Abstract
Polycyclic aromatic hydrocarbons and their derivative nanostructures serve as the fun-damental organic inventory of the universe. Far from static, these species undergo a complex evolu-tionary pathway transitioning from isolated gas-phase molecules to hybrid three-dimensional archi-tectures, such as hydrogenated amorphous carbon and fullerenes. This mini-review reflects recentbreakthroughs across observational, laboratory, and theoretical astrochemistry. With the advent ofthe James Webb Space Telescope, we can now resolve the fine spatial and spectral structures ofphotodissociation regions and distant star-forming galaxies (z∼ 1–2), tracking specific topologi-cal defects in carbon skeletons. Parallel to these observational milestones, laboratory action spec-troscopy utilizing cryogenic ion traps has definitively linked the C+60cation to diffuse interstellarbands and revealed ultrafast radiative cooling mechanisms via recurrent fluorescence. On the theo-retical front, we highlight the critical shift from harmonic models to anharmonic cascade emissionand the deployment of ab initio metadynamics to simulate fullerene assembly. Finally, we explorehow machine learning and neural network potentials are breaking computational bottlenecks, en-abling on-the-fly kinetic modeling of amorphous dust growth.