Many-Body Configurational Spectral Splitting between Trion and Charged Exciton in a Monolayer Semiconductor

Abstract: Many-body electron-hole complexes in a semiconductor are important both from a fundamental physics point of view and for practical device applications. A three-body system of electrons (e) and holes (h) (2e1h, or 1e2h) in a two-band semiconductor is commonly believed to be associated with two spectral peaks for the exciton and trion (or charged exciton), respectively. But both the validity of this understanding and the physical meaning of a trion or charged exciton have not been thoroughly examined. From the physics point of view, there are two different configurations, (e)(eh) or (eeh), which could be considered charged exciton and trion, respectively. Here (...) represents an irreducible cluster with respect to Coulomb interactions. In this paper, we consider these issues related to the 2e1h three-body problem theoretically and experimentally using monolayer MoTe2 as an example. Our theoretical tools involve the three-body Bethe-Salpeter Equation (BSE) and the cluster expansion technique, especially their correspondence. Experimentally, we measure the photoluminescence spectrum on a gate-controlled monolayer MoTe2. We found two spectral peaks that are 21 and 4 meV, respectively, below the exciton peak, in contrast to the single "trion" peak from the conventional understanding. We show that, while the three-body BSE in a two-band model can reproduce all spectral features, the cluster-expansion technique shows that the two peaks correspond to the charged exciton (e)(eh) and trion (eeh), respectively. In other words, there is a spectral splitting due to the two different many-body configurations. Furthermore, we find that the trion only exists in the intervalley case, while the charged exciton exists both for the intervalley and intravalley cases.