A two-dimensional honeycomb lattice harbours a pair of inequivalent valleys in the k-space electronic structure, in the vicinities of the vertices of a hexagonal Brillouin zone, K±. It is particularly appealing to exploit this emergent degree of freedom of charge carriers, in what is termed 'valleytronics'. The physics of valleys mimics that of spin, and will make possible devices, analogous to spintronics, such as valley filter and valve, and optoelectronic Hall devices, all very promising for next-generation electronics. The key challenge lies with achieving valley polarization, of which a convincing demonstration in a two-dimensional honeycomb structure remains evasive. Here we show, using first principles calculations, that monolayer molybdenum disulphide is an ideal material for valleytronics, for which valley polarization is achievable via valley-selective circular dichroism arising from its unique symmetry. We also provide experimental evidence by measuring the circularly polarized photoluminescence on monolayer molybdenum disulphide, which shows up to 50% polarization.

We report polarization resolved photoluminescence from monolayer MoS2, a two-dimensional, non-centrosymmetric crystal with direct energy gaps at two different valleys in momentum space. The inherent chiral optical selectivity allows exciting one of these valleys and close to 90% polarized emission at 4K is observed with 40% polarization remaining at 300K. The high polarization degree of the emission remains unchanged in transverse magnetic fields up to 9T indicating robust, selective valley excitation.

Raman spectroscopy is the prime nondestructive characterization tool for graphene and related layered materials. The shear (C) and layer breathing modes (LBMs) are due to relative motions of the planes, either perpendicular or parallel to their normal. This allows one to directly probe the interlayer interactions in multilayer samples. Graphene and other two-dimensional (2d) crystals can be combined to form various hybrids and heterostructures, creating materials on demand with properties determined by the interlayer interaction. This is the case even for a single material, where multilayer stacks with different relative orientations have different optical and electronic properties. In twisted multilayer graphene there is a significant enhancement of the C modes due to resonance with new optically allowed electronic transitions, determined by the relative orientation of the layers. Here we show that this applies also to the LBMs, which can be now directly measured at room temperature. We find that twisting has a small effect on LBMs, quite different from the case of the C modes. This implies that the periodicity mismatch between two twisted layers mostly affects shear interactions. Our work shows that ultralow-frequency Raman spectroscopy is an ideal tool to uncover the interface coupling of 2d hybrids and heterostructures.