Topological Frenkel excitons in 2D molecular crystals

Collective molecular excitations govern energy transport in light-harvesting and optoelectronic materials. Theory predicts that excitonic band topology can generate edge-confined states, offering a route to direct energy flow in molecular systems, yet experimental evidence is lacking. Here we use scanning tunnelling microscopy-induced luminescence to image Frenkel excitons in two-dimensional zinc phthalocyanine molecular crystals with nanometer resolution. By varying cluster size, we observe the transition from discrete quantum-confined excitations to collective excitonic bands and directly resolve their real-space wavefunctions. We identify an excitonic state localized at the crystal perimeter and show, through comparison with microscopic theory, that it originates from the momentum-resolved non-trivial topology of the bulk excitonic bands. Our results establish molecular crystals as a platform for engineering topological excitonic states and provide a strategy for controlling energy transport through excitonic band engineering.