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Three-dimensional Dirac semimetals are an exotic state of matter that continue to attract increasing attention due to the unique properties of their low-energy excitations. Here, by performing angle-resolved photoemission spectroscopy, we investigate the electronic structure of Au_{2}Pb across a wide temperature range. Our experimental studies on the (111)-cleaved surface unambiguously demonstrate that Au_{2}Pb is a three-dimensional Dirac semimetal characterized by the presence of a bulk Dirac cone projected off-center of the bulk Brillouin zone (BZ), in agreement with our theoretical calculations. Unusually, we observe that the bulk Dirac cone is significantly shifted by more than 0.4 eV to higher binding energies with reducing temperature, eventually going through a Lifshitz transition. The pronounced downward shift is qualitatively reproduced by our calculations indicating that an enhanced orbital overlap upon compression of the lattice, which preserves C_{4} rotational symmetry, is the main driving mechanism for the Lifshitz transition. These findings not only broaden the range of currently known materials exhibiting three-dimensional Dirac phases, but also show a viable mechanism by which it could be possible to switch on and off the contribution of the degeneracy point to electron transport without external doping.
Assuntos
Chumbo , Espectroscopia Fotoeletrônica , TemperaturaRESUMO
Artificial graphene based on molecular networks enables the creation of novel 2D materials with unique electronic and topological properties. Landau quantization has been demonstrated by CO molecules arranged on the two-dimensional electron gas on Cu(111) and the observation of electron quantization may succeed based on the created gauge fields. Recently, it was reported that instead of individual manipulation of CO molecules, simple deposition of nonpolar C60 molecules on Cu(111) and Au(111) produces artificial graphene as evidenced by Dirac cones in photoemission spectroscopy. Here, we show that C60-induced Dirac cones on Au(111) have a different origin. We argue that those are related to umklapp diffraction of surface electronic bands of Au on the molecular grid of C60 in the final state of photoemission. We test this alternative explanation by precisely probing the dimensionality of the observed conical features in the photoemission spectra, by varying both the incident photon energy and the degree of charge doping via alkali adatoms. Using density functional theory calculations and spin-resolved photoemission we reveal the origin of the replicating Au(111) bands and resolve them as deep leaky surface resonances derived from the bulk Au sp-band residing at the boundary of its surface projection. We also discuss the manifold nature of these resonances which gives rise to an onion-like Fermi surface of Au(111).
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A nearly free electron metal and a Mott insulating state can be thought of as opposite ends of the spectrum of possibilities for the motion of electrons in a solid. Understanding their interaction lies at the heart of the correlated electron problem. In the magnetic oxide metal PdCrO2, nearly free and Mott-localized electrons exist in alternating layers, forming natural heterostructures. Using angle-resolved photoemission spectroscopy, quantitatively supported by a strong coupling analysis, we show that the coupling between these layers leads to an "intertwined" excitation that is a convolution of the charge spectrum of the metallic layer and the spin susceptibility of the Mott layer. Our findings establish PdCrO2 as a model system in which to probe Kondo lattice physics and also open new routes to use the a priori nonmagnetic probe of photoemission to gain insights into the spin susceptibility of correlated electron materials.
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Band inversions are key to stabilising a variety of novel electronic states in solids, from topological surface states to the formation of symmetry-protected three-dimensional Dirac and Weyl points and nodal-line semimetals. Here, we create a band inversion not of bulk states, but rather between manifolds of surface states. We realise this by aliovalent substitution of Nb for Zr and Sb for S in the ZrSiS family of nonsymmorphic semimetals. Using angle-resolved photoemission and density-functional theory, we show how two pairs of surface states, known from ZrSiS, are driven to intersect each other near the Fermi level in NbGeSb, and to develop pronounced spin splittings. We demonstrate how mirror symmetry leads to protected crossing points in the resulting spin-orbital entangled surface band structure, thereby stabilising surface state analogues of three-dimensional Weyl points. More generally, our observations suggest new opportunities for engineering topologically and symmetry-protected states via band inversions of surface states.
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We study the low-energy surface electronic structure of the transition-metal dichalcogenide superconductor PdTe_{2} by spin- and angle-resolved photoemission, scanning tunneling microscopy, and density-functional theory-based supercell calculations. Comparing PdTe_{2} with its sister compound PtSe_{2}, we demonstrate how enhanced interlayer hopping in the Te-based material drives a band inversion within the antibonding p-orbital manifold well above the Fermi level. We show how this mediates spin-polarized topological surface states which form rich multivalley Fermi surfaces with complex spin textures. Scanning tunneling spectroscopy reveals type-II superconductivity at the surface, and moreover shows no evidence for an unconventional component of its superconducting order parameter, despite the presence of topological surface states.
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Transition-metal dichalcogenides (TMDs) are renowned for their rich and varied bulk properties, while their single-layer variants have become one of the most prominent examples of two-dimensional materials beyond graphene. Their disparate ground states largely depend on transition metal d-electron-derived electronic states, on which the vast majority of attention has been concentrated to date. Here, we focus on the chalcogen-derived states. From density-functional theory calculations together with spin- and angle-resolved photoemission, we find that these generically host a co-existence of type-I and type-II three-dimensional bulk Dirac fermions as well as ladders of topological surface states and surface resonances. We demonstrate how these naturally arise within a single p-orbital manifold as a general consequence of a trigonal crystal field, and as such can be expected across a large number of compounds. Already, we demonstrate their existence in six separate TMDs, opening routes to tune, and ultimately exploit, their topological physics.
RESUMO
Engineering and enhancing the breaking of inversion symmetry in solids-that is, allowing electrons to differentiate between 'up' and 'down'-is a key goal in condensed-matter physics and materials science because it can be used to stabilize states that are of fundamental interest and also have potential practical applications. Examples include improved ferroelectrics for memory devices and materials that host Majorana zero modes for quantum computing. Although inversion symmetry is naturally broken in several crystalline environments, such as at surfaces and interfaces, maximizing the influence of this effect on the electronic states of interest remains a challenge. Here we present a mechanism for realizing a much larger coupling of inversion-symmetry breaking to itinerant surface electrons than is typically achieved. The key element is a pronounced asymmetry of surface hopping energies-that is, a kinetic-energy-coupled inversion-symmetry breaking, the energy scale of which is a substantial fraction of the bandwidth. Using spin- and angle-resolved photoemission spectroscopy, we demonstrate that such a strong inversion-symmetry breaking, when combined with spin-orbit interactions, can mediate Rashba-like spin splittings that are much larger than would typically be expected. The energy scale of the inversion-symmetry breaking that we achieve is so large that the spin splitting in the CoO2- and RhO2-derived surface states of delafossite oxides becomes controlled by the full atomic spin-orbit coupling of the 3d and 4d transition metals, resulting in some of the largest known Rashba-like spin splittings. The core structural building blocks that facilitate the bandwidth-scaled inversion-symmetry breaking are common to numerous materials. Our findings therefore provide opportunities for creating spin-textured states and suggest routes to interfacial control of inversion-symmetry breaking in designer heterostructures of oxides and other material classes.