Max Planck Institute for Chemical Physics of Solids

Topological insulators and topological semimetals are both new classes of quantum materials, which are characterized by surface states induced by the topology of the bulk band structure. Topological Dirac or Weyl semimetals show linear dispersion around nodes, termed the Dirac or Weyl points, as the three-dimensional analog of graphene. We review the basic concepts and compare these topological states of matter from the materials perspective with a special focus on Weyl semimetals. The TaAs family is the ideal materials class to introduce the signatures of Weyl points in a pedagogical way, from Fermi arcs to the chiral magnetotransport properties, followed by hunting for the type-II Weyl semimetals in WTe 2 , MoTe 2 , and related compounds. Many materials are members of big families, and topological properties can be tuned. As one example, we introduce the multifunctional topological materials, Heusler compounds, in which both topological insulators and magnetic Weyl semimetals can be found. Instead of a comprehensive review, this article is expected to serve as a helpful introduction and summary by taking a snapshot of the quickly expanding field.

The search for highly efficient and low-cost catalysts is one of the main driving forces in catalytic chemistry. Current strategies for the catalyst design focus on increasing the number and activity of local catalytic sites, such as the edge sites of molybdenum disulfides in the hydrogen evolution reaction (HER). Here, the study proposes and demonstrates a different principle that goes beyond local site optimization by utilizing topological electronic states to spur catalytic activity. For HER, excellent catalysts have been found among the transition-metal monopnictides-NbP, TaP, NbAs, and TaAs-which are recently discovered to be topological Weyl semimetals. Here the study shows that the combination of robust topological surface states and large room temperature carrier mobility, both of which originate from bulk Dirac bands of the Weyl semimetal, is a recipe for high activity HER catalysts. This approach has the potential to go beyond graphene based composite photocatalysts where graphene simply provides a high mobility medium without any active catalytic sites that have been found in these topological materials. Thus, the work provides a guiding principle for the discovery of novel catalysts from the emerging field of topological materials.

Weyl semimetals (WSMs) are topological quantum states wherein the electronic bands disperse linearly around pairs of nodes with fixed chirality, the Weyl points. In WSMs, nonorthogonal electric and magnetic fields induce an exotic phenomenon known as the chiral anomaly, resulting in an unconventional negative longitudinal magnetoresistance, the chiral-magnetic effect. However, it remains an open question to which extent this effect survives when chirality is not well-defined. Here, we establish the detailed Fermi-surface topology of the recently identified WSM TaP via combined angle-resolved quantum-oscillation spectra and band-structure calculations. The Fermi surface forms banana-shaped electron and hole pockets surrounding pairs of Weyl points. Although this means that chirality is ill-defined in TaP, we observe a large negative longitudinal magnetoresistance. We show that the magnetoresistance can be affected by a magnetic field-induced inhomogeneous current distribution inside the sample.

The search for large-gap quantum spin Hall (QSH) insulators and effective approaches to tune QSH states is important for both fundamental and practical interests. Based on first-principles calculations we find two-dimensional tin films are QSH insulators with sizable bulk gaps of 0.3 eV, sufficiently large for practical applications at room temperature. These QSH states can be effectively tuned by chemical functionalization and by external strain. The mechanism for the QSH effect in this system is band inversion at the Γ point, similar to the case of a HgTe quantum well. With surface doping of magnetic elements, the quantum anomalous Hall effect could also be realized.

INTRODUCTION Condensed-matter systems have recently become a fertile ground for the discovery of fermionic particles and phenomena predicted in high-energy physics; examples include Majorana fermions, as well as Dirac and Weyl semimetals. However, fermions in condensed-matter systems are not constrained by Poincare symmetry. Instead, they must only respect the crystal symmetry of one of the 230 space groups. Hence, there is the potential to find and classify free fermionic excitations in solid-state systems that have no high-energy counterparts. RATIONALE The guiding principle of our classification is to find irreducible representations of the little group of lattice symmetries at high-symmetry points in the Brillouin zone (BZ) for each of the 230 space groups (SGs), the dimension of which corresponds to the number of bands that meet at the high-symmetry point. Because we are interested in systems with spin-orbit coupling, we considered only the double-valued representations, where a 2π rotation gives a minus sign. Furthermore, we considered systems with time-reversal symmetry that squares to –1. For each unconventional representation, we computed the low-energy k · p Hamiltonian near the band crossings by writing down all terms allowed by the crystal symmetry. This allows us to further differentiate the band crossings by the degeneracy along lines and planes that emanate from the high-symmetry point, and also to compute topological invariants. For point degeneracies, we computed the monopole charge of the band-crossing; for line nodes, we computed the Berry phase of loops encircling the nodes. RESULTS We found that three space groups exhibit symmetry-protected three-band crossings. In two cases, this results in a threefold degenerate point node, whereas the third case results in a line node away from the high-symmetry point. These crossings are required to have a nonzero Chern number and hence display surface Fermi arcs. However, upon applying a magnetic field, they have an unusual Landau level structure, which distinguishes them from single and double Weyl points. Under the action of spatial symmetries, these fermions transform as spin-1 particles, as a consequence of the interplay between nonsymmorphic space group symmetries and spin. Additionally, we found that six space groups can host sixfold degeneracies. Two of these consist of two threefold degeneracies with opposite chirality, forced to be degenerate by the combination of time reversal and inversion symmetry, and can be described as “sixfold Dirac points.” The other four are distinct. Furthermore, seven space groups can host eightfold degeneracies. In two cases, the eightfold degeneracies are required; all bands come in groups of eight that cross at a particular point in the BZ. These two cases also exhibit fourfold degenerate line nodes, from which other semimetals can be derived: By adding strain or a magnetic field, these line nodes split into Weyl, Dirac, or line node semimetals. For all the three-, six- and eight-band crossings, nonsymmorphic symmetries play a crucial role in protecting the band crossing. Last, we found that seven space groups may host fourfold degenerate “spin-3/2” fermions at high symmetry points. Like their spin-1 counterparts, these quasiparticles host Fermi surfaces with nonzero Chern number. Unlike the other cases we considered, however, these fermions can be stabilized by both symmorphic and nonsymmorphic symmetries. Three space groups that host these excitations also host unconventional fermions at other points in the BZ. We propose nearly 40 candidate materials that realize each type of fermion near the Fermi level, as verified with ab initio calculations. Seventeen of these have been previously synthesized in single-crystal form, whereas others have been reported in powder form. CONCLUSION We have analyzed all types of fermions that can occur in spin-orbit coupled crystals with time-reversal symmetry and explored their topological properties. We found that there are several distinct types of such unconventional excitations, which are differentiated by their degeneracies at and along high-symmetry points, lines, and surfaces. We found natural generalizations of Weyl points: three- and four-band crossings described by a simple k · S Hamiltonian, where S i is the set of spin generators in either the spin-1 or spin-3/2 representations. These points carry a Chern number and, consequently, can exhibit Fermi arc surface states. We also found excitations with six- and eightfold degeneracies. These higher-band crossings create a tunable platform to realize topological semimetals by applying an external magnetic field or strain to the fourfold degenerate line nodes. Last, we propose realizations for each species of fermion in known materials, many of which are known to exist in single-crystal form. Fermi arcs from a threefold degeneracy. Shown is the surface density of states as a function of momentum for a crystal in SG 214 with bulk threefold degeneracies that project to (0.25, 0.25) and (–0.25, –0.25). Two Fermi arcs emanate from these points, indicating that their monopole charge is 2. The arcs then merge with the surface projection of bulk states near the origin.

Magnetic Weyl semimetals with broken time-reversal symmetry are expected to generate strong intrinsic anomalous Hall effects, due to their large Berry curvature. Here, we report a magnetic Weyl semimetal candidate, Co3Sn2S2, with a quasi-two-dimensional crystal structure consisting of stacked kagome lattices. This lattice provides an excellent platform for hosting exotic topological quantum states. We observe a negative magnetoresistance that is consistent with the chiral anomaly expected from the presence of Weyl fermions close to the Fermi level. The anomalous Hall conductivity is robust against both increased temperature and charge conductivity, which corroborates the intrinsic Berry-curvature mechanism in momentum space. Owing to the low carrier density in this material and the considerably enhanced Berry curvature from its band structure, the anomalous Hall conductivity and the anomalous Hall angle simultaneously reach 1,130 Ω−1 cm−1 and 20%, respectively, an order of magnitude larger than typical magnetic systems. Combining the kagome-lattice structure and the long-range out-of-plane ferromagnetic order of Co3Sn2S2, we expect that this material is an excellent candidate for observation of the quantum anomalous Hall state in the two-dimensional limit.

The rare-earth monopnictide LaBi exhibits exotic magneto-transport properties, including an extremely large and anisotropic magnetoresistance. Experimental evidence for topological surface states is still missing although band inversions have been postulated to induce a topological phase in LaBi. In this work, we have revealed the existence of surface states of LaBi through the observation of three Dirac cones: two coexist at the corners and one appears at the centre of the Brillouin zone, by employing angle-resolved photoemission spectroscopy in conjunction with ab initio calculations. The odd number of surface Dirac cones is a direct consequence of the odd number of band inversions in the bulk band structure, thereby proving that LaBi is a topological, compensated semimetal, which is equivalent to a time-reversal invariant topological insulator. Our findings provide insight into the topological surface states of LaBi's semi-metallicity and related magneto-transport properties.

Floquet engineering, the control of quantum systems using periodic driving, is an old concept in condensed matter physics dating back to ideas such as the inverse Faraday effect. However, there is a renewed interest in this concept owing to ( a) the rapid developments in laser and ultrafast spectroscopy techniques, ( b) discovery and understanding of various “quantum materials” hosting interesting exotic quantum properties, and ( c) communication with different areas of physics such as artificial matter and nonequilibrium quantum statistical physics. Here, starting from a nontechnical introduction with emphasis on the Floquet picture and effective Hamiltonians, we review the recent applications of Floquet engineering in ultrafast, nonlinear phenomena in the solid state. In particular, Floquet topological states and their application to ultrafast spintronics and strongly correlated electron systems are overviewed.

It is well established that the anomalous Hall effect displayed by a ferromagnet scales with its magnetization. Therefore, an antiferromagnet that has no net magnetization should exhibit no anomalous Hall effect. We show that the noncolinear triangular antiferromagnet Mn3Ge exhibits a large anomalous Hall effect comparable to that of ferromagnetic metals; the magnitude of the anomalous conductivity is ~500 (ohm·cm)(-1) at 2 K and ~50 (ohm·cm)(-1) at room temperature. The angular dependence of the anomalous Hall effect measurements confirms that the small residual in-plane magnetic moment has no role in the observed effect except to control the chirality of the spin triangular structure. Our theoretical calculations demonstrate that the large anomalous Hall effect in Mn3Ge originates from a nonvanishing Berry curvature that arises from the chiral spin structure, and that also results in a large spin Hall effect of 1100 (ħ/e) (ohm·cm)(-1), comparable to that of platinum. The present results pave the way toward the realization of room temperature antiferromagnetic spintronics and spin Hall effect-based data storage devices.

Magnetic Weyl semimetals Weyl semimetals (WSMs)—materials that host exotic quasiparticles called Weyl fermions—must break either spatial inversion or time-reversal symmetry. A number of WSMs that break inversion symmetry have been identified, but showing unambiguously that a material is a time-reversal-breaking WSM is tricky. Three groups now provide spectroscopic evidence for this latter state in magnetic materials (see the Perspective by da Silva Neto). Belopolski et al. probed the material Co 2 MnGa using angle-resolved photoemission spectroscopy, revealing exotic drumhead surface states. Using the same technique, Liu et al. studied the material Co 3 Sn 2 S 2 , which was complemented by the scanning tunneling spectroscopy measurements of Morali et al. These magnetic WSM states provide an ideal setting for exotic transport effects. Science , this issue p. 1278 , p. 1282 , p. 1286 ; see also p. 1248

Floquet engineering, the control of quantum systems using periodic driving, is an old concept in condensed matter physics dating back to ideas such as the inverse Faraday effect. However, there is a renewed interest in this concept owing to (a) the rapid developments in laser and ultrafast spectroscopy techniques, (b) discovery and understanding of various "quantum materials" hosting interesting exotic quantum properties, and (c) communication with different areas of physics such as artificial matter and nonequilibrium quantum statistical physics. Here, starting from a nontechnical introduction with emphasis on the Floquet picture and effective Hamiltonians, we review the recent applications of Floquet engineering in ultrafast, nonlinear phenomena in the solid state. In particular, Floquet topological states and their application to ultrafast spintronics and strongly correlated electron systems are overviewed.

Transition metal dichalcogenides have attracted research interest over the last few decades due to their interesting structural chemistry, unusual electronic properties, rich intercalation chemistry and wide spectrum of potential applications. Despite the fact that the majority of related research focuses on semiconducting transition-metal dichalcogenides (for example, MoS2), recently discovered unexpected properties of WTe2 are provoking strong interest in semimetallic transition metal dichalcogenides featuring large magnetoresistance, pressure-driven superconductivity and Weyl semimetal states. We investigate the sister compound of WTe2, MoTe2, predicted to be a Weyl semimetal and a quantum spin Hall insulator in bulk and monolayer form, respectively. We find that bulk MoTe2 exhibits superconductivity with a transition temperature of 0.10 K. Application of external pressure dramatically enhances the transition temperature up to maximum value of 8.2 K at 11.7 GPa. The observed dome-shaped superconductivity phase diagram provides insights into the interplay between superconductivity and topological physics.

We report a comprehensive small angle neutron scattering study of the magnetic phase diagram of the doped semiconductor ${\text{Fe}}_{1\ensuremath{-}x}{\text{Co}}_{x}\text{Si}$ for $x=0.2$. For magnetic field parallel to the neutron beam we observe a sixfold intensity pattern under field cooling. The regime of the skyrmion lattice is highly hysteretic and extents over a wide temperature range as may be expected due to the site disorder of the Fe and Co atoms. Our study identifies ${\text{Fe}}_{1\ensuremath{-}x}{\text{Co}}_{x}\text{Si}$ as the second material in which a skyrmion lattice forms and establishes that skyrmion lattices exist also in doped semiconductors.

Magnetic Weyl semimetals Weyl semimetals (WSMs)—materials that host exotic quasiparticles called Weyl fermions—must break either spatial inversion or time-reversal symmetry. A number of WSMs that break inversion symmetry have been identified, but showing unambiguously that a material is a time-reversal-breaking WSM is tricky. Three groups now provide spectroscopic evidence for this latter state in magnetic materials (see the Perspective by da Silva Neto). Belopolski et al. probed the material Co 2 MnGa using angle-resolved photoemission spectroscopy, revealing exotic drumhead surface states. Using the same technique, Liu et al. studied the material Co 3 Sn 2 S 2 , which was complemented by the scanning tunneling spectroscopy measurements of Morali et al. These magnetic WSM states provide an ideal setting for exotic transport effects. Science , this issue p. 1278 , p. 1282 , p. 1286 ; see also p. 1248

We investigate the orthorhombic phase $({T}_{d})$ of the layered transition-metal dichalcogenide ${\mathrm{MoTe}}_{2}$ as a Weyl semimetal candidate. ${\mathrm{MoTe}}_{2}$ exhibits four pairs of Weyl points lying slightly above $(\ensuremath{\sim}6\phantom{\rule{0.16em}{0ex}}\mathrm{meV})$ the Fermi energy in the bulk band structure. Different from its cousin ${\mathrm{WTe}}_{2}$, which was recently predicted to be a type-II Weyl semimetal, the spacing between each pair of Weyl points is found to be as large as 4% of the reciprocal lattice in ${\mathrm{MoTe}}_{2}$ (six times larger than that of ${\mathrm{WTe}}_{2}$). When projected onto the surface, the Weyl points are connected by Fermi arcs, which can be easily accessed by angle-resolved photoemission spectroscopy due to the large Weyl point separation. In addition, we show that the correlation effect or strain can drive ${\mathrm{MoTe}}_{2}$ from a type-II to a type-I Weyl semimetal.

Abstract Lead‐free double perovskites have great potential as stable and nontoxic optoelectronic materials. Recently, Cs 2 AgBiBr 6 has emerged as a promising material, with suboptimal photon‐to‐charge carrier conversion efficiency, yet well suited for high‐energy photon‐detection applications. Here, the optoelectronic and structural properties of pure Cs 2 AgBiBr 6 and alkali‐metal‐substituted (Cs 1− x Y x ) 2 AgBiBr 6 (Y: Rb + , K + , Na + ; x = 0.02) single crystals are investigated. Strikingly, alkali‐substitution entails a tunability to the material system in its response to X‐rays and structural properties that is most strongly revealed in Rb‐substituted compounds whose X‐ray sensitivity outperforms other double‐perovskite‐based devices reported. While the fundamental nature and magnitude of the bandgap remains unchanged, the alkali‐substituted materials exhibit a threefold boost in their fundamental carrier recombination lifetime at room temperature. Moreover, an enhanced electron–acoustic phonon scattering is found compared to Cs 2 AgBiBr 6 . The study thus paves the way for employing cation substitution to tune the properties of double perovskites toward a new material platform for optoelectronics.

The fourth version of the program package WinCSD is multi-purpose computer software for crystallographic calculations using single-crystal and powder X-ray and neutron diffraction data. The software environment and the graphical user interface are built using the platform of the Microsoft .NET Framework, which grants independence from changing Windows operating systems and allows for transferring to other operating systems. Graphic applications use the three-dimensional OpenGL graphics language. WinCSD covers the complete spectrum of crystallographic calculations, including powder diffraction pattern deconvolution, crystal structure solution and refinement in 3 + d space, refinement of the multipole model and electron density studies from diffraction data, and graphical representation of crystallographic information.

Quantum phase transitions arise in many-body systems because of competing interactions that promote rivaling ground states. Recent years have seen the identification of continuous quantum phase transitions, or quantum critical points, in a host of antiferromagnetic heavy-fermion compounds. Studies of the interplay between the various effects have revealed new classes of quantum critical points and are uncovering a plethora of new quantum phases. At the same time, quantum criticality has provided fresh insights into the electronic, magnetic, and superconducting properties of the heavy-fermion metals. We review these developments, discuss the open issues, and outline some directions for future research.

Gold surfaces host special electronic states that have been understood as a prototype of Shockley surface states. These surface states are commonly employed to benchmark the capability of angle-resolved photoemission spectroscopy (ARPES) and scanning tunnelling spectroscopy. Here we show that these Shockley surface states can be reinterpreted as topologically derived surface states (TDSSs) of a topological insulator (TI), a recently discovered quantum state. Based on band structure calculations, the Z2-type invariants of gold can be well-defined to characterize a TI. Further, our ARPES measurement validates TDSSs by detecting the dispersion of unoccupied surface states. The same TDSSs are also recognized on surfaces of other well-known noble metals (for example, silver, copper, platinum and palladium), which shines a new light on these long-known surface states.

Abstract A functional of the same‐spin electron pair density is proposed as a measure of electron localizability. This functional yields the average number of same‐spin electron pairs in a region Ω enclosing a fixed charge. The functional equals zero if the fixed charge in Ω originates from one electron only, with all other same‐spin electrons outside the region Ω. Then, the correlation of the electronic motion in Ω and thus the localizability of an electron is high. If the motion of the same‐spin electrons becomes less correlated, more electrons participate in the fixed charge contained in Ω, the average number of same‐spin electron pairs (the functional) increases. In the Hartree–Fock approximation the Taylor expansion of the proposed localizability functional can be related to the electron localization function of Becke and Edgecombe without using an arbitrary reference to the uniform electron gas. © 2003 Wiley Periodicals, Inc. Int J Quantum Chem, 2004