Hybrid Frenkel-Wannier excitons facilitate ultrafast energy transfer at a 2D-organic interface
Two-dimensional transition metal dichalcogenides (TMDs) and organic semiconductors (OSCs) have emerged as promising material platforms for next-generation optoelectronic devices. The combination of both is predicted to yield emergent properties while retaining the advantages of their individual comp...
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Zusammenfassung: | Two-dimensional transition metal dichalcogenides (TMDs) and organic
semiconductors (OSCs) have emerged as promising material platforms for
next-generation optoelectronic devices. The combination of both is predicted to
yield emergent properties while retaining the advantages of their individual
components. In OSCs the optoelectronic response is typically dominated by
localized Frenkel-type excitons, whereas TMDs host delocalized Wannier-type
excitons. However, much less is known about the spatial and electronic
characteristics of excitons at hybrid TMD/OSC interfaces, which ultimately
determine the possible energy and charge transfer mechanisms across the
2D-organic interface. Here, we use ultrafast momentum microscopy and many-body
perturbation theory to elucidate a hybrid exciton at an TMD/OSC interface that
forms via the ultrafast resonant F\"orster energy transfer process. We show
that this hybrid exciton has both Frenkel- and Wannier-type contributions:
Concomitant intra- and interlayer electron-hole transitions within the OSC
layer and across the TMD/OSC interface, respectively, give rise to an exciton
wavefunction with mixed Frenkel-Wannier character. By combining theory and
experiment, our work provides previously inaccessible insights into the nature
of hybrid excitons at TMD/OSC interfaces. It thus paves the way to a
fundamental understanding of charge and energy transfer processes across
2D-organic heterostructures. |
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DOI: | 10.48550/arxiv.2411.14993 |