Abstract
A new aryl-imido polyoxometalate non-linear optical chromophore (POMophore) with a diphenylamino donor group attains the highest
β
zzz, 0
value (196 × 10
−30
esu by Hyper-Rayleigh Scattering, HRS), and best transparency/non-linearity trade off yet for such materials. Stark spectroscopic and DFT investigation of this compound, plus NMe
2
and carbazole analogues, show that its high performance results from a combination of strongly dipolar electronic transitions, and strong electronic communication across the π-system.