Instability of Pa3‾\overline 3 Cs3_{3}C60_{60} at ambient pressure and superconducting state of the FCC phase

The alkali-doped fulleride Cs$_{3}$C$_{60}$, crystallized in the space group Fm$\overline 3$m or Pm$\overline 3$n, exhibits unconventional $s$-wave superconductivity under pressure with a maximum $T_c\sim 38$ K. Recently, a new primitive-cubic-structured Cs$_{3}$C$_{60}$ phase corresponding to the space group Pa$\overline 3$ has been reported (arXiv:2208.09429) and the authors observed superconductivity at ambient pressure. Using density-functional theory (DFT) calculations, we show that the proposed Pa$\overline 3$ structure is not stable under ionic relaxation, but transforms into the FCC structure. We study the normal and superconducting state of the stable FCC phase at different temperatures and volumes using DFT plus dynamical mean-field theory (DFT+DMFT) in the Nambu formalism. As temperature increases, the transition between superconductor and normal metal (Mott insulator) at small (big) volume is found to be second (first) order. The recently developed maximum entropy analytic continuation method for the anomalous-self-energy is used to study the momentum-resolved spectra and optical conductivity.Comment: 6 pages + 4 pages, 1 Tabl

Crystal structure and phase transitions across the metal-superconductor boundary in the SmFeAsO1-xFx (0 < x < 0.20) family

The fluorine-doped rare-earth iron oxyarsenides, REFeAsO1-xFx (RE =rare earth) have recently emerged as a new family of high-temperature superconductors with transition temperatures (Tc) as high as 55 K (refs 1-4). Early work has provided compelling evidence that the undoped parent materials exhibit spin-density-wave (SDW) antiferromagnetic order and undergo a structural phase transition from tetragonal to orthorhombic crystal symmetry upon cooling.5 Both the magnetic and structural instabilities are suppressed upon doping with fluoride ions before the appearance of superconductivity.6,7 Here we use high-resolution synchrotron X-ray diffraction to study the structural properties of SmFeAsO1-xFx (0 < x < 0.20) in which superconductivity emerges near x ~ 0.07 and Tc increases monotonically with doping up to x ~ 0.20.8 We find that orthorhombic symmetry survives through the metal-superconductor boundary well into the superconducting regime 2 and the structural distortion is only suppressed at doping levels, x > 0.15 when the superconducting phase becomes metrically tetragonal. Remarkably this crystal symmetry crossover coincides with reported drastic anomalies in the resistivity and the Hall coefficient8 and a switch of the pressure coefficient of Tc from positive to negative,9 thereby implying that the low-temperature structure plays a key role in defining the electronic properties of these superconductors

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

Mott localization in the correlated superconductor Cs3C60 resulting from the molecular Jahn-Teller effect

Cs3C60 is a correlated superconductor under pressure, but an insulator under ambient conditions. The mechanism causing this insulating behavior is the combination of Mott localization and the dynamic Jahn-Teller effect. We show evidence from infrared spectroscopy for the dynamic Jahn-Teller distortion. The continuous change with temperature of the splitting of infrared lines is typical Jahn-Teller behavior, reflecting the change in population of solid-state conformers. We conclude that the electronic and magnetic solid-state properties of the insulating state are controlled by molecular phenomena. We estimate the time scale of the dynamic Jahn-Teller effect to be above 10^(-11) s and the energy difference between the conformers less than 20 cm-1

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

Optimized unconventional superconductivity in a molecular Jahn-Teller metal

Understanding the relationship between the superconducting, the neighboring insulating, and the normal metallic state above Tc is a major challenge for all unconventional superconductors. The molecular A3C60 fulleride superconductors have a parent antiferromagnetic insulator in common with the atom-based cuprates, but here, the C603– electronic structure controls the geometry and spin state of the structural building unit via the on-molecule Jahn-Teller effect. We identify the Jahn-Teller metal as a fluctuating microscopically heterogeneous coexistence of both localized Jahn-Teller–active and itinerant electrons that connects the insulating and superconducting states of fullerides. The balance between these molecular and extended lattice features of the electrons at the Fermi level gives a dome-shaped variation of Tc with interfulleride separation, demonstrating molecular electronic structure control of superconductivity

Crystal structure of the new FeSe1-x superconductor

The newly discovered superconductor FeSe1-x (x=0.08, Tconset=13.5 K at ambient pressure rising to 27 K at 1.48 GPa) exhibits a structural phase transition from tetragonal to orthorhombic below 70 K at ambient pressure - the crystal structure in the superconducting state shows remarkable similarities to that of the REFeAsO1-xFx (RE = rare earth) superconductorsComment: Chem. Commun. (2008

Structural and electronic response upon hole-doping of rare-earth iron oxyarsenides Nd1-xSrxFeAsO (0 < x < 0.2)

Hole-doping of NdFeAsO via partial replacement of Nd3+ by Sr2+ is a successful route to obtain superconducting phases (Tc = 13.5 K for a Sr2+ content of 20%); however, the structural and electronic response with doping is different from and non-symmetric to that in the electron-doped side of the phase diagram.Comment: 4 pages, 4 figure