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Superconducting critical field far above the Pauli limit in one-dimensional Li$_{0.9}$Mo$_6$O$_{17}$

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 Added by Nigel Hussey
 Publication date 2012
  fields Physics
and research's language is English




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The upper critical field $H_{c2}$ of purple bronze Li$_{0.9}$Mo$_6$O$_{17}$ is found to exhibit a large anisotropy, in quantitative agreement with that expected from the observed electrical resistivity anisotropy. With the field aligned along the most conducting axis, $H_{c2}$ increases monotonically with decreasing temperature to a value five times larger than the estimated paramagnetic pair-breaking field. Theories for the enhancement of $H_{c2}$ invoking spin-orbit scattering or strong-coupling superconductivity are shown to be inadequate in explaining the observed behavior, suggesting that the pairing state in Li$_{0.9}$Mo$_6$O$_{17}$ is unconventional and possibly spin-triplet.



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We report a detailed magnetotransport study of the highly anisotropic quasi-one-dimensional oxide Li$_{0.9}$Mo$_6$O$_{17}$ whose in-chain electrical resistivity diverges below a temperature $T_{rm min} sim$ 25 K. For $T < T_{rm min}$, a magnetic field applied parallel to the conducting chain induces a large negative magnetoresistance and ultimately, the recovery of a metallic state. We show evidence that this insulator/metal crossover is a consequence of field-induced suppression of a density-wave gap in a highly one-dimensional conductor. At the highest fields studied, there is evidence for the possible emergence of a novel superconducting state with an onset temperature $T_c >$ 10 K.
Thermopower and electrical resistivity measurements transverse to the conducting chains of the quasi-one-dimensional metal Li(0.9)Mo(6)O(17) are reported in the temperature range 5 K <= T <= 500 K. For T>= 400 K the interchain transport is determined by thermal excitation of charge carriers from a valence band ~ 0.14 eV below the Fermi level, giving rise to a large, p-type thermopower that coincides with a small, n-type thermopower along the chains. This dichotomy -- semiconductor-like in one direction and metallic in a mutually perpendicular direction -- gives rise to substantial transverse thermoelectric (TE) effects and a transverse TE figure of merit among the largest known for a single compound.
A correlation between lattice parameters, oxygen composition, and the thermoelectric and Hall coefficients is presented for single-crystal Li(0.9)Mo(6)O(17), a quasi-one-dimensional (Q1D) metallic compound. The possibility that this compound is a compensated metal is discussed in light of a substantial variability observed in the literature for these transport coefficients.
The Nernst coefficient for the quasi-one-dimensional metal, Li(0.9)Mo(6)O(17), is found to be among the largest known for metals (~500 microV/KT at T~20K), and is enhanced in a broad range of temperature by orders of magnitude over the value expected from Boltzmann theory for carrier diffusion. A comparatively small Seebeck coefficient implies that Li(0.9)Mo(6)O(17) is bipolar with large, partial Seebeck coefficients of opposite sign. A very large thermomagnetic figure of merit, ZT~0.5, is found at high field in the range T~35-50K.
Long-range order in quasi-one-dimensional (q1D) arrays of superconducting nanowires is established via a dimensional crossover from a fluctuating 1D regime to a phase-coherent 3D ground state. If a homogeneous crystalline superconductor exhibits sufficiently high uniaxial anisotropy, a similar 1D$rightarrow$3D crossover has been predicted to occur, provided that single-particle hopping transverse to the 1D axis is absent in the normal state. Here we present magnetic penetration depth and electrical transport data in single crystals of q1D Tl$_2$Mo$_6$Se$_6$, which reveal a 1D$rightarrow$3D superconducting dimensional crossover. Both experimental techniques uncover multiple energy scales within the superconducting transition, which describe a sequence of fluctuating regimes. As the temperature is reduced below $T_{ons}=$~6.7~K, 1D pairing fluctuations are replaced by 1D phase slips below $T_psim$~5.9~K. These give way to 3D phase fluctuations below $T_{ab}=$~4.9~K, prior to dimensional crossover at $T_{x2}sim$~4.4~K. The electrical resistivity below $T_{ab}$ is quantitatively consistent with the establishment of phase coherence through gradual binding of Josephson vortex strings to form 3D loops. An anomalously low superfluid density persist down to $sim$3~K before rising steeply --- in agreement with a theoretical model for crossovers in q1D superconductors, and suggesting that a small population of unbound, weakly-pinned vortices survives below the crossover. The observation of a dimensional crossover within the superconducting state has important consequences for the low-temperature normal state in Tl$_2$Mo$_6$Se$_6$ and similar q1D metals, which may exhibit one-dimensional behavior over far greater temperature ranges than band structure calculations suggest.
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