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Authors
M. R. Norman
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It is shown that the Weyl semimetal TaAs can have a significant polar vector contribution to its optical activity. This is quantified by ab initio calculations of the resonant x-ray diffraction at the Ta L1 edge. For the Bragg vector (400), this polar vector contribution to the circular intensity differential between left and right polarized x-rays is predicted to be comparable to that arising from linear dichroism. Implications this result has in regards to optical effects predicted for topological Weyl semimetals are discussed.
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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.
We investigate polarization-dependent ultrafast photocurrents in the Weyl semimetal TaAs using terahertz (THz) emission spectroscopy. Our results reveal that highly directional, transient photocurrents are generated along the non-centrosymmetric c-axis regardless of incident light polarization, while helicity-dependent photocurrents are excited within the ab-plane. This is consistent with earlier static photocurrent experiments, and demonstrates on the basis of both the physical constraints imposed by symmetry and the temporal dynamics intrinsic to current generation and decay that optically induced photocurrents in TaAs are inherent to the underlying crystal symmetry of the transition metal monopnictide family of Weyl semimetals.
The magnetic-field dependence of optical reflectivity [$R(omega)$] and optical conductivity [$sigma(omega)$] spectra of the ideal type-I Weyl semimetal TaAs has been investigated at the temperature of 10 K in the terahertz (THz) and infrared (IR) regions. The obtained $sigma(omega)$ spectrum in the THz region of $hbaromegaleq15$ meV is strongly affected by the applied magnetic field ($B$): The Drude spectral weight is rapidly suppressed and an energy gap originating from the optical transition in the lowest Landau levels appears with a gap size that increases in proportion to $sqrt{B}$, which suggests linear band dispersions. The obtained THz $sigma(omega)$ spectra could be scaled not only in the energy scale by $sqrt{B}$ but also in the intensity by $1/sqrt{B}$ as predicted theoretically. In the IR region for $hbaromegageq17$ meV, on the other hand, the observed $R(omega)$ peaks originating from the optical transitions in higher Landau levels are proportional to linear-$B$ suggesting parabolic bands. The different band dispersions originate from the crossover from the Dirac to the free-electron bands.
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.
Symmetry plays a central role in conventional and topological phases of matter, making the ability to optically drive symmetry change a critical step in developing future technologies that rely on such control. Topological materials, like the newly discovered topological semimetals, are particularly sensitive to a breaking or restoring of time-reversal and crystalline symmetries, which affect both bulk and surface electronic states. While previous studies have focused on controlling symmetry via coupling to the crystal lattice, we demonstrate here an all-electronic mechanism based on photocurrent generation. Using second-harmonic generation spectroscopy as a sensitive probe of symmetry change, we observe an ultrafast breaking of time-reversal and spatial symmetries following femtosecond optical excitation in the prototypical type-I Weyl semimetal TaAs. Our results show that optically driven photocurrents can be tailored to explicitly break electronic symmetry in a generic fashion, opening up the possibility of driving phase transitions between symmetry-protected states on ultrafast time scales.
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