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The dimensionality-driven two-photon absorption (2PA) enhancement effect is investigated in a series of functionalized bipyridyl Ru-complexes. Our design strategy leads to very high 2PA responses up to ∼1500 GM. However, we highlight that the 2PA performance vs. dimensionality correlation reaches an unexpected limit stemming from 'anti-cooperative' interchromophoric couplings.

Unexpected disruption of the dimensionality-driven two-photon absorption enhancement within a multipolar polypyridyl ruthenium complex series