Atomic Ordered Array and Vacancy Defect Codependences of Electromagnetic Response in Nanocarbon Bridged‐MXene Superlattices Absorbers

Abstract Binary nanocrystals superlattices with the atomic long range ordered array of different colloidal nanocrystals are deemed as potential electromagnetic wave absorption (EWA) materials in dealing with current electromagnetic radiation problem, as their inherent superiority stems from the cooperative effect of adjacent units and strong interfacial coupling. However, relevant researches remain underdeveloped due to daunting synthetic challenges and complex electromagnetic regulation mechanism. Here, nanocarbon‐bridged 2D‐2D MXene superlattice with tunable vacancy defects are prepared via molecular ligands induced self‐assembly and subsequently nitrogen‐doped pyrolysis strategy, which resulted in “carbon‐MXene‐carbon‐rGO‐carbon” architecture. Such a periodic ordered & nano‐bridging structure optimize axial charges transport over Van der Waals gap and suppressed interface formation between identical components, thereby boosting the charges localization and delocalization. Meanwhile, nitrogen doping further induce abundant Ti atom and Ti sub‐nm clusters vacancy defects, together with generation of diverse dipole polarization centers. The synergistic effects of two mechanisms enabled programmable regulation of sum (ε'+ε'') and quotient (ε''/ε') of permittivity into predicted window required for low matching thickness, resulting in predictable EWA performance (1.5 mm, −56.3 dB). This work provides a versatile strategy for fabrication of atomic long range ordered heterostructures, paving the way for the development of absorbers via structural rearrangement and surface modification.