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John A. Schlueter

Publications and source records attributed to John A. Schlueter.

32 records · Page 2Linked to original sources

Emergence of a Dynamic Super-Structural Order Integrating Antiferroelectric and Antiferrodistortive Competing Instabilities in EuTiO3

Microscopic structural instabilities of EuTiO3 single crystal were investigated by synchrotron x-ray diffraction. Antiferrodistortive (AFD) oxygen octahedral rotational order was observed alongside Ti derived antiferroelectric (AFE) distortions. The competition between the two instabilities is reconciled through a cooperatively modulated structure allowing both to coexist. The electric and magnetic field effect on the modulated AFD order shows that the origin of large magnetoelectric coupling is based upon the dynamic equilibrium between the AFD - antiferromagnetic interactions versus the electric polarization - ferromagnetic interactions.

cond-mat.mtrl-sci↗

Phase Diagram of Ba1-xKxFe2As2

We report the results of a systematic investigation of the phase diagram of the iron-based superconductor, Ba1-xKxFe2As2, from x = 0 to x = 1.0 using high resolution neutron and x-ray diffraction and magnetization measurements. The polycrystalline samples were prepared with an estimated compositional variation of \Deltax <~ 0.01, allowing a more precise estimate of the phase boundaries than reported so far. At room temperature, Ba1-xKxFe2As2 crystallizes in a tetragonal structure with the space group symmetry of I4/mmm, but at low doping, the samples undergo a coincident first-order structural and magnetic phase transition to an orthorhombic (O) structure with space group Fmmm and a striped antiferromagnet (AF) with space group Fcmm'm'. The transition temperature falls from a maximum of 139K in the undoped compound to 0K at x = 0.252, with a critical exponent as a function of doping of 0.25(2) and 0.12(1) for the structural and magnetic order parameters, respectively. The onset of superconductivity occurs at a critical concentration of x = 0.130(3) and the superconducting transition temperature grows linearly with x until it crosses the AF/O phase boundary. Below this concentration, there is microscopic phase coexistence of the AF/O and superconducting order parameters, although a slight suppression of the AF/O order is evidence that the phases are competing. At higher doping, superconductivity has a maximum Tc of 38 K at x = 0.4 falling to 3 K at x = 1.0. We discuss reasons for the suppression of the spin-density-wave order and the electron-hole asymmetry in the phase diagram.

cond-mat.supr-con↗

Dimensionality selection in a molecule-based magnet

Gaining control of the building blocks of magnetic materials and thereby achieving particular characteristics will make possible the design and growth of bespoke magnetic devices. While progress in the synthesis of molecular materials, and especially coordination polymers, represents a significant step towards this goal, the ability to tune the magnetic interactions within a particular framework remains in its infancy. Here we demonstrate a chemical method which achieves dimensionality selection via preferential inhibition of the magnetic exchange in an $S=1/2$ antiferromagnet along one crystal direction, switching the system from being quasi-two- to quasi-one-dimensional while effectively maintaining the nearest-neighbour coupling strength.

cond-mat.str-el↗

Field-induced length changes in the spin-liquid candidate $κ$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$

Measurements of the coefficient of thermal expansion on the spin-liquid candidate $κ$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ have revealed distinct and strongly anisotropic lattice effects around 6 K - a possible spin-liquid instability. In order to study the effects of a magnetic field on the low-temperature spin-liquid state, dilatometric measurements have been conducted both as a function of temperature at \emph{B} = const. and as a function of field at \emph{T} = const. While the 6 K anomaly is found to be insensitive to magnetic fields \emph{B} $\leq$ 10 T, the maximum field applied, surprisingly strong \emph{B}-induced effects are observed for magnetic fields applied along the in-plane \emph{b}-axis. Above a threshold field of 0.5 T < \emph{B}$_c$ $\leq$ 1 T, a jump-like anomaly is observed in the \emph{b}-axis lattice parameter. This anomaly, which is located at 8.7 K at \emph{B} = 1 T, grows in size and shifts to lower temperatures with increasing the magnetic field. Although the anomaly bears resemblance to a first-order phase transition, the lack of hysteresis suggests otherwise.

cond-mat.str-el↗

Temperature dependence of structural and electronic properties of the spin-liquid candidate kappa-(BEDT-TTF)2Cu2(CN)3

We investigate the effect that the temperature dependence of the crystal structure of a two dimensional organic charge-transfer salt has on the low-energy Hamiltonian representation of the electronic structure. For that, we determine the crystal structure of kappa-(BEDT-TTF)2Cu2(CN)3 for a series of temperatures between T=5 K and 300 K by single crystal X-ray diffraction and analyze the evolution of the electronic structure with temperature by using density functional theory and tight binding methods. We find a considerable temperature dependence of the corresponding triangular lattice Hubbard Hamiltonian parameters. We conclude that even in the absence of change of symmetry, the temperature dependence of quantities like frustration and interaction strength can be significant and should be taken into account.

cond-mat.str-el↗

Magnetic order in quasi-two-dimensional molecular magnets investigated with muon-spin relaxation

We present the results of a muon-spin relaxation (muSR) investigation into magnetic ordering in several families of layered quasi-two-dimensional molecular antiferromagnets based on transition metal ions such as S=1/2 Cu2+ bridged with organic ligands such as pyrazine. In many of these materials magnetic ordering is difficult to detect with conventional magnetic probes. In contrast, muSR allows us to identify ordering temperatures and study the critical behavior close to T_N . Combining this with measurements of in-plane magnetic exchange J and predictions from quantum Monte Carlo simulations we may assess the degree of isolation of the 2D layers through estimates of the effective inter-layer exchange coupling and in-layer correlation lengths at T_N . We also identify the likely metal-ion moment sizes and muon stopping sites in these materials, based on probabilistic analysis of the magnetic structures and of muon-fluorine dipole-dipole coupling in fluorinated materials.

cond-mat.str-el↗

Low-frequency charge-carrier dynamics in the vicinity of the Mott transition in quasi-two-dimensional organic superconductors $κ$-(BEDT-TTF)${}_{2}$X

We investigate the dynamics of correlated charge carriers in the vicinity of the Mott metal-to-insulator transition in various of the title quasi-two-dimensional organic charge-transfer salts by means of fluctuation (noise) spectroscopy. The observed $1/f$-type fluctuations are quantitatively very well described by a phenomenological model based on the concept of non-exponetial kinetics. The main result is a correlation-induced enhancement of the fluctuations accompanied by a substantial shift of spectral weight to low frequencies close to the Mott critical endpoint. This sudden slowing down of the electron dynamics may be a universal feature of metal-to-insulator transitons. For the less correlated metallic materials, we find a crossover/transition from hopping transport of more-or-less localized carriers at elevated temperatures to a low-temperature regime, where a metallic coupling of the layers allows for coherent interlayer transport of delocalized electrons.

cond-mat.str-el↗

Magnetoelastic Coupling in the Phase Diagram of Ba1-xKxFe2As2

We report a high resolution neutron diffraction investigation of the coupling of structural and magnetic transitions in Ba1xKxFe2As2. The tetragonal-orthorhombic and antiferromagnetic transitions are suppressed with potassium-doping, falling to zero at x <~ 0.3. However, unlike Ba(Fe1xCox)2As2, the two transitions are first-order and coincident over the entire phase diagram, with a biquadratic coupling of the two order parameters. The phase diagram is refined showing that the onset of superconductivity is at x = 0.133 with all three phases coexisting until x >~ 0.24.

cond-mat.supr-con↗

Energy scales for electronic noise processes in the quasi-two-dimensional organic Mott system $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl

Resistance noise spectroscopy is applied to bulk single crystals of the quasi-two-dimensional organic Mott insulator $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl both under moderate pressure and at ambient-pressure conditions. When pressurized, the system can be shifted to the inhomogeneous coexistence region of antiferromagnetic insulating and superconducting phases, where percolation effects dominate the electronic fluctuations [J. Müller {\it et al.}, Phys. Rev. Lett. {\bf 102}, 047004 (2009)]. Independent of the pressure conditions, at higher temperatures we observe generic $1/f^α$-type spectra. The magnitude of the electronic noise is extremely enhanced compared to typical values of homogeneous semiconductors or metals. This indicates that a highly inhomogeneous current distribution may be an intrinsic property of organic charge-transfer salts. The temperature dependence of the nearly $1/f$ spectra can be very well described by a generalized random fluctuation model [Dutta, Dimon, and Horn, Phys. Rev.\ Lett. {\bf 43}, 646 (1979)]. We find that the number of fluctuators and/or their coupling to the electrical resistance depends on the temperature, which possibly relates to the electronic scattering mechanisms determining the electrical resistance. The phenomenological model explains a pronounced peak structure in the low-frequency noise at around 100 K, which is not observed in the resistivity itself, in terms of the thermally-activated conformational degrees of freedom of the ET molecules' ethylene endgroups.

cond-mat.supr-con↗

Different superconducting percolation regimes in the layered organic Mott system $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl -- evidence from fluctuation spectroscopy

Fluctuation spectroscopy is used to investigate the organic bandwidth-controlled Mott system $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl. We find evidence for percolative-type superconductivity in the spatially inhomogeneous coexistence region of antiferromagnetic insulating and superconducting states which develops under pressure at low temperatures. When the superconducting transition is driven by a magnetic field, percolation seems to be dominated by unstable superconducting clusters upon approaching $T_c (B)$ from above, before a "classical" type of percolation is resumed at low fields, dominated by the fractional change of superconducting clusters. The $1/f$ noise is resolved into Lorentzian spectra in the crossover region where the action of an individual mesoscopic fluctuator is enhanced.

cond-mat.str-el↗

Dissipation in the superconducting state of kappa-(BEDT-TTF)2Cu(NCS)2

We have studied the interlayer resistivity of the prototypical quasi-two-dimensional organic superconductor $κ$-(BEDT-TTF)$_2$Cu(NCS)$_2$ as a function of temperature, current and magnetic field, within the superconducting state. We find a region of non-zero resistivity whose properties are strongly dependent on magnetic field and current density. There is a crossover to non-Ohmic conduction below a temperature that coincides with the 2D vortex solid -- vortex liquid transition. We interpret the behaviour in terms of a model of current- and thermally-driven phase slips caused by the diffusive motion of the pancake vortices which are weakly-coupled in adjacent layers, giving rise to a finite interlayer resistance.

cond-mat.supr-con↗

Can a single molecule trap the electron?

We suggest that it might be possible to trap the electron in a cavity of a macrocycle molecule, in the same way this trapping occurs cooperatively, by several solvent molecules, in hydroxylic liquids. Such an encapsulated electron is a "molecular capacitor," in which the excess electron is largely decoupled from valence electrons in the trap. A specific design for such a trap that is based on calix[4]cyclohexanol is discussed in detail. It is shown theoretically, by ab initio and density functional theory (DFT) modeling, that one of the conformations of this molecule forms the optimum tetrahedral trap for the electron. The resulting "encapsulated electron" strikingly resembles the solvated electron in alcohols and water.

physics.chem-ph↗

Comparison of the normal state properties of $κ$-(BEDT-TTF)$_2$Cu(NCS)$_2$ and its deuterated analogue in high magnetic fields and under high hydrostatic pressures

Details of the Fermi-surface topology of deuterated $κ$-(BEDT-TTF)$_2$Cu(NCS)$_2$ ~have been measured as a function of pressure, and compared with equivalent measurements of the undeuterated salt. We find that the superconducting transition temperature is much more dramatically suppressed by increasing pressure in the deuterated salt. It is suggested that this is linked to pressure-induced changes in the Fermi-surface topology, which occur more rapidly in the deuterated salt than in the undeuterated salt as the pressure is raised. Our data suggest that the negative isotope effect observed on deuteration is due to small differences in Fermi-surface topology caused by the isotopic substitution.

cond-mat.str-el↗

Millimeter-Wave Spectroscopy of the Organic spin-Peierls System b'-(ET)2SF5CF2SO3

The first purely organic BEDT-TTF spin-Peierls system, b'-(ET)2SF5CF2SO3, has been confirmed using a high-frequency electron spin resonance (EPR) cavity perturbation technique. The material exhibits the characteristics of a quasi-one-dimensional (1D) Heisenberg antiferromagnetic spin system above 30 K, but undergoes a second-order transition, at TSP = 33 K, to a singlet ground state, due to a progressive spin-lattice dimerization. The spin-Peierls state is evidenced by a sharp drop in the spin susceptibility below 24 K for the magnetic field parallel to each of the three principle axes (i.e. H7a, H7b, and H7c). The 1D chain axis has been identified as the crystallographic b axis from the g value analysis. The singlet-triplet gap, Ds(0) = 114 (+-21)K, was determined using a modified BCS theory. Also, we describe in some detail the millimeter-wave vector network analyzer (MVNA) for researchers who have interest in precision EPR measurements at higher magnetic fields and frequencies.

cond-mat.mtrl-sci↗