Ultrafast phonon diffuse scattering as a tool for observing chiral phonons in monolayer hexagonal lattices

At the 2D limit, hexagonal systems such as monolayer transition metal dichalcogenides (TMDs) and graphene exhibit unique coupled spin and momentum-valley physics (valley pseudospin) owing to broken spatial inversion symmetry and strong spin-orbit coupling. Circularly polarized light provides the means for pseudospin-selective excitation of excitons (or electrons and holes) and can yield momentum-valley polarized populations of carriers that are the subject of proposed valleytronic applications. The chirality of these excited carriers has important consequences for the available relaxation/scattering pathways, which must conserve (pseudo)angular momentum as well as energy. One available relaxation channel that satisfies these constraints is coupling to chiral phonons. Here, we show that chiral carrier-phonon coupling following valley-polarized photoexcitation is expected to lead to a strongly valley-polarized chiral phonon distribution when this relaxation mechanism is dominant. This momentum valley phonon polarization is directly measurable using ultrafast phonon diffuse scattering techniques. Using ab initio calculations, we show how the dynamic phonon occupations and valley anisotropy determined by nonequilibrium observations can provide a new window on the physical processes that drive carrier valley depolarization in monolayer TMDs.