Nodal Surface Research Articles

Full Wave Function Optimization with Quantum Monte Carlo-A Study of the Dissociation Energies of ZnO, FeO, FeH, and CrS.

The dissociation energies of four transition-metal dimers are determined using diffusion Monte Carlo. The Jastrow, configuration interaction, and molecular orbital parameters of the wave function are both partially and fully optimized with respect to the variational energy. The pivotal role is thereby ascribable to the optimization of the molecular orbital parameters of a complete active space wave function in the presence of a Jastrow correlation function. Excellent results are obtained for ZnO, FeO, FeH, and CrS. In addition, potential energy curves are computed for the first three compounds at the multireference diffusion Monte Carlo (MR-DMC) level, from which spectroscopic constants such as the equilibrium bond distance, the harmonic frequency, and the anharmonicity are extracted. All of these quantities agree well with the experiment. Furthermore, it is shown for CrS that a restricted active space calculation can yield improved initial orbitals by including single and double excitations from the original active space into a set of virtual orbitals. We demonstrated in this study that the fixed-node error in DMC can be systematically reduced for multireference systems by orbital optimization in compact active spaces. Although DMC calculations with a large number of determinants are possible and very accurate, our results demonstrate that compact wave functions may be sufficient in order to obtain accurate nodal surfaces, which determine the accuracy of DMC, even in the case of transition-metal compounds.

Topological nodal lines in three-dimensional single wall carbon nanotube network

Topological semimetals, including Dirac, Weyl, node-line, triply degenerate semimetal and so on, receive a great deal of attention due to their interesting topological nature and intriguing physical phenomena. In present work, we find that the band crossing topological node-line semimetal states can be realized in a three-dimensional (3,3) single wall carbon nanotube ((3,3) SWCNT) network when spin-orbit coupling (SOC) of C atom is ignored. Detailed symmetry and effective model analysis reveal that time-reversal (T) and space inversion (P) symmetries, as well as mirror symmetries in the system are the origin of the topological node-line in the system. Unexpectedly, the nodal lines are contained in a kind of nodal surface around the Γ originated from accidental band degeneracy. The topological nodal lines and trivial nodal surface in the carbon nanotube network will deepen our understanding of the formation of the nodal line semimetal states.

Topologically nontrivial photonic nodal surface in a photonic metamaterial

The recent development of topological photonics has revealed a variety of intriguing phenomena such as Weyl degeneracy. However, topologically non-trivial degeneracy with higher dimension has not been reported in photonics. In this Letter, topologically charged photonic surface degeneracy in a helix structure possessing two-fold screw symmetry is demonstrated. Calculated Chern number and photonic Fermi arcs support topological phase of the surface degeneracy. We also show that the photonic system can work in both metamaterial and photonic crystal regime, which have an order of magnitude different frequency range by the choice of material for the helix. This work suggests the possibilities of unprecedented photonic topological features with higher dimensions.

Density functional orbitals in quantum Monte Carlo: The importance of accurate densities.

There has been significant recent attention surrounding the accuracy of electronic densities produced by modern parameterized density functional approximations (DFAs). Here, we investigate the impact of using orbitals from density functional calculations in fixed-node Diffusion Monte Carlo (DMC) methods, which is common practice in the calculation of large systems. We find that the accuracy of the density is a strong indicator of the quality of the many-body nodal surface produced by a determinant of the corresponding Kohn-Sham orbitals. Functionals which produce the most accurate electronic densities also produce the lowest variational DMC energies, while functionals that produce poor densities lead to significantly higher energies. This result simplifies the process of choosing orbitals for DMC calculations of large systems and suggests that prioritizing accurate densities in the future development of DFAs would also contribute to the continued improvement of DMC.

Dirac nodal surfaces and nodal lines in ZrSiS.

Topological semimetals are characterized by symmetry-protected band crossings, which can be preserved in different dimensions in momentum space, forming zero-dimensional nodal points, one-dimensional nodal lines, or even two-dimensional nodal surfaces. Materials harboring nodal points and nodal lines have been experimentally verified, whereas experimental evidence of nodal surfaces is still lacking. Here, using angle-resolved photoemission spectroscopy (ARPES), we reveal the coexistence of Dirac nodal surfaces and nodal lines in the bulk electronic structures of ZrSiS. As compared with previous ARPES studies on ZrSiS, we obtained pure bulk states, which enable us to extract unambiguously intrinsic information of the bulk nodal surfaces and nodal lines. Our results show that the nodal lines are the only feature near the Fermi level and constitute the whole Fermi surfaces. We not only prove that the low-energy quasiparticles in ZrSiS are contributed entirely by Dirac fermions but also experimentally realize the nodal surface in topological semimetals.

Composite topological nodal lines penetrating the Brillouin zone in orthorhombic AgF2

It has recently been found that nonsymmorphic symmetries can bring many exotic band crossings. Here, based on symmetry analysis, we predict that materials with time-reversal symmetry in the space group of Pbca (No. 61) possess rich symmetry-enforced band crossings, including nodal surfaces, fourfold degenerate nodal lines and hourglass Dirac loops, which appear in triplets as ensured by the cyclic permutation symmetry. We take Pbca AgF2 as an example in real systems and studied its band structures with ab initio calculations. Specifically, in the absence of spin-orbit coupling (SOC), besides the above-mentioned band degeneracies, this system features a nodal chain and a nodal armillary sphere penetrating the Brillouin zone (BZ). While with SOC, we find a new configuration of the hourglass Dirac loop/chain with the feature traversing the BZ, which originates from the splitting of a Dirac loop confined in the BZ. Furthermore, guided by the bulk-surface correspondence, we calculated the surface states to explore these bulk nodal phenomena. The evolution of these interesting nodal phenomena traversing the BZ under two specific uniaxial strains is also discussed.

High frequency cavity modes of a Helmholtz resonator excited by an air jet

In 1990, Khosropour and Millet reported on a study of the internal spectrum of a Helmholtz resonator excited by an air jet and reported that the data for frequency and amplitude of the Helmholtz mode as a function of jet speed show a series of domains separated by narrow transition regions [JASA 88, 1211–1221 (1990)]. The idea was to observe the behavior of the air jet when the resonator effectively has just a single mode, and does not overblow to higher frequency modes at moderate jet velocities. Further research explored the effects of changes in neck length and jet angle, but higher resonator modes were ignored. This paper presents characterizations of some of the higher modes of cavity vibration, which can be excited at high jet velocities. Unlike the Helmholtz mode, these modes depend on the shape of the cavity shape as well as the volume. Several of these modes were observed, sometimes with more than one mode sounding simultaneously. Guided by finite element simulations, the nature of these higher cavity modes was verified experimentally by observing frequencies and locating nodal surfaces.

Assessing the accuracy of the Jastrow antisymmetrized geminal power in the H4 model system.

We report a quantum Monte Carlo study, on a very simple but nevertheless very instructive model system of four hydrogen atoms, recently proposed in Gasperich et al. [J. Chem. Phys. 147, 074106 (2017)]. We find that the Jastrow correlated Antisymmetrized Geminal Power (JAGP) is able to recover most of the correlation energy even when the geometry is symmetric and the hydrogens lie on the edges of a perfect square. Under such conditions, the diradical character of the molecule ground state prevents a single determinant Ansatz to achieve an acceptable accuracy, whereas the JAGP performs very well for all geometries. Remarkably, this is obtained with a similar computational effort. Moreover, we find that the Jastrow factor is fundamental in promoting the correct resonances among several configurations in the JAGP, which cannot show up in the pure Antisymmetrized Geminal Power (AGP). We also show the extremely fast convergence of this approach in the extension of the basis set. Remarkably, only the simultaneous optimization of the Jastrow and the AGP part of our variational Ansatz is able to recover an almost perfect nodal surface, yielding therefore state of the art energies, almost converged in the complete basis set limit, when the so called diffusion Monte Carlo is applied.

Symmetry-protected nodal phases in non-Hermitian systems

Non-Hermitian (NH) Hamiltonians have become an important asset for the effective description of various physical systems that are subject to dissipation. Motivated by recent experimental progress on realizing the NH counterparts of gapless phases such as Weyl semimetals, here we investigate how NH symmetries affect the occurrence of exceptional points (EPs), that generalize the notion of nodal points in the spectrum beyond the Hermitian realm. Remarkably, we find that the dimension of the manifold of EPs is generically increased by one as compared to the case without symmetry. This leads to nodal surfaces formed by EPs that are stable as long as a protecting symmetry is preserved, and that are connected by open Fermi volumes. We illustrate our findings with analytically solvable two-band lattice models in one and two spatial dimensions, and show how they are readily generalized to generic NH crystalline systems.

Clean and Convenient Tessellations for Number Counting Jastrow Factors.

We introduce a basis of counting functions that, by cleanly tessellating three-dimensional space, allows real space number counting Jastrow factors to be straightforwardly applied to general molecular situations. By exerting direct control over electron populations in local regions of space and encoding pairwise correlations between these populations, these Jastrow factors allow even very simple reference wave functions to adopt nodal surfaces well suited to many strongly correlated settings. Being trivially compatible with traditional Jastrow factors and diffusion Monte Carlo and having the same cubic per-sample cost scaling as a single determinant trial function, these Jastrow factors thus offer a powerful new route to the simultaneous capture of weak and strong electron correlation effects in a wide variety of molecular and materials settings. In multiple strongly correlated molecular examples, we show that even when paired with the simplest possible single determinant reference, these Jastrow factors allow quantum Monte Carlo to out-perform coupled cluster theory and approach the accuracy of traditional multireference methods.

Progress on topological nodal line and nodal surface

Electronic band crossing can not only form zero-dimensional nodal points, but also one dimensional nodal lines and two dimensional nodal surfaces. These topological band features have been attracting significant research interest, as they may lead to many special physical properties. In this article, we review the progress in this field, including the conceptual development, the character and classification of these nodal structures, and the material realization.

Influence of pseudopotentials on excitation energies from selected configuration interaction and diffusion Monte Carlo

Due to their diverse nature, the faithful description of excited states within electronic structure theory methods remains one of the grand challenges of modern theoretical chemistry. Quantum Monte Carlo (QMC) methods have been applied very successfully to ground state properties but still remain generally less effective than other non-stochastic methods for electronically excited states. Nonetheless, we have recently reported accurate excitation energies for small organic molecules at the fixed-node diffusion Monte Carlo (FN-DMC) within a Jastrow-free QMC protocol relying on a deterministic and systematic construction of nodal surfaces using the selected configuration interaction (sCI) algorithm known as CIPSI (Configuration Interaction using a Perturbative Selection made Iteratively). Albeit highly accurate, these all-electron calculations are computationally expensive due to the presence of core electrons. One very popular approach to remove these chemically-inert electrons from the QMC simulation is to introduce pseudopotentials (also known as effective core potentials). Taking the water molecule as an example, we investigate the influence of Burkatzki-Filippi-Dolg (BFD) pseudopotentials and their associated basis sets on vertical excitation energies obtained with sCI and FN-DMC methods. Although these pseudopotentials are known to be relatively safe for ground state properties, we evidence that special care may be required if one strives for highly accurate vertical transition energies. Indeed, comparing all-electron and valence-only calculations, we show that using pseudopotentials with the associated basis sets can induce differences of the order of 0.05 eV on the excitation energies. Fortunately, a reasonable estimate of this shift can be estimated at the sCI level.

Coulomb-induced instabilities of nodal surfaces

We consider the stability of nodal surfaces in fermionic band systems with respect to the Coulomb repulsion. It is shown that nodal surfaces at the Fermi level are gapped out at low temperatures due to emergent particle-hole orders. Energy dispersion of the nodal surface suppresses the instability through an inhomogenous phase. We argue that around criticality the order parameter fluctuations can induce superconductivity. We show that by tuning doping and disorder one could access various phases, establishing fermionic nodal surface systems as a versatile platform to study emergent quantum orders.

Mirror protected multiple nodal line semimetals and material realization

The conventional k.p method fails to capture the full and essential physics of many symmetry enriched multiple nodal line structures in the three dimensional Brillouin zone. Here we present a new and systematical method to construct the effective lattice model of mirror symmetry protected three-dimensional multiple nodal line semimetals, when the spin-orbit interaction is ignored. For systems with a given pair of perpendicular nodal rings, we obtain all the effective lattice models and eleven inequivalent nodal line Fermi surfaces together with their related constraints. By means of first-principles calculations, we first propose a family of real materials, beta phase of ternary nitrides X2GeN2 (X = Ca; Sr; Ba), that support one kind of these novel Fermi surfaces. Therefore, our work deepens the understanding of the nodal line structures and promotes the experimental progress of topological nodal line semimetals.

Excitation energies from diffusion Monte Carlo using selected configuration interaction nodes.

Quantum Monte Carlo (QMC) is a stochastic method that has been particularly successful for ground-state electronic structure calculations but mostly unexplored for the computation of excited-state energies. Here, we show that within a Jastrow-free QMC protocol relying on a deterministic and systematic construction of nodal surfaces using selected configuration interaction (sCI) expansions, one is able to obtain accurate excitation energies at the fixed-node diffusion Monte Carlo (FN-DMC) level. This evidences that the fixed-node errors in the ground and excited states obtained with sCI wave functions cancel out to a large extent. Our procedure is tested on two small organic molecules (water and formaldehyde) for which we report all-electron FN-DMC calculations. For both the singlet and triplet manifolds, accurate vertical excitation energies are obtained with relatively compact multideterminant expansions built with small (typically double-ζ) basis sets.

On K3 double planes covering Enriques surfaces

The moduli space of nodal Enriques surfaces is irreducible of dimension 9. A nodal Enriques surface is shown to be the quotient of a double cover of the plane by a lift of the Cremona involution. We also show that this gives a straightforward proof of the known description of the automorphism group for the generic such surface.

On the challenge to improve the density response with unusual gradient approximations

Certain excitations, especially ones of long-range charge transfer character, are poorly described by time-dependent density functional theory (TDDFT) when typical (semi-)local functionals are used. A proper description of these excitations would require an exchange-correlation response differing substantially from the usual (semi-)local one. It has recently been shown that functionals of the generalized gradient approximation (GGA) type can yield unusual potentials, mimicking features of the exact exchange derivative discontinuity and showing divergences on orbital nodal surfaces. We here investigate whether these unusual potential properties translate into beneficial response properties. Using the Sternheimer formalism we closely investigate the response obtained with the 2013 exchange approximation by Armiento and K\"ummel (AK13) and the 1988 exchange approximation by Becke (B88), both of which show divergences on orbital nodal planes. Numerical calculations for Na2 as well as analytical and numerical calculations for the hydrogen atom show that the response of AK13 behaves qualitatively different from usual semi local functionals. However, the AK13 functional leads to fundamental instabilities in the asymptotic region that prevent its practical application in TDDFT. Our findings may help the development of future improved functionals, and corroborate that the frequency-dependent Sternheimer formalism is excellently suited for running and analyzing TDDFT calculations.

Nodal loop and nodal surface states in the Ti3Al family of materials

Topological metals and semimetals are new states of matter which attract great interest in current research. Here, based on first-principles calculations and symmetry analysis, we propose that the family of titanium-based compounds Ti3X (X=Al, Ga, Sn, Pb) are unexplored topological semimetals. These materials feature the coexistence of a nodal loop and a nodal surface in their low-energy band structure. Taking Ti3Al as an example, we show that the material has an almost ideal nodal loop in the sense that the loop is close to the Fermi level and it is nearly flat in energy with energy variation <0.25 meV. The loop is protected by either one of the two independent symmetries: the combined spacetime inversion symmetry and the mirror reflection symmetry. The nodal surface at the k_z=\pi plane is guaranteed by the nonsymmorphic screw rotational symmetry and the time reversal symmetry. We discuss the effect of spin-orbit coupling and construct an effective model for describing the nodal loop. Our findings indicate that the Ti3Al family compounds can serve as an excellent material platform for studying new topological phases and particularly the interplay between nodal-loop and nodal-surface fermions.

What can Andreev bound states tell us about superconductors?

Zero-energy Andreev bound states, which manifest themselves in the tunnelling spectra as zero-bias conductance peaks (ZBCPs), are abundant at interfaces between superconductors and other materials and on the nodal surface of high-temperature superconductors. In this review, we focus on the information such excitations can provide on the properties of superconductor systems. First, a general introduction to the physics of Andreev bound states in superconductor/normal metal interfaces is given with a particular emphasis on why they appear at zero energy in d-wave superconductors. Then, specific spectroscopic tunnelling studies of thin films, bilayers and junctions are described, focusing on the corresponding ZBCP features. Scanning tunnelling spectroscopy (STS) studies show that the ZBCPs on the c-axis YBa2Cu3O7-δ (YBCO) films are correlated with the surface morphology and appear only in proximity to (110) facets. STS on c-axis La1.88Sr0.12CuO4 (LSCO) films exhibiting the 1/8 anomaly shows spatially modulated peaks near zero bias associated with the anti-phase ordering of the d-wave order parameter predicted at this doping level. ZBCPs were also found in micrometre-size edge junctions of YBCO/SrRuO3/YBCO, where SrRuO3 is ferromagnetic. Here, the results are consistent with a crossed Andreev reflection effect (CARE) at the narrow domain walls of the SrRuO3 ZBCPs measured in STS studies of manganite/cuprate bilayers could not be attributed to CARE because the manganite's domain wall is much larger than the coherence length in YBCO, and instead are attributed to proximity-induced triplet-pairing superconductivity with non-conventional symmetry. And finally, ZBCPs found in junctions of non-intentionally doped topological insulator films of Bi2Se3 and the s-wave superconductor NbN are attributed to proximity-induced px + ipy triplet order parameter in the topological material.This article is part of the theme issue 'Andreev bound states'.

Coincidence Structures and Hard-Core Few-Body Interactions

The symmetry and topology of the coincidence structure, i.e. the locus of points in configuration space corresponding to particles in the same position, plays a critical role in extracting universal properties for few-body models with hard-core interactions. The coincidence structure is a scale-invariant union of manifolds possessing rich symmetry. When there are zero-range hard-core two-body interactions, the coincidence structure forms a nodal surface for finite-energy wave functions in configuration space. More generally, it acts like a defect that changes the topology of configuration space in a way that depends on the dimension of the underlying space, the total number of particles, and the number of particles in the hard-core interaction. We show that for the specific case of three-body hard-core interactions in one-dimension, the configuration space is no longer simply-connected, providing a topological explanation for several models that exhibit anyonic behavior.