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Water hydrogen bonding is extremely versatile; approximately 20 ice structures and several types of clathrate hydrate structures have been identified. These crystalline water structures form at temperatures below room temperature and/or at high pressure. We used transmission electron microscopy to study a new crystalline water structure in a clathrate state that is prepared by sandwiching gas-supersaturated water between graphene layers under ambient conditions. In this clathrate state, water molecules form a three-dimensional hydrogen bonding network that encloses gas-filled cages 2-4 nm in size. We derived the crystalline water structure by recording and analyzing electron diffraction patterns and performing first-principles calculations. The structure consists purely of pentagonal rings and has a topology similar to that of water ice XVII. The study proposed a mechanism for the formation of the clathrate state. The present results improve the understanding of interactions among water and small nonpolar molecules and offer novel insights into the local structures of ambient liquid water.

The electronic structure and phonon dispersion of XS$_2$ with X = Co, Tc, Ti, Ru, Nb, and Rh in the monolayer MoS$_2$ structure with trigonal-prismatic coordination are studied from first principles. Although each XS$_2$ is dynamically unstable, CoS$_2$, TcS$_2$, RuS$_2$, and RhS$_2$ can be stabilized by developing charge density waves in the (2$\times$2) supercell, leading to metal-insulator transitions. Without really needing the metal-insulator transitions and large atomic distortions, additional energy may be gained in the total energy by mixing transition metal elements to create high-entropy combinations for X, presenting a wide range of high-entropy XS$_2$ compounds that exhibit a variety of band structures, including direct- and indirect-gap semiconductors, metals, and semimetals., Comment: 5 pages, 3 figures, 1 table

Charge density wave (CDW) resulted from a small distortion in the lattice is able to create new orders beyond the original lattice. In 2H-NbSe2, one of the layered transition metal dichalcogenides (TMD), the 3x3 charge order appears in two-dimensional (2D) layers. Although CDW is usually described by a sine wave, the spatial distribution within a 2D layer has never been systematically visualized. Here by using scanning tunneling microscopy (STM) and density functional theory (DFT), we have monitored the evolution of 3x3 CDW along c-axis and realized a nearly tomography scan of CDW of the topmost layer. The results show that the strength of 3x3 charge order varies while increasing the tunneling current. The 3x3 charge order is relatively strong at the outermost Se level and decreases while probing in between Se and Nb levels. Interestingly, the 3x3 charge order gets strong again as reaching Nb level but along with a phase shift. We further calculated the orbital charge distributions and found that both CDW intensity modulation and phase shift are strongly correlated with the distribution of Se p orbitals and Nb d orbitals., Comment: 12 pages, 4 figures

The formation of a charge density wave (CDW) in two-dimensional (2D) materials caused by Peierls instability is a controversial topic. This study investigates the extensively debated role of Fermi surface nesting in causing the CDW state in 2H-NbSe$_{2}$ materials. Four NbSe$_{2}$ structures (i.e., normal, stripe, filled, and hollow structures) are identified on the basis of the characteristics in scanning tunneling microscopy images and first-principles simulations. The calculations reveal that the filled phase corresponds to Peierls' description; that is, it exhibits fully opened gaps at the CDW Brillouin zone boundary, resulting in a drop at the Fermi level in the density of states and the scanning tunneling spectroscopy spectra. The electronic susceptibility and phonon instability in the normal phase indicate that the Fermi surface nesting is triggered by two nesting vectors, whereas the involvement of only one nesting vector leads to the stripe phase. This comprehensive study demonstrates that the filled phase of NbSe$_{2}$ can be categorized as a Peierls-instability-induced CDW in 2D systems., Comment: 4 figures

Silicon and germanium are the well-known materials used to manufacture electronic devices for the integrated circuits but they themselves are not considered as promising options for interconnecting the devices due to their semiconducting nature. We have discovered that both Si and Ge atoms can form unexpected metallic monolayer structures which are more stable than the extensively studied semimetallic silicene and germanene, respectively. More importantly, the newly discovered two-dimensional allotropes of Si and Ge have Fermi velocities superior to the Dirac fermions in graphene, indicating that the metal wires needed in the silicon-based integrated circuits can be made of Si atom itself without incompatibility, allowing for all-silicon-based integrated circuits., Comment: 10 pages, 3 figures, 1 table

The intersections of topology, geometry and strong correlations offer many opportunities for exotic quantum phases to emerge in condensed matter systems. Weyl fermions, in particular, provide an ideal platform for exploring the dynamical instabilities of single-particle physics under interactions. Despite its fundamental role in relativistic field theory, the concept of causality and the associated spacetime light cone and event horizon has not been considered in connection with interacting Weyl fermionic excitations in quantum matter. Here, by using charge-density wave (CDW) as an example, we unveil the behavior of interacting Weyl fermions and show that a Weyl fermion in a system can open a band gap by interacting only with other Weyl fermions that lie within its energy-momentum dispersion cone. In this sense, causal connections or interactions are only possible within overlapping dispersion cones and each dispersion cone thus constitutes a solid-state analogue of the more conventional `event horizon' of high-energy physics. Our study provides a universal framework for considering interacting relativistic quasiparticles in condensed matter by separating them into energy-like and momentum-like relationships in analogy with the time-like and space-like events in high-energy physics. Finally, we consider two different candidate materials for hosting the Weyl CDW phase: (TaSe$_4$)$_2$I and Mo$_3$Al$_2$C. Our study greatly enriches the phenomenology and unveils new connections between condensed matter and high-energy physics.

The representative cuprate, La$_{2-x}$M$_x$CuO$_4$, with M = Sr and $x = 1/8$ is studied via first-principles calculations in the high-temperature tetragonal (HTT), low-temperature orthorhombic (LTO), and low-temperature less-orthorhombic (LTLO) structures. By suppressing the magnetism and superconductivity, the LTLO phase, which has rarely been observed in La$_{2-x}$Sr$_x$CuO$_4$, is found to be the ground state, where the structural phase transitions, HTT$\rightarrow$LTO$\rightarrow$LTLO, can be understood via phonon instability. While the La-O composition is identified to be responsible for the phonon softening, the superconducting CuO$_2$ layer is dynamically stable. The LTLO phase, which can exhibit a $\sim$20 meV splitting in the density of states, is proposed to have an intimate relationship with the observed pseudogap and the charge density wave giving the stripe. We argue that at low temperatures, the superconducting LTO La$_{1.875}$Sr$_{0.125}$CuO$_4$ competes with the phonon-preferred LTLO phase by spontaneously forming the Cooper pairs, resulting in suppressing the stripe. Therefore, the revealed LTLO phase is indispensable for understanding La$_{2-x}$Sr$_x$CuO$_4$., Comment: 5 pages, 4 figures

A method to analyze optical transitions is developed by combining the Kubo-Greenwood formula with the unfolding method to construct an unfolded electronic band structure with optical transition weights, which allows us to investigate how optical transitions are perturbed by imperfections such as impurity, vacancy, and structural distortions. Based on the Kubo-Greenwood formula, we first calculate frequency-dependent optical conductivity based on the first-principles electronic structure calculations using the linear combinations of atomic orbitals. Benefiting from the atomic orbital basis sets, the frequency-dependent optical conductivity can be traced back to their individual components before summations over all of $k$ points and bands. As a result, optical transition weights of the material can be put on the unfolded electronic band structure to show contributions at different $k$ points and bands. This method is especially useful to study the effects of broken symmetry in the optical transitions due to presence of impurities in the materials. As a demonstration, decomposed optical transition weights of a monolayer Si-doped graphene are shown in the electronic band structure., Comment: 9 pages, 6 figures, and 1 table

Ge atoms segregating on zirconium diboride thin films grown on Ge(111) were found to crystallize into a two-dimensional bitriangular structure which was recently predicted to be a flat band material. Angle-resolved photoemission experiments together with theoretical calculations verified the existence of a nearly flat band in spite of non-negligible in-plane long-range hopping and interactions with the substrate. This provides the first experimental evidence that a flat band can emerge from the electronic coupling between atoms and not from the geometry of the atomic structure.

First-principles phonon calculations have been widely performed for studying vibrational properties of condensed matter, where the dynamical matrix is commonly constructed via supercell force-constant calculations or the linear response approach. With different manners, a supercell can be introduced in both methods. Unless the supercell is large enough, the interpolated phonon property highly depends on the shape and size of the supercell and the imposed periodicity could give unphysical results that can be easily overlooked. Along this line, the concept of partition of force constants is discussed, and addressed by NaCl, PbTiO$_3$, monolayer CrI$_3$, and twisted bilayer graphene as examples for illustrating the effects of the imposed supercell periodicity. To diminish the unphysical effects, a simple method of partitioning force constants, which relies only on the translational symmetry and interatomic distances, is demonstrated to be able to deliver reasonable results. The partition method is also compatible with the mixed-space approach for describing LO-TO splitting. The proper partition is especially important for studying moderate-size systems with low symmetry, such as two-dimensional materials on substrates, and useful for the implementation of phonon calculations in first-principles packages using atomic basis functions, where symmetry operations are usually not applied owing to the suitability for large-scale calculations., Comment: 12 pages, 8 figures

The interplay of hopping parameters that can give rise to flat bands in consequence of quantum interference in electronic, photonic, and other interesting materials has become an extensively studied topic. Most of the recognized structures having flat bands are the lattices that can be understood by the mathematical theory of line graphs, such as the Lieb, kagome, and checkerboard lattices. Here, we demonstrate that the structures that can realize the same kind of flat bands given by those well-known lattices hosting exotic quantum phases are more flexible. The flat bands belonging to the recognized structures can be ideally embedded into the new structures that cannot be considered as the original ones in terms of a unitary transformation. The uncovered mechanism enriches the understanding of physics behind the localized quantum states and broadens the choice of materials that can be used for designing electronic and photonic devices from the zero band dispersion., Comment: accepted for publication in PRB; 6 pages, 3 figures, 1 table

We present a general formula for the tight-binding representation of momentum matrix elements needed for calculating the conductivity based on the Kubo-Greenwood formula using atomic orbitals, which are in general not orthogonal to other orbitals at different sites. In particular, the position matrix element is demonstrated to be important for delivering the exact momentum matrix element. This general formula, applicable to both orthonormal and non-orthonormal bases, solely needs the information of the position matrix elements and the ingredients that have already contained in the tight-binding representation. We then study the anomalous Hall conductivity in the standard example, ferromagnetic bcc Fe, by a first-principles tight-binding Hamiltonian. By assuming the commutation relation $\hat{\vec{p}} = (i m_e/\hbar) [\hat{H},\hat{\vec{r}}]$, the obtained frequency-dependent Hall conductivity is found to be in good agreement with existing theoretical and experimental results. Better agreement with experiments can be reached by introducing a reasonable bandwidth renormalization, evidencing the strong correlation among 3$d$ orbitals in bcc Fe. Since a tight-binding Hamiltonian can be straightforwardly obtained after finishing a first-principles calculation using atomic basis functions that are generated before the self-consistent calculation, the derived formula is particularly useful for those first-principles calculations., Comment: 8 pages, 2 figures

Detecting the spectroscopic signatures of Dirac-like quasiparticles in emergent topological materials is crucial for searching their potential applications. Magnetometry is a powerful tool for fathoming electrons in solids, yet its ability for discerning Dirac-like quasiparticles has not been recognized. Adopting the probes of magnetic torque and parallel magnetization for the archetype Weyl semimetal TaAs in strong magnetic field, we observed a quasi-linear field dependent effective transverse magnetization and a strongly enhanced parallel magnetization when the system is in the quantum limit. Distinct from the saturating magnetic responses for massive carriers, the non-saturating signals of TaAs in strong field is consistent with our newly developed magnetization calculation for a Weyl fermion system in an arbitrary angle. Our results for the first time establish a thermodynamic criterion for detecting the unique magnetic response of 3D massless Weyl fermions in the quantum limit., Comment: Submitted on 14th November 17. Version of original submission. SI is not included

Engineering atomic-scale structures allows great manipulation of physical properties and chemical processes for advanced technology. We show that the B atoms deployed at the centers of honeycombs in boron sheets, borophene, behave as nearly perfect electron donors for filling the graphitic $\sigma$ bonding states without forming additional in-plane bonds by first-principles calculations. The dilute electron density distribution owing to the weak bonding surrounding the center atoms provides easier atomic-scale engineering and is highly tunable via in-plane strain, promising for practical applications, such as modulating the extraordinarily high thermal conductance that exceeds the reported value in graphene. The hidden honeycomb bonding structure suggests an unusual energy sequence of core electrons that has been verified by our high-resolution core-level photoelectron spectroscopy measurements. With the experimental and theoretical evidence, we demonstrate that borophene exhibits a peculiar bonding structure and is distinctive among two-dimensional materials., Comment: 5 pages, 3 figures, 1 table

We propose that the quasi-one-dimensional molybdenum selenide compound Tl2-xMo6Se6 is a time-reversal-invariant topological superconductor induced by inter-sublattice pairing, even in the absence of spin-orbit coupling (SOC). No noticeable change in superconductivity is observed in Tl-deficient (0<=x<=0.1) compounds. At weak SOC, the superconductor prefers the triplet d vector lying perpendicular to the chain direction and two-dimensional E2u symmetry, which is driven to a nematic order by spontaneous rotation symmetry breaking. The locking energy of the d vector is estimated to be weak and hence the proof of its direction would rely on tunnelling or phase-sensitive measurements., Comment: 6 pages, 3 figures, 1 table

A way to represent the band structure that distinguishes between energy-momentum and energy-crystal momentum relationships is proposed upon the band-unfolding concept. This momentum-resolved band structure offers better understanding of the physical processes requiring the information of wave functions in momentum space and provides a good description of angle-resolved photoelectron spectroscopy (ARPES) spectra together with a still informative band structure. Following this approach, we demonstrate that Dirac cones in graphene are intrinsically broken in momentum space and can be described by a conceptual unit cell smaller than the primitive unit cell. This hidden degree of freedom can be measured by ARPES experiments as missing weight that is retrievable by probing the chirality and Berry phases by linearly and circularly polarized light. Having the energy-momentum relationship, we provide alternative understanding of the retrieved momentum intensity, that is, the retrieved momentum intensity is assisted with the properties of final states, not from the Dirac cones directly. The revealed broken Dirac cones and momenta supplied by the lattice give interesting ingredients for designing advanced nanodevices., Comment: 6 pages, 2 figures

Orbital-related physics attracts growing interest in condensed matter research, but direct real-space access of the orbital degree of freedom is challenging. Here we report a first, real-space, imaging of a surface- assisted orbital ordered structure on a cobalt-terminated surface of the well-studied heavy fermion compound CeCoIn5. Within small tip-sample distances, the cobalt atoms on a cleaved (001) surface take on dumbbell shapes alternatingly aligned in the [100] and [010] directions in scanning tunneling microscopy topographies. First- principles calculations reveal that this structure is a consequence of the staggered dxz-dyz orbital order triggered by enhanced on-site Coulomb interaction at the surface. This so-far-overlooked surface-assisted orbital ordering may prevail in transition metal oxides, heavy fermion superconductors and other materials., Comment: 15 pages, 7 figures

The recent discovery of a Weyl semimetal in TaAs offers the first Weyl fermion observed in nature and dramatically broadens the classification of topological phases. However, in TaAs it has proven challenging to study the rich transport phenomena arising from emergent Weyl fermions. The series Mo$_x$W$_{1-x}$Te$_2$ are inversion-breaking, layered, tunable semimetals already under study as a promising platform for new electronics and recently proposed to host Type II, or strongly Lorentz-violating, Weyl fermions. Here we report the discovery of a Weyl semimetal in Mo$_x$W$_{1-x}$Te$_2$ at $x = 25\%$. We use pump-probe angle-resolved photoemission spectroscopy (pump-probe ARPES) to directly observe a topological Fermi arc above the Fermi level, demonstrating a Weyl semimetal. The excellent agreement with calculation suggests that Mo$_x$W$_{1-x}$Te$_2$ is the first Type II Weyl semimetal. We also find that certain Weyl points are at the Fermi level, making Mo$_x$W$_{1-x}$Te$_2$ a promising platform for transport and optics experiments on Weyl semimetals.

Recent studies of core-level X-ray photoelectron spectroscopy (XPS) spectra of silicene on ZrB$_2$(0001) were found to be inconsistent with the density of states (DOS) of a planar-like structure that has been proposed as the ground state by density functional theory (DFT). To resolve the discrepancy, a reexamination of the XPS spectra and direct theoretical access of accurate single-particle excitation energies are desired. By analyzing the XPS data using symmetric Voigt functions, different binding energies and its sequence of Si $2p$ orbitals can be assigned from previously reported ones where asymmetric pseudo-Voigt functions are adopted. Theoretically, we have adopted an approach developed very recently, which follows the sophisticated $\Delta$ self-consistent field ($\Delta$SCF) methods, to study the single-particle excitation of core states. In the calculations, each single-particle energy and the renormalized core-hole charge density are calculated straightforwardly via two SCF calculations. By comparing the results, the theoretical core-level absolute binding energies including the splitting due to spin-orbit coupling are in good agreement with the observed high-resolution XPS spectra. The good agreement not only resolves the puzzling discrepancy between experiment and theory (DOS) but also advocates the success of DFT in describing many-body interactions of electrons at the surface., Comment: 8 pages, 3 figures, 3 tables

A general method is presented to calculate absolute binding energies of core levels in metals and insulators, based on a penalty functional and an exact Coulomb cutoff method in a framework of the density functional theory. The spurious interaction of core holes between supercells is avoided by the exact Coulomb cutoff method, while the variational penalty functional enables us to treat multiplet splittings due to chemical shift, spin-orbit coupling, and exchange interaction on equal footing, both of which are not accessible by previous methods. It is demonstrated that the absolute binding energies of core levels for both metals and insulators are calculated by the proposed method in a mean absolute (percentage) error of 0.4 eV (0.16~\%) for eight cases compared to experimental values measured with X-ray photoemission spectroscopy within a generalized gradient approximation to the exchange-correlation functional., Comment: 6 pages, 4 figures, a supplemental table

It has recently been proposed that electronic band structures in crystals give rise to a previously overlooked type of Weyl fermion, which violates Lorentz invariance and, consequently, is forbidden in particle physics. It was further predicted that Mo$_x$W$_{1-x}$Te$_2$ may realize such a Type II Weyl fermion. One crucial challenge is that the Weyl points in Mo$_x$W$_{1-x}$Te$_2$ are predicted to lie above the Fermi level. Here, by studying a simple model for a Type II Weyl cone, we clarify the importance of accessing the unoccupied band structure to demonstrate that Mo$_x$W$_{1-x}$Te$_2$ is a Weyl semimetal. Then, we use pump-probe angle-resolved photoemission spectroscopy (pump-probe ARPES) to directly observe the unoccupied band structure of Mo$_x$W$_{1-x}$Te$_2$. For the first time, we directly access states $> 0.2$ eV above the Fermi level. By comparing our results with $\textit{ab initio}$ calculations, we conclude that we directly observe the surface state containing the topological Fermi arc. Our work opens the way to studying the unoccupied band structure as well as the time-domain relaxation dynamics of Mo$_x$W$_{1-x}$Te$_2$ and related transition metal dichalcogenides., Comment: Incorporates earlier results presented in arXiv:1512.09099, by the same authors

The recent discovery of the first Weyl semimetal in TaAs provides the first observation of a Weyl fermion in nature and demonstrates a novel type of anomalous surface state, the Fermi arc. Like topological insulators, the bulk topological invariants of a Weyl semimetal are uniquely fixed by the surface states of a bulk sample. Here, we present a set of distinct conditions, accessible by angle-resolved photoemission spectroscopy (ARPES), each of which demonstrates topological Fermi arcs in a surface state band structure, with minimal reliance on calculation. We apply these results to TaAs and NbP. For the first time, we rigorously demonstrate a non-zero Chern number in TaAs by counting chiral edge modes on a closed loop. We further show that it is unreasonable to directly observe Fermi arcs in NbP by ARPES within available experimental resolution and spectral linewidth. Our results are general and apply to any new material to demonstrate a Weyl semimetal., Comment: Accepted by Physical Review Letters. Incorporates earlier results presented in arXiv:1509.07465, by the same authors, but with additional analysis, interpretation and commentary

Weyl semimetals provide the realization of Weyl fermions in solid-state physics. Among all the physical phenomena that are enabled by Weyl semimetals, the chiral anomaly is the most unusual one. Here, we report signatures of the chiral anomaly in the magneto-transport measurements on the first Weyl semimetal TaAs. We show negative magnetoresistance under parallel electric and magnetic fields, that is, unlike most metals whose resistivity increases under an external magnetic field, we observe that our high mobility TaAs samples become more conductive as a magnetic field is applied along the direction of the current for certain ranges of the field strength. We present systematically detailed data and careful analyses, which allow us to exclude other possible origins of the observed negative magnetoresistance. Our transport data, corroborated by photoemission measurements, first-principles calculations and theoretical analyses, collectively demonstrate signatures of the Weyl fermion chiral anomaly in the magneto-transport of TaAs., Comment: This is an extended version of arXiv:1503.02630. This new version, which includes additional data and analyses, is published in Nature Communications 7, 10735 (2016). http://www.nature.com/ncomms/2016/160225/ncomms10735/full/ncomms10735.html

Weyl semimetals have sparked intense research interest, but experimental work has been limited to the TaAs family of compounds. Recently, a number of theoretical works have predicted that compounds in the Mo$_x$W$_{1-x}$Te$_2$ series are Weyl semimetals. Such proposals are particularly exciting because Mo$_x$W$_{1-x}$Te$_2$ has a quasi two-dimensional crystal structure well-suited to many transport experiments, while WTe$_2$ and MoTe$_2$ have already been the subject of numerous proposals for device applications. However, with available ARPES techniques it is challenging to demonstrate a Weyl semimetal in Mo$_x$W$_{1-x}$Te$_2$. According to the predictions, the Weyl points are above the Fermi level, the system approaches two critical points as a function of doping, there are many irrelevant bulk bands, the Fermi arcs are nearly degenerate with bulk bands and the bulk band gap is small. Here, we study Mo$_x$W$_{1-x}$Te$_2$ for $x = 0.07$ and 0.45 using pump-probe ARPES. The system exhibits a dramatic response to the pump laser and we successfully access states $> 0.2$eV above the Fermi level. For the first time, we observe direct, experimental signatures of Fermi arcs in Mo$_x$W$_{1-x}$Te$_2$, which agree well with theoretical calculations of the surface states. However, we caution that the interpretation of these features depends sensitively on free parameters in the surface state calculation. We comment on the prospect of conclusively demonstrating a Weyl semimetal in Mo$_x$W$_{1-x}$Te$_2$., Comment: 24 pages, 4 figures

Weyl semimetals are extremely interesting. Although the first Weyl semimetal was recently discovered in TaAs, research progress is still significantly hindered due to the lack of robust and ideal materials candidates. In order to observe the many predicted exotic phenomena that arise from Weyl fermions, it is of critical importance to find robust and ideal Weyl semimetals, which have fewer Weyl nodes and more importantly whose Weyl nodes are well separated in momentum space and are located close to the chemical potential in energy. In this paper, we propose by far the most robust and ideal Weyl semimetal candidate in the inversion breaking, single crystalline compound tantalum sulfide Ta$_3$S$_2$ with new and novel properties beyond TaAs. We find that Ta$_3$S$_2$ has only 8 Weyl nodes, all of which have the same energy that is merely 10 meV below the chemical potential. Crucially, our results show that Ta$_3$S$_2$ has the largest $k$-space separation between Weyl nodes among known Weyl semimetal candidates, which is about twice larger than TaAs and twenty times larger than the predicted value in WTe$_2$. Moreover, we predict that increasing the lattice by $<4\%$ can annihilate all Weyl nodes, driving a novel topological metal-to-insulator transition from a Weyl semimetal state to a topological insulator state. We further discover that changing the lattice constant can move the Weyl nodes and the van Hove singularities with enhanced density of states to the chemical potential. Our prediction provides a critically needed robust candidate for this rapidly developing field. The well separated Weyl nodes, the topological metal-to-insulator transition and the remarkable tunabilities suggest Ta$_3$S$_2$'s potential as the ideal platform in future device-applications based on Weyl semimetals., Comment: 25 pages, 6 figures

The recent discovery of the first Weyl semimetal in TaAs provides the first observation of a Weyl fermion in nature. Such a topological semimetal features a novel type of anomalous surface state, the Fermi arc, which connects a pair of Weyl nodes through the boundary of the crystal. Here, we present theoretical calculations of the quasi-particle interference (QPI) patterns that arise from the surface states including the topological Fermi arcs in the Weyl semimetals TaAs and NbP. Most importantly, we discover that the QPI exhibits termination-points that are fingerprints of the Weyl nodes in the interference pattern. Our results, for the first time, propose an interference signature of the topological Fermi arcs in TaAs, which provides important guidelines for STM measurements on this prototypical Weyl semimetal compound. The scattering channels presented here is relevant to transport phenomena on the surface of the TaAs class of Weyl semimetals. Our work is also the first systematic calculation of the quantum interferences from the Fermi arc surface states, which is in general useful for future STM studies on other Weyl semimetals., Comment: 15pages, 6 figures

Weyl semimetals may open a new era in condensed matter physics, materials science and nanotech after graphene and topological insulators. We report the first atomic scale view of the surface states of a Weyl semimetal (NbP) using scanning tunneling microscopy/spectroscopy. We observe coherent quantum interference patterns that arise from the scattering of quasiparticles near point defects on the surface. The measurements reveal the surface electronic structure both below and above the chemical potential in both real and reciprocal spaces. Moreover, the interference maps uncover the scattering processes of NbP's exotic surface states. Through comparison between experimental data and theoretical calculations, we further discover that the scattering channels are largely restricted by the orbital and/or spin texture of the surface band. The visualization of the scattering processes can help design novel transport effects and electronics on the topological surface of a Weyl semimetal., Comment: Submitted October 2015

A Weyl semimetal is a new state of matter that host Weyl fermions as quasiparticle excitations. The Weyl fermions at zero energy correspond to points of bulk band degeneracy, Weyl nodes, which are separated in momentum space and are connected only through the crystal's boundary by an exotic Fermi arc surface state. We experimentally measure the spin polarization of the Fermi arcs in the first experimentally discovered Weyl semimetal TaAs. Our spin data, for the first time, reveal that the Fermi arcs' spin polarization magnitude is as large as 80% and possesses a spin texture that is completely in-plane. Moreover, we demonstrate that the chirality of the Weyl nodes in TaAs cannot be inferred by the spin texture of the Fermi arcs. The observed non-degenerate property of the Fermi arcs is important for the establishment of its exact topological nature, which reveal that spins on the arc form a novel type of 2D matter. Additionally, the nearly full spin polarization we observed (~80%) may be useful in spintronic applications., Comment: 4 figures, 15 pages

The recent experimental discovery of a Weyl semimetal in TaAs provides the first observation of a Weyl fermion in nature and demonstrates a novel type of anomalous surface state band structure, consisting of Fermi arcs. So far, work has focused on Weyl semimetals with strong spin-orbit coupling (SOC). However, Weyl semimetals with weak SOC may allow tunable spin-splitting for device applications and may exhibit a crossover to a spinless topological phase, such as a Dirac line semimetal in the case of spinless TaAs. NbP, isostructural to TaAs, may realize the first Weyl semimetal in the limit of weak SOC. Here we study the surface states of NbP by angle-resolved photoemission spectroscopy (ARPES) and we find that we $\textit{cannot}$ show Fermi arcs based on our experimental data alone. We present an $\textit{ab initio}$ calculation of the surface states of NbP and we find that the Weyl points are too close and the Fermi level is too low to show Fermi arcs either by (1) directly measuring an arc or (2) counting chiralities of edge modes on a closed path. Nonetheless, the excellent agreement between our experimental data and numerical calculations suggests that NbP is a Weyl semimetal, consistent with TaAs, and that we observe trivial surface states which evolve continuously from the topological Fermi arcs above the Fermi level. Based on these results, we propose a slightly different criterion for a Fermi arc which, unlike (1) and (2) above, does not require us to resolve Weyl points or the spin splitting of surface states. We propose that raising the Fermi level by $> 20$ meV would make it possible to observe a Fermi arc using this criterion in NbP. Our work offers insight into Weyl semimetals with weak spin-orbit coupling, as well as the crossover from the spinful topological Weyl semimetal to the spinless topological Dirac line semimetal., Comment: This work was based on the theoretical prediction of a Weyl semimetal in the TaAs family of compounds, http://www.nature.com/ncomms/2015/150612/ncomms8373/full/ncomms8373.html

Weyl semimetals may open a new era in condensed matter physics because they provide the first example of Weyl fermions, realize a new topological classification even though the system is gapless, exhibit Fermi arc surface states and demonstrate the chiral anomaly and other exotic quantum phenomena. So far, the only known Weyl semimetals are the TaAs class of materials. Here, we propose the existence of a tunable Weyl metallic state in Mo$_x$W$_{1-x}$Te$_2$ via our first-principles calculations. We demonstrate that a 2% Mo doping is sufficient to stabilize the Weyl metal state not only at low temperatures but also at room temperatures. We show that, within a moderate doping regime, the momentum space distance between the Weyl nodes and hence the length of the Fermi arcs can be continuously tuned from zero to ~ 3% of the Brillouin zone size via changing Mo concentration, thus increasing the topological strength of the system. Our results provide an experimentally feasible route to realizing Weyl physics in the layered compound Mo$_x$W$_{1-x}$Te$_2$, where non-saturating magneto-resistance and pressure driven superconductivity have been observed.

The family of binary compounds including TaAs, TaP, NbAs, and NbP was recently discovered as the first realization of Weyl semimetals. In order to develop a comprehensive description of the charge carriers in these Weyl semimetals, we performed systematic electronic structure calculations which reveal the nature of Fermi surfaces and their complex interconnectivity in TaAs, TaP, NbAs, and NbP. Our work report the first comparative and comprehensive study of Fermi surface topology and band structure details of all known members of the Weyl semimetal family and provide the necessary building blocks for advancing our understanding of their unique topologically protected low-energy Weyl fermion physics.

Weyl semimetals are expected to open up new horizons in physics and materials science because they provide the first realization of Weyl fermions and exhibit protected Fermi arc surface states. However, they had been found to be extremely rare in nature. Recently, a family of compounds, consisting of TaAs, TaP, NbAs and NbP was predicted as Weyl semimetal candidates. Here, we experimentally realize a Weyl semimetal state in TaP. Using photoemission spectroscopy, we directly observe the Weyl fermion cones and nodes in the bulk and the Fermi arcs on the surface. Moreover, we find that the surface states show an unexpectedly rich structure, including both topological Fermi arcs and several topologically-trivial closed contours in the vicinity of the Weyl points, which provides a promising platform to study the interplay between topological and trivial surface states on a Weyl semimetal's surface. We directly demonstrate the bulk-boundary correspondence and hence establish the topologically nontrivial nature of the Weyl semimetal state in TaP, by resolving the net number of chiral edge modes on a closed path that encloses the Weyl node. This also provides, for the first time, an experimentally practical approach to demonstrating a bulk Weyl fermion from a surface state dispersion measured in photoemission., Comment: Theoretical discovery of TaP as a Weyl Fermion material (November 2014) was made in http://www.nature.com/ncomms/2015/150612/ncomms8373/full/ncomms8373.html

Weyl nodes are topological objects in three-dimensional metals. Their topological property can be revealed by studying the high-field transport properties of a Weyl semimetal. While the energy of the lowest Landau band (LLB) of a conventional Fermi pocket always increases with magnetic field due to the zero point energy, the LLB of Weyl cones remains at zero energy unless a strong magnetic field couples the Weyl fermions of opposite chirality. In the Weyl semimetal TaP, we achieve such a magnetic coupling between the electron-like Fermi pockets arising from the W1 Weyl fermions. As a result, their LLBs move above chemical potential, leading to a sharp sign reversal in the Hall resistivity at a specific magnetic field corresponding to the W1 Weyl node separation. By contrast, despite having almost identical carrier density, the annihilation is unobserved for the hole-like pockets because the W2 Weyl nodes are much further separated. These key findings, corroborated by other systematic analyses, reveal the nontrivial topology of Weyl fermions in high-field measurements., Comment: the Fig2 and Fig 3 are not compatible with this version

We report the identification of a Topological Nodal-Line Semimetal state in PbTaSe2., Comment: 20 pages, 5 figures, Related papers at http://physics.princeton.edu/zahidhasangroup/

We report the discovery of Weyl semimetal NbAs featuring topological Fermi arc surface states., Comment: Accepted by NaturePhysics (in press), Theoretical discovery of NbAs as a Weyl Fermion material (November 2014): http://www.nature.com/ncomms/2015/150612/ncomms8373/full/ncomms8373.html

We identify a Weyl semimetal state in an inversion breaking, stoichiometric compound strontium silicide, SrSi$_2$, with many new and novel properties that are distinct from the TaAs family. We theoretically show that SrSi$_2$ is a Weyl semimetal even without spin-orbit coupling and that, after the inclusion of spin-orbit coupling, two Weyl fermions stick together forming an exotic double Weyl fermion with quadratic dispersions and a higher chiral topological charge of 2. Moreover, we find that the Weyl nodes with opposite charges are located at different energies due to the absence of mirror symmetry in SrSi$_2$, leading to a unique topological quantum response that an external magnetic field can induce a dissipationless current. Our systematic results not only identify a much-needed robust Weyl semimetal candidate but also open the door to new topological Weyl physics that is not possible in the TaAs family of materials., Comment: 15 pages, 4 Figures

We report the experimental discovery of Adler-Bell-Jackiw chiral anomaly in a Weyl semimetal crystal., Comment: 18 pages, 4 Figures; Related experimental papers at http://physics.princeton.edu/zahidhasangroup/index.html

We report discovery of a Weyl Fermion semimetal and Topological Fermi arcs in TaAs, Comment: This work (Science 2015) is based on the first theoretical prediction of TaAs family as Weyl Semimetals, see Nature Commun. (November, 2014) our earlier theory work at http://www.nature.com/ncomms/2015/150612/ncomms8373/full/ncomms8373.html (November, 2014), arXiv:1501.00755

The recent discoveries of Dirac fermions in graphene and on the surface of topological insulators have ignited worldwide interest in physics and materials science. A Weyl semimetal is an unusual crystal where electrons also behave as massless quasi-particles but interestingly they are not Dirac fermions. These massless particles, Weyl fermions, were originally considered in massless quantum electrodynamics but have not been observed as a fundamental particle in nature. A Weyl semimetal provides a condensed matter realization of Weyl fermions, leading to unique transport properties with novel device applications. Here, we THEORETICALLY identify the first Weyl semimetal in a class of stoichiometric materials (TaAs, NbAs, NbP, TaP), which break crystalline inversion symmetry, including TaAs, TaP, NbAs and NbP. Our first-principles calculation-based predictions on TaAs reveal the spin-polarized Weyl cones and Fermi arc surface states in this compound. We also observe pairs of Weyl points with the same chiral charge which project onto the same point in the surface Brillouin zone, giving rise to multiple Fermi arcs connecting to a given Weyl point. Our results show that TaAs is the first topological semimetal identified which does not depend on fine-tuning of chemical composition or magnetic order, greatly facilitating an exploration of Weyl physics in real materials. (Note added: This theoretical prediction of November 2014 (see paper in Nature Communications) was the basis for the first experimental discovery of Weyl Fermions and topological Fermi arcs in TaAs recently published in Science (2015) at http://www.sciencemag.org/content/early/2015/07/15/science.aaa9297.full.pdf), Comment: Submitted in November'14 (First theoretical prediction of TaAs family as Weyl Semimetals, see (November, 2014) submission date at http://www.nature.com/ncomms/2015/150612/ncomms8373/full/ncomms8373.html

The origin of the large-scale stripe pattern of epitaxial silicene on the ZrB$_2$(0001) surface observed by scanning tunneling microscope experiments is revealed by first-principles calculations. Without stripes, the ($\sqrt{3}\times\sqrt{3}$)-reconstructed, one-atom-thick Si layer is found to exhibit a "zero-frequency" phonon instability at the $M$ point. In order to avoid a divergent response, the relevant phonon mode triggers the spontaneous formation of a new phase with a particular stripe pattern offering a way to lower both the atomic surface density and the total energy of silicene on the particular substrate. The observed mechanism is a way for the system to handle epitaxial strain and may therefore be more common in two-dimensional epitaxial materials exhibiting a small lattice mismatch with the substrate., Comment: 5 pages, 4 figures

So far, it represents a challenging task to reproduce angle-resolved photoelectron (ARPES) spectra of epitaxial silicene by first-principles calculations. Here, we report on the resolution of the previously controversial issue related to the structural configuration of silicene on the ZrB$_2$(0001) surface and its band structure. In particular, by representing the band structure in a large Brillouin zone associated with a single Si atom, it is found that the imaginary part of the one-particle Green's function follows the spectral weight observed in ARPES spectra. By additionally varying the in-plane lattice constant, the results of density functional theory calculations and ARPES data obtained in a wide energy range converge into the "planar-like" phase and provide the orbital character of electronic states in the vicinity of the Fermi level. It is anticipated that the choice of a smaller commensurate unit cell for the representation of the electronic structure will be useful for the study of epitaxial two-dimensional materials on various substrates in general., Comment: 7 pages, 7 figures