High-temperature superconductivity from fine-tuning of Fermi-surface singularities in iron oxypnictides.

In the family of the iron-based superconductors, the REFeAsO-type compounds (with RE being a rare-earth metal) exhibit the highest bulk superconducting transition temperatures (Tc) up to 55 K and thus hold the key to the elusive pairing mechanism. Recently, it has been demonstrated that the intrinsic electronic structure of SmFe0.92Co0.08AsO (Tc = 18 K) is highly nontrivial and consists of multiple band-edge singularities in close proximity to the Fermi level. However, it remains unclear whether these singularities are generic to the REFeAsO-type materials and if so, whether their exact topology is responsible for the aforementioned record Tc. In this work, we use angle-resolved photoemission spectroscopy (ARPES) to investigate the inherent electronic structure of the NdFeAsO0.6F0.4 compound with a twice higher Tc = 38 K. We find a similarly singular Fermi surface and further demonstrate that the dramatic enhancement of superconductivity in this compound correlates closely with the fine-tuning of one of the band-edge singularities to within a fraction of the superconducting energy gap Δ below the Fermi level. Our results provide compelling evidence that the band-structure singularities near the Fermi level in the iron-based superconductors must be explicitly accounted for in any attempt to understand the mechanism of superconducting pairing in these materials.

Interaction-induced singular Fermi surface in a high-temperature oxypnictide superconductor.

In the family of iron-based superconductors, LaFeAsO-type materials possess the simplest electronic structure due to their pronounced two-dimensionality. And yet they host superconductivity with the highest transition temperature Tc ≈ 55K. Early theoretical predictions of their electronic structure revealed multiple large circular portions of the Fermi surface with a very good geometrical overlap (nesting), believed to enhance the pairing interaction and thus superconductivity. The prevalence of such large circular features in the Fermi surface has since been associated with many other iron-based compounds and has grown to be generally accepted in the field. In this work we show that a prototypical compound of the 1111-type, SmFe(0.92)Co(0.08)AsO , is at odds with this description and possesses a distinctly different Fermi surface, which consists of two singular constructs formed by the edges of several bands, pulled to the Fermi level from the depths of the theoretically predicted band structure by strong electronic interactions. Such singularities dramatically affect the low-energy electronic properties of the material, including superconductivity. We further argue that occurrence of these singularities correlates with the maximum superconducting transition temperature attainable in each material class over the entire family of iron-based superconductors.

1D to 2D Na+ ion diffusion inherently linked to structural transitions in Na0.7CoO2.

We report the observation of a stepwise "melting" of the low-temperature Na-vacancy order in the layered transition-metal oxide Na0.7CoO2. High-resolution neutron powder diffraction analysis indicates the existence of two first-order structural transitions, one at T1≈290 K followed by a second at T2≈400 K. Detailed analysis strongly suggests that both transitions are linked to changes in the Na mobility. Our data are consistent with a two-step disappearance of Na-vacancy order through the successive opening of first quasi-1D (T1>T>T2) and then 2D (T>T2) Na diffusion paths. These results shed new light on previous, seemingly incompatible, experimental interpretations regarding the relationship between Na-vacancy order and Na dynamics in this material. They also represent an important step towards the tuning of physical properties and the design of tailored functional materials through an improved control and understanding of ionic diffusion.

Single crystal study of the heavy-fermion antiferromagnet CePt2In7.

We report the synthesis, structure, and physical properties of single crystals of CePt(2)In(7). Single crystal x-ray diffraction analysis confirms the tetragonal I4/mmm structure of CePt(2)In(7) with unit cell parameters a = 4.5886(6) Å, c = 21.530(6) Å and V = 453.32(14) Å(3). The magnetic susceptibility, heat capacity, Hall effect and electrical resistivity measurements are all consistent with CePt(2)In(7) undergoing an antiferromagnetic order transition at T(N) = 5.5 K, which is field independent up to 9 T. Above T(N), the Sommerfeld coefficient of specific heat is γ ≈ 300 mJ mol(-1) K(-2), which is characteristic of an enhanced effective mass of itinerant charge carriers. The electrical resistivity is typical of heavy-fermion behavior and gives a residual resistivity ρ(0) ∼ 0.2 µΩ cm, indicating good crystal quality. CePt(2)In(7) also shows moderate anisotropy of the physical properties that is comparable to structurally related CeMIn(5) (M = Co, Rh, Ir) heavy-fermion superconductors.

Melting of the Na layers in solid Na0.8CoO2.

Data of 23Na NMR spectra and relaxation measurements are interpreted as suggesting that, upon increasing temperature, the Na layers in Na0.8CoO2 adopt a 2D liquid state at T=291 K. The corresponding first order phase transition is preceded by a rapidly increasing mobility and diffusion of Na ions above 200 K. Above 291 K, the 23Na NMR response is similar to that previously observed in superionic conductors with planar Na layers.

Direct link between low-temperature magnetism and high-temperature sodium order in NaxCoO2.

We prove the direct link between low-temperature (T) magnetism and high-T Na+ ordering in NaxCoO2 using the example of a so far unreported magnetic transition at 8 K which involves a weak ferromagnetic moment. The 8 K feature is characterized in detail and its dependence on a diffusive Na+ rearrangement around 200 K is demonstrated. Applying muons as local probes this process is shown to result in a reversible phase separation into distinct magnetic phases that can be controlled by specific cooling protocols. Thus the impact of ordered Na+ Coulomb potential on the CoO2 physics is evidenced opening new ways to experimentally revisit the NaxCoO2 phase diagram.

Field-effect-modulated Seebeck coefficient in organic semiconductors.

Central to the operation of organic electronic and optoelectronic devices is the transport of charge and energy in the organic semiconductor, and to understand the nature and dynamics of charge carriers is at the focus of intense research efforts. As a basic transport property of solids, the Seebeck coefficient S provides deep insight as it is given by the entropy transported by thermally excited charge carriers and involves in the simplest case only electronic contributions where the transported entropy is determined by details of the band structure and scattering events. We have succeeded for the first time to measure the temperature- and carrier-density-dependent thermopower in single crystals and thin films of two prototypical organic semiconductors by a controlled modulation of the chemical potential in a field-effect geometry. Surprisingly, we find the Seebeck coefficient to be well within the range of the electronic contribution in conventional inorganic semiconductors, highlighting the similarity of transport mechanisms in organic and inorganic semiconductors. Charge and entropy transport is best described as band-like transport of quasiparticles that are subjected to scattering, with exponentially distributed in-gap trap states, and without further contributions to S.

Superconductivity in single crystals of the fullerene C70.

The observation of superconductivity in doped C60 has attracted much attention, as these materials represent an entirely new class of superconductors. A maximum transition temperature (Tc) of 40 K has been reported for electron-doped C60 crystals, while a Tc of 52 K has been seen in hole-doped crystals; only the copper oxide superconductors have higher transition temperatures. The results for C60 raise the intriguing questions of whether conventional electron-phonon coupling alone can produce such high transition temperatures, and whether even higher transition temperatures might be observed in other fullerenes. There have, however, been no confirmed reports of superconductivity in other fullerenes, though it has recently been observed in carbon nanotubes. Here we report the observation of superconductivity in single crystals of electric-field-doped C70. The maximum transition temperature of about 7 K is achieved when the sample is doped to approximately four electrons per C70 molecule, which corresponds to a half-filled conduction band. We anticipate superconductivity in smaller fullerenes at temperatures even higher than in C60 if the right charge density can be induced.

High-temperature superconductivity in lattice-expanded C60.

C60 single crystals have been intercalated with CHCl3 and CHBr3 in order to expand the lattice. High densities of electrons and holes have been induced by gate doping in a field-effect transistor geometry. At low temperatures, the material turns superconducting with a maximum transition temperature of 117 K in hole-doped C60/CHBr3. The increasing spacing between the C60 molecules follows the general trend of alkali metal-doped C60 and suggests routes to even higher transition temperatures.

Universal crossover from band to hopping conduction in molecular organic semiconductors.

The charge transport in a variety of herringbone-stacked organic molecular semiconductors is investigated in the temperature range from 10 to 550 K. A crossover from coherent bandlike charge transport with mobilities up to several thousand cm (2)/V s at low temperature to an incoherent hopping motion at high temperatures is observed. This is attributed to the localization of the charge carrier due to increased electron-phonon interaction and, finally, the formation of a lattice polaron.

Josephson junctions with tunable weak links.

The electrical properties of organic molecular crystals, such as polyacenes or C60, can be tuned from insulating to superconducting by application of an electric field. By structuring the gate electrode of such a field-effect switch, the charge carrier density, and therefore also the superfluid density, can be modulated. Hence, weak links that behave like Josephson junctions can be fabricated between two superconducting regions. The coupling between the superconducting regions can be tuned and controlled over a wide range by the applied gate bias. Such devices might be used in superconducting circuits, and they are a useful scientific tool to study superconducting material parameters, such as the superconducting gap, as a function of carrier concentration or transition temperature.

Gate-induced superconductivity in a solution-processed organic polymer film.

The electrical and optical properties of conjugated polymers have received considerable attention in the context of potentially low-cost replacements for conventional metals and inorganic semiconductors. Charge transport in these organic materials has been characterized in both the doped-metallic and the semiconducting state, but superconductivity has not hitherto been observed in these polymers. Here we report a distinct metal-insulator transition and metallic levels of conductivity in a polymer field-effect transistor. The active material is solution-cast regioregular poly(3-hexylthiophene), which forms relatively well ordered films owing to self-organization, and which yields a high charge carrier mobility (0.05-0.1 cm2 V(-1) s(-1)) at room temperature. At temperatures below approximately 2.35 K with sheet carrier densities exceeding 2.5 x 10(14) cm(-2), the polythiophene film becomes superconducting. The appearance of superconductivity seems to be closely related to the self-assembly properties of the polymer, as the introduction of additional disorder is found to suppress superconductivity. Our findings therefore demonstrate the feasibility of tuning the electrical properties of conjugated polymers over the largest range possible-from insulating to superconducting.

Electron-phonon coupling spectrum in photodoped pentacene crystals.

The coupling between conduction charges and the vibrational modes of the molecular lattice plays a defining role in the transport characteristics of organic semiconductors. Using electron tunneling spectroscopy, we obtain the electron--optical-phonon coupling spectrum in photodoped pentacene crystals at energies <30 meV. Comparison of the tunneling spectrum to infrared absorption data on the optical phonon density of states yields the energy dependence of the electron-phonon scattering matrix element. The integrated spectral weight of the electron-phonon coupling shows that superconductivity in pentacene is likely of electron-phonon origin.

Superconductivity at 52 K in hole-doped C60.

Superconductivity in electron-doped C60 was first observed almost ten years ago. The metallic state and superconductivity result from the transfer of electrons from alkaline or alkaline-earth ions to the C60 molecule, which is known to be a strong electron acceptor. For this reason, it is very difficult to remove electrons from C60--yet one might expect to see superconductivity at higher temperatures in hole-doped than in electron-doped C60, because of the higher density of electronic states in the valence band than in the conduction band. We have used the technique of gate-induced doping in a field-effect transistor configuration to introduce significant densities of holes into C60. We observe superconductivity over an extended range of hole density, with a smoothly varying transition temperature Tc that peaks at 52 K. By comparison with the well established dependence of Tc on the lattice parameter in electron-doped C60, we anticipate that Tc values significantly in excess of 100 K should be achievable in a suitably expanded, hole-doped C60 lattice.