Three-Dimensional Resonant Exciton in Monolayer Tungsten Diselenide Actuated by Spin–Orbit Coupling

The intricate features of many-body interactions and spin–orbit coupling play a significant role in numerous physical phenomena. Particularly in two-dimensional transition metal dichalcogenides (2D-TMDs), excitonic dynamics are a key phenomenon that promises opportunities for diverse range of device applications. Here, we report the direct observation of a visible-range three-dimensional resonant exciton and its associated charged exciton in monolayer tungsten diselenide, as compared to monolayer molybdenum disulfide. A comprehensive experimental study that includes high-resolution TEM, Raman, high-resolution spectroscopic ellipsometry over a wide temperature range down to 4 K, high-energy temperature, and excitation power-dependent photoluminescence spectroscopy has been conducted. It is supported by first-principles calculations to unravel the influence of spin–orbit coupling in the formation of the resonant exciton and to identify its in-plane and out-of-plane features. Furthermore, we study the impact of temperature and thickness on the spin–orbit coupling strength in 2D-TMDs. This work is crucial in creating a platform in the fundamental understanding of high-energy resonant exciton in layered two-dimensional systems and that such high-energy optoelectronic features make them an increasingly attractive candidate for novel electronic and optoelectronic applications particularly in the aspects of solar cells and light-emitting diodes via the manipulation of excitonic states.