoluminescence (PL) of monolayer MoS2 in a broad spectral range at room temperature. The valley-polarized PL of the MoS2 using the antenna can reach up to ~47%, with approximately three orders of PL magnitude enhancement within the plasmonic nanogap. Besides, the K and K′ valleys under opposite circularly polarized light excitation exhibit different emission intensities and directivities in the far field, which can be attributed to the modulation of the valley-dependent excitons by the chiral antenna in both the excitation and emission processes. The distinct features of the ultracompact hybrid suggest potential applications for valleytronic and photonic devices, chiral quantum optics, and high-sensitivity detection.

A comprehensive understanding of the ultrafast electron dynamics in two-dimensional transition metal dichalcogenides (TMDs) is necessary for their applications in optoelectronic devices. In this work, we contribute a study of ultrafast electron cooling and decay dynamics in the supported and suspended monolayer WS2 by time- and energy-resolved photoemission electron microscopy (PEEM). Electron cooling in the Q valley of the conduction band is clearly resolved in energy and time, on a time scale of 0.3 ps. Electron decay is mainly via a defect trapping process on a time scale of several picoseconds. We observed that the trap states can be produced and increased by laser illumination under an ultrahigh vacuum, and the higher local optical-field intensity led to the faster increase of trap states. The enhanced defect trapping could significantly modify the carrier dynamics and should be paid attention to in photoemission experiments for two-dimensional materials.

Scattering and absorption properties of metal nanostructures have been well understood based on the classic oscillator theory. Here, we demonstrate that photoluminescence of metal nanostructures can also be explained based on a classic model. The model shows that inelastic radiation of an oscillator resembles its resonance band after external excitation, and is related to the photoluminescence from metallic nanostructures. The understanding based on the classic oscillator model is in agreement with that predicted by a quantum electromagnetic cavity model. Moreover, by correlating a two-temperature model and the electron distributions, we demonstrate that both one-photon and two-photon luminescence of the metal nanostructures undergo the same mechanism. Furthermore, the model explains most of the emission characteristics of the metallic nanostructures, such as quantum yield, spectral shape, excitation polarization and power dependence. The model based on an oscillator provides an intuitive description of the photoluminescence process and may enable rapid optimization and exploration of the plasmonic properties.

For versatile lead-halide perovskite materials, their trap states, both in the bulk and at the surface, significantly influence optoelectronic behaviors and the performance of the materials and devices. Direct observation of the trap dynamics at the nanoscale is necessary to understand and improve the device design. In this report, we combined the femtosecond pump–probe technique and photoemission electron microscopy (PEEM) to investigate the trap states of an inorganic perovskite CsPbBr3 single-crystal microplate with spatial–temporal–energetic resolving capabilities. Several shallow trap sites were identified within the microplate, while the deep traps were resolved throughout the surface. The results revealed high-defect tolerance to the shallow traps, while the surface dynamics were dominated by the surface deep traps. The ultrafast PEEM disclosed a full landscape of fast electron transfer and accumulation of the surface trap states. These discoveries proved the excellent electronic properties of perovskite materials and the importance of surface optimization.