![]() Compared with inorganic materials, organic counterparts exhibit the advantages of ultra-fast electro-optical response, low dielectric constant, and diverse molecular design possibility. ![]() Different types of nonlinear optical materials have received considerable attention in NLO optics. In addition to second harmonic generation (SHG), electro-optic modulation, and optical rectification, many applications would significantly benefit from nonlinear optical crystals, , ]. The design of a material with strong second-order nonlinear optical (NLO) responses is highly attractive, , ]. Moreover, the optical properties of the DABT, including its permittivity, absorption coefficient, and reflectance, were systematically investigated, revealing that the DABT crystal is an anisotropic and a new and promising material with hydrophobicity and anisotropy, holding great potential applications in nonlinear optics. Results indicate that the as-designed DABT crystal possesses non-centrosymmetric structure with space group P2 1, and particularly, it exhibits a large static first-order hyperpolarizability of ∼117 × 10 −30 esu. A simple approach that can be employed in rapidly and efficiently evaluating the second-order nonlinear properties of organic crystals based on its crystal structure information was also proposed. In this work, a new benzothiazolium-based ionic organic NLO material (E)-2-(4-(dimethylamino)styryl)-3-methylbenzothiazol-3-ium 4-methylbenzenesulfonate (DABT) containing strong electron donor and acceptor was designed and theoretically investigated. Second-order nonlinear optical (NLO) crystal materials are applied widely.
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