NDLI: Jahn–Teller orbital glass state in the expanded fcc Cs<sub>3</sub>C<sub>60</sub> fulleride

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Jahn–Teller orbital glass state in the expanded fcc Cs₃C₆₀ fulleride

Content Provider	Royal Society of Chemistry (RSC)
Author	Potočnik, A. Prassides, K. Jeglič, P. Heinmaa, I. Takabayashi, Y. Arčon, D. Stern, R. Rosseinsky, M. J. McDonald, M. T. Ganin, A. Y.
Copyright Year	2014
Abstract	The most expanded fcc-structured alkali fulleride, Cs3C60, is a Mott insulator at ambient pressure because of the weak overlap between the frontier t1u molecular orbitals of the C603− anions. It has a severely disordered antiferromagnetic ground state that becomes a superconductor with a high critical temperature, Tc of 35 K upon compression. The effect of the localised t1u3 electronic configuration on the properties of the material is not well-understood. Here we study the relationship between the intrinsic crystallographic C603− orientational disorder and the molecular Jahn–Teller (JT) effect dynamics in the Mott insulating state. The high-resolution 13C magic-angle-spinning (MAS) NMR spectrum at room temperature comprises three peaks in the intensity ratio 1 : 2 : 2 consistent with the presence of three crystallographically-inequivalent carbon sites in the fcc unit cell and revealing that the JT-effect dynamics are fast on the NMR time-scale of 10−5 s despite the presence of the frozen-in C603− merohedral disorder disclosed by the 133Cs MAS NMR fine splitting of the tetrahedral and octahedral 133Cs resonances. Cooling to sub-liquid-nitrogen temperatures leads to severe broadening of both the 13C and 133Cs MAS NMR multiplets, which provides the signature of an increased number of inequivalent 13C and 133Cs sites. This is attributed to the freezing out of the C603− JT dynamics and the development of a t1u electronic orbital glass state guided by the merohedral disorder of the fcc structure. The observation of the dynamic and static JT effect in the Mott insulating state of the metrically cubic but merohedrally disordered Cs3C60 fulleride in different temperature ranges reveals the intimate relation between charge localization, magnetic ground state, lifting of electronic degeneracy, and orientational disorder in these strongly-correlated systems.
Starting Page	3008
Ending Page	3017
Page Count	10
File Format	HTM / HTML PDF
ISSN	20416520
Volume Number	5
Issue Number	8
Journal	Chemical Science
DOI	10.1039/c4sc00670d
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Antiferromagnetism Jahn\u2013Teller effect Mott insulator Magic angle spinning Mott Superconductivity Alkali metal Nuclear magnetic resonance Carbon Jahn Crystal structure
Content Type	Text
Resource Type	Article
Subject	Chemistry

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