Just Accepted Articles have been posted online after technical editing and typesetting for immediate view. The final edited version with page numbers will appear in the Current Issue soon.
Global aromaticity; Macrocyclic π-systems; Topological π-systems; Three-dimensional aromaticity; Adaptive aromaticity
ABSTRACT
Aromaticity has evolved from a classical concept associated with local planar conjugated molecules into a multidimensional framework encompassing global electronic delocalization in macrocyclic and topological π-systems. This Perspective highlights recent advances in global aromaticity arising from nonalternant topologies, transition-metal incorporation, heteroatom doping, redox-state modulation, and fully π-conjugated three-dimensional molecular cages. These structural and electronic design strategies enable long-range delocalization beyond individual aromatic subunits, giving rise to distinctive magnetic, optical, and electronic properties as well as reversible aromaticity switching. We further discuss recent theoretical developments that distinguish genuine three-dimensional aromaticity from two-dimensional aromaticity embedded within three-dimensional frameworks and summarize emerging concepts such as adaptive aromaticity and excited-state aromaticity. Finally, we outline key challenges in understanding the interplay between local and global aromaticity and highlight future opportunities for the development of responsive functional materials, organic electronics, and quantum functional materials based on globally aromatic architectures.