Momentum-Locked Edge Excitons in 2D Molecular Crystals

In molecular crystals, molecular excitations can hybridize into collective Frenkel excitons. Here we show that doubly degenerate excitations in planar two-dimensional molecular crystals generate excitonic bands with nontrivial momentum-resolved topological characteristics and edge states appearing only for selected crystallographic terminations. Using a model inspired by aggregates of zinc phthalocyanine molecules deposited on insulating surfaces, we demonstrate that the existence of edge excitons depends sensitively on the crystallographic orientation of the boundary and is governed by the Zak phase of the underlying bulk bands. The resulting edge states exhibit momentum-locked elliptical polarization textures originating from the internal structure of the molecular excitations, potentially enabling directional optical coupling and excitation transport. Our results establish a route toward topological and polarization-textured excitonic states in two-dimensional molecular materials.