1,958 research outputs found

### Modified kagome physics in the natural spin-1/2 kagome lattice systems - kapellasite Cu3Zn(OH)6Cl2 and haydeeite Cu3Mg(OH)6Cl2

The recently discovered natural minerals Cu3Zn(OH)6Cl2 and Cu3Mg(OH)6Cl2 are
spin 1/2 systems with an ideal kagome geometry. Based on electronic structure
calculations, we develop a realistic model which includes couplings across the
kagome hexagons beyond the original kagome model that are intrinsic in real
kagome materials. Exact diagonalization studies for the derived model reveal a
strong impact of these couplings on the magnetic ground state. Our predictions
could be compared to and supplied with neutron scattering, thermodynamic and
NMR data.Comment: 5 pages, 5 figures, 1 tabl

### Coupled frustrated quantum spin-1/2 chains with orbital order in volborthite Cu3V2O7(OH)2(H2O)2

We present a microscopic magnetic model for the spin-liquid candidate
volborthite Cu3V2O7(OH)2(H2O)2. The essentials of this DFT-based model are (i)
the orbital ordering of Cu(1) 3d 3z2-r2 and Cu(2) 3d 3x2-y2, (ii) three
relevant couplings J_ic, J_1 and J_2, (iii) the ferromagnetic nature of J_1 and
(iv) frustration governed by the next-nearest-neighbor exchange interaction
J_2. Our model implies magnetism of frustrated coupled chains in contrast to
the previously proposed anisotropic kagome model. Exact diagonalization studies
reveal agreement with experiments.Comment: 5 pages, 4 figures + supplementar

### 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

### Intrinsic peculiarities of real material realizations of a spin-1/2 kagome lattice

Spin-1/2 magnets with kagome geometry, being for years a generic object of
theoretical investigations, have few real material realizations. Recently, a
DFT-based microscopic model for two such materials, kapellasite Cu3Zn(OH)6Cl2
and haydeeite Cu3Mg(OH)6Cl2, was presented [O. Janson, J. Richter and H.
Rosner, arXiv:0806.1592]. Here, we focus on the intrinsic properties of real
spin-1/2 kagome materials having influence on the magnetic ground state and the
low-temperature excitations. We find that the values of exchange integrals are
strongly dependent on O--H distance inside the hydroxyl groups, present in most
spin-1/2 kagome compounds up to date. Besides the original kagome model,
considering only the nearest neighbour exchange, we emphasize the crucial role
of the exchange along the diagonals of the kagome lattice.Comment: 4 pages, 4 figures. A paper for the proceedings of the HFM 2008
conferenc

### Magnetism of CuX2 frustrated chains (X = F, Cl, Br): the role of covalency

Periodic and cluster density-functional theory (DFT) calculations, including
DFT+U and hybrid functionals, are applied to study magnetostructural
correlations in spin-1/2 frustrated chain compounds CuX2: CuCl2, CuBr2, and a
fictitious chain structure of CuF2. The nearest-neighbor and second-neighbor
exchange integrals, J1 and J2, are evaluated as a function of the Cu-X-Cu
bridging angle, theta, in the physically relevant range 80-110deg. In the ionic
CuF2, J1 is ferromagnetic for theta smaller 100deg. For larger angles, the
antiferromagnetic superexchange contribution becomes dominant, in accord with
the Goodenough-Kanamori-Anderson rules. However, both CuCl2 and CuBr2 feature
ferromagnetic J1 in the whole angular range studied. This surprising behavior
is ascribed to the increased covalency in the Cl and Br compounds, which
amplifies the contribution from Hund's exchange on the ligand atoms and renders
J1 ferromagnetic. At the same time, the larger spatial extent of X orbitals
enhances the antiferromagnetic J2, which is realized via the long-range
Cu-X-X-Cu paths. Both, periodic and cluster approaches supply a consistent
description of the magnetic behavior which is in good agreement with the
experimental data for CuCl2 and CuBr2. Thus, owing to their simplicity, cluster
calculations have excellent potential to study magnetic correlations in more
involved spin lattices and facilitate application of quantum-chemical methods

### Decorated Shastry-Sutherland lattice in the spin-1/2 magnet CdCu2(BO3)2

We report the microscopic magnetic model for the spin-1/2 Heisenberg system
CdCu2(BO3)2, one of the few quantum magnets showing the 1/2-magnetization
plateau. Recent neutron diffraction experiments on this compound [M. Hase et
al., Phys. Rev. B 80, 104405 (2009)] evidenced long-range magnetic order,
inconsistent with the previously suggested phenomenological magnetic model of
isolated dimers and spin chains. Based on extensive density-functional theory
band structure calculations, exact diagonalizations, quantum Monte Carlo
simulations, third-order perturbation theory, as well as high-field
magnetization measurements, we find that the magnetic properties of CdCu2(BO3)2
are accounted for by a frustrated quasi-2D magnetic model featuring four
inequivalent exchange couplings: the leading antiferromagnetic coupling J_d
within the structural Cu2O6 dimers, two interdimer couplings J_t1 and J_t2,
forming magnetic tetramers, and a ferromagnetic coupling J_it between the
tetramers. Based on comparison to the experimental data, we evaluate the ratios
of the leading couplings J_d : J_t1 : J_t2 : J_it = 1 : 0.20 : 0.45 : -0.30,
with J_d of about 178 K. The inequivalence of J_t1 and J_t2 largely lifts the
frustration and triggers long-range antiferromagnetic ordering. The proposed
model accounts correctly for the different magnetic moments localized on
structurally inequivalent Cu atoms in the ground-state magnetic configuration.
We extensively analyze the magnetic properties of this model, including a
detailed description of the magnetically ordered ground state and its evolution
in magnetic field with particular emphasis on the 1/2-magnetization plateau.
Our results establish remarkable analogies to the Shastry-Sutherland model of
SrCu2(BO3)2, and characterize the closely related CdCu2(BO3)2 as a material
realization for the spin-1/2 decorated anisotropic Shastry-Sutherland lattice.Comment: 16 pages, 13 figures, 2 tables. Published version with additional QMC
dat

### Microscopic magnetic modeling for the $S$=1/2 alternating chain compounds Na$_3$Cu$_2$SbO$_6$ and Na$_2$Cu$_2$TeO$_6$

The spin-1/2 alternating Heisenberg chain system Na$_3$Cu$_2$SbO$_6$ features
two relevant exchange couplings: $J_{1a}$ within the structural Cu$_2$O$_6$
dimers and $J_{1b}$ between the dimers. Motivated by the controversially
discussed nature of $J_{1a}$, we perform extensive density-functional-theory
(DFT) calculations, including DFT+$U$ and hybrid functionals. Fits to the
experimental magnetic susceptibility using high-temperature series expansions
and quantum Monte Carlo simulations yield the optimal parameters $J_{1a}$ =
$-$217 K and $J_{1b}$ = 174 K with the alternation ratio $\alpha =
J_{1a}/J_{1b} \simeq$ $-$1.25. For the closely related system
Na$_2$Cu$_2$TeO$_6$, DFT yields substantially enhanced $J_{1b}$, but weaker
$J_{1a}$. The comparative analysis renders the buckling of the chains as the
key parameter altering the magnetic coupling regime. Numerical simulation of
the dispersion relations of the alternating chain model clarify why both
antiferromagnetic and ferrromagnetic $J_{1a}$ can reproduce the experimental
magnetic susceptibility data.Comment: published version: 11 pages, 8 figures, 5 tables + Supplemental
materia

### Magnetic pyroxenes LiCrGe2O6 and LiCrSi2O6: dimensionality crossover in a non-frustrated S=3/2 Heisenberg model

The magnetism of magnetoelectric $S$ = 3/2 pyroxenes LiCrSi$_2$O$_6$ and
LiCrGe$_2$O$_6$ 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 LiCrSi$_2$O$_6$, two relevant exchange
integrals, $J_1 \simeq$ 9 K along the structural chains and $J_{\text{ic1}}$
$\simeq$ 2 K between the chains, form a 2D anisotropic honeycomb lattice. In
contrast, the spin model of LiCrGe$_2$O$_6$ is constituted of three different
exchange couplings. Surprisingly, the leading exchange $J_{\text{ic1}}$
$\simeq$ 2.3 K operates between the chains, while $J_1$ $\simeq$ 1.2 K is about
two times smaller. The additional interlayer coupling $J_{\text{ic2}}$ $\simeq$
$J_1$ 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

### Crystal water induced switching of magnetically active orbitals in CuCl2

The dehydration of CuCl2*2(H2O) to CuCl2 leads to a dramatic change in
magnetic behavior and ground state. Combining density functional electronic
structure and model calculations with thermodynamical measurements we reveal
the microscopic origin of this unexpected incident -- a crystal water driven
switching of the magnetically active orbitals. This switching results in a
fundamental change of the coupling regime from a three-dimensional
antiferromagnet to a quasi one-dimensional behavior. CuCl2 can be well
described as a frustrated J1-J2 Heisenberg chain with ferromagnetic exchange J1
and J2/J1 ~ -1.5 for which a helical ground state is predicted.Comment: 6 pages, 5 figures, 1 table (PRB, accepted

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