To design nonlinear optical (NLO) materials, we focused on combinations of d metal cation (Cd)-based chloride and morpholine molecules to form organic-inorganic hybrids. The O of morpholine containing lone-pair electrons can be integrated with Cd by a ligand-to-metal charge transfer (LMCT) strategy to build acentric structures benefiting from the second-order Jahn-Teller effect. Introduction of the high-electronegativity chlorine can make polyhedrons of acentric crystals more distorted and conducive to a strong second harmonic generation (SHG) response. Therefore, (Morpholinium)CdCl crystals were constructed and synthesized by a solvent evaporation method. (Morpholinium)CdCl belongs to the orthorhombic 222 space group and shows a one-dimensional (1D) structure with distorted [CdCl] and [CdClO] octahedrons. The short cutoff edge of (Morpholinium)CdCl was determined to be about 230 nm. The SHG response of (Morpholinium)CdCl exhibited an intensity of approximately 0.73 × KDP as estimated by the powder second harmonic generation technique. Furthermore, related theoretical calculations were performed to study the relationship of the band structure, refractive anisotropy, electronic state, and nonlinear optical response. Besides, (Morpholinium)CdCl showed relatively good thermal stability. This work can serve as a guide for the design and synthesis of new large NLO hybrid crystals with d transition metals.
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