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Complex van der Waals heterostructures from layered molecular stacks arepromising optoelectronic materials offering means to efficient, modular chargeseparation and collection layers. The effect of stacking in the electrodynamicsof such hybrid organic-inorganic two-dimensional materials remains largelyunexplored, whereby molecular scale engineering could lead to advanced opticalphenomena. For instance, tunable Fano engineering could make possible on-demandtransparent conducting layers or photoactive elements, and passive cooling. Weemploy an adapted Gersten-Nitzan model and real time time-dependent densityfunctional tight-binding to study the optoelectronics of self-assembledmonolayers on graphene nanoribbons. We find Fano resonances that causeelectromagnetic induced opacity and transparency, and reveal an additionalincoherent process leading to interlayer exciton formation with acharacteristic charge transfer rate. These results showcase hybrid van derWaals heterostructures as paradigmatic 2D optoelectronic stacks, featuringtunable Fano optics and unconventional charge transfer channels.

Fano resonance and incoherent interlayer excitons in molecular van der Waals heterostructures