Organic NLO materials mainly fall into neutral molecular optical materials and ionic optical materials with an electron donor-π conjugate bridge-electron acceptor (D-π-A) configuration, , ]. 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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