Coordination complexes and polymers are central in inorganic and materials chemistry as a variety of metal centers and coordination geometries lead to a diverse range of interesting properties. Here, size and structure control of gem-like quality monocrystals is demonstrated at room temperature. Using the same set of precursors, the copper-to-melamine molar ratio is adjusted to synthesize either a novel coordination complex of dinuclear copper and melamine (Cu2M1), or a barely-studied coordination polymer of zigzag copper-chlorine chains (Cu4M1). Crystals of the former are dark green and square with a size up to 350 μm across. The latter is light green, octagonal, and as large as 5 mm across. The magnetic properties of both crystals reflect the low-dimensional arrangements of copper. The magnetic susceptibility of Cu2M1 is modelled with a spin-1/2 dimer, and that of Cu4M1 with a spin-1/2 one-dimensional Ising chain. Controlled synthesis of such quality magnetic crystals is a prerequisite for various magnetic and magneto-optical applications.
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