Valley and spin dynamics in monolayer MoS$_{2}$

Abstract

Valleytronics targets the exploitation of the additional degrees of freedom in materials where the energy of the carriers may assume several equal minimum values (valleys) at non-equivalent points of the reciprocal space. In single layers of transition metal dichalcogenides (TMDs) the lack of inversion symmetry, combined with a large spin-orbit interaction, leads to a conduction (valence) band with different spin-polarized minima (maxima) having equal energies. This offers the opportunity to manipulate information at the level of the charge (electrons or holes), spin (up or down) and crystal momentum (valley). Any implementation of these concepts, however, needs to consider the robustness of such degrees of freedom, which are deeply intertwined. Here we address the spin and valley relaxation dynamics of both electrons and holes with a combination of ultrafast optical spectroscopy techniques, and determine the individual characteristic relaxation times of charge, spin and valley in a MoS$_{2}$ monolayer. These results lay the foundations for understanding the mechanisms of spin and valley polarization loss in two-dimensional TMDs: spin/valley polarizations survive almost two-orders of magnitude longer for holes, where spin and valley dynamics are interlocked, than for electrons, where these degrees of freedom are decoupled. This may lead to novel approaches for the integration of materials with large spin-orbit in robust spintronic/valleytronic platforms.