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Exploration of new spin systems with low-dimensional subunits have been of great interest in the past decades due to their interesting physical properties and potential applications in molecular spintronics. Two inorganic supramolecular complexes, (Hg 3 S 2 )(FeCl 4 ) and (Hg 3 S 2 )(CoCl 4 ), with trigonally aligned 1-D infinite magnetic  ∞  1 (FeCl 4 ) 2−  or  ∞  1 (CoCl 4 ) 2−  chains have been prepared by solid-state reactions. They exhibit 3-D long-range spin order with strong field dependence and field induced metamagnetic behavior. The intrachain and interchain magnetic coupling constants were estimated by DFT+ U  and DFT+ U +SOC calculations and the both complexes can be regarded as partially frustrated spin systems. The spin Hamiltonian was constructed, the ground state is proposed to be incommensurate spiral spin order, which differs from the commensurate 120° spin structure ground state of fully frustrated trigonal case by a little canted angle. This study shows that cooperative magnetic ordering induced by geometric frustration can be realized in inorganic supramolecular systems assembled by weak van der Waals’ interactions.

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Partial Geometric Frustration in Inorganic Supramolecular Spin Systems with One-Dimensional Trigonally Aligned Magnetic Chains ∞1(MCl4)2− (M = Fe2+, Co2+)