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In this study, we investigated reversible intermolecular proton shifting (IPS) coupled with spin transition (ST) in a novel FeII complex. The host FeII complex and the guest carboxylic acid anion were connected by intermolecular hydrogen bonds (IHBs). We extended the intramolecular proton transfer coupled ST phenomenon to the intermolecular system. The dynamic phenomenon was confirmed by variable‐temperature single‐crystal X‐ray diffraction, neutron crystallography, and infrared spectroscopy. The mechanism of IPS was further validated using density functional theory calculations. The discovery of IPS‐coupled ST in crystalline molecular materials provides good insights into fundamental processes and promotes the design of novel multifunctional materials with tunable properties for various applications, such as optoelectronics, information storage, and molecular devices. [ABSTRACT FROM AUTHOR]

We synthesized new Fe(II) compounds consisting of [Fe(L)2] (HL: 2-Acetylpyridine isonicotinoylhydrazone) and dicarboxylic acids. Single crystal analysis shows that short hydrogen bonds are formed between [Fe(L)2] and dicarboxylic acids. The hydrogen bonding interactions between metal complexes and dicarboxylic acids are complemented by π-π interactions, forming two-dimensional network structures. Magnetic properties show that the Fe(II) compounds exhibit gradual spin crossover behavior around room temperature and a T1/2 value is dependent on the halogen substituent on the dicarboxylic acids. [ABSTRACT FROM AUTHOR]