Optical signatures of multifold fermions in the chiral topological semimetal CoSi
B. Xu, Z. Fang, M. A. Sánchez-Martínez, J. W. F. Venderbos, Z. Ni, T. Qiu, K. Manna, K. Wang, J. Paglione, C. Bernhard, C. Felser, E. J. Mele, A. G. Grushin, A. M. Rappe, Liang Wu
发表信息：
Proceedings of the National Academy of Sciences, 117(44), 27104-27110 (2020)
We report the optical conductivity in high-quality crystals of the chiral topological semimetal CoSi, which hosts exotic quasiparticles known as multifold fermions. We find that the optical response is separated into several distinct regions as a function of frequency, each dominated by different types of quasiparticles. The low-frequency intraband response is captured by a narrow Drude peak from a high-mobility electron pocket of double Weyl quasi-particles, and the temperature dependence of the spectral weight is consistent with its Fermi velocity. By subtracting the low-frequency sharp Drude and phonon peaks at low temperatures, we reveal two intermediate quasi-linear inter-band contributions separated by a kink at 0.2 eV. Using Wannier tight-binding models based on first-principle calculations, we link the optical conductivity above and below 0.2 eV to interband transitions near the double Weyl fermion and a threefold fermion, respectively. We analyze and determine the chemical potential relative to the energy of the threefold fermion, revealing the importance of transitions between a linearly dispersing band and a flat band. More strikingly, below 0.1 eV our data are best explained if spin-orbit coupling is included, suggesting that at these energies the optical response is governed by transitions between a previously unobserved four-fold spin-3/2 node and a Weyl node. Our comprehensive combined experimental and theoretical study provides a way to resolve different types of multifold fermions in CoSi at different energy. More broadly our results provide the necessary basis to interpret the burgeoning set of optical and transport experiments in chiral topological semimetals.
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…
We report the identification of symmetry-enforced nodal planes (NPs) in CoSi providing the missing topological charges in an entire network of band-crossings comprising in addition multifold degeneracies and Weyl points, such that the fermion doubling theorem is satisfied. In our study we have combined measurements of Shubnikov-de Haas (SdH) oscillations in CoSi with material-specific calculations of the electronic structure and Berry curvature, as well as a general analysis of the band topology of space group (SG) 198. The observation of two nearly dispersionless SdH frequency branches provid…
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…
The circular photogalvanic effect (CPGE) is the only possible quantized signal in Chiral Weyl and multi-fold semimetals with inversion and mirror symmetries broken. Here, we review CPGE in the chiral multifold semimetals in terms of classification of CPGE tensor, the quantization of CPGE from k.p effective model and topological semimetal RhSi family. Firstly, we give complete symmetric analysis of CPGE tensors for all nonmagnetic point groups, and get a table classifying matrix of response tensors. Secondly, the CPGE becomes a quantized response in the noncentrosymmetric topological semimetals…
Plasmonics in topological semimetals offers exciting opportunities for fundamental physics exploration as well as for technological applications. Here, we investigate plasmons in the exemplar chiral crystal CoSi, which hosts a variety of multifold fermionic excitations. We show that CoSi hosts two distinct plasmon modes in the infrared regime at 0.1 eV and 1.1 eV in the long-wavelength limit. The 0.1 eV plasmon is found to be highly dispersive, and originates from intraband collective oscillations associated with a double spin-1 excitation, while the 1.1 eV plasmon is dispersionless and it inv…
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 …
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…
Multifold fermion systems feature free fermionic excitations, which have no counterparts in high-energy physics, and exhibit several unconventional properties. Using first-principles calculations, we predict that strain engineering can be used to control the distribution of topological charges in transition metal silicide candidate CoSi, hosting multifold fermions. We demonstrate that breaking the rotational symmetry of the system, by choosing a suitable strain, destroys the multifold fermions, and at the same time results in the creation of Weyl points. We introduce a low energy effective mod…
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…
Nontrivial band topologies in semimetals lead to robust surface states that can contribute dominantly to the total conduction. This may result in reduced resistivity with decreasing feature size contrary to conventional metals, which may highly impact the semiconductor industry. Here we study the resistivity scaling of a representative topological semimetal CoSi using realistic band structures and Green's function methods. We show that there exists a critical thickness d_c dividing different scaling trends. Above d_c, when the defect density is low such that surface conduction dominates, resis…
Non-symmorphic chiral topological crystals host exotic multifold fermions, and their associated Fermi arcs helically wrap around and expand throughout the Brillouin zone between the high-symmetry center and surface-corner momenta. However, Fermi-arc splitting and realization of the theoretically proposed maximal Chern number rely heavily on the spin-orbit coupling (SOC) strength. In the present work, we investigate the topological states of a new chiral crystal, PtGa, which has the strongest SOC among all chiral crystals reported to date. With a comprehensive investigation using high-resolutio…
Higher-fold chiral fermions that go beyond two-fold Weyl fermions have recently been reported in crystalline systems. Here, we focus on such excitations in several binary, ternary and quaternary alloys/compounds with CoGe, BiSbPt and KMgBO3 as the representative examples that belong to the crystal space group (SG) 198. We found distinct three-fold, four-fold and six-fold chiral fermions in the bulk via Density Functional computations. We provide general symmetry arguments for the protection of these degeneracies with special emphasis on the four-fold fermions. Our surface spectra simulations s…
We report single crystal growth of CoSi, which has recently been recognized as a new type of topological semimetal hosting fourfold and sixfold degenerate nodes. The Shubnikov-de Haas quantum oscillation (QO) is observed on our crystals. There are two frequencies originating from almost isotropic bulk electron Fermi surfaces, in accordance with band structure calculations. The effective mass, scattering rate, and QO phase difference of the two frequencies are extracted and discussed.
Chiral fermions in solid state feature "Fermi arc" states, connecting the surface projections of the bulk chiral nodes. The surface Fermi arc is a signature of nontrivial bulk topology. Unconventional chiral fermions with an extensive Fermi arc traversing the whole Brillouin zone have been theoretically proposed in CoSi. Here, we use scanning tunneling microscopy / spectroscopy to investigate quasiparticle interference at various terminations of a CoSi single crystal. The observed surface states exhibit chiral fermion-originated characteristics. These reside on (001) and (011) but not (111) su…
We survey the electrical transport properties of the single-crystalline, topological chiral semimetal CoSi which was grown via different methods. High-quality CoSi single crystals were found in the growth from tellurium solution. The sample's high carrier mobility enables us to observe, for the first time, quantum oscillations (QOs) in its thermoelectrical signals. Our analysis of QOs reveals two spherical Fermi surfaces around the R point in the Brillouin zone corner. The extracted Berry phases of these electron orbits are consistent with the -2 chiral charge as reported in DFT calculations. …
We assess the viability of topological semimetals for application in advanced interconnect technology, where conductor size is on the order of a few nanometers and grain boundaries are expected to be prevalent. We investigate the electron transport properties and grain boundary scattering in thin films of the topological semimetals CoSi and CoGe using first-principles calculations combined with the Non-Equilibrium Green's Function (NEGF) technique. Unlike conventional interconnect metals like Cu and Al, we find that CoSi and CoGe conduct primarily through topologically-protected surface states…
We review recent theoretical progress in the understanding and prediction of novel topological semimetals. Topological semimetals define a class of gapless electronic phases exhibiting topologically stable crossings of energy bands. Different types of topological semimetals can be distinguished based on the degeneracy of the band crossings, their codimension (e.g., point or line nodes), as well as the crystal space group symmetries on which the protection of stable band crossings relies. The dispersion near the band crossing is a further discriminating characteristic. These properties give ris…
The resistance bottleneck in metal-interconnect scaling calls for new interconnect materials. This paper explores topological semimetals as a potential solution. After reviewing the desirable properties of topological semimetals for back-end-of-line (BEOL) interconnects, we use CoSi as an example to demonstrate the decreasing resistance-area product with scaling and provide material-search guidelines.
Spin-1 chiral semimetal is a new state of quantum matter hosting unconventional chiral fermions that extend beyond the common Dirac and Weyl fermions. B20-type CoSi is a prototypal material that accommodates such an exotic quasiparticle. To date, the spin transport properties in the spin-1 chiral semimetals, have not been explored yet. In this work, we fabricated B20-CoSi thin films on sapphire c-plane substrates by magnetron sputtering and studied the spin Hall effect (SHE) by combining experiments and first-principles calculations. The SHE of CoSi using CoSi/CoFeB/MgO heterostructures was in…
Here, we study the thermoelectric properties of topological semimetal CoSi in the temperature range $300-800$ K by using combined experimental and density functional theory (DFT) based methods. CoSi is synthesized using arc melting technique and the Rietveld refinement gives the lattice parameters of a = b = c = 4.445 Å. The measured values of Seebeck coefficient (S) shows the non-monotonic behaviour in the studied temperature range with the value of $\sim-$81 $μ$V/K at room temperature. The $|S|$ first increases till 560 K ($\sim-$93 $μ$V/K) and then decreases up to 800 K ($\sim-$84 $μ$V/K) i…
Transition metal monosilicides CoSi, CoGe, RhSi and RhGe in the chiral cubic B20 structure have recently been found to host unconventional chiral fermions beyond spin-1/2 WFs, and also exhibit exotic physical phenomena such as long Fermi arc surface states, GME and quantized CPGE. Thus, exploring novel spin-related transports in these unconventional chiral fermion semimetals may open a new door for spintronics and spin caloritronics. In this paper, we study the intrinsic SHE and SNE in the CoSi family based on ab initio relativistic band structure calculations. First, we find that unlike nonch…
Topological semimetals materialize a new state of quantum matter where massless fermions protected by a specific crystal symmetry host exotic quantum phenomena. Distinct from well-known Dirac and Weyl fermions, structurally-chiral topological semimetals are predicted to host new types of massless fermions characterized by a large topological charge, whereas such exotic fermions are yet to be experimentally established. Here, by using angle-resolved photoemission spectroscopy, we experimentally demonstrate that a transition-metal silicide CoSi hosts two types of chiral topological fermions, spi…
We perform a systematic study of the Zitterbewegung effect of fermions, which are described by a Gaussian wave with broken spatial-inversion symmetry in a three-dimensional low-energy Weyl semimetal. Our results show that the motion of fermions near the Weyl points is characterized by rectilinear motion and Zitterbewegung oscillation. The ZB oscillation is affected by the width of the Gaussian wave packet, the position of the Weyl node, and the chirality and anisotropy of the fermions. By introducing a one-dimensional cosine potential, the new generated massless fermions have lower Fermi Veloc…
We investigate the effects of a magnetic impurity in a multiband touching fermion system, specifically, a triple-component semimetal with a flat band, which can be realized in a family of transition metal silicides (CoSi family). When the chemical potential coincides with the flat band, it is expected that the impurity response of this system will be very different from that of an ordinary Dirac or Weyl semimetal of which the density of states at the Fermi level vanishes. We first determine the phase diagram within the mean-field approximation. Then, we study the local moment regime by employi…
In Weyl semimetals, charge density wave (CDW) order can spontaneously break the chiral symmetry, gap out the Weyl nodes, and drive the material into the axion insulating phase. Investigations have however been limited since CDWs are rarely seen in Weyl semimetals. Here, using scanning tunneling microscopy/spectroscopy, we report the discovery of a novel unidirectional CDW order on the (001) surface of chiral crystal CoSi - a unique Weyl semimetal with unconventional chiral fermions. The CDW is incommensurate with both lattice momentum and crystalline symmetry directions, and exhibits an intra …
We perform a detailed analysis of the magnetotransport and de Haas-van Alphen (dHvA) oscillations in crystal PdGa which is predicted to be a typical chiral Fermion semimetal from CoSi family holding a large Chern number. The unsaturated quadratic magnetoresistance (MR) and nonlinear Hall resistivity indicate that PdGa is a multi-band system without electron-hole compensation. Angle-dependent resistivity in PdGa shows weak anisotropy with twofold or threefold symmetry when the magnetic field rotates within the (1$\bar{1}$0) or (111) plane perpendicular to the current. Nine or three frequencies …
We study the low-temperature electrical and thermal conductivity of CoSi and Co$_{1-x}$M$_x$Si alloys (M = Fe, Ni; $x \leq$ 0.06). Measurements show that the low-temperature electrical conductivity of Co$_{1-x}$Fe$_{x}$Si alloys decreases at $x > $ 0.01 by an order of magnitude compared with that of pure CoSi. It was expected that both the lattice and electronic contributions to thermal conductivity would decrease in the alloys. However, our experimental results revealed that at temperatures below 20K the thermal conductivity of Fe- and Ni-containing alloys is several times larger than that of…
Quantized Photocurrents in Gapless Topological Matter
Princeton University（普林斯顿大学）；Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室）；Nanyang Technological University（南洋理工大学）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Indian Institute of Technology Delhi（德里印度理工学院）；Stanford University（斯坦福大学）；Paul Scherrer Institute（保罗谢尔研究所）；Bruker Scientific, LLC（布鲁克科学有限责任公司）；University of California, Los Angeles（加州大学洛杉矶分校）
Topological phases of matter have established a new paradigm in physics, bringing quantum phenomena to the macroscopic scale and hosting exotic emergent quasiparticles. In this thesis, I theoretically and experimentally demonstrate with my collaborators the first Weyl semimetal, TaAs, using angle-resolved photoemission spectroscopy (ARPES), directly observing its emergent Weyl fermions and topological Fermi arc surface states [Science 349, 6248 (2015); Nat. Commun. 6, 7373 (2015); PRL 116, 066802 (2016)]. Next, I discover high-degeneracy topological chiral fermions in the chiral crystals RhSi …
