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Anthony D. Rice

Publications and source records attributed to Anthony D. Rice.

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Toward Tunable Magnetic Dirac Semimetals: Mn Doping of Cd$_3$As$_2$

Magnetic impurities provide a route toward increasing functionality in electronic materials, often enabling new device concepts and architectures. In the case of topological semimetals, dilute magnetic doping presents a particularly attractive approach for inducing a Dirac to Weyl phase change via time reversal symmetry breaking. However, efforts to realize changes in the electronic structure have been limited by challenges in incorporating magnetic impurities into crystals with sufficiently high electron mobilities to detect them via transport or spectroscopic techniques. Here, we demonstrate incorporation of Mn into Cd$_3$As$_2$ Dirac semimetal thin films grown by molecular beam epitaxy (MBE). Using As-rich growth conditions and [001] oriented thin films, Mn compositions of >10% are achieved. Films contain uniform distributions of Mn with no evidence of secondary phases and exhibit electron mobilities greater than 10,000-30,000 cm$^2$/Vs up to 5% Mn. An evolution in the magnetization behavior along with the emergence of a second quantum oscillation frequency at low Mn concentrations provide preliminary evidence of Mn-induced changes in the electronic structure that are consistent with a Weyl phase. This work demonstrates the potential of magnetically doping topological semimetal thin films and a pathway for synthesizing them.

cond-mat.mtrl-sci

Interplay of Quasi-Quantum Hall Effect and Coulomb Disorder in Semimetals

Low carrier densities in topological semimetals (TSMs) enable the exploration of novel magnetotransport in the quantum limit (QL). Recent findings consistent with 3D quasi-quantum Hall effect (QQHE) have positioned TSMs as promising platforms for exploring 3D quantum Hall transport, but the lack of tunability in the Fermi level has thus far limited the ability to observe a QQHE signal. Here, we tune the defect concentrations in the Dirac semimetal Cd${}_3$As${}_2$ to achieve ultra-low carrier concentrations at 2 K around $2.9\times10^{16}$cm${}^{-3}$, giving way to QQHE signal at modest fields near 10 T. At low carrier densities, where QQHE is most accessible, we find that clear QQHE is obscured by a carrier density dependent background originating from Coulomb disorder from charged point defects and Landau level broadening. Our results highlight the interplay between QQHE and Coulomb disorder, demonstrating that clear observation of QQHE in TSMs intricately depends on Fermi level and disorder magnitudes. We find that Coulomb disorder, as theoretically predicted, is an essential ingredient for understanding the magnetoresistivity for a spectrum of Fermi levels in Cd${}_3$As${}_2$, anchoring the role of defects and charged disorder in TSM applications. We discuss future constraints and opportunities in exploring 3D QQHE and quantum Hall effects in TSMs.

cond-mat.mtrl-sci

Thin film TaAs: developing a platform for Weyl semimetal devices

MX monopnictide compounds (M=Nb,Ta, X = As,P) are prototypical three-dimensional Weyl semimetals (WSMs) that have been shown in bulk single crystal form to have potential for a wide variety of novel devices due to topologically protected band structures and high mobilities. However, very little is known about thin film synthesis, which is essential to enable device applications. We synthesize TaAs(001) epilayers by molecular beam epitaxy on GaAs(001) and provide an experimental phase diagram illustrating conditions for single phase, single-crystal-like growth. We investigate the relationship between nanoscale defects and electronic structure, using angle-resolved photoemission spectroscopy, Kelvin probe microscopy and transmission electron microscopy. Our results provide a roadmap and platform for developing 3D WSMs for device applications.

cond-mat.mtrl-sci

Direct link between disorder, mobility and magnetoresistance in topological semimetals

The extent to which disorder influences the properties of topological semimetals remains an open question and is relevant to both the understanding of topological states and the use of topological materials in practical applications. Here, we achieve unmatched and systematic control of point defect concentrations in the prototypical Dirac semimetal Cd$_3$As$_2$ to gain important insight into the role of disorder on electron transport behavior. We find that arsenic vacancies introduce localized states near the Fermi level and strongly influence the electron mobility. Reducing arsenic vacancies by changing the As/Cd flux ratio used during deposition results in an increase in the magnetoresistance from 200%-1000% and an increase in mobility from 5000-18,000 cm$^2$/Vs. However, the degree of linear magnetoresistance, which has previously been linked to disorder, is found here to correlate inversely with measures of disorder, including disorder potential and disorder correlation lengths. This finding yields important new information in the quest to identify the origin of linear magnetoresistance in a wider range of materials.

cond-mat.mtrl-sci

Surface Reconstructions of Heusler Compounds in the Ni-Ti-Sn (001) System

As progress is made on thin-film synthesis of Heusler compounds, a more complete understanding of the surface will be required to control their properties, especially as functional heterostructures are explored. Here, the surface reconstructions of semiconducting half-Heusler NiTiSn(001), and Ni1+xTiSn(001) (x=0.0-1.0) are explored as a way to optimize growth conditions during molecular beam epitaxy. Density functional theory (DFT) calculations were carried out to guide the interpretation of the experimental results. For NiTiSn(001) a c(2x2) surface reconstruction was observed for Sn rich samples, while a (1x1) unreconstructed surface was observed for Ti-rich samples. A narrow range around 1:1:1 stoichiometry exhibited a (2x1) surface reconstruction. Electrical transport is used to relate the observed reflection high energy electron diffraction (RHEED) pattern during and after growth with carrier concentration and stoichiometry. Scanning tunneling microscopy and RHEED were used to examine surface reconstructions, the results of which are in good agreement with density functional calculations. X-ray photoelectron spectroscopy was used to determine surface termination and stoichiometry. Atomic surface models are proposed, which suggest Sn-dimers form in reconstructed Ni1+xTiSn(001) half-Heusler surfaces (x<0.25) with a transition to Ni terminated surfaces for x > 0.25.

cond-mat.mtrl-sci

Growth, electrical, structural, and magnetic properties of half-Heusler CoTi$_{1-x}$Fe$_x$Sb

Epitaxial thin films of the substitutionally alloyed half-Heusler series CoTi$_{1-x}$Fe$_x$Sb were grown by molecular beam epitaxy on InAlAs/InP(001) substrates for concentrations 0.0$\leq$x$\leq$1.0. The influence of Fe on the structural, electronic, and magnetic properties was studied and compared to that expected from density functional theory. The films are epitaxial and single crystalline, as measured by reflection high-energy electron diffraction and X-ray diffraction. Using in-situ X-ray photoelectron spectroscopy, only small changes in the valence band are detected for x$\leq$0.5. For films with x$\geq$0.05, ferromagnetism is observed in SQUID magnetometry with a saturation magnetization that scales linearly with Fe content. A dramatic decrease in the magnetic moment per formula unit occurs when the Fe is substitutionally alloyed on the Co site indicating a strong dependence on the magnetic moment with site occupancy. A crossover from both in-plane and out-of-plane magnetic moments to only in-plane moment occurs for higher concentrations of Fe. Ferromagnetic resonance indicates a transition from weak to strong interaction with a reduction in inhomogeneous broadening as Fe content is increased. Temperature-dependent transport reveals a semiconductor to metal transition with thermally activated behavior for x$\leq$0.5. Anomalous Hall effect and large negative magnetoresistance (up to -18.5% at 100 kOe for x=0.3) are observed for higher Fe content films. Evidence of superparamagnetism for x=0.3 and x=0.2 suggests for moderate levels of Fe, demixing of the CoTi$_{1-x}$Fe$_x$Sb films into Fe rich and Fe deficient regions may be present. Atom probe tomography is used to examine the Fe distribution in a x=0.3 film. Statistical analysis reveals a nonhomogeneous distribution of Fe atoms throughout the film, which is used to explain the observed magnetic and electrical behavior.

cond-mat.mtrl-sci