High-symmetry Directions Research Articles

Angle-resolved photoemission spectroscopy of electronic structure of 1<i>T</i>-NbSeTe

Transition metal dichalcogenides (TMDs) have attracted a lot of interest in condensed matter physics research due to the existence of multiple novel physical phenomena, including superconductivity and charge density wave order, and also TMDs provide a unique window for studying the interactions between different ground states. In this work, the electronic structure of 1<i>T</i>-NbSeTe is systematically examined by angle-resolved photoemission spectroscopy (ARPES) for the first time. A van Hove singularity (VHS) is identified at the <i>M</i> point, with binding energy of 250 meV below the Fermi level. Careful analysis is carried out to examine the band dispersions along different high symmetry directions and the possible many-body effect. However, the dispersion kink—a characteristic feature of electron-boson coupling is not obvious in this system. In TMD materials, the van Hove singularity near the Fermi level and the electron-boson (phonon) coupling are suggested to play an important role in forming charge density wave (CDW) and superconductivity, respectively. In this sense, our experimental results may provide a direct explanation for the weakened CDW and relatively low superconducting transition temperature in 1<i>T</i>-NbSeTe. These results may also provide an insight into the charge-density-wave orders in the relevant material systems.

Understanding Reentrance in Frustrated Magnets: The Case of the Er_{2}Sn_{2}O_{7} Pyrochlore.

Reentrance, the return of a system from an ordered phase to a previously encountered less-ordered one as a controlled parameter is continuously varied, is a recurring theme found in disparate physical systems, yet its microscopic cause is often not investigated thoroughly. Here, through detailed characterization and theoretical modeling, we uncover the microscopic mechanism behind reentrance in the strongly frustrated pyrochlore antiferromagnet Er_{2}Sn_{2}O_{7}. We use single crystal heat capacity measurements to expose that Er_{2}Sn_{2}O_{7} exhibits multiple instances of reentrance in its magnetic field B vs temperature T phase diagram for magnetic fields along three cubic high symmetry directions. Through classical MonteCarlo simulations, mean field theory, and classical linear spin-wave expansions, we argue that the origins of the multiple occurrences of reentrance observed in Er_{2}Sn_{2}O_{7} are linked to soft modes. These soft modes arise from phase competition and enhance thermal fluctuations that entropically stabilize a specific ordered phase, resulting in an increased transition temperature for certain field values and thus the reentrant behavior. Our work represents a detailed examination into the mechanisms responsible for reentrance in a frustrated magnet and may serve as a template for the interpretation of reentrant phenomena in other physical systems.

Experimental and Theoretical Investigation of the Surface Electronic Structure of ZnGa2O4(100) Single‐Crystals

Herein, a detailed experimental and theoretical investigation on the surface electronic structure of ZnGa2O4(100) bulk single‐crystals, with a special emphasis on the surface preparation, is presented. The surface crystallizes in the bulk‐derived structure, even at low annealing temperatures. Thermal treatments in ultra‐high vacuum have detrimental effects, as they cannot remove the carbon contamination and induce substantial zinc losses, further exacerbated by sputtering. A short sputtering duration and annealing in oxygen atmosphere dramatically reduce the zinc and oxygen losses in the crystal surface, leading to a contamination‐free, crystalline surface of nearly stoichiometric composition. The investigation of the valence states along the high symmetry directions of the Brillouin zone compares favorably with ab initio pseudopotential calculations, indicating a good surface quality and overall agreement with theory. An in‐depth analysis of the measured and simulated valence band peak intensities reveals difficulties associated with the precise description of the metal‐oxygen hybridization. This study provides a first fundamental understanding of the electronic structure of ZnGa2O4, while also indicating that the surface thermal instability is a challenging task that should be taken into account for the fabrication of heterostructures based on ZnGa2O4.

Growth of pentacene molecules on Tsai-type quasicrystals and related crystal surfaces

We present a study of the adsorption of pentacene (Pn) molecules on the high symmetry (fivefold, threefold, and twofold) surfaces of the icosahedral (i) Ag–In–Yb quasicrystal. We also compare the results with adsorption of Pn on a surface of a periodic crystal related to this quasicrystal, the (111) surface of the Au–Al–Tb 1/1 approximant. Scanning tunneling microscopy reveals that Pn molecules on the quasicrystal surfaces are aligned along the high symmetry directions of the substrates and selectively adsorb on Yb atoms and thus exhibit quasicrystalline order. Pn molecules on the Au–Al–Tb approximant surface also preferably adopt Tb sites. The behavior of selective adsorption can be understood in terms of the geometry and electronic properties of the adsorbate and substrate. The Yb–Yb (Tb–Tb) separations are comparable to the C–C or H–H distances in a Pn molecule. Pn is an electron donor, whereas the unoccupied electronic states of the substrate are dominated by the rare earth atoms, suggesting that there is an electronic transfer between the Pn molecules and Yb (Tb) atoms.

Searching for a promising topological Dirac nodal-line semimetal by angle resolved photoemission spectroscopy

Topological semimetals, in which conduction and valence bands cross each other at either discrete points or along a closed loop with symmetry protected in the momentum space, exhibited great potential in applications of optical devices as well as heterogeneous catalysts or antiferromagnetic spintronics, especially when the crossing points/lines matches Fermi level (E F). It is intriguing to find the ‘ideal’ topological semimetal material, in which has a band structure with Dirac band-crossing located at E F without intersected by other extraneous bands. Here, by using angle resolved photoemission spectroscopy, we investigate the band structure of the so-called ‘square-net’ topological material ZrGeS. The Brillouin zone (BZ) mapping shows the Fermi surface of ZrGeS is composed by a diamond-shaped nodal line loop at the center of BZ and small electron-like Fermi pockets around X point. The Dirac nodal line band-crossing located right at E F, and shows clearly the linear Dirac band dispersions within a large energy range >1.5 eV below E F, without intersected with other bands. The obtained Fermi velocities and effective masses along Γ–X, Γ–M and M–X high symmetry directions were 4.5–5.9 eV Å and 0–0.50 m e, revealing an anisotropic electronic property. Our results suggest that ZrGeS, as a promising topological nodal line semimetal, could provide a promising platform to investigate the Dirac-fermions related physics and the applications of topological devising.

Design of mesoscopic self-collimating photonic crystals under oblique incidence.

Mesoscopic Photonic Crystals (MPhCs) are composed of alternating natural or artificial materials with compensating spatial dispersion. In their simplest form, as presented here, MPhCs are composed by the periodic repetition of a MPhC supercell made of a short slab of bulk material and a short slab of Photonic Crystal (PhCs). Therefore, MPhCs present a multiscale periodicity with a subwavelength periodicity within each PhC slab and with a few-wavelength periodicity for its supercell. Thanks to this mesoscopic structure, MPhCs allow the self-collimation of light, through a mechanism called mesoscopic self-collimation (MSC), along both directions of high symmetry and directions oblique with respect to the MPhCs slab interfaces. Here, we propose a new design method useful for conceiving MPhCs that allow MSC under oblique incidence, avoiding in-plane scattering and ensuring propagation via purely guided modes, without out-of-plane radiation losses. In addition, the proposed method allows a systematic search for optimal MSC structures, which also simultaneously satisfy the impedance matching condition at MPhC interfaces, thus reducing the effect of multiple reflections between bulk-PhC interfaces. The proposed design method has the advantage of an extreme analytical simplicity and it allows direct design of oblique-incidence MPhC structures. Its accuracy is validated through Finite Difference Time Domain simulations and the MSC performances of the designed structures are evaluated, in terms of angular direction, beam waist, overall transmittance, and through discussion of a Figure of Merit that accounts for residual beam curvature. This simple yet powerful method can pave the way for the design of advanced MSC-based photonic interconnects and circuits that are immune to crosstalk and out-of-plane losses.

Low-field onset of Wannier-Stark localization in a polycrystalline hybrid organic inorganic perovskite

Methylammonium lead iodide perovskite (MAPbI3) is renowned for an impressive power conversion efficiency rise and cost-effective fabrication for photovoltaics. In this work, we demonstrate that polycrystalline MAPbI3s undergo drastic changes in optical properties at moderate field strengths with an ultrafast response time, via transient Wannier Stark localization. The distinct band structure of this material - the large lattice periodicity, the narrow electronic energy bandwidths, and the coincidence of these two along the same high-symmetry direction – enables relatively weak fields to bring this material into the Wannier Stark regime. Its polycrystalline nature is not detrimental to the optical switching performance of the material, since the least dispersive direction of the band structure dominates the contribution to the optical response, which favors low-cost fabrication. Together with the outstanding photophysical properties of MAPbI3, this finding highlights the great potential of this material in ultrafast light modulation and novel photonic applications.

Field-induced magnetic states in geometrically frustrated SrEr2O4

We report an unusual in-field behaviour of SrEr_22O_44 for a magnetic field applied along two high-symmetry directions, the a and c axes. This geometrically frustrated magnet hosts two crystallographically inequivalent Er ions, Er1 and Er2, that are both located on triangular zigzag ladders, but only one site, Er1, forms a long-range magnetic order at low temperatures in a zero field. We follow the sequence of peculiar field induced states in SrEr_22O_44 with detailed single-crystal magnetisation and neutron diffraction experiments. On application of an external field along the cc axis, the long-range antiferromagnetic order of the Er1 ions is rapidly destroyed and replaced, in fields between 2 and 5 kOe, by a state with shorter-range correlations. The change in correlation length coincides with a fast increase in magnetisation during the metamagnetic transition above which a long-range order is reestablished and maintained into the high fields. The high-field ferromagnet-like order is characterised by significantly different magnetic moments on the two Er sites, with the Er1 site dominating the magnetisation process. For the field applied parallel to the a axis, in the field range of 4 to 12 kOe, the planes of diffuse magnetic scattering observed in zero field due to the one-dimensional correlations between the Er2 moments are replaced by much more localised but still diffuse features corresponding to the establishment of an up-up-down structure associated with a one-third magnetisation plateau. Above 14 kOe, a ferromagnet-like high-field order is induced following another phase transition. For this direction of the field, the Er2 moments dictate the succession of transitions while the Er1 moments remain significantly less polarised. A complete field polarisation of both Er sites is not achieved even at 50~kOe for either field direction, reflecting the strongly anisotropic nature of magnetisation process in SrEr_22O_44.

Plasmon polaritons in nanoparticle supercrystals: Microscopic quantum theory beyond the dipole approximation

Crystals of plasmonic metal nanoparticles have intriguing optical properties. They reach the regimes of ultrastrong and deep strong light-matter coupling, where the photonic states need to be included in the simulation of material properties. We propose a quantum description of the plasmon polaritons in supercrystals that starts from the dipole and quadrupole excitations of the nanoparticle building blocks and their coupling to photons. Our model excellently reproduces results of finite difference time domain simulations. It provides detailed insight into the emergence of the polariton states. Using the example of a face centered cubic crystals we show that the dipole and quadrupole states mix in many high symmetry directions of the Brilouin zone. A proper description of the plasmon and plasmon-polariton band structure is only possible when including the quadrupole-derived states. Our model leads to an expression of the reduced coupling strength in nanoparticle supercrystals that we show to enter the deep strong coupling regime for metal fill fractions above $0.8$. In addition to the plasmon-polariton energies we analyse the relative contributions of the dipole, quadrupole, and photonic states to their eigenfunctions and are able to demonstrate the decoupling of light in the deep strong coupling regime. Our results pave the way for a better understanding of the quantum properties of metallic nanoparticle supercrystals in the ultrastrong and deep-strong coupling regime.

First-principles study of spin spirals in the multiferroic BiFeO3

We carry out density functional theory (DFT) calculations to explore the antiferromagnetic (AFM) spin cycloid in multiferroic ${\mathrm{BiFeO}}_{3}$ of the $R3c$ ground state structure. We calculate the energy dispersion $E(\mathbf{q})$ of cycloidal spin spirals along the high symmetry directions of the pseudo-cubic unit cell and find a flat AFM spin spiral (or cycloid) ground state with a periodicity of $\ensuremath{\sim}80$ nm, which is in good agreement with experiments. To investigate which structural distortion of the $R3c$ phase is the driving mechanism for the stabilization of this cycloid, we further study three artificial phases: cubic, $R\overline{3}c$, and $R3m$. In all cases, we find a large exchange frustration. The comparison between these phases provides detailed insight about how polarization and octahedral antiphase tilting affect the different magnetic interactions and the magnetic ground state in ${\mathrm{BiFeO}}_{3}$. In $R3c\phantom{\rule{4pt}{0ex}}{\mathrm{BiFeO}}_{3}$, the magnetic ground state is driven by a competition between the frustrated exchange stemming from the hybridization between the elements Bi, Fe, O and the Dzyaloshinskii-Moriya (DM) interaction due to the Fe-Bi ferroelectric displacement. The cycloid appears to be stable because the anisotropy energy in $R3c\phantom{\rule{4pt}{0ex}}{\mathrm{BiFeO}}_{3}$ is relatively small to enforce a collinear order.

First-principles study of the electronic structure and elastic properties of SrGa2 under pressure

Determination of detailed electronic and lattice dynamical properties of hexagonal SrGa2 binary system under external pressure with the aid of first-principles calculation methods is of great importance in terms of the basic characteristics of binary system. On this basis, the phonon dispersion curves are calculated by the high-symmetry directions and related phonon frequencies parameters at the Brillouin zone center using density functional perturbation theory when the elastic constants are computed through the metric-tensor formulation. Besides, the fundamental quantities such as the electronic band structures, Fermi surface topologies, and detailed phonon dispersions are sensitively examined. At the same time, it is examined whether there is a close relationship between the determined properties and superconducting properties of SrGa2 material. However, the calculations clearly show that the information obtained directly from the electronic band structure and Fermi surfaces is insufficient to explain the superconductivity phenomenon of such materials.

Electric-field-tunable electronic nematic order in twisted double-bilayer graphene

Graphene-based moiré systems have attracted considerable interest in recent years as they display a remarkable variety of correlated phenomena. Besides insulating and superconducting phases in the vicinity of integer fillings of the moiré unit cell, there is growing evidence for electronic nematic order both in twisted bilayer graphene and twisted double-bilayer graphene (tDBG), as signaled by the spontaneous breaking of the threefold rotational symmetry of the moiré superlattices. Here, we combine symmetry-based analysis with a microscopic continuum model to investigate the structure of the nematic phase of tDBG and its experimental manifestations. First, we perform a detailed comparison between the theoretically calculated local density of states and recent scanning tunneling microscopy data (arXiv:2009.11645) to resolve the internal structure of the nematic order parameter in terms of the layer, sublattice, spin, and valley degrees of freedom. We find strong evidence that the dominant contribution to the nematic order parameter comes from states at the moiré scale rather than at the microscopic scale of the individual graphene layers, which demonstrates the key role played by the moiré degrees of freedom and confirms the correlated nature of the nematic phase in tDBG. Secondly, our analysis reveals an unprecedented tunability of the orientation of the nematic director in tDBG by an externally applied electric field, allowing the director to rotate away from high-symmetry crystalline directions. We compute the expected fingerprints of this rotation in both STM and transport experiments, providing feasible ways to probe it. Rooted in the strong sensitivity of the flat bands of tDBG to the displacement field, this effect opens an interesting route to the electrostatic control of electronic nematicity in moiré systems.

Canted antiferromagnetic order and spin dynamics in the honeycomb-lattice compound Tb2Ir3Ga9

Single crystal neutron diffraction, inelastic neutron scattering, bulk magnetization measurements, and first-principles calculations are used to investigate the magnetic properties of the honeycomb lattice $\rm Tb_2Ir_3Ga_9$. While the $R\ln2$ magnetic contribution to the low-temperature entropy indicates a $\rm J_{eff}=1/2$ moment for the lowest-energy crystal-field doublet, the Tb$^{3+}$ ions form a canted antiferromagnetic structure below 12.5 K. Due to the Dzyalloshinskii-Moriya interactions, the Tb moments in the $ab$ plane are slightly canted towards $b$ by $6^\circ$ with a canted moment of 1.22 $\mu_{\rm B} $ per formula unit. A minimal $xxz$ spin Hamiltonian is used to simultaneously fit the spin-wave frequencies along the high symmetry directions and the field dependence of the magnetization along the three crystallographic axes. Long-range magnetic interactions for both in-plane and out-of-plane couplings up to the second nearest neighbors are needed to account for the observed static and dynamic properties. The $z$ component of the exchange interactions between Tb moments are larger than the $x$ and $y$ components. This compound also exhibits bond-dependent exchange with negligible nearest exchange coupling between moments parallel and perpendicular to the 4$f$ orbitals. Despite the $J_{{\rm eff}}=1/2$ moments, the spin Hamiltonian is denominated by a large in-plane anisotropy $K_z \sim -1$ meV. DFT calculations confirm the antiferromagnetic ground state and the substantial inter-plane coupling at larger Tb-Tb distances.

Observation of a chiral wave function in the twofold-degenerate quadruple Weyl system BaPtGe

Topological states in quantum materials are defined by non-trivial topological invariants, such as the Chern number, which are properties of their bulk wave functions. A remarkable consequence of topological wave functions is the emergence of edge modes, a phenomenon known as bulk-edge correspondence, that gives rise to quantized or chiral physical properties. While edge modes are widely presented as signatures of non-trivial topology, how bulk wave functions can manifest explicitly topological properties remains unresolved. Here, using high-resolution inelastic x-ray spectroscopy (IXS) combined with first principles calculations, we report experimental signatures of chiral wave functions in the bulk phonon spectrum of BaPtGe, which we show to host a previously undiscovered twofold degenerate quadruple Weyl node. The chirality of the degenerate phononic wave function yields a non-trivial phonon dynamical structure factor, S(Q,$\omega$), along high-symmetry directions, that is in excellent agreement with numerical and model calculations. Our results establish IXS as a powerful tool to uncover topological wave functions, providing a key missing ingredient in the study of topological quantum matter.

Magnetotransport evidence for the nontrivial topological states in the fully spin-polarized Kondo semimetal CeBi

Combination of nontrivial topology of band structure and magnetism in a single material would provide an excellent platform for studying their interplay as well as for discovering exotic physical properties. Alternative to the angle-resolved photoemission spectroscopy measurement that usually suffers disturbance from magnetic domains, the magnetotransport could support useful clues about the nontrivial topological states by measuring the Fermi surface of a magnetic topological system. We report herein the magnetization and magnetotransport measurements of the Kondo semimetal CeBi, a proposed magnetic topological semimetal. The magnetotransport measurements unveil striking Shubnikov-de Haas oscillations associated with a nontrivial Berry phase in its spin-polarized state. The behavior could be interpreted by the appearance of a pair of Weyl points close to the Fermi level on the Γ-X high symmetry direction as uncovered by the first principles calculations. The results would be valuable for verifying a Kondo magnetic topological semimetal as well as be instructive for the study of nontrivial topological states in the Kondo-lattice system.

Mapping the evolution of Bi/Ge(111) empty states: From the wetting layer to pseudo-cubic islands

Semiconductors interfaced with heavy elements possessing a strong atomic spin–orbit coupling are important building blocks for the development of new spintronic devices. Here, we present a microscopic and spin-resolved spectroscopic investigation of ultrathin Bi films grown onto a Ge(111) substrate. At monolayer coverage, a Bi wetting layer is formed, characterized by a semiconducting behavior and a (3×3)R30° superstructure. The wetting layer supports the subsequent growth of Bi islands with a pseudo-cubic structure similar to that of Bi(110), showing a well-defined orientation with respect to the substrate high-symmetry directions. We performed photoemission and spin-resolved inverse photoemission experiments at off-normal electron emission and incidence, respectively, along the substrate Γ¯K¯ direction. Inverse photoemission, in particular, highlights the presence of a spin-polarized empty Bi state, not reported so far, due to the strong spin–orbit effects characteristic of the Bi surface and thin layers. Finally, scanning tunneling spectroscopy is employed to link the observed spectroscopic features to either the wetting layer or the Bi islands.

Ab-initio investigations on dynamical and lattice thermal behaviours of ThC

In this study, the vibrational and lattice thermal behaviours of ThC are investigated through the density functional theory. Thermal characteristics of ThC are studied under the novel models based on the Debye–Grϋneisen and full quasi-harmonic approximation. The Gibbs free energy, thermal Grϋneisen ratio, adiabatic bulk moduli, vibrational contributions of Helmholtz free energy, internal energy and entropy of ThC are studied for the first time. The structural properties including lattice constant (a0), bulk modulus (B0) and the first derivative of the bulk modulus ( $$B^{\prime}_0$$ ) are calculated and compared with other theoretical and experimental works that revealed a good agreement. Phonon band structure was calculated using density functional perturbation theory along the several high symmetry directions in the first Brillouin zone. The absence of imaginary phonon frequencies in the whole Brillouin zone is characteristic of the dynamical stability of the crystalline structure. Thermodynamic computations show that the vibrational Helmholtz free energy, Gibbs free energy and adiabatic bulk modulus decreased with increase in the temperature at a given pressure.

Symmetry analysis of tensors in the honeycomb lattice of edge-sharing octahedra

We obtain the most general forms of rank-2 and rank-3 tensors allowed by the crystal symmetries of the honeycomb lattice of edge-sharing octahedra for crystals belonging to different crystallographic point groups, including the monoclinic point group $2/m$ and the trigonal (or rhombohedral) point group $\bar{3}$. Our results are relevant for two-dimensional materials, such as $\alpha$-RuCl$_3$, CrI$_3$, and the honeycomb iridates. We focus on the magnetic-field-dependent thermal conductivity tensor $\kappa_{ij}(\mathbf{H})$, which describes a system's longitudinal and thermal Hall responses, for the cases when the magnetic field is applied along high-symmetry directions, perpendicular to the plane and in the plane. We highlight some unexpected results, such as the equality of fully-longitudinal components to partially-transverse components in rank-3 tensors for systems with three-fold rotational symmetry, and make testable predictions for the thermal conductivity tensor.

Field angle dependent vortex lattice phase diagram in MgB2

Using small-angle neutron scattering we have studied the superconducting vortex lattice (VL) phase diagram in MgB2 as the applied magnetic field is rotated away from the c axis and towards the basal plane. The field rotation gradually suppresses the intermediate VL phase which exists between end states aligned with two high symmetry directions in the hexagonal basal plane for H || c. Above a critical angle, the intermediate state disappears, and the previously continuous transition becomes discontinuous. The evolution towards the discontinuous transition can be parameterized by a vanishing twelvefold anisotropy term in the VL free energy.

Cubic metamaterial crystal supporting broadband isotropic chiral phonons

Chiral metamaterials can support chiral phonons leading to acoustical activity, the acoustical counterpart of optical activity. However, the properties of early metamaterial designs have been very highly anisotropic, and chiral acoustical phonons occurred only for selected high-symmetry directions. The authors propose a novel chiral metamaterial based on ``twisting'' a truncated octahedron in a simple-cubic unit cell. Not supported by crystal symmetry alone but rather by a tuned degeneracy, chiral phonons and large broadband acoustical activity are obtained for all phonon propagation directions in 3D. This result is notable because even isotropic achiral acoustical phonons are rare for crystalline materials.