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Enhanced values of the second molecular hyperpolarizability, γ, are reported for molecules that undergo significant multidirectional charge redistributions between the ground and excited states, e.g., charge is displaced from the periphery to the center, or vice versa, upon excitation, in during large changes in electric moments higher than dipole moments. The γ-values are compared with those for polyene-like molecules having a similar number of π-electrons. It is demonstrated that the “periphery-to-center charge-transfer” design concept is fruitful and should lead to new molecules with high γ-values.