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

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. The dimensionality-induced two-photon absorption enhancement is rationalized within a multipolar Ru-complex series with an unexpected disruptive effect emerging from inter-branch 'anti-cooperative' couplings.