4f-πMolecular Hybrid Exhibiting Rich Conductive Phases and Slow Relaxation of Magnetization

Yongbing Shen, Goulven Cosquer, Haitao Zhang, Brian K. Breedlove, Mengxing Cui, Masahiro Yamashita

Research output: Contribution to journalArticlepeer-review

Abstract

Cooperation between single-molecule magnets and electrical conductivity holds promise for preparing high-density magnetic devices; however, there are only a few reports so far. Here we report a 4f-I -based molecular hybrid, k-(ET)5Dy(NCS)7(KCl)0.5 (1) (ET = bis(ethylenedithio)tetrathiafulvalene, NCS- = thiocyanate), which undergoes slow relaxation of the magnetization and electrical conductivity. Unlike common ET-based conductive salts, K+ ions were intercalated into ET layers and coordinated with ET radicals. We found that the ET charges were sensitive to temperature, resulting in rich conductive phases at 75-300 K. In particular, the upturn in conductivity with a clear hysteresis loop was explained by the formation of partially oxidized states with charges close to 0.5+, which accounts for a metallic state. From the results of electronic structure calculations, the hole concentration increased to 125 K, which is consistent with a partially oxidized state upon cooling. The weak antiferromagnetic interactions accompanied by a dual magnetic relaxation process below 4 K are closely associated with the weak 4f-πinteractions.

Original languageEnglish
Pages (from-to)9543-9550
Number of pages8
JournalJournal of the American Chemical Society
Volume143
Issue number25
DOIs
Publication statusPublished - 2021 Jun 30

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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