Ultrafast pseudospin quantum beats in multilayer WSe2 and MoSe2

Nat Commun. 2022 Aug 25;13(1):4997. doi: 10.1038/s41467-022-32534-3.

Abstract

Layered van-der-Waals materials with hexagonal symmetry offer an extra degree of freedom to their electrons, the so-called valley index or valley pseudospin, which behaves conceptually like the electron spin. Here, we present investigations of excitonic transitions in mono- and multilayer WSe2 and MoSe2 materials by time-resolved Faraday ellipticity (TRFE) with in-plane magnetic fields, B, of up to 9 T. In monolayer samples, the measured TRFE time traces are almost independent of B, which confirms a close to zero in-plane exciton g factor g, consistent with first-principles calculations. In contrast, we observe pronounced temporal oscillations in multilayer samples for B > 0. Our first-principles calculations confirm the presence of a non-zero g for the multilayer samples. We propose that the oscillatory TRFE signal in the multilayer samples is caused by pseudospin quantum beats of excitons, which is a manifestation of spin- and pseudospin layer locking in the multilayer samples.