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Register a new userStoichiometry, structure, and transport in the quasi-one-dimensional metal, Li(0.9)Mo(6)O(17)
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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.
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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.
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.
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.
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.
We report a comparative study of the specific heat, electrical resistivity and thermal conductivity of the quasi-two-dimensional purple bronzes Na$_{0.9}$Mo$_6$O$_{17}$ and K$_{0.9}$Mo$_6$O$_{17}$, with special emphasis on the behavior near their respective charge-density-wave transition temperatures $T_P$. The contrasting behavior of both the transport and the thermodynamic properties near $T_P$ is argued to arise predominantly from the different levels of intrinsic disorder in the two systems. A significant proportion of the enhancement of the thermal conductivity above $T_P$ in Na$_{0.9}$Mo$_6$O$_{17}$, and to a lesser extent in K$_{0.9}$Mo$_6$O$_{17}$, is attributed to the emergence of phason excitations.
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