Novel fermions with relativistic linear dispersion can emerge as low-energy excitations in topological semimetal materials. Here, we show that the orbital moment contribution in the circular photomagnetic effect for these topological semimetals exhibit an unconventional $ω^{-1}$ frequency scaling, leading to significantly enhanced response in the low frequency window, which can be orders of magnitude larger than previous observations on conventional materials. Furthermore, the response tensor is directly connected to the Chern numbers of the emergent fermions, manifesting their topological character. Our work reveals a new signature of topological semimetals and suggests them as promising platforms for optoelectronics and spintronics applications.
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…
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…
We derive the phonon dynamics of magnetic metals in the presence of strong spin-orbit coupling. We show that both a dissipationless viscosity and a dissipative viscosity arise in the dynamics. While the dissipationless viscosity splits the dispersion of left-handed and right-handed circularly polarized phonons, the dissipative viscosity damps them differently, inducing circular phonon dichroism. The effect offers a new degree of manipulation of phonons, i.e., the control of the phonon polarization. We investigate the effect in Weyl semimetals. We find that there exists strong circular phonon d…
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…
Quantization of spin circular photogalvanic effect in altermagnetic Weyl semimetals
Institute of Science Tokyo（东京科学大学）；Max Planck Institute for the Physics of Complex Systems（马克斯·普朗克复杂系统物理研究所）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Czech Academy of Sciences（捷克科学院）；the University of Tokyo（东京大学）；Hiroshima University（广岛大学）；RIKEN（理化学研究所）
We study theoretically the ultrafast electron dynamics of three-dimensional Weyl semimetals in the field of a laser pulse. For a circularly-polarized pulse, such dynamics is governed by topological resonance, which manifests itself as a specific conduction band population distribution in the vicinity of the Weyl points. The topological resonance is determined by the competition between the topological phase and the dynamic phase and depends on the handedness of a circularly polarized pulse. Also, we show that the conduction band population induced by a circularly-polarized pulse that consists …
We theoretically investigate the optical activity of three dimensional Dirac semimetals (DSMs) using circular dichroism (CD). We show that DSMs in the presence of a magnetic field in any one of the mirror-symmetric planes of the materials exhibit a notable dichroic behavior. In particular, for different orientations of the light field with respect to the mirror-symmetric plane, the CD in type-II DSMs can detect the presence of mirror anomaly by showing sharply distinct patterns at the mirror-symmetric angle. Interestingly, CD can also distinguish type-II DSMs having only one Dirac point at a t…
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…
From the Kubo formula for transport in a tilted Weyl semimetal we calculate the absorptive part of the dynamic conductivity for both right and left handed circular polarized light. These depend on the real part of the longitudinal conductivity and the imaginary part of the transverse (Hall) conductivity. We include the effect of the chiral anomaly which pumps charge from negative to positive chirality node when the usual ${\bs E}\cdot{\bs B}$ term is included in the electrodynamics and obtain analytic expressions. To calculate the Hall angle we further provide expressions for the imaginary par…
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…
Giant and Broadband Circular Dichroism from Particle-Hole Symmetry Breaking in Weyl Semimetals
East China Normal University（华东师范大学）；Fudan University（复旦大学）；Sun Yat-sen University（中山大学）；Southern University of Science and Technology (SUSTech)（南方科技大学）
The ternary van der Waals material NbIrTe$_4$ is a Type-II Weyl semimetal. We use a tunable circularly polarized mid-infrared laser to investigate the existence of band-to-band excitations using transient reflectivity in an exfoliated nanoflake and photothermoelectric and photogalvanic signals in a device. Unpolarized photothermoelectric spectroscopy shows that the absorption in the Weyl semimetal increases rapidly above 0.3 eV as expected from the increase in the density of states from DFT calculations. However, the reflectivity shows a sign change in the circular dichroism of the reflected l…
We numerically demonstrate that a planar slab made of magnetic Weyl semimetal (a class of topological materials) can emit high-purity circularly polarized (CP) thermal radiation over a broad mid- and long-wave infrared wavelength range for a significant portion of its emission solid angle. This effect fundamentally arises from the strong infrared gyrotropy or nonreciprocity of these materials which primarily depends on the momentum separation between Weyl nodes in the band structure. We clarify the dependence of this effect on the underlying physical parameters and highlight that the spectral …
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…
Weyl semimetals are a three dimensional gapless topological phase in which bands intersect at arbitrary points -- the Weyl nodes -- in the Brillouin zone. These points carry a topological quantum number known as the \emph{chirality} and always appear in pairs of opposite chiralities. The notion of chirality leads to anomalous non-conservation of chiral charge, known as the \emph{chiral anomaly}, according to which charge can be pumped between Weyl nodes of opposite chiralities by an electromagnetic field with non-zero $\boldsymbol{E}\cdot\boldsymbol{B}$. Here, we propose probing the chiral ano…
Floquet engineering, the concept of tailoring a system by a periodic drive, is increasingly exploited to design and manipulate topological phases of matter. In this work, we study periodically driven higher-order topological Dirac semimetals associated with a $k$-dependent quantized quadrupole moment by applying circularly polarized light. The undriven Dirac semimetals feature gapless higher-order hinge Fermi arc states which are the consequence of the higher-order topology of the Dirac nodes. Floquet Weyl semimetal phases with hybrid-order topology, characterized by both a $k$-dependent quant…
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…
We calculate the A.C. optical response to circularly polarized light of a Weyl semimetal (WSM) with varying amounts of tilt of the Dirac cones. Both type-I and II (overtilted) WSM are considered in a continuum model with broken time reversal (TR) symmetry. The Weyl nodes appear in pairs of equal energies but of opposite momentum and chirality. For type-I the response of a particular node to right (RHP) and left (LHP) hand polarized light are distinct only in a limited range of photon energy $Ω$, $\frac{2}{1+C_{2}/v}<\fracΩμ<\frac{2}{1-C_{2}/v}$ with $μ$ the chemical potential and $C_{2}$ the t…
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 circularly polarized light-induced Floquet state in line-node semimetals with time-reversal symmetry and inversion symmetry. It is found that the Floquet state can show the photovoltaic anomalous Hall effect when an applied circularly polarized light gaps out the line node in the bulk and leave Weyl point nodes. The Hall conductivity is sensitive to the location of Fermi level: When the Fermi level locates at the node, the Hall conductivity depends on the radius of line node and is nearly independent of the intensity of light. Away from the line node, the Hall conduc…
We have studied helicity dependent photocurrent (HDP) in Bi-based Dirac semimetal thin films. HDP increases with film thickness before it saturates, changes its sign when the majority carrier type is changed from electrons to holes and takes a sharp peak when the Fermi level lies near the charge neutrality point. These results suggest that irradiation of circularly polarized light to Dirac semimetals induces an effective magnetic field that aligns the carrier spin along the light spin angular momentum and generates a spin current along the film normal. The effective magnetic field is estimated…
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 demonstrate that in Weyl semimetals, the momentum-space helical spin texture can couple to the chirality of the Weyl node to generate a frequency-independent magnetization in response to circularly polarized light through the inverse Faraday effect. This frequency-independence is rooted in the topology of the Weyl node. Since the helicity and the chirality are always locked for Weyl nodes, this effect is not subject to any symmetry constraint. Finally, we show that the photoinduced frequency-independent magnetization is robust against lattice effect and has a magnitude large enough to reali…
As the development of topological band theory, comprehensive databases about time reversal and crystalline symmetries protected nonmagnetic topological materials were developed via first-principles calculations recently. However, owing to the low symmetry requirement of Weyl points, the symmetry-based topological indicator cannot be applied to Weyl semimetals (WSMs). Hitherto, the WSMs with Weyl points in arbitrary positions are still absent in the well-known databases. In this work, we develop an efficient algorithm to search for Weyl points automatically and establish a database of nonmagnet…
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…
We generalize a semiclassical theory and use the argument of angular momentum conservation to examine the ballistic transport in lightly-doped Weyl semimetals, taking into account various phase-space Berry curvatures. We predict universal transverse shifts of the wave-packet center in transmission and reflection, perpendicular to the direction in which the Fermi energy or velocities change adiabatically. The anomalous shifts are opposite for electrons with different chirality, and can be made imbalanced by breaking inversion symmetry. We discuss how to utilize local gates, strain effects, and …
$α$-Sn is well known as a typical Luttinger semimetal with a quadratic band touching at the $Γ$ point. Based on the effective $k\cdot p$ analysis as well as first-principles calculations, we demonstrate that multiple topological phases with a rich diagram, including topological insulator, Dirac semimetal, and Weyl semimetal phases, can be induced and engineered in $α$-Sn by external strains, magnetic fields, and circularly polarized light (CPL). Intriguingly, not only the conventional type-I Weyl nodes, but also type-II Weyl nodes and double-Weyl nodes can be generated directly from the quadra…
Using Hall photovoltage measurements, we demonstrate that an anomalous Hall-voltage can be induced in few layer WTe2 under circularly polarized light illumination. By applying a bias voltage along different crystal axes, we find that the photo-induced anomalous Hall conductivity coincides with a particular crystal axis. Our results are consistent with the underlying Berry-curvature exhibiting a dipolar distribution due to the breaking of crystal inversion symmetry. Using a time-resolved optoelectronic auto-correlation spectroscopy, we find that the decay time of the anomalous Hall voltage exce…
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. Recen…
Creating and manipulating topological states is a key goal of condensed matter physics. Periodic driving offers a powerful method to manipulate electronic states, and even to create topological states in solids. Here, we investigate the tunable Floquet states in a periodically driven higher-order nodal line semimetal with both spatial inversion and time-reversal symmetries. We found that the Floquet Weyl semimetal states, which support both one-dimensional hinge Fermi arc and two-dimensional surface Fermi arc states, can be induced in the higher-order nodal-line semimetal by shining circularly…
Parallel electric and magnetic fields applied to Weyl semimetals pump axial charge via the axial anomaly until balanced by intervalley relaxation. The resulting nonequilibrium steady state exhibits the chiral magnetic effect as well as the anomalous Hall effect, which coupled with Maxwell's equations leads to unstable electromagnetic waves at low frequency and long wavelength. Here, we show that such chiral magnetic instability manifests itself as anomalous reflectance of the surface of pumped Weyl semimetal. Depending on electric, chiral magnetic, and anomalous Hall conductivities, the reflec…
Asymmetric Weyl semimetals, which possess an inherently chiral structure, have different energies and dispersion relations for left- and right-handed fermions. They exhibit certain effects not found in symmetric Weyl semimetals, such as the quantized circular photogalvanic effect and the helical magnetic effect. In this work, we derive the conditions required for breaking chiral symmetry by applying an external field in symmetric Weyl semimetals. We explicitly demonstrate that in certain materials with the $T_d$ point group, magnetic fields along low symmetry directions break the symmetry betw…
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…
The Weyl semimetal is characterized by three-dimensional linear band touching points called Weyl nodes. These nodes come in pairs with opposite chiralities. We show that the coupling of circularly polarized photons with these chiral electrons generates a Hall conductivity without any applied magnetic field in the plane orthogonal to the light propagation. This phenomenon comes about because with all three Pauli matrices exhausted to form the three-dimensional linear dispersion, the Weyl nodes cannot be gapped. Rather, the net influence of chiral photons is to shift the positions of the Weyl no…
The photogalvanic effect -- a rectified current induced by light irradiation -- requires the intrinsic symmetry of the medium to be sufficiently low, which strongly limits candidate materials for this effect. In this work we explore how in Weyl semimetals the photogalvanic effect can be enabled and controlled by design of the material surface. Specifically, we provide a theory of ballistic linear and circular photogalvanic current in a Weyl semimetal spatially confined to a slab under general and variable surface boundary conditions. The results are applicable to Weyl semimetals with an arbitr…
We propose a mechanism to generate a static magnetization via {\em axial magnetoelectric effect} (AMEE). Magnetization ${\bf M} \sim {\bf E}_5(ω)\times {\bf E}_5^{*}(ω)$ appears as a result of the transfer of the angular momentum of the axial electric field ${\bf E}_5(t)$ into the magnetic moment in Dirac and Weyl semimetals. We point out similarities and differences between the proposed AMEE and a conventional inverse Faraday effect (IFE). As an example, we estimated the AMEE generated by circularly polarized acoustic waves and find it to be on the scale of microgauss for gigahertz frequency …
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…
It is necessary to study the properties of Weyl semimetal nanostructures for potential applications in nanoelectronics. Here we study the Weyl semimetal quantum dot with a most simple model Hamiltonian with only two Weyl points. We focus on the low-energy electronic structure and show the correspondence to that of three-dimensional Weyl semimetal, such as Weyl point and Fermi arc. We find that there exist both surface and bulk states near Fermi level. The direct gap of bulk states reaches the minimum with the location determined by Weyl point. There exists a quantum number with only several va…
In this work, the near-field radiative heat transfer (NFRHT) between two Weyl semimetal (WSM) nanoparticles (NPs) is investigated. The numerical results show that negative differential thermal conductance (NDTC) effect can be obtained in this system, i.e., when the temperature of the emitter is fixed, the heat flux does not decrease monotonically with the increase of the temperature of the receiver. Specifically, when the temperature of the emitter is 300 K, the heat flux is identical when the temperature of the receiver is 50 K or 280 K. The NDTC effect is attributed to the fact that the perm…
We study nonlinear magneto-optical responses of metals by a semiclassical Boltzmann equation approach. We derive general formulas for linear and second order nonlinear optical effects in the presence of magnetic fields that include both Berry curvature and orbital magnetic moment. Applied to Weyl fermions, the semiclassical approach (i) captures the directional anisotropy of linear conductivity under magnetic field as a consequence of an anisotropic $B^2$ contribution, which may explain the low-field regime of recent experiments; (ii) predicts strong second harmonic generation proportional to …
When a Dirac semimetal is subject to a circularly polarized laser, it is predicted that the Dirac cone splits into two Weyl nodes and a nonequilibrium transient state called the Floquet Weyl semimetal is realized. We focus on the previously unexplored low-frequency regime, where the upper and lower Dirac bands resonantly couple with each other through multi-photon processes, which is a realistic situation in solid state ultrafast pump-probe experiments. We find a series of new Weyl nodes emerging in pairs when the Floquet replica bands hybridize with each other. The nature of the Floquet Weyl …
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 …
