Search

Radio-frequency (14.6 MHz) AC magnetic susceptibility, $\chi^{\prime}_{AC}$, of \dytio\ was measured using a self-oscillating tunnel-diode resonator. Measurements were made with the excitation AC field parallel to the superimposed DC magnetic field up 5 T in a wide temperature range from 50 mK to 100 K. At 14.6 MHz a known broad peak of $\chi^{\prime}_{AC}(T)$ from kHz - range audio-frequency measurements around 15~K for both [111] and [110] directions shifts to 45~K, continuing the Arrhenius activated behavior with the same activation energy barrier of $E_a \approx 230$~K. Magnetic field dependence of $\chi^{\prime}_{AC}$ along [111] reproduces previously reported low-temperature two-in-two-out to three-in-one-out spin configuration transition at about 1~T, and an intermediate phase between 1 and 1.5~T. The boundaries of the intermediate phase show reasonable overlap with the literature data and connect at a critical endpoint of the first-order transition line, suggesting that these low-temperature features are frequency independent. An unusual upturn of magnetic susceptibility at $T \to 0$ was observed in magnetic fields between 1.5~T and 2~T for both magnetic field directions, before fully polarized configuration sets in above 2~T.

The Ising chain in transverse field is a paradigmatic model for a host of physical phenomena, including spontaneous symmetry breaking, topological defects, quantum criticality, and duality. Although the quasi-1D ferromagnet CoNb$_2$O$_6$ has been put forward as the best material example of the transverse field Ising model, it exhibits significant deviations from ideality. Through a combination of THz spectroscopy and theory, we show that CoNb$_2$O$_6$ in fact is well described by a different model with strong bond dependent interactions, which we dub the {\it twisted Kitaev chain}, as these interactions share a close resemblance to a one-dimensional version of the intensely studied honeycomb Kitaev model. In this model the ferromagnetic ground state of CoNb$_2$O$_6$ arises from the compromise between two distinct alternating axes rather than a single easy axis. Due to this frustration, even at zero applied field domain-wall excitations have quantum motion that is described by the celebrated Su-Schriefer-Heeger model of polyacetylene. This leads to rich behavior as a function of field. Despite the anomalous domain wall dynamics, close to a critical transverse field the twisted Kitaev chain enters a universal regime in the Ising universality class. This is reflected by the observation that the excitation gap in CoNb$_2$O$_6$ in the ferromagnetic regime closes at a rate precisely twice that of the paramagnet. This originates in the duality between domain walls and spin-flips and the topological conservation of domain wall parity. We measure this universal ratio `2' to high accuracy -- the first direct evidence for the Kramers-Wannier duality in nature., Comment: 6 pages, 3 figures; 5 pages, 7 figures (Supplemental)

Cobalt pyrochlore fluoride NaCaCo$_2$F$_7$ is a disordered frustrated magnet composed of Co$^{2+}$ ions with an effective spin-$\frac{1}{2}$ magnetic moment and exhibits spin freezing below $T_f \sim$2.4 K. We perform ultrasound velocity measurements on a single crystal of the cubic NaCaCo$_2$F$_7$. The temperature dependence of the bulk modulus (the breathing elastic mode) exhibits Curie-type softening upon cooling below $\sim$20 K down to $T_f$, which is suppressed by the magnetic field. This Curie-type softening should be a precursor to the enhancement of the strength of exchange disorder via the spin-lattice coupling, which causes the spin freezing. In contrast to the magnetic-field-suppressed Curie-type softening in the bulk modulus, the trigonal shear modulus exhibits softening with a characteristic minimum upon cooling, which is enhanced by the magnetic field at temperatures below $\sim$20 K. This magnetic-field-enhanced elastic anomaly in the trigonal shear modulus suggests a coupling of the lattice to the dynamical spin-cluster state. For NaCaCo$_2$F$_7$, the observed elastic anomalies reveal an occurrence of magnetic-field-induced crossover from an isostructural lattice instability toward the spin freezing to a trigonal lattice instability arising from the emergent dynamical spin-cluster state., Comment: 8 pages, 5 figures

We report high-frequency/high-field electron spin resonance (ESR) and high-field magnetization studies on single crystals of the bond-disordered pyrochlore NaCaCo$_2$F$_7$. Frequency- and temperature-dependent ESR investigations above the freezing temperature $T_f \sim 2.4$ K reveal the coexistence of two distinct magnetic phases. A cooperative paramagnetic phase, evidenced by a gapless excitation mode, is found as well as a spin-glass phase developing below 20 K which is associated with a gapped low-energy excitation. Effective $g$-factors close to 2 are obtained for both modes in line with pulsed high-field magnetization measurements which show an unsaturated isotropic behavior up to 58 T at 2 K. In order to describe the field-dependent magnetization in high magnetic fields, we propose an empirical model accounting for highly anisotropic ionic $g$-tensors expected for this material and taking into account the strongly competing interactions between the spins which lead to a frustrated ground state. As a detailed quantitative relation between effective $g$-factors as determined from ESR and the local $g$-tensors obtained by neutron scattering [Ross et al., Phys. Rev. B 93, 014433 (2016)] is still sought after, our work motivates further theoretical investigations of the low-energy excitations in bond-disordered pyrochlores., Comment: 9 pages, 6 figures

A new pyrochlore compound, NaCaNi$_2$F$_7$, was recently synthesized and has a single magnetic site with spin-1 Ni$^{2+}$. We present zero field (ZF) and longitudinal field (LF) muon spin rotation ($\mu$SR) measurements on this pyrochlore. Density functional theory (DFT) calculations show that the most likely muon site is located between two fluorine ions, but off-centre. A characteristic F-$\mu$-F muon spin polarization function is observed at high temperatures where Ni spin fluctuations are sufficiently rapid. The Ni$^{2+}$ spins undergo spin freezing into a disordered ground state below 4~K, with a characteristic internal field strength of 140~G. Persistent Ni spin dynamics are present to our lowest temperatures (75~mK), a feature characteristic of many geometrically frustrated magnetic systems.

The antiferromagnetic pyrochlore material NaCaCo$_2$F$_7$ is a thermal spin liquid over a broad temperature range (~ 140 K down to $T_F = 2.4 $K), in which magnetic correlations between Co$^{2+}$ dipole moments explore a continuous manifold of antiferromagnetic XY states. The thermal spin liquid is interrupted by spin freezing at a temperature that is ~ 2 % of the mean field interaction strength, leading to short range static XY clusters with distinctive relaxation dynamics. Here we report the low energy inelastic neutron scattering response from the related compound NaSrCo$_2$F$_7$, confirming that it hosts the same static and dynamic spin correlations as NaCaCo$_2$F$_7$. We then present the single-ion levels of Co$^{2+}$ in these materials as measured by inelastic neutron scattering. An intermediate spin orbit coupling model applied to an ensemble of trigonally distorted octahedral crystal fields accounts for the observed transitions. The single-ion ground state of Co$^{2+}$ is a Kramers doublet with a strongly XY-like $g$-tensor ($g_{xy}/g_{z}$ ~ 3). The local disorder inherent from the mixed pyrochlore $A$ sites (Na$^{+}$/Ca$^{2+}$ and Na$^{+}$/Sr$^{2+}$) is evident in these measurements as exaggerated broadening of some of the levels. A simple model that reproduces the salient features of the single-ion spectrum produces approximately 8.4 % and 4.1 % variation in the $z$ and $xy$ components of the $g$-tensor, respectively. This study confirms that an $S_{eff} =1/2$ model with XY antiferromagnetic exchange and weak exchange disorder serves as a basic starting point in understanding the low temperature magnetic behavior of these strongly frustrated magnets., Comment: 12 pages, 7 figures

The crystal structures and magnetic properties of three previously unreported A2B2F7 pyrochlore materials, NaSrMn2F7, NaCaFe2F7, and NaSrFe2F7 are presented. In these compounds, either S=2 Fe2+ or S=5/2 Mn2+ is on the B site, while nonmagnetic Na and Ca (Na and Sr) are disordered on the A site. The materials, which were grown as crystals via the floating zone method, display high effective magnetic moments and large Curie-Weiss thetas. Despite these characteristics, freezing of the magnetic spins, characterized by peaks in the susceptibility or specific heat, is not observed until low temperatures. The empirical frustration index, f=- {\theta}cw/Tf, for the materials are 36 (NaSrMn2F7), 27 (NaSrFe2F7), and 19 (NaCaFe2F7). AC susceptibility, DC susceptibility, and heat capacity measurements are used to characterize the observed spin glass behavior. The results suggest that the compounds are frustrated pyrochlore antiferromagnets with weak bond disorder. The magnetic phenomena that these fluoride pyrochlores exhibit, in addition to their availability as relatively large single crystals, make them promising candidates for the study of geometric magnetic frustration.

Optical measurements and band structure calculations are reported on 3D Dirac materials. The electronic properties associated with the Dirac cone are identified in the reflectivity spectra of Cd$_3$As$_2$ and Na$_3$Bi single crystals. In Na$_3$Bi, the plasma edge is found to be strongly temperature dependent due to thermally excited free carriers in the Dirac cone. The thermal behavior provides an estimate of the Fermi level $E_F=25$ meV and the z-axis Fermi velocity $v_z = 0.3 \text{ eV} \AA$ associated with the heavy bismuth Dirac band. At high energies above the $\Gamma$-point Lifshitz gap energy, a frequency and temperature independent $\epsilon_2$ indicative of Dirac cone interband transitions translates into an ab-plane Fermi velocity of $3 \text{ eV} \AA$. The observed number of IR phonons rules out the $\text{P}6_3\text{/mmc}$ space group symmetry but is consistent with the $\text{P}\bar{3}\text{c}1$ candidate symmetry. A plasmaron excitation is discovered near the plasmon energy that persists over a broad range of temperature. The optical signature of the large joint density of states arising from saddle points at $\Gamma$ is strongly suppressed in Na$_3$Bi consistent with band structure calculations that show the dipole transition matrix elements to be weak due to the very small s-orbital character of the Dirac bands. In Cd$_3$As$_2$, a distinctive peak in reflectivity due to the logarithmic divergence in $\epsilon_1$ expected at the onset of Dirac cone interband transitions is identified. The center frequency of the peak shifts with temperature quantitatively consistent with a linear dispersion and a carrier density of $n=1.3\times10^{17}\text{ cm}^{-3}$. The peak width gives a measure of the Fermi velocity anisotropy of $10\%$, indicating a nearly spherical Fermi surface. The lineshape gives an upper bound estimate of 7 meV for the potential fluctuation energy scale., Comment: 15 pages, 6 figures, 3 tables

We present results of $^{23}$Na and $^{19}$F nuclear magnetic resonance (NMR) measurements on NaCaCo$_2$F$_7$, a frustrated pyrochlore magnet with a Curie-Weiss temperature, $T_{cw}$ ~-140 K, and intrinsic bond disorder. Below 3.6 K both the $^{23}$Na and $^{19}$F spectra broaden substantially in comparison to higher temperatures accompanied by a considerable reduction (80 \%) of the NMR signal intensity: This proves a broad quasi-static field distribution. The $^{19}$F spin-lattice relaxation rate $^{19}(1/T_1$) exhibits a peak at 2.9 K already starting to develop below 10 K. We attribute the spin freezing to the presence of bond disorder. This is corroborated by large-scale Monte-Carlo simulations of a classical bond-disordered XY model on the pyrochlore lattice. The low freezing temperature, together with the very short magnetic correlation length not captured by the simulations, suggesting that quantum effects play a decisive role in NaCaCo$_2$F$_7$., Comment: 11 pages, 11 figures, Substantial changes have been made

The recent discovery of extreme magnetoresistance in LaSb introduced lanthanum monopnictides as a new platform to study topological semimetals (TSMs). In this work we report the discovery of extreme magnetoresistance in LaBi, confirming lanthanum monopnictides as a promising family of TSMs. These binary compounds with the simple rock-salt structure are ideal model systems to search for the origin of extreme magnetoresistance. Through a comparative study of magnetotransport effects in LaBi and LaSb, we construct a triangular temperature-field phase diagram that illustrates how a magnetic field tunes the electronic behavior in these materials. We show that the triangular phase diagram can be generalized to other topological semimetals with different crystal structures and different chemical compositions. By comparing our experimental results to band structure calculations, we suggest that extreme magnetoresistance in LaBi and LaSb originates from a particular orbital texture on their qasi-2D Fermi surfaces. The orbital texture, driven by spin-orbit coupling, is likely to be a generic feature of various topological semimetals., Comment: 9 pages, 11 figures

The niobium rich selenide compound Nb5Se4 was synthesized at ambient pressure by high-temperature solid-state reaction in a sealed Ta tube. Resistivity and heat capacity measurements reveal that this compound is superconducting, with a T_c = 1.85K. The electronic contribution to the specific heat {\gamma} and the Debye temperature are found to be 18.1 mJ/mol/K^2 and 298 K respectively. The calculated electron-phonon coupling constant {\lambda}_ep = 0.5 and the {\Delta}C_p/{\gamma}Tc = 1.42 ratio imply that Nb5Se4 is a weak coupling BCS superconductor. The upper critical field and coherence length are found to be 1.44 T and 15.1 nm, respectively.

NaCaNi$_2$F$_7$ is an insulating, frustrated A$_2$B$_2$F$_7$ pyrochlore with magnetic S = 1 Ni$^{2+}$ on the pyrochlore B site. Non-magnetic Na and Ca are disordered on the A-site. Magnetic susceptibility measurements made on an oriented single crystal, grown in a floating zone furnace, show isotropic behavior at temperatures between 5 and 300 K, with an effective moment of 3.7 $\mu_B$/Ni. Despite displaying a large Curie-Weiss theta (-129 K), spin-ordering-related features are not seen in the susceptibility or specific heat until a spin glass transition at 3.6 K. This yields an empirical frustration index of f = -${\theta}_{CW}$/T$_f$ $\approx$ 36. The spin glass behavior is substantiated by a shift of the freezing temperature with frequency in the AC susceptibility, bifurcation in the DC susceptibility, and by a broad maximum in the magnetic specific heat. The observations as made on large single crystals suggest that NaCaNi$_2$F$_7$ is likely a realization of a frustrated spin 1 pyrochlore antiferromagnet with weak bond disorder., Comment: 15 Pages, 5 Figures, 2 Tables

We report the crystal growth, crystal structure and basic magnetic properties of a new cobalt-based pyrochlore, NaSrCo$_2$F$_7$. Na and Sr are completely disordered on the non-magnetic large atom A sites, while magnetic S=3/2 Co$^{2+}$ fully occupies the pyrochlore lattice B sites. This system exhibits an isotropic magnetic susceptibility with strong antiferromagnetic interactions (${\theta}_{CW}$ = -127(1)), a large effective moment (${\rho_{eff}}$ = 5.9(1) ${\mu_B}$/Co) and no spin freezing until 3 K. Thus NaSrCo$_2$F$_7$ is a geometrically frustrated antiferromagnet with a frustration index f = -${\theta_{CW}}$/T$_f$ = 42. AC susceptibility, DC susceptibility, and heat capacity are utilized to characterize the spin freezing at low temperatures. We propose that NaSrCo$_2$F$_7$, compared here to the related material NaCaCo$_2$F$_7$, may be the realization of a frustrated pyrochlore antiferromagnet with weak bond disorder. The strong magnetic frustration at an easily accessible temperature and the availability of large single crystals make this one of the potentially interesting alternatives to the more commonly studied rare earth oxide pyrochlores., Comment: 14 pages, 5 figures, 2 tables

We employ the chemical fragment formalism to perform a targeted superconductor search in the Nb-Ru-B system, yielding the orthorhombic metal-rich boride NbRuB, which displays BCS-like superconductivity with a Tc = 3.1 K. NbRuB is derived from the chemical fragments Nb3B2 + Ru3B, in which the Nb3B2 fragment contains B-B dimers and the Ru3B fragment contains isolated B atoms. A charge transfer occurs between the fragments. The results indicate that the fragment formalism is a useful chemical tool for the design of new intermetallic superconductors much the same way as the charge reservoir concept has been a useful chemical tool for the design of new copper oxide superconductors.

A topological Dirac semimetal is a novel state of quantum matter which has recently attracted much attention as an apparent 3D version of graphene. In this paper, we report critically important results on the electronic structure of the 3D Dirac semimetal Na3Bi at a surface that reveals its nontrivial groundstate. Our studies, for the first time, reveal that the two 3D Dirac cones go through a topological change in the constant energy contour as a function of the binding energy, featuring a Lifshitz point, which is missing in a strict 3D analog of graphene (in other words Na3Bi is not a true 3D analog of graphene). Our results identify the first example of a band saddle point singularity in 3D Dirac materials. This is in contrast to its 2D analogs such as graphene and the helical Dirac surface states of a topological insulator. The observation of multiple Dirac nodes in Na3Bi connecting via a Lifshitz point along its crystalline rotational axis away from the Kramers point serves as a decisive signature for the symmetry-protected nature of the Dirac semimetal's topological groundstate., Comment: 5 pages, 4 Figures, Related papers on topological Fermi arcs and Weyl Semimetals (WSMs) are at http://physics.princeton.edu/zahidhasangroup/index.html

We report a corrected crystal structure for the CePt2In7 superconductor, refined from single crystal x-ray diffraction data. The corrected crystal structure shows a different Pt-In stacking along the c-direction in this layered material than was previously reported. In addition, all the atomic sites are fully occupied with no evidence of atom site mixing, resolving a discrepancy between the observed high resistivity ratio of the material and the atomic disorder present in the previous structural model The Ce-Pt distance and coordination is typical of that seen in all other reported Ce_nM_mIn_3n+2m compounds. Our band structure calculations based on the correct structure reveal three bands at the Fermi level that are more three dimensional than those previously proposed, and Density functional theory (DFT) calculations show that the new structure has a significantly lower energy., Comment: accepted by JPCM

The transverse Ising magnet Hamiltonian describing the Ising chain in a transverse magnetic field is the archetypal example of a system that undergoes a transition at a quantum critical point (QCP). The columbite CoNb$_2$O$_6$ is the closest realization of the transverse Ising magnet found to date. At low temperatures, neutron diffraction has observed a set of discrete collective spin modes near the QCP. We ask if there are low-lying spin excitations distinct from these relatively high energy modes. Using the heat capacity, we show that a significant band of gapless spin excitations exists. At the QCP, their spin entropy rises to a prominent peak that accounts for 30$\%$ of the total spin degrees of freedom. In a narrow field interval below the QCP, the gapless excitations display a fermion-like, temperature-linear heat capacity below 1 K. These novel gapless modes are the main spin excitations participating in, and affected, by the quantum transition., Comment: 14 pages total, 8 figures

We report the magnetic characterization of the frustrated transition metal pyrochlore NaCaCo$_2$F$_7$. This material has high spin Co$^{2+}$ in CoF$_6$ octahedra in a pyrochlore lattice, and disordered non-magnetic Na and Ca on the large-atom sites in the structure. Large crystals grown by the floating zone method were studied. The magnetic susceptibility is isotropic, the Co moment is larger than the spin-only value, and in spite of the large Curie Weiss theta (-140 K), freezing of the spin system, as characterized by peaks in the ac and dc susceptibility and specific heat, does not occur until around 2.4 K. This yields a frustration index of f = $-\theta_{CW}$/$T_f$ $\approx$ 56, an indication that the system is highly frustrated. The observed entropy loss at the freezing transition is low, indicating that magnetic entropy remains present in the system at 0.6 K. The compound may be the realization of a frustrated pyrochlore antiferromagnet with weak bond disorder. The high magnetic interaction strength, strong frustration, and the availability of large single crystals makes NaCaCo$_2$F$_7$ an interesting alternative to rare earth oxide pyrochlores for the study of geometric magnetic frustration in pyrochlore lattices., Comment: Submitted to PRL; 14 pages, 4 figures, 2 tables

Resistivity, dc magnetization, and heat capacity measurements are reported for superconducting NaBi. Tc, the electronic contribution to the specific heat {\gamma}, the {\Delta}Cp/{\gamma}Tc ratio, and the Debye temperature are found to be 2.15 K, 3.4 mJmol-1K-2, 0.78, and 140 K respectively. The calculated electron-phonon coupling constant ({\lambda}ep = 0.62) implies that NaBi is a moderately coupled superconductor. The upper critical field and coherence length are found to be 250 Oe and 115 nm, respectively. Electronic structure calculations show NaBi to be a good metal, in agreement with the experiments; the px and py orbitals of Bi dominate the electronic states at the Fermi Energy., Comment: 14 pages, 5 figures

Symmetry or topology protected Dirac fermion states in two and three dimensions constitute novel quantum systems that exhibit exotic physical phenomena. However, none of the studied spin-orbit materials are suitable for realizing bulk multiplet Dirac states for the exploration of interacting Dirac physics. Here we present experimental evidence, for the first time, that the compound Na3Bi hosts a bulk spin-orbit Dirac multiplet and their interaction or overlap leads to a Lifshitz transition in momentum space - a condition for realizing interactions involving Dirac states. By carefully preparing the samples at a non-natural-cleavage (100) crystalline surface, we uncover many novel electronic and spin properties in Na3Bi by utilizing high resolution angle- and spin-resolved photoemission spectroscopy measurements. We observe two bulk 3D Dirac nodes that locate on the opposite sides of the bulk zone center point $\Gamma$, which exhibit a Fermi surface Lifshitz transition and a saddle point singularity. Furthermore, our data shows evidence for the possible existence of theoretically predicted weak 2D nontrivial spin-orbit surface state with helical spin polarization that are nestled between the two bulk Dirac cones, consistent with the theoretically calculated (100) surface-arc-modes. Our main experimental observation of a rich multiplet of Dirac structure and the Lifshitz transition opens the door for inducing electronic instabilities and correlated physical phenomena in Na3Bi, and paves the way for the engineering of novel topological states using Na3Bi predicted in recent theory., Comment: 23 pages, 5 Figures

We report the structural and magnetic characterizations of Ba3TeCo3P2O14, Pb3TeCo3P2O14, and Pb3TeCo3V2O14, compounds that are based on the mineral Dugganite, which is isostructural to Langasites. The magnetic part of the structure consists of layers of Co2+ triangles. Nuclear and magnetic structures were determined through a co-refinement of synchrotron and neutron powder diffraction data. In contrast to the undistorted P321 Langasite structure of Ba3TeCo3P2O14, a complex structural distortion yielding a large supercell is found for both Pb3TeCo3P2O14 and Pb3TeCo3V2O14. Comparison of the three compounds studied along with the zinc analog Pb3TeZn3P2O14, also characterized here, suggests that the distortion is driven by Pb2+ lone pairs; as such, the Pb compounds crystallize in a pyroelectric space group, P2. Magnetic susceptibility, magnetization, and heat capacity measurements were performed to characterize the magnetic behavior. All three compounds become antiferromagnetic with N\'eel temperatures TN ~ 21 K (Ba3TeCo3P2O14), ~ 13 K (Pb3TeCo3P2O14), and ~ 8 K (Pb3TeCo3V2O14), and they exhibit magnetic transitions at high applied magnetic fields, suggesting intrinsically complex magnetic behavior for tetrahedrally coordinated d7 Co2+ in this structure type., Comment: Submitted to Chemistry of Materials, 37 double spaced pages, 8 tables, 12 figures