Iyengar Sathvik Ajay, Tripathi Manoj, Srivastava Anchal, Biswas Abhijit, Gray Tia, Terrones Mauricio, Dalton Alan B, Pimenta Marcos A, Vajtai Robert, Meunier Vincent, Ajayan Pulickel M
Department of Materials Science and NanoEngineering, Rice University, Houston, TX, 77005, USA.
Department of Physics and Astronomy, School of Mathematical and Physical Sciences, University of Sussex, Brighton, BN1 9QH, UK.
Adv Mater. 2025 Aug;37(34):e2419136. doi: 10.1002/adma.202419136. Epub 2025 May 28.
2D materials provide ideal platforms for breakthroughs in both fundamental science and practical, real-world applications. Despite the broad diversity of 2D materials, most integration efforts have focused on homo/hetero-structural stacking and Janus structures. In this paper, we introduce "glaphene"-a hybrid of two fundamentally different materials: 2D silica glass and graphene. We propose a metastable hybrid structure based on first-principles calculations, synthesize it via scalable liquid precursor-based vapor-phase growth, and chemically validate the interlayer structure and hybridization using extensive optical and electron spectroscopy, mass spectrometry, and atomic-resolution electron microscopy. Using probe microscopy, we reveal that electronic cloud redistribution at the interface-beyond conventional van der Waals interactions-drives interlayer hybridization via a strong electronic proximity effect. By reconstructing the energy level diagram of glaphene through both theory and experiment, we show that the combination of semi-metallic graphene (E≈0 eV) and insulating 2D silica glass (E≈8.2 eV, E≈7 eV) results in a semiconducting "glaphene" (E≈3.6 eV, E≈4 eV) formed through out-of-plane p hybridization. This work paves the way for scalable, bottom-up methodologies to bring interlayer hybridization and its emergent properties to the 2D materials toolbox.
二维材料为基础科学和实际应用中的突破提供了理想平台。尽管二维材料种类繁多,但大多数集成工作都集中在同/异质结构堆叠和Janus结构上。在本文中,我们介绍了“glaphene”——一种由两种截然不同的材料组成的混合物:二维石英玻璃和石墨烯。我们基于第一性原理计算提出了一种亚稳混合结构,通过基于可扩展液体前驱体的气相生长方法合成了它,并使用广泛的光学和电子光谱、质谱以及原子分辨率电子显微镜对层间结构和杂化进行了化学验证。通过探针显微镜,我们揭示了界面处的电子云重新分布——超越了传统的范德华相互作用——通过强大的电子近邻效应驱动层间杂化。通过理论和实验重建glaphene的能级图,我们表明半金属石墨烯(E≈0 eV)和绝缘二维石英玻璃(E≈8.2 eV,E≈7 eV)的组合导致通过面外p杂化形成了半导体“glaphene”(E≈3.6 eV,E≈4 eV)。这项工作为可扩展的自下而上方法铺平了道路,将层间杂化及其新出现的特性引入二维材料工具箱。