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We report evidence for superconductivity with onset temperatures up to 11 K in thin films of the infinite-layer nickelate parent compound NdNiO$_2$. A combination of oxide molecular-beam epitaxy and atomic hydrogen reduction yields samples with high crystallinity and low residual resistivities, a substantial fraction of which exhibit superconducting transitions. We survey a large series of samples with a variety of techniques, including electrical transport, scanning transmission electron microscopy, x-ray absorption spectroscopy, and resonant inelastic x-ray scattering, to investigate the possible origins of superconductivity. We propose that superconductivity could be intrinsic to the undoped infinite-layer nickelates but suppressed by disorder due to its nodal order parameter, a finding which would necessitate a reconsideration of the nickelate phase diagram. Another possible hypothesis is that the parent materials can be hole doped from randomly dispersed apical oxygen atoms, which would suggest an alternative pathway for achieving superconductivity., Comment: Main: 10 pages, 6 figures. Supplementary: 9 pages, 10 figures

Biased bilayer graphene (BBG) is an important system for studies of excitonic effects in graphene--based systems, with its easily tunable bandgap. This bandgap is governed by an external gate voltage, allowing one to tune the optical response of the system. In this paper, we study the excitonic linear and nonlinear optical response of Bernal stacked BBG as a function of the gate voltage, both for in--plane (IP) and out--of--plane (OOP) directions. Based on a semi-analytical model of the electronic structure of BBG describing the influence of gate voltage on excitonic binding energies, we focus our discussion on both the IP and OOP excitonic response. Both linear and second harmonic generation (SHG) nonlinear responses are shown to be very sensitive to the gate voltage, as both the interband momentum matrix elements and the bandgap of the system will vary greatly with bias potential., Comment: 18 pages, 8 figures

Efforts are underway to magnetically confine electron--positron pair plasmas to study their unique behavior, which is characterized by significant changes in plasma time and length scales, supported waves, and unstable modes. However, use of conventional plasma diagnostics presents challenges with these low-density and annihilating matter-antimatter plasma. To address this problem, we propose to develop techniques based on the distinct emission provided by annihilation. This emission exhibits two spatial correlations: the distance attenuation of isotropic sources and the back-to-back propagation of momentum-preserving 2-$\gamma$ annihilation. We present the results of our analysis of the $\gamma$ emission rate and the spatial profile of the annihilation in a magnetized pair plasma from direct pair collisions, from the formation and decay of positronium, as well as from transport processes. In order to demonstrate the effectiveness of annihilation-based techniques, we tested them on annular $\gamma$ emission profiles produced by a $\beta^+$ radioisotope on a rotating turntable. Direct and positronium-mediated annihilation result in overlapping volumetric $\gamma$ sources, and the 2-$\gamma$ emission from these volumetric sources can be tomographically reconstructed from coincident counts in multiple detectors. Transport processes result in localized annihilation where field lines intersect walls, limiters, or internal magnets. These localized sources can be identified by the fractional $\gamma$ counts on spatially distributed detectors., Comment: 21 pages, 11 figures, 2 tables, contribution to the 13th International Workshop on Non-Neutral Plasmas

FeSe$_{1-x}$S$_x$ remains one of the most enigmatic systems of Fe-based superconductors. While much is known about the orthorhombic parent compound, FeSe, the tetragonal samples, FeSe$_{1-x}$S$_x$ with x>0.17, remain relatively unexplored. Here, we provide an in-depth investigation of the electronic states of tetragonal FeSe$_{0.81}$S$_{0.19}$, using scanning tunneling microscopy and spectroscopy (STM/S) measurements, supported by angle-resolved photoemission spectroscopy (ARPES) and theoretical modeling. We demonstrate that by analyzing modulations of the local density of states (LDOS) near and away from Fe vacancy defects separately, we can identify quasiparticle interference (QPI) signals originating from multiple regions of the Brillouin zone, including the bands at the M and A points. We also observe that QPI signals coexist with a much stronger LDOS modulation for states near the Fermi level whose period is independent of energy. Our measurements further reveal that this strong pattern appears in the STS measurements as short range stripe patterns that are locally two-fold symmetric. Since these stripe patterns coexist with four-fold symmetric QPI around Fe-vacancies, the origin of their local two-fold symmetry must be distinct from that of nematic states in orthorhombic samples. To further understand these stripe patterns, we explore several aspects related to them, such as the role of S and Fe vacancy defects, and whether they can be explained by QPI. We consider the possibility that the observed stripe patterns may represent incipient charge order correlations, similar to those observed in the cuprates.

The optical properties of two-dimensional materials are exceptional in several respects. They are highly anisotropic and frequently dominated by excitonic effects. Dipole-allowed second order non-linear optical properties require broken inversion symmetry. Hence, several two-dimensional materials show strong in-plane (IP) non-linearity but negligible out-of-plane (OOP) response due to vertical symmetry. By considering buckled hexagonal monolayers, we analyze the critical role of broken vertical symmetry on their excitonic optical response. Both linear as well as second order shift current and second harmonic response are studied. We demonstrate that substantial OOP non-linear response can be obtained, in particular, through off-diagonal tensor elements coupling IP excitation to OOP response. Our findings are explained by excitonic selection rules for OOP response and the impact of dielectric screening on excitons is elucidated., Comment: 20 pages, 8 figures

The creation of an electron space charge in a dipole magnetic trap and the subsequent injection of positrons has been experimentally demonstrated. Positrons (5eV) were magnetically guided from their source and injected into the trapping field generated by a permanent magnet (0.6T at the poles) using a cross field E $\times$ B drift, requiring tailored electrostatic and magnetic fields. The electron cloud is created by thermionic emission from a tungsten filament. The maximum space charge potential of the electron cloud reaches -42V, which is consistent with an average electron density of ($4 \pm 2$) $\times 10^{12}$ $\text{m}^{-3}$ and a Debye length of ($2 \pm 1$) $\text{cm}$. We demonstrate that the presence of this space potential does not hamper efficient positron injection. Understanding the effects of the negative space charge on the injection and confinement of positrons represents an important intermediate step towards the production of a confined electron-positron pair plasma.

The C2DB is a highly curated open database organizing a wealth of computed properties for more than 4000 atomically thin two-dimensional (2D) materials. Here we report on new materials and properties that were added to the database since its first release in 2018. The set of new materials comprise several hundred monolayers exfoliated from experimentally known layered bulk materials, (homo)bilayers in various stacking configurations, native point defects in semiconducting monolayers, and chalcogen/halogen Janus monolayers. The new properties include exfoliation energies, Bader charges, spontaneous polarisations, Born charges, infrared polarisabilities, piezoelectric tensors, band topology invariants, exchange couplings, Raman- and second harmonic generation spectra. We also describe refinements of the employed material classification schemes, upgrades of the computational methodologies used for property evaluations, as well as significant enhancements of the data documentation and provenance. Finally, we explore the performance of Gaussian process-based regression for efficient prediction of mechanical and electronic materials properties. The combination of open access, detailed documentation, and extremely rich materials property data sets make the C2DB a unique resource that will advance the science of atomically thin materials., Comment: 30 pages, 26 figures

We present a method for producing high quality KCo2As2 crystals, stable in air and suitable for a variety of measurements. X-ray diffraction, magnetic susceptibility, electrical transport and heat capacity measurements confirm the high quality and an absence of long range magnetic order down to at least 2 K. Residual resistivity values approaching 0.25 $\mu\Omega$~cm are representative of the high quality and low impurity content, and a Sommerfeld coefficient $\gamma$ = 7.3 mJ/mol K$^2$ signifies weaker correlations than the Fe-based counterparts. Together with Hall effect measurements, angle-resolved photoemission experiments reveal a Fermi surface consisting of electron pockets at the center and corner of the Brillouin zone, in line with theoretical predictions and in contrast to the mixed carrier types of other pnictides with the ThCr2Si2 structure. A large, linear magnetoresistance of 200\% at 14~T, together with an observed linear and hyperbolic, rather than parabolic, band dispersions are unusual characteristics of this metallic compound and may indicate more complex underlying behavior., Comment: 9 pages, 4 figures

High-temperature superconducting cuprates exhibit an intriguing phenomenology for the low-energy elementary excitations. In particular, an unconventional temperature dependence of the coherent spectral weight (CSW) has been observed in the superconducting phase by angle-resolved photoemission spectroscopy (ARPES), both at the antinode where the d-wave paring gap is maximum, as well as along the gapless nodal direction. Here, we combine equilibrium and time-resolved ARPES to track the temperature dependent meltdown of the nodal CSW in Bi-based cuprates with unprecedented sensitivity. We find the nodal suppression of CSW upon increasing temperature to be ubiquitous across single- and double-layer Bi cuprates, and uncorrelated to superconducting and pseudogap onset temperatures. We quantitatively model both the lineshape of the nodal spectral features and the anomalous suppression of CSW within the Fermi-Liquid framework, establishing the key role played by the normal state electrodynamics in the description of nodal quasiparticles in superconducting cuprates., Comment: 6 pages, 3 figures; Supplementary Materials available upon request

The technical and economic feasibility to deliver sustainable liquid biocrude through hydrothermal liquefaction (HTL) while enabling negative carbon dioxide emissions is evaluated in this paper, looking into the potential of the process in the context of negative emission technologies (NETs) for climate change mitigation. In the HTL process, a gas phase consisting mainly of carbon dioxide is obtained as a side product driving a potential for the implementation of carbon capture and storage in the process (BECCS) that has not been explored yet in the existing literature and is undertaken in this study. To this end, the process is divided in a standard HTL base and a carbon capture add-on, having forestry residues as feedstock. The Selexol technology is adapted in a novel scheme to simultaneously separate the CO2 from the HTL gas and recover the excess hydrogen for biocrude upgrading. The cost evaluation indicates that the additional cost of the carbon capture can be compensated by revenues from the excess process heat and the European carbon allowance market. The impact in the MFSP of the HTL base case ranges from -7% to 3%, with -15% in the most favorable scenario, with a GHG emissions reduction potential of 102-113% compared to the fossil baseline. These results show that the implementation of CCS in the HTL process is a promising alternative from technical, economic and environmental perspective in future scenarios in which advanced liquid biofuels and NETs are expected to play a role in the decarbonization of the energy system.

Raman spectroscopy is frequently used to identify composition, structure and layer thickness of 2D materials. Here, we describe an efficient first-principles workflow for calculating resonant first-order Raman spectra of solids within third-order perturbation theory employing a localized atomic orbital basis set. The method is used to obtain the Raman spectra of 733 different monolayers selected from the computational 2D materials database (C2DB). We benchmark the computational scheme against available experimental data for 15 known monolayers. Furthermore, we propose an automatic procedure for identifying a material based on an input experimental Raman spectrum and illustrate it for the cases of MoS$_2$ (H-phase) and WTe$_2$ (T$^\prime$-phase). The Raman spectra of all materials at different excitation frequencies and polarization configurations are freely available from the C2DB. Our comprehensive and easily accessible library of \textit{ab initio} Raman spectra should be valuable for both theoreticians and experimentalists in the field of 2D materials, Comment: 17 pages, 7 figures

The magneto-optical response of monolayer transition metal dichalcogenides (TMDs), including excitonic effects, is studied using a nanoribbon geometry. We compute the diagonal optical conductivity and the Hall conductivity. Comparing the excitonic optical Hall conductivity to results obtained in the independent particle approximation, we find an increase in the amplitude corresponding to one order of magnitude when excitonic effects are included. The Hall conductivities are used to calculate Faraday rotation spectra for MoS2 and WSe2. Finally, we have also calculated the diamagnetic shift of the exciton states of WSe2 in different dielectric environments. Comparing the calculated diamagnetic shift to recent experimental measurements, we find a very good agreement between the two.

We propose an analytical approach for calculating the linear and nonlinear optical (NLO) responses of monolayer transition metal dichalcogenides (TMDs) including excitonic effects. An effective Hamiltonian reproducing the trigonal warping (TW) of the energy dispersion, is used to derive analytical expressions for excitonic matrix elements. Based on this approach, we provide an informative diagram, which encompasses all excitonic selection rules. The diagram enables us to identify main transitions for the first-, second- and third-order optical responses. As a case study, we calculate the optical conductivity and second/third harmonic generation responses of monolayer MoS2 and demonstrate that the analytical approach accurately reproduces the spectra obtained using the Bethe-Salpeter equation (BSE). Therefore, the analytical approach provides an efficient and reliable method for calculating the NLO spectra as accurate as the full BSE method. Moreover, it enables us to obtain valuable physical insight into the fundamental transitions responsible for individual resonances, which is not straightforward in the full BSE method., Comment: 12 pages, 6 figures, 1 table, 3 appendices

Two-dimensional materials constitute an exciting platform for nonlinear optics with large nonlinearities that are tunable by gating. Hence, gate-tunable harmonic generation and intensity-dependent refraction have been observed in e.g. graphene and transition-metal dichalcogenides, whose electronic structures are accurately modelled by the (massive) Dirac equation. We exploit on the simplicity of this model and demonstrate here that arbitrary nonlinear response functions follow from a simple iterative approach. The power of this approach is illustrated by analytical expressions for harmonic generation and intensity-dependent refraction, both computed up to ninth order in the pump field. Moreover, the results allow for arbitrary band gaps and gating potentials. As illustrative applications, we consider (i) gate-dependence of third- and fifth-harmonic generation in gapped and gapless graphene, (ii) intensity-dependent refractive index of graphene up to ninth order, and (iii) intensity-dependence of high-harmonic generation., Comment: 6 pages, 5 figures. Supplemental material: 6 pages, 2 figures

We propose and analyze a mechanism for inducing spin Hall currents in ordinary (1H phase) monolayer transition metal dichalcogenides (TMDs) due to the nonlinear process of optical rectification. The photo-induced spin current is proportional to the light intensity, and originates from the intrinsic spin-orbit coupling in TMDs. The spin current spectrum is strongly influenced by electron-hole interactions, i.e. excitonic effects, analogous to the optical absorption. Remarkably, excitons change the temperature dependence of the induced spin current, to the point that the current direction can even be reversed by varying the temperature. This peculiar excitonic behavior is shown to emerge from the relative strength of two distinct mechanisms contributing to the optical response, i.e. a purely interband part and a mixed inter/intraband contribution. Furthermore, we investigate the valley dichrosim of second-harmonic charge and spin currents, and demonstrate different valley polarization of $s$ and $p$ excitons that stem from their distinct angular momenta. Our findings pave the path to the generation of dc spin currents in ordinary TMDs without external static electric or magnetic fields., Comment: Main text: 6 pages, 3 figures; Supplementary: 13 pages, 4 figures, 1 table

Using an equation of motion (EOM) approach, we calculate excitonic properties of monolayer transition metal dichalcogenides (TMDs) perturbed by an external magnetic field. We compare our findings to the widely used Wannier model for excitons in two-dimensional materials and to recent experimental results. We find good agreement between the calculated excitonic transition energies and the experimental results. In addition, we find that the exciton energies calculated using the EOM approach are slightly lower than the ones calculated using the Wannier model. Finally, we also show that the effect of the dielectric environment on the magnetoexciton transition energy is minimal due to counteracting changes in the exciton energy and the exchange self-energy correction., Comment: 14 pages, 7 figures

We study the equivalence of four different approaches to calculate the excitonic linear and nonlinear optical response of multiband semiconductors. These four methods derive from two choices of gauge, i.e. length and velocity gauges, and two ways of computing the current density, i.e. direct evaluation and evaluation via the time-derivative of the polarization density. The linear and quadratic response functions are obtained for all methods by employing a perturbative density matrix approach within the mean-field approximation. The equivalence of all four methods is shown rigorously, when a correct interaction Hamiltonian is employed for the velocity gauge approaches. The correct interaction is written as a series of commutators containing the unperturbed Hamiltonian and position operators, which becomes equivalent to the conventional velocity gauge interaction in the limit of infinite Coulomb screening and infinitely many bands. As a case study, the theory is applied to hexagonal boron nitride monolayers, and the linear and nonlinear optical response found in different approaches are compared., Comment: 11 pages, 3 figures

We compute the nonlinear optical response of doped mono- and bilayer graphene using the full dispersion based on tight-binding models. The response is derived with the density matrix formalism using the length gauge and is valid for any periodic system, with arbitrary doping. By collecting terms that define effective nonlinear response tensors, we identify all nonlinear Drude-like terms (up to third-order) and show that all additional spurious divergences present in the induced current vanish. The nonlinear response of graphene comprises a large Drude-like divergence and three resonances that are tightly connected with transitions occurring in the vicinity of the Fermi level. The analytic solution derived using the Dirac approximation captures accurately the first- and third-order responses in graphene, even at very high doping levels. The quadratic response of gapped graphene is also strongly enhanced by doping, even for systems with small gaps such as commensurate structures of graphene on SiC. The nonlinear response of bilayer graphene is significantly richer, combining the resonances that stem from doping with its intrinsic strong low-energy resonances., Comment: Revised manuscript 18 pages, 6 figures

We study the effects of a truncated band structure on the linear and nonlinear optical response of crystals using four methods. These are constructed by (i) choosing either length or velocity gauge for the perturbation and (ii) computing the current density either directly or via the time-derivative of the polarization density. In the infinite band limit, the results of all four methods are identical, but basis truncation breaks their equivalence. In particular, certain response functions vanish identically and unphysical low-frequency divergences are observed for few-band models in the velocity gauge. Using hexagonal boron nitride (hBN) monolayer as a case study, we analyze the problems associated with all methods and identify the optimal one. Our results show that the length gauge calculations provide the fastest convergence rates as well as the most accurate spectra for any basis size and, moreover, that low-frequency divergences are eliminated., Comment: 11 pages, 7 figures

We present a calculation of Third Harmonic Generation (THG) for two-band systems using the length gauge that avoids unphysical divergences otherwise present in the evaluation of the third order current density response. The calculation is applied to bulk and monolayer black Phosphorus (bP) using a non-orthogonal tight-binding model. Results show that the low energy response is dominated by mixed inter-intraband processes and estimates of the magnitude of THG susceptibility are comparable to recent experimental reports for bulk bP samples., Comment: 9 pages, 5 figures

Using the narrowband all-sky imager mode of the LWA1 we have now detected 30 transients at 25.6 MHz, 1 at 34 MHz, and 93 at 38.0 MHz. While we have only optically confirmed that 37 of these events are radio afterglows from meteors, evidence suggests that most, if not all, are. Using the beam-forming mode of the LWA1 we have also captured the broadband spectra between 22.0 and 55.0 MHz of four events. We compare the smooth, spectral components of these four events and fit the frequency dependent flux density to a power law, and find that the spectral index is time variable, with the spectrum steepening over time for each meteor afterglow. Using these spectral indices along with the narrow band flux density measurements of the 123 events at 25.6 and 38 MHz, we predict the expected flux densities and rates for meteor afterglows potentially observable by other low frequency radio telescopes., Comment: 28 Pages and 7 Figures

Sources of error fields were indirectly inferred in a stellarator by reconciling computed and numerical flux surfaces. Sources considered so far include the displacements and tilts (but not the deformations, yet) of the four circular coils featured in the simple CNT stellarator. The flux surfaces were measured by means of an electron beam and phosphor rod, and were computed by means of a Biot-Savart field-line tracing code. If the ideal coil locations and orientations are used in the computation, agreement with measurements is poor. Discrepancies are ascribed to errors in the positioning and orientation of the in-vessel interlocked coils. To that end, an iterative numerical method was developed. A Newton-Raphson algorithm searches for the coils' displacements and tilts that minimize the discrepancy between the measured and computed flux surfaces. This method was verified by misplacing and tilting the coils in a numerical model of CNT, calculating the flux surfaces that they generated, and testing the algorithm's ability to deduce the coils' displacements and tilts. Subsequently, the numerical method was applied to the experimental data, arriving at a set of coil displacements whose resulting field errors exhibited significantly improved quantitative and qualitative agreement with experimental results., Comment: Special Issue on the 20th International Stellarator-Heliotron Workshop

We calculate the spin transport of hydrogenated graphene using the Landauer-B\"uttiker formalism with a spin-dependent tight-binding Hamiltonian. The advantages of using this method is that it simultaneously gives information on sheet resistance and localization length as well as spin relaxation length. Furthermore, the Landauer-B\"uttiker formula can be computed very efficiently using the recursive Green's function technique. Previous theoretical results on spin relaxation time in hydrogenated graphene have not been in agreement with experiments. Here, we study magnetic defects in graphene with randomly aligned magnetic moments, where interference between spin-channels is explicitly included. We show that the spin relaxation length and sheet resistance scale nearly linearly with the impurity concentration. Moreover, the spin relaxation mechanism in hydrogenated graphene is Markovian only near the charge neutrality point or in the highly dilute impurity limit.

In order to use graphene for semiconductor applications, such as transistors with high on/off ratios, a band gap must be introduced into this otherwise semimetallic material. A promising method of achieving a band gap is by introducing nanoscale perforations (antidots) in a periodic pattern, known as a graphene antidot lattice (GAL). A graphene antidot barrier (GAB) can be made by introducing a 1D GAL strip in an otherwise pristine sheet of graphene. In this paper, we will use the Dirac equation (DE) with a spatially varying mass term to calculate the electronic transport through such structures. Our approach is much more general than previous attempts to use the Dirac equation to calculate scattering of Dirac electrons on antidots. The advantage of using the DE is that the computational time is scale invariant and our method may therefore be used to calculate properties of arbitrarily large structures. We show that the results of our Dirac model are in quantitative agreement with tight-binding for hexagonal antidots with armchair edges. Furthermore, for a wide range of structures, we verify that a relatively narrow GAB, with only a few antidots in the unit cell, is sufficient to give rise to a transport gap.

The Stark effect in hydrogen and the cubic anharmonic oscillator furnish examples of quantum systems where the perturbation results in a certain ionization probability by tunneling processes. Accordingly, the perturbed ground-state energy is shifted and broadened, thus acquiring an imaginary part which is considered to be a paradigm of nonperturbative behavior. Here we demonstrate how the low order coefficients of a divergent perturbation series can be used to obtain excellent approximations to both real and imaginary parts of the perturbed ground state eigenenergy. The key is to use analytic continuation functions with a built in analytic structure within the complex plane of the coupling constant, which is tailored by means of Bender-Wu dispersion relations. In the examples discussed the analytic continuation functions are Gauss hypergeometric functions, which take as input fourth order perturbation theory and return excellent approximations to the complex perturbed eigenvalue. These functions are Borel-consistent and dramatically outperform widely used Pad\'e and Borel-Pad\'e approaches, even for rather large values of the coupling constant., Comment: 5 pages, 3 figures, PDFLaTeX

The electronic properties of graphene may be changed from semimetallic to semiconducting by introducing perforations (antidots) in a periodic pattern. The properties of such graphene antidot lattices (GALs) have previously been studied using atomistic models, which are very time consuming for large structures. We present a continuum model that uses the Dirac equation (DE) to describe the electronic and optical properties of GALs. The advantages of the Dirac model are that the calculation time does not depend on the size of the structures and that the results are scalable. In addition, an approximation of the band gap using the DE is presented. The Dirac model is compared with nearest-neighbour tight-binding (TB) in order to assess its accuracy. Extended zigzag regions give rise to localized edge states, whereas armchair edges do not. We find that the Dirac model is in quantitative agreement with TB for GALs without edge states, but deviates for antidots with large zigzag regions., Comment: 15 pages, 7 figures. Accepted by Journal of Physics: Condensed matter

We compute the dynamical polarization function for a graphene antidot lattice in the random-phase approximation. The computed polarization functions display a much more complicated structure than what is found for pristine graphene (even when evaluated beyond the Dirac-cone approximation); this reflects the miniband structure and the associated van Hove singularities of the antidot lattice. The polarization functions depend on the azimuthal angle of the {\bf q}-vector. We develop approximations to ease the numerical work, and critically evaluate the performance of the various schemes. We also compute the plasmon dispersion law, and find an approximate square-root dependence with a suppressed plasmon frequency as compared to doped graphene. The plasmon dispersion is nearly isotropic, and the developed approximation schemes agree well with the full calculation.