The electron flow between a metallic aggregate and an organic molecule after excitation with light is a crucial step on which are based the hybrid photovoltaic nanomaterials. So far, designing...
Complex van der Waals heterostructures from layered molecular stacks are promising optoelectronic materials offering the means to efficient, modular charge separation and collection layers. The effect of stacking in the electrodynamics of such hybrid organic−inorganic two-dimensional materials remains largely unexplored, whereby molecular scale engineering could lead to advanced optical phenomena. For instance, tunable Fano engineering could make possible on-demand transparent conducting layers or photoactive elements, and passive cooling. We employ an adapted Gersten−Nitzan model and real time time-dependent density functional tight-binding to study the optoelectronics of self-assembled monolayers on graphene nanoribbons. We find Fano resonances that cause electromagnetic induced opacity and transparency and reveal an additional incoherent process leading to interlayer exciton formation with a characteristic charge transfer rate. These results showcase hybrid van der Waals heterostructures as paradigmatic 2D optoelectronic stacks, featuring tunable Fano optics and unconventional charge transfer channels.
Graphene nanoribbon heterostructures and heterojunctions
have attracted
interest as next-generation molecular diodes with atomic precision.
Their mass production via solution methods and prototypical device
integration remains to be explored. Here, the bottom-up solution synthesis
and characterization of liquid-phase-processable graphene nanoribbon
heterostructures (GNRHs) are demonstrated. Joint photoresponsivity
measurements and simulations provide evidence of the structurally
defined heterostructure motif acting as a type-I heterojunction. Real-time,
time-dependent density functional tight-binding simulations further
reveal that the photocurrent polarity can be tuned at different excitation
wavelengths. Our results introduce liquid-phase-processable, self-assembled
heterojunctions for the development of nanoscale diode circuitry and
adaptive hardware.
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