Intrinsic Second-Order Topological Insulator in Two-Dimensional Covalent Organic Frameworks

As an intriguing topological phase, higher-order topological insulators have attracted tremendous attention, but the candidate materials are limited in artificial and inorganic systems. In this work, we propose a universal approach to search for two-dimensional (2D) second-order topological insulators (SOTIs) in covalent organic frameworks (COFs) with C 3 symmetric cores. The underlying mechanism is illustrated through tight-binding calculations in a star lattice, showing the 2D SOTI in an overlooked energy window between two Kagome-bands with four types of nontrivial band structures. The emergence of the unique topological edge and corner states can be understood from the Su–Schrieffer–Heeger model. Furthermore, using the frontier orbital of the monomer building block as an indicator, the 2D SOTI is directly confirmed in three realistic COFs by first-principles calculations. Our results not only extend the concept of organic topological insulators from first-order to second-order but also demonstrate the universal existence of intrinsic higher-order topology in 2D COFs.