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Two melamine‐based metal halides, (C3N6H7)(C3N6H6)HgCl3 (I) and (C3N6H7)3HgCl5 (II), are synthesized by incorporating the heavy d10 cation, Hg2+, and the halide anion, Cl−. The noncentrosymmetric structure of I results from two unique attributes: large asymmetric secondary building units produced by direct covalent coordination of melamine to Hg2+ and a small dihedral angle between melamine molecules...
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