Kavli Affiliate: Jeffrey B. Neaton
| First 5 Authors: Tomojit Chowdhury, Aurélie Champagne, Patrick Knüppel, Zehra Naqvi, Ariana Ray
| Summary:
Bilayer crystals, built by stacking crystalline monolayers, generate
interlayer potentials that govern excitonic phenomena but are constrained by
fixed covalent lattices and orientations. Replacing one layer with an
atomically thin molecular crystal overcomes this limitation, as diverse
functional groups enable tunable molecular lattices and interlayer potentials,
tailoring a wide range of excitonic properties. Here, we report hybrid excitons
in four-atom-thick hybrid bilayer crystals (HBCs), directly synthesized with
single-crystalline perylene diimide (PDI) molecular crystal atop WS2
monolayers. These excitons arise from a hybridized bilayer band structure,
revealed by lattice-scale first-principles calculations, inheriting properties
from both monolayers. They exhibit bright photoluminescence with near-unity
polarization above and below the WS2 bandgap, along with spectral signatures of
exciton delocalization, supported by theory, while their energies and
intensities are tuned by modifying the HBC composition by synthesis. Our work
introduces a molecule-based 2D quantum materials platform for bottom-up design
and control of optoelectronic properties.
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