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

Abstract

We develop a general theory for how an exciton in an atomically thin transition metal dichacogenide (TMD) monolayer couples to spin and charge correlations in an adjacent moire lattice created by a TMD bi-layer. Virtual tunneling of charge carriers, assumed for concreteness to be holes, between the moire lattice and the monolayer combined with the presence of bound hole-exciton states, i.e. trions, give rise to an effective interaction between the moire 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 moire holes, which may be in- as well as out-of-plane. We then use our theory to examine two specific examples where the moire holes form in-plane ferromagnetic or anti-ferromagnetic order. In both cases, the exciton creates spin waves in the moire lattice, which we analyse 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 moire lattice sites below. For the anti-ferromagnet, 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 moire bi-layer. All these phenomena have clear signatures in the exciton spectrum, and as such our results illustrate that excitons are promising probes providing optical access to the spin correlations of new quantum phases predicted to exist in TMD materials.