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Structural superlubricity is a special frictionless contact in which two crystals are in incommensurate arrangement such that relative in-plane translation is associated with vanishing energy barrier crossing. So far, it has been realized in multilayer graphene and other van der Waals two-dimensional crystals with hexagonal or triangular crystalline symmetries, leading to isotropic frictionless contacts. Directional structural superlubricity, to date unrealized in two-dimensional systems, is possible when the reciprocal lattices of the two crystals coincide in one direction only. Here, we evidence directional structural superlubricity a $\alpha$-bismuthene/graphite van der Waals system, manifested by spontaneous hopping of the islands over hundreds of nanometres at room temperature, resolved by low-energy electron microscopy and supported by registry simulations. Statistical analysis of individual and collective $\alpha$-bismuthene islands populations reveal a heavy-tailed distribution of the hopping lengths and sticking times indicative of L{\'e}vy flight dynamics, largely unobserved in condensed-matter systems., Comment: 14 pages, 10 figures (including Supplementary Information and Supplementary Figures)

The density fluctuation spectrum captures many fundamental properties of strange metals. Using momentum-resolved electron energy-loss spectroscopy (M-EELS), we recently showed that the density response of the strange metal Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$ (Bi-2212) at large momentum, $q$, exhibits a constant-in-frequency continuum [Mitrano, PNAS $\textbf{115}$, 5392 (2018); Husain, PRX $\textbf{9}$, 041062 (2019)] reminiscent of the marginal Fermi liquid (MFL) hypothesis of the late 1980s [Varma, PRL $\textbf{63}$, 1996 (1989)]. However, reconciling this observation with infrared (IR) optics experiments, which show a well-defined plasmon excitation at $q \sim 0$, has been challenging. Here we report M-EELS measurements of Bi-2212 using 4$\times$ improved momentum resolution, allowing us to reach the optical limit. For momenta $q<0.04$ r.l.u., the M-EELS data show a plasmon feature that is quantitatively consistent with IR optics. For $q>0.04$ r.l.u., the spectra become incoherent with an MFL-like, constant-in-frequency form. We speculate that, at finite frequency, $\omega$, and nonzero $q$, some attribute of this Planckian metal randomizes the probe electron, causing it to lose information about its own momentum., Comment: 9 pages, 7 figures; copy editing, improved figure resolution

A two-dimensional (2D) Weyl semimetal featuring a spin-polarized linear band dispersion and a nodal Fermi surface is a new topological phase of matter. It is a solid-state realization of Weyl fermions in an intrinsic 2D system. The nontrivial topology of 2D Weyl cones guarantees the existence of a new form of topologically protected boundary states, Fermi string edge states. In this work, we report the realization of a 2D Weyl semimetal in monolayer-thick epitaxial bismuthene grown on SnS(Se) substrate. The intrinsic band gap of bismuthene is eliminated by the space-inversion-symmetry-breaking substrate perturbations, resulting in a gapless spin-polarized Weyl band dispersion. The linear dispersion and spin polarization of the Weyl fermion states are observed in our spin and angle-resolved photoemission measurements. In addition, the scanning tunneling microscopy/spectroscopy reveals a pronounced local density of states at the edge, suggesting the existence of Fermi string edge states. These results open the door for the experimental exploration of the exotic properties of Weyl fermion states in reduced dimensions., Comment: 5 figures

Electrons and holes can spontaneously form excitons and condense in a semimetal or semiconductor, as predicted decades ago. This type of Bose condensation can happen at much higher temperatures in comparison with dilute atomic gases. Two-dimensional (2D) materials with reduced Coulomb screening around the Fermi level are promising for realizing such a system. Here we report a change in the band structure accompanied by a phase transition at about 180 K in single-layer ZrTe2 based on angle-resolved photoemission spectroscopy (ARPES) measurements. Below the transition temperature, gap opening and development of an ultra-flat band top around the zone center are observed. This gap and the phase transition are rapidly suppressed with extra carrier densities introduced by adding more layers or dopants on the surface. The results suggest the formation of an excitonic insulating ground state in single-layer ZrTe2, and the findings are rationalized by first principles calculations and a self-consistent mean-field theory. Our study provides evidence for exciton condensation in a 2D semimetal and demonstrates strong dimensionality effects on the formation of intrinsic bound electron-hole pairs in solids.

We present a systematic investigation of the edge states of two-dimensional {\alpha}-bismuthene ({\alpha}-Bi) structures self-assembled on HOPG substrates, using scanning tunnelling microscopy and scanning tunnelling spectroscopy. The measurements are carried out for 3ML, 5ML and 7ML thick Bi structures. Our spectroscopy studies reveal clear features at the edges of the 5ML and 7ML thick structures, and the positions of the edge states (ESs) coincide with the topographical step edges. In contrast, in 3ML structures the ESs appear to be absent and instead new states are sometimes observed, far from the topographical edge. These states are associated with a moir\'e pattern and result from strain-induced modulation of the topology. Our observations demonstrate the impact on the edge states of coupling to adjacent structures., Comment: 17 pages, 6 figures

Doped SrTi1-xNbxO3 exhibits superconductivity and a mid-infrared optical response reminiscent of copper-oxide superconductors. Strangely, its plasma frequency, omega_p, increases by a factor of ~3 when cooling from 300 K to 20 K, without any accepted explanation. Here, we present momentum-resolved electron energy loss spectroscopy (M-EELS) measurements of SrTi1-xNbxO3 at nonzero momentum, q. We find that the infrared feature previously identified as a plasmon is present at large q in insulating SrTiO3, where it exhibits the same temperature dependence and may be identified as an anharmonic, multiphonon background. Doping with Nb increases its peak energy and total spectral weight, drawing this background to lower q where it becomes visible in IR optics experiments. We conclude that the "plasmon" in doped SrTi1-xNbxO3 is not a free-carrier mode, but a composite excitation that inherits its unusual properties from the lattice anharmonicity of the insulator., Comment: 5 pages, 4 figures

The discovery of graphene has stimulated enormous interest in two-dimensional (2D) electron gas with linear band structure. 2D Dirac materials possess many intriguing physical properties such as high carrier mobility and zero-energy Landau level thanks to the relativistic dispersion and chiral spin/pseudospin texture. 2D Dirac states discovered so far are exclusively pinned at high-symmetry points of the Brillouin zone, for example, surface Dirac states at $\overline{\Gamma}$ in topological insulators Bi$_2$Se(Te)$_3$ and Dirac cones at $K$ and $K'$ in graphene. In this work, we report the realization of 2D Dirac states at generic $k$-points in antimony atomic layers with phosphorene structure ($i.e.$ $\alpha$-antimonene). The unpinned nature enables versatile ways to control the locations of the Dirac points in momentum space. In addition, dispersions around the unpinned Dirac points exhibit intrinsically anisotropic behaviors due to the reduced symmetry of generic momentum points. These properties make the $\alpha$-antimonene films a promising platform for exploring interesting physics in unpinned 2D Dirac fermions that are distinct from the conventional Dirac states in graphene., Comment: 5 figures

The quasi-one-dimensional chiral charge density wave (CDW) material (TaSe$_4$)$_2$I has been recently predicted to host Kramers-Weyl (KW) fermions which should exist in the vicinity of high symmetry points in the Brillouin zone in chiral materials with strong spin-orbit coupling. However, direct spectroscopic evidence of KW fermions is limited. Here we use helicity-dependent laser-based angle resolved photoemission spectroscopy (ARPES) in conjunction with tight-binding and first-principles calculations to identify KW fermions in (TaSe$_4$)$_2$I. We find that topological and symmetry considerations place distinct constraints on the (pseudo-) spin texture and the observed spectra around a KW node. We further reveal an interplay between the spin texture around the chiral KW node and the onset of CDW order in (TaSe$_4$)$_2$I. Our findings highlight the unique topological nature of (TaSe$_4$)$_2$I and provide a pathway for identifying KW fermions in other chiral materials.

Tuning interactions between Dirac states in graphene has attracted enormous interest because it can modify the electronic spectrum of the two-dimensional material, enhance electron correlations, and give rise to novel condensed-matter phases such as superconductors, Mott insulators, Wigner crystals and quantum anomalous Hall insulators. Previous works predominantly focus on the flat band dispersion of coupled Dirac states from different graphene layers. In this work, we propose a new route to realizing flat band physics in monolayer graphene under a periodic modulation from substrates. We take gaphene/SiC heterostructure as a role model and demonstrate experimentally the substrate modulation leads to Dirac fermion cloning and consequently, the proximity of the two Dirac cones of monolayer graphene in momentum space. Our theoretical modeling captures the cloning mechanism of Dirac states and indicates that flat bands can emerge at certain magic lattice constants of substrate when the period of modulation becomes nearly commensurate with the $(\sqrt{3}\times\sqrt{3})R30^{\circ}$ supercell of graphene. The results show that the epitaxial monolayer graphene is a promising platform for exploring exotic many-body quantum phases arising from interactions between Dirac electrons.

We use first-principles simulation and virtual crystal approximation to reveal the unique double band inversion and topological phase transition in Ge1-xSnx alloys. Wavefunction parity, spatial charge distribution and surface state spectrum analyses suggest that the band inversion in Ge1-xSnx is relayed by its first valence band. As the system evolves from Ge to {\alpha}-Sn, its conduction band moves down, and inverts with the first and the second valence bands consecutively. The first band inversion makes the system nontrivial, while the second one does not change the topological invariant of the system. Both the band inversions yield surface modes spanning the individual inverted gaps, but only the surface mode in the upper gap associates with the nontrivial nature of tensile-strained {\alpha}-Sn., Comment: 5 pages, 6 figures

State-of-the-art topological devices require the use topological surface states to drive electronic transport. In this study, we examine a tunable topological system, $Ge(Bi_{x}Sb_{1-x})_{2}Te_{4}$, for a range of 'x' values from 0 to 1, using a combination of Fourier Transform Scanning Tunneling Spectroscopy (FT-STS) and Angle-Resolved Photoemission Spectroscopy (ARPES). Our results show that the Dirac point shifts linearly with 'x', crossing the Fermi energy near x = 0.7. This novel observation of a smoothly tunable, isolated Dirac point crossing through the topological transport regime and having strong linear dependence with substitution can be critical for future topological spintronics applications., Comment: 18 Pages, 9 Figures, including Appendix

Atomic-scale smooth thin films are keys to successful integration and proper function of many multilayer-structured devices. However, the intrinsic island-like growth mode prevents human being from realizing such ultrasmooth films of many important functional materials. To solve this problem, we propose a negative entropy-infusing method that employs evanescent waves to enhance the downward interlayer diffusion of adatoms and thus transform the island-like growth mode to the layer-by-layer growth mode. The formulas of the optical force and the lowered diffusion barrier were derived, and the application of this theory on a simplified example demonstrates significantly improved surface morphologies through numerical simulations., Comment: It contribute a generic approach to alter intrinsic 3D growth mode to 2D growth mode using an external effect arising from evanescent waves, which is expected to remove the obstacle of intrinsic island-like growth mode from growing ultra-smooth thin films

Understanding carrier creation and evolution in materials initiated by pulsed optical excitation is central to developing ultrafast optoelectronics. We demonstrate herein that the dynamic response of a system can be drastically modified when its physical dimension is reduced to the atomic scale, the ultimate limit of device miniaturization. A comparative study of single-layer (SL) tungsten diselenide(WSe2) relative to bulk WSe2 shows substantial differences in the transient response as measured by time- and angle-resolved photoemission spectroscopy (TRARPES). The conduction-band minimum in bulk WSe2, populated by optical pumping, decays promptly. The corresponding decay for SL WSe2 is much slower and exhibits two time constants. The results indicate the presence of two distinct decay channels in the SL that are correlated with the breaking of space inversion symmetry in the two-dimensional limit. This symmetry breaking lifts the spin degeneracy of the bands, which in turn causes the blockage of decay for one spin channel. The stark contrast between the single layer and the bulk illustrates the basic carrier scattering processes operating at different timescales that can be substantially modified by dimensional and symmetry-reduction effects.

Interfacial electron-phonon coupling in ultrathin films has attracted much interest; it can give rise to novel effects and phenomena, including enhanced superconductivity. Here we report an observation of strong kinks in the energy dispersions of quantum well states in ultrathin Yb films grown on graphite. These kinks, arising from interfacial electron-phonon coupling, are most prominent for films with a preferred ("magic") thickness of 4 monolayers, which are strained and hole doped by the substrate. The energy position of the kinks agrees well with the optical phonon energy of graphite, and the extracted electron-phonon coupling strength {\lambda} shows a large subband dependence, with a maximum value up to 0.6. The kinks decay rapidly with increasing film thickness, consistent with its interfacial origin. The variation of {\lambda} is correlated with evolution of the electronic wave function amplitudes at the interface. A Lifshitz transition occurs just beyond the magic thickness where the heavy Yb 5d bands begin to populate right below the Fermi level., Comment: 4 figures

Two-dimensional (2D) Dirac-like electron gases have attracted tremendous research interest ever since the discovery of free-standing graphene. The linear energy dispersion and non-trivial Berry phase play the pivotal role in the remarkable electronic, optical, mechanical and chemical properties of 2D Dirac materials. The known 2D Dirac materials are gapless only within certain approximations, for example, in the absence of SOC. Here we report a route to establishing robust Dirac cones in 2D materials with nonsymmorphic crystal lattice. The nonsymmorphic symmetry enforces Dirac-like band dispersions around certain high-symmetry momenta in the presence of SOC. Through $\mu$-ARPES measurements we observe Dirac-like band dispersions in $\alpha$-bismuthene. The nonsymmorphic lattice symmetry is confirmed by $\mu$-LEED and STM. Our first-principles simulations and theoretical topological analysis demonstrate the correspondence between nonsymmorphic symmetry and Dirac states. This mechanism can be straightforwardly generalized to other nonsymmorphic materials. The results open the door for the search of symmetry enforced Dirac fermions in the vast uncharted world of nonsymmorphic 2D materials.

Combining angle-resolved photoemission spectroscopy and magneto-transport measurements, we systematically investigated the possible origin of the extreme magnetoresistance in Pr/Sm mono-antimonides/bismuthides (PrSb, SmSb, PrBi, SmBi). Our photoemission measurements reveal that the bulk band inversion and surface states are absent (present) in Pr/Sm antimonides (bismuthides), implying that topological surface states are unlikely to play an important role for the observed extreme magnetoresistance. We found that the electron-hole compensation is well satisfied in all these compounds and the bulk band structure exhibits no obvious temperature dependence from 10 K up to 150 K. Simultaneous fittings of the magnetoresistance and Hall coefficient reveal that the carrier mobility is dramatically enhanced at low temperature, which naturally explains the suppression of extreme magnetoresistance at high temperatures. Our results therefore show that the extreme magnetoresistance in these compounds can be well accounted for by the two-band model with good electron-hole compensation. Finally, we found that both PrSb and SmSb exhibit highly linear bulk bands near the X point and lie close to the transition point between a topologically trivial and nontrivial phase, which might be relevant for the observed anomalous quantum oscillations., Comment: 6 figures

Elastic strain has the potential for a controlled manipulation of the band gap and spin-polarized Dirac states of topological materials, which can lead to pseudo-magnetic-field effects, helical flat bands and topological phase transitions. However, practical realization of these exotic phenomena is challenging and yet to be achieved. Here, we show that the Dirac surface states of the topological insulator Bi2Se3 can be reversibly tuned by an externally applied elastic strain. Performing in-situ x-ray diffraction and in-situ angle-resolved photoemission spectroscopy measurements during tensile testing of epitaxial Bi2Se3 films bonded onto a flexible substrate, we demonstrate elastic strains of up to 2.1% and quantify the resulting reversible changes in the topological surface state. Our study establishes the functional relationship between the lattice and electronic structures of Bi2Se3 and, more generally, demonstrates a new route toward momentum-resolved mapping of strain-induced band structure changes.

Layered quasi-two-dimensional transition metal dichalcogenides (TMDCs), which can be readily made in ultrathin films, offer excellent opportunities for studying how dimensionality affects electronic structure and physical properties. Among all TMDCs, NbSe2 is of special interest; bulk NbSe2 hosts a charge-density-wave phase at low temperatures and has the highest known superconducting transition temperature, and these properties can be substantially modified in the ultrathin film limit. Motivated by these effects, we report herein a study of few-layer NbSe2 films, with a well-defined single-domain orientation, epitaxially grown on Gallium Arsenide (GaAs). Angle-resolved photoemission spectroscopy (ARPES) was used to determine the electronic band structure and the Fermi surface as a function of layer thickness; first-principles band structure calculations were performed for comparison. The results show interesting changes as the film thickness increases from a monolayer (ML) to several layers. The most notable changes occur between a ML and a bilayer, where the inversion symmetry in bulk NbSe2 is preserved in the bilayer but not in the ML. The results illustrate some basic dimensional effects and provide a basis for further exploring and understanding the properties of NbSe2., Comment: 15 pages, 4 figures

Here we report the evolution of bulk band structure and surface states in rare earth mono-bismuthides with partially filled f shell. Utilizing synchrotron-based photoemission spectroscopy, we determined the three-dimensional bulk band structure and identified the bulk band inversions near the X points, which, according to the topological theory, could give rise to nontrivial band topology with odd number of gapless topological surface states. Near the surface Gamma bar point, no clear evidence for predicted gapless topological surface state is observed due to its strong hybridization with the bulk bands. Near the M bar point, the two surface states, due to projections from two inequivalent bulk band inversions, interact and give rise to two peculiar sets of gapped surface states. The bulk band inversions and corresponding surface states can be tuned substantially by varying rare earth elements, in good agreement with density-functional theory calculations assuming local f electrons. Our study therefore establishes rare earth mono-bismuthides as an interesting class of materials possessing tunable electronic properties and magnetism, providing a promising platform to search for novel properties in potentially correlated topological materials., Comment: 7 figures

Stanene (single-layer grey tin), with an electronic structure akin to that of graphene but exhibiting a much larger spin-orbit gap, offers a promising platform for room-temperature electronics based on the quantum spin Hall (QSH) effect. This material has received much theoretical attention, but a suitable substrate for stanene growth that results in an overall gapped electronic structure has been elusive; a sizable gap is necessary for room-temperature applications. Here, we report a study of stanene epitaxially grown on the (111)B-face of indium antimonide (InSb). Angle-resolved photoemission spectroscopy (ARPES) measurements reveal a gap of 0.44 eV, in agreement with our first-principles calculations. The results indicate that stanene on InSb(111) is a strong contender for electronic QSH applications., Comment: 15 pages, 4 figures

Van der Waals heterostructures have recently been identified as providing many opportunities to create new two-dimensional materials, and in particular to produce materials with topologically interesting states. Here we show that it is possible to create such heterostructures with multiple topological phases in a single nanoscale island. We discuss their growth within the framework of diffusion-limited aggregation, the formation of moir\'e patterns due to the differing crystallographies of the materials comprising the heterostructure, and the potential to engineer both the electronic structure as well as local variations of topological order. In particular we show that it is possible to build islands which include both the hexagonal $\beta$- and rectangular $\alpha$-forms of antimonene, on top of the topological insulator $\alpha$-bismuthene. This is the first experimental realisation of $\alpha$-antimonene, and we show that it is a topologically non-trivial material in the quantum spin Hall class., Comment: 6 pages, 3 figures, plus Supplementary material (9 pages, 6 figures)

Three-dimensional (3D) topological Dirac semimetals (TDSs) are rare but important as a versatile platform for exploring exotic electronic properties and topological phase transitions. A quintessential feature of TDSs is 3D Dirac fermions associated with bulk electronic states near the Fermi level. Using angle-resolved photoemission spectroscopy (ARPES), we have observed such bulk Dirac cones in epitaxially-grown {\alpha}-Sn films on InSb(111), the first such TDS system realized in an elemental form. First-principles calculations confirm that epitaxial strain is key to the formation of the TDS phase. A phase diagram is established that connects the 3D TDS phase through a singular point of a zero-gap semimetal phase to a topological insulator (TI) phase. The nature of the Dirac cone crosses over from 3D to 2D as the film thickness is reduced.