11^{11}B and 27^{27}Al NMR spin-lattice relaxation and Knight shift study of Mg1−x_{1-x}Alx_xB2_2. Evidence for anisotropic Fermi surface

We report a detailed study of $^{11}$B and $^{27}$Al NMR spin-lattice relaxation rates ($1/T_1$), as well as of $^{27}$Al Knight shift (K) of Mg$_{1-x}$Al$_x$B$_2$, $0\leq x\leq 1$. The obtained ($1/T_1T$) and K vs. x plots are in excellent agreement with ab initio calculations. This asserts experimentally the prediction that the Fermi surface is highly anisotropic, consisting mainly of hole-type 2-D cylindrical sheets from bonding $2p_{x,y}$ boron orbitals. It is also shown that the density of states at the Fermi level decreases sharply on Al doping and the 2-D sheets collapse at $x\approx 0.55$, where the superconductive phase disappears

Evidence of a structural anomaly at 14 K in polymerised CsC60

We report the results of a high-resolution synchrotron X-ray powder diffraction study of polymerised CsC$_{60}$ in the temperature range 4 to 40 K. Its crystal structure is monoclinic (space group I2/m), isostructural with RbC$_{60}$. Below 14 K, a spontaneous thermal contraction is observed along both the polymer chain axis, $a$ and the interchain separation along [111], $d_1$. This structural anomaly could trigger the occurrence of the spin-singlet ground state, observed by NMR at the same temperature.Comment: 8 pages, 5 figures, submitte

Low Temperature Magnetic Instabilities in Triply Charged Fulleride Polymers

The electronic properties of the C603- polymer in Na2Rb0.3Cs0.7C60 were studied by X-band and high field (109.056 GHz) ESR. They are characteristic of a strongly correlated quasi-one-dimensional metal down to 45 K. On further cooling, a pseudogap of magnetic origin opens at the Fermi level below 45 K with three-dimensional magnetic ordering occurring below TN≈15K, as confirmed by the observation of an antiferromagnetic resonance mode. The Na2Rb1-xCsxC60 family of polymers offers a unique way to chemically control the electronic properties, as the opening of the gap in this system of predominantly itinerant electrons is an extremely sensitive function of the interchain separation

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

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

Two-electronic component behavior in the multiband FeSe0.42_{0.42}Te0.58_{0.58} superconductor

We report X-band EPR and $^{125}$Te and $^{77}$Se NMR measurements on single-crystalline superconducting FeSe$_{0.42}$Te$_{0.58}$ ($T_c$ = 11.5(1) K). The data provide evidence for the coexistence of intrinsic localized and itinerant electronic states. In the normal state, localized moments couple to itinerant electrons in the Fe(Se,Te) layers and affect the local spin susceptibility and spin fluctuations. Below $T_c$, spin fluctuations become rapidly suppressed and an unconventional superconducting state emerges in which $1/T_1$ is reduced at a much faster rate than expected for conventional $s$- or $s_\pm$-wave symmetry. We suggest that the localized states arise from the strong electronic correlations within one of the Fe-derived bands. The multiband electronic structure together with the electronic correlations thus determine the normal and superconducting states of the FeSe$_{1-x}$Te$_x$ family, which appears much closer to other high-$T_c$ superconductors than previously anticipated.Comment: 5 pages, 4 figure

Spin frustration and magnetic ordering in theS=12molecular antiferromagnetfcc−Cs3C60

We have investigated the low-temperature magnetic state of face-centered-cubic (fcc) Cs3C60, a Mott insulator and the first molecular analog of a geometrically frustrated Heisenberg fcc antiferromagnet with S=1/2 spins. Specific heat studies reveal the presence of both long-range antiferromagnetic ordering and a magnetically disordered state below TN=2.2 K, which is in agreement with local probe experiments. These results together with the strongly suppressed TN are unexpected for conventional atom-based fcc antiferromagnets, implying that the fulleride molecular degrees of freedom give rise to the unique magnetic ground state

ROTATIONAL-DYNAMICS OF SOLID C-70 - A NEUTRON-SCATTERING STUDY

PMID: 10011126PMID: 10011126 This work at the University of Sussex at supported by the Science and Engineering Research Council, U.K.PMID: 10011126 This work at the University of Sussex at supported by the Science and Engineering Research Council, U.K.PMID: 10011126 This work at the University of Sussex at supported by the Science and Engineering Research Council, U.K.We report the results of neutron-diffraction and low-energy neutron-inelastic-scattering experiments on high-purity solid C-70 between 10 and 640 K. Thermal hysteresis effects are found to accompany structural changes both on cooling and on heating. The observed diffuse scattering intensity does not change with temperature. At 10 K broad librational peaks are observed at 1.82(16) meV [full width at half maximum=1.8(5) meV]. The peaks soften and broaden further with increasing temperature. At and above room temperature, they collapse into a single quasielastic line. At 300 K, the diffusive reorientational motion appears to be somewhat anisotropic, becoming less so with increasing temperature. An isotropic rotational diffusion model, in which the motions of adjacent molecules are uncorrelated, describes well the results at 525 K. The temperature dependence of the rotational diffusion constants is consistent with a thermally activated process having an activation energy of 32(7) meV.This work at the University of Sussex at supported by the Science and Engineering Research Council, U.K

Spin-freezing in the two-dimensional spin-gap systems SrCu 2Àx Mg x (BO 3 ) 2 (x=0, 0.04, 0.12)

Abstract The magnetic properties of the two-dimensional dimer spin-gap system SrCu 2 (BO 3 ) 2 were investigated by the m + SR technique. The relatively slow fluctuations of spin-dimers slow down with decreasing temperature and an unusual spinfreezing process is unraveled at T f o3:75 K, well within the spin-gap temperature range (T SG E20 K). This quasi-static phase displays a Gaussian field distribution with a remarkable stability with applied longitudinal fields. In support of the criticality of the SrCu 2 (BO 3 ) 2 spin-gap ground state towards an antiferromagnetic transition, Knight-shift measurements suggest that implanted muons may liberate spin density at ToT SG that undergoes spin-freezing at very low temperatures. On the other hand, non-magnetic impurity-doping of the copper sublattice does not suppress the spin-gap ground state and does not lead to magnetic ordering effects of static nature.

Adsorption of fullerene and azafullerene on Cu(111) studied by electron energy loss spectroscopy

Fullerene and azafullerene films were studied by electron energy loss spectroscopy in reflection geometry. Compared to C60, (C59N)2 multilayers show additional vibrational modes that are characteristic of the dimer structure. The (C59N)2 is semiconductor-like and giant optically allowed excitonic transitions are found in the gap in drastic contrast with C60. The azafullerene monolayer on Cu(111) no longer shows the presence of dimers, indicating monomer adsorption. Similarly to C60, azafullerene molecules in contact with the metal substrate receive a transferred charge between two and three electrons. However, the C59N appears more covalently bound to Cu because it decomposes when heated above 660 K while C60 only desorbs.

Strong electron correlations in the normal state of FeSe0.42Te0.58

We investigate the normal state of the '11' iron-based superconductor FeSe0.42Te0.58 by angle resolved photoemission. Our data reveal a highly renormalized quasiparticle dispersion characteristic of a strongly correlated metal. We find sheet dependent effective carrier masses between ~ 3 - 16 m_e corresponding to a mass enhancement over band structure values of m*/m_band ~ 6 - 20. This is nearly an order of magnitude higher than the renormalization reported previously for iron-arsenide superconductors of the '1111' and '122' families but fully consistent with the bulk specific heat.Comment: 5 pages, 4 figures, to appear in Phys. Rev. Let