Affiliation:
1. Institute for Materials Research Tohoku University 2-1-1 Katahira Aoba-ku Sendai 980–8577 Japan
2. Department of Chemistry Graduate School of Science Tohoku University 6-3 Aramaki-Aza-Aoba Aoba-ku Sendai 980-8578 Japan
3. Department of Materials Engineering Science Osaka University 1-3 Machikaneyama-chou Toyonaka Osaka 560-0043 Japan
4. College of Chemistry and Molecular Sciences Wuhan University Wuhan 430072 China
Abstract
AbstractPartial charge fluctuations in the charge‐ordered state of a material, often triggered by structural disorders and/or defects, can significantly alter its physical characteristics, such as magnetic long‐range ordering. However, it is difficult to post‐chemically fix such accidental partial fluctuations to reconstruct a uniform charge‐ordered state. Herein, we report CO2‐aided charge ordering demonstrated in a CO2‐post‐captured layered magnet, [{Ru2(o‐ClPhCO2)4}2{TCNQ(OMe)2}] ⋅ CO2 (1⊃CO2; o‐ClPhCO2−=ortho‐chlorobenzoate; TNCQ(OMe)2=2,5‐dimethoxy‐7,7,8,8‐tetracyanoquinodimethane). Pristine porous layered magnet 1 had a partially charge‐fluctuated ordered state, which provided ferrimagnetic ordering at TC=65 K. Upon loading CO2, 1 adsorbed one mole of CO2, forming 1⊃CO2, and raising TC to 100 K. This was because of the vanishing charge fluctuations without significantly changing the framework structure. This research illustrates the post‐accessible host–guest chemistry delicately combined with charge, spin, and lattice ordering in a spongy magnet. Furthermore, it highlights how this innovative approach opens up new possibilities for technology and nanoscale magnetism manipulation.