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We report an unconventional quantum spin Hall phase in the monolayer T$_\text{d}$-WTe$_2$, which exhibits hitherto unknown features in other topological materials. The low-symmetry of the structure induces a canted spin texture in the $yz$ plane, which dictates the spin polarization of topologically protected boundary states. Additionally, the spin Hall conductivity gets quantized ($2e^2/h$) with a spin quantization axis parallel to the canting direction. These findings are based on large-scale quantum simulations of the spin Hall conductivity tensor and nonlocal resistances in multi-probe geometries using a realistic tight-binding model elaborated from first-principle methods. The observation of this canted quantum spin Hall effect, related to the formation of topological edge states with nontrivial spin polarization, demands for specific experimental design and suggests interesting alternatives for manipulating spin information in topological materials., Comment: For comments please contact josehugo.garcia@icn2.cat

The spin polarization induced by the spin Hall effect (SHE) in thin films typically points out of the plane. This is rooted on the specific symmetries of traditionally studied systems, not in a fundamental constraint. Recently, experiments on few-layer ${\rm MoTe}_2$ and ${\rm WTe}_2$ showed that the reduced symmetry of these strong spin-orbit coupling materials enables a new form of {\it canted} spin Hall effect, characterized by concurrent in-plane and out-of-plane spin polarizations. Here, through quantum transport calculations on realistic device geometries, including disorder, we predict a very large gate-tunable SHE figure of merit $\lambda_s\theta_{xy}\sim 1\text{--}50$ nm in ${\rm MoTe}_2$ and ${\rm WTe}_2$ monolayers that significantly exceeds values of conventional SHE materials. This stems from a concurrent long spin diffusion length ($\lambda_s$) and charge-to-spin interconversion efficiency as large as $\theta_{xy} \approx 80$\%, originating from momentum-invariant (persistent) spin textures together with large spin Berry curvature along the Fermi contour, respectively. Generalization to other materials and specific guidelines for unambiguous experimental confirmation are proposed, paving the way towards exploiting such phenomena in spintronic devices. These findings vividly emphasize how crystal symmetry and electronic topology can govern the intrinsic SHE and spin relaxation, and how they may be exploited to broaden the range and efficiency of spintronic materials and functionalities., Comment: Published version, Phys. Rev. Reserach

The ability to switch magnetic elements by spin-orbit-induced torques has recently attracted much attention for a path towards high-performance, non-volatile memories with low power consumption. Realizing efficient spin-orbit-based switching requires harnessing both new materials and novel physics to obtain high charge-to-spin conversion efficiencies, thus making the choice of spin source crucial. Here we report the observation of spin-orbit torque switching in bilayers consisting of a semimetallic film of 1T'-MoTe2 adjacent to permalloy. Deterministic switching is achieved without external magnetic fields at room temperature, and the switching occurs with currents one order of magnitude smaller than those typical in devices using the best-performing heavy metals. The thickness dependence can be understood if the interfacial spin-orbit contribution is considered in addition to the bulk spin Hall effect. Further threefold reduction in the switching current is demonstrated with resort to dumbbell-shaped magnetic elements. These findings foretell exciting prospects of using MoTe2 for low-power semimetal material based spin devices.

We explore in detail the electronic phases of a system consisting of three non-colinear arrays of coupled quantum wires, each rotated 120 degrees with respect to the next. A perturbative renormalization-group analysis reveals that multiple correlated states can be stabilized: a $s$-wave or $d \pm id$ superconductor, a charge density wave insulator, a two-dimensional Fermi liquid, and a 2D Luttinger liquid (also known as smectic metal or sliding Luttinger liquid). The model provides an effective description of electronic interactions in small-angle twisted bilayer graphene and we discuss its implications in relation to the recent observation of correlated and superconducting groundstates near commensurate densities in magic-angle twisted samples, as well as the ``strange metal'' behavior at finite temperatures as a natural outcome of the 2D Luttinger liquid phase.

We adapted a recently proposed framework to characterize the optical response of interacting electrons in solids in order to expedite its computation without compromise in accuracy at the microscopic level. Our formulation is based on reliable parameterizations of Hamiltonians and Coulomb interactions, which allows economy and flexibility in obtaining response functions. It is suited to computing the optical response to fields of arbitrary temporal shape and strength, to arbitrary order in the field, and natively accounts for excitonic effects. We demonstrate the approach by computing the frequency-dependent susceptibilities of MoS2 and hexagonal BN monolayers up to the third-harmonic. Grounded on a generic non-equilibrium many-body perturbation theory, this framework allows extensions to handle generic interaction models or to describe electronic processes taking place at ultrafast time scales., Comment: This update contains the published version. 20 pages, 9 figures

Recent theoretical advances have proposed a new class of topological crystalline insulator (TCI) phases protected by rotational symmetries. Distinct from topological insulators (TIs), rotational symmetry-protected TCIs are expected to show unique topologically protected boundary modes: First, the surface normal to the rotational axis features unpinned Dirac surface states whose Dirac points are located at generic k points. Second, due to the higher-order bulk boundary correspondence, a 3D TCI also supports 1D helical edge states. Despite the unique topological electronic properties, to date, purely rotational symmetry-protected TCIs remain elusive in real materials. Using first-principles band calculations and theoretical modeling, we identify the van der Waals material $\alpha$-Bi4Br4 as a TCI purely protected by rotation symmetry. We show that the Bi4Br4's (010) surface exhibits a pair of unpinned topological Dirac fermions protected by the two-fold rotational axis. These unpinned Dirac fermions show an exotic spin texture highly favorable for spin transport and a band structure consisting of van Hove singularities due to Lifshitz transition. We also identify 1D topological hinge states along the edges of an $\alpha$-Bi4Br4 rod. We further discuss how the proposed topological electronic properties in $\alpha$-Bi4Br4 can be observed by various experimental techniques.

The nature of Fermi surface defines the physical properties of conductors and many physical phenomena can be traced to its shape. Although the recent discovery of a current-dependent nonlinear magnetoresistance in spin-polarized non-magnetic materials has attracted considerable attention in spintronics, correlations between this phenomenon and the underlying fermiology remain unexplored. Here, we report the observation of nonlinear magnetoresistance at room temperature in a semimetal WTe2, with an interesting temperature-driven inversion. Theoretical calculations reproduce the nonlinear transport measurements and allow us to attribute the inversion to temperature-induced changes in Fermi surface convexity. We also report a large anisotropy of nonlinear magnetoresistance in WTe2, due to its low symmetry of Fermi surfaces. The good agreement between experiments and theoretical modeling reveals the critical role of Fermi surface topology and convexity on the nonlinear magneto-response. These results lay a new path to explore ramifications of distinct fermiology for nonlinear transport in condensed-matter.

Starting from the strong-coupling limit of an extended Hubbard model, we develop a spin-fermion theory to study the insulating phase and pairing symmetry of the superconducting phase in twisted bilayer graphene. Assuming that the insulating phase is an anti-ferromagnetic insulator, we show that fluctuations of the anti-ferromagnetic order in the conducting phase can mediate superconducting pairing. Using a self-consistent mean-field analysis, we find that the pairing wave function has a chiral d-wave symmetry. Consistent with this observation, we show explicitly the existence of chiral Majorana edge modes by diagonalizing our proposed Hamiltonian on a finite-sized system. These results establish twisted bilayer graphene as a promising platform to realize topological superconductivity.

The photon-like electronic dispersion of graphene bestows its charge carriers with unusual confinement properties that depend strongly on the geometry and strength of the surrounding potential. Here we report bottom-up synthesis of atomically-precise one-dimensional (1D) arrays of point charges aimed at exploring supercritical confinement of carriers in graphene for new geometries. The arrays were synthesized by arranging F4TCNQ molecules into a 1D lattice on back-gated graphene devices, allowing precise tuning of both the molecular charge state and the array periodicity. Dilute arrays of ionized F4TCNQ molecules are seen to behave like isolated subcritical charges but dense arrays show emergent supercriticality. In contrast to compact supercritical clusters, extended 1D charge arrays exhibit both supercritical and subcritical characteristics and belong to a new physical regime termed frustrated supercritical collapse. Here carriers in the far-field are attracted by a supercritical charge distribution, but have their fall to the center frustrated by subcritical potentials in the near-field, similar to the trapping of light by a dense cluster of stars in general relativity.

In relation to our original paper [M. Droth et al., Phys. Rev. B 94, 075404 (2016)], the Comment by Li et al. [Phys. Rev. B 98, 167403 (2018)] claims to have identified a "mistake in constructing the adiabatic process of the piezoelectricity". More specifically, they write that in our original work "the erroneous usage of the polarization difference formula in Eq. (4) leads to an invalid analytical expression of piezoelectric constant in Eq. (12) of Reference 1". We explain below why these and other minor claims in the Comment are unwarranted, and why we maintain that our result is correct and physically sound., Comment: 4 pages manuscript + 8 pages supplemental material

We introduce a McMillan-Ginzburg-Landau theory to describe the cooperative coexistence of charge-density and superconducting order in two-dimensional crystals. With a free-energy that explicitly accounts for the competition between commensurate and incommensurate ground states, we are able to map the transition between these phases and monitor the development of discommensurations in the near-commensurate regime. Attributing the enhancement of superconducting order to density-wave fluctuations, we propose a coupling scheme that yields a phase diagram in qualitative agreement with experiments in conducting transition metal dichalcogenides. The model predicts the development of non-uniform superconductivity similar to that arising from a pair-density wave, with a spatial texture driven by the underlying charge-density wave fluctuations.

Topological crystalline insulators (TCI) are insulating electronic phases of matter with nontrivial topology originating from crystalline symmetries. Recent theoretical advances have provided powerful guidelines to search for TCIs in real materials. Using density functional theory, we identify a class of new TCI states in the tetragonal lattice of the Ca$_2$As material family. On both top and side surfaces, we observe topological surface states protected independently by rotational and mirror symmetries. We show that a particular lattice distortion can single out the newly proposed topological protection by the rotational symmetry. As a result, the Dirac points of the topological surface states are moved to generic locations in momentum space away from any high symmetry lines. Such topological surface states have not been seen before. Moreover, the other family members, including Ca$_2$Sb, Ca$_2$Bi and Sr$_2$Sb, feature different topological surface states due to their distinct topological invariants. We thus further propose topological phase transitions in the pseudo-binary systems such as (Ca$_{1-x}$Sr$_x$)$_2$As and Ca$_2$As$_x$Sb$_{1-x}$. Our work reveals rich and exotic TCI physics across the Ca$_2$As family of materials, and suggests the feasibility of materials database search methods to discover new TCIs., Comment: 5 pages, 4 figures

The details of the superconducting to quantum metal transition (SQMT) at T=0 are an open problem that invokes much interest in the nature of this exotic and unexpected ground state1-3. However, the SQMT was not yet investigated in a crystalline 2D superconductor with coexisting and fluctuating quantum orders. Here, we report the observation of a SQMT in 2D ion-gel gated 1T-TiSe24, driven by magnetic field. A field-induced crossover between Bose quantum metal and vortex quantum creeping with increasing field is observed. We discuss the interplay between superconducting and CDW fluctuations (discommensurations) and their relation to the anomalous quantum metal (AQM) phase. From our findings, gate-tunable 1T-TiSe2 emerges as a privileged platform to scrutinize, in a controlled way, the details of the SQMT, the role of coexisting fluctuating orders and, ultimately, obtain a deeper understanding of the fate of superconductivity in strictly two-dimensional crystals near zero temperature.

We report the first detailed characterization of the sheet third-harmonic optical susceptibility, $\chi_{s}^{(3)}$, of tungsten diselenide (WSe$_{2}$). With a home-built confocal microscope setup developed to study harmonics generation, we map the second- and third-harmonic intensities as a function of position in the sample, pump power and polarization angle, for single and few layers flakes of WSe$_{2}$. We register a value of $|\chi_{s}^{(3)}| \approx$ 0.91 $\times$ 10$^{-28}$ m$^{3}$ V$^{-2}$ at a fundamental excitation frequency of $\hbar\omega$ = 0.8 eV, which is comparable in magnitude to the third-harmonic susceptibility of other group-VI transition metal dichalcogenides. The simultaneously recorded second-harmonic susceptibility is found to be $|\chi_{s}^{(2)}| \approx$ 0.70 $\times$ 10$^{-19}$ m$^{2}$ V$^{-1}$ in very good agreement on the order of magnitude with recent reports for WSe$_{2}$, which asserts the robustness of our values for $|\chi_{s}^{(3)}|$., Comment: 20 pages, 8 figures, 1 table

We investigate the excitonic spectrum of MoS$_2$ monolayers and calculate its optical absorption properties over a wide range of energies. Our approach takes into account the anomalous screening in two dimensions and the presence of a substrate, both cast by a suitable effective Keldysh potential. We solve the Bethe-Salpeter equation using as a basis a Slater-Koster tight-binding model parameterized to fit ab initio MoS$_2$ band structure calculations. The resulting optical conductivity is in good quantitative agreement with existing measurements up to ultraviolet energies. We establish that the electronic contributions to the C excitons arise not from states in the vicinity of the $\Gamma$ point, but from a set of $k$-points over extended portions of the Brillouin zone. Our results reinforce the advantages of approaches based on effective models to expeditiously explore the properties and tunability of excitons in TMD systems., Comment: Published version, 16 pages, 10 figures

Recent experiments suggest that excitonic degrees of freedom play an important role in precipitating the charge density wave (CDW) transition in $1T$-$\mathrm{TiSe}_2$. Through systematic calculations of the electronic and phonon spectrum based on density functional perturbation theory, we show that the predicted critical doping of the CDW phase overshoots the experimental value by 1 order of magnitude. In contrast, an independent self-consistent many-body calculation of the excitonic order parameter and renormalized band structure is able to capture the experimental phase diagram in extremely good qualitative and quantitative agreement. This demonstrates that electron-electron interactions and the excitonic instability arising from direct electron-hole coupling are pivotal to accurately describe the nature of the CDW in this system. This has important implications to understand the emergence of superconductivity within the CDW phase of this and related systems.

Valley polarization (VP), an induced imbalance in the populations of a multi-valley electronic system, allows emission of second harmonic (SH) light even in centrosymmetric crystals such as graphene. Whereas in systems such as MoS$\mathrm{_2}$ or BN this adds to their intrinsic quadratic response, SH generation in a multi-valley inversion-symmetric crystal can provide a direct measure of valley polarization. By computing the nonlinear response and characterizing theoretically the respective SH as a function of polarization, temperature, electron density, and degree of VP, we demonstrate the possibility of disentangling and individually quantifying the intrinsic and valley contributions to the SH. A specific experimental setup is proposed to obtain direct quantitative information about the degree of VP and allow its remote mapping. This approach could prove useful for direct, contactless, real-space monitoring of valley injection and other applications of valley transport and valleytronics., Comment: Updating with published version, including typesetting corrections to eqs 3 and 4; 7 pages, 5 figures

Charge density wave (CDW) phases are symmetry-reduced states of matter in which a periodic modulation of the electronic charge frequently leads to drastic changes of the electronic spectrum, including the emergence of energy gaps. We analyze the CDW state in a 1T-TiSe$_2$ monolayer within a density functional theory framework and show that, similarly to its bulk counterpart, the monolayer is unstable towards a commensurate $2{\times}2$ periodic lattice distortion (PLD) and CDW at low temperatures. Analysis of the electron and phonon spectrum establishes the PLD as the stable $T=0$ K configuration with a narrow bandgap, whereas the undistorted and semi-metalic state is stable only above a threshold temperature. The lattice distortions as well as the unfolded and reconstructed band structure in the CDW phase agree well with experimental results. We also address evidence in our results for the role of electron-electron interactions in the CDW instability of 1T-TiSe$_2$ monolayers., Comment: 5 pages, 4 figures

The extreme mechanical resilience of graphene and the peculiar coupling it hosts between lattice and electronic degrees of freedom have spawned a strong impetus towards strain-engineered graphene where, on the one hand, strain augments the richness of its phenomenology and makes possible new concepts for electronic devices and, on the other hand, new and extreme physics might take place. Here, we demonstrate that the shape of substrates supporting graphene sheets can be optimized for approachable experiments where strain-induced pseudomagnetic fields (PMF) can be tailored by pressure for directionally selective electronic transmission and pinching-off of current flow down to the quantum channel limit. The Corbino-type layout explored here furthermore allows filtering of charge carriers according to valley and current direction, which can be used to inject or collect valley-polarized currents, thus realizing one of the basic elements required for valleytronics. Our results are based on a framework developed to realistically determine the combination of strain, external parameters, and geometry optimally compatible with the target spatial profile of a desired physical property --- the PMF in this case. Characteristic conductance profiles are analyzed through quantum transport calculations on large graphene devices having the optimal shape., Comment: 5+7 figures. Supporting information included

We introduce the first multiorbital effective tight-binding model to describe the effect of electron-electron interactions in this system. Upon fixing all the effective hopping parameters in the normal state against an ab initio band structure, and with only the overall scale of the interactions as the sole adjustable parameter, we find that a self-consistent Hartree-Fock solution reproduces extremely well the experimental behavior of the charge density wave (CDW) order parameter in the full range $0

Bottom-up fabrication of graphene antidot lattices (GALs) has previously yielded atomically precise structures with sub-nanometer periodicity. Focusing on this type of experimentally realized GAL, we perform density functional theory calculations on the pristine structure as well as GALs with edge carbon atoms substituted with boron or nitrogen. We show that p- and n-type doping levels emerge with activation energies that depend on the level of hydrogenation at the impurity. Furthermore, a tight-binding parameterization together with a Green's function method are used to describe more dilute doping., Comment: 8 pages, 7 figures

DC photoelectrical currents can be generated purely as a non-linear effect in uniform media lacking inversion symmetry without the need for a material junction or bias voltages to drive it, in what is termed photogalvanic effect. These currents are strongly dependent on the polarization state of the radiation, as well as on topological properties of the underlying Fermi surface such as its Berry curvature. In order to study the intrinsic photogalvanic response of gapped graphene (GG), biased bilayer graphene (BBG), and hexagonal boron nitride (hBN), we compute the non-linear current using a perturbative expansion of the density matrix. This allows a microscopic description of the quadratic response to an electromagnetic field in these materials, which we analyze as a function of temperature and electron density. We find that the intrinsic response is robust across these systems and allows for currents in the range of pA cm/W to nA cm/W. At the independent-particle level, the response of hBN-based structures is significant only in the ultra-violet due to their sizeable band-gap. However, when Coulomb interactions are accounted for by explicit solution of the Bethe-Salpeter equation, we find that the photoconductivity is strongly modified by transitions involving exciton levels in the gap region, whose spectral weight dominates in the overall frequency range. Biased bilayers and gapped monolayers of graphene have a strong photoconductivity in the visible and infrared window, allowing for photocurrent densities of several nA cm/W. We further show that the richer electronic dispersion of BBG at low energies and the ability to change its band-gap on demand allows a higher tunability of the photocurrent, including not only its magnitude but also, and significantly, its polarity., Comment: Updating with published version and respective references; 14 pages, 11 figures

The quantum transport properties of a graphene kirigami similar to those studied in recent experiments are calculated in the regime of elastic, reversible deformations. Our results show that, at low electronic densities, the conductance profile of such structures replicates that of a system of coupled quantum dots, characterized by a sequence of minibands and stop-gaps. The conductance and I-V curves have different characteristics in the distinct stages of elastic deformation that characterize the elongation of these structures. Notably, the effective coupling between localized states is strongly reduced in the small elongation stage, whereas in the large elongation regime the development of strong, localized pseudomagnetic field barriers can reinforce the coupling and reestablish resonant tunneling across the kirigami. This provides an interesting example of interplay between geometry and pseudomagnetic field-induced confinement. The alternating miniband and stop-gaps in the transmission lead to I-V characteristics with negative differential conductance in well defined energy/doping ranges. These effects should be stable in a realistic scenario that includes edge roughness and Coulomb interactions, as these are expected to further promote localization of states at low energies in narrow segments of graphene nanostructures., Comment: 10 pages, 10 figures

Due to their low surface mass density, two-dimensional materials with a strong piezoelectric response are interesting for nanoelectromechanical systems with high force sensitivity. Unlike graphene, the two sublattices in a monolayer of hexagonal boron nitride (hBN) are occupied by different elements, which breaks inversion symmetry and allows for piezoelectricity. This has been confirmed with density functional theory calculations of the piezoelectric constant of hBN. Here, we formulate an entirely analytical derivation of the electronic contribution to the piezoelectric response in this system based on the concepts of strain-induced pseudomagnetic vector potential and the modern theory of polarization that relates the polar moment to the Berry curvature. Our findings agree with the symmetry restrictions expected for the hBN lattice and reproduce well the magnitude of the piezoelectric effect previously obtained ab-initio., Comment: 6 pages, 1 figure

We investigate the impact of strained nanobubbles on the conductance characteristics of graphene nanoribbons using a combined molecular dynamics - tight-binding simulation scheme. We describe in detail how the conductance, density of states, and current density of zigzag or armchair graphene nanoribbons are modified by the presence of a nanobubble. In particular, we establish that low-energy electrons can be confined in the vicinity or within the nanobubbles by the delicate interplay between the pseudomagnetic field pattern created by the shape of the bubble, mode mixing, and substrate interaction. The coupling between confined evanescent states and propagating modes can be enhanced under different clamping conditions, which translates into Fano resonances in the conductance traces., Comment: 13 pages, 8 figures

One of the enticing features common to most of the two-dimensional electronic systems that are currently at the forefront of materials science research is the ability to easily introduce a combination of planar deformations and bending in the system. Since the electronic properties are ultimately determined by the details of atomic orbital overlap, such mechanical manipulations translate into modified electronic properties. Here, we present a general-purpose optimization framework for tailoring physical properties of two-dimensional electronic systems by manipulating the state of local strain, allowing a one-step route from their design to experimental implementation. A definite example, chosen for its relevance in light of current experiments in graphene nanostructures, is the optimization of the experimental parameters that generate a prescribed spatial profile of pseudomagnetic fields in graphene. But the method is general enough to accommodate a multitude of possible experimental parameters and conditions whereby deformations can be imparted to the graphene lattice, and complies, by design, with graphene's elastic equilibrium and elastic compatibility constraints. As a result, it efficiently answers the inverse problem of determining the optimal values of a set of external or control parameters that result in a graphene deformation whose associated pseudomagnetic field profile best matches a prescribed target. The ability to address this inverse problem in an expedited way is one key step for practical implementations of the concept of two-dimensional systems with electronic properties strain-engineered to order. The general-purpose nature of this calculation strategy means that it can be easily applied to the optimization of other relevant physical quantities which directly depend on the local strain field, not just in graphene but in other two-dimensional electronic membranes., Comment: 37 pages, 9 figures. This submission contains low-resolution bitmap images; high-resolution images can be found in version 1, which is ~13.5 MB

Analysis of the strain-induced pseudomagnetic fields (PMFs) generated in graphene nanobulges under three different substrate scenarios shows that, in addition to the shape, the graphene-substrate interaction can crucially determine the overall distribution and magnitude of strain and those fields, in and outside the bulge. We utilize a combination of classical molecular dynamics, continuum mechanics, and tight-binding electronic structure calculations as an unbiased means of studying pressure-induced deformations and the resulting PMF in graphene nanobubbles of various geometries. The interplay among substrate aperture geometry, lattice orientation, internal gas pressure, and substrate type is analyzed in view of strain-engineered graphene nanostructures capable of confining and/or guiding electrons at low energies. Except in highly anisotropic geometries, the magnitude of the PMF is generally significant only near the boundaries of the aperture and rapidly decays towards the center because under gas pressure at the scales considered here there is considerable bending at the edges and the central region displays nearly isotropic strain. When the deflection lead to sharp bends at the edges, curvature and the tilting of the $p_z$ orbitals cannot be ignored and contributes substantially to the total field. The strong and localized nature of the PMF at the boundaries and its polarity-changing profile can be exploited to trap electrons inside the bubble or of guiding them in channel-like geometries defined by edges. However, we establish that slippage of graphene against the substrate is an important factor in determining the degree of concentration of PMFs in or around the bulge since it can lead to considerable softening of the strain gradients there. The nature of the substrate emerges thus as a decisive factor determining the effectiveness of nanoscale PMFs tailoring in graphene., Comment: 20 pages, 20 figures including appendices, references updated