Weyl semimetals are crystals in which electron bands cross at isolated points in momentum space. Associated with each crossing point (or Weyl node) is an integer topological invariant known as the Berry monopole charge. The discovery of new classes of Weyl materials is driving the search for novel properties that derive directly from the Berry charge. The circular photogalvanic effect (CPGE), whereby circular polarized light generates a current whose direction depends on the helicity of the absorbed photons, is a striking example of a macroscopic property that emerges from Weyl topology. Recently, it was predicted that the rate of current generation associated with optical transitions near a Weyl node is proportional to its monopole charge and independent of material-specific parameters. In Weyl semimetals that retain mirror symmetry this universal photogalvanic current is strongly suppressed by opposing contributions from energy equivalent nodes of opposite charge. However, when all mirror symmetries are broken, as in chiral Weyl systems, nodes with opposite topological charge are no longer degenerate, opening a window of photon energies where the topological CPGE can emerge. In this work we test this theory through measurement of the photon-energy dependence of the CPGE in the chiral Weyl semimetal RhSi. The spectrum is fully consistent with a topological CPGE, as it reveals a response in a low-energy window that closes at 0.65 eV, in quantitative agreement with the theoretically-derived bandstucture.
Recent experiments in the topological Weyl semimetal TaAs have observed record-breaking second-harmonic generation, a non-linear optical response at $2ω$ generated by an incoming light source at $ω$. However, whether second-harmonic generation is enhanced in topological semimetals in general is a challenging open question because their band structure entangles the contributions arising from trivial bands and topological band crossings. In this work, we circumvent this problem by studying RhSi, a chiral topological semimetal with a simple band structure with topological multifold fermions close…
Chiral topological semimetals are materials that break both inversion and mirror symmetries. They host interesting phenomena such as the quantized circular photogalvanic effect (CPGE) and the chiral magnetic effect. In this work, we report a comprehensive theoretical and experimental analysis of the linear and non-linear optical responses of the chiral topological semimetal RhSi, which is known to host multifold fermions. We show that the characteristic features of the optical conductivity, which display two distinct quasi-linear regimes above and below 0.4 eV, can be linked to excitations of …
Despite the fundamental nature of the edge state in topological physics, direct measurement of electronic and optical properties of the Fermi arcs of topological semimetals has posed a significant experimental challenge, as their response is often overwhelmed by the metallic bulk. However, laser-driven currents carried by surface and bulk states can propagate in different directions in nonsymmorphic crystals, allowing for the two components to be easily separated. Motivated by a recent theoretical prediction \cite{chang20}, we have measured the linear and circular photogalvanic effect currents…
We propose a new type of photoresponse induced in asymmetric Weyl semimetals in an external magnetic field. In usual symmetric Weyl semimetals in a magnetic field, the particles and holes produced by an incident light in different Weyl cones have opposite helicities and hence move in opposite directions, canceling each others's contributions to the photocurrent. However this cancelation does not occur if the Weyl semimetal possesses both a broken particle-hole symmetry and a broken spatial inversion symmetry. We call the resulting generation of photocurrent the helical magnetic effect because …
We present results of a theoretical study of photocurrents in the Weyl semimetals belonging to the gyrotropic symmetry classes. We show that, in weakly gyrotropic symmetry classes C$_{nv}$ ($n = 3,4,6$), the circular photocurrent transverse to the incidence direction appears only with account, in the electron effective Hamiltonian, for both linear and quadratic or cubic in quasi-momentum spin-dependent terms as well as a spin-independent term resulting in the tilt of the cone dispersion. A polarization-independent magneto-induced photocurrent is predicted which is also allowed in gyrotropic sy…
We develop a theory of the direct interband and indirect intraband photogalvanic effects in Weyl semimetals belonging to the gyrotropic classes with improper symmetry operations. At zero magnetic field, an excitation of such a material with circularly polarized light leads to a photocurrent whose direction depends on the light helicity. We show that in the semimetals of the C$_{2v}$ symmetry, an allowance for the tilt term in the effective Hamiltonian is enough to prevent cancellation of the photocurrent contributions from the Weyl cones of opposite chiralities. In the case of the C$_{4v}$ sym…
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 i…
The generation of photocurrent in an ideal two-dimensional Dirac spectrum is symmetry-forbidden. In sharp contrast, we show that three-dimensional Weyl semimetals can generically support significant photocurrent generations due to the combination of inversion symmetry breaking and finite tilts of the Weyl spectra. Symmetry properties, chirality relations and various dependences on the system and light sources are explored in details. Our results suggest that noncentrosymmetric Weyl materials can be advantageously applied to room temperature detections of mid- and far-infrared radiations.
A new 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 ex…
We study the effect of the strain on the energy bands of TaIrTe4 sheet and the photocurrent in the Cu-TaIrTe4-Cu heterojunction by using the quantum transport simulations. It is found that the Weyl points can be completely broken with increasing of the strain along z dirction. One can obtain a large photocurrent in the Cu-TaIrTe4-Cu heterojunction in the absence of the strain. While the photocurrent can be sharply enhanced by the strain and reach a large value. Accordingly, the maximum values of the photocurrent can be explained in terms of the transitions between peaks of density of states an…
We build a Cu-MoTe2-Cu device model and use first-principles density functional theory to study the transport properties of single-layer Td-MoTe2. We obtained the effect of strain on the energy band structure, transport properties, and photocurrent. The strain-induced photocurrent shows an anisotropy that reflects the modulation of the energy bands, including the Weyl point, by strain. The photocurrent can be suppressed to almost zero when the strain is applied along the vacuum direction. In contrast, the photocurrent can be significantly increased when the strain is applied along the transpor…
We study the second-order nonlinear optical response of a Weyl semimetal (WSM), i.e. a three-dimensional metal with linear band touchings acting as point-like sources of Berry curvature in momentum space, termed "Weyl-Berry monopoles". We first show that the anomalous second-order photocurrent of WSMs can be elegantly parametrized in terms of Weyl-Berry dipole and quadrupole moments. We then calculate the corresponding charge and node conductivities of WSMs with either broken time-reversal invariance or inversion symmetry. In particular, we predict a universal dissipationless second-order anom…
Theory of light absorption and circular photocurrent in Weyl semimetals is developed for arbitrary large light intensities with account for both elastic and inelastic relaxation processes of Weyl fermions. The direct optical transition rate is shown to saturate at large intensity, and the saturation behaviour depends on the light polarization and on the ratio of the elastic and inelastic relaxation times. The linear-circular dichroism in absorption is shown to exceed 10~\% at intermediate light wave amplitudes and fast energy relaxation. At large intensity $I$, the light absorption coefficient…
One of the hallmarks of light-spin interaction in solids is the appearance of photocurrent that depends on the light helicity. Recent studies have shown that helicity dependent photocurrent (HDP) emerges due to light induced spin current and the inverse spin Hall effect of semimetal thin films. We have studied HDP in metal/semimetal bilayers. Compared to Bi single layer films, we find the HDP is enhanced in metal/Bi bilayers. For the bilayers, the sign of HDP under back illumination reverses from that of front illumination. The back illumination photocurrent is the largest for Ag/Bi bilayers a…
The nonlinear optical responses from topological semimetals are crucial in both understanding the fundamental properties of quantum materials and designing next-generation light-sensors or solar-cells. However, previous work was focusing on the optical effects from bulk states only, disregarding topological surface responses. Here we propose a new (hitherto unknown) surface-only topological photocurrent response from chiral Fermi arcs. Using the ideal topological chiral semimetal RhSi as a representative, we quantitatively compute the topologically robust photocurrents from Fermi arcs on diffe…
The photovoltaic effect in a Weyl semimetal due to the adiabatic quantum phase is studied. We particularly focus on the case in which an external ac electric field is applied to the semimetal. In this setup, we show that a photocurrent is induced by the ac electric field. By considering a generalized Weyl Hamiltonian with nonlinear terms, it is shown that the photocurrent is induced by circularly, rather than linearly, polarized light. This photovoltaic current can be understood as an emergent electromagnetic induction in the momentum space; the Weyl node is a magnetic monopole in the momentum…
We theoretically study the effect of the Berry curvature on the transport properties of Weyl semimetals in the nonadiabatic process, which results in nonlinear optical responses. In the adiabatic process, the Berry curvature, which involves the time derivative of the Bloch states, contributes to the transport properties such as the adiabatic Thouless pump. Although this effect is very weak in usual solids, it is enhanced in Weyl semimetals, where the Berry curvature contributes to observable nonlinear optical responses due to its nodal structure. In this paper, using semiclassical Boltzmann th…
The family of three-dimensional topological insulators opens new avenues to discover novel photophysics and to develop novel types of photodetectors. ZrTe5 has been shown to be a Dirac semimetal possessing unique topological electronic and optical properties. Here we present spatially-resolved photocurrent measurements on devices made of nanoplatelets of ZrTe5, demonstrating the photothermoelectric origin of the photoresponse. Due to the high electrical conductivity and good Seebeck coefficient, we obtain noise-equivalent powers as low as 42 pW/Hz1/2 at room temperature for visible light illum…
Photo sensing and energy harvesting based on exotic properties of quantum materials and new operation principles have great potentials to break the fundamental performance limit of conventional photodetectors and solar cells. As topological nontrivial materials, Weyl semimetals have demonstrated novel optoelectronic properties that promise potential applications in photo detection and energy harvesting arising from their gapless linear dispersion near Weyl nodes and Berry field enhanced nonlinear optical effect at the vicinity of Weyl nodes. In this work, we demonstrate robust photocurrent gen…
The circular photogalvanic effect (CPGE) is the photocurrent generated in an optically active material in response to an applied ac electric field, and it changes sign depending on the chirality of the incident circularly polarized light. It is a non-linear dc current as it is second-order in the applied electric field, and for a certain range of low frequencies, takes on a quantized value proportional to the topological charge for a system which is a source of nonzero Berry flux. We show that for a non-interacting double-Weyl node, the CPGE is proportional to two quanta of Berry flux. On exam…
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 photocurr…
We report on a room-temperature photodetector utilizing semimetal bismuth nanowire arrays coupled with graphene. The structural flatness and high electron mobility of graphene exhibit great potential for future generations of electronic materials. Bismuth nanowire arrays coupled with graphene have strong absorption because of light trapping. Bismuth (Bi), as a semimetal, complements graphene's gapless and mobility characteristics. Bi also features a long screening length (4 nm) comparable to semiconductors. Raman spectroscopy is used to characterize the charge transfer between graphene and Bi.…
The chiral photocurrent or circular photogalvanic effect (CPGE) is a photocurrent that depends on the sense of circular polarization. In a disorder-free, noninteracting chiral Weyl semimetal, the magnitude of the effect is approximately quantized with a material-independent quantum $e^3/h^2$ for reasons of band topology. We study the first-order corrections due to the Coulomb and Hubbard interactions in a continuum model of a Weyl semimetal in which known corrections from other bands are absent. We find that the inclusion of interactions generically breaks the quantization. The corrections are…
We have studied theoretically the Weyl semimetals the point symmetry group of which has reflection planes and which contain equivalent valleys with opposite chiralities. These include the most frequently studied compounds, namely the transition metals monopnictides TaAs, NbAs, TaP, NbP, and also Bi$_{1-x}$Sb$_x$ alloys. The circular photogalvanic current, which inverts its direction under reversal of the light circular polarization, has been calculated for the light absorption under direct optical transitions near the Weyl points. In the studied materials, the total contribution of all the val…
When two lasers are applied to a non-centrosymmetric material, light can be generated at the difference of the incoming frequencies $Δω$, a phenomenon known as difference frequency generation (DFG), well characterized in semiconductors. In this work, we derive a general expression for DFG in metals, which we use to show that the DFG in chiral topological semimetals under circular polarized light is quantized in units of $e^3/h^2$ and independent of material parameters, including the scattering time $τ$, when $Δω\gg τ^{-1}$. In this regime, DFG provides a simpler alternative to measure a quanti…
We theoretically study the impact of impurities on the photogalvanic effect (PGE) in Weyl semimetals with weakly tilted Weyl cones. Our calculations are based on a two-nodes model with an inversion symmetry breaking offset and we employ a kinetic equation approach in which both optical transitions as well as particle-hole excitations near the Fermi energy can be taken into account. We focus on the parameter regime with a single photoactive node and control the calculation in small impurity concentration. Internode scattering is treated generically and therefore our results allow to continuousl…
We study the low-frequency properties of the bulk photovoltaic effect in topological semimetals. The bulk photovoltaic effect is a nonlinear optical effect that generates DC photocurrents under uniform irradiation, allowed by noncentrosymmetry. It is a promising mechanism for a terahertz photodetection based on topological semimetals. Here, we systematically investigate the low-frequency behavior of the second-order optical conductivity in point-node semimetals. Through symmetry and power-counting analysis, we show that Dirac and Weyl points with tilted cones show the leading low-frequency div…
Weyl semimetals are gapless topological states of matter with broken inversion and/or time reversal symmetry, which can support unconventional responses to externally applied electrical, optical and magnetic fields. Here we report a new photogalvanic effect in type-II WSMs, MoTe2 and Mo0.9W0.1Te2, which are observed to support a circulating photocurrent when illuminated by circularly polarized light at normal incidence. This effect occurs exclusively in the inversion broken phase, where crucially we find that it is associated with a spatially varying beam profile via a new dispersive contribut…
The recent discovery of the quantum nonlinear Hall effect has revived the field of nonlinear transport. Here, we predict magnetic field-induced nonlinear Hall effect in time-reversal symmetric Weyl semimetal. We show that the interplay of the band geometric quantities, such as the Berry curvature, and the magnetic part of the Lorentz force can give rise to finite nonlinear Hall conductivity that is linear in the magnetic field. Such nonlinear Hall conductivity can manifest through nonlinear transport measurement as well as nonlinear optical phenomena like photocurrent and the second harmonic g…
Chiral multifold fermions are quasiparticles described by higher spin generalizations of the Weyl equation, and are realized as low energy excitations near symmetry protected band crossings in certain chiral crystals. In this work we calculate the linear optical conductivity of all chiral multifold fermions. We show that it is enhanced with respect to that of Weyl fermions with the same Fermi velocity, and features characteristic activation frequencies for each multifold fermion class, providing an experimental fingerprint to detect them. We calculate the conductivity for realistic chiral mult…
Using first-principles calculations, we investigate the photogalvanic effect in the Weyl semimetal material TaAs. We find colossal photocurrents caused by the Weyl points in the band structuure in a wide range of laser frequency. Our calculations reveal that the photocurrent is predominantly contributed by the three-band transition from the occupied Weyl band to the empty Weyl band via an intermediate band away from the Weyl cone, for excitations both by linearly and circularly polarized lights. Therefore, it is significant to sum over all three-band transitions by considering a full set of Bl…
Circularly polarized light (CPL) can induce an asymmetry between the number of left- and right-handed 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…
The absence of mirror symmetry, or chirality, is behind striking natural phenomena found in systems as diverse as DNA and crystalline solids. A remarkable example occurs when chiral semimetals with topologically protected band degeneracies are illuminated with circularly polarized light. Under the right conditions, the part of the generated photocurrent that switches sign upon reversal of the light's polarization, known as the circular photogalvanic effect, is predicted to depend only on fundamental constants. The conditions to observe quantization are non-universal, and depend on material par…
So far, the circular photogalvanic effect (CPGE) is the only possible quantized signal in Weyl semimetals. With inversion and mirror symmetries broken, Weyl and multifold fermions in band structures with opposite chiralities can stay at different energies and generate a net topological charge. Such kind of net topological charge can present as a quantized signal in the circular polarized light induced injection current. According to current theoretical understanding, RhSi and its counterparts are believed to be the most promising candidate for the experimental observation of the quantized CPGE…
A Weyl semimetal (WSM) is a novel topological phase of matter, in which Weyl fermions (WFs) arise as pseudo-magnetic monopoles in its momentum space. The chirality of the WFs, given by the sign of the monopole charge, is central to the Weyl physics, since it directly serves as the sign of the topological number and gives rise to exotic properties such as Fermi arcs and the chiral anomaly. Despite being the defining property of a WSM, the chirality of the WFs has never been experimentally measured. Here, we directly detect the chirality of the WFs by measuring the photocurrent in response to ci…
Dirac semimetals are expected to forbid the manifestation of the circular photogalvanic effect (CPGE) because of their crystal inversion symmetry. Here, we report the observation of the CPGE in Cd3As2 nanobelt field effect transistors, when the photoexcitation is focused in the vicinity of the metal contacts up to room temperature. We attribute the CPGE to the Schottky electric field induced symmetry breaking, which results in the photocurrent modulation by circularly polarized photoexcitation via spin-momentum locking. The hypothesis is supported by a suite of experiments including spatially …
Weyl semimetals (WSM) have been discovered in time-reversal symmetric materials, featuring monopoles of Berry's curvature in momentum space. WSM have been distinguished between Type-I and II where the velocity tilting of the cone in the later ensures a finite area Fermi surface. To date it has not been clear whether the two types results in any qualitatively new phenomena. Here we focus on the shift-current response ($σ_{shift}(ω)$), a second order optical effect generating photocurrents. Surprisingly we find that up to an order unity constant, $σ_{shift}(ω)\sim \frac{e^3}{h^2}\frac{1}ω$ in Ty…
Noncentrosymmetric metals are anticipated to exhibit a $dc$ photocurrent in the nonlinear optical response caused by the Berry curvature dipole in momentum space. Weyl semimetals (WSMs) are expected to be excellent candidates for observing these nonlinear effects because they carry a large Berry curvature concentrated in small regions, i.e., near the Weyl points. We have implemented the semiclassical Berry curvature dipole formalism into an $ab~initio$ scheme and investigated the second-order nonlinear response for two representative groups of materials: the TaAs-family type-I WSMs and MoTe$_2…
Weyl semimetal (WSM) is expected to be an ideal spintronic material owing to its spin currents carried by the bulk and surface states with spin-momentum locking. A photocurrent generation in noncentrosymmetric WSM was also predicted owing to its broken inversion symmetry and linear energy dispersion which are unique to Weyl systems. In our recent measurements, the circular photogalvanic effect (CPGE) has been demonstrated in WSM of TaAs. The CPGE voltage is proportional to the helicity of the incident light and reverses its direction on changing the radiation helicity from left handed to right…
