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Spin-state switching driven by divergent structural evolutions in a 3D spin-crossover material
Meng-Ling Wu†, Jun-Hui Liang†, Yan-Ru Chen, Kang Chen, Ze-Yu Ruan, Si-Guo Wu*, Wei-Zhao Cai*, Ming-Liang Tong*
https://doi.org/10.1016/j.cjsc.2026.100941
Spin crossover; Pressure; Symmetry breaking; Stimuli-responsive; Spin-state regulation
ABSTRACT
The exploration of structural evolutions in dynamic crystals under multiple stimuli is of high interest. Herein, we develop a cyanide-bridged bimetallic coordination polymer [Fe{Ag(CN)2}2(imipz)] (1-Fe, imipz = imidazo[1,2-a]pyrazine) featuring one-dimensional zigzag Ag chains with argentophilic interactions. 1-Fe exhibits an incomplete spin-crossover (SCO) behavior with a hysteresis loop of 19 K. Notably, temperature and pressure drive distinct crystal evolution pathways that lead to divergent spin-state regulation. Under thermal annealing, the intermediate spin-state is achieved mainly through the deflection of the imipz ligand and leads to the formation of non-equivalent SCO-active centers. Under hydrostatic compression, Ag−CN−Fe linkages undergo significant structural deformations, resulting in enhanced argentophilic interactions and anisotropic compressibility in the lattice. Concomitantly, a reversible pressure-induced electronic configuration modulation occurs, transitioning from a high-spin to a low-spin state accompanied by an isostructural phase transition. These results highlighted in this work elucidate the stimuli-responsive mechanisms for spin-state trapping via dynamic structural deformations, and provide a novel perspective for the design of addressable functional crystals.
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CN 35–1112/TQ, ISSN 0254–5861, Online ISSN: 2949-768X Copyright @ 2022 Chinese Journal of Structural Chemistry-www.Chinese Journal of Structural Chemistry.net. All Rights Reserved 闽ICP备2022002645号-1