Abstract
Organic/metal interfaces play crucial roles in the formation of intermolecular networks on metal surfaces and the performance of organic devices. Although their purity and uniformity have profound effects on the operation of organic devices, the formation of organic thin films with high interfacial uniformity on metal surfaces has suffered from the intrinsic limitation of molecular ordering imposed by irregular surface structures. Here we demonstrate a supramolecular carpet with widely uniform interfacial structure and high adaptability on a metal surface via a one-step process. The high uniformity is achieved with well-balanced interfacial interactions and site-specific molecular rearrangements, even on a pre-annealed amorphous gold surface. Co-existing electronic structures show selective availability corresponding to the energy region and the local position of the system. These findings provide not only a deeper insight into organic thin films with high structural integrity, but also a new way to tailor interfacial geometric and electronic structures.
Highlights
Organic/metal interfaces play crucial roles in the formation of intermolecular networks on metal surfaces and the performance of organic devices
The strong non-bonding intermolecular interactions induced by the partial positive charge of the S atoms and the partial negative charge of the N atoms of BTDA-TCNQ, and the surface–molecule interactions on both surface steps and terraces enable the step-flow growth mode for the self-organized supramolecular carpet (SMC) domain
Owing to the well-balanced interfacial interactions, the SMC of BTDA-TCNQ on the Au surface can extend over multiple surface steps and terraces without losing its structural integrity, accompanying the unidirectional alignment of the molecular orbital (MO)
Summary
Organic/metal interfaces play crucial roles in the formation of intermolecular networks on metal surfaces and the performance of organic devices. The strong non-bonding intermolecular interactions, balanced with surface–molecule interfacial interactions and site-specific rearrangements of the BTDATCNQ molecules near surface step edges, enable the step-flow growth mode for the SMC formation[35,36] This can lead to an extension of the SMC over step edges of the Au surface without loss of its structural integrity, and results in a covering with high interfacial uniformity over multiple surface steps and terraces, even on the pre-annealed amorphous Au surface prepared on a glass substrate. Different types and dimensionalities of the interfacial electronic structures are distinctively observed in the SMC of BTDA-TCNQ on the Au(111) surface, corresponding to the energy region and the local position of the system, implying that various types of electronic structures projected onto the SMC can be selectively accessible These results suggest that the SMC has great potential for applications in organic electronics, and provide important guidelines to develop novel materials forming seamless OTFs on various surfaces
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