Abstract

Identifying quantum numbers to label elementary excitations is essential for the correct description of light-matter interaction in solids. In monolayer semiconducting transition metal dichalcogenides (TMDs) such as MoSe2_2 or WSe2_2, most optoelectronic phenomena are described well by labelling electron and hole states with the spin projection along the normal to the layer (Sz_z). In contrast, for WSe2_2/MoSe2_2 interfaces recent experiments show that taking Sz_z as quantum number is not a good approximation, and spin mixing needs to be always considered. Here we argue that the correct quantum number for these systems is not Sz_z, but the zz-component of the total angular momentum -- Jz_z = Lz_z + Sz_z -- associated to the C3_3 rotational lattice symmetry, which assumes half-integer values corresponding modulo 3 to distinct states. We validate this conclusion experimentally through the observation of strong intervalley scattering mediated by chiral optical phonons that -- despite carrying angular momentum 1 -- cause resonant intervalley transitions of excitons, with an angular momentum difference of 2.

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