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Electronic nematicity, the breaking of the crystal lattice rotational symmetry by the electronic fluid, is a fascinating quantum state of matter. In this work, using electronic transport under strain we investigate the electronic nematicity of BaNi2(As1−xPx)2, a candidate system for charge-induced nematicity. We report a large B1g elastoresistance coefficient that is maximized at the tetragonal-to-orthorhombic transition temperature, that slightly precedes the first-order triclinic transition. An hysteretic behavior is observed in the resistance versus strain sweeps and interpreted as the pinning of orthorhombic domains. Remarkably, the elastoresistance only onsets together with a strong enhancement of the incommensurate charge density wave of the material, strongly suggesting that this electronic instability is uniaxial in nature and drive the orthorhombic transition. The absence of sizeable elastoresistance above this electronic phase clearly contrasts dynamic and static electronic nematicity. Finally, the elastoresistance temperature dependence that strongly differs from the Curie-Weiss form of iron-based superconductors reveals major differences for the respective coupling of electronic nematicity to the lattice. Our results uncover an extremely strain-sensitive platform to study electronic anisotropy induced by a charge-density-wave instability.

Among two-dimensional materials, Fe3GeTe2 has come to occupy a very important place owing to its ferromagnetic nature with one of the highest Curie temperatures among known van der Waals materials and the potential for hosting skyrmions. In this combined experimental and theoretical work, we investigate the magnetic bubble domains as well as the microscopic domain wall profile using spin-polarized scanning tunneling microscopy in combination with atomistic spin-dynamics simulations performed with parameters from density functional theory calculations. We find a weak magneto-electric effect influencing the domain wall width by the electric field in the tunneling junction and determine the critical magnetic field for the collapse of the bubble domains. Our findings shed light on the origins of complex magnetism that Fe3GeTe2 exhibits.

Single crystals of intermediate valent EuPd$_2$Si$_2$ were grown from an Eu-rich melt by the Bridgman as well as the Czochralski technique. The chemical and structural characterization of an extracted single crystalline Czochralski-grown specimen yielded a slight variation of the Si-Pd ratio along the growth direction and confirms the existence of a finite Eu(Pd$_{1-m}$Si$_m$)$_2$ homogeneity range. The thorough physical characterization carried out on the same crystal showed that this tiny variation in the composition strongly affects the temperature T$_v$ at which the valence transition occurs. These experiments demonstrate a strong coupling between structural and physical properties in the prototypical valence-fluctuating system EuPd$_2$Si$_2$ and explain the different reported values of T$_v$.

Strain is a powerful experimental tool to explore new electronic states and understand unconventional superconductivity. Here, we investigate the effect of uniaxial strain on the nematic and superconducting phase of single crystal FeSe using magnetotransport measurements. We find that the resistivity response to the strain is strongly temperature dependent and it correlates with the sign change in the Hall coefficient being driven by scattering, coupling with the lattice and multiband phenomena. Band structure calculations suggest that under strain the electron pockets develop a large in-plane anisotropy as compared with the hole pocket. Magnetotransport studies at low temperatures indicate that the mobility of the dominant carriers increases with tensile strain. Close to the critical temperature, all resistivity curves at constant strain cross in a single point, indicating a universal critical exponent linked to a strain-induced phase transition. Our results indicate that the superconducting state is enhanced under compressive strain and suppressed under tensile strain, in agreement with the trends observed in FeSe thin films and overdoped pnictides, whereas the nematic phase seems to be affected in the opposite way by the uniaxial strain. By comparing the enhanced superconductivity under strain of different systems, our results suggest that strain on its own cannot account for the enhanced high $T_c$ superconductivity of FeSe systems., Comment: 11 pages, 8 figures

We study the elastoresistance of the highly correlated material CsFe_{2}As_{2} in all symmetry channels. Neutralizing its thermal expansion by means of a piezoelectric-based strain cell is demonstrated to be essential. The elastoresistance response in the in-plane symmetric channel is found to be large, while the response in the symmetry-breaking channels is weaker and provides no evidence for a divergent nematic susceptibility. Rather, our results can be interpreted naturally within the framework of a coherence-incoherence crossover, where the low-temperature coherent state is sensitively tuned by the in-plane atomic distances.

The layered van der Waals ferromagnetic ${\mathrm{Fe}}_{3}{\mathrm{GeTe}}_{2}$ harbors an unconventional interplay between topology and magnetism, leading to a large anomalous Hall conductivity at low temperatures. Here, we investigate the temperature dependence of its charge dynamics and reveal that upon entering the ferromagnetic state at ${T}_{C}\ensuremath{\sim}200$ K and further lowering the temperature there is the onset of a gradual spectral weight reshuffling from the mid-infrared range towards far- as well as near-infrared frequencies. This twofold spectral weight transfer indicates the important role of the Hund's coupling as primary source for electronic correlations and signals an incoherent-coherent crossover at low temperatures. Our findings also convey the electronic environment, based on nodal-line topological states, favoring the large anomalous Hall conductivity.

By band engineering the iron chalcogenide Fe(Se,Te) via ab initio calculations, we search for topological surface states and realizations of Majorana bound states. Proposed topological states are expected to occur for nonstoichiometric compositions on a surface Dirac cone where issues like disorder scattering and charge transfer between relevant electronic states have to be addressed. However, this surface Dirac cone is well above the Fermi level. Our goal is to theoretically design a substituted crystal in which the surface Dirac cone is shifted toward the Fermi level by modifying the bulk material without disturbing the surface. Going beyond conventional density functional theory, we apply the Blackman, Esterling, and Berk coherent potential approximation in a mixed basis pseudopotential framework to scan the substitutional phase space of cosubstitutions on the Se sites. We have identified iodine as a promising candidate for intrinsic doping. Our specific proposal is that ${\mathrm{FeSe}}_{0.325}{\mathrm{I}}_{0.175}{\mathrm{Te}}_{0.5}$ is a very likely candidate to exhibit a Dirac cone right at the Fermi energy without inducing strong disorder scattering.

Authors acknowledge Diamond Light Source for time on beamline I05-ARPES under Proposal SI23890. L.C.R. acknowledges funding from the Royal Commission for the Exhibition of 1851. We measure the electronic structure of FeSe from within individual orthorhombic domains. Enabled by an angle-resolved photoemission spectroscopy beamline with a highly focused beam spot (nano-ARPES), we identify clear stripelike orthorhombic domains in FeSe with a length scale of approximately 1-5 μm. Our photoemission measurements of the Fermi surface and band structure within individual domains reveal a single electron pocket at the Brillouin zone corner. This result provides clear evidence for a one-electron-pocket electronic structure of FeSe, observed without the application of uniaxial strain, and calls for further theoretical insight into this unusual Fermi surface topology. Our results also showcase the potential of nano-ARPES for the study of correlated materials with local domain structures. Publisher PDF

We present a combined study from angle-resolved photoemission and density-functional-theory calculations of the temperature-dependent electronic structure in the excitonic insulator candidate Ta2NiSe5. Our experimental measurements unambiguously establish the normal state as a semimetal with a significant band overlap of >100 meV. Our temperature-dependent measurements indicate how these low-energy states hybridize when cooling through the well-known 327 K phase transition in this system. From our calculations and polarizationdependent photoemission measurements, we demonstrate the importance of a loss of mirror symmetry in enabling the band hybridization, driven by a shearlike structural distortion which reduces the crystal symmetry from orthorhombic to monoclinic. Our results thus point to the key role of the lattice distortion in enabling the phase transition of Ta2NiSe5.

FeSe is a unique superconductor that can be manipulated to enhance its superconductivity using different routes while its monolayer form grown on different substrates reaches a record high temperature for a two-dimensional system. In order to understand the role played by the substrate and the reduced dimensionality on superconductivity, we examine the superconducting properties of exfoliated FeSe thin flakes by reducing the thickness from bulk down towards 9 nm. Magnetotransport measurements performed in magnetic fields up to 16T and temperatures down to 2K help to build up complete superconducting phase diagrams of different thickness flakes. While the thick flakes resemble the bulk behaviour, by reducing the thickness the superconductivity of FeSe flakes is suppressed. In the thin limit we detect signatures of a crossover towards two-dimensional behaviour from the observation of the vortex-antivortex unbinding transition and strongly enhanced anisotropy. Our study provides detailed insights into the evolution of the superconducting properties from three-dimensional bulk behaviour towards the two-dimensional limit of FeSe in the absence of a dopant substrate., 18 pages, 13 figures

Magnetic skyrmions are two-dimensional magnetization swirls that stack in the form of tubes in the third dimension, and which are proposed as prospective information carriers for nonvolatile memory devices due to their unique topological properties. From resonant elastic x-ray scattering measurements on Cu2OSeO3 with an in-plane magnetic field we find that a state of perpendicularly ordered skyrmions forms - in stark contrast to the well-studied bulk state. The surface state is stable over a wide temperature range, unlike the bulk state in out-of-plane fields which is confined in a narrow region of the temperature-field phase diagram. In contrast to ordinary skyrmions found in the bulk, the surface state skyrmions result from the presence of magnetic interactions unique to the surface which stabilize them against external perturbations. The surface-guiding makes the robust state particular interesting for racetrack-like devices, ultimately allowing for much higher storage densities due to the smaller lateral footprint of the perpendicular skyrmions.

Understanding superconductivity requires detailed knowledge of the normal electronic state from which it emerges. A nematic electronic state that breaks the rotational symmetry of the lattice can potentially promote unique scattering relevant for superconductivity. Here, we investigate the normal transport of superconducting FeSe$_{1-x}$S$_x$ across a nematic phase transition using high magnetic fields up to 69 T to establish the temperature and field-dependencies. We find that the nematic state is an anomalous non-Fermi liquid, dominated by a linear resistivity at low temperatures that can transform into a Fermi liquid, depending on the composition $x$ and the impurity level. Near the nematic end point, we find an extended temperature regime with $T^{1.5}$ resistivity. The transverse magnetoresistance inside the nematic phase has as a $H^{1.55}$ dependence over a large magnetic field range and it displays an unusual peak at low temperatures inside the nematic phase. Our study reveals anomalous transport inside the nematic phase, driven by the subtle interplay between the changes in the electronic structure of a multi-band system and the unusual scattering processes affected by large magnetic fields and disorder, Comment: 18 pages, 14 figures

The full H-T phase diagram in the nematic superconductor FeSe is mapped out using specific-heat and thermal-expansion measurements down to 0.7 K and up to 30 T for both field directions. A clear thermodynamic signal of an underlying vortex-melting transition is found in both datasets and could be followed down to low temperatures. The existence of significant Gaussian thermal superconducting fluctuations is demonstrated by a scaling analysis, which also yields the mean-field upper critical field Hc2(T). For both field orientations, Hc2(T) shows Pauli-limiting behavior. Whereas the temperature dependence of the vortex-melting line is well described by the model of Houghton et al., Phys. Rev. B 40, 6763 (1989) down to the lowest temperatures for H $\perp$ FeSe layers, the vortex-melting line exhibits an unusual behavior for fields parallel to the planes, where the Pauli limitation is much stronger. Here, the vortex-melting anomaly is only observed down to T*= 2-3 K, and then merges with the Hc2(T) line as predicted by Adachi and Ikeda, Phys. Rev. B 68 184510 (2003). Below T*, Hc2(T) also exhibits a slight upturn possibly related to the occurence of a Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state., 7 figures, 11 pages

The nematic electronic state and its associated critical fluctuations have emerged as a potential candidate for the superconducting pairing in various unconventional superconductors. However, in most materials their coexistence with magnetically ordered phases poses a significant challenge in determining their importance. Here, by combining chemical and hydrostatic physical pressure in FeSe0.89S0.11, we access a nematic quantum phase transition isolated from any other competing magnetic phases. From quantum oscillations in high magnetic fields, we trace the evolution of the Fermi surface and electronic correlations as a function of applied pressure and detect a Lifshitz transition that separates two distinct superconducting regions. One emerges from the nematic phase with a small Fermi surface and strong electronic correlations, while the other one has a large Fermi surface and weak correlations that promotes nesting and stabilization of a magnetically ordered phase at high pressures. The absence of mass divergence at the nematic quantum phase transition suggests that the nematic fluctuations could be quenched by the strong coupling to the lattice or local strain effects. A direct consequence is the weakening of superconductivity at the nematic quantum phase transition in the absence of magnetically driven fluctuations.

We report on the lattice and spin dynamics in monopnictide CrAs using polarized Raman scattering. This system exhibits a first-order magnetostructural phase transition at ${T}_{N}\ensuremath{\sim}265\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, below which the magnetic moments of Cr form an incommensurate double helical magnetic structure while the unit-cell volume abruptly expands. Across the transition, the frequencies of the fully symmetric ${A}_{g}$ phonons strongly renormalize, which along with the results of first-principles calculations suggests the presence of a sizeable coupling of the phonons to the magnetic degrees of freedom in this compound. In addition, we observe two broad modes at around 350 and $1700\phantom{\rule{0.16em}{0ex}}\mathrm{c}{\mathrm{m}}^{\ensuremath{-}1}$ in the magnetic phase, which we associate with two-magnon Raman scattering. This work provides one of the few examples of magnetic Raman scattering from a noncollinear magnet.

Superconductivity in FeSe has recently attracted a great deal of attention because it emerges out of an electronic nematic state of elusive character. Here we study both the electronic normal state and the superconducting gap structure using heat-capacity measurements on high-quality single crystals. The specific-heat curve, from 0.4 K to ${T}_{c}=9.1\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, is found to be consistent with a recent gap determination using Bogoliubov quasiparticle interference [P. O. Sprau et al., Science 357, 75 (2017)]; however, only if nodes are introduced on either the electron or the hole Fermi-surface sheets. Our analysis, which is consistent with quantum-oscillation measurements, relies on the presence of one hole and one electron band only, and thus the fate of the theoretically predicted second electron pocket remains mysterious.

We report an Fe $L$-edge resonant inelastic x-ray scattering (RIXS) study of the unusual superconductor $\ensuremath{\beta}$-FeSe. The high-energy resolution of this RIXS experiment ($\ensuremath{\approx}55\phantom{\rule{3.33333pt}{0ex}}\mathrm{meV}$ FWHM) made it possible to resolve low-energy excitations of the Fe $3d$ manifold. These include a broad peak which shows dispersive trends between 100 and 200 meV along the $(\ensuremath{\pi},0)$ and $(\ensuremath{\pi},\ensuremath{\pi})$ directions of the one-Fe square reciprocal lattice, and which can be attributed to paramagnon excitations. The multiband valence state of FeSe is among the most metallic in which such excitations have been discerned by soft x-ray RIXS.

We use high-resolution angle-resolved photoemission spectroscopy to map the three-dimensional momentum dependence of the superconducting gap in FeSe. We find that on both the hole and electron Fermi surfaces, the magnitude of the gap follows the distribution of dyz orbital weight. Furthermore, we theoretically determine the momentum dependence of the superconducting gap by solving the linearized gap equation using a tight-binding model which quantitatively describes both the experimental band dispersions and orbital characters. By considering a Fermi surface only including one electron pocket, as observed spectroscopically, we obtain excellent agreement with the experimental gap structure. Our finding of a scaling between the superconducting gap and the dyz orbital weight supports the interpretation of superconductivity mediated by spin fluctuations in FeSe. Publisher PDF

Iron-based chalcogenides are complex superconducting systems in which orbitally-dependent electronic correlations play an important role. Here, using high-resolution angle-resolved photoemission spectroscopy, we investigate the effect of these electronic correlations outside the nematic phase in the tetragonal phase of superconducting FeSe1-xSx (x = 0; 0:18; 1). With increasing sulfur substitution, the Fermi velocities increase significantly and the band renormalizations are suppressed towards a factor of 1.5-2 for FeS. Furthermore, the chemical pressure leads to an increase in the size of the quasi-two dimensional Fermi surface, compared with that of FeSe, however, it remains smaller than the predicted one from first principle calculations for FeS. Our results show that the isoelectronic substitution is an effective way to tune electronic correlations in FeSe1-xSx, being weakened for FeS with a lower superconducting transition temperature. This suggests indirectly that electronic correlations could help to promote higher-Tc superconductivity in FeSe., 4 pages, 3 figures

Due to its highly tunable unconventional superconductivity, FeSe is one of the most intriguing materials among the iron-based superconductors. In addition, it exhibits a tetragonal to orthorhombic ``nematic'' phase transition in the absence of static magnetic order. This article presents a set of tight-binding parameters, optimized directly with respect to experimental angle-resolved photoemission spectroscopy (ARPES) data obtained at 100 K. It thus provides a quantitatively accurate model of the electronic structure of the tetragonal phase of FeSe and, hence, a coherent foundation for the understanding of the unique physical properties of this system. The authors go on to predict a feature that has so far remained unnoticed in simpler DFT-based tight-binding-model analyses, namely, a significant temperature dependence of the chemical potential in FeSe. This is confirmed by performing ARPES on FeSe single crystals, whereby a 25-meV rigid chemical potential shift is detected across the entire Brillouin zone over the temperature range between 100 K and 300 K. The finding has important implications for any future theoretical models of nematicity and superconductivity in FeSe and related materials.

We have accurately determined the exciton binding energy and reduced mass of single crystals of methylammonium lead tri-iodide using magneto-reflectivity at very high magnetic fields. The single crystal has excellent optical properties with a narrow line width of $\sim 3$meV for the excitonic transitions and a 2s transition which is clearly visible even at zero magnetic field. The exciton binding energy of $16 \pm 2$meV in the low temperature orthorhombic phase is almost identical to the value found in polycrystalline samples, crucially ruling out any possibility that the exciton binding energy depends on the grain size. In the room temperature tetragonal phase, an upper limit for the exciton binding energy of $12 \pm 4$ meV is estimated from the evolution of 1s-2s splitting at high magnetic field., 5 pages, 4 figures

We report a high-resolution laser-based angle-resolved photoemission spectroscopy (laser-ARPES) study of single crystals of FeSe, focusing on the temperature-dependence of the hole-like bands around the ${\rm \Gamma}$ point. As the system cools through the tetragonal-orthorhombic "nematic" structural transition at 90~K, the splitting of the $d_{xz}$/$d_{yz}$ bands is observed to increase by a magnitude of 13 meV. Moreover, the onset of a $\sim$10 meV downward shift of the $d_{xy}$ band is also at 90~K. These measurements provide clarity on the nature, magnitude and temperature-dependence of the band shifts at the ${\rm \Gamma}$ point in the nematic phase of FeSe.

Depending on the crystal growth conditions, an orthorhombic (O-type) or a tetragonal (T-type) structure can be found in the solid solution ${\rm Cs}_{2}{\rm CuCl}_{4-x}{\rm Br}_{x}~(0\leq x\leq 4)$ . Here, we present measurements of the temperature-dependent magnetic susceptibility and isothermal magnetization on the T-type compounds $x=1.6$ and 1.8 and compare these results with the magnetic properties recently derived for the O-type variant. The systems were found to exhibit quite dissimilar magnetic properties, which can be assigned to differences in the Cu coordination in these two structural variants. Whereas the tetragonal compounds can be classified as quasi-2-D ferromagnets, characterized by ferromagnetic layers with a weak antiferromagnetic interlayer coupling, the orthorhombic materials, notably the border compounds $x=0$ and 4, are model systems for frustrated 2-D Heisenberg antiferromagnets.

The presence of ${d}_{xz}\text{\ensuremath{-}}{d}_{yz}$ orbital ordering is often considered a hallmark of the nematic phase of Fe-based superconductors, including FeSe, but the details of the order parameter remain controversial. Here, we report a high-resolution angle-resolved photoemission spectroscopy study of single crystals of FeSe, accounting for the photon-energy dependence and making a detailed analysis of the temperature dependence. We find that the hole pocket undergoes a fourfold-symmetry-breaking distortion in the nematic phase below 90 K, but, in contrast, the changes to the electron pockets do not require fourfold symmetry breaking. Instead, there is an additional separation of the existing ${d}_{xy}$ and ${d}_{xz/yz}$ bands, which themselves are not split within resolution. These observations lead us to propose a scenario of ``unidirectional nematic bond ordering'' to describe the low-temperature electronic structure of FeSe, supported by good agreement with ten-orbital tight-binding model calculations.

We report a high-resolution angle-resolved photo-emission spectroscopy study of the evolution of the electronic structure of FeSe1-xSx single crystals. Isovalent S substitution onto the Se site constitutes a chemical pressure which subtly modifies the electronic structure of FeSe at high temperatures and induces a suppression of the tetragonal-symmetry-breaking structural transition temperature from 87K to 58K for x=0.15. With increasing S substitution, we find smaller splitting between bands with dyz and dxz orbital character and weaker anisotropic distortions of the low temperature Fermi surfaces. These effects evolve systematically as a function of both S substitution and temperature, providing strong evidence that an orbital ordering is the underlying order parameter of the structural transition in FeSe1-xSx. Finally, we detect the small inner hole pocket for x=0.12, which is pushed below the Fermi level in the orbitally-ordered low temperature Fermi surface of FeSe., Latex, 5 pages, 4 figures

The possibility for an appreciable many-body contribution to the electron-phonon interaction (EPI) in Fe-pnictides is discussed in the model where EPI is due to the electronic polarization of As- ions. The EPI-pol coupling ismuch larger than the one obtained in the LDA band structure calculations. It contributes significantly to the intra-band s-wave pairing and an appreciable positive As-isotope effect in the superconducting critical temperature is expected. In the Fe-breathing mode the linear (in the Fe-displacements) EPI-pol coupling vanishes, while the non-linear (quadratic) one is very strong. The part of the EPI-pol coupling, which is due to the "potential" energy (the Hubbard U) changes, is responsible for the giant magneto-elastic effects in MFe_{2}As_{2}, M=Ca, Sr, Ba since it gives much larger contribution to the magnetic pressure than the band structure effects do. This mechanism is contrary to the LDA prediction where the magneto-elastic effects are due to the "kinetic" energy effects, i.e. the changes in the density of states by the magneto-elastic effects. The proposed $EPI-pol is expected to be operative (and strong) in other Fe-based superconductors with electronically polarizable ions such as Se, Te, S etc., and in high-temperature superconductors due to the polarizability of the O-ions., 6 pages, 2 figures; new References are added, text improved, typos corrected

Muon spin rotation measurements have been performed on a powder sample ofα-RuCl3, a layered material in which Ru ions are arranged on a honeycomb lattice and which previously has been proposed to be close to a quantum spin liquid ground state. Our data reveal two distinct transitions at 11 and 14 K, which we interpret as originating from the onset of three-dimensional order and in-plane magnetic order, respectively. We identify, with the help of density functional theory calculations, likely muon stopping sites and combine these with dipolar field calculations to show that the two measured muon rotation frequencies are consistent with two inequivalent muon sites within a zigzag antiferromagnetic structure proposed previously.

Clathrates are candidate materials for thermoelectric applications because of a number of unique properties. The clathrate I phases in the Ba-Ni-Ge ternary system allow controlled variation of the charge carrier concentration by adjusting the Ni content. Depending on the Ni content, the physical properties vary from metal-like to insulator-like and show a transition from p-type to n-type conduction. Here we present first results on the characterization of millimeter-sized single crystals grown by the Bridgman technique. Single crystals with a composition of Ba8Ni3.5Ge42.1□0.4 show metallic behavior (dρ/dT > 0) albeit with high resistivity at room temperature [ρ (300 K) = 1 mΩ cm]. The charge carrier concentration at 300 K, as determined from Hall-effect measurements, is 2.3 e−/unit cell. The dimensionless thermoelectric figure of merit estimated at 680 K is ZT ≈ 0.2.

The layered honeycomb magnet $\ensuremath{\alpha}\ensuremath{-}{\mathrm{RuCl}}_{3}$ has been proposed as a candidate to realize a Kitaev spin model with strongly frustrated, bond-dependent, anisotropic interactions between spin-orbit entangled ${j}_{\mathrm{eff}}=\frac{1}{2}\phantom{\rule{4.pt}{0ex}}{\mathrm{Ru}}^{3+}$ magnetic moments. Here, we report a detailed study of the three-dimensional crystal structure using x-ray diffraction on untwinned crystals combined with structural relaxation calculations. We consider several models for the stacking of honeycomb layers and find evidence for a parent crystal structure with a monoclinic unit cell corresponding to a stacking of layers with a unidirectional in-plane offset, with occasional in-plane sliding stacking faults, in contrast with the currently assumed trigonal three-layer stacking periodicity. We report electronic band-structure calculations for the monoclinic structure, which find support for the applicability of the ${j}_{\mathrm{eff}}=\frac{1}{2}$ picture once spin-orbit coupling and electron correlations are included. Of the three nearest-neighbor Ru-Ru bonds that comprise the honeycomb lattice, the monoclinic structure makes the bond parallel to the $b$ axis nonequivalent to the other two, and we propose that the resulting differences in the magnitude of the anisotropic exchange along these bonds could provide a natural mechanism to explain the previously reported spin gap in powder inelastic neutron scattering measurements, in contrast to spin models based on the three-fold symmetric trigonal structure, which predict a gapless spectrum within linear spin wave theory. Our susceptibility measurements on both powders and stacked crystals, as well as magnetic neutron powder diffraction, show a single magnetic transition upon cooling below ${T}_{\mathrm{N}}\ensuremath{\approx}13$ K. The analysis of our neutron powder diffraction data provides evidence for zigzag magnetic order in the honeycomb layers with an antiferromagnetic stacking between layers. Magnetization measurements on stacked single crystals in pulsed field up to 60 T show a single transition around 8 T for in-plane fields followed by a gradual, asymptotic approach to magnetization saturation, as characteristic of strongly anisotropic exchange interactions.

Magnetoresistivity ${\ensuremath{\rho}}_{xx}$ and Hall resistivity ${\ensuremath{\rho}}_{xy}$ in ultrahigh magnetic fields up to 88 T are measured down to 0.15 K to clarify the multiband electronic structure in high-quality single crystals of superconducting FeSe. At low temperatures and high fields we observe quantum oscillations in both resistivity and the Hall effect, confirming the multiband Fermi surface with small volumes. We propose a novel approach to identify from magnetotransport measurements the sign of the charge carriers corresponding to a particular cyclotron orbit in a compensated metal. The observed significant differences in the relative amplitudes of the quantum oscillations between the ${\ensuremath{\rho}}_{xx}$ and ${\ensuremath{\rho}}_{xy}$ components, together with the positive sign of the high-field ${\ensuremath{\rho}}_{xy}$, reveal that the largest pocket should correspond to the hole band. The low-field magnetotransport data in the normal state suggest that, in addition to one hole and one almost compensated electron band, the orthorhombic phase of FeSe exhibits an additional tiny electron pocket with a high mobility.

The 5 K superconductor La2Sb shares some structural similarities with the iron-pnictides and -chalgogenides, especially the so-called 122-compounds, despite lacking a 3d-metal component. In order to look for similarities and dissimilarities of this layered metal pnictide with the higher-Tc Fe-based superconductors, we have performed a combined experimental and theoretical investigation of the effects of hydrostatic pressure. Magnetic measurements reveal a linear increase of Tc with pressure at a rate dTc/dP=(0.71±0.01)KGPa−1. Band structure calculations show that (i) the states at the Fermi level have predominantly La 5d character and (ii) that the density of states increases linearly with increasing pressure. By using these theoretical results and a BCS formalism, a quantitative description of the experimentally revealed pressure dependence of Tc is possible within a reasonable range of parameters. Our results indicate that La2Sb, despite its structural similarities to the 122 Fe-based superconductors, exhibits a BCS-type of superconductivity.

One of the key requirements for good thermoelectric materials is a low lattice thermal conductivity. Here we present a combined neutron scattering and theoretical investigation of the lattice dynamics in the type I clathrate system Ba-Ge-Ni, which fulfills this requirement. We observe a strong hybridization between phonons of the Ba guest atoms and acoustic phonons of the Ge-Ni host structure over a wide region of the Brillouin zone, which is in contrast with the frequently adopted picture of isolated Ba atoms in Ge-Ni host cages. It occurs without a strong decrease of the acoustic phonon lifetime, which contradicts the usual assumption of strong anharmonic phonon--phonon scattering processes. Within the framework of ab initio density-functional theory calculations we interpret these hybridizations as a series of anticrossings which act as a low-pass filter, preventing the propagation of acoustic phonons. To highlight the effect of such a phononic low-pass filter on the thermal transport, we compute the contribution of acoustic phonons to the thermal conductivity of Ba${}_{8}$Ge${}_{40}$Ni${}_{6}$ and compare it to those of pure Ge and a Ge${}_{46}$ empty-cage model system.

Starting from Cs2CuCl4 and Cs2CuBr4 our project focuses on the growth of the Cs2CuCl4-xBrx mixed crystals from aqueous solution and the investigation of the occurring structural variations. The well known orthorhombic structure (space group Pnma) of the end members of this system is interrupted within the intermediate composition range Cs2CuCl3Br1 - Cs2CuCl2Br2, if the growth takes place at room temperature. Within this range a new tetragonal phase is found (space group I4/mmm). However, in case the growth temperature will be increased to 50 {\deg}C, the existence of the orthorhombic structure can be extended over the whole Cs2CuCl4-xBrx mixed system. A detailed analysis of the composition dependence of the lattice parameters is used to draw conclusions on the incorporation of Cl- and Br-ions at different sites which is important for the magnetic interactions between the Cu-ions., Comment: 16 pages,8 figures

We report on synthesis, structural characterization, resistivity, magnetic and thermal expansion measurements on the as yet unexplored $\delta'$-phase of FeSe$_{1-x}$, here synthesized under ambient- (AP) and high-pressure (HP) conditions. We show that in contrast to $\beta$-FeSe$_{1-x}$, monophasic superconducting $\delta'$-FeSe$_{1-x}$ can be obtained in off-stoichiometric samples with excess Fe atoms preferentially residing in the van der Waals gap between the FeSe layers. The AP $\delta'$-FeSe$_{1-x}$ sample studied here ($T_c$ $\simeq$ 8.5\,K) possesses an unprecedented residual resistivity ratio RRR $\simeq$ 16. Thermal expansion data reveal a small feature around $\sim$90\,K, which resembles the anomaly observed at the structural and magnetic transitions for other Fe-based superconductors, suggesting that some kind of "magnetic state" is formed also in FeSe. %indicative of a fluctuating magnetic ordering. For HP samples (RRR $\simeq$ 3), the disorder within the FeSe layers is enhanced through the introduction of vacancies, the saturated magnetic moment of Fe is reduced and only spurious superconductivity is observed., Comment: 7 pages, 8 figures, published version

Single crystals of the type-I clathrate Ba(8)Ni(3.5)Ge(42.1)square(0.4) (space group Pm3n, no. 223, a = 10.798(2) A, l = 30 mm, slashed circle = 8 mm) were grown from the melt using the Bridgman technique. Their composition, determined by microprobe analysis, reveals a distinctly lower Ni content than previously reported for the lower limit (x = 5.4) of the homogeneity range of the clathrate-I phase Ba(8)Ni(x)Ge(46-x). From single crystal X-ray diffraction data we introduce a crystal structure model that takes point defects (vacancies) square in the Ge network into account. It reveals that both Ni and square accumulate at a single site (6c) and that, as a consequence, the Ge network distorts considerably. Ba(8)Ni(3.5)Ge(42.1)square(0.4) shows metal-like behaviour (drho/dT0) albeit with high resistivity at room temperature (rho(300 K) approximately 1 mOmega cm). Together with the low charge carrier concentration of 2.3 e(-)/unit cell at 300 K this is typical of a degenerate semiconductor. The lattice thermal conductivity is distinctly smaller than that of Ba(8)Ge(43)square(3), where the vacancies partially order, and smaller than those of Ba-Ni-Ge type-I clathrates without vacancies, suggesting that disordered vacancies efficiently scatter heat-transporting phonons. We provide evidence that the maximum value of the thermoelectric figure of merit reached in Ba(8)Ni(3.5)Ge(42.1)square(0.4), ZT(680 K) congruent with 0.21, can be further improved by adjusting the charge carrier concentration.

Single crystals of pyrochlore-type vanadates A2V 2O7 where A = Er, Y, and Dy have been successfully grown under high pressure and high temperature, using a multianvil technique. The temperature gradient method was applied for the crystal growth. The crystal structure of all three compounds has been determined from the Rietveld analysis of X-ray powder diffraction (XRD) data and confirmed a cubic pyrochlore structure in space group Fd3̄m (No. 227). The unit cell parameters were a = 9.9924(1), 10.01438(8), and 10.0372(3) Å for Er2V 2O7, Y2V2O7, and Dy 2V2O7, respectively. Their compositions were investigated by energy dispersive X-ray analysis. A single crystal of Dy 2V2O7 was characterized by a single-crystal XRD method. © 2008 American Chemical Society.

Y2V2O7 with pyrochlore structure has been synthesized under a high pressure of 5 GPa at 1200 °C. The crystal structure has been determined by Rietveld analysis of the X-ray diffraction data. The structure is cubic with a=10.0143(8) Å and can be described by the space group F d -3 m (no. 227). Scanning electron microscopy data suggest the efficiency of the grain growth method for single crystal growth of Y2V2O7 under high pressure and high temperature conditions. Magnetic susceptibility data conforming to the Curie-Weiss law in the range 150-300 K with an effective moment peff of 1.76μB/V4+ ion and θ=+68 K indicates the predominance of ferromagnetic interactions. © 2007 Elsevier B.V. All rights reserved.

We present a comprehensive study of the evolution of the nematic electronic structure of FeSe using high resolution angle-resolved photoemission spectroscopy (ARPES), quantum oscillations in the normal state and elastoresistance measurements. Our high resolution ARPES allows us to track the Fermi surface deformation from four-fold to two-fold symmetry across the structural transition at ~87 K which is stabilized as a result of the dramatic splitting of bands associated with dxz and dyz character. The low temperature Fermi surface is that a compensated metal consisting of one hole and two electron bands and is fully determined by combining the knowledge from ARPES and quantum oscillations. A manifestation of the nematic state is the significant increase in the nematic susceptibility as approaching the structural transition that we detect from our elastoresistance measurements on FeSe. The dramatic changes in electronic structure cannot be explained by the small lattice effects and, in the absence of magnetic fluctuations above the structural transition, points clearly towards an electronically driven transition in FeSe stabilized by orbital-charge ordering., Comment: Latex, 8 pages, 4 figures

In this work we explore the overall structural behaviour of the [(CH 3)2NH2][Mn(HCOO)3] multiferroic compound across the temperature range where its ferroelectric transition takes place by means of calorimetry, thermal expansion measurements and variable temperature powder and single crystal X-ray diffraction. The results clearly prove the presence of a structural phase transition at Tt ~ 187 K (the temperature at which the dielectric transition occurs) that involves a symmetry change from R3c to Cc, twinning of the crystals, a discontinuous variation of the unit cell parameters and unit cell volume, and a sharp first-order-like anomaly in the thermal expansion. In addition, the calorimetric results show a 3-fold order-disorder transition. The calculated pressure dependence of the transition temperature is rather large (dTt/dP = 4.6 ± 0.1 K kbar-1) in that it should be feasible to shift it to room temperature under adequate thermodynamic conditions, for instance by application of an external pressure. © 2014 the Partner Organisations.

We use angle-resolved photoemission spectroscopy (ARPES) to explore the electronic structure of single crystals of FeSe over a wide range of binding energies and study the effects of strong electron-electron correlations. We provide evidence for the existence of ``Hubbard-like bands'' at high binding energies consisting of incoherent many-body excitations originating from Fe $3d$ states in addition to the renormalized quasiparticle bands near the Fermi level. Many high-energy features of the observed ARPES data can be accounted for when incorporating the effects of strong local Coulomb interactions in calculations of the spectral function via dynamical mean-field theory, including the formation of a Hubbard-like band. This shows that over the energy scale of several eV, local correlations arising from the on-site Coulomb repulsion and Hund's coupling are essential for a proper understanding of the electronic structure of FeSe and other related iron-based superconductors.