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We present the results of microscopic investigations of antiferromagnetic CeNiGe$_3$, using neutron powder diffraction (NPD), inelastic neutron scattering (INS), and muon spin relaxation ($\mu$SR) measurements. CeNiGe$_3$ crystallizes in a centrosymmetric orthorhombic crystal structure (space group: $Cmmm$) and undergoes antiferromagnetic (AFM) ordering. The occurrence of long-range AFM ordering at $T_{\rm N} \approx 5.2$~K is confirmed by magnetic susceptibility, heat capacity, neutron diffraction, and $\mu$SR measurements. The NPD data characterize the AFM state with an incommensurate helical magnetic structure having a propagation vector $k$ = (0, 0.41, 1/2). In addition, INS measurements at 10~K identified two crystal electric field (CEF) excitations at 9.17~meV and 18.42~meV. We analyzed the INS data using a CEF model for an orthorhombic environment of Ce$^{3+}$ ($J=5/2$) and determined the CEF parameters and ground state wavefunctions of CeNiGe$_3$. Moreover, zero-field $\mu$SR data for CeNiGe$_3$ at $T< T_{\rm N}$ show long-range AFM ordering with three distinct oscillation frequencies corresponding to three different internal fields at the muon sites. The internal fields at the muon-stopping sites have been further investigated using density functional theory calculations., Comment: 13 pages, 9 figures

Cu2Se and Cu2S are excellent model systems of superionic conductors with large diffusion coefficients that have been reported to exhibit different solid-liquid-like Cu-ion diffusion. In this paper, we clarify the atomic dynamics of these compounds with temperature-dependent ab-initio molecular dynamics (AIMD) simulations and inelastic neutron scattering (INS) experiments. Using the dynamical structure factor and Van-Hove correlation function, we interrogate the jump-time, hopping length distribution and associated diffusion coefficients. In cubic-Cu2Se at 500 K, we find solid-like diffusion with Cu-jump lengths matching well the first-neighbour Cu-Cu distance of ~3 {\AA} in the crystal, and clearly defined optic phonons involving Cu-vibrations. Above 700 K, the jump-length distribution becomes a broad maximum cantered around 4 {\AA}, spanning the first and second neighbour lattice distances, and a concurrent broadening of the Cu-phonon density of states. Further, above 900 K, the Cu-diffusion becomes close to liquid-like, with distributions of Cu-atoms continuously connecting crystal sites, while the vibrational modes involving Cu motions are highly damped, though still not fully over-damped as in a liquid. At low temperatures, the solid-like diffusion is consistent with previous X-ray diffraction and quasielastic neutron scattering experiments, while the higher-temperature observation of the liquid-like diffusion is in agreement with previous AIMD simulations. We also report AIMD simulations in Cu2S in the hexagonal and cubic superionic phases, and observe similar solid and liquid-like diffusion at low- and high-temperatures, respectively. The calculated ionic-conductivity is in fair agreement with reported experimental values., Comment: 29 Pages, 7 Figures

The interactions between atoms and molecules may be described by a potential energy function of the nuclear coordinates. Non-bonded interactions are dominated by repulsive forces at short range and attractive dispersion forces at long range. Experimental data on the detailed interaction potentials for non-bonded interatomic and intermolecular forces is scarce. Here we use terahertz spectroscopy and inelastic neutron scattering to determine the potential energy function for the non-bonded interaction between single He atoms and encapsulating C60 fullerene cages, in the helium endofullerenes 3He and 4He, synthesised by molecular surgery techniques. The experimentally derived potential is compared to estimates from quantum chemistry calculations, and from sums of empirical two-body potentials., Comment: 25 pages, 14 figures, submitted to Journal of Chemical Physics

The dynamic magnetic properties of the Kondo-insulator state in CeFe2Al10 (spin gap, resonance mode) have been investigated using polarized neutrons on a single crystal of pure CeFe2Al10. The results indicate that the magnetic excitations are polarized mainly along the orthorhombic a axis and their dispersion along the orthorhombic c direction could be determined. Polycrystalline samples of Nd- and Rh-doped CeFe2Al0 were also studied by the time-of-flight technique, with the aim of finding out how the low-energy magnetic excitation spectra change upon isoelectronic substitution of the rare-earth (Nd) on the magnetic Ce site or electron doping (Rh) on the transition-element Fe sublattice. The introduction of magnetic Nd impurities strongly modifies the spin gap in the Ce dynamic magnetic response and causes the appearance of a quasielastic signal. The crystal-field excitations of Nd, studied in both LaFe2Al10 and CeFe2Al10, also reveal a significant influence of f-electron hybridization (largest in the case of Ce) on the crystal-field potential. As a function of the Rh concentration, a gradual change is observed from a Kondo-insulator to a metallic Kondo-lattice response, likely reflecting the decrease in the hybridization energy., Comment: 27 pages, 15 figures

In this article we present some particularly important issues regarding the CeCo$_{1-x}$Fe$_{x}$Ge$_{3}$ alloys. Firstly, the electrical resistivity below 2 K, down to 500 mK is studied to confirm the non-Fermi-liquid behavior around the critical substitution range x~0.65. Secondly, the scheme of the crystal electric field (CEF) levels has been investigated employing methods like inelastic neutron scattering, specific heat, and magnetic susceptibility. It aims to clarify different reports on the parent CeCoGe$_{3}$ compound and to provide first data concerning CEF in the entire CeCo$_{1-x}$Fe$_{x}$Ge$_{3}$ series. Third, the effect of hydrogenation, especially around the quantum critical point (QCP) (x~0.65) is verified., Comment: 11 pages, 5 figures

We report investigation of phonons and oxygen diffusion in Bi2O3 and (Bi0.7Y0.3)2O3. The phonon spectra have been measured in Bi2O3 at high temperatures up to 1083 K using inelastic neutron scattering. Ab-initio calculations have been used to compute the individual contributions of the constituent atoms in Bi2O3 and (Bi0.7Y0.3)2O3 to the total phonon density of states. Our computed results indicate that as temperature is increased, there is a complete loss of sharp peak structure in the vibrational density of states. Ab-initio molecular dynamics simulations show that even at 1000 K in {\delta}-phase Bi2O3, Bi-Bi correlations remain ordered in the crystalline lattice while the correlations between O-O show liquid like disordered behavior. In the case of (Bi0.7Y0.3)2O3, the O-O correlations broadened at around 500 K indicating that oxygen conductivity is possible at such low temperatures in (Bi0.7Y0.3)2O3 although the conductivity is much less than that observed in the undoped high temperature {\delta}-phase of Bi2O3. This result is consistent with the calculated diffusion coefficients of oxygen and observation by QENS experiments. Our ab-initio molecular dynamics calculations predict that macroscopic diffusion is attainable in (Bi0.7Y0.3)2O3 at much lower temperatures, which is more suited for technological applications. Our studies elucidate the easy directions of diffusion in {\delta}-Bi2O3 and (Bi0.7Y0.3)2O3.

We have performed ab-initio lattice dynamics and molecular dynamics studies of Li2X (X=O, S and Se) to understand the ionic conduction in these compounds. The inelastic neutron scattering measurements on Li2O have been performed across its superionic transition temperature of about 1200 K. The experimental spectra show significant changes around the superionic transition temperature, which is attributed to large diffusion of lithium as well as its large vibrational amplitude. We have identified a correlation between the chemical pressure (ionic radius of X atom) and the superionic transition temperature. The simulations are able to provide the ionic diffusion pathways in Li2X., Comment: 25 Pages, 15 Figures

The magnetic properties of a pressure induced noncentrosymmetric heavy-fermion superconductor CeIrGe$_3$ have been investigated by muon spin relaxation ($\mu$SR), powder neutron diffraction (ND) and inelastic neutron scattering (INS) techniques at ambient pressure. For completeness we have also measured the ac magnetic susceptibility $\chi_{\rm ac}(T)$, dc magnetic susceptibility $\chi(T)$, dc isothermal magnetization $M(H)$ and heat capacity $C_{\rm p}(T,H)$ down to 2 K. CeIrGe$_{3}$ is known to exhibit pressure induced superconductivity ($T_{\rm c}\approx 1.5$ K) at a pressure of 20 GPa and antiferromagnetic ordering at 8.7 K, 4.7 K and 0.7 K at ambient pressure. Our $\chi_{\rm ac}(T)$ and $\chi(T)$ data show an additional anomaly near 6.2 K which is also captured in $C_{\rm p}(T)$ data. From $\chi_{\rm ac}(T)$, $\chi(T)$ and $C_{\rm p}(T)$ measurements we infer three antiferromagnetic transitions above 2 K at $T_{\rm N1}= 8.5$ K, $T_{\rm N2}= 6.0$ K and $T_{\rm N3}= 4.6$ K. Our $\mu$SR study also confirms the presence of three transitions through the observation of one frequency for $T_{\rm N2} < T\leq T_{\rm N1}$, two frequencies for $T_{\rm N3} < T\leq T_{\rm N2}$ and three frequencies for $T\leq T_{\rm N3}$ in the oscillatory asymmetry. The ND data reveal an incommensurate nature of the magnetic ordering at $T=7$ K with the propagation vector k = (0,0,0.688(3)), and a commensurate magnetic structure at $T=1.5$ K with the propagation vector locked to the value k = (0,0,2/3) and magnetic moments oriented along the $c$ axis. The commensurate structure couples a macroscopic ferromagnetic component, resulting in a strong dependence of the lock-in transition temperature on external magnetic field. The INS data show two well defined crystal electric field (CEF) excitations arising from the CEF-split Kramers doublet ground state of Ce$^{3+}$., Comment: 13 pages, 16 figures, 1 table

We investigate detailed lattice dynamics of copper halides CuX (X=Cl, Br, I) using neutron inelastic scattering measurements and ab-initio calculations aimed at a comparative study of their thermal expansion behavior. We identify the low energy phonons which soften with pressure and are responsible for negative thermal expansion. The eigenvector analysis of these modes suggests that softening of the transverse-acoustic modes would lead to NTE in these compounds. The calculations are in very good agreement with our measurements of phonon spectra and thermal expansion behavior as reported in the literature. Our calculations at high pressure further reveal that large difference in negative thermal expansion behavior in these compounds is associated with the difference of the unit cell volume., Comment: 23 Pages, 14 Figures, 3 Tables

The crystalline electric field (CEF) is investigated in Pr$_3$Pt$_{23}$Si$_{11}$ and Nd$_3$Pt$_{23}$Si$_{11}$ by neutron spectroscopy (NS). At low temperature, the number of observed CEF excitations is consistent with the orthorhombic symmetry at the rare earth site. This agrees with previous results on Ce$_3$Pt$_{23}$Si$_{11}$. For Pr- and Nd$_3$Pt$_{23}$Si$_{11}$, the number of CEF parameters is too large to allow for an unambiguous determination. This determination is possible for Ce$_3$Pt$_{23}$Si$_{11}$, due to a reduced number of parameters and to the availability of extensive experimental data. A specific procedure is developed for this purpose that combines genetic algorithmics and optimization methods. An unique set of CEF parameters is found for Ce$_3$Pt$_{23}$Si$_{11}$. It reveals a strong anisotropy at the orthorhombic site, responsible for an easy threefold magnetization axis in the cubic system. Using a microscopic, mean-field, description, the magnetization processes in the paramagnetic and ferromagnetic phases of Ce$_3$Pt$_{23}$Si$_{11}$ are well reproduced. Ce$_3$Pt$_{23}$Si$_{11}$ is shown to realize a model for systems where conflicting anisotropies are forced to cooperate., Comment: 8 pages, 11 figures

Sr$_2$CuTeO$_6$ presents an opportunity for exploring low-dimensional magnetism on a square lattice of $S=1/2$ Cu$^{2+}$ ions. We employ ab initio multi-reference configuration interaction calculations to unravel the Cu$^{2+}$ electronic structure and to evaluate exchange interactions in Sr$_2$CuTeO$_6$. The latter results are validated by inelastic neutron scattering using linear spin-wave theory and series-expansion corrections for quantum effects to extract true coupling parameters. Using this methodology, which is quite general, we demonstrate that Sr$_2$CuTeO$_6$ is an almost realization of a nearest-neighbor Heisenberg antiferromagnet but with relatively weak coupling of 7.18(5) meV., Comment: 10 pages, 7 figures

We report measurement of temperature dependence of phonon spectra in quasi one-dimensional metal cyanides MCN (M=Cu, Ag and Au). Ab initio lattice dynamics calculations have been performed to interpret the phonon-spectra as well as to understand the anamolous thermal expansion behavior in these compounds. We bring out the differences in the phonon mode behavior to explain the differences in the thermal expansion behavior among the three compounds. The chain-sliding modes are found to contribute maximum to the negative thermal expansion along c axis in the Cu and Ag compounds, while the same modes contribute to positive thermal expansion in the Au compound. Several low energy transverse modes lead to positive thermal expansion along a and b axis in all the compounds. The calculated elastic constants and Born effective charges are correlated with the difference in nature of bonding among these metal cyanides., Comment: 22 pages 10 figures

The mineral haydeeite, alpha-MgCu3(OD)6Cl2, is a S=1/2 kagome ferromagnet that displays long-range magnetic order below TC=4.2 K with a strongly reduced moment. Our inelastic neutron scattering data show clear spin-wave excitations that are well described by a Heisenberg Hamiltonian with ferromagnetic nearest-neighbor exchange J1=-38 K and antiferromagnetic exchange Jd=+11 K across the hexagons of the kagome lattice. These values place haydeeite very close to the quantum phase transition between ferromagnetic order and non-coplanar twelve-sublattice cuboc2 antiferromagnetic order. Diffuse dynamic short-range ferromagnetic correlations observed above TC persist well into the ferromagnetically ordered phase with a behavior distinct from critical scattering.

The two-dimensional polymer structure and lattice dynamics of the superionic conductor Li4 C60 are investigated by neutron diffraction and spectroscopy. The peculiar bonding architecture of this compound is definitely confirmed through the precise localisation of the carbon atoms involved in the intermolecular bonds. The spectral features of this phase are revealed through ab-initio lattice dynamics calculations and inelastic neutron scattering experiments. The neutron observables are found to be in very good agreement with the simulations which predict a partial charge transfer from the Li atoms to the C60 cage. The absence of a well defined band associated to one category of the Li atoms in the experimental spectrum suggests that this species is not ordered even at the lowest temperatures. The calculations predict an unstable Li sublattice at a temperature of 200 K, that we relate to the large ionic diffusivity of this system. This specificity is discussed in terms of coupling between the low frequency optic modes of the Li ions to the soft structure of the polymer., Comment: 29 pages, 13 Figures

Lattice dynamics and high pressure phase transitions in AWO4 (A = Ba, Sr, Ca and Pb) have been investigated using inelastic neutron scattering experiments, ab-initio density functional theory calculations and extensive molecular dynamics simulations. The vibrational modes that are internal to WO4 tetrahedra occur at the highest energies consistent with the relative stability of WO4 tetrahedra. The neutron data and the ab-initio calculations are found to be in excellent agreement. The neutron and structural data are used to develop and validate an interatomic potential model. The model is used for classical molecular dynamics simulations to study their response to high pressure. We have calculated the enthalpies of the scheelite and fergusonite phases as a function of pressure, which confirms that the scheelite to fergusonite transition is second order in nature. With increase in pressure, there is a gradual change in the AO8 polyhedra, while there is no apparent change in the WO4 tetrahedra. We found that that all the four tungstates amorphize at high pressure. This is in good agreement with available experimental observations which show amorphization at around 45 GPa in BaWO4 and 40 GPa in CaWO4. On amorphization, there is an abrupt increase in the coordination of the W atom while the bisdisphenoids around A atom are considerably distorted. The pair correlation functions of the various atom pairs corroborate these observations. Our observations aid in predicting the pressure of amorphization in SrWO4 and PbWO4, which have not been experimentally reported., Comment: 15 pages, 8 figures

We have carried out an extensive phonon study on multiferroic GaFeO3 to elucidate its dynamical behavior. Inelastic neutron scattering measurements are performed over a wide temperature range, 150 to 1198 K. First principles lattice dynamical calculations are done for the sake of the analysis and interpretation of the observations. The comparison of the phonon spectra from magnetic and non-magnetic calculations highlights pronounced differences. The energy range of the vibrational atomistic contributions of the Fe and O ions are found to differ significantly in the two calculation types. Therefore, magnetism induced by the active spin degrees of freedom of Fe cations plays a key role in stabilizing the structure and dynamics of GaFeO3. Moreover, the computed enthalpy in various phases of GaFeO3 is used to gain deeper insights into the high pressure phase stability of this material. Further, the volume dependence of the phonon spectra is used to determine its thermal expansion behavior., Comment: 23 pages, 9 Figures

Sodium niobate (NaNbO3) exhibits most complex sequence of structural phase transitions in perovskite family and therefore provides as excellent model system for understanding the mechanism of structural phase transitions. We report temperature dependence of inelastic neutron scattering measurements of phonon densities of states in sodium niobate. The measurements are carried out in various crystallographic phases of this material at various temperatures from 300 K to 1048 K. The phonon spectra exhibit peaks centered around 19, 37, 51, 70 and 105 meV. Interestingly, the peak around 70 meV shifts significantly towards lower energy with increasing temperature, while the other peaks do not exhibit an appreciable change. The phonon spectra at 783 K show prominent change and become more diffusive as compared to those at 303 K. In order to better analyze these features, we have performed first principles lattice dynamics calculations based on the density functional theory. The computed phonon density of states is found to be in good agreement with the experimental data. Based on our calculation we are able to assign the characteristic Raman modes in the antiferroelectric phase to the A1g symmetry, which are due to the folding of the T (w=95 cm-1) and delta(w=129 cm-1) points of the cubic Brillouin zone., Comment: 19 pages, 8 figures, 2 tables

Lithium transition metal phospho-olivines are useful electrode materials, owing to their stability, high safety, low cost and cyclability. We report phonon studies using neutron inelastic scattering experiments, ab-initio density functional theory calculations and potential model calculations on LiMPO4 (M=Mn, Fe) at ambient and high temperature to understand the microscopic picture of Li sub-lattice. The experiments are in good agreement with calculations. The lattice dynamics calculations indicate instability of a zone-centre as well as zone-boundary modes along (100) at volume corresponding to high temperature. The unstable phonon modes show mainly large vibration of Li atoms in the x-z plane of the orthorhombic structure (space group Pbnm). Molecular dynamics simulations with increasing temperature indicate large mean square displacement of Li as compared to other constituent atoms. The computed pair-correlations between various atom pairs show that there is local disorder occurring in the lithium sub-lattice with increasing temperature, while other pairs show minimal changes. The results find the two compounds to be thermally stable up to high temperatures, which is a desirable trait for its battery applications., Comment: 19 Pages, 12 Figures

We report a comparative study of the dynamics of Cu2O, Ag2O and Au2O (i.e. M2O with M = Au, Ag and Cu) using first principle calculations based on the density functional theory. Here for the first time we show that the nature of chemical bonding and open space in the unit cell are directly related to the magnitude of thermal expansion coefficient. A good match between the calculated phonon density of states and that derived from inelastic neutron scattering measurements is obtained for Cu2O and Ag2O. The calculated thermal expansions of Ag2O and Cu2O are negative, in agreement with available experimental data, while it is found to be positive for Au2O. We identify the low energy phonon modes responsible for this anomalous thermal expansion. We further calculate the charge density in the three compounds and find that the magnitude of the ionic character of the Ag2O, Cu2O, and Au2O crystals is in decreasing order, with an Au-O bond of covalent nature strongly rigidifying the Au4O tetrahedral units. The nature of the chemical bonding is also found to be an important ingredient to understand the large shift of the phonon frequencies of these solids with pressure and temperature. In particular, the quartic component of the anharmonic term in the crystal potential is able to account for the temperature dependence of the phonon modes., Comment: 24 Pages, 13 Figures, Supplementary material

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 Figures

LuCuGaO4 has magnetic Cu2+ and diamagnetic Ga3+ ions distributed on a triangular bilayer and is suggested to undergo a spin-glass transition with T_g approximately 0.4 K. Using muSR and neutron scattering measurements, we show that at low temperature the spins form a short-range correlated state with spin fluctuations detectable over a wide range of timescales: at 0.05 K magnetic fluctuations can be detected in both the muSR time window and also extending beyond 7 meV in the inelastic neutron scattering response, indicating magnetic fluctuations spanning timescales between 1E-5 and 1E-10 seconds. The dynamical susceptibility scales according to the form \chi''(\omega)T^\alpha, with \alpha=1, throughout the measured temperature range (0.05 - 50 K). These effects are associated with quantum fluctuations and some degree of structural disorder in ostensibly quite different materials, including certain heavy fermion alloys, kagome spin liquids, quantum spin glasses, and valence bond glasses. We therefore suggest LuCuGaO4 is an interesting model compound for the further examination of disorder and quantum magnetism., Comment: 19 pages, 10 figures; new version including new data

We report detailed measurements of temperature dependence and ab initio lattice dynamical calculations of the phonon density-of-states of two Sr based iron pnictide parent compounds; SrFe2As2 and SrFeAsF. Although both compounds undergo a magnetic as well as a tetragonal-to-orthorhombic structural phase transitions, no drastic change of their phonon spectra is found in the temperature range from 2 to 300 K.. In both the systems the Fe-As stretching modes at 32 meV react to the temperature change and shift towards higher energies with decreasing temperature. Furthermore, we found that in the antiferromagnetic phase of SrFe2As2 at 180 K a peak at 25 meV, due to Fe vibrations, moves slightly to higher energies and become narrower on cooling from 300 K. However we did not find any evidence of softening of low energy phonon modes in both SrFe2As2 and SrFeAsF on decreasing the temperature from 300 K in their paramagnetic phase. This is contrary to our earlier observation of phonon softening in CaFe2As2, Ca0.6Na0.4Fe2As2 and Sr0.6K0.4Fe2As2. For the sake of comparison, the previously studied Ca- and Ba-cases are also presented and the role of the magnetic ordering on the calculated phonon spectra in these two families of pnictides is reported., Comment: Paper has been withdrawn by the author. We have submitted new version at arXiv. The new arXiv Ref is arXiv:1007.1711

Our recent neutron scattering measurements of phonons and other quasi-particle excitations in solid deuterium (sD$_2$) and the extraction of the density of states for phonons and rotational transitions in sD2 have led us to a new understanding of the production of ultra-cold neutrons (UCN) in sD2. This new picture is somehow different to earlier published results for sD2. The cross section for UCN production in sD2 has been determined by using the density of states G1(E) in combination with the incoherent approximation and by a direct calibration of our measured neutron cross sections with the known cross section of the J=1 -> 0 rotational transition in deuterium. Both methods deliver new data on this cross section and agree quite well with direct measurements of this energy averaged UCN production cross section., Comment: 4 pages, 6 figures

The dynamics of solid deuterium (sD2) is studied by means of inelastic scattering (coherent and incoherent) of thermal and cold neutrons at different temperatures and para-ortho ratios. In this paper, the results for the generalized density of states (GDOS) are presented and discussed. The measurements were performed at the thermal neutron time-of-flight (TOF) instrument IN4 at ILL Grenoble and at the cold neutron TOF instrument TOFTOF at FRM II Garching. The GDOS comprises besides the hcp phonon excitations of the sD2 the rotational transitions J = 0 ->1 and J = 1 -> 2. The intensities of these rotational excitations depend strongly on the ortho-D2 molecule concentration co in sD2. Above E = 10 meV there are still strong excitations, which very likely may originate from higher energy damped optical phonons and multi-phonon contributions. A method for separating the one- and multi-phononon contributions to the density of states willbe presented and discussed.

We report detailed measurements of composition as well as temperature dependence of the phonon density-of-states in a new series of FeAs compounds with composition CaFe1\_{1-x}Co\_{x}AsF (x = 0, 0.06, 0.12). The composition as well as temperature dependence of phonon spectra for CaFe\_{1-x}Co\_{x}AsF (x = 0, 0.06, 0.12) compounds have been measured using time of flight IN4C and IN6 spectrometers at ILL, France. The comparison of phonon spectra at 300 K in these compounds shows that acoustic phonon modes up to 12 meV harden in the doped compounds in comparison to the parent CaFeAsF. While intermediate energy phonon modes from 15 meV to 25 meV are also found to shift towards high energies only in the 12 % Co doped CaFeAsF compound. The experimental results for CaFe\_{1-x}Co\_{x}AsF (x = 0, 0.06, 0.12) are quite different from our previous phonon studies on parent and superconducting MFe2As2 (M=Ba, Ca, Sr) where low-energy acoustic phonon modes do not react with doping, while the phonon spectra in the intermediate range from 15 to 25 K are found to soften in these compounds. We argue that stronger spin phonon interaction play an important role for the emergence of superconductivity in these compounds. The lattice dynamics of CaFe\_{1-x}Co\_{x}AsF (x = 0, 0.06, 0.12) compounds is also investigated using the ab-initio as well as shell model phonon calculations. We show that the nature of the interaction between the Ca and the Fe-As layers in CaFeAsF compounds is quite different compared with our previous studies on CaFe2As2., Comment: 19 pages, 5 figures

We report the pressure and temperature dependence of the phonon density-of-states in superconducting Ca0.6Na0.4Fe2As2 (Tc=21 K) and the parent compound CaFe2As2, using inelastic neutron scattering. We observe no significant change in the phonon spectrum for Ca0.6Na0.4Fe2As2 at 295 K up to pressures of 5 kbar. The phonon spectrum for CaFe2As2 shows softening of the low-energy modes by about 1 meV when decreasing the temperature from 300 K to 180 K. There is no appreciable change in the phonon density of states across the structural and anti-ferromagnetic phase transition at 172 K. These results, combined with our earlier temperature dependent phonon density of states measurements for Ca0.6Na0.4Fe2As2, indicate that the softening of low-energy phonon modes in these compounds may be due to the interaction of phonons with electron or short-range spin fluctuations in the normal state of the superconducting compound as well as in the parent compound. The phonon spectra are analyzed with ab-initio and empirical model calculations giving partial densities of states and dispersion relations., Comment: 14 pages, 6 figures

We report inelastic neutron scattering measurements of the phonon density-of-states in superconducting Sr0.6K0.4Fe2As2 (Tc=30 K) and Ca0.6Na0.4Fe2As2 (Tc=18 K). Compared with the parent compound BaFe2As2 doping affects mainly the lower and intermediate frequency part of the vibrations. Mass effects and lattice contraction cannot explain these changes. A lattice dynamical model has been used to identify the character of the various phonon bands. Softening of phonon modes below 10 meV has been observed in both samples on cooling from 300 K to 140 K. In the Ca doped compound the softening amounts to about 1 meV while for the Sr doped compound the softening is about 0.5 meV. There is no appreciable change in the phonon density of states when crossing Tc., Comment: 5 pages, 4 figures

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.

We report here first extensive measurements of the temperature dependence of phonon density of states of BaFe2As2, the parent compound of the newly discovered FeAs-based superconductors, using inelastic neutron scattering. The experiments were carried out on the thermal time-of-flight neutron spectrometer IN4 at the ILL on a polycrystalline sample. There is no appreciable change in the spectra between T = 10 K and 200 K, although the sample undergoes a magnetic as well as a tetragonal-to-orthorhombic structural phase transition at 140 K. This indicates a rather harmonic phonon system. Shell model lattice dynamical calculations based on interatomic potentials are carried out to characterize the phonon data. The calculations predict a shift of the Ba-phonons to higher energies at 4 GPa. The average energy of the phonons of the Ba-sublattice is also predicted to increase on partial substitution of Ba by K to Ba0.6K0.4. The calculations show good agreement with the experimental phonon spectra, and also with the specific heat data from the literature., Comment: 10 pages, 4 figures