The specific features of phononic and magnetic subsystems of type-VII clathrate EuNi2P4.

A type-VII clathrate with a Eu2+ guest embedded into a Ni-P covalent framework, EuNi2P4, was synthesized by a standard two-stage ampoule synthesis and confirmed to crystallize in the orthorhombic space group Fddd with unit cell parameters a = 5.1829(1) Å, b = 9.4765(1) Å, and c = 18.9900(1) Å. A general technique for studying the lattice and magnetic properties of REE containing compounds is proposed. The temperature and field dependences of electrical resistivity ρ(T,H), magnetization M(T,H), magnetic susceptibility χ(T,H), heat capacity Cp(T), and unit cell parameters a(T), b(T), c(T), and volume V(T) were experimentally studied and analyzed at different pressures in the temperature range of 2-300 K. A cascade of anomalies in the studied dependences was identified and attributed to the magnetic phase transformation and peculiar lattice contributions at temperatures below 20 K. As a result of comparison with an isostructural clathrate SrNi2P4, the parameters of the magnetic and lattice contributions were determined. It is characteristic that the phase transition from the paramagnetic to the magnetically ordered state is not reflected in the temperature changes of the lattice parameters due to weak bonds between guest europium atoms and the Ni-P host matrix. We have constructed a tentative H-T phase diagram based on the M(T) and M(H) data, which includes 6 different phases. It is established that the anomalous lattice contribution to the clathrate heat capacity CTLS(T) appears due to the effect of two-level systems (TLS) in the Eu2+ subsystem on the thermodynamic properties of EuNi2P4. The values of TLS parameters as well as the parameters of the magnetic subsystem of the clathrate were determined.

Thermodynamic properties and lattice dynamics investigation of LuB2C: experiment and ab initio calculations.

A sample of lutetium carboboride LuB2C was synthesized from a mixture of lutetium hydride, boron and carbon by annealing in argon. The temperature dependence of the heat capacity Cp(T) (2-300 K) and lattice parameters a(T), b(T), and c(T) (5-300 K) of the carboboride was experimentally determined. The experimental values of the heat capacity were fitted with the approximation Cp(T) = aT + ΣCD + CE + CTLS(T). Here the first term is the electronic contribution, the second is the sum of the Debye components, the third is the Einstein contribution, and the fourth is the contribution to the heat capacity due to the vibrations of the two-level systems which are formed in the Lu-subsystem due to the asymmetry of the B-C atomic arrangement around the Lu3+-ions and, as a consequence, the possible transition of the lutetium atoms between spatially close, but energetically non-equivalent positions. A strong anisotropy of the thermal expansion of the carboboride was revealed. Along the c axis the coefficient of thermal expansion monotonically increases; in the basal plane, the expansion is practically not observed. The temperature dependence of the unit cell volume Vu(T) has been analyzed in the Debye-Einstein approximation taking into account the electronic contribution and effect of two-level systems. The values of the Gruneisen parameters corresponding to different modes of the phonon spectrum of the carboboride have been determined. The frequencies of the lattice vibrations, determined in a Raman scattering experiment, are in satisfactory agreement with the parameters obtained from Cp(T) using the Debye-Einstein approximation. Using ab initio band theory methods and an exchange-correlation functional in the PBE form in the VASP package, it was established that the total energies of these two crystal structures differ by no more than 0.01 eV f.u.-1. Calculations of the thermodynamic properties of LuB2C yielded similar results for orthorhombic and tetragonal phases of the carboboride.

Nonequilibrium Pair Breaking in Ba(Fe_{1-x}Co_{x})_{2}As_{2} Superconductors: Evidence for Formation of a Photoinduced Excitonic State.

Ultrafast terahertz (THz) pump-probe spectroscopy reveals an unusual out-of-equilibrium Cooper pair nonlinear dynamics and a nonequilibrium state driven by femtosecond (fs) photoexcitation of superconductivity (SC) in iron pnictides. Following fast SC quench via hot-phonon scattering, a second, abnormally slow (many hundreds of picoseconds), SC quench regime is observed prior to any recovery. Importantly, a nonlinear pump fluence dependence is identified for this remarkably long prebottleneck dynamics that are sensitive to both doping and temperature. Using quantum kinetic modeling we argue that the buildup of excitonic interpocket correlation between electron-hole (e-h) quasiparticles (QP) quenches SC after fs photoexcitation leading to a long-lived, many-QP excitonic state.

Hedgehog Spin-Vortex Crystal Antiferromagnetic Quantum Criticality in CaK(Fe_{1-x}Ni_{x})_{4}As_{4} Revealed by NMR.

Two ordering states, antiferromagnetism and nematicity, have been observed in most iron-based superconductors (SCs). In contrast to those SCs, the newly discovered SC CaK(Fe_{1-x}Ni_{x})_{4}As_{4} exhibits an antiferromagnetic (AFM) state, called hedgehog spin-vortex crystal (SVC) structure, without nematic order, providing the opportunity for the investigation into the relationship between spin fluctuations and SC without any effects of nematic fluctuations. Our ^{75}As nuclear magnetic resonance studies on CaK(Fe_{1-x}Ni_{x})_{4}As_{4} (0≤x≤0.049) revealed that CaKFe_{4}As_{4} is located close to a hidden hedgehog SVC AFM quantum-critical point (QCP). The magnetic QCP without nematicity in CaK(Fe_{1-x}Ni_{x})_{4}As_{4} highlights the close connection of spin fluctuations and superconductivity in iron-based SCs. The advantage of stoichiometric composition also makes CaKFe_{4}As_{4} an ideal platform for further detailed investigation of the relationship between magnetic QCP and superconductivity in iron-based SCs without disorder effects.

Effect of Biaxial Strain on the Phase Transitions of Ca(Fe_{1-x}Co_{x})_{2}As_{2}.

We study the effect of applied strain as a physical control parameter for the phase transitions of Ca(Fe_{1-x}Co_{x})_{2}As_{2} using resistivity, magnetization, x-ray diffraction, and ^{57}Fe Mössbauer spectroscopy. Biaxial strain, namely, compression of the basal plane of the tetragonal unit cell, is created through firm bonding of samples to a rigid substrate via differential thermal expansion. This strain is shown to induce a magnetostructural phase transition in originally paramagnetic samples, and superconductivity in previously nonsuperconducting ones. The magnetostructural transition is gradual as a consequence of using strain instead of pressure or stress as a tuning parameter.

Origin of the Resistivity Anisotropy in the Nematic Phase of FeSe.

The in-plane resistivity anisotropy is studied in strain-detwinned single crystals of FeSe. In contrast to other iron-based superconductors, FeSe does not develop long-range magnetic order below the tetragonal-to-orthorhombic transition at T_{s}≈90 K. This allows for the disentanglement of the contributions to the resistivity anisotropy due to nematic and magnetic orders. Comparing direct transport and elastoresistivity measurements, we extract the intrinsic resistivity anisotropy of strain-free samples. The anisotropy peaks slightly below T_{s} and decreases to nearly zero on cooling down to the superconducting transition. This behavior is consistent with a scenario in which the in-plane resistivity anisotropy is dominated by inelastic scattering by anisotropic spin fluctuations.

Enhancement of the Superconducting Gap by Nesting in CaKFe_{4}As_{4}: A New High Temperature Superconductor.

We use high resolution angle resolved photoemission spectroscopy and density functional theory with measured crystal structure parameters to study the electronic properties of CaKFe_{4}As_{4}. In contrast to the related CaFe_{2}As_{2} compounds, CaKFe_{4}As_{4} has a high T_{c} of 35 K at stochiometric composition. This presents a unique opportunity to study the properties of high temperature superconductivity in the iron arsenides in the absence of doping or substitution. The Fermi surface consists of several hole and electron pockets that have a range of diameters. We find that the values of the superconducting gap are nearly isotropic (within the explored portions of the Brillouin zone), but are significantly different for each of the Fermi surface (FS) sheets. Most importantly, we find that the momentum dependence of the gap magnitude plotted across the entire Brillouin zone displays a strong deviation from the simple cos(k_{x})cos(k_{y}) functional form of the gap function, proposed by the scenario of Cooper pairing driven by a short range antiferromagnetic exchange interaction. Instead, the maximum value of the gap is observed on FS sheets that are closest to the ideal nesting condition, in contrast to previous observations in other ferropnictides. These results provide strong support for the multiband character of superconductivity in CaKFe_{4}As_{4}, in which Cooper pairing forms on the electron and the hole bands interacting via a dominant interband repulsive interaction, enhanced by band nesting.

Competing Magnetic Fluctuations in Iron Pnictide Superconductors: Role of Ferromagnetic Spin Correlations Revealed by NMR.

In the iron pnictide superconductors, theoretical calculations have consistently shown enhancements of the static magnetic susceptibility at both the stripe-type antiferromagnetic and in-plane ferromagnetic (FM) wave vectors. However, the possible existence of FM fluctuations has not yet been examined from a microscopic point of view. Here, using ^{75}As NMR data, we provide clear evidence for the existence of FM spin correlations in both the hole- and electron-doped BaFe_{2}As_{2} families of iron-pnictide superconductors. These FM fluctuations appear to compete with superconductivity and are thus a crucial ingredient to understanding the variability of T_{c} and the shape of the superconducting dome in these and other iron-pnictide families.

Remarkably Robust and Correlated Coherence and Antiferromagnetism in (Ce(1-x)La(x))Cu2Ge2.

We present magnetic susceptibility, resistivity, specific heat, and thermoelectric power measurements on (Ce(1-x)La(x))Cu2Ge2 single crystals (0≤x≤1). With La substitution, the antiferromagnetic temperature TN is suppressed in an almost linear fashion and moves below 0.36 K, the base temperature of our measurements for x>0.8. Surprisingly, in addition to robust antiferromagnetism, the system also shows low temperature coherent scattering below Tcoh up to ∼0.9 of La, indicating a small percolation limit ∼9% of Ce. Tcoh as a function of magnetic field was found to have different behavior for x<0.9 and x>0.9. Remarkably, (Tcoh)(2) at H=0 was found to be linearly proportional to TN. The jump in the magnetic specific heat δCm at TN as a function of TK/TN for (Ce(1-x)La(x))Cu2Ge2 follows the theoretical prediction based on the molecular field calculation for the S=1/2 resonant level model.

Measurements of nematic susceptibility with phase sensitive nuclear magnetic resonance in pulsed strain fields.

We present nuclear magnetic resonance data in BaFe2As2 in the presence of pulsed strain fields that are interleaved in time with the radio frequency excitation pulses. In this approach, the preceding nuclear magnetization acquires a phase shift that is proportional to the strain and pulse time. The sensitivity of this approach is limited by the homogeneous decoherence time, T2, rather than the inhomogeneous linewidth. We measure the nematic susceptibility as a function of temperature and demonstrate a three orders of magnitude improvement in sensitivity. This approach will enable studies of the strain response in a broad range of materials that previously were inaccessible due to inhomogeneous broadening.

Semi-classical origin of the extreme magnetoresistance in PtSn4.

The so-called "extreme magnetoresistance" (XMR) found in few conductors poses interesting conceptual challenges which address needs in technology. In contrast to the more common XMR in semi-metals, PtSn4 stands out as a rare example of a high carrier density multi-band metal exhibiting XMR, sparking an active debate about its microscopic origin. Here we report a sharp sensitivity of its XMR upon the field angle, with an almost complete collapse only for one specific current and field direction (B//b, I//a). Corroborated by band-structure calculations, we identify a singular open orbit on one of its Fermi surface sheets as the origin of this collapse. This remarkably switchable XMR resolves the puzzle in PtSn4 as a semi-classical effect of an ultra-pure, compensated carrier metal. It further showcases the importance of Ockham's razor in uncommon magnetotransport phenomena and demonstrates the remarkable physical properties conventional metals can exhibit given they are superbly clean.

Anomalous reduction of the Lorenz ratio at the quantum critical point in YbAgGe.

We report measurements of the electrical and thermal transport on the hexagonal heavy-fermion metal YbAgGe for temperatures T ≥ 40 mK and in magnetic fields H∥ab up to 14 T. This distorted kagome-lattice system displays a series of magnetic states and a quantum critical point at H(c) = 4.5 T. The Lorenz ratio L(T)/L0 displays a marked reduction only close to H(c). A T-linear contribution below 120 mK, present at all different fields, allows us to extrapolate the Lorenz ratio towards T = 0. At the critical field this yields L/L0 = 0.92±0.03, suggesting a violation of the Wiedemann-Franz law due to strong inelastic scattering.

Quantum bicriticality in the heavy-fermion metamagnet YbAgGe.

Bicritical points, at which two distinct symmetry-broken phases become simultaneously unstable, are typical for spin-flop metamagnetism. Interestingly, the heavy-fermion compound YbAgGe also possesses such a bicritical point (BCP) with a low temperature T(BCP)≈0.3 K at a magnetic field of µH(BCP)≈4.5 T. In its vicinity, YbAgGe exhibits anomalous behavior that we attribute to the influence of a quantum bicritical point that is close in parameter space yet can be reached by tuning T(BCP) further to zero. Using high-resolution measurements of the magnetocaloric effect, we demonstrate that the magnetic Grüneisen parameter ΓH indeed both changes sign and diverges as required for quantum criticality. Moreover, ΓH displays a characteristic scaling behavior but only on the low-field side H≲H(BCP), indicating a pronounced asymmetry with respect to the critical field. We speculate that the small value of T(BCP) is related to the geometric frustration of the Kondo lattice of YbAgGe.

Unusual temperature dependence of band dispersion in Ba(Fe(1-x)Ru(x))2As2 and its consequences for antiferromagnetic ordering.

We have performed detailed studies of the temperature evolution of the electronic structure in Ba(Fe(1-x)Ru(x))(2)As(2) using angle resolved photoemission spectroscopy. Surprisingly, we find that the binding energy of both hole and electron bands changes significantly with temperature in both pure and Ru substituted samples. The hole and electron pockets are well nested at low temperature in unsubstituted (BaFe(2)As(2)) samples, which likely drives the spin density wave and resulting antiferromagnetic order. Upon warming, this nesting is degraded as the hole pocket shrinks and the electron pocket expands. Our results demonstrate that the temperature dependent nesting may play an important role in driving the antiferromagnetic-paramagnetic phase transition.

Magnonlike dispersion of spin resonance in Ni-doped BaFe2As2.

Inelastic neutron scattering measurements on Ba(Fe0.963Ni0.037)2As2 manifest a neutron spin resonance in the superconducting state with anisotropic dispersion within the Fe layer. Whereas the resonance is sharply peaked at the antiferromagnetic (AFM) wave vector Q(AFM) along the orthorhombic a axis, the resonance disperses upwards away from Q(AFM) along the b axis. In contrast to the downward dispersing resonance and hourglass shape of the spin excitations in superconducting cuprates, the resonance in electron-doped BaFe2As2 compounds possesses a magnonlike upwards dispersion.

Coexistence of cluster spin glass and superconductivity in Ba(Fe(1-x)Co(x))2As2 for 0.060≤x≤0.071.

We present 75As nuclear magnetic resonance data from measurements of a series of Ba(Fe(1-x)Co(x))2As2 crystals with 0.00≤x≤0.075 that reveals the coexistence of frozen antiferromagnetic domains and superconductivity for 0.060≤x≤0.071. Although bulk probes reveal no long range antiferromagnetic order beyond x=0.06, we find that the local spin dynamics reveal no qualitative change across this transition. The characteristic domain sizes vary by more than an order of magnitude, reaching a maximum variation at x=0.06. This inhomogeneous glassy dynamics may be an intrinsic response to the competition between superconductivity and antiferromagnetism in this system.

Inelastic neutron scattering study of a nonmagnetic collapsed tetragonal phase in nonsuperconducting CaFe2As2: evidence of the impact of spin fluctuations on superconductivity in the iron-arsenide compounds.

The relationship between antiferromagnetic spin fluctuations and superconductivity has become a central topic of research in studies of superconductivity in the iron pnictides. We present unambiguous evidence of the absence of magnetic fluctuations in the nonsuperconducting collapsed tetragonal phase of CaFe2As2 via inelastic neutron scattering time-of-flight data, which is consistent with the view that spin fluctuations are a necessary ingredient for unconventional superconductivity in the iron pnictides. We demonstrate that the collapsed tetragonal phase of CaFe2As2 is nonmagnetic, and discuss this result in light of recent reports of high-temperature superconductivity in the collapsed tetragonal phase of closely related compounds.

Antiferromagnetic order and its interplay with superconductivity in CaK(Fe1-xMnx)4As4.

The magnetic order for several compositions of CaK(Fe1-xMnx)4As4has been studied by nuclear magnetic resonance (NMR), Mössbauer spectroscopy, and neutron diffraction. Our observations for the Mn-doped 1144 compound are consistent with the hedgehog spin vortex crystal (hSVC) order which has previously been found for Ni-dopedCaKFe4As4. The hSVC state is characterized by the stripe-type propagation vectors(π0)and(0π)just as in the doped 122 compounds. The hSVC state preserves tetragonal symmetry at the Fe site, and only this SVC motif with simple antiferromagnetic (AFM) stacking alongcis consistent with all our observations using NMR Mössbauer spectroscopy, and neutron diffraction. We find that the hSVC state in the Mn-doped 1144 compound coexists with superconductivity, and by combining the neutron scattering and Mössbauer spectroscopy data we can infer a quantum phase transition, hidden under the superconducting dome, associated with the suppression of the AFM transition temperature (TN) to zero forx ≈ 0.01. In addition, unlike several 122 compounds and Ni-doped 1144, the ordered magnetic moment is not observed to decrease at temperatures below the superconducting transition temperature (Tc).

Effects of transition metal substitutions on the incommensurability and spin fluctuations in BaFe2As2 by elastic and inelastic neutron scattering.

The spin fluctuation spectra from nonsuperconducting Cu-substituted, and superconducting Co-substituted, BaFe(2)As(2) are compared quantitatively by inelastic neutron scattering measurements and are found to be indistinguishable. Whereas diffraction studies show the appearance of incommensurate spin-density wave order in Co and Ni substituted samples, the magnetic phase diagram for Cu substitution does not display incommensurate order, demonstrating that simple electron counting based on rigid-band concepts is invalid. These results, supported by theoretical calculations, suggest that substitutional impurity effects in the Fe plane play a significant role in controlling magnetism and the appearance of superconductivity, with Cu distinguished by enhanced impurity scattering and split-band behavior.

Magnetic field screening in hydrogen-rich high-temperature superconductors.

In the last few years, the superconducting transition temperature, Tc, of hydrogen-rich compounds has increased dramatically, and is now approaching room temperature. However, the pressures at which these materials are stable exceed one million atmospheres and limit the number of available experimental studies. Superconductivity in hydrides has been primarily explored by electrical transport measurements, whereas magnetic properties, one of the most important characteristic of a superconductor, have not been satisfactory defined. Here, we develop SQUID magnetometry under extreme high-pressure conditions and report characteristic superconducting parameters for Im-3m-H3S and Fm-3m-LaH10-the representative members of two families of high-temperature superconducting hydrides. We determine a lower critical field Hc1 of ∼0.82 T and ∼0.55 T, and a London penetration depth λL of ∼20 nm and ∼30 nm in H3S and LaH10, respectively. The small values of λL indicate a high superfluid density in both hydrides. These compounds have the values of the Ginzburg-Landau parameter κ ∼12-20 and belong to the group of "moderate" type II superconductors, rather than being hard superconductors as would be intuitively expected from their high Tcs.