Charge dynamics in the 2D/3D semiconductor heterostructure WSe₂/GaAs

Understanding the relaxation and recombination processes of excited states in two-dimensional (2D)/three-dimensional (3D) semiconductor heterojunctions is essential for developing efficient optical and (opto)electronic devices which integrate new 2D materials with more conventional 3D ones. In this work, we unveil the carrier dynamics and charge transfer in a monolayer of WSe$_2$ on a GaAs substrate. We use time-resolved differential reflectivity to study the charge relaxation processes involved in the junction and how they change when compared to an electrically decoupled heterostructure, WSe$_2$/hBN/GaAs. We observe that the monolayer in direct contact with the GaAs substrate presents longer optically-excited carrier lifetimes (3.5 ns) when compared with the hBN-isolated region (1 ns), consistent with a strong reduction of radiative decay and a fast charge transfer of a single polarity. Through low-temperature measurements, we find evidence of a type-II band alignment for this heterostructure with an exciton dissociation that accumulates electrons in the GaAs and holes in the WSe$_2$. The type-II band alignment and fast photo-excited carrier dissociation shown here indicate that WSe$_2$/GaAs is a promising junction for new photovoltaic and other optoelectronic devices, making use of the best properties of new (2D) and conventional (3D) semiconductors.