As a fascinating topological phase of matter, Weyl semimetals host chiral fermions with distinct chiralities and spin textures. Optical excitations involving those chiral fermions can induce exotic carrier responses, and in turn lead to novel optical phenomena. Here, we discover strong coherent chiral terahertz emission from the Weyl semimetal TaAs and demonstrate unprecedented manipulation over its polarization on a femtosecond timescale. Such polarization control is achieved via the colossal ultrafast photocurrents in TaAs arising from the circular or linear photogalvanic effect. We unravel that the chiral ultrafast photocurrents are attributed to the large band velocity changes when the Weyl fermions are excited from the Weyl bands to the high-lying bands. The photocurrent generation is maximized at near-IR frequency range close to 1.5 eV. Our findings provide an entirely new design concept for creating chiral photon sources using quantum materials and open up new opportunities for developing ultrafast opto-electronics using Weyl physics.

Circularly polarized light (CPL) can induce an asymmetry between the number of left-and righthanded chiral quasiparticles in Dirac and Weyl semimetals. We show that if the photoresponse of the material is dominated by chiral quasiparticles, the total chiral charge induced in the material by CPL can be evaluated in a model-independent way through the chiral anomaly. In the presence of an external magnetic field perpendicular to the incident CPL, this allows to predict the linear density of the induced photocurrent resulting from the chiral magnetic effect. The predicted effect should exist in any kind of Dirac or Weyl materials, with both symmetric and asymmetric band structure. An estimate of the resulting chiral magnetic photocurrent in a typical Dirac semimetal irradiated by an infrared laser of intensity 5 × 10 6 W/m 2 and a wavelength of λ 10 µm in an external magnetic field B 2 T yields a current J 50 nA in the laser spot of size 50 µm. This current scales linearly with the magnetic field and wavelength, opening up possibilities for applications in photonics, optoelectronics, and THz sensing.

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A class of photocurrents is predicted to occur in both type-I and type-II Weyl semimetals. Unlike the previously studied photocurrents in chiral materials, the proposed current requires neither circularly polarized light nor an absence of symmetry with respect to a plane of reflection. We show that if a Weyl semimetal has a broken inversion symmetry then linearly polarized light can induce a photocurrent transverse to the direction of an applied magnetic field, in spite of the symmetry with respect to a reflection plane and the time reversal symmetry. The class of materials in which we expect this to occur is sufficiently broad and includes the transition metal monopnictides such as TaAs. The effect stems from the dynamics of Weyl chiral quasiparticles in a magnetic field, restricted by the symmetries described above; because the resulting current is transverse to the direction of magnetic field, we call it the transverse chiral magnetic photocurrent. The magnitude of the resulting photocurrent is predicted to be significant in the THz frequency range, about 0.75 μA for type-I and 2.5 μA for type-II Weyl semimetals. This opens the possibility to utilize the predicted transverse chiral magnetic photocurrent for sensing unpolarized THz radiation.