arXiv subjects

A. M. Rappe

Publications and source records attributed to A. M. Rappe.

10 recordsLinked to original sources

arXiv2020

Optical signatures of multifold fermions in the chiral topological semimetal CoSi

We report the optical conductivity in high-quality crystals of the chiral topological semimetal CoSi, which hosts exotic quasiparticles known as multifold fermions. We find that the optical response is separated into several distinct regions as a function of frequency, each dominated by different types of quasiparticles. The low-frequency intraband response is captured by a narrow Drude peak from a high-mobility electron pocket of double Weyl quasi-particles, and the temperature dependence of the spectral weight is consistent with its Fermi velocity. By subtracting the low-frequency sharp Drude and phonon peaks at low temperatures, we reveal two intermediate quasi-linear inter-band contributions separated by a kink at 0.2 eV. Using Wannier tight-binding models based on first-principle calculations, we link the optical conductivity above and below 0.2 eV to interband transitions near the double Weyl fermion and a threefold fermion, respectively. We analyze and determine the chemical potential relative to the energy of the threefold fermion, revealing the importance of transitions between a linearly dispersing band and a flat band. More strikingly, below 0.1 eV our data are best explained if spin-orbit coupling is included, suggesting that at these energies the optical response is governed by transitions between a previously unobserved four-fold spin-3/2 node and a Weyl node. Our comprehensive combined experimental and theoretical study provides a way to resolve different types of multifold fermions in CoSi at different energy. More broadly our results provide the necessary basis to interpret the burgeoning set of optical and transport experiments in chiral topological semimetals.

cond-mat.mtrl-sci↗

arXiv2018

Wallpaper Fermions and the Nonsymmorphic Dirac Insulator

Recent developments in the relationship between bulk topology and surface crystal symmetry have led to the discovery of materials whose gapless surface states are protected by crystal symmetries. In fact, there exists only a very limited set of possible surface crystal symmetries, captured by the 17 "wallpaper groups." We show that a consideration of symmetry-allowed band degeneracies in the wallpaper groups can be used to understand previous topological crystalline insulators, as well as to predict new examples. In particular, the two wallpaper groups with multiple glide lines, $pgg$ and $p4g$, allow for a new topological insulating phase, whose surface spectrum consists of only a single, fourfold-degenerate, true Dirac fermion. Like the surface state of a conventional topological insulator, the surface Dirac fermion in this "nonsymmorphic Dirac insulator" provides a theoretical exception to a fermion doubling theorem. Unlike the surface state of a conventional topological insulator, it can be gapped into topologically distinct surface regions while keeping time-reversal symmetry, allowing for networks of topological surface quantum spin Hall domain walls. We report the theoretical discovery of new topological crystalline phases in the A$_2$B$_3$ family of materials in SG 127, finding that Sr$_2$Pb$_3$ hosts this new topological surface Dirac fermion. Furthermore, (100)-strained Au$_2$Y$_3$ and Hg$_2$Sr$_3$ host related topological surface hourglass fermions. We also report the presence of this new topological hourglass phase in Ba$_5$In$_2$Sb$_6$ in SG 55. For orthorhombic space groups with two glides, we catalog all possible bulk topological phases by a consideration of the allowed non-abelian Wilson loop connectivities, and we develop topological invariants for these systems. Finally, we show how in a particular limit, these crystalline phases reduce to copies of the SSH model.

cond-mat.mes-hall↗

arXiv2016

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO$_3$

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply sub-picosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO$_3$ ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond timescales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables direct comparison with first-principles-based molecular dynamics simulations, with good agreement obtained.

cond-mat.mtrl-sci↗

arXiv2015

Double Dirac Semimetals in Three Dimensions

We study a class of Dirac semimetals that feature an eightfold-degenerate double Dirac point. We show that 7 of the 230 space groups can host such Dirac points and argue that they all generically display linear dispersion. We introduce an explicit tight-binding model for space groups 130 and 135, showing that 135 can host an intrinsic double Dirac semimetal -- one with no additional degeneracies at the Fermi energy. We consider symmetry-lowering perturbations and show that uniaxial compressive strain in different directions leads to topologically distinct insulating phases. In addition, the double Dirac semimetal can accommodate topological line defects that bind helical modes. Potential materials realizations are discussed.

cond-mat.mtrl-sci↗

arXiv2015

Modiffied Schottky emission to explain thickness dependence and slow depolarization in BaTiO$_3$ nanowires

We investigate the origin of the depolarization rates in ultrathin adsorbate-stabilized ferroelectric wires. By applying density functional theory calculations and analytic modeling, we demonstrate that the depolarization results from the leakage of charges stored at the surface adsorbates, which play an important role in the polarization stabilization. The depolarization speed varies with thickness and temperature, following several complex trends. A comprehensive physical model is presented, in which quantum tunneling, Schottky emission and temperature dependent electron mobility are taken into consideration. This model simulates experimental results, validating the physical mechanism. We also expect that this improved tunneling-Schottky emission model could be applied to predict the retention time of polarization and the leakage current for various ferroelectric materials with different thicknesses and temperatures.

cond-mat.mtrl-sci↗

arXiv2012

Dirac semimetal in three dimensions

In a Dirac semimetal, the conduction and valence bands contact only at discrete (Dirac) points in the Brillouin zone (BZ) and disperse linearly in all directions around these critical points. Including spin, the low energy effective theory around each critical point is a four band Dirac Hamiltonian. In two dimensions (2D), this situation is realized in graphene without spin-orbit coupling. 3D Dirac points are predicted to exist at the phase transition between a topological and a normal insulator in the presence of inversion symmetry. Here we show that 3D Dirac points can also be protected by crystallographic symmetries in particular space-groups and enumerate the criteria necessary to identify these groups. This reveals the possibility of 3D analogs to graphene. We provide a systematic approach for identifying such materials and present ab initio calculations of metastable β-cristobalite BiO_2 which exhibits Dirac points at the three symmetry related X points of the BZ.

cond-mat.mes-hall↗

arXiv2010

Local Probing of Mesoscopic Physics of Ferroelectric Domain Walls

Domain wall dynamics in ferroic materials underpins functionality of data storage and information technology devices. Using localized electric field of a scanning probe microscopy tip, we experimentally demonstrate a surprisingly rich range of polarization reversal behaviors in the vicinity of the initially flat 180°ferroelectric domain wall. The nucleation bias is found to increase by an order of magnitude from a 2D nucleus at the wall to 3D nucleus in the bulk. The wall is thus significantly ferroelectrically softer than the bulk. The wall profoundly affects switching on length scales of the order of micrometers. The mechanism of correlated switching is analyzed using analytical theory and phase-field modeling. The long-range effect is ascribed to wall bending under the influence of a tip bias well below the bulk nucleation field and placed many micrometers away from the wall. These studies provide an experimental link between the macroscopic and mesoscopic physics of domain walls and atomistic models of nucleation.

cond-mat.mtrl-sci↗

arXiv2007

Optimized norm-conserving Hartree-Fock pseudopotentials for plane-wave calculations

We report Hartree-Fock (HF) based pseudopotentials suitable for plane-wave calculations. Unlike typical effective core potentials, the present pseudopotentials are finite at the origin and exhibit rapid convergence in a plane-wave basis; the optimized pseudopotential method [A. M. Rappe et. al, Phys. Rev. B 41 1227--30 (1990)] improves plane-wave convergence. Norm-conserving HF pseudopotentials are found to develop long-range non-Coulombic behavior which does not decay faster than 1/r, and is non-local. This behavior, which stems from the nonlocality of the exchange potential, is remedied using a recently developed self-consistent procedure [J. R. Trail and R. J. Needs, J. Chem. Phys. 122, 014112 (2005)]. The resulting pseudopotentials slightly violate the norm conservation of the core charge. We calculated several atomic properties using these pseudopotentials, and the results are in good agreement with all-electron HF values. The dissociation energies, equilibrium bond lengths, and frequency of vibrations of several dimers obtained with these HF pseudopotentials and plane waves are also in good agreement with all-electron results.

cond-mat.mtrl-sci↗

arXiv2000

n-Alkyl Thiol Head Group Interactions with the Au(111) Surface

State-of-the-art first principles calculations based on density functional theory were performed on CH_3(CH_2)_{n-1}S-Au(111) systems. We show that the adsorption site of methylthiolate at low coverage on the Au(111) surface is the fcc site, not the hcp site as has been recently reported. Further, we report results for chain length dependency and the electronic structure of the system.

cond-mat.mtrl-sci↗

arXiv1997

Theoretical examination of stress fields in Pb(Zr_0.5Ti_0.5)O_3

In this paper, we develop a rigorous formulation of the local stress field. This approach can be used in conjuction with any first-principles method to study stress fields in complex bonded systems. In particular we investigate the induced stress fields resulting from homogeneous deformations for tetragonal PbTiO_3 and rhombohedral PbZrO_3. As an extension of these findings we also compute the induced stress fields resulting from homogeneous deformations of the (100) and (111) orderings of Pb(Zr_0.5Ti_0.5)O_3. The stress-field responses in these four materials are compared and their piezoelectric responses are discussed.

cond-mat.mtrl-sci↗