No Arabic abstract
We present a systematic study of both the temperature and frequency dependence of the optical response in TaAs, a material that has recently been realized to host the Weyl semimetal state. Our study reveals that the optical conductivity of TaAs features a narrow Drude response alongside a conspicuous linear dependence on frequency. The width of the Drude peak decreases upon cooling, following a $T^{2}$ temperature dependence which is expected for Weyl semimetals. Two linear components with distinct slopes dominate the 5-K optical conductivity. A comparison between our experimental results and theoretical calculations suggests that the linear conductivity below $sim$230~cm$^{-1}$ is a clear signature of the Weyl points lying in very close proximity to the Fermi energy.
We report a polarized Raman study of Weyl semimetal TaAs. We observe all the optical phonons, with energies and symmetries consistent with our first-principles calculations. We detect additional excitations assigned to multiple-phonon excitations. These excitations are accompanied by broad peaks separated by 140~cm$^{-1}$ that are also most likely associated with multiple-phonon excitations. We also noticed a sizable B$_1$ component for the spectral background, for which the origin remains unclear.
In 1929, H. Weyl proposed that the massless solution of Dirac equation represents a pair of new type particles, the so-called Weyl fermions [1]. However the existence of them in particle physics remains elusive for more than eight decades. Recently, significant advances in both topological insulators and topological semimetals have provided an alternative way to realize Weyl fermions in condensed matter as an emergent phenomenon: when two non-degenerate bands in the three-dimensional momentum space cross in the vicinity of Fermi energy (called as Weyl nodes), the low energy excitation behaves exactly the same as Weyl fermions. Here, by performing soft x-ray angle-resolved photoemission spectroscopy measurements which mainly probe bulk band structure, we directly observe the long-sought-after Weyl nodes for the first time in TaAs, whose projected locations on the (001) surface match well to the Fermi arcs, providing undisputable experimental evidence of existence of Weyl fermion quasiparticles in TaAs.
While all media can exhibit first-order conductivity describing current linearly proportional to electric field, $E$, the second-order conductivity, $sigma^{(2)}$ , relating current to $E^2$, is nonzero only when inversion symmetry is broken. Second order nonlinear optical responses are powerful tools in basic research, as probes of symmetry breaking, and in optical technology as the basis for generating currents from far-infrared to X-ray wavelengths. The recent surge of interest in Weyl semimetals with acentric crystal structures has led to the discovery of a host of $sigma^{(2)}$ -related phenomena in this class of materials, such as polarization-selective conversion of light to dc current (photogalvanic effects) and the observation of giant second-harmonic generation (SHG) efficiency in TaAs at photon energy 1.5 eV. Here, we present measurements of the SHG spectrum of TaAs revealing that the response at 1.5 eV corresponds to the high-energy tail of a resonance at 0.7 eV, at which point the second harmonic conductivity is approximately 200 times larger than seen in the standard candle nonlinear crystal, GaAs. This remarkably large SHG response provokes the question of ultimate limits on $sigma^{(2)}$ , which we address by a new theorem relating frequency-integrated nonlinear response functions to the third cumulant (or skewness) of the polarization distribution function in the ground state. This theorem provides considerable insight into the factors that lead to the largest possible second-order nonlinear response, specifically showing that the spectral weight is unbounded and potentially divergent when the possibility of next-neighbor hopping is included.
Weyl semimetals are a class of materials that can be regarded as three-dimensional analogs of graphene breaking time reversal or inversion symmetry. Electrons in a Weyl semimetal behave as Weyl fermions, which have many exotic properties, such as chiral anomaly and magnetic monopoles in the crystal momentum space. The surface state of a Weyl semimetal displays pairs of entangled Fermi arcs at two opposite surfaces. However, the existence of Weyl semimetals has not yet been proved experimentally. Here we report the experimental realization of a Weyl semimetal in TaAs by observing Fermi arcs formed by its surface states using angle-resolved photoemission spectroscopy. Our first-principles calculations, matching remarkably well with the experimental results, further confirm that TaAs is a Weyl semimetal.
Since the early days of Dirac flux quantization, magnetic monopoles have been sought after as a potential corollary of quantized electric charge. As opposed to magnetic monopoles embedded into the theory of electromagnetism, Weyl crystals exhibit Berry flux monopoles in reciprocal parameter space. As a function of crystal momentum, such monopoles locate at the degeneracy point of the Weyl cone. Here, we report momentum-resolved spectroscopic signatures of Berry flux monopoles in TaAs as a paradigmatic Weyl semimetal. We have probed the orbital and spin angular momentum (OAM and SAM) of the Weyl-fermion states by angle-resolved photoemission spectroscopy at bulk-sensitive soft X-ray energies (SX-ARPES) combined with photoelectron spin detection and circular dichroism. Supported by first-principles calculations, our measurements image characteristics of a topologically non-trivial winding of the OAM at the Weyl nodes and unveil a chirality-dependent SAM of the Weyl bands. Our results experimentally visualize the non-trivial momentum-space topology in a Weyl semimetal, promising to have profound implications for the study of quantum-geometric effects in solids.