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Destructive interference of electron hopping on the frustrated kagome lattice generates Dirac nodes, saddle points, and flat bands in the electronic structure. The latter provides the narrow bands and a peak in the density of states that can generate correlated electron behavior when the Fermi level lies within them. In the kagome metal CoSn, this alignment is not realized, and the compound is a Pauli paramagnet. Here we show that replacing part of the tin with indium (CoSn1-xInx) moves the Fermi energy into the flat band region, with support from band structure calculations, heat capacity measurements, and angle resolved photoemission spectroscopy. The associated instability results in the emergence of itinerant antiferromagnetism with a Neel temperature up to 30K. Long range magnetic order is confirmed by neutron diffraction measurements, which indicate an ordered magnetic moment of 0.1-0.2 Bohr magnetons per Co (for x = 0.4). Thus, CoSn1-xInx provides a rare example of an itinerant antiferromagnet with a small ordered moment. This work provides clear evidence that flat bands arising from frustrated lattices in bulk crystals represent a viable route to new physics, evidenced here by the emergence of magnetic order upon introducing a non-magnetic dopant into a non-magnetic kagome metal.

We report the observation of photo-induced plasmon-phonon coupled modes in the group IV-VI semiconductor PbTe using Fourier-transform inelastic X-ray scattering at the Linac Coherent Light Source (LCLS). We measure the near-zone-center dispersion of the heavily screened longitudinal optical (LO) phonon branch as extracted from differential changes in x-ray diffuse scattering intensity following above band gap photoexcitation., Comment: 5 pages, 2 figures

CoSn is a Pauli paramagnet with relatively flat d-bands centered about 100 meV below the Fermi energy Ef. Single crystals of CoSn lightly doped with Fe, In, or Ni are investigated using x-ray and neutron scattering, magnetic susceptibility and magnetization, ac susceptibility, specific heat and resistivity measurements. Within the rigid band approximation, hole doping with a few percent of Fe or In should move the flat bands closer to Ef, whereas electron doping with Ni should move the flat bands further away from Ef. We provide evidence that this indeed occurs. Fe and In doping drive CoSn toward magnetism, while Ni doping suppresses CoSn's already weak magnetic response. The resulting ground state is different for Fe versus In doping. For Fe-doped crystals, Co1-xFexSn, with 0.02 < x < 0.27, the magnetic and specific heat data are consistent with the formation of a spin glass, with a glass transition temperature, Tg, ranging from 1 K for x=0.02 to 10 K for x= 0.27. Powder and single crystal neutron diffraction found no evidence of long-range magnetic order below Tg with x = 0.17. For In-doped crystals, CoSn1-yIny, both the magnetic susceptibility and the Sommerfeld coefficient, gamma, increase substantially relative to pure CoSn, but with no clear indication of a magnetic transition for 0.05 < y < 0.2. CoSn crystals doped with Ni (Co0.93Ni0.07Sn) have a significantly smaller magnetic susceptibility and gamma than pure CoSn, consistent with the flat bands further from Ef., Comment: 20 pages, 10 figures

MnBi$_4$Te$_{7}$ and MnBi$_6$Te$_{10}$ are two members with n=2 and 3 in the family of MnBi$_{2n}$Te$_{3n+1}$ where the n=1 member, MnBi$_2$Te$_{4}$, has been intensively investigated as the first intrinsic antiferromagnetic topological insulator. Here we report the A-type antiferromagnetic order in these two compounds by measuring magnetic properties, electrical and thermal transport, specific heat, and single crystal neutron diffraction. Both compounds order into an A-type antiferromagnetic structure as does MnBi$_2$Te$_{4}$ with ferromagnetic planes coupled antiferromagnetically along the crystallographic \textit{c} axis. While no evidence for any in-plane ordered moment is found for MnBi$_2$Te$_{4}$ or MnBi$_6$Te$_{10}$, weak reflections at half-L positions along the [0 0 L] direction are observed for MnBi$_4$Te$_{7}$ suggesting an in-plane ordered moment around 0.15$\mu_{B}$/Mn. The ordering temperature, T$_N$, is 13\,K for MnBi$_4$Te$_{7}$ and 11\,K for MnBi$_6$Te$_{10}$. The magnetic order is also manifested in the anisotropic magnetic properties. For both compounds, the interlayer coupling is weak and a spin flip transition occurs when a magnetic field of around 1.6\,kOe is applied along the \textit{c}-axis at 2\,K. As observed in MnBi$_2$Te$_4$, when cooling across T$_N$, no anomaly was observed in the temperature dependence of thermopower. On the other hand, critical scattering effects are observed in thermal conductivity although the effect is less pronounced than that in MnBi$_2$Te$_{4}$., Comment: 15 pages, 14 figures

Here we report the evolution of structural, magnetic and transport properties in MnBi$_{2-x}$Sb$_x$Te$_4$ (0$\leq x \leq$2) single crystals. MnSb$_2$Te$_4$, isostructural to MnBi$_2$Te$_4$, has the lattice parameters of \textit{a}=4.2445(3)$\AA$ and \textit{c}=40.869(5)$\AA$, respectively. With increasing Sb content in MnBi$_{2-x}$Sb$_x$Te$_4$, the \textit{a}-lattice decreases linearly following the Vegards law while the \textit{c}-lattice shows little compositional dependence. The \textit{a}-lattice contraction occurs by reducing Mn-Te-Mn bond angle while Mn-Te bond length remains nearly constant. The anisotropic magnetic properties suggest an antiferromagnetic order below T$_N$=19\,K for MnSb$_2$Te$_4$ with the magnetic moments aligned along the crystallographic \textit{c}-axis. The antiferromagnetic ordering temperature slightly decreases from 24\,K for MnBi$_2$Te$_4$ to 19\,K for MnSb$_2$Te$_4$. More dramatic change was observed for the critical magnetic fields required for the spin-flop transition and moment saturation. With increasing Sb content, both critical fields decrease and in MnSb$_2$Te$_4$ a small field of 3\,kOe is enough to saturate the moment. In high magnetic fields, the saturation moment shows significant suppression from 3.56$\mu_B$/Mn for MnBi$_2$Te$_4$ to 1.57$\mu_B$/Mn for MnSb$_2$Te$_4$. Data analyses suggest that both the interlayer magnetic interaction and single ion anisotropy decrease with increasing Sb content. The partial substitution of Bi by Sb also dramatically affects the transport properties. A crossover from n-type to p-type conducting behavior is observed around x=0.63. Our results show close correlation between structural, magnetic and transport properties in MnBi$_{2-x}$Sb$_x$Te$_4$ and that partial substitution of Bi by Sb is an effective approach to fine tuning both the magnetism and transport properties of MnBi$_{2-x}$Sb$_x$Te$_4$.

Static and dynamic properties of the quasi-two-dimensional antiferromagnet K$_2$V$_3$O$_8$ have been investigated by $^{51}$V-NMR experiments on nonmagnetic V$^{5+}$ sites. Above the structural transition temperature $T_{\rm{S}}$ = 115 K, NMR spectra are fully compatible with the $P4bm$ space group symmetry. The formation of superstructure below $T_{\rm{S}}$ causes splitting of the NMR lines, which get broadened at lower temperatures so that individual peaks are not well resolved. Evolution of NMR spectra with magnetic field along $c$-axis below the magnetic transition temperature $T_{\rm{N}} \sim 4$ K is qualitatively consistent with a simple N\'{e}el order and a spin flop transition. However, broad feature of the spectra does not rule out possible incommensurate spin structure. The spin-lattice relaxation rate $1/T_1$ below $T_{\rm{N}}$ shows huge enhancement for a certain range of magnetic field, which is independent of temperature and attributed to cross relaxation due to anomalously large nuclear spin-spin coupling between V$^{5+}$ and magnetic V$^{4+}$ sites. The results indicate strong gapless spin fluctuations, which could arise from incommesurate orders or complex spin textures., Comment: 13 pages, 14 figures

Millimeter-sized MnBi$_2$Te$_4$ single crystals are grown out of Bi-Te flux and characterized by measuring magnetic and transport properties, scanning tunneling microscope (STM) and spectroscopy (STS). The magnetic structure of MnBi$_2$Te$_4$ below T$_N$ is determined by powder and single crystal neutron diffraction measurements. Below T$_N$=24\,K, Mn$^{2+}$ moments order ferromagnetically in the \textit{ab} plane but antiferromagnetically along the crystallographic \textit{c} axis. The ordered moment is 4.04(13) $\mu_{B}$/Mn at 10\,K and aligned along the crystallographic \textit{c}-axis. The electrical resistivity drops upon cooling across T$_N$ or when going across the metamagnetic transition in increasing fields below T$_N$. A critical scattering effect was observed in the vicinity of T$_N$ in the temperature dependence of thermal conductivity. However, A linear temperature dependence was observed for thermopower in the temperature range 2K-300K without any anomaly around T$_N$. These indicate that the magnetic order in Mn-Te layer has negligible effect on the electronic band structure, which makes possible the realization of proposed topological properties in MnBi$_2$Te$_4$ after fine tuning of the electronic band structure.

We systematically investigate the magnetic properties and local structure of Ba2YIrO6 to demonstrate that Y and Ir lattice defects in the form of antiphase boundary or clusters of antisite disorder affect the magnetism observed in this $d^4$ compound. We compare the magnetic properties and atomic imaging of (1) a slow cooled crystal, (2) a crystal quenched from 900\degree C after growth, and (3) a crystal grown using a faster cooling rate than the slow cooled one. Atomic imaging by scanning transmission electron microscopy (STEM) shows that quenching from 900oC introduces antiphase boundary to the crystals, and a faster cooling rate during crystal growth leads to clusters of Y and Ir antisite disorder. STEM study suggests the antiphase boundary region is Ir-rich with a composition of Ba2YIrO6. The magnetic measurements show that Ba2YIrO6 crystals with clusters of antisite defects have a larger effective moment and a larger saturation moment than the slow-cooled crystals. Quenched crystals with Ir-rich antiphase boundary shows a slightly suppressed saturation moment than the slow cooled crystals, and this seems to suggest that antiphase boundary is detrimental to the moment formation. Our DFT calculations suggest magnetic condensation is unlikely as the energy to be gained from superexchange is small compared to the spin-orbit gap. However, once Y is replaced by Ir in the antisite disordered region, the picture of local non-magnetic singlets breaks down and magnetism can be induced. This is because of (a) enhanced interactions due to increased overlap of orbitals between sites, and, (b) increased number of orbitals mediating the interactions. Our work highlights the importance of lattice defects in understanding the experimentally observed magnetism in Ba2YIrO6 and other J=0 systems.

Flux growth of single crystals is normally performed in a vertical configuration with an upright refractory container holding the flux melt. At high temperatures, flux dissolves the charge forming a homogeneous solution before nucleation and growth of crystals take place under proper supersaturation generated by cooling or evaporating the flux. In this work, we report flux growth in a horizontal configuration with a temperature gradient along the horizontal axis: a liquid transport growth analogous to the vapor transport technique. In a typical liquid transport growth, the charge is kept at the hot end of the refractory container and the flux melt dissolves the charge and transfers it to the cold end. Once the concentration of charge is above the solubility limit at the cold end, the thermodynamically stable phase nucleates and grows. Compared to the vertical flux growth, the liquid transport growth can provide a large quantity of crystals in a single growth since the charge/flux ratio is not limited by the solubility limit at the growth temperature. This technique is complementary to the vertical flux growth and can be considered when a large amount of crystals are needed but the yield from the conventional vertical flux growth is limited. We applied this technique to the growth of IrSb$_3$, Mo$_3$Sb$_7$, MnBi from self flux, and the growth of FeSe, CrTe$_3$, NiPSe$_3$, FePSe$_3$, and InCuP$_2$S$_6$ from a halide flux.

The importance of electron-hole interband interactions is widely acknowledged for iron-pnictide superconductors with high transition temperatures (Tc). However, high-Tc superconductivity without hole carriers has been suggested in FeSe single-layer films and intercalated iron-selenides, raising a fundamental question whether iron pnictides and chalcogenides have different pairing mechanisms. Here, we study the properties of electronic structure in the high-Tc phase induced by pressure in bulk FeSe from magneto-transport measurements and first-principles calculations. With increasing pressure, the low-Tc superconducting phase transforms into high-Tc phase, where we find the normal-state Hall resistivity changes sign from negative to positive, demonstrating dominant hole carriers in striking contrast to other FeSe-derived high-Tc systems. Moreover, the Hall coefficient is remarkably enlarged and the magnetoresistance exhibits anomalous scaling behaviors, evidencing strongly enhanced interband spin fluctuations in the high-Tc phase. These results in FeSe highlight similarities with high-Tc phases of iron pnictides, constituting a step toward a unified understanding of iron-based superconductivity.

Prior to the superconducting transition at Tc = 2.3 K, Mo3Sb7 undergoes a symmetry-lowering, cubic-to-tetragonal structural transition at Ts = 53 K. We have monitored the pressure dependence of these two transitions by measuring the resistivity of Mo3Sb7 single crystals under various hydrostatic pressures up to 15 GPa. The application of external pressure enhances Tc but suppresses Ts until Pc ~ 10 GPa, above which a pressure-induced first order structural transition takes place and is manifested by the phase coexistence in the pressure range 8 < P < 12 GPa. The cubic phase above 12 GPa is also found to be superconducting with a higher Tc =6 K that decreases slightly with further increasing pressure. The variations with pressure of Tc and Ts satisfy the Bilbro-McMillan equation, i.e. Tc^nTs^(1-n) = constant, thus suggesting the competition of superconductivity with the structural transition that has been proposed to be accompanied with a spin-gap formation at Ts. This scenario is supported by our first-principles calculations which imply the plausible importance of magnetism that competes with the superconductivity in Mo3Sb7., Comment: 6 figures, Submitted to PRB

We report a neutron diffraction study of the multiferroic mechanism in (ND4)2FeCl5D2O, a molecular compound that exhibits magnetically induced ferroelectricity. This material exhibits two successive magnetic transitions on cooling: a long-range order transition to an incommensurate (IC) collinear sinusoidal spin state at TN=7.3 K, followed by a second transition to an IC cycloidal spin state at TFE=6.8 K, the later of which is accompanied by spontaneous ferroelectric polarization. The cycloid structure is strongly distorted by spin-lattice coupling as evidenced by the observations of both odd and even higher-order harmonics associated with the cycloid wave vector, and a weak commensurate phase that coexists with the IC phase. The appearance of the 2nd-order harmonic coincides with the onset of the electric polarization, thereby providing unambiguous evidence that the induced electric polarization is mediated by the spin-lattice interaction. Our results for this system, in which the orbital angular momentum is expected to be quenched, are remarkably similar to those of the prototypical TbMnO3, in which the magnetoelectric effect is attributed to spin-orbit coupling., Comment: 5 pages, 4 figures

The high-temperature ferromagnet MnBi continues to receive attention as a candidate to replace rare-earth-containing permanent magnets in applications above room temperature. This is due to a high Curie temperature, large magnetic moments, and a coercivity that increases with temperature. The synthesis of MnBi also allows for crystals that are free of interstitial Mn, enabling more direct access to the key interactions underlying the physical properties of binary Mn-based ferromagnets. In this work, we use inelastic neutron scattering to measure the spin waves of MnBi in order to characterize the magnetic exchange at low temperature. Consistent with the spin reorientation that occurs below 140 K, we do not observe a spin gap in this system above our experimental resolution. A Heisenberg model was fit to the spin wave data in order to characterize the long-range nature of the exchange. It was found that interactions up to sixth nearest neighbor are required to fully parameterize the spin waves. Surprisingly, the nearest-neighbor term is antiferromagnetic, and the realization of a ferromagnetic ground state relies on the more numerous ferromagnetic terms beyond nearest neighbor, suggesting that the ferromagnetic ground state arises as a consequence of the long-ranged interactions in the system., Comment: 5 pages, 2 figures, 2 tables; Supplemental Information has 2 pages, 1 figure

The singlet ground state magnetism in pyrochlore osmates Y$_2$Os$_2$O$_7$ and Ho$_2$Os$_2$O$_7$ is studied by DC and AC susceptibility, specific heat, and neutron powder diffraction measurements. Despite the expected non-magnetic singlet in the strong spin-orbit coupling (SOC) limit for Os$^{4+}$ ($5d^4$), Y$_2$Os$_2$O$_7$ exhibits a spin-glass (SG) ground state below 4 K with weak magnetism, suggesting possible proximity to a quantum phase transition between the non-magnetic state in the strong SOC limit and the magnetic state in the strong superexchange limit. Ho$_2$Os$_2$O$_7$ has the same structural distortion as occurs in Y$_2$Os$_2$O$_7$. However, the Os sublattice in Ho$_2$Os$_2$O$_7$ shows long-range magnetic ordering below 36\,K. The sharp difference of the magnetic ground state between Y$_2$Os$_2$O$_7$ and Ho$_2$Os$_2$O$_7$ signals the singlet ground state magnetism in $R_2$Os$_2$O$_7$ is fragile and can be disturbed by the weak $4f-5d$ interactions., Comment: 7 pages, 6 figures

The coexistence and competition between superconductivity and electronic orders, such as spin or charge density waves, have been a central issue in high transition-temperature (${T_{\rm c}}$) superconductors. Unlike other iron-based superconductors, FeSe exhibits nematic ordering without magnetism whose relationship with its superconductivity remains unclear. More importantly, a pressure-induced fourfold increase of ${T_{\rm c}}$ has been reported, which poses a profound mystery. Here we report high-pressure magnetotransport measurements in FeSe up to $\sim9$ GPa, which uncover a hidden magnetic dome superseding the nematic order. Above ${\sim6}$ GPa the sudden enhancement of superconductivity (${T_{\rm c}\le38.3}$ K) accompanies a suppression of magnetic order, demonstrating their competing nature with very similar energy scales. Above the magnetic dome we find anomalous transport properties suggesting a possible pseudogap formation, whereas linear-in-temperature resistivity is observed above the high-${T_{\rm c}}$ phase. The obtained phase diagram highlights unique features among iron-based superconductors, but bears some resemblance to that of high-${T_{\rm c}}$ cuprates., Comment: 15 pages, 4 figures

The interactions between electrons and phonons drive a large array of technologically relevant material properties including ferroelectricity, thermoelectricity, and phase-change behaviour. In the case of many group IV-VI, V, and related materials, these interactions are strong and the materials exist near electronic and structural phase transitions. Their close proximity to phase instability produces a fragile balance among the various properties. The prototypical example is PbTe whose incipient ferroelectric behaviour has been associated with large phonon anharmonicity and thermoelectricity. Experimental measurements on PbTe reveal anomalous lattice dynamics, especially in the soft transverse optical phonon branch. This has been interpreted in terms of both giant anharmonicity and local symmetry breaking due to off-centering of the Pb ions. The observed anomalies have prompted renewed theoretical and computational interest, which has in turn revived focus on the extent that electron-phonon interactions drive lattice instabilities in PbTe and related materials. Here, we use Fourier-transform inelastic x-ray scattering (FT-IXS) to show that photo-injection of free carriers stabilizes the paraelectric state. With support from constrained density functional theory (CDFT) calculations, we find that photoexcitation weakens the long-range forces along the cubic direction tied to resonant bonding and incipient ferroelectricity. This demonstrates the importance of electronic states near the band edges in determining the equilibrium structure., Comment: 9 page, 3 figures

Single crystals of (Nd1-xCex)2Fe14B are grown out of Fe-(Nd,Ce) flux. Chemical and structural analysis of the crystals indicates that (Nd1-xCex)2Fe14B forms a solid solution until at least x = 0.38 with a Vegard-like variation of the lattice constants with x. Refinements of single crystal neutron diffraction data indicate that Ce has a slight site preference (7:3) for the 4g rare earth site over the 4f site. Magnetization measurements show that for x = 0.38 the saturation magnetization at 400 K, a temperature important to applications, falls from 29.8 for the parent Nd2Fe14B to 27.6 (mu)B/f.u., the anisotropy field decreases from 5.5 T to 4.7 T, and the Curie temperature decreases from 586 to 543 K. First principles calculations carried out within density functional theory are used to explain the decrease in magnetic properties due to Ce substitution. Though the presence of the lower-cost and more abundant Ce slightly affects these important magnetic characteristics, this decrease is not large enough to affect a multitude of applications. Ce-substituted Nd2Fe14B is therefore a potential high-performance permanent magnet material with substantially reduced Nd content., Comment: 11 Pages, 8 figures, 5 tables

We investigate the magnetic properties of the series Sr2Ir1-xRuxO4 with neutron, resonant x-ray and magnetization measurements. The results indicate an evolution and coexistence of magnetic structures via a spin flop transition from ab-plane to c-axis collinear order as the 5d Ir4+ ions are replaced with an increasing concentration of 4d Ru4+ ions. The magnetic structures within the ordered regime of the phase diagram (x<0.3) are reported. Despite the changes in magnetic structure no alteration of the Jeff=1/2 ground state is observed. The behavior of Sr2Ir1-xRuxO4 is consistent with electronic phase separation and diverges from a standard scenario of hole doping. The role of lattice alterations with doping on the magnetic and insulating behavior is considered. The results presented here provide insight into the magnetic insulating states in strong spin-orbit coupled materials and the role perturbations play in altering the behavior.

Mo$_3$Sb$_7$ single crystals lightly doped with Cr, Ru, or Te are studied in order to explore the interplay between superconductivity, magnetism, and the cubic-tetragonal structural transition. The structural transition at 53\,K is extremely sensitive to Ru or Te substitution which introduce additional electrons, but robust against Cr substitution. No sign of a structure transition was observed in superconducting Mo$_{2.91}$Ru$_{0.09}$Sb$_7$ and Mo$_3$Sb$_{6.975}$Te$_{0.025}$. In contrast, 3at\% Cr doping only slightly suppresses the structural transition to 48\,K while leaving no trace of superconductivity above 1.8\,K. Analysis of magnetic properties suggests that the interdimer interaction in Mo$_3$Sb$_7$ is near a critical value and essential for the structural transition. All dopants suppress the superconductivity of Mo$_3$Sb$_7$. The tetragonal structure is not necessary for superconductivity., Comment: 6 pages, 5 figures, to appear in Phys. Rev. B

Compounds based on the Fe2P structure have continued to attract interest because of the interplay between itinerant and localized magnetism in a non-centrosymmetric crystal structure, and because of the recent developments of these materials for magnetocaloric applications. Here we report the growth and characterization of mm size single crystals of FeMnP0.8Si0.2. Single crystal x-ray diffraction, magnetization, resistivity, Hall and heat capacity data are reported. Surprisingly, the crystals exhibit itinerant antiferromagnetic order below 158 K with no hint of ferromagnetic behavior in the magnetization curves and with the spins ordered primarily in the ab plane. The room temperature resistivity is close to the Ioffe-Regel limit for a metal. Single crystal x-ray diffraction indicates a strong preference for Mn to occupy the larger pyramidal 3g site. The cation site preference in the as-grown crystals and the antiferromagnetism are not changed after high temperature anneals and a rapid quench to room temperature., Comment: 9 Pages, 7 Figures, 2 Tables

The high temperature magnetic order in SrRu$_2$O$_6$ was studied by measuring magnetization and neutron powder diffraction with both polarized and unpolarized neutrons. SrRu$_2$O$_6$ crystallizes into the hexagonal lead antimonate (PbSb$_2$O$_6$, space group \textit{P}$\overline{3}$1\textit{m}) structure with layers of edge-sharing RuO$_6$ octahedra separated by Sr$^{2+}$ ions. SrRu$_2$O$_6$ orders at $T_N$=565\,K with Ru moments coupled antiferromagnetically both in-plane and out-of-plane. The magnetic moment is 1.30(2) $\mu_\mathrm{B}$/Ru at room temperature and is along the crystallographic \textit{c}-axis in the G-type magnetic structure. We performed density functional calculations with constrained RPA to obtain the electronic structure and effective intra- and inter-orbital interaction parameters. The projected density of states show strong hybridization between Ru 4$d$ and O 2$p$. By downfolding to the target $t_{2g}$ bands we extracted the effective magnetic Hamiltonian. We performed Monte Carlo simulations to determine the transition temperature as a function of inter- and intra-plane couplings and find weak inter plane coupling, 3\% of the intra-plane coupling, permits three dimensional magnetic order at $T_N$. As suggested by the magnetic susceptibility, two-dimensional correlations persist above $T_N$ due to the strong intra-plane coupling., Comment: 5 pages, 4 figures

High quality single crystals of BaFe$_{12}$O$_{19}$ were grown using the floating zone technique in flowing oxygen pressurized to 100 atm. Single crystal neutron diffraction was used to determine the nuclear and magnetic structure of BaFe$_{12}$O$_{19}$ at 4 K and 295 K. At both temperatures, there exist local electric dipoles formed by the off-mirror-plane displacements of magnetic Fe$^{3+}$ ions at the bipyramidal sites. The displacement at 4 K is about half of that at room temperature. The temperature dependence of the specific heat shows no anomaly associated with long range polar ordering in the temperature range from 1.90-300 K. The inverse dielectric permittivity, $1/\varepsilon$, along the c-axis shows a $T^2$ temperature dependence between 10 K and 20 K, with a significantly reduced temperature dependence displayed below 10 K. Moreover, as the sample is cooled below 1.4 K there is an anomalous sharp upturn in $1/\varepsilon$. These features resemble those of classic quantum paraelectrics such as SrTiO$_3$. The presence of the upturn in $1/\varepsilon$ indicates that BaFe$_{12}$O$_{19}$ is a critical quantum paraelectric system with Fe$^{3+}$ ions involved in both magnetic and electric dipole formation., Comment: 9 pages, 9 figures, submitted to APL Materials

La$_{0.4}$Na$_{0.6}$Fe$_2$As$_2$ single crystals have been grown out of an NaAs flux in an alumina crucible and characterized by measuring magnetic susceptibility, electrical resistivity, specific heat, as well as single crystal x-ray and neutron diffraction. La$_{0.4}$Na$_{0.6}$Fe$_2$As$_2$ single crystals show a structural phase transition from a high temperature tetragonal phase to a low-temperature orthorhombic phase at T$_s$\,=\,125\,K. This structural transition is accompanied by an anomaly in the temperature dependence of electrical resistivity, anisotropic magnetic susceptibility, and specific heat. Concomitant with the structural phase transition, the Fe moments order along the \emph{a} direction with an ordered moment of 0.7(1)\,$\mu_{\textup{B}}$ at \emph{T}\,=\,5 K. The low temperature stripe antiferromagnetic structure is the same as that in other \emph{A}Fe$_{2}$As$_{2}$ (\emph{A}\,=\,Ca, Sr, Ba) compounds. La$_{0.5-x}$Na$_{0.5+x}$Fe$_2$As$_2$ provides a new material platform for the study of iron-based superconductors where the electron-hole asymmetry could be studied by simply varying La/Na ratio., Comment: 9 pages, 7 figures, to appear in Physical Review B

Using inelastic neutron scattering, we show that the onset of superconductivity in underdoped Ba(Fe$_{1-x}$Co$_{x}$)$_{2}$As$_{2}$ coincides with a crossover from well-defined spin waves to overdamped and diffusive spin excitations. This crossover occurs despite the presence of long-range stripe antiferromagnetic order for samples in a compositional range from x=0.04-0.055, and is a consequence of the shrinking spin-density wave gap and a corresponding increase in the particle-hole (Landau) damping. The latter effect is captured by a simple itinerant model relating Co doping to changes in the hot spots of the Fermi surface. We argue that the overdamped spin fluctuations provide a pairing mechanism for superconductivity in these materials.

Materials with very low thermal conductivity are of high interest for both thermoelectric and optical phase-change applications. Synthetic nanostructuring is most promising to suppress thermal conductivity by scattering phonons, but challenges remain in producing bulk samples. We show that in crystalline AgSbTe$_2$, a spontaneously-forming nanostructure leads to a suppression of thermal conductivity to a glass-like level. Our mapping of the phonon mean-free-paths provides a novel bottom-up microscopic account of thermal conductivity, and also reveals intrinsic anisotropies associated with the nanostructure. Ground-state degeneracy in AgSbTe$_2$ leads to the natural formation of nanoscale domains with different orderings on the cation sublattice, and correlated atomic displacements, which efficiently scatter phonons. This mechanism is general and points to a new avenue in nano-scale engineering of materials, to achieve low thermal conductivities for efficient thermoelectric converters and phase-change memory devices.

The anharmonic lattice dynamics of rock-salt thermoelectric compounds SnTe and PbTe are investigated with inelastic neutron scattering (INS) and first-principles calculations. The experiments show that, surprisingly, although SnTe is closer to the ferroelectric instability, phonon spectra in PbTe exhibit a more anharmonic character. This behavior is reproduced in first-principles calculations of the temperature-dependent phonon self-energy. Our simulations reveal how the nesting of phonon dispersions induces prominent features in the self-energy, which account for the measured INS spectra and their temperature dependence. We establish that the phase-space for three-phonon scattering processes, rather than just the proximity to the lattice instability, is the mechanism determining the complex spectrum of the transverse-optical ferroelectric mode.

The Jeff=1/2 state is manifested in systems with large cubic crystal field splitting and spin-orbit coupling that are comparable to the on-site Coulomb interaction, U. 5d transition metal oxides host parameters in this regime and strong evidence for this state in Sr2IrO4, and additional iridates, has been presented. All the candidates, however, deviate from the cubic crystal field required to provide an unmixed canonical Jeff=1/2 state, impacting the development of a robust model of this novel insulating and magnetic state. We present results that not only show Ca4IrO6 hosts the state, but furthermore uniquely resides close to the ideal case required for an unmixed Jeff=1/2 state.

TM-doped IrTe2(TM=Mn, Fe, Co, Ni) compounds were synthesized by solid state reaction. Single crystal x-ray diffraction experiments indicate that part of the doped TM ions (TM=Fe, Co, and Ni) substitute for Ir, and the rest intercalate into the octahedral interstitial sites located in between IrTe2 layers. Due to the lattice mismatch between MnTe2 and IrTe2, Mn has limited solubility in IrTe2 lattice. The trigonal structure is stable in the whole temperature range 1.80

Measurements of magnetization, specific heat, electrical resistivity, Hall effect, and magnetoresistance on single crystalline samples of LaFeAsO grown in a NaAs flux are reported. While this material is known to be a semimetal, the temperature dependence of the electrical resistivity data presented herein is reminiscent of semiconducting behavior and exhibits distinct features associated with a structural transition and spin density wave (SDW) order. Magnetoresistance and Hall coefficient measurements were performed in magnetic fields up to 9 T applied perpendicular to the basal plane using a van der Pauw configuration. The charge carrier density and mobility indicate that electrons are the majority charge carriers and exhibit features indicative of the structural transition and SDW formation. Low temperature X-ray diffraction measurements have confirmed that the structural transition in these samples occurs near 140 K, compared to a transition temperature of 156 K observed in polycrystalline samples. Isotherms of magnetoresistivity measured as a function of magnetic field can be scaled onto a single curve in which the scaling field is a linear function of temperature between 2.2 K and 180 K., Comment: 8 pages, 9 figures, submitted to Physical Review B (July 2013)

The Fe1+yTe1-xSex series of materials is one of the prototype families of Fe-based superconductors. To provide further insight into these materials we present systematic inelastic neutron scattering measurements of the low energy spin excitations for x=0.27, 0.36, 0.40, 0.49. These measurements show an evolution of incommensurate spin excitations towards the (1/2 1/2 0) wave vector with doping. Concentrations (x=0.40 and 0.49) which exhibit the most robust superconducting properties have spin excitations closest to (1/2 1/2 0) and also exhibit a strong spin resonance in the spin excitation spectrum below Tc. The resonance signal appears to be closer to (1/2 1/2 0) than the underlying spin excitations. We discuss the possible relationship between superconductivity and spin excitations at the (1/2 1/2 0) wave vector and the role that interstitial Fe may play., Comment: 5 figures

Millimeter sized single crystals of Mo3Sb7 are grown using the self-flux technique and a thorough characterization of their structural, magnetic, thermal and transport properties is reported. The structure parameters for the high-temperature cubic phase and the low-temperature tetragonal phase were, for the first time, determined with neutron single crystal diffraction. Both X-ray powder diffraction and neutron single crystal diffraction at room temperature confirmed that Mo3Sb7 crystallizes in Ir3Ge7-type cubic structure with space group Im-3m. The cubic-tetragonal structure transition at 53K is verified by the peak splitting of (4 0 0) reflection observed by X-ray single crystal diffraction and the dramatic intensity change of (12 0 0) peak observed by neutron single crystal diffraction. The structural transition is accompanied by a sharp drop in magnetic susceptibility, electrical resistivity, and thermopower while cooling. A weak lambda anomaly was also observed around 53K in the temperature dependence of specific heat and the entropy change across the transition is estimated to be 1.80J/molMoK. The temperature dependence of magnetic susceptibility was measured up to 750K and it follows a Curie-Weiss behavior above room temperature. Analysis of the low-temperature magnetic susceptibility suggests a spin gap of 110K around 53K. A typical phonon thermal conductivity was observed in the low temperature tetragonal phase. A glassy phonon thermal conductivity above 53K suggests a structural instability in a wide temperature range. Superconductivity was observed at 2.35K in the as-grown crystals and the dimensionless specific heat jump was determined to be 1.49, which is slightly larger than the BCS value of 1.43 for the weak-coupling limit., Comment: 9 pages, 10 figures, accepted for publication in Phys. Rev. B

The chiral helimagnet Cr1/3NbS2 has been investigated by magnetic, transport and thermal properties measurements on single crystals and by first principles electronic structure calculations. From the measured field and temperature dependence of the magnetization for fields applied perpendicular to the c axis, the magnetic phase diagram has been constructed in the vicinity of the phase transitions. A transition from a paramagnetic to a magnetically ordered phase occurs near 120 K. With increasing magnetic field and at temperatures below 120 K, this material undergoes transitions from a helimagnetic to a soliton-lattice phase near 900 Oe, and then to a ferromagnetic phase near 1300 Oe. The transitions are found to strongly affect the electrical transport. The resistivity decreases sharply upon cooling near 120 K, and the spin reorientation from the helimagnetic ground state to the commensurate ferromagnetic state is evident in the magnetoresistance. At high fields a large magnetoresistance (55 % at 140 kOe) is observed near the magnetic transition temperature. Heat capacity and electronic structure calculations show the density of states at the Fermi level is low in the magnetically ordered state. Effects of spin fluctuations are likely important in understanding the behavior of Cr1/3NbS2 near and above the magnetic ordering transitions.

The molecular compound [Fe$_{2}$($\mu_{2}$-oxo)(C$_{3}$H$_{4}$N$_{2}$)$_{6}$(C$_{2}$O$_{4}$)$_{2}$] was designed and synthesized for the first time and its structure was determined using single-crystal X-ray diffraction. The magnetic susceptibility of this compound was measured from 2 to 300 K. The analysis of the susceptibility data using protocols developed for other spin singlet ground-state systems indicates that the quantum entanglement would remain at temperatures up to 732 K, significantly above the highest entanglement temperature reported to date. The large gap between the ground state and the first-excited state (282 K) suggests that the spin system may be somewhat immune to decohering mechanisms. Our measurements strongly suggest that molecular magnets are promising candidate platforms for quantum information processing.

The layered 5d transition metal oxide Sr2IrO4 has been shown to host a novel Jeff=1/2 Mott spin orbit insulating state with antiferromagnetic ordering, leading to comparisons with the layered cuprates. Here we study the effect of substituting Mn for Ir in single crystals of Sr2Ir0.9Mn0.1O4 through an investigation involving bulk measurements and resonant x-ray and neutron scattering. We observe a new long range magnetic structure emerge upon doping through a reordering of the spins from the basal plane to the c-axis with a reduced ordering temperature compared to Sr2IrO4. The strong enhancement of the magnetic x-ray scattering intensity at the L3 edge relative to the L2 edge indicates that the Jeff=1/2 state is robust and capable of hosting a variety of ground states.

We use core-valence-valence (CVV) Auger spectra to probe the Coulomb repulsion between holes in the valence band of Fe pnictide superconductors. By comparing the two-hole final state spectra to density functional theory calculations of the single particle density of states, we extract a measure of the electron correlations that exist in these systems. Our results show that the Coulomb repulsion is highly screened and can definitively be considered as weak. We also find that there are differences between the 1111 and 122 families and even a small variation as a function of the doping, x, in Ba(Fe1 xCox)2As2. We discuss how the values of the hole-hole Coulomb repulsion obtained from our study relate to the onsite Coulomb parameter "U" used in model and first principles calculations based on dynamical mean field theory, and establish an upper bound for its effective value. Our results impose stringent constraints on model based phase diagrams, Comment: 16 pages, 4 figures

Lattice dynamics and magnetic excitations are investigated to elucidate the origin of magneto-dielectric effects in the S=1/2 two-dimensional quantum spin compound K$_2$V$_3$O$_8$. We find evidence for lattice instabilities at 110 K and 60 K as optical phonon anomalies and a soft mode at 26 cm$^{-1}$ in A$_1$ symmetry. Two-magnon excitations in B$_1$ symmetry show an unconventional double-peak structure and temperature dependence. This suggests the existence of a split mode near the zone boundary caused by a mixing of spin and lattice modes., Comment: 7 pages, 7 figures, accepted for publication in PRB

The noncentrosymmetric ferromagnet Cr11Ge19 has been investigated by electrical transport, AC and DC magnetization, heat capacity, x-ray diffraction, resonant ultrasound spectroscopy, and first principles electronic structure calculations. Complex itinerant ferromagnetism in this material is indicated by nonlinearity in conventional Arrott plots, unusual behavior of AC susceptibility, and a weak heat capacity anomaly near the Curie temperature (88 K). The inclusion of spin wave excitations was found to be important in modeling the low temperature heat capacity. The temperature dependence of the elastic moduli and lattice constants, including negative thermal expansion along the c axis at low temperatures, indicate strong magneto-elastic coupling in this system. Calculations show strong evidence for itinerant ferromagnetism and suggest a noncollinear ground state may be expected.

A direct and element-specific measurement of the local Fe spin moment has been provided by analyzing the Fe 3s core level photoemission spectra in the parent and optimally doped CeFeAsO1-xFx (x = 0, 0.11) and Sr(Fe1 xCox)2As2 (x = 0, 0.10) pnictides. The rapid time scales of the photoemission process allowed the detection of large local spin moments fluctuating on a 10-15 s time scale in the paramagnetic, anti-ferromagnetic and superconducting phases, indicative of the occurrence of ubiquitous strong Hund's magnetic correlations. The magnitude of the spin moment is found to vary significantly among different families, 1.3 \muB in CeFeAsO and 2.1 \muB in SrFe2As2. Surprisingly, the spin moment is found to decrease considerably in the optimally doped samples, 0.9 \muB in CeFeAsO0.89F0.11 and 1.3 \muB in Sr(Fe0.9Co0.1)2As2. The strong variation of the spin moment against doping and material type indicates that the spin moments and the motion of itinerant electrons are influenced reciprocally in a self-consistent fashion, reflecting the strong competition between the antiferromagnetic super-exchange interaction among the spin moments and the kinetic energy gain of the itinerant electrons in the presence of a strong Hund's coupling. By describing the evolution of the magnetic correlations concomitant with the appearance of superconductivity, these results constitute a fundamental step toward attaining a correct description of the microscopic mechanisms shaping the electronic properties in the pnictides, including magnetism and high temperature superconductivity.

We present inelastic neutron scattering measurements and first principles calculations examining the intermetallic marcasite CrSb2. The observed spin wave dispersion implies that the magnetic interactions are strongly one-dimensional with antiferromagnetic chains parallel to the crystalline c-axis. Such low-dimensional excitations are unexpected in a semiconducting intermetallic system. Moreover this material may be further interesting in that the magnetic anisotropy may enhance thermoelectric properties along particular crystallographic directions., Comment: 5 pages, 4 figures, Submitted to an APS journal

We report inelastic neutron scattering measurements of crystal field transitions in PrFeAsO, PrFeAsO0.87F0.13, and NdFeAsO0.85F0.15. Doping with fluorine produces additional crystal field excitations, providing evidence that there are two distinct charge environments around the rare earth ions, with probabilities that are consistent with a random distribution of dopants on the oxygen sites. The 4f electrons of the Pr3+ and Nd3+ ions have non-magnetic and magnetic ground states, respectively, indicating that the enhancement of Tc compared to LaFeAsO1-xFx is not due to rare earth magnetism., Comment: 4 pages 4 figures

We report the temperature dependence of the resistivity and thermoelectric power under hydrostatic pressure of the itinerant antiferromagnet BaFe2As2 and the electron-doped superconductor Ba(Fe0.9Co0.1)2As2. We observe a hole-like contribution to the thermopower below the structural-magnetic transition in the parent compound that is suppressed in magnitude and temperature with pressure. Pressure increases the contribution of electrons to transport in both the doped and undoped compound. In the 10% Co-doped sample, we used a two-band model for thermopower to estimate the carrier concentrations and determine the effect of pressure on the band structure.

Understanding the microscopic processes affecting the bulk thermal conductivity is crucial to develop more efficient thermoelectric materials. PbTe is currently one of the leading thermoelectric materials, largely thanks to its low thermal conductivity. However, the origin of this low thermal conductivity in a simple rocksalt structure has so far been elusive. Using a combination of inelastic neutron scattering measurements and first-principles computations of the phonons, we identify a strong anharmonic coupling between the ferroelectric transverse optic (TO) mode and the longitudinal acoustic (LA) modes in PbTe. This interaction extends over a large portion of reciprocal space, and directly affects the heat-carrying LA phonons. The LA-TO anharmonic coupling is likely to play a central role in explaining the low thermal conductivity of PbTe. The present results provide a microscopic picture of why many good thermoelectric materials are found near a lattice instability of the ferroelectric type.

The spin dynamics of a quasi one dimensional $S=1$ bond alternating spin-gap antiferromagnet Ni(C$_9$H$_{24}$N$_4$)NO$_2$(ClO$_4$) (abbreviated as NTENP) is studied by means of electron spin resonance (ESR) technique. Five modes of ESR transitions are observed and identified: transitions between singlet ground state and excited triplet states, three modes of transitions between spin sublevels of collective triplet states and antiferromagnetic resonance absorption in the field-induced antiferromagnetically ordered phase. Singlet-triplet and intra-triplet modes demonstrate a doublet structure which is due to two maxima in the density of magnon states in the low-frequency range. A joint analysis of the observed spectra and other experimental results allows to test the applicability of the fermionic and bosonic models. We conclude that the fermionic approach is more appropriate for the particular case of NTENP., Comment: 11 pages, 11 figures, published in Phys.Rev.B

It is shown that attempts to accurately deduce the magnetic penetration depth of overdoped BaFe_{1.82}Co_{0.18}As2 single crystals by transverse-field muon spin rotation (TF-muSR) are thwarted by field-induced magnetic order and strong vortex-lattice disorder. We explain how substantial deviations from the magnetic field distribution of a nearly perfect vortex lattice by one or both of these factors is also significant for other iron-based superconductors, and this introduces considerable uncertainty in the values of the magnetic penetration depth obtained by TF-muSR., Comment: 4 pages, 4 figures

We report the temperature dependence of the low-temperature specific heat down to 400 mK of the electron-doped Ba(Fe$_{0.92}$Co$_{0.08}$)$_{2}$As$_{2}$ superconductors. We have measured two samples extracted from the same batch: first sample has been measured just after preparation with no additional heat treatment. The sample shows $T_{c}$=20 K, residual specific heat $\gamma_{0}$=3.6 mJ/mol K$^{2}$ and a Schottky-like contribution at low temperatures. A second sample has been annealed at 800 $^{o}C$ for two weeks and shows $T_{c}$ = 25 K and $\gamma_{0}$=1.4 mJ/mol~K$^{2}$. By subtracting the lattice specific heat, from pure BaFe$_{2}$As$_{2}$, the temperature dependence of the electronic specific heat has been obtained and studied. For both samples the temperature dependence of $C_{el}(T)$ clearly indicate the presence of low-energy excitations in the system. Their specific heat data cannot be described by single clean s- or d-wave models and the data requires an anisotropic gap scenario which may or may not have nodes, Comment: SCES 2010, 5 pages, 2 figures

We report an extensive study on the intrinsic bulk electronic structure of the high-temperature superconductor CeFeAsO0.89F0.11 and its parent compound CeFeAsO by soft and hard x-ray photoemission, x-ray absorption and soft-x-ray emission spectroscopies. The complementary surface/bulk probing depth, and the elemental and chemical sensitivity of these techniques allows resolving the intrinsic electronic structure of each element and correlating it with the local structure, which has been probed by extended-x-ray absorption fine structure spectroscopy. The measurements indicate a predominant 4f1 (i.e. Ce3+) initial state configuration for Cerium and an effective valence-band-to-4f charge-transfer screening of the core hole. The spectra also reveal the presence of a small Ce f0 initial state configuration, which we assign to the occurrence of an intermediate valence state. The data reveal a reasonably good agreement with the partial density of states as obtained in standard density functional calculations over a large energy range. Implications for the electronic structure of these materials are discussed., Comment: Accepted for publication in Phys. Rev. B

High-resolution scanning tunneling microscopy (STM) measurements on BaFe2As2-one of the parent compounds of the iron-based superconductors-reveals a (1x1) As-terminated unit cell on the (001) surface. However, there are significant differences of the surface unit cell compared to the bulk: only one of the two As atoms in the unit cell is imaged and domain walls between different (1x1) regions display a C2 symmetry at the surface. It should have been C2v if the STM image reflected the geometric structure of the surface or the orthorhombic bulk. The inequivalent As atoms and the bias dependence of the domain walls indicate that the origin of the STM image is primarily electronic not geometric. We argue that the surface electronic topography mirrors the bulk spin structure of BaFe2As2, via strong orbital-spin coupling.

We report a doping, magnetic field and low-temperature dependent study of the specific heat of the iron-arsenide Ba(Fe$_{1-x}$Co$_{x}$)$_{2}$As$_{2}$ at under (x=0.045), optimal (x=0.08) and overdoped (x=0.103 and 0.105) regimes. By subtracting the lattice specific heat the temperature and magnetic field dependence of the electronic specific heat has been studied. The temperature and field dependencies of the superconducting part of $C_{p}$ exhibit similar behavior for all doping concentrations. The temperature variation of the electronic specific heat as well as its field dependence cannot be described by a single isotropic s-wave gap, pointing to a complex gap structure in the system. The lack of doping dependence indicates that the gap structure does not change significantly as a function of doping. We also observe a significant residual linear term of unknown origin in the specific heat of Ba(Fe$_{1-x}$Co$_{x}$)$_{2}$As$_{2}$ which suggests that inhomogeneity may be an important factor in Co-doped BaFe$_{2}$As$_{2}$

The spatially resolved electrical transport properties have been studied on the surface of optimally-doped superconducting Ba(Fe1-xCox)2As2 single crystal by using a four-probe scanning tunneling microscopy. While some non-uniform contrast appears near the edge of the cleaved crystal, the scanning electron microscopy (SEM) reveals mostly uniform contrast. For the regions that showed uniform SEM contrast, a sharp superconducting transition at TC = 22.1 K has been observed with a transition width (delta)Tc = 0.2 K. In the non-uniform contrast region, TC is found to vary between 19.6 and 22.2 K with (delta)Tc from 0.3 to 3.2 K. The wavelength dispersive x-ray spectroscopy reveals that Co concentration remains 7.72% in the uniform region, but changes between 7.38% and 7.62% in the non-uniform region. Thus the variations of superconductivity are associated with local compositional change., Comment: 18 pages, 5 figures

The orbital symmetries of electron doped iron-arsenide superconductors Ba(Fe1-xCox)2As2 have been measured with x-ray absorption spectroscopy. The data reveal signatures of Fe d electron itinerancy, weak electronic correlations, and a high degree of Fe-As hybridization related to the bonding topology of the Fe dxz+yz states, which are found to contribute substantially at the Fermi level. The energies and detailed orbital character of Fe and As derived unoccupied s and d states are found to be in remarkably good agreement with the predictions of standard density functional theory., Comment: Accepted for publication in Phys. Rev. B, 3 figures. Minor corrections added