Prototypical three-dimensional (3D) topological Dirac semimetals (DSMs), such as Cd$_3$As$_2$ and Na$_3$Bi, contain electrons that obey a linear momentum-energy dispersion with different Fermi velocities along the three orthogonal momentum dimensions. Despite being extensively studied in recent years, the inherent \emph{Fermi velocity anisotropy} has often been neglected in the theoretical and numerical studies of 3D DSMs. Although this omission does not qualitatively alter the physics of light-driven massless quasiparticles in 3D DSMs, it does \emph{quantitatively} change the optical coefficients which can lead to nontrivial implications in terms of nanophotonics and plasmonics applications. Here we study the linear optical response of 3D DSMs for general Fermi velocity values along each direction. Although the signature conductivity-frequency scaling, $σ(ω) \propto ω$, of 3D Dirac fermion is well-protected from Fermi velocity anisotropy, the linear optical response exhibits strong linear dichroism as captured by the \emph{universal} extinction ratio scaling law, $Λ_{ij} = (v_i/v_j)^2$ (where $i\neq j$ denotes the three spatial coordinates $x,y,z$, and $v_i$ is the $i$-direction Fermi velocity), which is independent of frequency, temperature, doping, and carrier scattering lifetime. For Cd$_3$As$_2$ and Na$_3$Bi$_3$, an exceptionally strong extinction ratio larger than 15 and covering broad terahertz window is revealed. Our findings shed new light on the role of Fermi velocity anisotropy in the optical response of Dirac semimetals and open up novel polarization-sensitive functionalities, such as photodetection and light modulation.
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）
Metamaterials and metasurfaces operating in the visible and near-infrared (NIR) offer a promising route towards next-generation photodetectors and devices for solar energy harvesting. While numerous metamaterials and metasurfaces using metals and semiconductors have been demonstrated, semimetals-based metasurfaces in the vis-NIR range are notably missing. Here, we experimentally demonstrate a broadband metasurface superabsorber based on large area, semimetallic, van der Waals PtSe2 thin films in agreement with electromagnetic simulations. Our results show that PtSe2 is an ultrathin and scalabl…
The high brightness, broad spectral coverage and pulsed characteristics of infrared synchrotron radiation enable time-resolved spectroscopy under throughput-limited optical systems, as can occur with the high-field magnet cryostat systems used to study electron dynamics and cyclotron resonance by far-infrared techniques. A natural extension for magnetospectroscopy is to sense circular dichroism, i.e. the difference in a material's optical response for left and right circularly polarized light. A key component for spectroscopic circular dichroism is an achromatic 1/4 wave retarder functioning o…
Under symmetry breaking, a three-dimensional nodal-line semimetal can turn into a topological insulator or Weyl semimetal, accompanied by the generation of momentum-space Berry curvature. We develop a theory that unifies their circular dichroism and highlights the roles of Berry curvature distribution and light incident direction. Nontrivially, these phases exhibit distinct dichroic optical absorption and radial Hall effects, with characteristic scalings with photon energy and electric field. Our findings offer a new diagnosis tool for examining topological phases of matter.
We present an optical conductivity study of the multifold semimetal PdGa, performed in a broad spectral range (100 - 20000 cm-1; 12 meV - 2.5 eV) down to T = 10 K. The conductivity at frequencies below 4000 cm-1 is dominated by free carriers while at higher frequencies interband transitions provide the major contribution. The spectra do not demonstrate a significant temperature evolution: only the intraband part changes as a function of temperature with the plasma frequency remaining constant. The interband contribution to the conductivity exhibits a broad peak at around 5500 cm-1 and increase…
Highly anisotropic Drude-weight-reduction and enhanced linear-dichroism in van der Waals Weyl semimetal Td-MoTe2 with coherent interlayer electronic transport
本研究结合线偏振光谱与电输运测量，揭示 Td-MoTe2 在 II 型外尔半金属相中沿 a 轴的高度各向异性 Drude 权重降低，并发现约 0.68 的增强归一化线二色性。
Photodetectors with broadband optical response have promising applications in many advanced optoelectronic and photonic devices. Especially, those with the detection range up to mid-infrared at room temperature are very challenging and highly desired. Recently, Weyl semimetal has been discovered and proposed to be favorable for photodetection since in general it breaks Lorentz invariance to have tilted chiral Weyl cones around Fermi level, which leads to chirality dependent photocurrents at arbitrarily long wavelength. Furthermore, the linear dispersion bands in Weyl cones result in very high …
The electromagnetic response of Dirac semimetals in the infrared and terahertz frequency ranges is attracting growing interest for potential applications in optoelectronics and nonlinear optics. The interplay between the free-carrier response and interband transitions in the gapless, linear dispersion relation plays a key role in enabling novel functionalities. Here we investigate ultrafast dynamics in thin films of a photoexcited Dirac semimetal Cd$_3$As$_2$ by probing the broadband response functions as complex quantities in the multiterahertz region (10-45 THz, 40-180 meV, or 7-30 $μ$m), wh…
The past decade has witnessed numerous discoveries of two-dimensional (2D) semimetals and insulators, whereas 2D metals are rarely identified. Borophene, a monolayer boron sheet, has recently emerged as a perfect 2D metal with unique structure and electronic properties. Here we study collective excitations in borophene, which exhibit two major plasmon modes with low damping rates extending from infrared to ultraviolet regime. The anisotropic 1D plasmon originates from electronic excitations of tilted Dirac cones in borophene, analogous to that in heavily doped Dirac semimetals. These features …
Weyl Fermions (WFs) in the type-II Weyl Semimetal (WSM) WTe$_2$ are difficult to resolve experimentally because the Weyl bands disperse in an extremely narrow region of the (E-k) space. Here, by using DFT-assisted high-resolution $^{125}$Te solid-state NMR (ssNMR) in the temperature range $50$K - $700$K, we succeeded in detecting low energy WF excitations and monitor their evolution with temperature. Remarkably, WFs appear to emerge at T$\sim 120$K; at lower temperatures WTe$_2$ behaves as a metal. This intriguing metal-to-WSM phase transition is shown to be induced by the rapid raise of the F…
We describe the development of a broadband magneto-optical spectrometer with femtosecond temporal resolution. The absorption spectrometer is based on a white-light supercontinuum (ca. 320 - 750 nm) using shot-to-shot temporal and spectral referencing at 1 kHz. Static and transient absorption spectra using circularly polarised light are collected in a magnetic field. The difference spectra with respect to the external field direction give the static and transient magneto-optical Faraday rotation (magnetic optical rotary dispersion) and ellipticity (magnetic circular dichroism) spectra. An achro…
Pulse-duration-sensitive high harmonics and attosecond locally-chiral light from a chiral topological Weyl semimetal
Max Planck Institute for the Structure and Dynamics of Matter（马克斯·普朗克物质与结构动力学研究所）；Center for Free-Electron Laser Science（自由电子激光科学中心）；Technion Israel Institute of Technology（以色列理工学院）；Center for Computational Quantum Physics（计算量子物理中心）；The Flatiron Institute（平顿研究所）
The optical properties of some nanomaterials can be controlled by an external magnetic field, providing active functionalities for a wide range of applications, from single-molecule sensing to nanoscale nonreciprocal optical isolation. Materials with broadband tunable magneto-optical response are therefore highly desired for various components in next-generation integrated photonic nanodevices. Concurrently, hyperbolic metamaterials received a lot of attention in the past decade since they exhibit unusual properties that are rarely observed in nature and provide an ideal platform to control th…
Mid-wave infrared (IR) and long-wave IR spectral ranges are of growing interest in various applications such as thermal imaging, thermography-based remote sensing, and night vision. Materials widely used for IR photodetectors in this regime include cadmium mercury telluride alloys and nanostructures of compound semiconductor. The materials development for IR optics will drive down the cost of IR optical systems and enable larger scale deployment. Here, we report a mid-wave IR responsive material composed of earth abundant and non-toxic elements, Sr1+xTiS3. It has a highly anisotropic quasi-one…
Characterized by bulk Dirac or Weyl cones and surface Fermi-arc states, topological semimetals have sparked enormous research interest in recent years. The nanostructures, with large surface-to-volume ratio and easy field-effect gating, provide ideal platforms to detect and manipulate the topological quantum states. Exotic physical properties originating from these topological states endow topological semimetals attractive for future topological electronics (topotronics). For example, the linear energy dispersion relation is promising for broadband infrared photodetectors, the spin-momentum lo…
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…
Using broadband (12-45 THz) multi-terahertz spectroscopy, we show that stimulated Rayleigh scattering dominates the transient optical conductivity of cadmium arsenide, a Dirac semimetal, under an optical driving field at 30 THz. The characteristic dispersive lineshape with net optical gain is accounted for by optical transitions between light-induced Floquet subbands, strikingly enhanced by the longitudinal plasma mode. Stimulated Rayleigh scattering with an unprecedentedly large refractive index change may pave the way for slow light generation in conductive solids at room temperature.
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 …
Here we show how time-resolved broadband optical spectroscopy can be used to quantify, with femtometer resolution, the oscillation amplitudes of coherent phonons through a displacive model without free tuning parameters, except an overall scaling factor determined by comparison between experimental data and density functional theory calculations. $WTe_2$ is used to benchmark this approach. In this semimetal, the response is anisotropic and provides the spectral fingerprints of two $A_1$ optical phonons at $\sim$8 and $\sim$80 $cm^-$$^1$. In principle, this methodology can be extended to any ma…
Identifying open-orbit topological surface states in dual topological semimetal TaSb$_2$
Leibniz Institute for Solid State and Materials Research, IFW Dresden（德累斯顿铁电研究所）；S. N. Bose National Centre for Basic Sciences（S.N. 玻色基础科学国家中心）；Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）；Helmholtz-Zentrum Berlin für Materialien und Energie, Elektronenspeicherring BESSY II（柏林亥姆霍兹材料与能源中心）
Thickness-Dependent Spintronic Terahertz Emission in MBE-Grown PtTe$_2$: From Semiconductor to Type-II Dirac Semimetal
Univ. Grenoble Alpes, CEA, CNRS, IRIG-SPINTEC（格勒诺布尔阿尔卑斯大学、法国原子能和替代能源委员会、法国国家科学研究中心、IRIG自旋技术中心）；Centre for Nanodiagnostics of Materials, Faculty of Materials Science and Technology, Slovak University of Technology（材料纳米诊断中心、材料与科技学院、斯洛伐克科技大学）
