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 language | English |
|---|---|
| Pages (from-to) | 635-643 |
| Number of pages | 9 |
| Journal | Nature Chemistry |
| Volume | 9 |
| Issue number | 7 |
| DOIs | |
| Publication status | Published - Jul 1 2017 |
| Externally published | Yes |
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ASJC Scopus subject areas
- Chemistry(all)
- Chemical Engineering(all)
Cite this
π-electron S = 1/2 quantum spin-liquid state in an ionic polyaromatic hydrocarbon. / Takabayashi, Yasuhiro; Menelaou, Melita; Tamura, Hiroyuki; Takemori, Nayuta; Koretsune, Takashi; Štefančič, Aleš; Klupp, Gyöngyi; Buurma, A. Johan C.; Nomura, Yusuke; Arita, Ryotaro; Arčon, Denis; Rosseinsky, Matthew J.; Prassides, Kosmas.
In: Nature Chemistry, Vol. 9, No. 7, 01.07.2017, p. 635-643.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - π-electron S = 1/2 quantum spin-liquid state in an ionic polyaromatic hydrocarbon
AU - Takabayashi, Yasuhiro
AU - Menelaou, Melita
AU - Tamura, Hiroyuki
AU - Takemori, Nayuta
AU - Koretsune, Takashi
AU - Štefančič, Aleš
AU - Klupp, Gyöngyi
AU - Buurma, A. Johan C.
AU - Nomura, Yusuke
AU - Arita, Ryotaro
AU - Arčon, Denis
AU - Rosseinsky, Matthew J.
AU - Prassides, Kosmas
PY - 2017/7/1
Y1 - 2017/7/1
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85021262447&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85021262447&partnerID=8YFLogxK
U2 - 10.1038/nchem.2764
DO - 10.1038/nchem.2764
M3 - Article
C2 - 28644474
AN - SCOPUS:85021262447
VL - 9
SP - 635
EP - 643
JO - Nature Chemistry
JF - Nature Chemistry
SN - 1755-4330
IS - 7
ER -