Kavli Affiliate: Jeffrey B. Neaton
| First 5 Authors: Tomojit Chowdhury, Aurélie Champagne, Patrick Knüppel, Zehra Naqvi, Mengyu Gao
| Summary:
Bilayer crystals, formed by stacking monolayers of two-dimensional (2D)
crystals, create interlayer potentials that govern excitonic phenomena but are
constrained by their fixed covalent lattices. Replacing one layer with an
atomically thin molecular crystal overcomes this limitation, as precise control
of functional groups enables tunable 2D molecular lattices and, consequently,
electronic structures. Here, we report molecular tuning of lattices and
excitons in four-atom-thick hybrid bilayer crystals (HBCs), synthesized as
monolayers of perylene-based molecular and transition metal dichalcogenide
(TMD) single crystals. In HBCs, we observe an anisotropic photoluminescence
signal exhibiting characteristics of both molecular and TMD excitons, directly
tuned by molecular geometry and HBC composition. Ab initio calculations reveal
that this anisotropic emission arises from hybrid excitons, which inherit
properties from both layers through a hybridized bilayer band structure. Our
work establishes a synthetically derived, molecule-based 2D quantum materials
platform with the potential for engineering interlayer potentials.
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