Evolution of magnetic surfboards and spin glass behavior in (Fe1-pGap)2TiO5.

The unusual anisotropy of the spin glass (SG) transition in the pseudobrookite system Fe2TiO5has been interpreted as arising from an induced, van der Waals-like, interaction among magnetic clusters. Here we present susceptibility (χ) and specific heat data (C) for Fe2TiO5diluted with non-magnetic Ga, (Fe1-pGap)2TiO5, for disorder parameterp= 0, 0.11, and 0.42, and elastic neutron scattering data forp= 0.20. A uniform suppression ofTgis observed upon increasingp, along with a value ofχTgthat increases asTgdecreases, i.e.dχ(Tg)/dTg<0We also observeCT∝T2in the low temperature limit. The observed behavior places (Fe1-pGap)2TiO5in the category of a strongly geometrically frustrated SG.

Assessing Nontrivial Topology in Weyl Semimetals by Dichroic Photoemission.

The electronic structure of Weyl semimetals features Berry flux monopoles in the bulk and Fermi arcs at the surface. While angle-resolved photoelectron spectroscopy (ARPES) is successfully used to map the bulk and surface bands, it remains a challenge to explicitly resolve and pinpoint these topological features. Here we combine state-of-the-art photoemission theory and experiments over a wide range of excitation energies for the Weyl semimetals TaAs and TaP. Our results show that simple surface-band-counting schemes, proposed previously to identify nonzero Chern numbers, are ambiguous due to pronounced momentum-dependent spectral weight variations and the pronounced surface-bulk hybridization. Instead, our findings indicate that dichroic ARPES provides an improved approach to identify Fermi arcs but requires an accurate description of the photoelectron final state.

Phase Diagram for Light-Induced Superconductivity in κ-(ET)_{2}-X.

Resonant optical excitation of certain molecular vibrations in κ-(BEDT-TTF)_{2}Cu[N(CN)_{2}]Br has been shown to induce transient superconductinglike optical properties at temperatures far above equilibrium T_{c}. Here, we report experiments across the bandwidth-tuned phase diagram of this class of materials, and study the Mott insulator κ-(BEDT-TTF)_{2}Cu[N(CN)_{2}]Cl and the metallic compound κ-(BEDT-TTF)_{2}Cu(NCS)_{2}. We find nonequilibrium photoinduced superconductivity only in κ-(BEDT-TTF)_{2}Cu[N(CN)_{2}]Br, indicating that the proximity to the Mott insulating phase and possibly the presence of preexisting superconducting fluctuations are prerequisites for this effect.

Momentum-space signatures of Berry flux monopoles in the Weyl semimetal TaAs.

Since the early days of Dirac flux quantization, magnetic monopoles have been sought after as a potential corollary of quantized electric charge. As opposed to magnetic monopoles embedded into the theory of electromagnetism, Weyl semimetals (WSM) exhibit Berry flux monopoles in reciprocal parameter space. As a function of crystal momentum, such monopoles locate at the crossing point of spin-polarized bands forming the Weyl cone. Here, we report momentum-resolved spectroscopic signatures of Berry flux monopoles in TaAs as a paradigmatic WSM. We carried out angle-resolved photoelectron spectroscopy at bulk-sensitive soft X-ray energies (SX-ARPES) combined with photoelectron spin detection and circular dichroism. The experiments reveal large spin- and orbital-angular-momentum (SAM and OAM) polarizations of the Weyl-fermion states, resulting from the broken crystalline inversion symmetry in TaAs. Supported by first-principles calculations, our measurements image signatures of a topologically non-trivial winding of the OAM at the Weyl nodes and unveil a chirality-dependent SAM of the Weyl bands. Our results provide directly bulk-sensitive spectroscopic support for the non-trivial band topology in the WSM TaAs, promising to have profound implications for the study of quantum-geometric effects in solids.

Quantum Critical Point in the Itinerant Ferromagnet Ni_{1-x}Rh_{x}.

We report a chemical substitution-induced ferromagnetic quantum critical point in polycrystalline Ni_{1-x}Rh_{x} alloys. Through magnetization and muon spin relaxation measurements, we show that the ferromagnetic ordering temperature is suppressed continuously to zero at x_{crit}=0.375 while the magnetic volume fraction remains 100% up to x_{crit}, pointing to a second order transition. Non-Fermi liquid behavior is observed close to x_{crit}, where the electronic specific heat C_{el}/T diverges logarithmically, while immediately above x_{crit} the volume thermal expansion coefficient α_{V}/T and the Grüneisen ratio Γ=α_{V}/C_{el} both diverge logarithmically in the low temperature limit, further indication of a ferromagnetic quantum critical point in Ni_{1-x}Rh_{x}.

Evidence for undoped Weyl semimetal charge transport in Y2Ir2O7.

Weyl fermions scattering from a random Coulomb potential are predicted to exhibit resistivity versus temperature [Formula: see text] in a single particle model. Here we show that, in closed-environment-grown polycrystalline samples of Y2Ir2O7, [Formula: see text] over four orders of magnitude in [Formula: see text]. While the measured prefactor, [Formula: see text], is obtained from the model using reasonable materials parameters, the [Formula: see text] behavior extends far beyond the model's range of applicability. In particular, the behavior extends into the low-temperature, high-resistivity region where the Ioffe-Regel parameter, [Formula: see text]. Strong on-site Coulomb correlations, instrumental for predicting a Weyl semimetal state in Y2Ir2O7, are the possible origin of such 'bad' Weyl semimetal behavior.

Effects of chemical disorder in the itinerant antiferromagnet Ti1-x V x Au.

The fragile nature of itinerant magnetism can be exploited using non-thermal parameters to study quantum criticality. The recently discovered quantum critical point (QCP) in the Sc-doped (hole-like doping) itinerant antiferromagnet TiAu (Ti1-x Sc x Au) raised questions about the effects of the crystal and electronic structures on the overall magnetic behavior. In this study, doping with V (electron-like doping) in Ti1-x V x Au introduces chemical disorder which suppresses antiferromagnetic order from [Formula: see text] 36 K for x = 0 down to 10 K for x = 0.15, whereupon a solubility limit is reached. Signatures of non-Fermi-liquid behavior are observed in transport and specific heat measurements similar to Ti1-x Sc x Au, even though Ti1-x V x Au is far from a QCP for the accessible compositions [Formula: see text].

Uncovering the behavior of Hf2Te2P and the candidate Dirac metal Zr2Te2P.

Results are reported for single crystal specimens of Hf2Te2P and compared to its structural analogue Zr2Te2P, which was recently proposed to be a potential reservoir for Dirac physics [1]. Both materials are produced using the iodine vapor phase transport method and the resulting crystals are exfoliable. The bulk electrical transport and thermodynamic properties indicate Fermi liquid behavior at low temperature for both compounds. Quantum oscillations are observed in magnetization measurements for fields applied parallel but not perpendicular to the c-axis, suggesting that the Fermi surfaces are quasi-two dimensional. Frequencies are determined from quantum oscillations for several parts of the Fermi surfaces. Lifshitz-Kosevich fits to the temperature dependent amplitudes of the oscillations reveal small effective masses, with a particularly small value [Formula: see text] for the α branch of Zr2Te2P. Electronic structure calculations are in good agreement with quantum oscillation results and illustrate the effect of a stronger spin-orbit interaction going from Zr to Hf. These results suggest that by using appropriate tuning parameters this class of materials may deepen the pool of novel Dirac phenomena.

An itinerant antiferromagnetic metal without magnetic constituents.

The origin of magnetism in metals has been traditionally discussed in two diametrically opposite limits: itinerant and local moments. Surprisingly, there are very few known examples of materials that are close to the itinerant limit, and their properties are not universally understood. In the case of the two such examples discovered several decades ago, the itinerant ferromagnets ZrZn2 and Sc3In, the understanding of their magnetic ground states draws on the existence of 3d electrons subject to strong spin fluctuations. Similarly, in Cr, an elemental itinerant antiferromagnet with a spin density wave ground state, its 3d electron character has been deemed crucial to it being magnetic. Here, we report evidence for an itinerant antiferromagnetic metal with no magnetic constituents: TiAu. Antiferromagnetic order occurs below a Néel temperature of 36 K, about an order of magnitude smaller than in Cr, rendering the spin fluctuations in TiAu more important at low temperatures. This itinerant antiferromagnet challenges the currently limited understanding of weak itinerant antiferromagnetism, while providing insights into the effects of spin fluctuations in itinerant-electron systems.

Impact of vacancy ordering on thermal transport in crystalline phase-change materials.

Controlling thermal transport in solids is of paramount importance for many applications. Often thermal management is crucial for a device's performance, as it affects both reliability and power consumption. A number of intricate concepts have been developed to address this challenge, such as diamond-like coatings to enhance the thermal conductivity or low symmetry complex super-structures to reduce it. Here, a different approach is pursued, where we explore the potential of solids with a high yet controllable degree of disorder. Recently, it has been demonstrated that an unconventionally high degree of structural disorder characterizes a number of crystalline phase-change materials (PCMs). This disorder strongly impacts electronic transport and even leads to disorder induced localization (Anderson localization). This raises the question how thermal transport is affected by such conditions. Here thermal transport in highly disordered crystalline Ge-Sb-Te (GST) based PCMs is investigated. Glass-like thermal properties are observed for several crystalline PCMs, which are attributed to strong scattering by disordered point defects. A systematic study of different compounds along the pseudo-binary line between GeTe and Sb2Te3 reveals that disordered vacancies act as point defects responsible for pronounced phonon scattering. Annealing causes a gradual ordering of the vacancies and leads to a more 'crystal-like' thermal conductivity. While both vibrational and electronic degrees of freedom are affected by disorder, the consequences differ for different stoichiometries. This opens up a pathway to tune electrical and thermal transport by controlling the degree of disorder. Materials with tailored transport properties may not only help to improve power efficiency and scaling in upcoming phase-change memories but are also of fundamental interest in the field of thermoelectric materials.

A facility for X-ray diffraction in magnetic fields up to 25 T and temperatures between 15 and 295 K.

A facility for X-ray diffraction has been developed at the National High Magnetic Field Laboratory. It brings diffraction capability to the 25 T Florida split coil magnet and implements temperature control in a range of 15-295 K using a cold finger helium cryostat. This instrument represents an alternative to pulsed magnetic field systems, and it exceeds the static magnetic fields currently available at synchrotron facilities. Magnetic field compatibility of an X-ray source and detectors with the sizable magnetic fringe fields emanating from the magnet constrained the design of the diffractometer.

Superconductivity with extremely large upper critical fields in Nb2Pd0.81S5.

Here, we report the discovery of superconductivity in a new transition metal-chalcogenide compound, i.e. Nb2Pd0.81S5, with a transition temperature Tc is approximately equal to 6.6 K. Despite its relatively low Tc, it displays remarkably high and anisotropic superconducting upper critical fields, e.g. µ0Hc2 (T → 0 K) > 37 T for fields applied along the crystallographic b-axis. For a field applied perpendicularly to the b-axis, µ0Hc2 shows a linear dependence in temperature which coupled to a temperature-dependent anisotropy of the upper critical fields, suggests that Nb2Pd0.81S5 is a multi-band superconductor. This is consistent with band structure calculations which reveal nearly cylindrical and quasi-one-dimensional Fermi surface sheets having hole and electron character, respectively. The static spin susceptibility as calculated through the random phase approximation, reveals strong peaks suggesting proximity to a magnetic state and therefore the possibility of unconventional superconductivity.

Co[V2]o4: a spinel approaching the itinerant electron limit.

Studies of the structure, magnetization, and resistivity under pressure on stoichiometric normal spinel Co[V(2)]O(4) single crystals show (i) absence of a structural distortion, (ii) abnormal magnetic critical exponents, and (iii) metallic conductivity induced by pressures at low temperatures. All these results prove that Co[V(2)]O(4) sits on the edge of the itinerant-electron limit. Compared with similar measurements on Fe[V(2)]O(4) and other A[V(2)]O(4) studies, it is shown that a critical V-V separation for a localized-itinerant electronic phase transition exists.

Disorder-induced localization in crystalline phase-change materials.

Localization of charge carriers in crystalline solids has been the subject of numerous investigations over more than half a century. Materials that show a metal-insulator transition without a structural change are therefore of interest. Mechanisms leading to metal-insulator transition include electron correlation (Mott transition) or disorder (Anderson localization), but a clear distinction is difficult. Here we report on a metal-insulator transition on increasing annealing temperature for a group of crystalline phase-change materials, where the metal-insulator transition is due to strong disorder usually associated only with amorphous solids. With pronounced disorder but weak electron correlation, these phase-change materials form an unparalleled quantum state of matter. Their universal electronic behaviour seems to be at the origin of the remarkable reproducibility of the resistance switching that is crucial to their applications in non-volatile-memory devices. Controlling the degree of disorder in crystalline phase-change materials might enable multilevel resistance states in upcoming storage devices.

Cupric oxide as an induced-multiferroic with high-TC.

Materials that combine coupled electric and magnetic dipole order are termed 'magnetoelectric multiferroics'. In the past few years, a new class of such materials, 'induced-multiferroics', has been discovered, wherein non-collinear spiral magnetic order breaks inversion symmetry, thus inducing ferroelectricity. Spiral magnetic order often arises from the existence of competing magnetic interactions that reduce the ordering temperature of a more conventional collinear phase. Hence, spiral-phase-induced ferroelectricity tends to exist only at temperatures lower than approximately 40 K. Here, we propose that copper(II) oxides (containing Cu2+ ions) having large magnetic superexchange interactions can be good candidates for induced-multiferroics with high Curie temperature (T(C)). In fact, we demonstrate ferroelectricity with T(C)=230 K in cupric oxide, CuO (tenorite), which is known as a starting material for the synthesis of high-T(c) (critical temperature) superconductors. Our result provides an important contribution to the search for high-temperature magnetoelectric multiferroics.

Crystallization of charge holes in the spin ladder of Sr14Cu24O41.

Determining the nature of the electronic phases that compete with superconductivity in high-transition-temperature (high-T(c)) superconductors is one of the deepest problems in condensed matter physics. One candidate is the 'stripe' phase, in which the charge carriers (holes) condense into rivers of charge that separate regions of antiferromagnetism. A related but lesser known system is the 'spin ladder', which consists of two coupled chains of magnetic ions forming an array of rungs. A doped ladder can be thought of as a high-T(c) material with lower dimensionality, and has been predicted to exhibit both superconductivity and an insulating 'hole crystal' phase in which the carriers are localized through many-body interactions. The competition between the two resembles that believed to operate between stripes and superconductivity in high-T(c) materials. Here we report the existence of a hole crystal in the doped spin ladder of Sr14Cu24O41 using a resonant X-ray scattering technique. This phase exists without a detectable distortion in the structural lattice, indicating that it arises from many-body electronic effects. Our measurements confirm theoretical predictions, and support the picture that proximity to charge ordered states is a general property of superconductivity in copper oxides.

Amorphouslike density of gap states in single-crystal pentacene.

We show that optical and electrical measurements on pentacene single crystals can be used to extract the density of states in the highest occupied molecular orbital-lowest unoccupied molecular orbital band gap. It is found that these highly purified crystals possess band tails broader than those typically observed in inorganic amorphous solids. Results on field-effect transistors fabricated from similar crystals imply that the gap state density is much larger within 5-10 nm of the gate dielectric. Thus, organic thin-film transistors for such applications as flexible displays might be significantly improved by reducing these defects.

Bias-dependent generation and quenching of defects in pentacene.

We describe a defect generation phenomenon that is new to organic semiconductors. A defect in pentacene single crystals can be created by bias-stress and persists at room temperature for an hour in the dark but only seconds with 420 nm illumination. The defect gives rise to a hole trap at Ev+0.38 eV and causes metastable transport effects at room temperature. Creation and decay rates of the hole trap have a 0.67 eV activation energy with a small (10(8) s(-1)) prefactor, suggesting that atomic motion plays a key role in the generation and quenching process.

Synthesis, structure and physical properties of the first one-dimensional phenalenyl-based neutral radical molecular conductor.

We report the preparation, crystallization, and solid-state characterization of a benzyl-substituted spirobiphenalenyl radical. The crystal structure shows that the radical is monomeric in the solid state, with the molecules packed in an unusual one-dimensional (1-D) fashion that we refer to as a pi-step stack. This particular mode of 1-D stacking is forced on the lattice arrangement by the presence of the orthogonal phenalenyl units that were specifically incorporated to prevent the crystallization of low-dimensional structures. The structure shows that this strategy is effective, and neighboring molecules in the stack can only interact via the overlap of one pair of active (spin-bearing) carbon atoms per phenalenyl unit, leading to the pi-step structure in which the remaining four active carbon atoms per phenalenyl unit do not interact with nearest neighbor molecules. The magnetic susceptibility data in the temperature range 4-360 K may be fit to an antiferromagnetic Heisenberg S = 1/2 linear chain model with intrachain spin coupling J = -52.3 cm(-1). Despite the uniform stacking, the material has a room temperature conductivity of 1.4 x 10(-3) S/cm and is best described as a Mott insulator.