1,069 research outputs found
Local motifs in GeS-GaS glasses
The structure of (GeS)(GaS) and
(GeS)(GaS) glasses was investigated by Raman
scattering, high energy X-ray diffraction and extended X-ray absorption fine
structure (EXAFS) measurements at the Ga and Ge K-edges. The reverse Monte
Carlo simulation technique (RMC) was used to obtain structural models
compatible with diffraction and EXAFS datasets. It was found that the
coordination number of Ga is close to four. While Ge atoms have only S
neighbors, Ga binds to S as well as to Ga atoms showing a violation of chemical
ordering in GeS-GaS glasses. Analysis of the corner- and
edge-sharing between [GeS] units revealed that about 30% of germanium
atoms participate in the edge-shared tetrahedra.Comment: 23 pages, 7 figures, accepted for publication in Journal of Alloys
and Compound
The quantum origins of skyrmions and half-skyrmions in Cu2OSeO3
The Skyrme-particle, the , was introduced over half a century ago
and used to construct field theories for dense nuclear matter. But with
skyrmions being mathematical objects - special types of topological solitons -
they can emerge in much broader contexts. Recently skyrmions were observed in
helimagnets, forming nanoscale spin-textures that hold promise as information
carriers. Extending over length-scales much larger than the inter-atomic
spacing, these skyrmions behave as large, classical objects, yet deep inside
they are of quantum origin. Penetrating into their microscopic roots requires a
multi-scale approach, spanning the full quantum to classical domain. By
exploiting a natural separation of exchange energy scales, we achieve this for
the first time in the skyrmionic Mott insulator CuOSeO. Atomistic ab
initio calculations reveal that its magnetic building blocks are strongly
fluctuating Cu tetrahedra. These spawn a continuum theory with a skyrmionic
texture that agrees well with reported experiments. It also brings to light a
decay of skyrmions into half-skyrmions in a specific temperature and magnetic
field range. The theoretical multiscale approach explains the strong
renormalization of the local moments and predicts further fingerprints of the
quantum origin of magnetic skyrmions that can be observed in CuOSeO,
like weakly dispersive high-energy excitations associated with the Cu
tetrahedra, a weak antiferromagnetic modulation of the primary ferrimagnetic
order, and a fractionalized skyrmion phase.Comment: 5 pages, 3 figure
Magnetic pyroxenes LiCrGe2O6 and LiCrSi2O6: dimensionality crossover in a non-frustrated S=3/2 Heisenberg model
The magnetism of magnetoelectric = 3/2 pyroxenes LiCrSiO and
LiCrGeO is studied by density functional theory (DFT) calculations,
quantum Monte Carlo (QMC) simulations, neutron diffraction, as well as
low-field and high-field magnetization measurements. In contrast with earlier
reports, we find that the two compounds feature remarkably different, albeit
non-frustrated magnetic models. In LiCrSiO, two relevant exchange
integrals, 9 K along the structural chains and
2 K between the chains, form a 2D anisotropic honeycomb lattice. In
contrast, the spin model of LiCrGeO is constituted of three different
exchange couplings. Surprisingly, the leading exchange
2.3 K operates between the chains, while 1.2 K is about
two times smaller. The additional interlayer coupling
renders this model 3D. QMC simulations reveal excellent agreement between
our magnetic models and the available experimental data. Underlying mechanisms
of the exchange couplings, magnetostructural correlations, as well as
implications for other pyroxene systems are discussed.Comment: 11 pages, 8 figures, 3 tables + Supplementary informatio
Electronic and magnetic structure of CsVO
We have studied the electronic structure of the spin-gapped system
CsVO by means of an ab initio calculation.
Our analysis and a re-examination of the susceptibility data indicate that
the behavior of this system is much closer to that of an alternating spin-1/2
antiferromagnetic chain with significant inter-dimer coupling and weaker
inter-chain couplings than that of isolated dimers as was initially proposed.
Comparison to the vanadate family members -NaVO,
-LiVO and isostructural compounds like
(VO)PO (VOPO) is discussed.Comment: revised version. To appear in Phys. Rev.
Intermediate Phases, structural variance and network demixing in chalcogenides: the unusual case of group V sulfides
We review Intermediate Phases (IPs) in chalcogenide glasses and provide a
structural interpretation of these phases. In binary group IV selenides, IPs
reside in the 2.40 < r < 2.54 range, and in binary group V selenides they shift
to a lower r, in the 2.29< r < 2.40 range. Here r represents the mean
coordination number of glasses. In ternary alloys containing equal proportions
of group IV and V selenides, IPs are wider and encompass ranges of respective
binary glasses. These data suggest that the local structural variance
contributing to IP widths largely derives from four isostatic local structures
of varying connectivity r; two include group V based quasi-tetrahedral (r =
2.29) and pyramidal (r = 2.40) units, and the other two are group IV based
corner-sharing (r = 2.40) and edge-sharing (r = 2.67) tetrahedral units.
Remarkably, binary group V (P, As) sulfides exhibit IPs that are shifted to
even a lower r than their selenide counterparts; a result that we trace to
excess Sn chains either partially (As-S) or completely (P-S) demixing from
network backbone, in contrast to excess Sen chains forming part of the backbone
in corresponding selenide glasses. In ternary chalcogenides of Ge with the
group V elements (As, P), IPs of the sulfides are similar to their selenide
counterparts, suggesting that presence of Ge serves to reign in the excess Sn
chain fragments back in the backbone as in their selenide counterparts
Coupled Al/Si and O/N order/disorder in BaYb[Si4–xAlxOxN7–x]sialon
The fractions of aluminium, [Al]/[Al + Si], and oxygen, [O]/[O + N], in crystallographically distinct sites of BaYb[Si4–xAlxOxN7–x] oxonitridoaluminosilicate (space group P63mc, No. 186) were refined based on the results of neutron powder diffraction for a synthetic sample with the composition of x = 2.2(2) and simulated as functions of temperature for the compositions x = 2 and x = 2.3 using a combination of static lattice energy calculations (SLEC) and Monte Carlo simulations. The SLEC calcu lations have been performed on a set of 800 structures differing in the distribution of Al/Si and O/N within the 2 × 2 × 2 supercell containing 36 formula units of BaYb[Si4–xAlxOxN7–x]. The SLEC were based on a transferable set of empirical interatomic potentials developed within the present study. The static lattice energies of these structures have been expanded in the basis set of pair-wise ordering energies and on-site chemical potentials. The ordering energies and the chemical potentials have been used to calculate the configuration energies of the oxonitridoaluminosilicates (so-called sialons) using a Monte Carlo algorithm. The simulations suggest that Al and O are distributed unevenly over two non-equivalent T(Si/Al) and three L(N/O) sites, respectively, and the distribution shows strong dependence both on the temperature and the composition. Both simulated samples exhibit order/disorder transitions in the temperature range 500–1000 K to phases with partial long-range order below these temperatures. Above the transition temperatures the Si/Al and N/O distributions are affected by short-range ordering. The predicted site occupancies are in a qualitative agreement with the neutron diffraction results
v-P 2 O 5 micro-clustering in P-doped silica studied by a first-principles Raman investigation
Synthetic vitreous silica is currently the preferred material for the production of optical fibres because of the several excellent properties of this glass, e.g. high transmission in the visible and IR domains, high mechanical strength, chemical durability, and ease of doping with various materials. For instance, fiber lasers and amplifiers exploit the light amplification properties provided by rare-earth ions employed as dopants in the core of silica-based optical fibers. The structure and composition of the nearest neighbor shell surrounding rare-earth ions in silica-based optical fibers and amplifiers have been intensively debated in the last decade. To reduce aggregation effects between rare-earth ions, co-dopants such as phosphorus and aluminium are added as structural modifiers; phosphorus-doping, in particular, has proved to be very efficient in dissolving rare-earth ions. In this work, we provide further insights concerning the embedding of P atoms into the silica network, which may be relevant for explaining the ease of formation of a phosphorus pentoxide nearest-neighbor shell around a rare-earth dopant. In particular, by means of first-principles calculations, we discuss alternative models for an irradiation (UV, x\u2013, \u3b3-rays) induced paramagnetic center, i.e. the so called room-temperature phosphorus-oxygen-hole center, and its precursors. We report that the most likely precursor of a room-temperature phosphorus-oxygen-hole center comprises of a micro-cluster of a few (at least two) neighboring phosphate tetrahedra, and correspondingly that the occurrence of isolated [(O-) 2 P(=O) 2 ] 12 units is unlikely even at low P-doping concentrations. In fact, this work predicts that the symmetric stretching of P=O bonds in isolated [(O-) 2 P(=O) 2 ] 12 units appears as a Raman band at a frequency of ~1110 cm 121 , and only by including at least another corner-sharing phosphate tetrahedron, it is shown to shift to higher frequencies (up to ~40 cm 121 ) due to the shortening of P=O bonds, thereby leading to an improved agreement with the observed Raman band located at ~1145 cm 121
Large quantum fluctuations in the strongly coupled spin-1/2 chains of green dioptase: a hidden message from birds and trees
The green mineral dioptase Cu6Si6O18(H2O)6 has been known since centuries and
plays an important role in esoteric doctrines. In particular, the green
dioptase is supposed to grant the skill to speak with trees and to understand
the language of birds. Armed with natural samples of dioptase, we were able to
unravel the magnetic nature of the mineral (presumably with hidden support from
birds and trees) and show that strong quantum fluctuations can be realized in
an essentially framework-type spin lattice of coupled chains, thus neither
frustration nor low-dimensionality are prerequisites. We present a microscopic
magnetic model for the green dioptase. Based on full-potential DFT
calculations, we find two relevant couplings in this system: an
antiferromagnetic coupling J_c, forming spiral chains along the hexagonal c
axis, and an inter-chain ferromagnetic coupling J_d within structural Cu2O6
dimers. To refine the J_c and J_d values and to confirm the proposed spin
model, we perform quantum Monte-Carlo simulations for the dioptase spin
lattice. The derived magnetic susceptibility, the magnetic ground state, and
the sublattice magnetization are in remarkably good agreement with the
experimental data. The refined model parameters are J_c = 78 K and J_d = -37 K
with J_d/J_c ~ -0.5. Despite the apparent three-dimensional features of the
spin lattice and the lack of frustration, strong quantum fluctuations in the
system are evidenced by a broad maximum in the magnetic susceptibility, a
reduced value of the Neel temperature T_N ~ 15 K >> J_c, and a low value of the
sublattice magnetization m = 0.55 Bohr magneton. All these features should be
ascribed to the low coordination number of 3 that outbalances the
three-dimensional nature of the spin lattice.Comment: Dedicated to Stefan-Ludwig Drechsler on the occasion of his 60th
birthday (9 pages, 6 figures
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