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Register a new userAn Experimental and Semi-Empirical Method to Determine the Pauli-Limiting Field in Quasi 2D Superconductors as applied to $kappa$-(BEDT-TTF)$_2$Cu(NCS)$_2$: Strong Evidence of a FFLO State
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We present upper critical field data for $kappa$-(BEDT-TTF)$_2$Cu(NCS)$_2$ with the magnetic field close to parallel and parallel to the conducting layers. We show that we can eliminate the effect of vortex dynamics in these layered materials if the layers are oriented within 0.3 degrees of parallel to the applied magnetic field. Eliminating vortex effects leaves one remaining feature in the data that corresponds to the Pauli paramagnetic limit ($H_p$). We propose a semi-empirical method to calculate the $H_p$ in quasi 2D superconductors. This method takes into account the energy gap of each of the quasi 2D superconductors, which is calculated from specific heat data, and the influence of many body effects. The calculated Pauli paramagnetic limits are then compared to critical field data for the title compound and other organic conductors. Many of the examined quasi 2D superconductors, including the above organic superconductors and CeCoIn$_5$, exhibit upper critical fields that exceed their calculated $H_p$ suggesting unconventional superconductivity. We show that the high field low temperature state in $kappa$-(BEDT-TTF)$_2$Cu(NCS)$_2$ is consistent with the Fulde Ferrell Larkin Ovchinnikov state.
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Superconductivity is a quantum phenomena arising, in its simplest form, from pairing of fermions with opposite spin into a state with zero net momentum. Whether superconductivity can occur in fermionic systems with unequal number of two species distinguished by spin, atomic hyperfine states, flavor, presents an important open question in condensed matter, cold atoms, and quantum chromodynamics, physics. In the former case the imbalance between spin-up and spin-down electrons forming the Cooper pairs is indyced by the magnetic field. Nearly fifty years ago Fulde, Ferrell, Larkin and Ovchinnikov (FFLO) proposed that such imbalanced system can lead to exotic superconductivity in which pairs acquire finite momentum. The finite pair momentum leads to spatially inhomogeneous state consisting of of a periodic alternation of normal and superconducting regions. Here, we report nuclear magnetic resonance (NMR) measurements providing microscopic evidence for the existence of this new superconducting state through the observation of spin-polarized quasiparticles forming so-called Andreev bound states.
The specific heat of the layered organic superconductor $kappa$-% (BEDT-TTF)$_2$Cu(NCS)$_2$, where BEDT-TTF is bisethylenedithio-% tetrathiafulvalene, has been studied in magnetic fields up to 28 T applied perpendicular and parallel to the superconducting layers. In parallel fields above 21 T, the superconducting transition becomes first order, which signals that the Pauli-limiting field is reached. Instead of saturating at this field value, the upper critical field increases sharply and a second first-order transition line appears within the superconducting phase. Our results give strong evidence that the phase, which separates the homogeneous superconducting state from the normal state is a realization of a Fulde-Ferrell-Larkin-Ovchinnikov state.
Single crystals of the layered organic type II superconductor, $kappa$-(BEDT-TTF)$_{2}$Cu(NCS)$_{2}$, have been studied in magnetic fields of up to 33 T and at temperatures between 0.5 K and 11 K using a compact differential susceptometer. When the magnetic field lies precisely in the quasi-two-dimensional planes of the material, there is strong evidence for a phase transition from the superconducting mixed state into a Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state, manisfested as a change in the rigidity of the vortex system. The behaviour of the transition as a function of temperature is in good agreement with theoretical predictions.
The suppression of superconductivity by nonmagnetic disorder is investigated systematically in the organic superconductor $kappa$-(BEDT-TTF)$_2$Cu(NCS)$_2$. We introduce a nonmagnetic disorder arising from molecule substitution in part with deuterated BEDT-TTF or BMDT-TTF for BEDT-TTF molecules and molecular defects introduced by X-ray irradiation. A quantitative evaluation of the scattering time $tau_{rm dHvA}$ is carried out by de Haas-van Alphen (dHvA) effect measurement. A large reduction in $T_{rm c}$ with a linear dependence on $1/tau_{rm dHvA}$ is found in the small-disorder region below $1/tau_{rm dHvA} simeq$ 1 $times$ 10$^{12}$ s$^{-1}$ in both the BMDT-TTF molecule-substituted and X-ray-irradiated samples. The observed linear relation between $T_{rm c}$ and $1/tau_{rm dHvA}$ is in agreement with the Abrikosov-Gorkov (AG) formula, at least in the small-disorder region. This observation is reasonably consistent with the unconventional superconductivity proposed thus far for the present organic superconductor. A deviation from the AG formula, however, is observed in the large-disorder region above $1/tau_{rm dHvA} simeq$ 1 $times$ 10$^{12}$ s$^{-1}$, which reproduces the previous transport study (J. G. Analytis {it et al.}: Phys. Rev. Lett. {bf 96} (2006) 177002). We present some interpretations of this deviation from the viewpoints of superconductivity and the inherent difficulties in the evaluation of scattering time.
Geometrical frustration, quantum entanglement and disorder may prevent long-range order of localized spins with strong exchange interactions, resulting in a novel state of matter. $kappa$-(BEDT-TTF)$_2$-Cu$_2$(CN)$_3$ is considered the best approximation of this elusive quantum-spin-liquid state, but its ground-state properties remain puzzling. Here we present a multi-frequency electron-spin resonance study down to millikelvin temperatures, revealing a rapid drop of the spin susceptibility at $T^*=6,mathrm{K}$. This opening of a spin gap, accompanied by structural modifications, suggests the enigmatic `$6,mathrm{K}$-anomaly as the transition to a valence-bond-solid ground state. We identify an impurity contribution that becomes dominant when the intrinsic spins form singlets. Only probing the electrons directly manifests the pivotal role of defects for the low-energy properties of quantum-spin systems without magnetic order.
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