Engineering Dipole-Dipole Couplings for Enhanced Cooperative Light-Matter Interactions

Cooperative optical effects are enabled and controlled by interactions between molecular dipoles, meaning that their mutual orientation is of paramount importance to, for example, superabsorbing light-harvesting antennas. Here we show how to move beyond the possibilities of simple geometric tailoring, demonstrating how a metallic sphere placed within a ring of parallel dipoles engineers an effective Hamiltonian that generates “guide-sliding” states within the ring system. This allows steady-state superabsorption in noisy room temperature environments, outperforming previous designs while being significantly simpler to implement. As exemplified by this showcase, our approach represents a powerful design paradigm for tailoring cooperative light-matter effects in molecular structures that extends beyond superabsorbing systems to a huge array of quantum energy transport systems. Published by the American Physical Society 2025