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The photosynthetic apparatus of plants and bacteria combine atomicallyprecise pigment-protein complexes with dynamic membrane architectures tocontrol energy transfer on the 10-100 nm length scales. Recently, syntheticmaterials have integrated photosynthetic antennae proteins to enhance excitontransport, though the influence of artificial packing on the excited-statedynamics in these biohybrid materials remains unclear. Here, we use theadaptive Hierarchy of Pure States (adHOPS) to perform a formally exactsimulation of excitation energy transfer within artificial aggregates of lightharvesting complex 2 (LH2) with a range of packing densities. We find that LH2aggregates support a remarkable exciton diffusion length ranging from 100 nm ata biological packing density to 300 nm at the densest packing previouslysuggested in an artificial aggregate. The unprecedented scale of thesecalculations also underscores the efficiency with which adHOPS simulatesexcited-state processes in realistic molecular materials.

Formally Exact Simulations of Mesoscale Exciton Diffusion in a Photosynthetic Aggregate