Search

Layered narrow band gap semiconductor Bi2Se3 is composed of heavy elements with strong spin-orbital coupling (SOC), which has been identified both as a good candidate of thermoelectric material of high thermoelectric figure-of-merit (ZT) and a topological insulator of Z2-type with a gapless surface band in Dirac cone shape. The existence of a conjugated pi-bond system on the surface of each Bi2Se3 quintuple layer is proposed based on an extended valence bond model having valence electrons distributed in the hybridized orbitals. Supporting experimental evidences of a 2D conjugated pi-bond system on each quintuple layer of Bi2Se3 are provided by electron energy-loss spectroscopy (EELS) and electron density (ED) mapping through inverse Fourier transform of X-ray diffraction data. Quantum chemistry calculations support the pi-bond existence between partially filled 4pz orbitals of Se via side-to-side orbital overlap positively. The conjugated pi-bond system on the surface of each quintuple Bi2Se3 layer is proposed being similar to that found in graphite (graphene) and responsible for the unique 2D conduction mechanism. The van der Waals (vdW) attractive force between quintuple layers is interpreted being coming from the anti-ferroelectrically ordered effective electric dipoles which are constructed with pi-bond trimer pairs on Se-layers across the vdW gap of minimized Coulomb repulsion., Comment: 12 pages, 9 figures, to be published in Phys. Rev. Materials

The peculiar field-dependent magnetism of Na0.82CoO2 has been investigated through an analysis of its DC and AC spin susceptibilities. To account for the easily activated narrow b2g-a1g gap of the crystal field for Co in the cobalt oxide layer, the spin-state transition of Co3+ (3d6) between the low spin (LS) state b2g^2-a1g^0 of S=0 and the intermediate spin (IS) state b2g^1-a1g^1 of S=1 is thus seen as thermally activated and exhibits a Boltzmann distribution. The IS state of Co3+ within each sqrt(13a) hexagonal superlattice formed by the S=1/2 state of the Co4+ ions appears randomly within each supercell and shows significant temperature and field dependence. The magnetic field is found to assist in pinning down the thermally activated state of Co3+ and swings the Boltzmann distribution weight toward a higher fraction of the IS state. The field dependence of the in-plane magnetic moment from the added number of S=1 spins is used to explain the origin of A-type antiferromagnetic (AF) ordering, particularly that the ferromagnetic (FM)-like behavior below TN at low field is actually a ferrimagnetic IS spin ordering of Co3+., Comment: 5 pages, 4 figures, to be published in PRB

The B20 magnets with the Dzyaloshinskii-Moriya (D-M) interaction exhibit spin helix and Skyrmion spin textures unattainable in traditional Heisenberg ferromagnets. We have determined the intrinsic resistivity of the spin helix, which is a macroscopic Bloch domain wall, in B20 (Fe-Co)Si magnets. We found a universal resistance ratio of gamma = 1.35 with current parallel and perpendicular to the helix, independent of composition and temperature. This gamma value is much smaller than 3, the well-known minimum value for domain wall resistivity in traditional ferromagnets, due to the significant spin-orbit coupling in the B20 magnets.

The B20 chiral magnets with broken inversion symmetry and C4 rotation symmetry have attracted much attention. The broken inversion symmetry leads to the Dzyaloshinskii-Moriya that gives rise to the helical and Skyrmion states. We report the unusual magnetoresistance (MR) of B20 chiral magnet Fe0.85Co0.15Si that directly reveals the broken C4 rotation symmetry. We present a microscopic theory, a minimal theory with two spin-orbit terms, that satisfies all the symmetry requirements and accounts for the transport experiments.

Plasmons dispersion and nonvertical interband transitions in Bi2Se3 single crystals were investigated by electron energy-loss spectroscopy in conjunction with (scanning) transmission electron microscopy, (S)TEM-EELS. Both volume plasmons ({\pi} plasmon at 7 eV and {\pi}+{\sigma} plasmon at 17 eV) and surface plasmons (~5.5 and 10 eV) were demonstrated in STEM-EELS spectra and the corresponding spectral imaging in real space. In the further EELS experiments in reciprocal space, the momentum-dependent spectra reveal very different dispersion behavior between {\pi} and {\pi}+{\sigma} plasmons, with {\pi}+{\sigma} plasmons showing a typical quadratic dependence whereas the {\pi} plasmon exhibiting a linear dispersion analogous to what was reported for graphene. Furthermore, a low energy excitation 0.7~1.6 eV was also observed which is attributed to direct nonvertical interband transitions along the gamma-F direction.

In the spin ladder compound BiCu$_2$PO$_6$ there exists a decisive dynamics of spin excitations that we classify and characterize using inelastic light scattering. We observe low-energy singlets and a broad triplon continuum extending from 36 cm$^{-1}$ to 700 cm$^{-1}$ in ($aa$), ($bb$), and ($cc$) light scattering polarizations. Though isolated spin ladder physics can roughly account for the observed excitations at high energies, frustration and interladder interactions need to be considered to fully describe the spectral distribution and scattering selection rules at low and intermediate energies. More significantly, an interladder singlet bound mode at 24 cm$^{-1}$, lying below the continuum, shows its largest scattering intensity in interladder ($ab$) polarization. In contrast, two intraladder bound states at 62 cm$^{-1}$ and 108 cm$^{-1}$ with energies comparable to the continuum are observed with light polarization along the leg ($bb$) and the rung ($cc$). We attribute the rich spectrum of singlet bound modes to a melting of a dimer crystal. Our study provides evidence for a Z$_2$ quantum phase transition from a dimer to a resonating valence bond state driven by singlet fluctuations., Comment: 14 pages, 4 figures, Accepted for publication in PRL

A hybrid orbital model for the topological insulator Bi2Se3 is proposed and compared to that of graphene. The existence of a pi-bond trimer on the Se1 layer at the van der Waals gap and on the surface is thought to be responsible for the unusual surface conduction mechanism found in Bi2Se3 as a topological insulator. The three pi-bonds are locked as permanent electric dipoles between the Se1 layers in the van der Waals gap as an attractive force for the bulk as a gapped semiconductor. In contrast, the pi-bond trimers on the surface are unlocked and exhibit two degenerate quantum states, creating a local charge transfer mechanism in the cross-bridge model that is responsible for the surface conduction. The role of pi-bonds on the Bi2Se3 surface is compared with that in graphene for a similar 2D band structure containing Dirac cones., Comment: 6pages, 6figures

The existence of pi-bonds on topological insulator surfaces is found to be closely related to the phenomena of surface conduction and surface band spin polarization. A pi-bond trimer or pi-bond dimer on the surface can form open conjugated systems that are responsible for the unique surface conduction mechanism of a topological insulator. Parity operation in 2D is identified for a pi-bond trimer within a six-fold symmetry coordination and a pi-bond dimer within a four-fold symmetry coordination. Spontaneous 2D parity symmetry breaking is found to be closely related to the theoretically predicted pi Berry's phase and the observed surface band spin polarization. The role of pi-bonds on a cleaved Bi2Se3 surface is compared to that for graphene with a 2D band structure containing Dirac cones. Similar pi-bond dimers within a four-fold 2D symmetry coordination can also be identified in strained alpha-Sn of diamond structure as a theoretically predicted topological insulator., Comment: 5pages, 6figures

The impact of oxygen deficiency on physical properties of Na2/3CoO2-x has been investigated. From the combined thermogravimetric, magnetic susceptibility and synchrotron X-ray Laue diffraction studies, it is demonstrated that Na2/3CoO2 shows no superlattice ordering due to Na ions; however Na2/3CoO1.98, which has the same Co valence as that of Na0.71CoO2, shows nearly identical magnetic and transport properties and the same simple hexagonal superlattice ordering of sqrt(12)a. It is proposed that the Na ion ordering found in Na2/3CoO1.98 is identical to the ideal Na0.71CoO2 of large sqrt(12)a x sqrt(12)a x 3c superlattice but with additional Na vacancies which are bound to the oxygen defects at room temperature. We conclude that oxygen vacancies play a key role in stabilizing the superlattice structure and must be accounted for in its modeling., Comment: 5 pages, 4 figures

Phase diagram of Na$_x$CoO$_2$ (x $\gtrsim$ 0.71) has been reinvestigated using electrochemically fine tuned single crystals. Both phase separation and staging phenomena as a result of sodium multi-vacancy cluster ordering have been found. Phase separation phenomenon is observed in the narrow ranges of 0.76 $\lesssim$ x $\lesssim$ 0.82 and 0.83 $\lesssim$ x $\lesssim$ 0.86. While x = 0.820 shows A-type antiferromagnetic (A-AF) ordering below 22K, x = 0.833 is confirmed to have a magnetic ground state of A-AF ordering below $\sim$8K and is only reachable through slow cooling. In addition, x = 0.859 is found to be responsible for the highest A-AF transition temperature at about 29K. Staging model based on ordered stacking of multi-vacancy layers is proposed to explain the hysteretic behavior and A-AF correlation length for x $\sim$ 0.82-0.86., 6 pages, 6 figures, to be published in PRB

Here we report the observation of Fermi surface (FS) pockets via the Shubnikov de Haas effect in Na$_x$CoO$_2$ for $x = 0.71$ and 0.84, respectively. Our observations indicate that the FS expected for each compound intersects their corresponding Brillouin zones, as defined by the previously reported superlattice structures, leading to small reconstructed FS pockets, but only if a precise number of holes per unit cell is \emph{localized}. For $0.71 \leq x < 0.75$ the coexistence of itinerant carriers and localized $S =1/2$ spins on a paramagnetic triangular superlattice leads at low temperatures to the observation of a deviation from standard Fermi-liquid behavior in the electrical transport and heat capacity properties, suggesting the formation of some kind of quantum spin-liquid ground state., 4 pages, 4 figures