Exciton interacting with a moiré lattice: Polarons, strings, and optical probing of spin correlations

Abstract

The ability to create and stack different atomically thin transition metal dichacogenide (TMD) layers on top of each other has opened up a rich playground for exploring new and interesting two-dimensional (2D) quantum phases. As a consequence of this remarkable development, there is presently a need for new sensors to probe these 2D layers, since conventional techniques for bulk materials such as x-ray and neutron scattering are inefficient. Here, we develop a general theory for how an exciton in a TMD monolayer couples to spin and charge correlations in an adjacent moiré lattice created by a TMD bilayer. Virtual tunneling of charge carriers, assumed for concreteness to be holes, between the moiré lattice and the monolayer combined with the presence of bound hole-exciton states, i.e., trions, give rise to an effective interaction between the moiré holes and the exciton. In addition to the Umklapp scattering, we show that this interaction is spin-dependent and therefore couples the exciton to the spin correlations of the moiré holes, which may be in- as well as out-of-plane. We then use our theory to examine two specific examples where the moiré holes form in-plane ferromagnetic or antiferromagnetic order. In both cases, the exciton creates spin waves in the moiré lattice, which we analyze by using a self-consistent Born approximation that includes such processes to infinite order. We show that the competition between magnetic order and exciton motion leads to the formation of a well-defined quasiparticle consisting of the exciton surrounded by a cloud of magnetic frustration in the moiré lattice sites below. For the antiferromagnet, we furthermore demonstrate the presence of the elusive geometric string excitations and discuss how they can be observed via their smoking gun energy dependence on the spin-spin coupling, which can be tuned by varying the twist angle of the moiré bilayer. All these phenomena have clear signatures in the exciton spectrum, and as such our results illustrate that excitons are promising quantum probes providing optical access to the spin correlations of new phases predicted to exist in TMD materials.