arXiv subjects

S. Rols

Publications and source records attributed to S. Rols.

At least 19 recordsLinked to original sources

arXiv2025

Spin liquid state in a three-dimensional pyrochlore-like frustrated magnet

The three-dimensional frustrated spin lattice in MgCrGaO4, where Cr3+ ions occupy a pyrochlore-like network, exemplifies a quantum magnet with competing interactions, macroscopic degeneracy, and exotic low-energy excitations. Using thermodynamic, electron spin resonance (ESR), muon spin relaxation (muSR), and inelastic neutron scattering (INS) techniques, we observe no magnetic order or spin freezing down to 57 mK, despite a sizable exchange interaction (J= 58 K) between Cr3+ (S=3/2) moments and inherent site disorder. Below the characteristic exchange energy scale, all experimental probes detect the emergence of antiferromagnetic short-range spin correlations, corroborated by magnetic diffuse scattering in the wave vector dependence of low-energy magnetic excitations centered on Q = 1.5 A^-1 in inelastic neutron scattering experiments. The low-temperature specific heat follows a near-quadratic dependence without a gap, consistent with algebraic spin correlations. These results establish MgCrGaO4 as a rare three-dimensional classical spin liquid featuring a highly degenerate ground-state manifold and gapless excitations, offering a strong impetus for the experimental realization of spin liquids in higher-dimensional frustrated quantum magnets.

cond-mat.str-el↗

arXiv2024

Magnetic structure and crystal field states of antiferromagnetic CeNiGe$_3$: Neutron scattering and $\mu$SR investigations

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.

cond-mat.str-el↗

arXiv2022

Solid-like to Liquid-like Behavior of Cu Diffusion in Superionic Cu2X (X=S, Se): An Inelastic Neutron Scattering and Ab-Initio Molecular Dynamics Investigation

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 Å 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 Å, 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.

cond-mat.mtrl-sci↗

arXiv2021

Experimental Determination of the Interaction Potential between a Helium Atom and the Interior Surface of a C60 Fullerene Molecule

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.

physics.chem-ph↗

arXiv2020

Effect of Nd and Rh substitution on the spin dynamics of Kondo insulator CeFe2Al10

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.

cond-mat.str-el↗

arXiv2020

CeCo$_{1-x}$Fe$_{x}$Ge$_{3}$ -- crystal electric field effects and fine tuning around critical substitution

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.

cond-mat.str-el↗

arXiv2019

Lithium Diffusion in Li2X(X=O, S and Se): Ab-initio Simulations and Neutron Inelastic Scattering Measurements

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.

cond-mat.mtrl-sci↗

arXiv2018

Understanding the magnetism in noncentrosymmetric CeIrGe3: Muon spin relaxation and neutron scattering studies

The magnetic properties of a pressure induced noncentrosymmetric heavy-fermion superconductor CeIrGe$_3$ have been investigated by muon spin relaxation ($μ$SR), powder neutron diffraction (ND) and inelastic neutron scattering (INS) techniques at ambient pressure. For completeness we have also measured the ac magnetic susceptibility $χ_{\rm ac}(T)$, dc magnetic susceptibility $χ(T)$, 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 $χ_{\rm ac}(T)$ and $χ(T)$ data show an additional anomaly near 6.2 K which is also captured in $C_{\rm p}(T)$ data. From $χ_{\rm ac}(T)$, $χ(T)$ 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 $μ$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$^{3+}$.

cond-mat.str-el↗

arXiv2016

Investigating Anomalous Thermal Expansion of Copper Halides by Inelastic Neutron Scattering and Ab-inito Phonon Calculations

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.

cond-mat.mtrl-sci↗

arXiv2016

Crystal field investigation in the light rare earth R$_3$Pt$_{23}$Si$_{11}$ compounds

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.

cond-mat.str-el↗

arXiv2016

Magnetic excitations and electronic interactions in Sr$_2$CuTeO$_6$: a spin-1/2 square lattice Heisenberg antiferromagnet

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.

cond-mat.str-el↗

arXiv2015

Lattice Dynamics and Thermal Expansion Behavior in Metal Cyanides, MCN (M=Cu, Ag, Au): Neutron Inelastic Scattering and First Principles Calculations

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.

cond-mat.mtrl-sci↗

arXiv2015

Structure and dynamics of the fullerene polymer Li4 C60 studied with neutron 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.

cond-mat.mtrl-sci↗

arXiv2015

Haydeeite: a spin-1/2 kagome ferromagnet

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.

cond-mat.str-el↗

arXiv2014

Inelastic Neutron Scattering Studies of Phonon Spectra and Simulations in Tungstates, AWO4 (A = Ba, Sr, Ca and Pb)

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.

cond-mat.mtrl-sci↗

arXiv2014

Spin-Phonon Coupling, High Pressure Phase Transitions and Thermal Expansion of Multiferroic GaFeO3: A Combined First Principles and Inelastic Neutron Scattering Study

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.

cond-mat.mtrl-sci↗

arXiv2013

Phonon Dynamics and Inelastic Neutron Scattering of Sodium Niobate

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.

cond-mat.mtrl-sci↗

arXiv2013

Phonons and Thermodynamics of LiMPO4 (M=Mn, Fe)

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.

cond-mat.mtrl-sci↗