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text:
\section{Introduction}

Magnetic and semiconducting manganese sulphides attracted attention of solid
state chemists since the early days of X-ray crystallography and magnetic
structure investigations$^{1-5}$ done on haurite (MnS$_{2})$ and alabandite
(MnS). They exhibit high magnetic moments due to the coordination of
Mn$^{2+}$ in MnS$_{6}$ octahedra where it prefers a high spin state with
five unpaired electrons. However, MnS$_{2}$ has been discussed as a rare
example of a high spin to low spin transition under high pressure$^{6, 7}$.

In the past few years the chemistry of magnetic manganese materials was
enriched by fascinating discoveries mainly on multinary manganese oxides$^{6-8}$.
Properties like the giant and colossal magnetoresistance (GMR, CMR)
inspired new fields of research on magnetic semiconductors. Besides
promising technological applications and experimental challenges there is an
increasing demand and success of theoretical understanding of the underlying
chemical bonding and electronic properties. The development and application
of effective density functional (DFT) methods within the local spin density
approximation (LSDA) still plays an increasing role herein$^{9-11}$.

Fascinating properties were also discovered on manganese chalcogenides. MnS
and MnS$_{2}$ show antiferromagnetic ordering while diluted magnetic semiconductors
(DMS) based on MnS exhibit outstanding properties related to spintronic applications$^{12-14}$.
Multinary materials like MnCr$_{2}$S$_{4}$ provide additional potential with respect to
anisotropic resistivity and magnetic properties$^{15,16}$.

Due to its reduced dimensionality MnSb$_{2}$S$_{4}$ serves as a promising
low dimensional magnetic semiconducting material. Contrary to spinel type
MnCr$_{2}$S$_{4}$ with Mn$^{2+}$ in MnS$_{4}$ tetrahedra one finds MnS$_{6}$
octahedra in MnSb$_{2}$S$_{4}$. Therein, it is related to MnS and MnS$_{2}$ as
well as in the observation of phase transitions. Orthorhombic MnSb$_{2}$S$_{4}$
is accessible by hydrothermal synthesis and was earlier shown$^{17}$ to be isotypic to FeSb$_{2}$S$_{4}$ which is an
antiferromagnetic material$^{18}$. Recently a new monoclinic modification
(\textit{mC28}) of MnSb$_{2}$S$_{4}$ was synthesized by high temperature methods$^{19}$.
MnSb$_{2}$S$_{4}$ (\textit{mC28}) can be transformed reversibly into the orthorhombic
modification (\textit{oP28}) at high pressure$^{20}$. By electrical conductivity and
magnetic susceptibility measurements it was found that MnSb$_{2}$S$_{4}$ (\textit{mC28}) is
a semiconducting antiferromagnet with $T_{N}$ = 26.5 K and an electronic band
gap of 0.77 eV$^{19,20}$. Concerning the bonding situation one faces 1D
magnetic interactions, as well as bonds with and within the
[$SbS_{3}]^{3-}$ ligand network that is related to Sb$_{2}$S$_{3}$ $^{24}$.
However, no theoretical investigations are reported yet. Considering
MnS and MnS$_{2}$ again as prominent examples, LSDA calculations$^{21-23}$
achieved good agreement with experimental results, {\it i.e.} the prediction of
semiconducting and magnetic ground states with moments around 4.5 \textit{$\mu $}$_{B}$ for
Mn$^{2+}$. For $\alpha $-MnS the antiferromagnetic ground state was correctly found$^{21,22}$.
LSDA total energy calculations on MnS$_{2}$ supported the possibility of a
low spin/high spin phase transition for a compressed cell$^{22}$.

To discuss the differences and relations of the bonding, spin states and
magnetic ordering in \textit{mC28} and \textit{oP28} MnSb$_{2}$S$_{4}$ first principles
calculations are subsequently reported modelling non magnetic (NM), ferromagnetic (FM),
ferrimagnetic (FIM for the monoclinic system) and antiferromagnetic (AFM) structures in order to identify the ground state configuration. The applied augmented spherical wave (ASW) method was successfully used in
previous calculations on magnetic semiconducting manganites$^{11}$. The
crystal structures, computational details, and results of the calculations
on non-magnetic, ferromagnetic, and antiferromagnetic configurations are
presented, as well as electronic band structures, site projected densities
of states and chemical bonding characteristics.

\section{Crystal structures of orthorhombic and monoclinic phases}
For the calculations presented herein, the crystal structures of both
MnSb$_{2}$S$_{4}$ modifications as determined by single crystal X-ray
diffraction were taken as the starting points$^{17,19,20}$. The space groups and the
relevant lattice parameters used in the calculation are given in the first part of Table 1.
Both modifications are based on chains of edge-sharing MnS$_{6}$ octahedra (Fig. 1). These
chains of octahedra are linked by [$SbS_{3}]^{3-}$ units to form
layers in the case of MnSb$_{2}$S$_{4}$ (\textit{mC28}) and a three dimensional (3D)
network in the case of MnSb$_{2}$S$_{4}$ (\textit{oP28}).

The Sb-S bonds determine both the structural anisotropies and the
differences between the modifications. Sb atoms exhibit a 3+2+$x$ ($x$ = 1, 2)
coordination with three Sb-S bonds of about 2.5 {\AA} and two Sb-S bonds
between 2.9 and 3.1 {\AA} (``secondary bonds''). In addition, there are
so-called non bonding distances 3.1 {\AA}$<d$(Sb-S) $<$ 4 {\AA}. Distinguishing
these three types of Sb-S interactions we find all short Sb-S bonds linking
edge sharing MnS$_{6}$-octahedra of one chain in MnSb$_{2}$S$_{4}$ (\textit{mC28}).
Slightly longer bonds link the octahedra to form a layered structure (Fig. 1).
Between the layers (along the $c$ axis) only so-called non-bonding Sb-S
distances are found. In the case of MnSb$_{2}$S$_{4}$ (\textit{oP28}) one finds double
chains of octahedra which are interlinked by short and secondary Sb-S bonds.
These double chains form a kind of fishbone scheme and non-bonding
Sb-S distances between them result in a 3D network. The density of the title
compound increases from 4.24 g/cm$^{3}$ (\textit{mC28})$^{19}$ to 4.51 g/cm$^{3}$
(\textit{oP28}) $^{17}$, showing that the orthorhombic modification is the high pressure
form. The distances $d$(Mn-S) vary from around 2.6 \AA~  (Table 1) in both
modifications. Thus, they show a slightly broader range than in the pure
manganese sulphides with octahedral coordination of manganese, {\it i.e.},
$d$(Mn-S) = 2.61 {\AA} in $\alpha $-MnS $^{2}$ and $d$(Mn-S) = 2.59 {\AA} in
MnS$_{2}$ $^{1}$. There are two different Mn positions in MnSb$_{2}$S$_{4}$
(\textit{mC28}), with a higher site symmetry than the single Mn position in
MnSb$_{2}$S$_{4}$ (\textit{oP28}). The distortions of the MnS$_{6}$ octahedra are due to
the structural anisotropy imposed by the [$SbS_{3}]^{3-}$ units. They result in tetragonally
distorted MnS$_{6}$ octahedra with a coordination number of 2+4 in (\textit{mC28}) MnSb$_{2}$S$_{4}$
 and a coordination number of 1+1+2+2 in MnSb$_{2}$S$_{4}$ (\textit{oP28}),
respectively. Further details are provided in refs.$^{17,19}$.

Considering the magnetic coupling of manganese in the two polymorphs of
MnSb$_{2}$S$_{4}$ the structural anisotropy provided by the MnS$_{6}$ chains
has to be kept in mind. Thus, only two contacts $d$(Mn-Mn) $\approx $ 3.8 {\AA}
are present in the title compound, and all other distances between Mn atoms
are larger than 6 {\AA}. This situation is quite different from the isotropic Mn
sublattices of, e.g., $\alpha $-MnS (12 x $d$(Mn-Mn) $\approx $ 3.7 {\AA}), and
MnS$_{2}$ (12 x $d$(Mn-Mn) $\approx $ 4.3 {\AA}). This allows to investigate FM
models with equal Mn spin directions and AFM models with alternating Mn
spins along the chains in MnSb$_{2}$S$_{4}$.

\section{Computational framework}
The electronic properties have been self-consistently calculated in the
framework of the density functional theory DFT$^{25,26}$ using the ASW method
as implemented by Williams {\it et al.}$^{27}$ and Eyert$^{28}$. The effects of
exchange and correlation were parameterized according to the local spin density
approximation (LSDA) scheme of Vosko, Wilk and Nusair$^{29}$.
All valence electrons, including 4$d$(Sb) ones, were treated as band states.
In the minimum ASW basis set, we chose the outermost shells to represent
the valence states and the matrix elements were constructed using partial waves
up to $l_{max.}$ = 2 quantum number. The ASW method uses the atomic sphere approximation
(ASA) which assumes overlapping spheres centered on the atomic sites where the
potential has a spherical symmetry. In order to represent the correct shape of the
crystal potential in the large voids of the respective crystal structures, additional
augmentation spheres were inserted$^{28}$ to avoid an otherwise too large overlap
between the actual atomic spheres.

The calculations implicit of zero entropy ($T$ = 0 K) were started assuming a
non-magnetic configuration which is non spin polarized (NSP) meaning that spin
degeneracy was enforced for all species (atoms and empty spheres). Note that this configuration does not translate a paramagnetic state which
would actually require a supercell with different orientations of the spins over the crystal sites.
In a second step spin polarized (SP) calculations were performed by initially
allowing for differing spin occupations, $i.e.$, majority (spin up $\uparrow $)
and minority (spin down $\downarrow $) spins for all atomic species.
The occupancies were self-consistently changed until convergence of the
total energy ($\Delta$E$\leq$~10$^{-6}$ Ry.) and of the charges ($\Delta$Q$\leq$~10$^{-6}$) between two subsequent iterations was reached. For that a sufficiently large number of $k$ points was used with respect to selfconsistancy of the results. In view of the large cells especially when symmetry is broken by introducing the antiferromagnetic orderings, we used up to 12*12*12, {\it i.e.}\ 1728 points to produce respectively 216 and 468 {\it k} points in the irreducible wedges of the orthorhombic and monoclinic Brillouin zones.
Calculations are implicit of collinear magnetic structures. However non-collinear magnetic structures can occur in manganese based compounds such as in the nitride Mn$_{4}$N which was studied in the same calculational framework$^{30}$. In fact such heavy calculations could be achieved with great accuracy in energy differences between the magnetic configurations provided one considers high symmetry structures such as that of cubic anti-perovskite Mn$_{4}$N.
When one magnetic/crystallographic sublattice of all species
is accounted for, a ferromagnetic order (FM) is described. Two magnetic
sublattices need to be accounted for to calculate the AFM configurations.
This can be achieved by symmetry breaking of the system, half of the
constituents being ``spin up'' and the other half being ``spin down''. This
approach accounts for the effect of low spin and high spin Mn$^{2+}$ and
spin spin interactions in AFM and FM models for MnSb$_{2}$S$_{4}$ similar to
the incommensurate magnetic structure of FeSb$_{2}$S$_{4}$$^{18}$. Indeed,
spin reorientation, spin disorder, and the competition between AFM and FM
orientation are discussed to play an important role in magnetic systems. We
are aware of the fact that our models do not simulate spin dynamics.
However, any spin spin interaction as for example in the incommensurate AFM
structure of FeSb$_{2}$S$_{4}$ has to be expected between the states given
by the AFM, FM and NM models.
Considering  the orthorhombic structure which has four MnSb$_{2}$S$_{4}$ formula units, two AFM configurations were accounted for, {\it i.e.} with the spin aligned oppositely in MnS$_{6}$ octahedral chains, this will be called hereafter AFM1 and another one with spins aligned parallel within a chain and oppositely between chains (AFM2).
As for the monoclinic variety, the unit cell has two different manganese sites Mn1 and Mn2. This leads to a first possibility which is to account for antiparallel spin alignment between Mn1 and Mn2 sites leading to a ferrimagnetic (FIM) order. The other possibility is to double the cell along the third lattice vector c with Mn1 and Mn2 all up-$\uparrow$ in the first cell and Mn1 and Mn2 all down-$\downarrow$ in second cell, {\it i.e.} conforming with the spin spiral found  for MnSb$_{2}$S$_{4}$ (\textit{mC28})$^{31}$. Needless to say that  the symmetry breaking due to the magnetic lattice orderings among Mn($\uparrow$) and Mn($\downarrow$) in both structures computations are much heavier to carry out whence the limitation in the Brillouin zone integration in {\it k} points presented above.

Further  information about the nature of the interaction between atomic constituents can be provided using overlap population (OP) leading to the so-called COOP (crystal orbital overlap population)$^{32}$ or alternatively introducing the Hamiltonian based population COHP (crystal orbital Hamiltonian population)$^{33}$. Both approaches lead to a qualitative description of the chemical interactions between two atomic species by assigning a bonding, non-bonding or antibonding character.  A
slight refinement of the COHP was recently proposed in form of the ``covalent bond energy'' E$_{COV}$  which combines both COHP and COOP so as to make the resulting quantity independent of the choice of the zero of potential$^{34}$. The E$_{COV }$ was recently implemented within the ASW method$^{35}$. Our experience with both COOP and E$_{COV}$ shows that they give similar general trends although COOP exagerate the magnitude of antibonding states. We shall be using the E$_{COV}$ description of the chemical bonding.

\section{Calculation results and discussion}
\subsection{Total energy and magnetic moments}
Charge transfer is observed from Mn towards Sb, S and the empty spheres; nonetheless its amount is not significant in terms of an ionic description (such as Mn$^{2+}$), which is rarely observed in the framework of such calculations. A more meaningful picture is provided from the quantum mixing of the valence states as it will be shown in the plots of the density of states (DOS) and the chemical bonding (E$_{COV}$) in next sections.
The two polymorphs show similar trends concerning the total energy
calculated for the non magnetic (NM) and spin polarized (SP) ferromagnetic -FM-  and antiferromagnetic -AFM- models. Further ferrimagnetic calculations in the monoclinic system were carried out.  This is detailed in table 1 which presents the results obtained after self consistent computations for the different magnetic configurations considered. For both modifications the FM state is favored with respect to the non magnetic one. The large gain in energy arises from the magnetic exchange of coupled high spin Mn$^{2+}$ when spin polarization is accounted for. In FM configuration the resulting total magnetization per formula unit is close to 5 $\mu_B$. For formally Mn$^{2+}$ two configurations are possible for the spin arrangements within the octahedral field of sulphur: A high spin -HS- configuration $t_{2g}^{3}$, $e_{g}^{2}$ with 5 unpaired spins and a low spin -LS- one: $t_{2g}^{5}$, $e_{g}^{0}$ resulting in only one unpaired spin. From this it can be suggested that at least in the ferromagnetic state divalent manganese is HS. However the total magnetization arises from all constituents of the lattice (Table 1) with the main contribution due to manganese. The SP-FM Mn moment amounts to 4.38 $\mu_B$ within (\textit{oP28}) MnSb$_{2}$S$_{4}$ and 4.23 \textit{$\mu$}$_{B}$ for (\textit{mC28}) MnSb$_{2}$S$_{4}$. This agrees with the value calculated for Mn$^{2+}$ in MnTe$^{21}$ and lies in the range of further LSDA results on high spin Mn$^{2+}$ from 4.3 to 4.6  \textit{$\mu $}$_{B}$$^{21-23}$. When the ferrimagnetic configuration is accounted for within the monoclinic variety a further stabilization is obtained and there is a cancelling out between moments so that  total magnetization is zero. The AFM configurations show a further energy lowering for both varieties with a smaller energy difference in the orthorhombic structure. This would suggest a lower N\'eel temperature for the high pressure orthorhombic variety. Within this structure the AFM1 configuration with the spins aligned oppositely in MnS$_{6}$ octahedral chains is found to be favored with respect to the AFM2 one ({\it i.e.} with spins aligned parallel within a chain and oppositely between chains). The small lowering in the moment carried by Mn$^{2+}$ (4.34 \textit{$\mu $}$_{B})$ agrees with the value observed for $\alpha $-MnS (4.1 \textit{$\mu $}$_{B}$)$^{22}$. For MnSb$_{2}$S$_{4}$ (\textit{mC28}) we find the same order of energies. Thus, the applied method predicts the preference of an antiparallel coupling of the spins of Mn-$d$ electrons in a high spin state against a parallel coupling. The close magnitudes of the moments between the FM and the AFM configurations lead to propose that the magnetic order might be Heisenberg-like whereby the magnetic susceptibility should obey a Bonner-Fischer behavior$^{36}$ which is characteristic to linear spin chains.

\subsection{Non-spin polarized calculation DOS and chemical bonding}
The suggested NSP situation for MnSb$_{2}$S$_{4}$ (\textit{oP28}) and (\textit{mC28}) results in a metallic behavior, analogous to studies on MnS and MnS$_{2}$$^{20-22}$. The site projected DOS are shown in fig. 2 a and b. The highest occupied states cross the Fermi level $E_{F}$ at a high density of states which is attributed to t$_{2g}$ states from a crystal field analysis of Mn $d$ states projections given in fig. 2c. These Mn$^{2+}$ $t_{2g}$ states are only partly occupied by five electrons. The next bands above $E_{F}$ are formed by the Mn $e_{g}$-states (fig. 2c). The splitting of the $e_{g}$ states results from deviations of the MnS$_{6}$-groups from octahedral symmetry. Antimony and sulphur $p$-states form broad bonding states with the metal states in the energy range [-6,- 1eV] (see next paragraph). The DOS at low energies are $s$-bands of Sb (-10 eV) and S (-15 eV); the latter are found at lower energy due to the higher electronegativity of sulphur as compared to antimony.

The chemical bonding within both orthorhombic and monoclinic MnSb$_{2}$S$_{4}$ are examined in the framework of the E$_{COV}$$^{34,35}$ for Mn-S, Mn-Sb and Sb-S pair interactions. The corresponding covalent bond energy E$_{COV}$ plots are given in fig. 3 a and b. Negative, positive and nil E$_{COV}$ magnitudes are relevant to bonding, antibonding and non-bonding characteristics. From this the major part of the valence band VB is bonding due to Mn-S interactions as well as to Sb-S albeit with a smaller magnitude; this contributes to the stabilization of the crystal lattice. The Sb-S interaction is observed with smaller magnitude and it remains bonding within the conduction band above E$_{F}$. This somehow provides an illustration for the description of the bonding given in the crystal structure section above. Mn-Sb interaction plays little role -as with respect to Mn-S one- within the major range of the VB.  At the top of the VB the system becomes largely destabilized as the Fermi level is reached, {\it i.e.} where  a large Mn-S E$_{COV}$ as well as Mn-Sb antibonding interactions with smaller magnitude can be observed.  Although a large part of the Mn(t$_{2g}$) are not engaged into Mn-S antibonding interaction in asfar as they are responsible for the onset of the Mn magnetic moment, the non magnetic configuration is clearly not favored from that. Lastly Mn-Mn interaction were observed too but with a much smaller magnitudes than all other explicited ones in both crystal varieties, so they are not shown here. Nevertheless it will be discussed below that these bonds can have consequences on the electronic structure (cf. section III.C particularly for the monoclinic band structures).

\subsection{The electronic structure of spin polarized MnSb$_{2}$S$_{4}$ }
\subsubsection{Ferromagnetic state}
As shown by the site projected DOS in figs. 4  a  and  b, the spin polarization causes Mn 3$d$ levels to split into majority spin ($\uparrow $) states which are lowered in energy relative to minority spin ($\downarrow $) states at higher energy. Majority Mn $d$ spin states completely lie below $E_{F}$, thus being fully occupied by 5 electrons. The minority Mn $d$ states are found above $E_{F}$ thus being completely empty. This indicates a closely non metallic situation with a small energy  gap in the orthorhombic variety which reduces to a closing in (\textit{mC28}) MnSb$_{2}$S$_{4}$. The DOS for manganese in both varieties exhibit peaks which closely resemble the $t_{2g}(\uparrow$)-$e_{g}(\uparrow $) manifolds. Thus, the highest occupied states in the valence band are formed by Mn up spin $e_{g}$ states and the lowest unoccupied ones by down spin $t_{2g}$ states. Concerning Sb and S DOS the latter can be observed to closely follow the shape of Mn pointing to the Mn-S coordination, {\it i.e.} with  MnS$_{6}$ octahedra within which the major part of the bonding within the lattice occurs as discussed above. Spin polarization mainly affects Mn states so that there is hardly any energy shift between ($\uparrow $) and ($\downarrow $) spin populations for Sb and S although residual moments were computed in both orthorhombic and monoclinic systems (Table 1).

\subsubsection{Ferrimagnetic (FIM) model in  MnSb$_{2}$S$_{4}$(\textit{mC28}) } A first possibility to account for antiparallel spin alignment within (\textit{mC28}) MnSb$_{2}$S$_{4}$ was to allow for it between the two singly occupied Mn sublattices within the base centered monoclinic structure. The resulting energy differences shown in Table 1 are found in favor of this FIM configuration by 13.3 meV with respect to FM. The magnitudes of the moments are within range of FM calculations but the resulting magnetization is zero. The DOS and band structure given in fig. 5 a and b respectively. The DOS plot  shows some similar features to FM (fig. 4b)  but there is now a gap opening  in the minority spins whereas a metallic behaviour is observed for majority spins. From the band structure plot in the same energy window the gap of $\sim$0.6 eV can be observed between the VB and the CB  in U(A-E) direction which is along the $k_z$ axis of the monoclinic Brillouin zone. It is along this direction that the metallic behavior is obtained too as resulting from  the crossing of single bands from the VB and the CB due to a large dispersion. Thus the monoclinic system, in an intermediate magnetic state (see relative energies in Table 1), is not a semiconductor but a half-metallic ferrimagnet with a relatively low DOS at E$_{F}$ due to single band crossing.

\subsubsection{Antiferromagnetic (AFM) models}
For all systems the energy differences shown in Table 1 are in favor of AFM ground state configurations (AFM1 for \textit{oP28}). The  result of enforced AF configuration is that the total up spin and down spin projected densities of states present the same contributions. As a consequence plots for one magnetic sublattice within each structure will be shown. In a narrow energy window around the Fermi level meant to exhibit the relevant features of the AFM ground state, figs. 6 and  7  give the DOS and band structure for orthorhombic and monoclinic AFM MnSb$_{2}$S$_{4}$ respectively.
The MnSb$_{2}$S$_{4}$ (\textit{oP28}) projected DOS (fig. 6) show a larger splitting around E$_{F}$ than in the FM DOS (fig. 4a). The larger gap is likely to arise from a shift of unoccupied minority Mn states to higher energies within the CB which can be a result of Mn-Mn interactions throughout the MnS$_{6}$ chains.  From fig. 6b showing the band structure its magnitude amounts to $\sim$~0.7 eV between $\Gamma$$_{VB}$ and $\Gamma$$_{CB}$ for instance in the orthorhombic Brillouin zone.  This results in a nonconducting state. Note that this gap for the AFM state is close to the experimental value of 0.77 eV$^{20}$.  Our calculations indicate the preference of an AFM configuration (AFM1, cf. energy differences in table 1) based on a simple model of alternating Mn moments along the rods. This is somehow similar to the $\alpha $-MnS case examined by Tappero {\it et al.}$^{23}$.

AFM ground state site projected DOS of  MnSb$_{2}$S$_{4}$(\textit{mC28}) (fig. 7) show different features from the ferrimagnetic case (fig. 5a) because both Mn1 and Mn2 are now polarized up or down within a magnetic sublattice (see for instance the change of orientation of Mn1 and Mn2 DOS above E$_{F}$); this results in larger $n(E_{F})$. In termes of band structure (fig. 7b) this involves enhanced band crossing along AE direction (along $k_z$ direction) as it can be observed from the confrontation with the ferrimagnetic band structure (fig. 5b). From such a band dispersion and crossing the system is obtained as weakly metallic. This is somehow opposed to the semiconducting state proposed experimentally. Nevertheless both monoclinic and orthorhombic varieties have been shown to possess similar features and the final answer on the question for the coupling of the magnetic moments will be given by neutron diffraction. Related investigations are in progress$^{31}$.

\section{Conclusion}

The electronic structure of MnSb$_{2}$S$_{4}$ in both, the orthorhombic
and the monoclinic modifications were calculated within the
local spin approximation for non magnetic as well as for spinpolarized
ferromagnetic, ferrimagnetic and antiferromagnetic models.
According to total energy calculations the spin polarized states with high
spin Mn$^{2+}$ are largely preferred to a non spin polarized one (Table 1).
Magnetic moments of $\sim$4.3 \textit{$\mu $}$_{B}$ are calculated in
agreement with high spin Mn$^{2+}$ configuration known from MnS and
MnS$_{2}$. For both MnSb$_{2}$S$_{4}$ varieties the AFM model shows
an additional energy gain, thus becoming the ground state. These results
are accompanied by significant differences in the electronic structures
of the models. The NSP model leads to a metallic behavior for both modifications
with a partly filled VB formed by Mn $t_{2g}$ and the CB by the empty Mn $e_{g}$
bands shown by a crystal field analysis. In the orthorhombic system FM and AFM
models lead to the experimentally observed semiconducting characteristics
with a larger gap obtained for the AFM ground state. Differences in the electronic
structures concerning the CB and the VB are due to the crystal structures.
Calculations for MnSb$_{2}$S$_{4}$ (\textit{oP28}) reveal a
band gap of 0.7 eV, close to the experimental value of 0.77 eV.
In  MnSb$_{2}$S$_{4}$(\textit{mC28})  two Mn sites are
present which have a significantly different environment by sulphur and
therefore the site projected DOS for Mn shows a broadening, hence the VB is
broadened too in comparison to the orthorhombic modification. On the other hand,
the empty minority spin Mn $d$ states in the conduction band are sharper for
the monoclinic modification. This is related to the higher local symmetry at
the Mn sites. The computed intermediate ferrimagnetic state exhibits a half metallic
behavior due to single Mn bands crossing along the AE direction in the Brillouin zone,
{\it i.e. } along $k_z$. This is enhanced in the  AFM ground state. Although the
antiferromagnetic nature of the ground state of both
modifications of MnSb$_{2}$S$_{4}$ becomes evident by the present
calculations, further investigations of electrical conductivity to reveal the semiconducting
properties are needed, they are underway.

\begin{acknowledgments}
Computational facilities were provided within the intensive numerical simulation
facilities network M3PEC of the University Bordeaux 1, partly financed by
the {\it Conseil R\'egional d'Aquitaine}.
Support from the Deutsche
Forschungsgemeinschaft (DFG) through Sonderforschungsbereich 484 is equally acknowledged.
\end{acknowledgments}

redpajama_set_name: RedPajamaArXiv


Since my first post of 2018 there hasn't been much activity on Aliciouslog. As in, I literally haven't published a single post on this blog. Well, this is about to change. Drumroll, please!Whilst I have been really active on social media, mostly Instagram (I now have more than 1,000 followers!!!), I haven't deemed my posts complete enough to post (whatever this means). Mind you, a whole array of posts on different topics, ranging from hiking in Mallorca to my vegan guides to Melbourne and Sydney, have been sitting in my draft folder.
Why I didn't just hit the button and send my texts and pictures out into the world? I don't know.
Also, then came the new EU data privacy law which resulted in some extra admin work on my blog that I wasn't exactly happy to implement immediately as it required some deep reading and understanding of details I wasn't completely familiar with.
Now, Aliciouslog is up and running again. We're done hibernating and ready to roll.
I am not yet sure how often and regularly I'll be posting in the future but I aim on keeping Tuesdays for travel-related content and Fridays for food.
Food will still be mostly simple vegan meals you'll be able to prepare with minimum effort and equipment (such as in a hostel kitchen or an ill-equipped Airbnb apartment).
Needless to say, I'll also share the vegan delicacies I come across whilst being out and about and my favourite places to re-stock my energy.
My travel section will definitely have an even stronger focus on the outdoors and I'll regularly be posting hikes most of which won't require any special skills or gear.
Because I strongly believe that we don't need any more complicated how-tos in our life and because I always strive for simple, yet brilliant.
Let me know in the comments what you think! Is there anything you would especially like covered?
It's so great to see you back!! I can't wait for the posts (especially the vegan guides because melbourne is on my have-to-visit-very-soon-list!).
Thank you, Bianca <3 You will definitely love Melbourne and my post (which is going live very soon) will only foster your wish to travel there. It's awesome. I would move there immediately if I could get a visa.


2. MidnightMidnight is the transition time period from one day to the next: the moment when the date changes. In the Roman time system, midnight was halfway between sunset and sunrise, varying according to the seasons. Solar midnight is that time opposite of solar noon, when the sun is closest to nadir and the night is equidistant from dusk and dawn.


text:
Q: Remove Alpha numeric from string in MS Access or SQL I have a column with street addresses in MS Access. I need to remove the "st", "nd", "rd", and "th" from the e.g., 21st, 32nd, 33rd, 44th... and keep the numbers...
Any ideas how can I do this?
Thanks!

A: The Val() function could be useful here.  It will read digits from a string until it encounters a character which it doesn't recognize as part of a number.  See the help topic for more details.
? Val("21st")
 21
? Val("32nd")
 32
? Val("33rd")
 33
? Val("44th")
 44

redpajama_set_name: RedPajamaStackExchange


This Bandana Scarf Black can veritably be called the tuxedo of tube bandanas. With its jet-black color it looks both distinguished and mysterious, but also adventurous and dangerous. James Bond could have been wearing this multifunctional headwear with pleasure during one of his adventures.
Fortunately, this amazing bandana scarf is also available for you. You can wear it in various ways during all kinds of outdoor sports. It is easy to combine with ski- or motorcycle goggles and /or a helmet, hat or beanie.


text:
using namespace mlir;

namespace {

// TODO(andydavis) Add common surrounding loop depth-wise dependence checks.
/// Checks dependences between all pairs of memref accesses in a Function.
struct TestMemRefDependenceCheck
    : public FunctionPass<TestMemRefDependenceCheck> {
  SmallVector<Operation *, 4> loadsAndStores;
  void runOnFunction() override;
};

} // end anonymous namespace

std::unique_ptr<OpPassBase<FuncOp>>
mlir::createTestMemRefDependenceCheckPass() {
  return std::make_unique<TestMemRefDependenceCheck>();
}

// Returns a result string which represents the direction vector (if there was
// a dependence), returns the string "false" otherwise.
static std::string
getDirectionVectorStr(bool ret, unsigned numCommonLoops, unsigned loopNestDepth,
                      ArrayRef<DependenceComponent> dependenceComponents) {
  if (!ret)
    return "false";
  if (dependenceComponents.empty() || loopNestDepth > numCommonLoops)
    return "true";
  std::string result;
  for (unsigned i = 0, e = dependenceComponents.size(); i < e; ++i) {
    std::string lbStr = "-inf";
    if (dependenceComponents[i].lb.hasValue() &&
        dependenceComponents[i].lb.getValue() !=
            std::numeric_limits<int64_t>::min())
      lbStr = std::to_string(dependenceComponents[i].lb.getValue());

    std::string ubStr = "+inf";
    if (dependenceComponents[i].ub.hasValue() &&
        dependenceComponents[i].ub.getValue() !=
            std::numeric_limits<int64_t>::max())
      ubStr = std::to_string(dependenceComponents[i].ub.getValue());

    result += "[" + lbStr + ", " + ubStr + "]";
  }
  return result;
}

// For each access in 'loadsAndStores', runs a dependence check between this
// "source" access and all subsequent "destination" accesses in
// 'loadsAndStores'. Emits the result of the dependence check as a note with
// the source access.
static void checkDependences(ArrayRef<Operation *> loadsAndStores) {
  for (unsigned i = 0, e = loadsAndStores.size(); i < e; ++i) {
    auto *srcOpInst = loadsAndStores[i];
    MemRefAccess srcAccess(srcOpInst);
    for (unsigned j = 0; j < e; ++j) {
      auto *dstOpInst = loadsAndStores[j];
      MemRefAccess dstAccess(dstOpInst);

      unsigned numCommonLoops =
          getNumCommonSurroundingLoops(*srcOpInst, *dstOpInst);
      for (unsigned d = 1; d <= numCommonLoops + 1; ++d) {
        FlatAffineConstraints dependenceConstraints;
        llvm::SmallVector<DependenceComponent, 2> dependenceComponents;
        DependenceResult result = checkMemrefAccessDependence(
            srcAccess, dstAccess, d, &dependenceConstraints,
            &dependenceComponents);
        assert(result.value != DependenceResult::Failure);
        bool ret = hasDependence(result);
        // TODO(andydavis) Print dependence type (i.e. RAW, etc) and print
        // distance vectors as: ([2, 3], [0, 10]). Also, shorten distance
        // vectors from ([1, 1], [3, 3]) to (1, 3).
        srcOpInst->emitRemark("dependence from ")
            << i << " to " << j << " at depth " << d << " = "
            << getDirectionVectorStr(ret, numCommonLoops, d,
                                     dependenceComponents);
      }
    }
  }
}

// Walks the Function 'f' adding load and store ops to 'loadsAndStores'.
// Runs pair-wise dependence checks.
void TestMemRefDependenceCheck::runOnFunction() {
  // Collect the loads and stores within the function.
  loadsAndStores.clear();
  getFunction().walk([&](Operation *op) {
    if (isa<AffineLoadOp>(op) || isa<AffineStoreOp>(op))
      loadsAndStores.push_back(op);
  });

  checkDependences(loadsAndStores);
}

static PassRegistration<TestMemRefDependenceCheck>
    pass("test-memref-dependence-check",
         "Checks dependences between all pairs of memref accesses.");

redpajama_set_name: RedPajamaGithub


text:
Home Link of the Day Blog Domestic Violence Frequently Asked Questions
Domestic Violence Frequently Asked Questions
October is Domestic Violence Awareness Month (DVAM), and here on Christian Feminism Today we are featuring a variety of links about this important topic.
Learn answers to questions that many people have about domestic violence including:
Do abusers show any potential warning signs?
Is it possible for abusers to change?
Why do victims sometimes return to or stay with abusers?
Learn answers to these questions and many more on the National Network to End Domestic Violence website.
Rev. Dr. Christy Gunter
https://drchristysim.wordpress.com/
Christy graduated from St. Paul's School of Theology in Kansas with a doctorate in Global Health and Wholeness. Her main area of research was in healing after domestic violence, and her dissertation was titled Body, Theology, and Intimate Partner Violence: Healing Fragmentation through Spiritual Play. She also holds an M.Div. from Nazarene Theological Seminary in Kansas City and is listed in the Scientific Reviewer and Adviser database for the Center for Disease Control and Prevention (CDC) as an expert in Domestic Violence, Sexual Assault, and Teen Dating Violence. In June, 2018, she helped organize the "For Such a Time as This Rally," speaking outside the Southern Baptist Convention annual meeting, encouraging pastors and ministry leaders to respond to domestic violence and sexual assault in trauma-informed and survivor-centered ways. Her new book Survivor Care: What Religious Professionals Need to Know about Healing Traumacame out in spring 2019 (Wesley Foundry Books).
Behind the Scenes Theodicy: Three Stories of Why It Happened
An Interview with Ashley Easter
Redemption from Biblical Battering: Your Path to Faith-Based Freedom
Survivor Care: What Religious Professionals Need to Know About Healing Trauma

redpajama_set_name: RedPajamaCommonCrawl


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text:
Powerhouse on the market
Austadiums | Wednesday 4th December 2002
After eleven years and a number of renewals, electrical accessories brand Clipsal has decided not to renew its naming rights sponsorship of the Clipsal Powerhouse when the existing deal expires on December 31, 2002. Clipsal will remain as a corporate sponsor of the Adelaide Pura Milk 36ers.
The move means the 36ers have placed that naming rights package for the stadium on the market. Mark Robinson, marketing and operations manager for the club, told On Sport that the package consists of a variety of benefits including internal and external stadium signage, logo placement on the 36ers home & away playing uniform, corporate hospitality and other branding opportunities.
The venue, which is owned and operated by the Basketball Association of South Australia, is Adelaide's largest indoor sporting arena with a seating capacity of 7,500 and boasting 3 basketball courts, fully contained catering facilities, on site parking and several function rooms. Robinson indicated that discussions are currently underway with a number of prospects and whilst confirmation of a new sponsor by January 1 would probably be unlikely, they expect to secure a deal before the end of the current NBL Season.
Robinson did not provide a range of what they are asking for the naming rights but did say the property was very cost effective in comparison to similar stadia. Sources indicate the price would be around the $400-500K mark per year.
copyright � 2002 pando Publishing
On Sport Newsletter is a weekly subscriber only news service for sport administrators and professionals. For further information contact 02 9281 6355 or visit www.onsport.com.au
Titanium Security Arena
Rebranded Australian Sports Museum to open February
Sport and Stadiums rally for Bushfire Relief
$51m Concord Oval redevelopment approved
Countdown on to North Queensland Stadium opening


Could the 3DS be underpriced?
When Nintendo announced the price of the 3DS, jaws dropped. 25,000 Yen converts, as you undoubtedly know by now, to just under $300 -- a figure the gaming world howled was too high. Many gamers initially assumed the system would carry the same price tag when it hit the states, and the outrage increased. Analysts and industry observers predicted (after currency conversion and other factors) that the U.S. launch price would likely be closer to $250, but this did little to mollify people.
What many people tend to ignore or forget, though, is that Nintendo made some enormous pricing mistakes with the Wii -- leaving millions of dollars on the table. And with the 3DS, the company's taking steps to ensure it doesn't repeat those gaffes. $250 (or even $300, if the company decides to surprise everyone and roll the dice) is, admittedly, an extraordinarily high price for a handheld gaming device... particularly one that has a single function. And this pricing strategy could backfire and give Apple a window to increase its market share. But from a pure business standpoint, it's a sure way for Nintendo to regain the confidence of its investors.
The Wii, as you'll recall, was the Holy Grail among shoppers for the better part of two years. Stores couldn't keep them in stock and Nintendo couldn't make them fast enough (let's ignore those conspiracy theories that the company was deliberately creating a shortage). The demand came, in part, because the company had created something that was truly novel. And it has a chance to do that again with the 3DS.
The most expensive Nintendo handheld yet?
The Wii was a huge gamble for Nintendo; it was so dramatically different from anything the video game industry had offered before, that no one was entirely certain how the general public would react. So pricing that console at $250 -- an extremely affordable price for a new system -- made sense. It was, in many ways, a carrot meant to attract people.
It worked, but it soon became obvious that Nintendo could have charged considerably more and still had sellouts. At the same time, it sent a message to consumers: Nintendo might have some unusual ideas, but they're fun. Now Nintendo hopes that people remember this when the 3DS hits shelves.
"Demand will be greater than the manufacturing capacity for the first few months," says Michael Pachter, an analyst with Wedbush Securities. "You satisfy demand at whatever price you can get."
That's going to cause grumbling among some gamers, many of whom may vow that they will wait for the 3DS to come out of the stratosphere before they buy in. But those folks might want to get comfortable. Supply constraint for the system's 3D screen is likely to be a real issue; this is already being blamed for the system's delayed Japanese launch. And it's not something that's going to be corrected immediately (Pachter, in fact, says he would not be surprised if the company further delays the U.S. and European launch dates as those draw near).
Whatever the case, we're hoping this will be worth it!
That means sellouts -- and if Nintendo is going to sell every system it can make anyway, it makes a lot of sense to sell them at a higher price. And as soon as it looks like the demand is starting to decline, a timely price cut can keep the frenzy going for several more months. That's why $300 for a U.S. launch price isn't as insane as it might sound. If anything, it would give the company a revenue bump for at least six months... and if they're forced to slash prices, they're still able to get $250 as holiday 2011 rolls around.
Nintendo, of course, is famous for never selling their hardware at a loss; they're likely to make a hefty profit on the 3DS at either $250 or $300. But even if supply constraints weren't an issue, the premium price tag would still be a wise move. After all, it works like a charm for Nintendo's biggest growing competitor: Apple.
Depending on whom you choose to believe, it only costs Apple between $230 and $270 to make a 16GB iPad (without 3G). That same product retails for $499 -- and is among the hottest items at retail today (the 3G-enabled, 64GB model is estimated to cost just $346 to produce, and sells for $849 -- a 145 percent markup). Despite that, Apple sold 4.5 million iPads in the first three months.
Are the iPad and the 3DS the same? Of course not, but the lesson here is.
Price isn't what makes or breaks a sale when it comes to new technology, especially in the entertainment world. Ultimately, it comes down to how novel your product is, and the consumer excitement it can generate. As we saw at this year's E3 Expo (and as Nintendo has reminded us in defending its pricing decision), the 3DS has plenty of excitement surrounding it.


The Missive Maven: Revolutionary, in less than a week!
Happy New Year, everyone! 2014 is an extra-special, super-exciting year in my household, because "Revolutionary," debut novel of my best beloved, Alex Myers, will be released. It will hit bookstore shelves in less than a week, on January 14, 2014. Hooray! Please take a look at his fabulous author website, which will tell you more about the book, and has all kinds of other excellent background information on the book and on Alex.
I will try to refrain from kvelling in my excitement about seeing the actual book in print - Alex got a few author copies a little bit in advance of the publication date, seen in boxes in the photo above - and instead tell you other, more practical things. First, for letter writers and mail enthusiasts (and really, why would you be reading this blog if you weren't a letter writer or mail enthusiast?), the novel has an epistolary element that I will not spoil here, except to say that letters play a very important role.
The book is available in eBook and hardcover on many fine internet retailers, including Amazon, IndieBound, and Bookish.
Facebook: please check out Alex Myers' author page on Facebook. Please like it. Show him some love. The power that Facebook likes hold in our strange modern world is mystifying, but if you're on Facebook, it would be ever so marvelous if you'd like his author page.
Twitter: he tweets some great stuff on writing, the Revolutionary war, feminism, gender and trans issues, and more. Follow him on Twitter at @MyersWriting.
I recognize that, being madly in love with and married to the author for many years, I am not entirely unbiased, but I think that this is a really brilliant, special novel, and if you are a fiction reader as well as a mail enthusiast, I think you'll enjoy it and highly encourage you to check it out.
P.S. I hear there is a movement afoot to get Deborah Samson on a U.S. postage stamp... you know I'm game for that endeavor!
kvelling...i LOVE it! congrats all around. no small feat!
I preordered last April and the second Revolutionary arrives in my mailbox, consider me a devoted reader for a day or so. Just me, my book and a glass or two of wine. I can't wait!


text:
Q: How to know context of the ContextMenu in JavaFX? Context menu, is, by definition, a menu, called against some context.
Unfortunately, I can't see any means to obtain this context in ContextMenu. Is this really impossible?

A: from my current understanding of what you want, you can not do that really
but try these
ContextMenu.getOwnerNode();
ContextMenu.getOwnerWidnow();

aside from that it has a userData so i guess, you could pass your "context" there


As you can see, orthodontics appliances are recommended for individuals with different dental conditions that require correction. They are not worn as aesthetic devices and you need the recommendation of a qualified orthodontist or a dentist. If you have a dental condition, contact your family dentist prior to settling on any particular appliance.


As a start point we review a practice's accounting records, to make sure that they are organised not just for year-end accounting but also as a management tool for internal reporting during the year.
In particular you need an early warning if profits are under pressure and we can help your practice manager to identify problems early on.
We review your profits and income to consider tax exposure and to look at opportunities for tax planning. We look at innovative solutions for you, which might include using limited companies within your structure, particularly if your income is such that you are 45% tax-payers – may be you could pay 19% tax instead!
Preparation of your annual accounts and tax returns. We aim to do this within 3 months of the year end, where possible, but we are flexible on scheduling.
Our accounts include a detailed benchmarking service which we go through with you to help you to understand how your finances compare to other practices and to pinpoint where you may be able to adapt and improve your profits.
We provide tax forecasts as soon as draft accounts are available so that you have plenty of warning of future tax hits. This also applies to any underpayments of NHS superannuation.
We look at drawings calculations and special pay-outs for partners to ensure that capital and current accounts remain in line with profit and capital sharing arrangements.
We come to see you at least once a year to meet all the partners and the management team. This is a comprehensive meeting to look at your accounts, tax planning and to talk to you about recent developments in your practice and in the national arena.
At your request we can meet you more regularly. This is usually when there is something specific going on, such as a new venture, or surgery build or when partners are leaving or joining the practice. We can help you to manage such changes painlessly.
We are regularly considering and supporting merging practices and working at scale organisations. At the outset we carry out due diligence, advise on structures and support GPs and practice managers through the set up process, working with lawyers experienced in this type of project, who we can introduce to the team.
We regularly assist practices with casflow management, using forecasts which we populate and review with our clients.
A current hot topic is the possible application of IR35 legislation where practices engage the services of locums, pharmacists etc on an ad hoc basis.
We advise on all aspects of the NHS pension scheme and how it works for GP principals and your staff. Currently we are talking to our clients about tax planning for the Lifetime Allowance and Annual Allowance.
We offer a book-keeping service which can be a very cost effective option for you.
We also offer access to a payroll bureau service as a long or short term solution.
If you are VAT registered – and we act as accountants for lots of dispensing practices who are – then we can help you with the complexities of VAT legislation and even do your VAT returns for you.
We can install accounting software and train your team to use this to give you a comprehensive internal accounting system, with useful management reports to look at throughout the year. This will become more important when HMRC roll out their Making Tax Digital programme from 2019.


Very beautiful! Can you link to the lights?
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One of the big disadvantages that GitHub has over for instance Gitorious is that there is no way to clone a repository over HTTP. The service is currently limited to cloning via git:// which is quite a problem if you're living behind for instance a corporate firewall.
I'm going to close this until more people ask for it. We plan to start keep track of clone stats so git-daemon is actually preferable.
So please everyone, vote for this ticket.