Up- and Down-Conversion between Intra- and Inter-Valley Excitons in Waveguide Coupled Monolayer WSe2

Abstract: The presence of two spin-split valleys in monolayer (1L) transition metal dichalcogenide (TMD) semiconductors supports versatile exciton species classified by their spin and valley quantum numbers. While the spin-0 intravalley exciton, known as the "bright" exciton, is readily observable, other types of excitons, such as the spin-1 intravalley (spin-dark) and spin-0 intervalley (momentum-dark) excitons, are more difficult to access. Here we develop a waveguide coupled 1L tungsten diselenide (WSe2) device to probe these exciton species. In particular, TM coupling to the atomic layer's out-of-plane dipole moments enabled us to not only efficiently collect, but also resonantly populate the spin-1 dark excitons, promising for developing devices with long valley lifetimes. Our work reveals several upconversion processes that bring out an intricate coupling network linking spin-0 and spin-1 intra- and inter-valley excitons, demonstrating that intervalley scattering and spin-flip are very common processes in the atomic layer. These experimental results deepen our understanding of tungsten diselenide exciton physics and illustrate that planar photonic devices are capable of harnessing versatile exciton species in TMD semiconductors.