Abstract
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, (Hg3S2)(FeCl4) and (Hg3S2)(CoCl4), with trigonally aligned 1-D infinite magnetic ∞1(FeCl4)2− or ∞1(CoCl4)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.
Highlights
Complexes with discrete one-dimensional (1-D) magnetic subunits have attracted much attention due to their high uniaxial magnetic anisotropy and quantum tunneling relaxation, which may find applications in the areas of information storage and molecular spintronics[1]
Geometric spin frustration is a type of spin configurations that can constraint a large fraction of magnetic sites to randomly adopt several nearly degenerate spin configurations resulting in disordered ground states[16]
Magnetic ordering phenomena in geometrically frustrated spin systems are subject of numerous studies, and it can lead to spiral spin order and E-type antimagnetic order in some multiferroics exhibiting multifunctional ferroelectricity and magnetism[7]
Summary
Two new inorganic supramolecular complexes, (Hg3S2)(FeCl4) (1) and (Hg3S2)(CoCl4) (2), in which 1-D infinite ∞1(FeCl4)2− or ∞1(CoCl4)2− chains penetrate perpendicularly the 2-D (Hg3S2)2+ layers through hexagonally aligned voids, assembled by Van der Waals forces, have been prepared by solid-state reactions The comparison among those metal chalcohalides with similar low-dimensional structure features indicates semiconductive Hg3Q2 chalcogenide layers exhibit high flexibility to stabilize different kinds of guest polyanions. Both complexes feature long-range spin order below critical temperatures ~37 K for 1 and ~10 K for 2 with strong field dependence, indicated by variable-temperature magnetic susceptibilities. Considering the semiconductive character of metal chalcohalides especially those without toxic elements and the assembling flexibility with transition metal halides, some chalcohalides of transition metals may be predicted to exhibit interesting multifunctional semiconductive and cooperative magnetic properties
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