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Jason W. Krizan

Publications and source records attributed to Jason W. Krizan.

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Real-space investigation of short-range magnetic correlations in fluoride pyrochlores NaCaCo$_2$F$_7$ and NaSrCo$_2$F$_7$ with magnetic pair distribution function analysis

We present time-of-flight neutron total scattering and polarized neutron scattering measurements of the magnetically frustrated compounds NaCaCo$_2$F$_7$ and NaSrCo$_2$F$_7$, which belong to a class of recently discovered pyrochlore compounds based on transition metals and fluorine. The magnetic pair distribution function (mPDF) technique is used to analyze and model the total scattering data in real space. We find that a previously-proposed model of short-range XY-like correlations with a length scale of 10-15 Å, combined with nearest-neighbor collinear antiferromagnetic correlations, accurately describes the mPDF data at low temperature, confirming the magnetic ground state in these materials. This model is further verified by the polarized neutron scattering data. From an analysis of the temperature dependence of the mPDF and polarized neutron scattering data, we find that short-range correlations persist on the nearest-neighbor length scale up to 200 K, approximately two orders of magnitude higher than the spin freezing temperatures of these compounds. These results highlight the opportunity presented by these new pyrochlore compounds to study the effects of geometric frustration at relatively high temperatures, while also advancing the mPDF technique and providing a novel opportunity to investigate a genuinely short-range-ordered magnetic ground state directly in real space.

cond-mat.str-el

Imaging electronic states on topological semimetals using scanning tunneling microscopy

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.

cond-mat.mtrl-sci

Static and dynamic XY-like short-range order in a frustrated magnet with exchange disorder

A single crystal of the Co2+ based pyrochlore NaCaCo2F7 was studied by inelastic neutron scattering. This frustrated magnet with quenched exchange disorder remains in a strongly correlated paramagnetic state down to one 60th of the Curie-Weiss temperature. Below T_f = 2.4 K, diffuse elastic scattering develops and comprises 30 +/- 10% of the total magnetic scattering, as expected for J_{eff} = 1/2 moments frozen on a time scale that exceeds \hbar/δE=3.8 ps. The diffuse scattering is consistent with short range XY antiferromagnetism with a correlation length of 16 Å. The momentum (Q) dependence of the inelastic intensity indicates relaxing XY-like antiferromagnetic clusters at energies below ~ 5.5 meV, and collinear antiferromagnetic fluctuations above this energy. The relevant XY configurations form a continuous manifold of symmetry-related states. Contrary to well-known models that produce this continuous manifold, order-by-disorder does not select an ordered state in NaCaCo2F7 despite evidence for weak (~12 %) exchange disorder. Instead, NaCaCo2F7 freezes into short range ordered clusters that span this manifold.

cond-mat.str-el

Differences in chemical doping matter - Superconductivity in Ti1-xTaxSe2 but not in Ti1-xNbxSe2

We report that 1T-TiSe2, an archetypical layered transition metal dichalcogenide, becomes superconducting when Ta is substituted for Ti but not when Nb is substituted for Ti. This is unexpected because Nb and Ta should be chemically equivalent electron donors. Superconductivity emerges near x = 0.02 for Ti1-xTaxSe2, while for Ti1-xNbxSe2, no superconducting transitions are observed above 0.4 K. The equivalent chemical nature of the dopants is confirmed by X-ray photoelectron spectroscopy. ARPES and Raman scattering studies show similarities and differences between the two systems, but the fundamental reasons why the Nb and Ta dopants yield such different behavior are unknown. We present a comparison of the electronic phase diagrams of many electron-doped 1T-TiSe2 systems, showing that they behave quite differently, which may have broad implications in the search for new superconductors. We propose that superconducting Ti0.8Ta0.2Se2 will be suitable for devices and other studies based on exfoliated crystal flakes.

cond-mat.supr-con

Synthesis, crystal structure, and magnetic properties of RE3Sb3Mg2O14 (RE=La, Pr, Sm, Eu, Tb, Ho): new 2D Kagome materials

We present the crystal structures and magnetic properties of RE3Sb3Mg2O14 (La3Sb3Mg2O14, Pr3Sb3Mg2O14, Sm3Sb3Mg2O14, Eu3Sb3Mg2O14, Tb3Sb3Mg2O14, and Ho3Sb3Mg2O14), a family of novel materials based on a perfect geometry 2D rare earth Kagome lattice. Structure refinements were performed by the Rietveld method using X-ray diffraction data, indicating that the layered compounds are fully structurally ordered. The compounds crystallize in a rhombohedral supercell of the cubic pyrochlore structure, in the space group R-3m. As indicated by magnetic susceptibility measurements, they exhibit predominantly antiferromagnetic interactions between rare earth moments. Except for possibly Pr3Sb3Mg2O14 and Eu3Sb3Mg2O14, none of the compounds show any signs of magnetic ordering above 2 K. This RE3Sb3Mg2O14 family of compounds is similar to that of RE3Sb3Zn2O14, except the series reported here features a fully ordered distribution of cations in both the nonmagnetic antimony and magnesium sites and the magnetic rare earth kagome sites. The compounds appear to be relatively defect-free and are therefore model systems for investigating magnetic frustration on an ideal 2D rare earth Kagome lattice.

cond-mat.str-el

Signature of the chiral anomaly in a Dirac semimetal: a current plume steered by a magnetic field

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.

cond-mat.str-el

Gold-Gold Bonding: The Key to Stabilizing the 19-Electron Ternary Phases LnAuSb (Ln = La-Nd and Sm) as New Dirac Semimetals

We report a new family of ternary 111 hexagonal LnAuSb (Ln = La-Nd, Sm) compounds that, with a 19 valence electron count, has one extra electron compared to all other known LnAuZ compound. The "19th" electron is accommodated by Au-Au bonding between the layers; this Au-Au interaction drives the phases to crystallize in the YPtAs-type structure rather than the more common LiGaGe-type. This is critical, as the YPtAs structure type has the symmetry-allowed band crossing necessary for the formation of Dirac semimetals. Band structure, density of stats, and crystal orbital calculations confirm this picture, which results in a nearly complete band gap between full and empty electronic states and stable compounds; we can thus present a structural stability phase diagram for the LnAuZ (Ln = Ge, As, Sn, Sb, Pb, Bi) family of phases. Those calculations also show that LaAuSb has a bulk Dirac cone below the Fermi level. The YPtAs-type LnAuSb family reported here is an example of the uniqueness of gold chemistry applied to a rigidly closed shell system in an unconventional way.

cond-mat.str-el

Observation of Fermi Arc Surface States in a Topological Metal: A New Type of 2D Electron Gas beyond Z2 Topological Insulators

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.

cond-mat.mes-hall

Polytypism, polymorphism and superconductivity in TaSe2-xTex

Polymorphism in materials often leads to significantly different physical properties - the rutile and anatase polymorphs of TiO2 are a prime example. Polytypism is a special type of polymorphism, occurring in layered materials when the geometry of a repeating structural layer is maintained but the layer stacking sequence of the overall crystal structure can be varied; SiC is an example of a material with many polytypes. Although polymorphs can have radically different physical properties, it is much rarer for polytypism to impact physical properties in a dramatic fashion. Here we study the effects of polytypism and polymorphism on the superconductivity of TaSe2, one of the archetypal members of the large family of layered dichalcogenides. We show that it is possible to access 2 stable polytypes and 2 stable polymorphs in the TaSe2-xTex solid solution, and find that the 3R polytype shows a superconducting transition temperature that is nearly 17 times higher than that of the much more commonly found 2H polytype. The reason for this dramatic change is not apparent, but we propose that it arises either from a remarkable dependence of Tc on subtle differences in the characteristics of the single layers present, or from a surprising effect of the layer stacking sequence on electronic properties that instead are expected to be dominated by the properties of a single layer in materials of this kind.

cond-mat.supr-con

A large new family of filled skutterudites stabilized by electron count

Based on the interplay of theory and experiment, a large new family of filled group 9 (Co, Rh and Ir) skutterudites is designed and synthesized. The new materials fill the empty cages in the structures of the known binary CoSb3, RhSb3 and IrSb3 skutterudites with alkaline, alkaline earth, and rare earth atoms to create compounds of the type AyB4X12; A atoms fill the cages to a fraction y, B are the group 9 transition metals, and X is a mixture of electronegative main group elements chosen to achieve chemical stability by adjusting the electron counts to electron-precise values. Forty-three new compounds are reported, antimony-tin and phosphorous-silicon based, with 63 compositional variations presented. The new family of compounds is large and general. The results described here can be extended to the synthesis of hundreds of new group 9 filled skutterudites.

cond-mat.mtrl-sci

Bulk crystal growth and electronic characterization of the 3D Dirac Semimetal Na3Bi

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.

cond-mat.str-el

Thermal Hall conductivity in the frustrated pyrochlore magnet Tb2Ti2O7

In a ferromagnet, the spin excitations are the well-studied magnons. In frustrated quantum magnets, long-range magnetic order fails to develop despite a large exchange coupling between the spins. In contrast to the magnons in conventional magnets, their spin excitations are poorly understood. Are they itinerant or localized? Here we show that the thermal Hall conductivity $κ_{xy}$ provides a powerful probe of spin excitations in the "quantum spin ice" pyrochlore Tb$_2$Ti$_2$O$_7$. The thermal Hall response is large even though the material is transparent. The Hall response arises from spin excitations with specific characteristics that distinguish them from magnons. At low temperature ($T<$ 1 K), the thermal conductivity imitates that of a dirty metal. Using the Hall angle, we construct a phase diagram showing how the excitations are suppressed by a magnetic field.

cond-mat.str-el

The Chemical Instability of Na2IrO3 in Air

We report that Na2IrO3, which has a layered honeycomb iridium oxide sublattice interleaved by Na planes, decomposes in laboratory air while maintaining the same basic crystal structure. The decomposition reaction was monitored by time-dependent powder x-ray diffraction under different ambient atmospheres, through which it was determined that it occurs only in the simultaneous presence of both CO2 and H2O. A hydrated sodium carbonate is the primary decomposition product along with altered Na2IrO3. The diffraction signature of the altered Na2IrO3 is quite similar to that of the pristine material, which makes the detection of decomposition difficult in a sample handled under ordinary laboratory conditions. The decomposed samples show a significantly decreased magnetic susceptibility and the disappearance of the low temperature antiferromagnetic transition considered to be characteristic of the phase. Samples that have never been exposed to air after synthesis display a previously unreported magnetic transition at 5K.

cond-mat.mtrl-sci