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Large, high-purity single-crystals of hexagonal BN (h-BN) are essential for exploiting its many desirable and interesting properties. Here, we demonstrate via X-ray tomography, X-ray diffraction and scanning electron microscopy that h-BN crystals can be grown by traveling-solvent floating-zone (TSFZ). The diameters of grown boules range from 3 -- 5 mm with lengths from 2 -- 7 mm. Tomography indicates variable grain sizes within the boules, with the largest having areas of $\approx$ 1 mm $\times$ 2 mm and thickness $\approx$ 0.5 mm. Although the boules contain macroscale flux inclusions, the h-BN lattice itself is of high quality for samples grown under optimized conditions. The currently optimized growth procedure employs an Fe flux, moderate N$_2$ pressure ($P_{N2} \approx$ 6 bar), and a growth rate of 0.1 mm/h.Raman spectroscopy for an optimized sample gives an average linewidth of 7.7(2) cm$^{-1}$ for the $E_{2g}$ intralayer mode at 1365.46(4) cm$^{-1}$ and 1.0(1) cm$^{-1}$ for the $E_{2g}$ interlayer shear mode at 51.78(9) cm$^{-1}$. The corresponding photoluminescence spectrum shows sharp phonon-assisted free exciton peaks and minimal signal in the energy range corresponding to carbon-related defects ($E$ = 3.9 -- 4.1 eV). Our work demonstrates the viability of growing h-BN by the TSFZ technique, thereby opening a new route towards larger, high-quality crystals and advancing the state of h-BN related research., Comment: 12 pages, 6 figures + supplementary information. Submitted to J. Cryst. Growth

Beyond the quantum limit, many-body effects are expected to induce unusual electronic phase transitions. Materials possessing metallic ground states with strong interactions between localized and itinerant electronic states are natural candidates for the realization of such quantum phases. However, the electronic correlations responsible for increasing the likelihood of novel phases simultaneously place the quantum limit beyond the reach of laboratory magnets. Here we propose these difficulties can be surmounted in materials with strong correlations and insulating ground states. Strong correlations in insulators and high magnetic fields conspire to fill Landau levels in the reverse order compared to conventional metals, such that the lowest Landau level is the first observed. Consequently, the quantum limit in strongly correlated insulators is reached in reverse and at fields accessible in laboratories. Quantum oscillations measured at high fields in YbB12 are shown to have features consistent with the reverse quantum limit. These include how quantum oscillations move in lock step with the angular evolution of the insulator-metal transition and the field dependence of the quantum oscillation frequency. We argue that close to the insulator-metal transition, the insulating state should be viewed through the lens of a magnetic field-induced electronic instability affecting the lowest Landau level states in the quantum limit.

Kondo insulators are predicted to undergo an insulator-to-metal transition under applied magnetic field, yet the extremely high fields required to date have prohibited a comprehensive investigation of the nature of this transition. Here we show that Ce3Bi4Pd3 provides an ideal platform for this investigation, owing to the unusually small magnetic field of B ~ 11 T required to overcome its Kondo insulating gap. Above Bc, we find a magnetic field-induced Fermi liquid state whose characteristic energy scale T_FL collapses near Bc in a manner indicative of a magnetic field-tuned quantum critical point. A direct connection is established with the process of Kondo singlet formation, which yields a broad maximum in the magnetic susceptibility as a function of temperature in weak magnetic fields that evolves progressively into a sharper transition at Bc as T -> 0., Comment: 10 pages including 10 figures

A recurring theme in topological matter is the protection of unusual electronic states by symmetry, for example, protection of the surface states in Z2 topological insulators by time reversal symmetry [1-3]. Recently interest has turned to unusual surface states in the large class of nonsymmorphic materials [4-11]. In particular KHgSb is predicted to exhibit double quantum spin Hall (QSH) states [10]. Here we report observation of a novel feature of the Hall conductivity in KHgSb in strong magnetic field B. In the quantum limit, the Hall conductivity is observed to fall exponentially to zero, but the diagonal conductivity is finite. A large gap protects this unusual zero-Hall state. We propose that, in this limit, the chemical potential drops into the bulk gap, intersecting equal numbers of right and left-moving QSH surface modes to produce the zero-Hall state., Comment: 7 pages, 4 figures

In the Dirac/Weyl semimetal, the chiral anomaly appears as an "axial" current arising from charge-pumping between the lowest (chiral) Landau levels of the Weyl nodes, when an electric field is applied parallel to a magnetic field $\bf B$. Evidence for the chiral anomaly was obtained from the longitudinal magnetoresistance (LMR) in Na$_3$Bi and GdPtBi. However, current jetting effects (focussing of the current density $\bf J$) have raised general concerns about LMR experiments. Here we implement a litmus test that allows the intrinsic LMR in Na$_3$Bi and GdPtBi to be sharply distinguished from pure current jetting effects (in pure Bi). Current jetting enhances $J$ along the mid-ridge (spine) of the sample while decreasing it at the edge. We measure the distortion by comparing the local voltage drop at the spine (expressed as the resistance $R_{spine}$) with that at the edge ($R_{edge}$). In Bi, $R_{spine}$ sharply increases with $B$ but $R_{edge}$ decreases (jetting effects are dominant). However, in Na$_3$Bi and GdPtBi, both $R_{spine}$ and $R_{edge}$ decrease (jetting effects are subdominant). A numerical simulation allows the jetting distortions to be removed entirely. We find that the intrinsic longitudinal resistivity $\rho_{xx}(B)$ in Na$_3$Bi decreases by a factor of 10.9 between $B$ = 0 and 10 T. A second litmus test is obtained from the parametric plot of the planar angular magnetoresistance. These results strenghthen considerably the evidence for the intrinsic nature of the chiral-anomaly induced LMR. We briefly discuss how the squeeze test may be extended to test ZrTe$_5$., Comment: 17 pages, 8 figures, new co-authors added, new Fig. 6a added. In press, PRX

Nodal-line semimetals (NLSs) represent a new type of topological semimetallic beyond Weyl and Dirac semimetals in the sense that they host closed loops or open curves of band degeneracies in the Brillouin zone. Parallel to the classification of type-I and type-II Weyl semimetals, there are two types of NLSs. The conventional NLS phase, in which the two bands forming the nodal line have opposite signs for their slopes along any direction perpendicular to the nodal line, has been proposed and realized in many compounds, whereas the exotic type-II NLS is very rare. Our first-principles calculations show that Mg$_3$Bi$_2$ is a material candidate that hosts a single type-II nodal loop around $\Gamma$. The band crossing is close to the Fermi level and the two crossing bands have the same sign in their slopes along the radial direction of the loop, indicating the type-II nature of the nodal line. Spin-orbit coupling generates only a small energy gap ($\sim$35 meV) at the nodal points and does not negate the band dispersion of Mg$_3$Bi$_2$ that yields the type-II nodal line. Based on this prediction we have synthesized Mg$_3$Bi$_2$ single crystals and confirmed the presence of the type-II nodal lines in the material. Our angle-resolved photoemission spectroscopy (ARPES) measurements agree well with our first-principles results and thus establish Mg$_3$Bi$_2$ as an ideal materials platform for studying the exotic properties of type-II nodal line semimetals.

Single crystals of CrSbSe$_3$, a structurally pseudo-one-dimensional ferromagnetic semiconductor, were grown using a high-temperature solution growth technique and were characterized by x-ray diffraction, anisotropic, temperature- and field-dependent magnetization, temperature-dependent resistivity and optical absorption measurements. A band gap of 0.7 eV was determined from both resistivity and optical measurements. At high temperatures, CrSbSe$_3$ is paramagnetic and isotropic with a Curie-Weiss temperature of $\sim$145 K and an effective moment of $\sim$4.1 $\mu_B$/Cr. A ferromagnetic transition occurs at $T_c$ = 71 K. The $a$-axis, perpendicular to the chains in the structure, is the magnetic easy axis, while the chain axis direction, along $b$, is the hard axis. Magnetic isotherms measured around $T_c$ do not follow the behavior predicted by simple mean field critical exponents for a second order phase transition. A tentative set of critical exponents is estimated based on a modified Arrott plot analysis, giving $\beta\sim$0.25, $\gamma\sim$1.38 and $\delta\sim$6.6., Comment: 6 pages, 7 figures

Half-metals are a class of materials that are metallic only for one spin direction, and are essential for spintronics applications where one needs to read, write, store and transfer spin-data. This spin sensitivity appears to restrict them to be magnetic, and the known examples indeed are. The fabrication of real spintronic devices from such materials is often hampered, however, by stray magnetic fields, domain walls, short spin coherence times, scattering on magnetic atoms or magnetically active interfaces, and other characteristics that come along with the magnetism. The surfaces of topological insulators, or Dirac or Weyl semimetals, could be an alternative, but production of high-quality thin films without the presence of the bulk states at the Fermi level remains very challenging. Here we introduce non-magnetic half-metals and demonstrate that this state is realized in IrBiSe. Using angle-resolved photoemission spectroscopy and band structure calculations we find a record-high Dresselhaus spin-orbit splitting, fully spin-polarized remnant Fermi surfaces and a chiral 3D spin-texture, all with no magnetism present. Promising applications include using IrBiSe as a source of spin-polarized electrons, and lightly doped IrBiSe is expected to generate electric-field-controlled spin-polarized currents, free from back scattering, and could host triplet superconductivity.

The growth and characterization of CePtIn4, stabilized by 10% Zn substitution for In, is reported. The new material is orthorhombic, space group Cmcm (No. 63), with lattice parameters a = 4.51751(4) {\AA}, b = 16.7570(2) {\AA}, and c = 7.36682(8) {\AA}, and the refined crystal composition has 10% of Zn substituted for In, i.e. the crystals are CePt(In3.6Zn0.1)4. Crystals were grown using a self-flux method: only growths containing Zn yielded CePtIn4 crystals, while Ce3Pt4In13 crystals formed when Zn was not present. Anisotropic temperature-dependent magnetic susceptibilities for single crystals show that Zn-stabilized CePtIn4 orders magnetically at ~1.9 K. High-temperature Curie-Weiss fits indicate an effective moment of ~2.30 muB/ Ce and a directionally averaged Weiss-temperature of approximately - 9 K. Specific heat data shows a peak consistent with the ordering temperature seen in the magnetic susceptibility data. Zn-stabilized CePtIn4 is metallic and displays no superconducting transition down to 0.14 K., Comment: 8 pages, 5 figures, 1 table

In this work, the magneto-resistance (MR) of ultra-thin WTe2/BN heterostructures far away from electron-hole equilibrium is measured. The change of MR of such devices is found to be determined largely by a single tunable parameter, i.e. the amount of imbalance between electrons and holes. We also found that the magnetoresistive behavior of ultra-thin WTe2 devices is well-captured by a two-fluid model. According to the model, the change of MR could be as large as 400,000%, the largest potential change of MR among all materials known, if the ultra-thin samples are tuned to neutrality when preserving the mobility of 167,000 cm2V-1s-1 observed in bulk samples. Our findings show the prospects of ultra-thin WTe2 as a variable magnetoresistance material in future applications such as magnetic field sensors, information storage and extraction devices, and galvanic isolators. The results also provide important insight into the electronic structure and the origin of the large MR in ultra-thin WTe2 samples., Comment: 13 pages, 6 figures and Supporting Information appended

The picture of how a gap closes in a semiconductor has been radically transformed by topological concepts. Instead of the gap closing and immediately re-opening, topological arguments predict that, in the absence of inversion symmetry, a metallic phase protected by Weyl nodes persists over a finite interval of the tuning parameter (e.g. pressure $P$) . The gap re-appears when the Weyl nodes mutually annihilate. We report evidence that Pb$_{1-x}$Sn$_x$Te exhibits this topological metallic phase. Using pressure to tune the gap, we have tracked the nucleation of a Fermi surface droplet that rapidly grows in volume with $P$. In the metallic state we observe a large Berry curvature which dominates the Hall effect. Moreover, a giant negative magnetoresistance is observed in the insulating side of phase boundaries, in accord with \emph{ab initio} calculations. The results confirm the existence of a topological metallic phase over a finite pressure interval., Comment: 16 pages, 11 figures, 1 table

Following the intense studies on topological insulators, significant efforts have recently been devoted to the search for gapless topological systems. These materials not only broaden the topological classification of matter but also provide a condensed matter realization of various relativistic particles and phenomena previously discussed mainly in high energy physics. Weyl semimetals host massless, chiral, low-energy excitations in the bulk electronic band structure, whereas a symmetry protected pair of Weyl fermions gives rise to massless Dirac fermions. We employed scanning tunneling microscopy/spectroscopy to explore the behavior of electronic states both on the surface and in the bulk of topological semimetal phases. By mapping the quasiparticle interference and emerging Landau levels at high magnetic field in Dirac semimetals Cd$_3$As$_2$ and Na$_3$Bi, we observed extended Dirac-like bulk electronic bands. Quasiparticle interference imaged on Weyl semimetal TaAs demonstrated the predicted momentum dependent delocalization of Fermi arc surface states in the vicinity of the surface-projected Weyl nodes.

Superconductivity is observed with critical temperature $T_{c}$ = 2.0 K in self-flux-grown single crystals of $CaBi_{2}$. This material adopts the $ZrSi_{2}$ structure type with lattice parameters a = 4.696(1) $\AA$, b = 7.081(2) $\AA$ and c = 4.611(1) $\AA$. The crystals of $CaBi_{2}$ were studied by means of magnetic susceptibility, specific heat and electrical resistivity measurements. The heat capacity jump at $T_{c}$ is $\Delta C/\gamma T_{c}$ = 1.41, confirming bulk superconductivity; the Sommerfeld coefficient $\gamma$ = 4.1 $mJ\: mol^{-1}\, K^{-2}$ and the Debye temperature $\Theta_{D}$ = 157 K. The electron-phonon coupling strength is $\lambda_{el-ph}$ = 0.59, and the thermodynamic critical field $H_{c}$ is low, between 111 and 124 Oe $CaBi_{2}$ is a moderate coupling type-I superconductor. Results of electronic structure calculations are reported and charge densities, electronic bands, densities of states and Fermi surfaces are discussed, focusing on the effects of spin\textendash orbit coupling and electronic property anisotropy. We find a mixed quasi-2D + 3D character in the electronic structure, which reflects the layered crystal structure of the material., Comment: 9 pages, 11 figures + Supplementary Material (4 pages, 3 figures); accepted for publication in Physical Chemistry Chemical Physics

Discovering Dirac fermions with novel properties has become an important front in condensed matter and materials sciences. Here, we report the observation of unusual Dirac fermion states in a strongly-correlated electron setting, which are uniquely distinct from those of graphene and conventional topological insulators. In strongly-correlated cerium monopnictides, we find two sets of highly anisotropic Dirac fermions that interpenetrate each other with negligible hybridization, and show a peculiar four-fold degeneracy where their Dirac nodes overlap. Despite the lack of protection by crystalline or time-reversal symmetries, this four-fold degeneracy is robust across magnetic phase transitions. Comparison of these experimental findings with our theoretical calculations suggests that the observed surface Dirac fermions arise from bulk band inversions at an odd number of high-symmetry points, which is analogous to the band topology which describes a $\mathbb{Z}_{2}$-topological phase. Our findings open up an unprecedented and long-sought-for platform for exploring novel Dirac fermion physics in a strongly-correlated semimetal.

The Dirac and Weyl semimetals are unusual materials in which the nodes of the bulk states are protected against gap formation by crystalline symmetry. The chiral anomaly~\cite{Adler,Bell}, predicted to occur in both systems, was recently observed as a negative longitudinal magnetoresistance (LMR) in Na$_3$Bi and in TaAs. An important issue is whether Weyl physics appears in a broader class of materials. We report evidence for the chiral anomaly in the half-Heusler GdPtBi. In zero field, GdPtBi is a zero-gap semiconductor with quadratic bands. In a magnetic field, the Zeeman energy leads to Weyl nodes. We have observed a large negative LMR with the field-steering properties specific to the chiral anomaly. The chiral anomaly also induces strong suppression of the thermopower. We report a detailed study of the thermoelectric response function $\alpha_{xx}$ of Weyl fermions. The scheme of creating Weyl nodes from quadratic bands suggests that the chiral anomaly may be observable in a broad class of semimetals., Comment: 8 pages, 4 figures (Added Supplement with 11 additional pages and 14 new figures)

We report a reinvestigation of superconducting Sn$_{1-x}$In$_{x}$Te at both low and high In doping levels. Analysis of the superconductivity reveals a fundamental change as a function of \textit{x}: the system evolves from a weakly coupled to a strongly coupled superconductor with increasing indium content. Hall Effect measurements further show that the carrier density does not vary linearly with Indium content; indeed at high Indium content, the samples are overall \textit{n}-type, which is contrary to expectations of the standard picture of In$^{1+}$ replacing Sn$^{2+}$ in this material. Density functional theory calculations probing the electronic state of In in SnTe show that it does not act as a trivial hole dopant, but instead forms a distinct, partly filled In 5\textit{s} - Te 5\textit{p} hybridized state centered around E$_F$, very different from what is seen for other nominal hole dopants such as Na, Ag, and vacant Sn sites. We conclude that superconducting In-doped SnTe therefore cannot be considered as a simple hole doped semiconductor., Comment: 12 pages and 7 figures

In this talk, we describe recent experimental progress in detecting the chiral anomaly in the Dirac semimetal Na$_3$Bi in the presence of a magnetic field. The chiral anomaly, which plays a fundamental role in chiral gauge theories, was predicted to be observable in crystals by Nielsen and Ninomiya in 1983 [1]. Theoretical progress in identifying and investigating Dirac and Weyl semimetals has revived strong interest in this issue [2-6]. In the Dirac semimetal, the breaking of time-reversal symmetry by a magnetic field $\bf B$ splits each Dirac node into two chiral Weyl nodes. If an electric field $\bf E$ is applied parallel to $\bf B$, charge is predicted to flow between the Weyl nodes. We report the observation in the Dirac semimetal Na$_3$Bi of a novel, negative and highly anisotropic magnetoresistance (MR). We show that the enhanced conductivity has the form of a narrowly defined plume that can be steered by the applied field. The novel MR is acutely sensitive to deviations of $\bf B$ from $\bf E$, a feature incompatible with conventional transport. The locking of the current plume to the field appears to be a defining signature of the chiral anomaly., Comment: 8 pages, 8 figures, based on a talk by NPO at APS March Meeting, San Antonio, 2015

Na3Bi is a Dirac semimetal with protected nodes that may be sensitive to the breaking of time-reversal invariance in a magnetic field B. We report experiments which reveal that both the conductivity and resistivity tensors exhibit robust anomalies in B. The resistivity $\rho_{xx}$ is B-linear up to 35 T, while the Hall angle exhibits an unusual profile approaching a step-function. The conductivities $\sigma_{xx}$ and $\sigma_{xy}$ share identical power-law dependences at large B. We propose that these significant deviations from conventional transport result from an unusual sensitivity of the transport lifetime to B. Comparison with Cd3As2 is made., Comment: 8 pages, 5 figures

High quality hexagon plate-like Na3Bi crystals with large (001) plane surfaces were grown from a molten Na flux. The freshly cleaved crystals were analyzed by low temperature scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES), allowing for the characterization of the three-dimensional (3D) Dirac semimetal (TDS) behavior and the observation of the topological surface states. Landau levels (LL) were observed, and the energy-momentum relations exhibited a linear dispersion relationship, characteristic of the 3D TDS nature of Na3Bi. In transport measurements on Na3Bi crystals the linear magnetoresistance and Shubnikov-de Haas (SdH) quantum oscillations are observed for the first time., Comment: To be published in a special issue of APL Materials

In a topological insulator, it is the electrons on the surface or edge that carry the signature of topology. Recently, a novel topological state has been proposed in metals or semimetals (gapless) whose band-structure is similar to that of a three-dimensional analog of graphene. However, to this date the signature of its topology remains an open question. We report the experimental discovery of a pair of polarized Fermi arc surface state modes in the form of a new type of two-dimensional polarized electron gas on the surfaces of Dirac semimetals. These Fermi arc surface states (FASS) are observed to connect across an even number of bulk band gapless nodes and found to have their spin uniquely locked to their momentum. We show that these states are distinctly different from the topological surface states (TSS) seen in all known topological insulators. Our observed exotic two-dimensional states not only uncover the novel topology of gapless Dirac metals (such as sodium tribismuth Na$_3$Bi) but also opens new research frontiers for the utilization of topological Fermi arc electron gases for a wide range of fundamental physics and spintronic studies., Comment: ScienceExpress (2014) adv.online, 18-Dec-2014; Related papers on the discovery of topological Fermi arcs and Weyl Semimetals (WSMs) are at http://physics.princeton.edu/zahidhasangroup/index_Lists.html