Novel low dipole moment (μ) and large first hyperpolarizability (β) electrooptic chromophores have been designed based on the special characteristic of reversed dipole moment in the excited state of exocyclic double bond (ECDB) conjugated bridge by the optimization of the substituted method, and their electronic and second-order nonlinear optical properties have been theoretically investigated by employing the AM1/FF and ZINDO/S-CI approaches. By extending the conjugation length and optimizing the donor/acceptor strength, the oscillator strength of the excited transition that contributes to the molecular nonlinearity can be further enhanced. The designed chromophores possess a larger figure of merit (FOM) than that of 4-N,N-dimethylamino-4’-nitrostilbene (DANS), and lower (5 D) ground state dipole moment.Novel low dipole moment (μ) and large first hyperpolarizability (β) electrooptic chromophores have been designed based on the special characteristic of reversed dipole moment in the excited state of Novel low dipole moment (μ) and large first hyperpolarizability (β) electrooptic chromophores have been designed based on the special characteristic of reversed-dipole moment in the excited state of exocyclic double bond (ECDB) conjugated bridge by the optimization of the substituted method, and their electronic and second-order nonlinear optical properties have been theoretically investigated employing employing the AM1 / FF and ZINDO / S-CI approaches. By extending the conjugation length and optimizing the donor / acceptor strength, the oscillator strength of the excited transition that contributes to The molecular nonlinearity can be further enhanced. The designed chromophores possess a larger figure of merit (FOM) than that of 4-N, N-dimethylamino-4’-nitrostilbene (DANS), and lower (5 D) ground state dipole moment. Novel low dipole moment (μ) and large first hyperpolarizability (β) electrooptic chromophores have been designed based on the special characteristic of reversed dipole moment in th e excited state of