Electronic Heat Capacity and Lattice Softening of Partially Deuterated Compounds of κ-(BEDT-TTF)2Cu[N(CN)2]Br

Thermodynamic investigation by calorimetric measurements of the layered organic superconductors, κ-(BEDT-TTF)2Cu[N(CN)2]Br and its partially deuterated compounds of κ-(d[2,2]-BEDT-TTF)2Cu[N(CN)2]Br and κ-(d[3,3]-BEDT-TTF)2Cu[N(CN)2]Br, performed in a wide temperature range is reported. The latter two compounds were located near the metal–insulator boundary in the dimer-Mott phase diagram. From the comparison of the temperature dependences of their heat capacities, we indicated that lattice heat capacities of the partially deuterated compounds were larger than that of the pristine compound below about 40 K. This feature probably related to the lattice softening was discussed also by the sound velocity measurement, in which the dip-like structures of the Δv/v were observed. We also discussed the variation of the electronic heat capacity under magnetic fields. From the heat capacity data at magnetic fields up to 6 T, we evaluated that the normal-state γ value of the partially deuterated compound, κ-(d[3,3]-BEDT-TTF)2Cu[N(CN)2]Br, was about 3.1 mJ K−2 mol−1. Under the magnetic fields higher than 3.0 T, we observed that the magnetic-field insulating state was induced due to the instability of the mid-gap electronic state peculiar for the two-dimensional dimer-Mott system. Even though the volume fraction was much reduced, the heat capacity of κ-(d[3,3]-BEDT-TTF)2Cu[N(CN)2]Br showed a small hump structure probably related to the strong coupling feature of the superconductivity near the boundary.

Merohedral disorder and impurity impacts on superconductivity of fullerenes

Local quasiparticle states around impurities provide essential insight into the mechanism of unconventional superconductivity, especially when the candidate materials are proximate to an antiferromagnetic Mott-insulating phase. While such states have been reported in atom-based cuprates and iron-based compounds, they are unexplored in organic superconductors which feature tunable molecular orientation. Here we employ scanning tunneling microscopy and spectroscopy to reveal multiple forms of robustness of an exotic s-wave superconductivity in epitaxial Rb3C60 films against merohedral disorder, non-magnetic single impurities and step edges at the atomic scale. Yu-Shiba-Rusinov (YSR) states, induced by deliberately incurred Fe adatoms that act as magnetic scatterers, have also been observed. The YSR bound states show abrupt spatial decay and vary in energy with the Fe adatom registry. These results and a doping-dependent study of superconductivity point towards local electron pairing in which the multiorbital electronic correlations and intramolecular phonons together drive the high-temperature superconductivity of doped fullerenes.

Interplay between Vortex Dynamics and Superconducting Gap Structure in Layered Organic Superconductors

Layered organic superconductors motivate intense investigations because they provide various unexpected issues associated with their low dimensionality and the strong electron correlation. Since layered organic superconductors possess simple Fermi surface geometry and they often share similarities to the high temperature oxide superconductors and heavy fermion compounds, research on layered organic superconductors is suitable for understanding the essence and nature of strongly correlated electron systems. In strongly correlated electron systems, one of the central problems concerning the superconducting (SC) state is the symmetry of the SC gap, which is closely related to the paring mechanism. Thus, experimental determination of the SC gap structure is of essential importance. In this review, we present the experimental results for the in-plane angular variation of the flux-flow resistance in layered organic superconductors k-(ET)2Cu(NCS)2, β″-(ET)2SF5CH2CF2SO3, and λ-(BETS)2GaCl4. The interplay between the vortex dynamics and nodal structures is discussed for these superconductors.

Absence of Superconductivity in the Hubbard Dimer Model for κ-(BEDT-TTF)2X

In the most studied family of organic superconductors κ-(BEDT-TTF)2X, the BEDT-TTF molecules that make up the conducting planes are coupled as dimers. For some anions X, an antiferromagnetic insulator is found at low temperatures adjacent to superconductivity. With an average of one hole carrier per dimer, the BEDT-TTF band is effectively 12-filled. Numerous theories have suggested that fluctuations of the magnetic order can drive superconducting pairing in these models, even as direct calculations of superconducting pairing in monomer 12-filled band models find no superconductivity. Here, we present accurate zero-temperature Density Matrix Renormalization Group (DMRG) calculations of a dimerized lattice with one hole per dimer. While we do find an antiferromagnetic state in our results, we find no evidence for superconducting pairing. This further demonstrates that magnetic fluctuations in the effective 12-filled band approach do not drive superconductivity in these and related materials.

Universal scaling of the critical temperature and the strange-metal scattering rate in unconventional superconductors

Dramatic evolution of properties with minute change in the doping level is a hallmark of the complex chemistry which governs copper oxide superconductivity as manifested in the celebrated superconducting domes as well as quantum criticality taking place at precise compositions. The strange metal state, where the resistivity varies linearly with temperature, has emerged as a central feature in the normal state of copper oxide superconductors. The ubiquity of this behavior signals an intimate link between the scattering mechanism and superconductivity. However, a clear quantitative picture of the correlation has been lacking. Here, we report the observation of quantitative scaling laws between the superconducting transition temperature Tc and the scattering rate associated with the strange metal state in electron-doped copper oxide La2-xCexCuO4 (LCCO) as a precise function of the doping level (x). High-resolution characterization of epitaxial composition-spread films, which encompass the entire overdoped range of LCCO has allowed us to systematically map its structural and transport properties with unprecedented accuracy and increment of Δx = 0.0015. We have uncovered the relations Tc ~ (xc-x)0.5 ~ (A1)0.5, where xc is the critical doping where superconductivity disappears on the overdoped side and A1 is the scattering rate of perfect T-linear resistivity per CuO2 plane. We argue that the striking similarity of the Tc vs A1 relation among copper oxides, iron-based and organic superconductors is an indication of a common mechanism of the strange metal behavior and unconventional superconductivity in these systems.

Evidence for metastable photo-induced superconductivity in K3C60

Excitation of high-Tc cuprates and certain organic superconductors with intense far-infrared optical pulses has been shown to create non-equilibrium states with optical properties that are consistent with transient high-temperature superconductivity. These non-equilibrium phases have been generated using femtosecond drives, and have been observed to disappear immediately after excitation, which is evidence of states that lack intrinsic rigidity. Here we make use of a new optical device to drive metallic K3C60 with mid-infrared pulses of tunable duration, ranging between one picosecond and one nanosecond. The same superconducting-like optical properties observed over short time windows for femtosecond excitation are shown here to become metastable under sustained optical driving, with lifetimes in excess of ten nanoseconds. Direct electrical probing, which becomes possible at these timescales, yields a vanishingly small resistance with the same relaxation time as that estimated by terahertz conductivity. We provide a theoretical description of the dynamics after excitation, and justify the observed slow relaxation by considering randomization of the order-parameter phase as the rate-limiting process that determines the decay of the light-induced superconductor.

Evolution of Shape and Volume Fraction of Superconducting Domains with Temperature and Anion Disorder in (TMTSF)2ClO4

In highly anisotropic organic superconductor (TMTSF)2ClO4, superconducting (SC) phase coexists with metallic and spin-density wave phases in the form of domains. Using the Maxwell-Garnett approximation (MGA), we calculate the volume ratio and estimate the shape of these embedded SC domains from resistivity data at various temperature and anion disorder, controlled by the cooling rate or annealing time of (TMTSF)2ClO4 samples. We found that the variation of cooling rate and of annealing time affect differently the shape of SC domains. In all cases the SC domains have oblate shape, being the shortest along the interlayer z-axis. This contradicts the widely assumed filamentary superconductivity along the z-axis, used to explain the anisotropic superconductivity onset. We show that anisotropic resistivity drop at the SC onset can be described by the analytical MGA theory with anisotropic background resistance, while the anisotropic Tc can be explained by considering a finite size and flat shape of the samples. Due to a flat/needle sample shape, the probability of percolation via SC domains is the highest along the shortest sample dimension (z-axis), and the lowest along the sample length (x-axis). Our theory can be applied to other heterogeneous superconductors, where the size d of SC domains is much larger than the SC coherence length ξ, e.g., cuprates, iron-based or organic superconductors. It is also applicable when the spin/charge-density wave domains are embedded inside a metallic background, or vice versa.