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Abstract Large crystal growth and characterization of the optical and terahertz (THz) properties of organic nonlinear optical (NLO) crystal NMBA (4‐Nitro‐4′‐methylbenzylidene aniline) is presented. The reported method of crystal growth consistently produces high‐quality single crystals. The THz generation efficiency and optical properties of NMBA to other THz generation crystals including BNA and MNA are compared. The low THz absorptions that make NMBA an ideal source for THz time‐domain spectroscopy are highlighted.
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