Abstract
The second-order polarizability components β zzz , β zyy and β yzy = β yyz of N,N′-dihexyl-1,3-diamino-4,6-dinitrobenzene (DHADNB) have been determined by combination of polarization dependent electric-field-induced second-harmonic generation (EFISHG) and hyper-Rayleigh scattering (HRS) experiments in dioxane solution at T=298 K. Dipole moments of the first three optically allowed excited singlet-states were obtained from electrooptical absorption measurements (EOAM) in methylcyclohexane solution. The results show that the second-order polarizability of this two-dimensional (2D) non-linear optical (NLO) chromophor is completely dominated by the off-diagonal components β zyy and β yzy = β yyz , whereas the contribution of β zzz is nearly insignificant. Independent quantum chemical calculations confirm these findings. Although DHADNB is a dipolar molecule, non-dipolar three-level contributions to β are found to be much larger than dipolar two-level contributions.
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