Tebyetekerwa, MikeCheng, YanhuaZhang, JianLi, WeiliLi, HongkunNeupane, GuruWang, BowenTruong, ThienXiao, ChuanxiaoAl-Jassim, Mowafak MYin, ZongyouLu, YueruiMacdonald, DanielNguyen, Hieu2022-07-131936-0851http://hdl.handle.net/1885/268816Organic–inorganic (O–I) heterostructures, consisting of atomically thin inorganic semiconductors and organic molecules, present synergistic and enhanced optoelectronic properties with a high tunability. Here, we develop a class of air-stable vertical O–I heterostructures comprising a monolayer of transition-metal dichalcogenides (TMDs), including WS2, WSe2, and MoSe2, on top of tetraphenylethylene (TPE) core-based aggregation-induced emission (AIE) molecular rotors. The created O–I heterostructures yields a photoluminescence (PL) enhancement of up to ∼950%, ∼500%, and ∼330% in the top monolayer WS2, MoSe2, and WSe2 as compared to PL in their pristine monolayers, respectively. The strong PL enhancement is mainly attributed to the efficient photogenerated carrier process in the AIE luminogens (courtesy of their restricted intermolecular motions in the solid state) and the charge-transfer process in the created type I O–I heterostructures. Moreover, we observe an improvement in photovoltaic properties of the TMDs in the heterostructures including the quasi-Fermi level splitting, minority carrier lifetime, and light absorption. This work presents an inspiring example of combining stable, highly luminescent AIE-based molecules, with rich photochemistry and versatile applications, with atomically thin inorganic semiconductors for multifunctional and efficient optoelectronic devices.This work is funded by the Australian Renewable Energy Agency (ARENA, RND017) and partially supported by the National Science Foundation of China (51973030). M.T. acknowledges the research support of the Australian Government Research Training Program (RTP) Scholarship. H.T.N. acknowledges the fellowship support from the Australian Centre for Advanced Photovoltaics (ACAP).application/pdfen-AU© 2020 American Chemical Societymonolayer semiconductorsphotoluminescence pumpingaggregation-induced emission (AIE)molecular rotorstransition metal dichalcogenidesorganic−inorganic heterostructures202010.1021/acsnano.0c030862021-08-01