J. Chakhalian, Z. Salman, J. Brewer, A. Froese, J. He, D. Mandrus, R. Jin
Muon spin relaxation measurements around the 25 K metal-insulator transition in Li$_{0.9}$Mo$_6$O$_{17}$ elucidate a profound role of disorder as a possible mechanism for this transition. The relaxation rate $1/T_1$ and the muon Knight shift are incompatible with the transition to a SDW state and thus exclude it.
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At ambient pressure, lithium molybdenum purple bronze (Li0.9Mo6O17) is a quasi-one dimensional solid in which the anisotropic crystal structure and the linear dispersion of the underlying bands produced by electronic correlations possibly bring about a rare experimental realization of Tomomaga-Luttinger liquid physics. It is also the sole member of the broader purple molybdenum bronzes family where a Peierls instability has not been identified at low temperatures. The present study reports a pressure-induced series of phase transitions between 0 and 12 GPa. These transitions are strongly refle…
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…
We introduce the first multiorbital effective tight-binding model to describe the effect of electron-electron interactions in this system. Upon fixing all the effective hopping parameters in the normal state against an ab initio band structure, and with only the overall scale of the interactions as the sole adjustable parameter, we find that a self-consistent Hartree-Fock solution reproduces extremely well the experimental behavior of the charge density wave (CDW) order parameter in the full range $0<T<T_{\text{c}}$, as well as the precise reciprocal space locations of the partial gap opening …
We investigate the role of inter-orbital fluctuations in the low energy physics of a quasi-1D material - lithium molybdenum purple bronze (LMO). It is an exceptional material that may provide us a long sought realization of a Tomonaga-Luttinger liquid (TLL) physics, but its behaviour at temperatures of the order of $T^*\approx 30$K remains puzzling despite numerous efforts. Here we make a conjecture that the physics around $T^*$ is dominated by multi-orbital excitations. Their properties can be captured using an excitonic picture. Using this relatively simple model we compute fermionic Green's…
We have measured resistivity along the a, b and c axes of Li$_{0.9}$Mo$_6$O$_{17}$ single crystal. The anisotropy $ρ$$_c$ / $ρ$$_a$ and $ρ$$_c$ / $ρ$$_b$ is given, confirming the quasi-one-dimensionality of the compound. The sharp decrease in the anisotropy below a certain temperature (T$_M$) indicates dimensional crossover. Superconductivity occurs at 1.8 K well below $T_M$. Negative MRs are observed with magnetic field (H) applied along b axis. This could be ascribed to suppression of energy gap associated with CDW state. While large positive MR is observed with H $\parallel$ c-axis. The MR …
Temperature dependent photoemission spectroscopy in Li0.9Mo6O17 contributes to evidence for one dimensional physics that is unusually robust. Three generic characteristics of the Luttinger liquid are observed, power law behavior of the k-integrated spectral function down to temperatures just above the superconducting transition, k-resolved lineshapes that show holon and spinon features, and quantum critical (QC) scaling in the lineshapes. Departures of the lineshapes and the scaling from expectations in the Tomonaga Luttinger model can be partially described by a phenomenological momentum broa…
We investigate the electronic structure of the strongly anisotropic, quasi low dimensional purple bronze Li0.9Mo6O17. Building on all-electron ab-initio band structure calculations we obtain an effective model in terms of four maximally localized Wannier orbitals, which turn out to be far from atomic like. We find two half-filled orbitals arranged in chains running along one crystallographic direction, and two full orbitals in perpendicular directions, respectively. The possibility to reduce this model to only two orbitals forming two chains per unit cell with inter-chain coupling is discussed…
We establish the quasi-one-dimensional Li purple bronze as a photoemission paradigm of Luttinger liquid behavior. We also show that generalized signatures of electron fractionalization are present in the angle resolved photoemission spectra for quasi-two-dimensional purple bronzes and certain cuprates. An important component of our analysis for the quasi-two-dimensional systems is the proposal of a ``melted holon'' scenario for the k-independent background that accompanies but does not interact with the peaks that disperse to define the Fermi surface.
Molybdenum purple bronze Li$_{0.9}$Mo$_{6}$O$_{17}$ is an exceptional material known to exhibit one dimensional (1D) properties for energies down to a few meV. This fact seems to be well established both in experiments and in band structure theory. We use the unusual, very 1-dimensional band dispersion obtained in \emph{ab-initio} DFT-LMTO band calculations as our starting point to study the physics emerging below 300meV. A dispersion perpendicular to the main dispersive direction is obtained and investigated in detail. Based on this, we derive an effective low energy theory within the Tomonag…
The band structures of ordered and thermally disordered Li$_2$Mo$_{12}$O$_{34}$ are calculated by use of ab-initio DFT-LMTO method. The unusual, very 1-dimensional band dispersion obtained in previous band calculations is confirmed for the ordered structure, and the overall band structure agrees reasonably with existing photoemission data. Dispersion and bandstructure perpendicular to the main dispersive direction is obtained. A temperature dependent band broadening is calculated from configurations with thermal disorder of the atomic positions within the unit cell. This leads a band broadenin…
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…
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