Clathrate hydrates (CHs) have recently attracted considerable research interest in fundamental science and practical applications because guest molecules with special electronic properties can be selectively trapped in the hydrogen-bonded water cages, and thus such CHs could be a novel class of promising functional materials. However, information about the electronic properties of CHs containing paramagnetic guest molecules and the spin-coupling mechanisms are quite scarce. In this work, at the ab initio molecular dynamics level, we first simulate the magnetic properties and spin-coupling mechanism of the structure I-type double O 2 CHs (O 2 @CHs) derived from the experimental crystal structure. The results show that these O 2 @CHs exhibit rich diversity of spin-coupling characteristics, depending on the O 2 -occupation patterns of the nanocages and relative orientations of two O 2 , which govern the orbital overlaps between the spin carriers. O 2 @CHs presents the antiferromagnetic coupling when two guest O 2 are encapsulated in two symmetric 5 12 6 2 cages or one 5 12 6 2 cage with parallel orientations, whereas it exhibits the paramagnetic state for all other population patterns. The direct O 2 •••O 2 spin couplings operate through the diffuse parts of the O 2 orbitals in these systems. Further, the elastic strain is examined for tuning their magnetic properties, finding that spin arrangement and magnetic characteristics can reversibly convert between the antiferromagnetic [
Although α-methylene-δ-valerolactone (MVL) as a biorenewable six membered lactone bearing an exocyclic double bond has shown great potential to prepare functional polyester with pendent modifiable vinyl group, the copolymerization of...
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