Density functional theory has been used to calculate the mu.beta(-2 nu;nu,nu,0) on a series of solution-phase hydrazones. Using the experimental and MP2(Full) calculated data as references, the qualitative trend of the Hartree-Fock, M06-HF and range-separated hybrids have been examined. Our results propose methods with long-range corrections, and without short-range exact exchange, are capable of qualitatively predicting the nonlinear optical responses of the hydrazones when reliable geometries have been provided. The same conclusion can also be applied to solution-phase push-pull phenylpolyenes. (C) 2013 Elsevier B.V. All rights reserved.