72 research outputs found
Can HCCH/HBNH Break B=N/C=C Bonds of Single-Wall BN/Carbon Nanotubes at Their Surface?
The iminoborane (HBNH) molecule, which prefers cycloaddition reactions, selectively breaks a B=N bond of smaller diameter single-wall BNNTs and expands a ring at their surface, either at the edges or at the middle of the tube. Density functional theory (DFT) is used to test whether its organic counterpart HCCH can do the same with BNNTs. HCCH-BNNT complexes are identified and transition states located for these combination reactions. Also explored are possible reactions of HBNH with SWNTs and HCCH with SWNTs. Data suggest that B=N (C=C) bond breaking, followed by ring expansion at the surface may be possible. Although [2+2] cycloaddition reaction seems possible for HBNH-BNNTs, a high energy barrier hinders the process for other combinations of host and guest. Introduction of substituents to HBNH/HCCH may allow a facile process. In most cases of HCCH-BNNTs, HBNH-SWNTs, and HCCH-SWNTs, transition states are identified and suggest an electron-rich guest might lower barrier heights to form stable complexes. Reaction with HCCH or HBNH at the bay-region of smaller diameter armchair tube is not favorable
Europium Underneath Graphene on Ir(111): Intercalation Mechanism, Magnetism, and Band Structure
The intercalation of Eu underneath Gr on Ir(111) is comprehensively
investigated by microscopic, magnetic, and spectroscopic measurements, as well
as by density functional theory. Depending on the coverage, the intercalated Eu
atoms form either a or a R superstructure with respect to Gr. We investigate the
mechanisms of Eu penetration through a nominally closed Gr sheet and measure
the electronic structures and magnetic properties of the two intercalation
systems. Their electronic structures are rather similar. Compared to Gr on
Ir(111), the Gr bands in both systems are essentially rigidly shifted to larger
binding energies resulting in n-doping. The hybridization of the Ir surface
state with Gr states is lifted, and the moire superperiodic potential is
strongly reduced. In contrast, the magnetic behavior of the two intercalation
systems differs substantially as found by X-ray magnetic circular dichroism.
The Eu structure displays plain paramagnetic behavior, whereas
for the R structure the large
zero-field susceptibility indicates ferromagnetic coupling, despite the absence
of hysteresis at 10 K. For the latter structure, a considerable easy-plane
magnetic anisotropy is observed and interpreted as shape anisotropy.Comment: 18 pages with 14 figures, including Supplemental Materia
Collective orbital excitations in orbitally ordered YVO3 and HoVO3
We study orbital excitations in the optical absorption spectra of YVO3 and
HoVO3. We focus on an orbital absorption band observed at 0.4 eV for
polarization E parallel c. This feature is only observed in the intermediate,
monoclinic phase. By comparison with the local crystal-field excitations in
VOCl and with recent theoretical predictions for the crystal-field levels we
show that this absorption band cannot be interpreted in terms of a local
crystal-field excitation. We discuss a microscopic model which attributes this
absorption band to the exchange of two orbitals on adjacent sites, i.e., to the
direct excitation of two orbitons. This model is strongly supported by the
observed dependence on polarization and temperature. Moreover, the calculated
spectral weight is in good agreement with the experimental result.Comment: 12 pages, 9 figure
Fractional and Integer Excitations in Quantum Antiferromagnetic Spin 1/2 Ladders
Spectral densities are computed in unprecedented detail for quantum
antiferromagnetic spin 1/2 two-leg ladders. These results were obtained due to
a major methodical advance achieved by optimally chosen unitary
transformations. The approach is based on dressed integer excitations.
Considerable weight is found at high energies in the two-particle sector.
Precursors of fractional spinon physics occur implying that there is no
necessity to resort to fractional excitations in order to describe features at
higher energies.Comment: 6 pages, 4 figures included, minor text changes, improved figure
Observation of two-magnon bound states in the two-leg ladders of (Ca,La)14Cu24O41
Phonon-assisted 2-magnon absorption is studied at T=4 K in the spin-1/2
two-leg ladders of Ca_14-x La_x Cu_24 O_41 (x=5 and 4) for polarization of the
electrical field parallel to the legs and the rungs, respectively. Two peaks at
about 2140 and 2800 1/cm reflect van-Hove singularities in the density of
states of the strongly dispersing 2-magnon singlet bound state, and a broad
peak at about 4000 1/cm is identified with the 2-magnon continuum. Two
different theoretical approaches (Jordan-Wigner fermions and perturbation
theory) describe the data very well for J_parallel = 1050 - 1100 1/cm and
J_parallel / J_perp = 1 - 1.1. A striking similarity of the high-energy
continuum absorption of the ladders and of the undoped high T_c cuprates is
observed.Comment: 4 pages, 3 figures, Revte
The Structure of Operators in Effective Particle-Conserving Models
For many-particle systems defined on lattices we investigate the global
structure of effective Hamiltonians and observables obtained by means of a
suitable basis transformation. We study transformations which lead to effective
Hamiltonians conserving the number of excitations. The same transformation must
be used to obtain effective observables. The analysis of the structure shows
that effective operators give rise to a simple and intuitive perspective on the
initial problem. The systematic calculation of n-particle irreducible
quantities becomes possible constituting a significant progress. Details how to
implement the approach perturbatively for a large class of systems are
presented.Comment: 12 pages, 1 figure, accepted by J. Phys. A: Math. Ge
Optical study of orbital excitations in transition-metal oxides
The orbital excitations of a series of transition-metal compounds are studied
by means of optical spectroscopy. Our aim was to identify signatures of
collective orbital excitations by comparison with experimental and theoretical
results for predominantly local crystal-field excitations. To this end, we have
studied TiOCl, RTiO3 (R=La, Sm, Y), LaMnO3, Y2BaNiO5, CaCu2O3, and K4Cu4OCl10,
ranging from early to late transition-metal ions, from t_2g to e_g systems, and
including systems in which the exchange coupling is predominantly
three-dimensional, one-dimensional or zero-dimensional. With the exception of
LaMnO3, we find orbital excitations in all compounds. We discuss the
competition between orbital fluctuations (for dominant exchange coupling) and
crystal-field splitting (for dominant coupling to the lattice). Comparison of
our experimental results with configuration-interaction cluster calculations in
general yield good agreement, demonstrating that the coupling to the lattice is
important for a quantitative description of the orbital excitations in these
compounds. However, detailed theoretical predictions for the contribution of
collective orbital modes to the optical conductivity (e.g., the line shape or
the polarization dependence) are required to decide on a possible contribution
of orbital fluctuations at low energies, in particular in case of the orbital
excitations at about 0.25 eV in RTiO3. Further calculations are called for
which take into account the exchange interactions between the orbitals and the
coupling to the lattice on an equal footing.Comment: published version, discussion of TiOCl extended to low T, improved
calculation of orbital excitation energies in TiOCl, figure 16 improved,
references updated, 33 pages, 20 figure
Fingerprints of Kitaev physics in the magnetic excitations of honeycomb iridates
In the quest for realizations of quantum spin liquids, the exploration of
Kitaev materials - spin-orbit entangled Mott insulators with strong
bond-directional exchanges - has taken center stage. However, in these
materials the local spin-orbital j=1/2 moments typically show long-range
magnetic order at low temperature, thus defying the formation of a spin-liquid
ground state. Using resonant inelastic x-ray scattering (RIXS), we here report
on a proximate spin liquid regime with clear fingerprints of Kitaev physics in
the magnetic excitations of the honeycomb iridates alpha-Li2IrO3 and Na2IrO3.
We observe a broad continuum of magnetic excitations that persists up to at
least 300K, more than an order of magnitude larger than the magnetic ordering
temperatures. We prove the magnetic character of this continuum by an analysis
of the resonance behavior. RIXS measurements of the dynamical structure factor
for energies within the continuum show that dynamical spin-spin correlations
are restricted to nearest neighbors. Notably, these spectroscopic observations
are also present in the magnetically ordered state for excitation energies
above the conventional magnon excitations. Phenomenologically, our data agree
with inelastic neutron scattering results on the related honeycomb compound
RuCl3, establishing a common ground for a proximate Kitaev spin-liquid regime
in these materials.Comment: 13 pages, 14 figure
Observation of out-of-phase bilayer plasmons in YBa_2Cu_3O_7-delta
The temperature dependence of the c-axis optical conductivity \sigma(\omega)
of optimally and overdoped YBa_2Cu_3O_x (x=6.93 and 7) is reported in the far-
(FIR) and mid-infrared (MIR) range. Below T_c we observe a transfer of spectral
weight from the FIR not only to the condensate at \omega = 0, but also to a new
peak in the MIR. This peak is naturally explained as a transverse out-of-phase
bilayer plasmon by a model for \sigma(\omega) which takes the layered crystal
structure into account. With decreasing doping the plasmon shifts to lower
frequencies and can be identified with the surprising and so far not understood
FIR feature reported in underdoped bilayer cuprates.Comment: 7 pages, 3 eps figures, Revtex, epsfi
Signatures of polaronic excitations in quasi-one-dimensional LaTiO
The optical properties of quasi-one-dimensional metallic LaTiO are
studied for the polarization along the and axes. With decreasing
temperature modes appear along both directions suggestive for a phase
transition. The broadness of these modes along the conducting axis might be due
to the coupling of the phonons to low-energy electronic excitations across an
energy gap. We observe a pronounced midinfrared band with a temperature
dependence consistent with (interacting) polaron models. The polaronic picture
is corroborated by the presence of strong electron-phonon coupling and the
temperature dependence of the dc conductivity.Comment: 5 pages, 5 figure
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