Quinn Gibson

Large, non-saturating magnetoresistance in WTe2

Magnetoresistance is the change in a material’s electrical resistance in response to an applied magnetic field. Materials with large magnetoresistance have found use as magnetic sensors, in magnetic memory, and in hard drives at room temperature, and their rarity has motivated many fundamental studies in materials physics at low temperatures. Here we report the observation of an extremely large positive magnetoresistance at low temperatures in the non-magnetic layered transition-metal dichalcogenide WTe2: 452,700 per cent at 4.5 kelvins in a magnetic field of 14.7 teslas, and 13 million per cent at 0.53 kelvins in a magnetic field of 60 teslas. In contrast with other materials, there is no saturation of the magnetoresistance value even at very high applied fields. Determination of the origin and consequences of this effect, and the fabrication of thin films, nanostructures and devices based on the extremely large positive magnetoresistance of WTe2, will represent a significant new direction in the study of magnetoresistivity.Magnetoresistance is the change of a material’s electrical resistance in response to an applied magnetic field. In addition to its intrinsic scientific interest, it is a technologically important property, placing it in “Pasteur’s quadrant” of res earch value: materials with large magnetorsistance have found use as magnetic sensors 1, in magnetic memory2, hard drives3, transistors4, and are the subject of frequent study in the field of spintronics5, 6. Here we report the observation of an extremely large one-dimensional posi tive magnetoresistance (XMR) in the layered transition metal dichalcogenide (TMD) WTe2; 452,700% at 4.5 Kelvin in a magnetic field of 14.7 Tesla, and 2.5 million% at 0.4 Kelvin in 45 Tesla, with no saturation. The XMR is highly anisotropic, maximized in the crystallographic direction where small pockets of holes and electrons are found in the electronic structure . The determination of the origin of this effect and the fabrication of nanostructures and devices based on the XMR of WTe2 will represent a significant new direction in the study and uses of magnetoresistivity.

Experimental realization of a three-dimensional Dirac semimetal.

We report the direct observation of the three-dimensional (3D) Dirac semimetal phase in cadmium arsenide (Cd(3)As(2)) by means of angle-resolved photoemission spectroscopy. We identify two momentum regions where electronic states that strongly disperse in all directions form narrow conelike structures, and thus prove the existence of the long sought 3D Dirac points. This electronic structure naturally explains why Cd(3)As(2) has one of the highest known bulk electron mobilities. This realization of a 3D Dirac semimetal in Cd(3)As(2) not only opens a direct path to a wide spectrum of applications, but also offers a robust platform for engineering topologically nontrivial phases including Weyl semimetals and quantum spin Hall systems.

Landau quantization and quasiparticle interference in the three-dimensional Dirac semimetal Cd3As2

Condensed-matter systems provide a rich setting to realize Dirac and Majorana fermionic excitations as well as the possibility to manipulate them for potential applications. It has recently been proposed that chiral, massless particles known as Weyl fermions can emerge in certain bulk materials or in topological insulator multilayers and give rise to unusual transport properties, such as charge pumping driven by a chiral anomaly. A pair of Weyl fermions protected by crystalline symmetry effectively forming a massless Dirac fermion has been predicted to appear as low-energy excitations in a number of materials termed three-dimensional Dirac semimetals. Here we report scanning tunnelling microscopy measurements at sub-kelvin temperatures and high magnetic fields on the II-V semiconductor Cd3As2. We probe this system down to atomic length scales, and show that defects mostly influence the valence band, consistent with the observation of ultrahigh-mobility carriers in the conduction band. By combining Landau level spectroscopy and quasiparticle interference, we distinguish a large spin-splitting of the conduction band in a magnetic field and its extended Dirac-like dispersion above the expected regime. A model band structure consistent with our experimental findings suggests that for a magnetic field applied along the axis of the Dirac points, Weyl fermions are the low-energy excitations in Cd3As2.

Resistivity plateau and extreme magnetoresistance in LaSb

Time reversal symmetry (TRS) protects the metallic surface modes of topological insulators (TIs). The transport signature of robust metallic surface modes of TIs is a plateau that arrests the exponential divergence of the insulating bulk with decreasing temperature. This universal behavior is observed in all TI candidates ranging from Bi2Te2Se to SmB6. Recently, several topological semimetals (TSMs) have been found that exhibit extreme magnetoresistance (XMR) and TI universal resistivity behavior revealed only when breaking TRS, a regime where TIs theoretically cease to exist. Among these new materials, TaAs and NbP are nominated for Weyl semimetal due to their lack of inversion symmetry, Cd3As2 is nominated for Dirac semimetal due to its linear band crossing at the Fermi level, and WTe2 is nominated for resonant compensated semimetal due to its perfect electron-hole symmetry. Here we introduce LaSb, a simple rock-salt structure material without broken inversion symmetry, without perfect linear band crossing, and without perfect electron-hole symmetry. Yet LaSb portrays all the exotic field induced behaviors of the aforementioned semimetals in an archetypal fashion. It shows (a) the universal TI resistivity with a plateau at 15 K, revealed by a magnetic field, (b) ultrahigh mobility of carriers in the plateau region, (c) quantum oscillations with a non-trivial Berry phase, and (d) XMR of about one million percent at 9 tesla rivaled only by WTe2 and NbP. Due to its dramatic simplicity, LaSb is the ideal model system to formulate a theoretical understanding of the exotic consequences of breaking TRS in TSMs.

p-Type CuRhO2 as a Self-Healing Photoelectrode for Water Reduction under Visible Light

Polycrystalline CuRhO2 is investigated as a photocathode for the splitting of water under visible irradiation. The band edge positions of this material straddle the water oxidation and reduction redox potentials. Thus, photogenerated conduction band electrons are sufficiently energetic to reduce water, while the associated valence band holes are energetically able to oxidize water to O2. Under visible illumination, H2 production is observed with ~0.2 V underpotential in an air-saturated solution. In contrast, H2 production in an Ar-saturated solution was found to be unstable. This instability is associated with the reduction of the semiconductor forming Cu(s). However, in the presence of air or O2, bulk Cu(s) was not detected, implying that CuRhO2 is self-healing when air is present. This property allows for the stable formation of H2 with ca. 80% Faradaic efficiency.

The Crystal and Electronic Structures of Cd3As2, the Three-Dimensional Electronic Analogue of Graphene

The structure of Cd3As2, a high-mobility semimetal reported to host electrons that act as Dirac particles, is reinvestigated by single-crystal X-ray diffraction. It is found to be centrosymmetric rather than noncentrosymmetric as previously reported. It has a distorted superstructure of the antifluorite (M2X) structure type with a tetragonal unit cell of a = 12.633(3) and c = 25.427(7) Å in the centrosymmetric I41/acd space group. The antifluorite superstructure can be envisioned as consisting of distorted Cd6□2 cubes (where □ = an empty cube vertex) in parallel columns, stacked with opposing chirality. Electronic structure calculations performed using the experimentally determined centrosymmetric structure are similar to those performed with the inversion symmetry absent but with the important implication that Cd3As2 is a three-dimensional (3D)-Dirac semimetal with no spin splitting; all bands are spin degenerate and there is a 4-fold degenerate bulk Dirac point at the Fermi energy along Γ-Z in the Brillouin zone. This makes Cd3As2 a 3D electronic analogue of graphene. Scanning tunneling microscopy experiments identify a 2 × 2 surface reconstruction in the (112) cleavage plane of single crystals; needle crystals grow with a [110] long axis direction.This is a revised version of a manuscript that was originally posted here in February of 2014. It has been accepted at the journal Inorganic Chemistry after reviews that included those of two crystallographers who made sure all the ts were crossed and the is were dotted. The old work (from 1968) that said that Cd3As2 was noncentrosymmetric was mistaken, with the authors of that study making a type of error that in the 1980s became infamous in crystallography. As a result of the increased scrutiny of the issue of centrosymmetricity of the 1980s, there are now much better analysis tools to resolve the issue fully, and its important to understand that not just our crystals are centrosymmetric, even the old guys crystals were centrosymmetric (and by implication everyones are). There is no shame in having made that error back in the day and those authors would not find the current centrosymmetric result controversial; their paper is excellent in all other aspects. This manuscript describes how the structure is determined, explains the structure schematically, calculates the electronic structure based on the correct centrosymmetric crystal structure, and gives the structural details that should be used for future analysis and modeling.

Three-dimensional Dirac semimetals: Design principles and predictions of new materials

Design principles and novel predictions of new 3D Dirac semimetals are presented, along with the context of currently known materials. Current materials include those based on a topological to trivial phase transition, such as in TlBiSe

Crystal Structure and Chemistry of Topological Insulators

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Evidence for massive bulk Dirac fermions in Pb 1− x Sn x Se from Nernst and thermopower experiments

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Observation of the quantum spin Hall effect up to 100 kelvin in a monolayer crystal

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