Kavli Affiliate: Jeffrey B. Neaton
| First 5 Authors: Aurélie Champagne, Aurélie Champagne, , ,
| Summary:
van der Waals stacking of two-dimensional (2D) materials offers a powerful
platform for engineering material interfaces with tailored electronic and
optical properties. While most van der Waals multilayers have featured
inorganic monolayers, incorporating molecular monolayers introduces new degrees
of tunability and functionality. Here, we investigate hybrid bilayers composed
of atomically thin perylene-based molecular crystals interfaced with monolayer
transition metal dichalcogenides (TMDs), specifically MoS2 and WS2. Using ab
initio many-body perturbation theory within the GW approximation and the
Bethe-Salpeter equation approach, we predict emergent properties beyond those
of the isolated constituent systems. Notably, we find substantial
renormalization of monolayer molecular crystal band gap due to TMD-induced
polarization. Furthermore, by varying the TMD monolayer, we demonstrate tuning
of the energy level alignment of the bilayer and subsequent control over a
diversity of lowest-energy excitons, which include strongly bound hybrid
excitons and long-lived charge-transfer excitons. These findings establish
organic-inorganic van der Waals heterostructures as a promising class of
materials for tunable optoelectronic devices and quantum excitonic phenomena,
expanding the design space for low-dimensional systems.
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