Photoinduced C鈥揅 Reactions on Insulators toward Photolithography of Graphene Nanoarchitectures

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• 作者：Carlos-Andres Palma ; Katharina Diller ; Reinhard Berger ; Alexander Welle ; Jonas Bj枚rk ; Jose Luis Cabellos ; Duncan J. Mowbray ; Anthoula C. Papageorgiou ; Natalia P. Ivleva ; Sonja Matich ; Emanuela Margapoti ; Reinhard Niessner ; Bernhard Menges ; Joachim Reichert ; Xinliang Feng ; Hans Joachim R盲der ; Florian Klappenberger ; Angel Rubio ; Klaus M眉llen ; Johannes V. Barth
• 刊名：Journal of the American Chemical Society
• 出版年：2014
• 出版时间：March 26, 2014
• 年：2014
• 卷：136
• 期：12
• 页码：4651-4658
• 全文大小：587K
• 年卷期：v.136,no.12(March 26, 2014)
• ISSN：1520-5126

文摘

On-surface chemistry for atomically precise sp² macromolecules requires top-down lithographic methods on insulating surfaces in order to pattern the long-range complex architectures needed by the semiconductor industry. Here, we fabricate sp²-carbon nanometer-thin films on insulators and under ultrahigh vacuum (UHV) conditions from photocoupled brominated precursors. We reveal that covalent coupling is initiated by C鈥揃r bond cleavage through photon energies exceeding 4.4 eV, as monitored by laser desorption ionization (LDI) mass spectrometry (MS) and X-ray photoelectron spectroscopy (XPS). Density functional theory (DFT) gives insight into the mechanisms of C鈥揃r scission and C鈥揅 coupling processes. Further, unreacted material can be sublimed and the coupled sp²-carbon precursors can be graphitized by e-beam treatment at 500 掳C, demonstrating promising applications in photolithography of graphene nanoarchitectures. Our results present UV-induced reactions on insulators for the formation of all sp²-carbon architectures, thereby converging top-down lithography and bottom-up on-surface chemistry into technology.