Mater Horiz
Institute of Physics and Astronomy, University of Potsdam, Karl-Liebknecht-Straße 24/25, 14476, Germany.
Published: January 2025
Two-dimensional transition metal dichalcogenides (2D TMDCs) can be combined with organic semiconductors to form hybrid van der Waals heterostructures. Specially, non-fullerene acceptors (NFAs) stand out due to their excellent absorption and exciton diffusion properties. Here, we couple monolayer tungsten diselenide (ML-WSe) with two well performing NFAs, ITIC, and IT-4F (fluorinated ITIC) to achieve hybrid architectures. Using steady state and time resolved spectroscopic techniques, we reveal sub-picosecond free charge generation in the heterostructure of ML-WSe with ITIC, where however, bimolecular recombination of spin uncorrelated charge carriers with possible contributions from geminate charge recombination cause rapid formation of low-lying triplet (T) states in ITIC. Importantly, this unwanted process is effectively suppressed when the fluorinated derivative of ITIC, IT-4F, is deposited on ML-WSe. We observe a similar scenario when replacing the ML-TMDC with copper thiocyanate (CuSCN) as the hole acceptor meaning that triplet state formation is not driven by the spin-orbit coupling of ML-WSe. From calculations based on density functional theory, we interpret the high triplet formation in the ML-WSe/ITIC hybrid bilayer due to changes in the nature and energies of the interfacial charge transfer (CT) levels. Our results highlight the delicate balance between excitons and charges in such inorganic/NFA heterostructures.
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http://dx.doi.org/10.1039/d4mh00894d | DOI Listing |
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