Search

Spin-flip dark excitons are optical-dipole-forbidden quasiparticles with remarkable potential in optoelectronics, especially when they are realized within cleavable van der Waals materials. Despite this potential, dark excitons have not yet been definitively identified in ferromagnetic van der Waals materials. Here, we report two dark excitons in a model ferromagnetic material CrI3 using high-resolution resonant inelastic x-ray scattering (RIXS) and show that they feature narrower linewidths compared to the bright excitons previously reported in this material. These excitons are shown to have spin-flip character, to disperse as a function of momentum, and to change through the ferromagnetic transition temperature. Given the versatility of van der Waals materials, these excitons hold promise for new types of magneto-optical functionality., Comment: 6 pages, 4 figures to appear in Physical Review X

In one-dimensional quantum materials, conducting electrons and the underlying lattices can undergo a spontaneous translational symmetry breaking, known as Peierls transition. For nearly a century, the Peierls transition has been understood within the paradigm of electron-electron interactions mediated by longitudinal acoustic phonons. This classical picture has recently been revised in topological semimetals, where transverse acoustic phonons can couple with conducting p-orbital electrons and give rise to an unconventional Fermi surface instability, dubbed the transverse Peierls transition (TPT). Most interestingly, the TPT induced lattice distortions can further break rotation or mirror/inversion symmetries, leading to nematic or chiral charge density waves (CDWs). Quantum materials that host the TPT, however, have not been experimentally established. Here, we report the experimental discovery of an incommensurate TPT in the tetragonal Dirac semimetal EuAl$_4$. Using inelastic x-ray scattering with meV resolution, we observe the complete softening of a transverse acoustic phonon at the CDW wavevector upon cooling, whereas the longitudinal acoustic phonon is nearly unchanged. Combining with first principles calculations, we show that the incommensurate CDW wavevector matches the calculated charge susceptibility peak and connects the nested Dirac bands with Al 3$p_{x}$ and 3$p_{y}$ orbitals. Supplemented by second harmonic generation measurements, we show that the CDW induced lattice distortions break all vertical and diagonal mirrors whereas the four-fold rotational symmetry is retained below the CDW transition. Our observations strongly suggest a chiral CDW in EuAl$_4$ and highlight the TPT as a new avenue for chiral quantum states., Comment: Supplementary materials are available upon request

Transition metal halides can host a large variety of novel phenomena, such as magnetism in the monolayer limit, quantum spin liquid and spiral spin liquid states, and topological magnons and phonons. Sizeable high quality single crystals are necessary for investigations of magnetic and lattice excitations by, for example, inelastic neutron scattering. In this paper, we review a less well-known vapor transport technique, self-selecting vapor growth, and report our growths of transition metal halides using this technique. We report the growth and characterizations of sizable single crystals of RuCl$_3$, CrCl$_3$, Ru$_{1-x}$Cr$_x$Cl$_3$, and CrBr$_3$. In order to expedite the conversion of starting powder to single crystals, we modified the technique by cooling the growth ampoule through an appropriate temperature range. Our work shows that the self-selecting vapor transport technique can provide large single crystals of transition metal halides, demonstrating its potential for providing high quality single crystals of quantum materials.

In this work, a temperature-induced valence-state transition is studied in a narrow composition range of Ba$_{2-x}$Sr$_x$TbIrO$_6$. The valence-state transition involves an electron transfer between Tb and Ir leading to the valence-state change between Tb$^{3+}$/Ir$^{5+}$ and Tb$^{4+}$/Ir$^{4+}$ phases. This first-order transition has a dramatic effect on the lattice, transport properties, and the long-range magnetic order at low temperatures for both Tb and Ir ions. Ir$^{5+}$ ion has an electronic configuration of 5$d^4$ ($J\rm_{eff}$ = 0) which is expected to be nonmagnetic. In contrast, Ir$^{4+}$ ion with a configuration of 5$d^5$($J\rm_{eff}$ = 1/2) favors a long-range magnetic order. For $x$ = 0.1 with Tb$^{3+}$/Ir$^{5+}$ configuration to the lowest temperature (2 K) investigated in this work, a spin-glass behavior is observed around 5 K indicating Ir$^{5+}$ ($J\rm_{eff}$ = 0) ions act as a spacer reducing the magnetic interactions between Tb$^{3+}$ ions. For $x$ = 0.5 with Tb$^{4+}$/Ir$^{4+}$ configuration below the highest temperature 400 K of this work, a long-range antiferromagnetic order at $T\rm_N$ = 40 K is observed highlighting the importance of Ir$^{4+}$ ($J\rm_{eff}$ = 1/2) ions in promoting the long-range magnetic order of both Tb and Ir ions. For 0.2 $\leqslant x \leqslant$ 0.375, a temperature-induced valence-state transition from high-temperature Tb$^{3+}$/Ir$^{5+}$ phase to low-temperature Tb$^{4+}$/Ir$^{4+}$ phase occurs in the temperature range 180 K $\leqslant T \leqslant$ 325 K and the transition temperature increases with $x$. The compositional dependence demonstrates the ability to tune the the valence state for a critical region of $x$ that leads to a concurrent change in magnetism and structure. This tuning ability could be employed with suitable strain in thin films to act as a switch as the magnetism is manipulated., Comment: 10 pages, 8 figures

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.

Topological semimetals are a frontier of quantum materials. In multi-band electronic systems, topological band-crossings can form closed curves, known as nodal lines. In the presence of spin-orbit coupling and/or symmetry-breaking operations, topological nodal lines can break into Dirac/Weyl nodes and give rise to novel transport properties, such as the chiral anomaly and giant anomalous Hall effect. Recently the time-reversal symmetry-breaking induced Weyl fermions are observed in a kagome-metal Co3Sn2S2, triggering interests in nodal-line excitations in multiband kagome systems. Here, using first-principles calculations and symmetry based indicator theories, we find six endless nodal lines along the stacking direction of kagome layers and two nodal rings in the kagome plane in nonmagnetic Ni3 In2 S2 . The linear dipsersive electronic structure, confirmed by angle-resolved photoemission spectroscopy, induces large magnetoresistance up to 2000% at 9 T. Our results establish a diverse topological landscape of multi-band kagome metals., Comment: 4 figures, 7 pages

Recently, transition-metal-based kagome metals have aroused much research interest as a novel platform to explore exotic topological quantum phenomena. Here we report on the synthesis, structure, and physical properties of a bilayer kagome lattice compound V3Sb2. The polycrystalline V3Sb2 samples were synthesized by conventional solid-state-reaction method in a sealed quartz tube at temperatures below 850 Celsius degree. Measurements of magnetic susceptibility and resistivity revealed consistently a density-wave-like transition at Tdw ~ 160 K with a large thermal hysteresis, even though some sample-dependent behaviors are observed presumably due to the different preparation conditions. Upon cooling through Tdw, no strong anomaly in lattice parameters and no indication of symmetry lowering were detected in powder x-ray diffraction measurements. This transition can be suppressed completely by applying hydrostatic pressures of about 1.8 GPa, around which no sign of superconductivity is observed down to 1.5 K. Specific-heat measurements reveal a relatively large Sommerfeld coefficient {\gamma} = 18.5 mJ/mol-K2, confirming the metallic ground state with moderate electronic correlations. Density functional theory calculations indicate that V3Sb2 shows a non-trivial topological crystalline property. Thus, our study makes V3Sb2 a new candidate of metallic kagome compound to study the interplay between density-wave-order, nontrivial band topology, and possible superconductivity., Comment: 22 pages, 8 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

The discovery of two-dimensional (2D) systems hosting intrinsic long-range magnetic order represents a seminal addition to the rich physical landscape of van der Waals (vdW) materials. CrI3 has emerged as perhaps the most salient example, as the interdependence of crystalline structure and magnetic order, along with strong light-matter interactions provides a promising platform to explore the optical control of magnetic, vibrational, and charge degrees of freedom at the 2D limit. However, the fundamental question of how this relationship between structure and magnetism manifests on their intrinsic timescales has rarely been explored. Here, we use ultrafast optical spectroscopy to probe magnetic and vibrational dynamics in CrI3, revealing demagnetization dynamics governed by spin-flip scattering and remarkably, a strong transient exchange-mediated interaction between lattice vibrations and spin oscillations. The latter yields a coherent spin-coupled phonon mode that is highly sensitive to the helicity of the driving pulse in the magnetically ordered phase. Our results shed light on the nature of spin-lattice coupling in vdW magnets on ultrafast timescales and highlight their potential for applications requiring non-thermal, high-speed control of magnetism at the nanoscale., Comment: 7 pages, 3 figures

An investigation of the structural, magnetic, thermodynamic, and charge transport properties of non-centrosymmetric hexagonal ScFeGe reveals it to be an anisotropic metal with a transition to a weak itinerant incommensurate helimagnetic state below $T_N = 36$ K. Neutron diffraction measurements discovered a temperature and field independent helical wavevector \textbf{\textit{k}} = (0 0 0.193) with magnetic moments of 0.53 $\mu_{B}$ per formula unit confined to the {\it ab}-plane. Density functional theory calculations are consistent with these measurements and find several bands that cross the Fermi level along the {\it c}-axis with a nearly degenerate set of flat bands just above the Fermi energy. The anisotropy found in the electrical transport is reflected in the calculated Fermi surface, which consists of several warped flat sheets along the $c$-axis with two regions of significant nesting, one of which has a wavevector that closely matches that found in the neutron diffraction. The electronic structure calculations, along with a strong anomaly in the {\it c}-axis conductivity at $T_N$, signal a Fermi surface driven magnetic transition, similar to that found in spin density wave materials. Magnetic fields applied in the {\it ab}-plane result in a metamagnetic transition with a threshold field of $\approx$ 6.7 T along with a sharp, strongly temperature dependent, discontinuity and a change in sign of the magnetoresistance for in-plane currents. Thus, ScFeGe is an ideal system to investigate the effect of in-plane magnetic fields on an easy-plane magnetic system, where the relative strength of the magnetic interactions and anisotropies determine the topology and magnetic structure., Comment: 15 pages, 13 figures

The research on layered van der Waals (vdW) magnets is rapidly progressing owing to exciting fundamental science and potential applications. In bulk crystal form, CrCl3 is a vdW antiferromagnet with in-plane ferromagnetic ordering below 17 K, and CrI3 is a vdW ferromagnet below 61 K. Here, we report on the electron spin resonance (ESR) properties of CrCl3 and CrI3 single crystals upon photo-excitation in the visible range. We noticed remarkable changes in the ESR spectra upon illumination. In the case of CrCl3, at 10 K, the ESR signal is shifted from g = 1.492 (dark) to 1.661 (light), line width increased from 376 to 506 Oe, and the signal intensity is reduced by 1.5 times. Most interestingly, the observed change in the signal intensity is reversible when the light is cycled on/off. We observed almost no change in the ESR spectral parameters in the paramagnetic phase (>20 K) upon illumination. Upon photo-excitation of CrI3, the ESR signal intensity is reduced by 1.9 times; the g-value increased from 1.956 to 1.990; the linewidth increased from 1170 to 1260 Oe at 60 K. These findings are discussed by taking into account the skin depth, the slow relaxation mechanism and the appearance of low-symmetry fields at the photo-generated Cr2+ Jahn-Teller centers. Such an increase in the g-value as a result of photo-generated Cr2+ ions is further supported by our many-body wavefunction calculations. This work has the potential to extend to monolayer vdWs magnets by combining ESR spectroscopy with optical excitation and detection., Comment: 21 pages, 9 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

We have synthesized single crystals of Na$_3$Co$_2$SbO$_6$ and characterized the structure and magnetic order by measuring anisotropic magnetic properties, heat capacity, x-ray and neutron single crystal diffraction. Magnetic properties and specific heat of polycrystalline Na$_3$Co$_2$SbO$_6$ were also measured for comparison. Na$_3$Co$_2$SbO$_6$ crystallizes in a monoclinic structure (space group $C2/m$) with [Co$_2$SbO$_6$]$^{3-}$ layers separated by Na$^+$ ions. The temperature dependence of magnetic susceptibility shows significant anisotropic behavior in the whole temperature range 2\,K-350\,K investigated in this work. An effective moment of about 5.5\,$\mu_B$/Co$^{2+}$ from a Curie-Weiss fitting of the magnetic susceptibility is larger than the spin only value and signals significant orbital contribution. Na$_3$Co$_2$SbO$_6$ single crystal undergoes a transition into a long-range antiferromagnetically ordered state below $T_N$=5\,K. Neutron single crystal diffraction confirmed the zigzag magnetic structure with a propagation vector k\,=\,(0.5, 0.5, 0). The ordered moment is found to be 0.9\,$\mu_B$ at 4\,K and align along the crystallographic \textit{b}-axis. Density functional theory calculations suggest that the experimentally observed zigzag order is energetically competing with the Neel order. It is also found that the covalency between Co $d$ and O $p$ is quite strong and competes with the local spin-orbit coupling, suggesting a $J_{eff}$=1/2 ground state may not be realized in this compound.

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$_4$.

We report a thorough study of Y$_{0.7}$La$_{0.3}$VO$_3$ single crystals by measuring magnetic properties, specific heat, thermal conductivity, x-ray and neutron diffraction with the motivation of revealing the lattice response to the spin-orbital entanglement in \textit{R}VO$_3$. Upon cooling from room temperature, the orbitally disordered paramagnetic state changes around T*$\sim$220\,K to spin-orbital entangled state which is then followed by a transition at T$_N$=116\,K to C-type orbital ordered (OO) and G-type antiferromagnetic ordered (AF) ground state. In the temperature interval T$_N

Results of magnetization and neutron diffraction measurements of the manganese vanadate system Mn$_5$(VO$_4$)$_2$(OH)$_4$ are reported. The crystal structure of this compound contains triangular [Mn$_3$O$_{13}$] building blocks that produce two-dimensional Mn$^{2+}$ magnetic networks with striped triangular topologies. The Mn sheets are connected through the nonmagnetic vanadate tetrahedra extending along the $a$-axis. Magnetization measurements performed on single crystals reveal the onset of a long-range antiferromagnetic order below approximately 45 K. The magnetic structure is N\'{e}el-type with nearest-neighbor Mn atoms coupled via three or four antiferromagnetic bonds. The magnetic moments are confined within the layers and are oriented parallel to the $b$ direction. The magnitudes of ordered moments are reduced, presumably by geometrical frustration and the low-dimensionality of the lattice structure., Comment: 5 pages, 4 figures

The topologically-protected, chiral soliton lattice is a unique state of matter offering intriguing functionality and it may serve as a robust platform for storing and transporting information in future spintronics devices. While the monoaxial chiral magnet Cr$_{1/3}$NbS$_2$ is known to host this exotic state in an applied magnetic field, its detailed microscopic origin has remained a matter of debate. Here we work towards addressing this open question by measuring the spin wave spectrum of Cr$_{1/3}$NbS$_2$ over the entire Brillouin zone with inelastic neutron scattering. The well-defined spin wave modes allow us to determine the values of several microscopic interactions for this system. The experimental data is well-explained by a Heisenberg Hamiltonian with exchange constants up to third nearest neighbor and an easy plane magnetocrystalline anisotropy term. Our work shows that both the second and third nearest neighbor exchange interactions contribute to the formation of the helimagnetic and chiral soliton lattice states in this robust three-dimensional magnet., Comment: Accepted by Applied Physics Letters

The physical properties of the spinel LiGaCr4S8 have been studied with neutron diffraction, X-ray diffraction, magnetic susceptibility and heat capacity measurements. The neutron diffraction and synchrotron X-ray diffraction data reveal negative thermal expansion (NTE) below 111(4) K. The magnetic susceptibility deviates from Curie-Weiss behavior with the onset of NTE. At low temperature a broad peak in the magnetic susceptibility at 10.3(3) K is accompanied by the return of normal thermal expansion. First principles calculations find a strong coupling between the lattice and the simulated magnetic ground state. These results indicate strong magnetoelastic coupling in LiGaCr4S8.

The perovskite SrIrO3 is an exotic narrow-band metal owing to a confluence of the strengths of the spin-orbit coupling (SOC) and the electron-electron correlations. It has been proposed that topological and magnetic insulating phases can be achieved by tuning the SOC, Hubbard interactions, and/or lattice symmetry. Here, we report that the substitution of nonmagnetic, isovalent Sn4+ for Ir4+ in the SrIr1-xSnxO3 perovskites synthesized under high pressure leads to a metal-insulator transition to an antiferromagnetic (AF) phase at TN > 225 K. The continuous change of the cell volume as detected by x-ray diffraction and the lamda-shape transition of the specific heat on cooling through TN demonstrate that the metal-insulator transition is of second-order. Neutron powder diffraction results indicate that the Sn substitution enlarges an octahedral-site distortion that reduces the SOC relative to the spin-spin exchange interaction and results in the type-G AF spin ordering below TN. Measurement of high-temperature magnetic susceptibility shows the evolution of magnetic coupling in the paramagnetic phase typical of weak itinerant-electron magnetism in the Sn-substituted samples. A reduced structural symmetry in the magnetically ordered phase leads to an electron gap opening at the Brillouin zone boundary below TN in the same way as proposed by Slater., Comment: 15 pages, 4 figures

Structural properties of LaCu$_{6-x}$Ag$_{x}$ have been investigated using neutron and x-ray diffraction, and resonant ultrasound spectroscopy (RUS) measurements. Diffraction measurements indicate a continuous structural transition from orthorhombic ($Pnma$) to monoclinic ($P2_1/c$) structure. RUS measurements show softening of natural frequencies at the structural transition, consistent with the elastic nature of the structural ground state. The structural transition temperatures in LaCu$_{6-x}$Ag$_{x}$ decrease with Ag composition until the monoclinic phase is completely suppressed at $x_c$ = 0.225. All of the evidence is consistent with the presence of an elastic quantum critical point in LaCu$_{6-x}$Ag$_{x}$., Comment: 5 pages, 3 figures, one table

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 structural properties of LaCu$_{6-x}$Au$_x$ have been studied using neutron diffraction, x-ray diffraction, and heat capacity measurements. The continuous orthorhombic-monoclinic structural phase transition in LaCu$_{6}$ is suppressed linearly with Au substitution until a complete suppression of the structural phase transition occurs at the critical composition, $x_{c}$ = 0.3. Heat capacity measurements at low temperatures indicate residual structural instability at $x_c$ that extends well into the orthorhombic phase. The instability is ferroelastic in nature, with density functional theory (DFT) calculations showing negligible coupling to electronic states near the Fermi level. The data and calculations presented here are consistent with the zero temperature termination of a continuous structural phase transition suggesting that the LaCu$_{6-x}$Au$_x$ series hosts an elastic quantum critical point., Comment: 9 pages, 11 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

Structure and composition of iron chalcogenides have a delicate relationship with magnetism and superconductivity. In this report we investigate the iron sulfide layered tetragonal phase (t-FeS), and compare with three-dimensional hexagonal phase (h-FeS). X-ray diffraction reveals the absence of structural transitions for both t- and h-FeS below room temperature, and gives phase compositions of Fe0.93(1)S and Fe0.84(1)S, respectively, for the samples studied here. The a lattice parameter of bigger than 3.68 A is significant for causing bulk superconductivity in iron sulfide, which is controlled by composition and structural details such as iron stoichiometry and concentration of vacancy. While h-FeS with a = 3.4436(1) A has magnetic ordering well above room temperature, our t-FeS with a =3.6779(8)A shows filamentary superconductivity below Tc = 4 K with less than 15% superconducting volume fraction. Also for t-FeS, the magnetic susceptibility shows an anomaly at ~ 15 K, and neutron diffraction reveals a commensurate antiferromagnetic ordering below TN = 116 K, with wave vector km= (0.25,0.25,0) and 0.46(2)uB/Fe. Although two synthesis routes are used here to stabilize t vs h crystal structures (hydrothermal vs solid-state methods), both FeS compounds order on two length-scales of ~1000 nm sheets or blocks and ~ 20 nm smaller particles, shown by neutron scattering. First principles calculations reveal a high sensitivity to the structure for the electronic and magnetic properties in t-FeS, predicting marginal antiferromagnetic instability for our compound (sulfur height of zS ~0.252) with an ordering energy of ~11 meV/Fe, while h-FeS is magnetically stable., Comment: 14 pages, 7 figures

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

Within the BaFe2As2 crystal lattice, we partially substitute thallium for barium and report the effects of interlayer coupling in Ba1-xTlxFe2As2 crystals. We demonstrate the unusual effects of magneto-elastic coupling and charge doping in this iron-arsenide material, whereby Neel temperature rises with small x, and then falls with additional x. Specifically, we find that Neel and structural transitions in BaFe2As2 (TN =Ts= 133 K) increase for x=0.05 (TN = 138 K, Ts = 140 K) from magnetization, heat capacity, resistivity, and neutron diffraction measurements. Evidence from single crystal X-ray diffraction and first principles calculations attributes the stronger magnetism in x=0.05 to magneto-elastic coupling related to the shorter intraplanar Fe-Fe bond distance. With further thallium substitution, the transition temperatures decrease for x = 0.09 (TN = Ts = 131 K), and this is due to charge doping. We illustrate that small changes related to 3d transition-metal state can have profound effects on magnetism., Comment: 10 pages; 4 figures

The structural and the magnetic properties of CeCu$_{6-x}$Ag$_x$ (0 $\leq$ $x$ $\leq$ 0.85) and CeCu$_{6-x}$Pd$_x$ (0 $\leq$ $x$ $\leq$ 0.4) have been studied using neutron diffraction, resonant ultrasound spectroscopy (RUS), heat capacity, x-ray diffraction measurements and first principles calculations. The structural and magnetic phase diagrams of CeCu$_{6-x}$Ag$_x$ and CeCu$_{6-x}$Pd$_x$ as a function of Ag/Pd composition are reported. The end member, CeCu$_6$, undergoes a structural phase transition from an orthorhombic ($Pnma$) to a monoclinic ($P2_1/c$) phase at 240 K. In CeCu$_{6-x}$Ag$_x$, the structural phase transition temperature (${T_{s}}$) decreases linearly with Ag concentration and extrapolates to zero at $x_{S}$ $\approx$ 0.1. The structural transition in CeCu$_{6-x}$Pd$_x$ remains unperturbed with Pd substitution within the range of our study. The lattice constant $b$ slightly decreases with Ag/Pd doping, whereas, $a$ and $c$ increase with an overall increase in the unit cell volume. Both systems, CeCu$_{6-x}$Ag$_x$ and CeCu$_{6-x}$Pd$_x$, exhibit a magnetic quantum critical point (QCP), at $x$ $\approx$ 0.2 and $x$ $\approx$ 0.05 respectively. Near the QCP, long range antiferromagnetic ordering takes place at an incommensurate wave vector ($\delta_1$ 0 $\delta_2$) where $\delta_1 \sim 0.62$, $\delta_2 \sim 0.25$, $x$ = 0.125 for CeCu$_{6-x}$Pd$_x$ and $\delta_1 \sim 0.64$, $\delta_2 \sim 0.3$, $x$ = 0.3 for CeCu$_{6-x}$Ag$_x$. The magnetic structure consists of an amplitude modulation of the Ce-moments which are aligned along the $c$-axis of the orthorhombic unit cell., Comment: 13 pages, 9 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

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

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

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.

Results of magnetic field and temperature dependent neutron diffraction and magnetization measurements on oxy-arsenate Rb$_{2}$Fe$_{2}$O(AsO$_{4}$)$_{2}$ are reported. The crystal structure of this compound contains pseudo-one-dimensional [Fe$_{2}$O$_{6}$]$^\infty$ sawtooth-like chains, formed by corner sharing isosceles triangles of $Fe^{3+}$ ions occupying two nonequivalent crystallographic sites. The chains extend infinitely along the crystallographic $b$-axis and are structurally confined from one another via diamagnetic (AsO$_{4}$)$^{3-}$ units along the $a$-axis, and Rb$^+$ cations along the $c$-axis direction. Neutron diffraction measurements indicate the onset of a long range antiferromagnetic order below approximately 25 K. The magnetic structure consists of ferrimagnetic chains which are antiferromagnetically coupled with each other. Within each chain, one of the two Fe sites carries a moment which lies along the \emph{b}-axis, while the second site bears a canted moment in the opposite direction. Externally applied magnetic field induces a transition to a ferrimagnetic state, in which the coupling between the sawtooth chains becomes ferromagnetic. Magnetization measurements performed on optically-aligned single crystals reveal evidence for an uncompensated magnetization at low magnetic fields that could emerge from to a phase-segregated state with ferrimagnetic inclusions or from antiferromagnetic domain walls. The observed magnetic states and the competition between them is expected to arise from strongly frustrated interactions within the sawtooth chains and relatively weak coupling between them.

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 spin and orbital ordering in Dy$_{1-x}$Tb$_{x}$VO$_3$ (x\,=\,0 and 0.2) was studied by measuring x-ray powder diffraction, magnetization, specific heat, and neutron single crystal diffraction. The results show that G-OO/C-AF and C-OO/G-AF phases coexist in Dy$_{0.8}$Tb$_{0.20}$VO$_3$ in the temperature range 2\,K$\sim$60\,K and the volume fraction of each phase is temperature and field dependent. The ordering of Dy moments at T*\,=\,12\,K induces a transition from G-OO/C-AF to a C-OO/G-AF phase. Magnetic fields suppress the long range order of Dy moments and thus the C-OO/G-AF phase below T*. The polarized moments induced at the Dy sublattice by external magnetic fields couple to the V 3d moments and this coupling favors the G-OO/C-AF state. Also discussed is the effect of the Dy-V magnetic interaction and local structure distortion on the spin and orbital ordering in Dy$_{1-x}$Tb$_{x}$VO$_3$., Comment: accepted for publication in Phys. Rev. B

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

We report time-of-flight neutron powder diffraction results on stoichiometric BaFe2As2. Pair distribution function analysis shows that the orthorhombic distortion in the a-b plane at short distances are significantly different from the average lattice distortion, indicating local variations in the lattice at the short-range. We propose that this local variation reflects a high density of nano-twins, short-ranged structures which locally affect the magnetic alignment. This results suggests that the discrepancies between the observed and calculated magnetic moments in BaFe2As2 arise partly from short-ranged variation of the lattice in the a-b plane., Comment: Accepted 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.

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

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 investigated size effects on thermoelectricity in thin films of a strongly correlated layered cobaltate. At room temperature, the thermopower is independent of thickness down to 6 nm. This unusual behavior is inconsistent with the Fuchs-Sondheimer theory, which is used to describe conventional metals and semiconductors, and is attributed to the strong electron correlations in this material. Although the resistivity increases, as expected, below a critical thickness of $\sim$ 30 nm. The temperature dependent thermopower is similar for different thicknesses but resistivity shows systematic changes with thickness. Our experiments highlight the differences in thermoelectric behavior of strongly correlated and uncorrelated systems when subjected to finite size effects. We use the atomic limit Hubbard model at the high temperature limit to explain our observations. These findings provide new insights on decoupling electrical conductivity and thermopower in correlated systems., Comment: Accepted by Physical Review B as a regular article

The thermoelectric transport properties of CaMg2Bi2, EuMg2Bi2, and YbMg2Bi2 were characterized between 2 and 650K. As synthesized, the polycrystalline samples are found to have lower p-type carrier concentrations than single-crystalline samples of the same empirical formula. These low carrier concentration samples possess the highest mobilities yet reported for materials with the CaAl2Si2 structure type, with a mobility of ~740cm$^2$/V/s observed in EuMg2Bi2 at 50K. Despite decreases in the Seebeck coefficient (\alpha) and electrical resistivity (\rho) with increasing temperature, the power factor (\alpha^2/\rho) increases for all temperatures examined. This behavior suggests a strong asymmetry in the conduction of electrons and holes. The highest figure of merit (zT) is observed in YbMg2Bi2, with zT approaching 0.4 at 600K for two samples with carrier densities of approximately 2x10^{18}cm^{-3} and 8x10^{18}cm^{-3} at room temperature. Refinements of neutron powder diffraction data yield similar behavior for the structures of CaMg2Bi2 and YbMg2Bi2, with smooth lattice expansion and relative expansion in $c$ being ~35% larger than relative expansion in $a$ at 973K. First principles calculations reveal an increasing band gap as Bi is replaced by Sb then As, and subsequent Boltzmann transport calculations predict an increase in \alpha for a given $n$ associated with an increased effective mass as the gap opens. The magnitude and temperature dependence of \alpha suggests higher zT is likely to be achieved at larger carrier concentrations, roughly an order of magnitude higher than those in the current polycrystalline samples, which is also expected from the detailed calculations.

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.