Authors
Ying-Ying Wu, Guang-Yan Xu, Zi-Han Yan, Xiao-Yong Zhou, Feng-Lei Yang, Jing-Wei Dai, Shu-Qi Wu, Zhao-Yang Li, Osamu Sato
Published in
Journal of the American Chemical Society. Mar 17, 2025. Epub Mar 17, 2025.
Abstract
The development of high-density information storage materials requires precise control of electron spin states. Multistep spin-crossover (SCO) materials with multiple stable spin states are prime candidates for this purpose. However, accurate control of the dynamic SCO behavior, including the dual dynamic modulation of the spin transition temperature (Tc) and transition steps, has been a significant hurdle. In this study, we propose a new two-dimensional SCO solid solution system, [FeIII(H0.5LI)2-2x(H0.5LCl)2x]·H2O, where H0.5LX (LX for short) denotes 5-X-2-hydroxybenzylidene-hydrazinecarbothioamide, with X being I or Cl and x ranging from 0 to 1. The proposed system exhibits a unique nonmonotonic variation in Tc with x, obtaining a minimum at x = 0.7, allowing fine-tuning of Tc across a 66 K range and control over transition steps from two steps to one step, accomplishing dual modulation. Single-crystal diffraction analysis and periodic density functional theory (DFT) calculations demonstrate that the doped ligand LCl modulates the FeIIIN2O2S2 ligand field with increasing doped LCl ligands during the HS → LS transition in solid solutions, enabling dual dynamic modulation of the Tc and the number of transition steps from two steps to one step through dynamic variation in the structural contraction modes (from b- and c-axis contraction to a-axis contraction). This study motivates the synthetic control of dynamic SCO solid solutions through the altered mode of structural contraction as a complementary route to adjust their SCO behavior.
PMID:
40096634
Bibliographic data and abstract were imported from PubMed on 18 Mar 2025.
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