Identification of Two-Dimensional Interlayer Excitons and Their Valley Polarization in MoSe2/WSe2 Heterostructure with h-BN Spacer Layer

Interlayer excitons (IXs) in the heterostructure of monolayer transition metal dichalcogenides (TMDs) are considered as a promising platform to study fundamental exciton physics and for potential applications of next generation optoelectronic devices. The IXs trapped in the moiré potential in a twisted monolayer TMD heterostructure such as MoSe₂/WSe₂ form zero-dimensional (0D) moiré excitons. Introducing an atomically thin insulating layer between TMD monolayers in a twisted heterostructure would modulate the moiré potential landscape, thereby tuning 0D IXs into 2D IXs. However, the optical characteristics of IXs have not been elucidated. Here, we have experimentally investigated the significant optical characteristics arising from IXs in a MoSe₂/h-BN/WSe₂ heterostructure by optical spectroscopy. The experimental results of time-resolved photoluminescence spectroscopy combined with phenomenological rate equation analysis reveal that the radiative decay rate of IXs in the MoSe₂/h-BN/WSe₂ heterostructure changes as a function of temperature, which strongly suggests the emergence of 2D IXs by the modulation of potential. Moreover, we demonstrate the valley polarization arising from the prolonged valley relaxation lifetime of 2D IXs reaching 100 ns at low temperature, which is dominated by electron-hole exchange interactions. These findings provide us with an effective strategy to tailor the dimensionality of IXs and elucidate the desired optoelectronic response of IXs in monolayer semiconductor heterostructures.