Gaps and excitations in fullerides with partially filled bands : NMR study of Na2C60 and K4C60

We present an NMR study of Na2C60 and K4C60, two compounds that are related by electron-hole symmetry in the C60 triply degenerate conduction band. In both systems, it is known that NMR spin-lattice relaxation rate (1/T1) measurements detect a gap in the electronic structure, most likely related to singlet-triplet excitations of the Jahn-Teller distorted (JTD) C60^{2-} or C60^{4-}. However, the extended temperature range of the measurements presented here (10 K to 700 K) allows to reveal deviations with respect to this general trend, both at high and low temperatures. Above room temperature, 1/T1 deviates from the activated law that one would expect from the presence of the gap and saturates. In the same temperature range, a lowering of symmetry is detected in Na2C60 by the appearance of quadrupole effects on the 23Na spectra. In K4C60, modifications of the 13C spectra lineshapes also indicate a structural modification. We discuss this high temperature deviation in terms of a coupling between JTD and local symmetry. At low temperatures, 1/T$_1$T tends to a constant value for Na2C60, both for 13C and 23Na NMR. This indicates a residual metallic character, which emphasizes the proximity of metallic and insulting behaviors in alkali fullerides.Comment: 12 pages, 13 figure

Sr 2 IrO 4 magnetic phase diagram, from resistivity

International audienceWe show that the transition to the antiferromagnetic state in zero magnetic field does show up in the transverse resistivity, for which we point out the possibility for a direct spin orientation effect. In an applied field, we propose that the transition is split into two lines, corresponding to in-plane and out-of-plane magnetic ordering. This picture is corroborated by transverse magnetization measurements. The magnetic phase diagram for Sr2IrO4 was investigated, using the angular dependence of the resistivity transverse to the IrO2 planes

Role of dynamic Jahn-Teller distortions in Na2C60 and Na2CsC60 studied by NMR

Through 13C NMR spin lattice relaxation (T1) measurements in cubic Na2C60, we detect a gap in its electronic excitations, similar to that observed in tetragonal A4C60. This establishes that Jahn-Teller distortions (JTD) and strong electronic correlations must be considered to understand the behaviour of even electron systems, regardless of the structure. Furthermore, in metallic Na2CsC60, a similar contribution to T1 is also detected for 13C and 133Cs NMR, implying the occurence of excitations typical of JT distorted C60^{2-} (or equivalently C60^{4-}). This supports the idea that dynamic JTD can induce attractive electronic interactions in odd electron systems.Comment: 3 figure

Mn local moments prevent superconductivity in iron-pnictides Ba(Fe 1-x Mn x)2As2

75As nuclear magnetic resonance (NMR) experiments were performed on Ba(Fe1-xMnx)2As2 (xMn = 2.5%, 5% and 12%) single crystals. The Fe layer magnetic susceptibility far from Mn atoms is probed by the75As NMR line shift and is found similar to that of BaFe2As2, implying that Mn does not induce charge doping. A satellite line associated with the Mn nearest neighbours (n.n.) of 75As displays a Curie-Weiss shift which demonstrates that Mn carries a local magnetic moment. This is confirmed by the main line broadening typical of a RKKY-like Mn-induced staggered spin polarization. The Mn moment is due to the localization of the additional Mn hole. These findings explain why Mn does not induce superconductivity in the pnictides contrary to other dopants such as Co, Ni, Ru or K.Comment: 6 pages, 7 figure

Evidence for distinct polymer chain orientations in KC60 and RbC60

The KC60 and RbC60 polymer phases exhibit contrasting electronic properties while powder diffraction studies have revealed no definite structural difference. We have performed single crystal X-ray diffraction and diffuse scattering studies of these compounds. It is found that KC60 and RbC60 possess different chain orientations about their axes, which are described by distinct space groups Pmnn and I2/m, respectively. Such a structural difference will be of great importance to a complete understanding of the physical properties.Comment: To be published in Phys. Rev. Let

Orientation-dependent C60 electronic structures revealed by photoemission

We observe, with angle-resolved photoemission, a dramatic change in the electronic structure of two C60 monolayers, deposited respectively on Ag (111) and (100) substrates, and similarly doped with potassium to half-filling of the C60 lowest unoccupied molecular orbital. The Fermi surface symmetry, the bandwidth, and the curvature of the dispersion at Gamma point are different. Orientations of the C60 molecules on the two substrates are known to be the main structural difference between the two monolayers, and we present new band-structure calculations for some of these orientations. We conclude that orientations play a key role in the electronic structure of fullerides.Comment: 4 pages, 4 figure

The degenerate 3-band Hubbard model with "anti-Hund's rule" interactions; a model for AxC60

We consider the orbitally degenerate 3-band Hubbard model with on-site interactions which favor low spin and low orbital angular momentum using standard second order perturbation theory in the large Hubbard-U limit. At even integer filling this model is a Mott insulator with a non-degenerate ground state that allows for a simple description of particle-hole excitations as well as gapped spin and orbital modes. We find that the Mott gap is generally indirect and that the single particle spectrum at low doping reappears close to even filling but rescaled by a factor 2/3 or 1/3. The model captures the basic phenomenology of the Mott insulating and metallic fullerides AxC60. This includes the existence of a smaller spin gap and larger charge gap at even integer filling, the fact that odd integer stoichiometries are generally metallic while even are insulating, as well as the rapid suppression of the density of states and superconducting transition temperatures with doping away from x=3.Comment: Revised with additional reference

Detection by NMR of a "local spin-gap" in quenched CsC60

We present a 13C and 133Cs NMR investigation of the CsC60 cubic quenched phase. Previous ESR measurements suggest that this phase is metallic, but NMR reveals contrasting electronic behavior on the local scale. The 13C spin-lattice relaxation time (T1) exhibits a typical metallic behavior down to 50 K, but indicates that a partial spin-gap opens for T<50 K. Unexpectedly, 133Cs NMR shows that there are two inequivalent Cs sites. For one of these sites, the NMR shift and (T1T)^{-1} follow an activated law, confirming the existence of a spin-gap. We ascribe this spin-gap to the occurrence of localized spin-singlets on a small fraction of the C60 molecules.Comment: 4 figure

Orbitally resolved lifetimes in Ba(Fe0.92Co0.08)2As2 measured by ARPES

Despite many ARPES investigations of iron pnictides, the structure of the electron pockets is still poorly understood. By combining ARPES measurements in different experimental configurations, we clearly resolve their elliptic shape. Comparison with band calculation identify a deep electron band with the dxy orbital and a shallow electron band along the perpendicular ellipse axis with the dxz/dyz orbitals. We find that, for both electron and hole bands, the lifetimes associated with dxy are longer than for dxz/dyz. This suggests that the two types of orbitals play different roles in the electronic properties and that their relative weight is a key parameter to determine the ground state