Abstract
In this manuscript, we report the solvent‐dependent synthesis of 1D coordination polymers derived from two planar N2O2‐coordinate iron(II) complexes FeL1 and FeL2, which incorporate TTF(py)2 as a bridging bis‐monodentate ligand. The obtained 1D polymers were characterized through elemental analysis, Mössbauer spectroscopy, single crystal structure analysis for 2a·2 DMF, magnetic susceptibility measurements, X‐ray powder diffraction, cyclic voltammetry and diffuse reflectance spectroscopy, supplemented by DFT computation. The results revealed additive electronic properties of the sub‐units FeL and TTF(py)2 with only minor mutual influence. Intriguingly however, the solvent‐of‐synthesis is found to be a steering factor of the magnetic spin crossover properties of the resulting materials, yielding divergent behavior if obtained from DMF, MeCN or EtOH. This becomes strikingly evident for the magnetic properties of the DMF‐derived polymer which is found trapped in the low‐spin state in the single crystal 2a· 2 DMF, but shows a gradual spin crossover if all solvent is removed.
Highlights
In recent years, the research of molecular magnetic materials has increased in interest due to the application potential in spintronics, memory devices or molecular actuators.[1,2]Switchable coordination compounds are extensively studied as building blocks of such functional molecular materials, often relying on spin crossover (SCO) between energetically close lying spin states
Coordination polymers were formed in a one-pot reaction from equimolar mixtures of the mononuclear iron(II) complexes [FeL1/2(MeOH)2] and the bridging ligand TTF(py
There are already several examples demonstrating that the choice of solvent is not trivial for the synthesis of coordination polymers of the general type [Fe(LN2O2eq)(Lax)]n, as co-crystallized solvent molecules can have a significant impact on the magnetic properties.[20]
Summary
Switchable coordination compounds are extensively studied as building blocks of such functional molecular materials, often relying on spin crossover (SCO) between energetically close lying spin states. It is, well established that octahedral complexes with an iron(II) metal center can be switched between the paramagnetic high spin (S = 2) and diamagnetic low spin (S = 0) state by external stimuli such as temperature, pressure or light, provided suitable ligands were selected.[3,4,5] To address the multifaceted challenges of today’s life, it is desirable to design materials that offer multifunctionality by integrating several properties. More recent studies have focused on the integration of SCO in redox-active materials.[10,11] Especially for a possible application in data storage devices, electrical conductivity is an interesting feature of the material.[12]
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