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

DOI: 10.1002/anie.202102984 DOI Help

Authors: Kejun Liu (TU Dresden) , Jiang Li (Helmholtz-Zentrum Dresden-Rossendorf) , Haoyuan Qi (Universitat Ulm) , Mike Hambsch (TU Dresden) , Jonathan Rawle (Diamond Light Source) , Adrián Romaní Vázquez (TU Dresden) , Ali Shaygan Nia (TU Dresden) , Alexej Pashkin (Helmholtz-Zentrum Dresden-Rossendorf) , Harald Schneider (Helmholtz-Zentrum Dresden-Rossendorf) , Mirosllav Polozij (TU Dresden) , Thomas Heine (TU Dresden) , Manfred Helm (Helmholtz-Zentrum Dresden-Rossendorf) , Stefan C. B. Mannsfeld (TU Dresden) , Ute Kaiser (Universitat Ulm) , Renhao Dong (TU Dresden) , Xinliang Feng (TU Dresden)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Angewandte Chemie International Edition

State: Published (Approved)
Published: April 2021
Diamond Proposal Number(s): 25070

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.

Journal Keywords: 2D polymer; graphene; van der Waals heterostructure; transient absorption spectroscopy; interfacial synthesis

Subject Areas: Materials, Chemistry


Instruments: I07-Surface & interface diffraction

Discipline Tags:

Organic Chemistry Material Sciences Chemistry

Technical Tags:

Diffraction Grazing Incidence X-ray Diffraction (GIXD)