Single-layer and multi-layer 2D polyimine films have been achieved through interfacial synthesis methods. However, it remains a great challenge to achieve the maximum degree of crystallinity in the 2D polyimines, which largely limits the long-range transport properties. Here we employ a surfactant-monolayer-assisted interfacial synthesis (SMAIS) method for the successful preparation of porphyrin and triazine containing polyimine-based 2D polymer (PI-2DP) films with square and hexagonal lattices, respectively. The synthetic PI-2DP films are featured with polycrystalline multilayers with tunable thickness from 6 to 200 nm and large crystalline domains (100–150 nm in size). Intrigued by high crystallinity and the presence of electroactive porphyrin moieties, the optoelectronic properties of PI-2DP are investigated by time-resolved terahertz spectroscopy. Typically, the porphyrin-based PI-2DP 1 film exhibits a p-type semiconductor behavior with a band gap of 1.38 eV and hole mobility as high as 0.01 cm2 V−1 s−1, superior to the previously reported polyimine based materials.
Bibliographical noteFunding Information:
This work was financially supported by ERC Grant on T2DCP, ERC Starting Grant (FC2DMOF, No. 852909), EU Graphene Flagship and COORNET (SPP 1928) as well as the German Science Council, Centre of Advancing Electronics Dresden, EXC1056, (cfaed) and OR 349/1. H.Q. and U.K. thank the financial support by the DFG in the framework of the ?SALVE? (Sub-Angstrom Low-Voltage Electron Microscopy) project as well the Ministry of Science, Research and the Arts (MWK) of Baden-Wuerttemberg in the framework of the SALVE project. Z.K. thanks financial support from the National Natural Science Foundation of China (51873236). We thank Dresden Center for Nanoanalysis (DCN) at TUD and Dr. Petr Formanek (Leibniz Institute for Polymer Research, IPF, Dresden) and Christine Damm (IFW) for the use of facilities. GIWAXS was carried out at DESY, a member of the Helmholtz Association (HGF), and at Helmholtz-Zentrum Berlin. We would like to thank M. Schwartzkopf for assistance (P03-MINAXS beamline) and Dr. Daniel T?bbens (KMC-2 beamline). We thank HGF and HZB for the allocation of neutron/synchrotron radiation beamtime and ZIH Dresden for computer time.
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