Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.124
Publication date: 23rd September 2021
Exciton transport and separation processes across organic-inorganic interfaces are key ingredients in emerging applications in energy conversion. In particular, heterostructures consisting of molecular crystals are widely explored. While advances in experimental methods allow direct observation and detection of exciton properties across such junctions, a detailed understanding of the exciton nature and its relation to the interface structure and composition is still largely lacking. In this talk I will present a computational assessment of the many-body interactions dominating the excitonic nature at the interface between the perylene diimide (PDI) molecular crystal and an Au substrate, using many-body perturbation theory within the GW and Bethe-Salpeter equation (BSE) approach. We study the effect of structural modifications on the dielectric screening, manifested through changes in the quasiparticle and excitation energy gaps, as well as the electron-hole binding. Our findings suggest a close look into local and non-local interactions dominating the excitation energies and the exciton binding and nature in the examined PDI molecular crystals, and shed light on the change in exciton nature and properties upon their adsorption on an inorganic, weakly-interacting substrate, offering structural design principles for excitonic tuning at organic-inorganic interfaces.
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