π-electron S = 1/2 quantum spin-liquid state in an ionic polyaromatic hydrocarbon

Yasuhiro Takabayashi, Melita Menelaou, Hiroyuki Tamura, Nayuta Takemori, Takashi Koretsune, Aleš Štefančič, Gyöngyi Klupp, A. Johan C. Buurma, Yusuke Nomura, Ryotaro Arita, Denis Arčon, Matthew J. Rosseinsky, Kosmas Prassides

Research output: Contribution to journalArticlepeer-review

22 Citations (Scopus)

Abstract

Molecular solids with cooperative electronic properties based purely on μ electrons from carbon atoms offer a fertile ground in the search for exotic states of matter, including unconventional superconductivity and quantum magnetism. The field was ignited by reports of high-temperature superconductivity in materials obtained by the reaction of alkali metals with polyaromatic hydrocarbons, such as phenanthrene and picene, but the composition and structure of any compound in this family remained unknown. Here we isolate the binary caesium salts of phenanthrene, Cs(C14H10) and Cs2(C14H10), to show that they are multiorbital strongly correlated Mott insulators. Whereas Cs2(C14H10) is diamagnetic because of orbital polarization, Cs(C14H10) is a Heisenberg antiferromagnet with a gapped spin-liquid state that emerges from the coupled highly frustrated Δ-chain magnetic topology of the alternating-exchange spiral tubes of S = 1/2 (C14H10).- radical anions. The absence of long-range magnetic order down to 1.8 K (T/J ≈ 0.02; J is the dominant exchange constant) renders the compound an excellent candidate for a spin-1/2 quantum-spin liquid (QSL) that arises purely from carbon μ electrons.

Original languageEnglish
Pages (from-to)635-643
Number of pages9
JournalNature Chemistry
Volume9
Issue number7
DOIs
Publication statusPublished - Jul 1 2017
Externally publishedYes

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

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