Ferroelectric brightening of spin‑forbidden dark excitons in a WSe2/hybrid-perovskite heterostructure

Abstract

Abstract Long-lived dark excitons in monolayer WSe 2 present promising candidates for carrying spin and valley information, but their optical access and spin manipulation have conventionally required the use of strong external magnetic fields. Here, using a ferroelectric hybrid perovskite heterostructure, we leverage the ferroelectric proximity effect to break the WSe 2 ’s in-plane rotational symmetry and brighten the spin-forbidden dark excitons under zero magnetic field conditions. Furthermore, we show that the twist angle between the WSe 2 and perovskite crystals controls the ferroelectric coupling strength and valley-contrasting polarization. Our proposed mechanism, supported by a four-band tight-binding model, suggests that the ferroelectric proximity effect induces an asymmetric intersublattice interaction, generating an effective in-plane spin-orbit coupling (SOC) field that rotates spin/valley polarization and brightens dark excitons. Our work establishes ferroelectric proximity coupling as a symmetry-tunable, magnetic-field-free strategy for spin exciton control in two-dimensional semiconductors.