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I07-Surface & interface diffraction	A two‐dimensional polyimide‐graphene heterostructure with ultra‐fast interlayer charge transfer Kejun Liu , Jiang Li , Haoyuan Qi , Mike Hambsch , Jonathan Rawle , Adrián Romaní Vázquez , Ali Shaygan Nia , Alexej Pashkin , Harald Schneider , Mirosllav Polozij , Thomas Heine , Manfred Helm , Stefan C. B. Mannsfeld , Ute Kaiser , Renhao Dong , Xinliang Feng Angewandte Chemie International Edition DOI: 10.1002/anie.202102984 Diamond Proposal Number(s): [25070] Open Access Show Abstract ▼ Abstract: Two‐dimensional polymers (2DPs) are a class of atomically/molecularly thin crystalline organic 2D materials. They are intriguing candidates for the development of unprecedented organic‐inorganic 2D van der Waals heterostructures (vdWHs) with exotic physicochemical properties. In this work, we demonstrate the on‐water surface synthesis of large‐area (cm 2 ), monolayer 2D polyimide (2DPI) with 3.1‐nm lattice. Such 2DPI comprises metal‐free porphyrin and perylene units linked by imide bonds. We further achieve a scalable synthesis of 2DPI‐graphene (2DPI‐G) vdWHs via a face‐to‐face co‐assembly of graphene and 2DPI on the water surface. Remarkably, femtosecond transient absorption spectroscopy reveals an ultra‐fast interlayer charge transfer (~60 fs) in the resultant 2DPI‐G vdWH upon protonation by acid, which is equivalent to that of the fastest reports among inorganic 2D vdWHs. Such large interlayer electronic coupling is ascribed to the interlayer cation‐π interaction between 2DP and graphene. Our work opens opportunities to develop 2DP‐based vdWHs via the on‐water surface synthesis strategy and highlights the unique interface‐induced optoelectronic properties.	Apr 2021

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I07-Surface & interface diffraction

A two‐dimensional polyimide‐graphene heterostructure with ultra‐fast interlayer charge transfer