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Abstract: Novel organic second-order nonlinear optical (NLO) chromophore with a large flexible rigid isolated group was prepared. The NLO properties were measured in solution and PMMA polymer films. The first order hyperpolarizabilities were equal to 4×10−28 esu and 7×10−29 esu at 1064nm Nd:YAG laser wavelength in solvent and polymer, respectively and these results are in agreement with quantum chemical calculations. Moreover, this chromophore has high thermal stability when thermal decomposition temperature is 270°C. Electrostatic interactions of the chromophores were effectively reduced by isolated group. No apparent change of the shape of UV absorption spectra versus concentration was found. [Copyright &y& Elsevier]

• Novel FTC-type NLO chromophore is designed to developing high performance EO material. • The obtained NLO chromophore possesses good film forming ability and obvious T g near 75 °C. • As EO molecular glass, the poled pure chromophore film displayed the r 33 value of 160 pm/V. To explore the simple strategy for developing excellent electro-optic (EO) materials, a monolithic EO molecular glass (EOMG1) based on thiophene π-conjugation and tricyanofuran acceptor (FTC) was synthesized. A tert -butyldiphenylsilyl (TBDPS) group was introduced to the FTC-based nonlinear optic (NLO) chromophore. The glass transition temperature (T g) of the amorphous films was near 75 ℃, confirmed EOMG1 's glassy state. The theoretical calculation shows that the first hyperpolarizability (β) and dipole moment (μ) of EOMG 1 were calculated to 584 × 10−30esu and 20.73 D. After poling, the poled films EOMG1 diplay large EO activity (r 33) of 160 pm/V at 1310 nm. The r 33 value is greatly enhanced compared to the reported side-chain EO polymer containing the similar FTC-type NLO chromophore due to the increased loading density of the pure chromophore films and the TBDPS group's role of effective isolation. [ABSTRACT FROM AUTHOR]