Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV24)
DOI: https://doi.org/10.29363/nanoge.hopv.2024.065
Publication date: 6th February 2024
Two-dimensional transition metal dichalcogenides (2D-TMDCs) can be combined with organic semiconductors to form hybrid van der Waals heterostructures [1]. Specially, non-fullerene acceptors (NFAs) stand out by their excellent absorption and exciton diffusion properties [2]. Here, we couple monolayer tungsten diselenide (ML-WSe2) 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 bilayer of ML-WSe2 with ITIC. However, bimolecular recombination of spin uncorrelated charge carriers in the bilayer causes rapid formation of low-lying triplet (T1) states in ITIC. Importantly, this unwanted process is effectively suppressed in the bilayers with the fluorinated derivative of ITIC, IT-4F. We observe a similar scenario when replacing the ML-TMDC by copper thiocyanate (CuSCN) as the hole acceptor meaning that triplet state formation is not driven by the spin-orbit coupling of ML-WSe2. From ab initio calculations using density functional theory, we interpret the high triplet formation in the ML-WSe2/ITIC hybrid bilayer as 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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