129 research outputs found
Ab initio lattice dynamics simulations and inelastic neutron scattering spectra for studying phonons in BaFe2As2: Effect of structural phase transition, structural relaxation and magnetic ordering
We have performed extensive ab initio calculations to investigate phonon
dynamics and their possible role in superconductivity in BaFe2As2 and related
systems. The calculations are compared to inelastic neutron scattering data
that offer improved resolution over published data [Mittal et al., PRB 78
104514 (2008)], in particular at low frequencies. Effects of structural phase
transition and full/partial structural relaxation, with and without magnetic
ordering, on the calculated vibrational density of states are reported. Phonons
are best reproduced using either the relaxed magnetic structures or the
experimental cell. Several phonon branches are affected by the subtle
structural changes associated with the transition from the tetragonal to the
orthorhombic phase. Effects of phonon induced distortions on the electronic and
spin structure have been investigated. It is found that for some vibrational
modes, there is a significant change of the electronic distribution and spin
populations around the Fermi level. A peak at 20 meV in the experimental data
falls into the pseudo-gap region of the calculation. This was also the case
reported in our recent work combined with an empirical parametric calculation
[Mittal et al., PRB 78 104514 (2008)]. The combined evidence for the coupling
of electronic and spin degrees of freedom with phonons is relevant to the
current interest in superconductivity in BaFe2As2 and related systems
Inelastic neutron scattering study of crystal field excitations of Nd<sup>3+</sup> in NdFeAsO
Inelastic neutron scattering experiments were performed to investigate the
crystalline electric field (CEF) excitations of Nd3+ (J = 9/2) in the iron
pnictide NdFeAsO. The crystal field level structures for both the
high-temperature paramagnetic phase and the low-temperature antiferromagnetic
phase of NdFeAsO are constructed. The variation of CEF excitations of Nd3+
reflects not only the change of local symmetry but also the change of magnetic
ordered state of the Fe sublattice. By analyzing the crystal field interaction
with a crystal field Hamiltonian, the crystal field parameters are obtained. It
was found that the sign of the fourth and sixth-order crystal field parameters
change upon the magnetic phase transition at 140 K, which may be due to the
variation of exchange interactions between the 4f and conduction electrons.Comment: 5 pages, 4 figure
Magneto-structural coupling and harmonic lattice dynamics in CaFeAs probed by M\"ossbauer spectroscopy
In this paper we present detailed M\"ossbauer spectroscopy study of
structural and magnetic properties of the undoped parent compound
CaFeAs single crystal. By fitting the temperature dependence of the
hyperfine magnetic field we show that the magneto-structural phase transition
is clearly first-order in nature and we also deduced the compressibility of our
sample to be . Within the Landau's theory of phase
transition, we further argue that the observed phase transition may stem from
the strong magneto-structural coupling effect. Temperature dependence of the
Lamb-M\"ossbauer factor show that the paramagnetic phase and the
antiferromagnetic phase exhibit similar lattice dynamics in high frequency
modes with very close Debye temperatures, 270\,K.Comment: 6 pages,5 figures Accepted by J. Phys.: Condens. Matte
Spin-Lattice Coupling in K0.8Fe1.6Se2 and KFe2Se2: Inelastic Neutron Scattering and ab-initio Phonon Calculations
We report measurements of the temperature dependence of phonon densities of
states in K0.8Fe1.6Se2 using inelastic neutron scattering technique. While
cooling down to 150 K, a phonon peak splitting around 25 meV is observed and a
new peak appears at 31 meV. The measurements support the recent Raman and
infra-red measurements indicating a lowering of symmetry of K0.8Fe1.6Se2 upon
cooling below 250 K. Ab-initio phonon calculations have been carried out for
K0.8Fe1.6Se2 and KFe2Se2. The comparison of the phonon spectra as obtained from
the magnetic as well as non magnetic calculations show pronounced differences.
We show that in the two calculations the energy range of the vibrational
contribution from both Fe and Se are quite different. We conclude that Fe
magnetism is correlated to the phonon dynamics and it plays an important role
in stabilizing the structure of K0.8Fe1.6Se2 as well as that of KFe2Se2. The
calculations highlight the presence of low energy librational modes in
K0.8Fe1.6Se2 as compared to KFe2Se2.Comment: 22 pages, 3 Tables, 7 Figure
Ultrafast Molecular Transport on Carbon Surfaces: The Diffusion of Ammonia on Graphite
We present a combined experimental and theoretical study of the
self-diffusion of ammonia on exfoliated graphite. Using neutron time-of-flight
spectroscopy we are able to resolve the ultrafast diffusion process of adsorbed
ammonia, NH, on graphite. Together with van der Waals corrected density
functional theory calculations we show that the diffusion of NH follows a
hopping motion on a weakly corrugated potential energy surface with an
activation energy of about 4 meV which is particularly low for this type of
diffusive motion. The hopping motion includes further a significant number of
long jumps and the diffusion constant of ammonia adsorbed on graphite is
determined with D=3.9 \cdot 10^{-8}~\mbox{m}^2 /\mbox{s} at 94 K
Striped Magnetic Ground State of the Kagome Lattice in Fe4Si2Sn7O16
We have experimentally identified a new magnetic ground state for the kagome
lattice, in the perfectly hexagonal Fe2+ (3d6, S = 2) compound Fe4Si2Sn7O16.
Representational symmetry analysis of neutron diffraction data shows that below
T_N = 3.5 K, the spins on 2/3 of the magnetic ions order into canted
antiferromagnetic chains, separated by the remaining 1/3 which are
geometrically frustrated and show no long-range order down to at least T = 0.1
K. Moessbauer spectroscopy confirms that there is no static order on the latter
1/3 of the magnetic ions - i.e., they are in a liquid-like rather than a frozen
state - down to at least 1.65 K. A heavily Mn-doped sample
Fe1.45Mn2.55Si2Sn7O16 has the same magnetic structure. Although the propagation
vector q = (0, 1/2 , 1/2 ) breaks hexagonal symmetry, we see no evidence for
magnetostriction in the form of a lattice distortion within the resolution of
our data. We discuss the relationship to partially frustrated magnetic order on
the pyrochlore lattice of Gd2Ti2O7, and to theoretical models that predict
symmetry breaking ground states for perfect kagome lattices.Comment: 5 pages, 5 figure
Anomalous thermal expansion in 1D transition-metal cyanides: what makes the novel trimetallic cyanide Cu1/3Ag1/3Au1/3CN behave differently?
The structural dynamics of a quasi-one-dimensional (1D) mixed-metal cyanide, Cu1/3Ag1/3Au1/3CN, with intriguing thermal properties is explored. All the current known related compounds with straight-chain structures, such as group 11 cyanides CuCN, AgCN, AuCN and bimetallic cyanides MxM’1-xCN (M, M’ = Cu, Ag, Au), exhibit 1D negative thermal expansion (NTE) along the chains and positive thermal expansion (PTE) perpendicular to them. Cu1/3Ag1/3Au1/3CN exhibits similar PTE perpendicular to the chains, however PTE, rather than NTE, is also observed along the chains. In order to understand the origin of this unexpected behavior, inelastic neutron scattering (INS) measurements were carried out, underpinned by lattice-dynamical density-functional-theory (DFT) calculations. Synchrotron-based pair-distribution-function (PDF) analysis and 13C solid-state nuclear-magnetic-resonance (SSNMR) measurements were also performed to build an input structural model for the lattice dynamical study. The results indicate that transverse motions of the metal ions are responsible for the PTE perpendicular to the chains, as is the case for the related group 11 cyanides. However NTE along the chain due to the tension effect of these transverse motions is not observed. As there are different metal-to-cyanide bond lengths in Cu1/3Ag1/3Au1/3CN, the metals in neighboring chains cannot all be truly co-planar in a straight-chain model. For this system, DFT-based phonon calculations predict small PTE along the chain due to low-energy chain-slipping modes induced by a bond-rotation effect on the weak metallophilic bonds. However the observed PTE is greater than that predicted with the straight-chain model. Small bends in the chain to accommodate truly co-planar metals provide an alternative explanation for thermal behavior. These would mitigate the tension effect induced by the transverse motions of the metals and, as temperature increases and the chains move further apart, a straightening could occur resulting in the observed PTE. This hypothesis is further supported by unusual evolution in the phonon spectra, which suggest small changes in local symmetry with temperature
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Chemistry and structure by design: ordered CuNi(CN)4 sheets with copper(II) in a square-planar environment
Layered copper–nickel cyanide, CuNi(CN)4, a 2-D negative thermal expansion material, is one of a series of copper(II)-containing cyanides derived from Ni(CN)2. In CuNi(CN)4, unlike in Ni(CN)2, the cyanide groups are ordered generating square-planar Ni(CN)4 and
Cu(NC)4 units. The adoption of square-planar geometry by Cu(II) in an extended solid is very unusual
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