arXiv subjects

M. Greenblatt

Publications and source records attributed to M. Greenblatt.

14 recordsLinked to original sources

arXiv2026

Anisotropic fully-gapped superconductivity in quasi-one-dimensional Li$_{0.9}$Mo$_6$O$_{17}$

Superconductivity in quasi-one-dimensional Li$_{0.9}$Mo$_6$O$_{17}$ emerges from an exotic, non-metallic normal state that exhibits signatures of Tomonaga-Luttinger liquid behavior, emergent symmetry and excitonic order. The high upper critical field, $H_{c2}$, in Li$_{0.9}$Mo$_6$O$_{17}$ suggests that that the favored pairing state is spin-triplet in nature. Here, we report measurements of the magnetic penetration depth down to $0.08\,\mathrm{K}$ ($T/T_c \lesssim 0.04$) and the specific heat down to $0.4\,\mathrm{K}$ ($T/T_c \lesssim 0.2$), and show that they are consistent with a moderately-coupled, fully-gapped superconducting state with marked gap anisotropy and a minimum ($\Delta_{\rm min} \simeq 0.4\,k_{\mathrm{B}}T_c$) occurring over a very narrow region in $k$-space. Combined with knowledge of $H_{c2}$, these measurements support the presence of a nodeless and possibly odd-parity spin-triplet superconducting order parameter in Li$_{0.9}$Mo$_6$O$_{17}$.

cond-mat.supr-con↗

arXiv2023

Wannier-Orbital theory and ARPES for the quasi-1D conductor LiMo$_{6}$O$_{17}$

In this set of three papers, we present the results of a combined study by density-functional (LDA) band theory (NMTO) and angle-resolved photoemission spectroscopy (ARPES) of lithium purple bronze, 2(Li$_{1x}$Mo$_{6}$O$_{17}$). This material is particularly notable for its unusually robust quasi-one-dimensional (quasi-1D) behavior. The band structure, in a large energy window around the Fermi energy, is basically 2D and formed by three Mo $t_{2g}$-like extended Wannier orbitals (WOs) per cell, each one giving rise to a 1D band running at a 120$^{\circ }$ angle to the two others. A structural "dimerization" from $\mathbf{c}/2$ to $\mathbf{c}$ gaps the $xz$ and $yz$ bands while leaving the $xy$ bands metallic in the gap but resonantly coupled to the gap edges and, hence, to the two other directions. The resulting complex shape of the quasi-1D Fermi surface (FS), verified by our ARPES, thus depends strongly on the Fermi energy position in the gap, implying a great sensitivity to Li stoichiometry of properties dependent on the FS, such as FS nesting or superconductivity. The band structure, expressed as a six-band, analytical tight-binding (TB) Hamiltonian, is verified in detail by the recognition and application of an ARPES selection rule that enables, for the first time, the separation in ARPES spectra of the two barely split $xy$ bands and the observation of their complex split FS. The strong resonances prevent either a two-band TB model or a related real-space ladder picture from giving a valid description of the low-energy electronic structure. Down to a temperature of 6$\,$K we find no evidence for a theoretically expected downward renormalization of perpendicular single particle hopping due to LL fluctuations in the quasi-1D chains.

cond-mat.str-el↗

arXiv2021

Pressure-induced structural transitions triggering dimensional crossover in lithium purple bronze Li0.9M6O17

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 reflected in infrared spectroscopy, Raman spectroscopy, and x-ray diffraction. The most dramatic effect seen in optical conductivity is the metallization of the c-axis, concomitant to the decrease of conductivity along the b-axis. This indicates that high pressure drives the material away from its quasi-one dimensional behavior at ambient pressure. While the first pressure-induced structure of the series is resolved, the identification of the underlying mechanisms driving the dimensional change in the physics remains a challenge.

cond-mat.str-el↗

arXiv2015

Anomalous charge and negative-charge-transfer insulating state in cuprate chain-compound KCuO_2

Using a combination of X-ray absorption spectroscopy experiments with first principle calculations, we demonstrate that insulating KCuO_2 contains Cu in an unusually-high formal-3+ valence state, the ligand-to-metal (O to Cu) charge transfer energy is intriguingly negative (Delta~ -1.5 eV) and has a dominant (~60%) ligand-hole character in the ground state akin to the high Tc cuprate Zhang-Rice state. Unlike most other formal Cu^{3+} compounds, the Cu 2p XAS spectra of KCuO_2 exhibits pronounced 3d^8 (Cu^{3+}) multiplet structures, which accounts for ~40% of its ground state wave-function. Ab-initio calculations elucidate the origin of the band-gap in KCuO_2 as arising primarily from strong intra-cluster Cu 3d - O 2p hybridizations (t_{pd}); the value of the band-gap decreases with reduced value of t_{pd}. Further, unlike conventional negative charge-transfer insulators, the band-gap in KCuO_2 persists even for vanishing values of Coulomb repulsion U, underscoring the importance of single-particle band-structure effects connected to the one-dimensional nature of the compound.

cond-mat.str-el↗

arXiv2013

Synthesis and properties of charge-ordered thallium halide perovskites, CsTl1+0.5Tl3+0.5X3 (X = F, Cl)- theoretical precursors for superconductivity?

Recently CsTlCl3 and CsTlF3 perovskites were theoretically predicted to be potential superconductors if they are optimally doped. The synthesis of these two compounds, together with a complete characterization of the samples are reported. CsTlCl3 is obtained as orange crystals in two different polymorphs: a tetragonal (I4/m) and a cubic (Fm-3m) phase. CsTlF3 is formed as a light brown powder, also as a double cubic perovskite (Fm-3m). In all three CsTlX3 phases Tl1+ and Tl3+ were located in two different crystallographic positions that accommodate their different bond lengths. In CsTlCl3 some Tl vacancies are found in the Tl1+ position. The charge ordering between Tl1+ and Tl3+ was confirmed by x-ray absorption and Raman spectroscopy. The Raman spectroscopy of CsTlCl3 under high pressure (58 GPa) did not indicate any phase transition to a possible single Tl2+ state. However, the highly insulating material becomes less resistive with increasing high pressure, while undergoing a change in the optical properties, from transparent to deeply opaque red, indicative of a decrease of the band gap. The theoretical design and experimental validation of the existence of CsTlF3 and CsTlCl3 cubic perovskites is the necessary first step in confirming the theoretical prediction of superconductivity in these materials.

cond-mat.mtrl-sci↗

arXiv2013

NMR evidence for spin fluctuations in the bilayer nickelate La3Ni2O6

We report nuclear magnetic resonance data in the bilayer nickelate La3Ni2O6. This material belongs to a family of low valence nickel oxides with square planar coordination of the Ni ions and is isoelectronic to the high temperature superconducting cuprates. Although the three layer nickelate compound exhibits a spin-state transition accompanied by antiferromagnetic order, the bilayer material shows no phase transition. The NMR data in the bilayer La3Ni2O6 reveal the presence of antiferromagnetic spin fluctuations down to 5K that are surprisingly similar to those present in the magnetically ordered trilayer La4Ni3O8, suggesting a similar electronic structure in the paramagnetic phase of both compounds.

cond-mat.str-el↗

arXiv2012

On the transport and thermodynamic properties of quasi-two-dimensional purple bronzes A$_{0.9}$Mo$_6$O$_{17}$ (A=Na, K)

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.

cond-mat.str-el↗

arXiv2012

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

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.

cond-mat.supr-con↗

arXiv2010

NMR evidence for antiferromagnetic order in a planar 3d9/3d8 nickelate

We report La-139 Nuclear Magnetic Resonance (NMR) data in La4Ni3O8 which reveals the presence of antiferromagnetic order below T_N ~ 105 K. This compound contains two-dimensional layers of NiO2 that are isostructural to the copper oxide planes of the high temperature superconductors. This compound is remarkable because the average Ni valence of 1.33+ for formally 2Ni1+ + Ni2+ indicates a 3d9/3d8 electronic configuration. Nickel oxides with Ni1+ valence are rare and unstable, yet may provide new routes to high temperature superconductivity. La4Ni3O8, with antiferromagnetic order of S=1/2 Ni1+ spins, is analogous to the parent compounds of the cuprate superconductors. Our data clearly reveal dramatic spectral changes and low energy antiferromagnetic correlations associated with the onset of long range order below T_N.

cond-mat.str-el↗

arXiv2008

Magnetic and electric properties of double-perovskites and estimation of their Curie temperatures by ab initio calculations

First principles electronic structure calculations have been carried out on ordered double perovskites Sr_2B'B"O_6 (for B' = Cr or Fe and B" 4d and 5d transition metal elements) with increasing number of valence electrons at the B-sites, and on Ba_2MnReO_6 as well as Ba_2FeMoO_6. The Curie temperatures are estimated ab initio from the electronic structures obtained with the local spin-density functional approximation, full-potential generalized gradient approximation and/or the LDA+U method (U - Hubbard parameter). Frozen spin-spirals are used to model the excited states needed to evaluate the spherical approximation for the Curie temperatures. In cases, where the induced moments on the oxygen was found to be large, the determination of the Curie temperature is improved by additional exchange functions between the oxygen atoms and between oxygen and B' and B" atoms. A pronounced systematics can be found among the experimental and/or calculated Curie temperatures and the total valence electrons of the transition metal elements.

cond-mat.mtrl-sci↗

arXiv2007

Ageing memory and glassiness of a driven vortex system

Many systems in nature, glasses, interfaces and fractures being some examples, cannot equilibrate with their environment, which gives rise to novel and surprising behaviour such as memory effects, ageing and nonlinear dynamics. Unlike their equilibrated counterparts, the dynamics of out-of- equilibrium systems is generally too complex to be captured by simple macroscopic laws. Here we investigate a system that straddles the boundary between glass and crystal: a Bragg glass formed by vortices in a superconductor. We find that the response to an applied force evolves according to a stretched exponential, with the exponent reflecting the deviation from equilibrium. After the force is removed, the system ages with time and its subsequent response time scales linearly with its age (simple ageing), meaning that older systems are slower than younger ones. We show that simple ageing can occur naturally in the presence of sufficient quenched disorder. Moreover, the hierarchical distribution of timescales, arising when chunks of loose vortices cannot move before trapped ones become dislodged, leads to a stretched-exponential response.

cond-mat.supr-con↗

arXiv2004

Structural aspects of the metal-insulator transition in BaVS3

A sequence of structural transitions occurring in the quasi-one-dimensional (1D) 3d1 system BaVS3 at low temperature was investigated by high resolution synchrotron X-ray diffraction. The orthorhombic Cmc21 structure of the intermediate-temperature (70K<T<240K) phase was confirmed. A model for the low-T (T<70K) k=(1 0 1/2)O superstructure (with Im symmetry) is proposed and refined. The formation of the superstructure is associated with the stabilization of a mixed bond order / charge density wave.

cond-mat.str-el↗

arXiv2004

Real Space Imaging of the Microscopic Origins of the Ultrahigh Dielectric Constant in Polycrystalline CaCu3Ti4O12

The origins of an ultrahigh dielectric constant in polycrystalline CaCu3Ti4O12 (CCTO) was studied using the combination of impedance spectroscopy, electron microscopy, and scanning probe microscopy (SPM). Impedance spectra indicate that the transport properties in the 0.1 Hz .. 1 MHz frequency range are dominated by a single parallel resistive-capacitive (RC) element with a characteristic relaxation frequency of 16 Hz. Dc potential distributions measurements by SPM illustrate that significant potential drops occur at the grain boundaries, which thus can be unambiguously identified as the dominant RC element. High frequency ac amplitude and phase distributions illustrate very weak contrast at the interfaces, which is indicative of strong capacitive coupling. These results demonstrate that the ultrahigh dielectric constant reported for polycrystalline CCTO materials are related to the grain boundary behavior.

cond-mat.mtrl-sci↗

arXiv2001

Edge and Bulk Transport in the Mixed State of a Type-II Superconductor

By comparing the voltage-current (V-I) curves obtained before and after cutting a sample of 2H-NbSe2, we separate the bulk and edge contributions to the transport current at various dissipation levels and derive their respective V- I curves and critical currents. We find that the edge contribution is thermally activated across a current dependent surface barrier. By contrast the bulk V-I curves are linear, as expected from the free flux flow model. The relative importance of bulk and edge contributions is found to depend on dissipation level and sample dimensions. We further show that the peak effect is a sharp bulk phenomenon and that it is broadened by the edge contribution.

cond-mat.supr-con↗