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Register a new userNon-stoichiometry and Defects in the Weyl Semimetals TaAs, TaP, NbP, and NbAs
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We report a structural study of the Weyl semimetals TaAs, TaP, NbP, and NbAs, utilizing diffraction techniques (single crystal x-ray diffraction and energy dispersive spectroscopy) and imaging techniques (transmission electron microscopy/scanning transmission electron microscopy). We observe defects of various degrees, leading to non-stoichiometric single crystals of all four semimetals. While TaP displays a large pnictide deficiency with composition TaP$_{0.83(3)}$, and stacking faults accompanied by anti-site disorder and site vacancies, TaAs displays transition metal deficiency with composition Ta$_{0.92(2)}$As and a high density of stacking faults. NbP also displays pnictide deficiency, yielding composition NbP$_{0.95(2)}$, and lastly, NbAs display very little deviation from a 1:1 composition, NbAs$_{1.00(3)}$, and is therefore recommended to serve as the model compound for these semimetals.
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We report a comparative polarized Raman study of Weyl semimetals TaAs, NbAs, TaP and NbP. The evolution of the phonon frequencies with the sample composition allows us to determine experimentally which atoms are mainly involved for each vibration mode. Our results confirm previous first-principles calculations indicating that the A$_1$, B$_1(2)$, E$(2)$ and E$(3)$ modes involve mainly the As(P) atoms, the B$_1(1)$ mode is mainly related to Ta(Nb) atoms, and the E$(1)$ mode involves both kinds of atoms. By comparing the energy of the different modes, we establish that the B$_1(1)$, B$_1(2)$, E$(2)$ and E$(3)$ become harder with chemical pressure increasing. This behavior differs from our observation on the A$_1$ mode, which decreases in energy, in contrast to its behavior under external pressure.
We report a structural study of the Weyl semimetals TaAs and TaP, utilizing diffraction and imaging techniques, where we show that they contain a high density of defects, leading to non-stoichiometric single crystals of both semimetals. Despite the observed defects and non-stoichiometry on samples grown using techniques already reported in the literature, de Haas-van Alphen measurements on TaP reveal quantum oscillations and a high carrier mobility, an indication that the crystals are of quality comparable to those reported elsewhere. Electronic structure calculations on TaAs reveal that the position of the Weyl points relative to the Fermi level shift with the introduction of vacancies and stacking faults. In the case of vacancies the Fermi surface becomes considerably altered, while the effect of stacking faults on the electronic structure is to allow the Weyl pockets to remain close to the Fermi surface. The observation of quantum oscillations in a non-stoichiometric crystal and the persistence of Weyl fermion pockets near the Fermi surface in a crystal with stacking faults point to the robustness of these quantum phenomena in these materials.
Weyl semimetals such as the TaAs family (TaAs, TaP, NbAs, NbP) host quasiparticle excitations resembling the long sought after Weyl fermions at special band-crossing points in the band structure denoted as Weyl nodes. They are predicted to exhibit a negative longitudinal magnetoresistance (LMR) due to the chiral anomaly if the Fermi energy is sufficiently close to the Weyl points. However, current jetting effects, i.e. current inhomogeneities caused by a strong, field-induced conductivity anisotropy in semimetals, have a similar experimental signature and therefore have hindered a determination of the intrinsic LMR in the TaAs family so far. This work investigates the longitudinal magnetoresistance of all four members of this family along the crystallographic $a$ and $c$ direction. Our samples are of similar quality as those previously studied in the literature and have a similar chemical potential as indicated by matching quantum oscillation (QO) frequencies. Care was taken to ensure homogeneous currents in all measurements. As opposed to previous studies where this was not done, we find a positive LMR that saturates in fields above 4 T in TaP, NbP and NbAs for $B||c$. Using Fermi-surface geometries from band structure calculations that had been confirmed by experiment, we show that this is the behaviour expected from a classical purely orbital effect, independent on the distance of the Weyl node to the Fermi energy. The TaAs family of compounds is the first to show such a simple LMR without apparent influences of scattering anisotropy. In configurations where the orbital effect is small, i.e. for $B||a$ in NbAs and NbP, we find a non-monotonous LMR including regions of negative LMR. We discuss a weak antilocalisation scenario as an alternative interpretation than the chiral anomaly for these results, since it can fully account for the overall field dependence.
TaAs and NbAs are two of the earliest identified Weyl semimetals that possess many intriguing optical properties, such as chirality-dependent optical excitations and giant second harmonic generation (SHG). Linear and nonlinear optics have been employed as tools to probe the Weyl physics in these crystals. Here we extend these studies to address two important points: determining the complete anisotropic dielectric response, and to explore if and how they can reveal essential Weyl physics. For the first time, we determine the complete anisotropic dielectric functions of TaAs and NbAs by combining spectroscopic ellipsometry and density functional theory (DFT). Parameterized Lorentz oscillators are reported from 1.2-6 eV (experiment) and 0-6 eV (DFT), and good agreement is shown between them. Both linear and nonlinear optical properties have been reported to reveal Weyl physics. We suggest that strong optical resonances from trivial bands are the likely origin of the large optical second harmonic generation previously reported at these energies. Furthermore, by comparing the contribution of a small k-space centered around the Weyl cones to the total linear dielectric function, we find that these contributions are highly anisotropic and are <25% of the total dielectric function below 0.5 eV; above 1eV, these contributions are negligible. Thus, the study of Weyl physics using optical techniques requires very low energies and even there, a careful assessment is required in distinguishing the much smaller contributions of the Weyl bands from the dominant contributions of the trivial bands and Drude response to the total dielectric function.
Chiral anomaly induced negative magnetoresistance (NMR) has been widely used as a critical transport evidence on the existence of Weyl fermions in topological semimetals. In this mini review, we discuss the general observation of the NMR phenomena in non-centrosymmetric NbP and NbAs. We show that NMR can be contributed by intrinsic chiral anomaly of Weyl fermions and/or extrinsic effects, such as superimposition of Hall signals, field-dependent inhomogeneous current flow in the bulk, i.e. current jetting, and weak localization (WL) of coexistent trivial carriers. Such WL controlled NMR is heavily dependent on sample quality, and is characterized by pronounced crossover from positive to negative MR growth at elevated temperatures, as a result of the competition between the phase coherence time and the spin-orbital scattering constant of the bulk trivial pockets. Thus, the correlation of NMR and chiral anomaly needs to be scrutinized, without the support of other complimentary techniques. Due to the lifting of spin degeneracy, the spin orientations of Weyl fermions are either parallel or antiparallel to the momentum, a unique physical property known as helicity. The conservation of helicity provides strong protection for the transport of Weyl fermions, which can only be effectively scattered by magnetic impurities. Chemical doping of magnetic and non-magnetic impurities are thus more convincing in probing the existence of Weyl fermions than the NMR method.
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