Quasielastic Signal Research Articles

Low-dimensional antiferromagnetic fluctuations in the heavy-fermion paramagnetic ladder compound UTe2

Inelastic-neutron-scattering measurements were performed on a single crystal of the heavy-fermion paramagnet UTe$_2$ above its superconducting temperature. We confirm the presence of antiferromagnetic fluctuations with the incommensurate wavevector $\mathbf{k}_1=(0,0.57,0)$. A quasielastic signal is found, whose momentum-transfer dependence is compatible with fluctuations of magnetic moments $\mu\parallel\mathbf{a}$, with a sine-wave modulation of wavevector $\mathbf{k}_1$ and in-phase moments on the nearest U atoms. Low dimensionality of the magnetic fluctuations, consequence of the ladder structure, is indicated by weak correlations along the direction $\mathbf{c}$. These fluctuations saturate below the temperature $T_1^*\simeq15$~K, in possible relation with anomalies observed in thermodynamic, electrical-transport and nuclear-magnetic-resonance measurements. The absence or weakness of ferromagnetic fluctuations, in our data collected at temperatures down to 2.1 K and energy transfers from 0.6 to 7.5 meV, is emphasized. These results constitute constraints for models of magnetically-mediated superconductivity in UTe$_2$.

Structure and Dynamics of Carbon Buckyballs Encapsulated to Single-Walled Carbon Nanotubes

The structural and dynamical attributes of C60 chains inserted inside Single Walled carbon Nanotubes (SWNT) have been investigated by x-ray and neutron refraction, and inelastic neutron scattering (INS). The mensuration have been performed on a large mass of a very high quality carbon peapods sample. We showed that powder refraction could hardly give definitive response on the way the C60s are bonded inside SWNT. However, the comparison of the neutron-derived generalized compression of states (GDOS) of the inserted C60 peas with the GDOS of the same objects derived from lattice dynamics computations led to unambiguous results. The witnessing of excitations in the 8-15 meV span is a clear evidence for the presence strong bonds among C60s in the sample. In the same time, the witnessing of a very weak quasi-elastic signal may be relevant to rotational motions of C60 monomers inside the SWNT. These results suggest that peapods are built of a mixed phase of C60 monomers and C60 n-mers.

Spectroscopic fingerprint of charge order melting driven by quantum fluctuations in a cuprate

Copper oxide high-TC superconductors possess a number of exotic orders that coexist with or are proximal to superconductivity. Quantum fluctuations associated with these orders may account for the unusual characteristics of the normal state, and possibly affect the superconductivity1–4. Yet, spectroscopic evidence for such quantum fluctuations remains elusive. Here, we use resonant inelastic X-ray scattering to reveal spectroscopic evidence of fluctuations associated with a charge order5–14 in nearly optimally doped Bi2Sr2CaCu2O8+δ. In the superconducting state, while the quasielastic charge order signal decreases with temperature, the interplay between charge order fluctuations and bond-stretching phonons in the form of a Fano-like interference increases, an observation that is incompatible with expectations for competing orders. Invoking general principles, we argue that this behaviour reflects the properties of a dissipative system near an order–disorder quantum critical point, where the dissipation varies with the opening of the pseudogap and superconducting gap at low temperatures, leading to the proliferation of quantum critical fluctuations, which melt charge order. X-ray scattering experiments show that the quantum fluctuations associated with charge order take a form that is incompatible with the idea of competition between charge order and superconductivity.

Effect of Nd and Rh substitution on the spin dynamics of the 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.

Evidence of precursor orthorhombic domains well above the electronic nematic transition temperature in Sr(Fe1−xCox)2As2

Raman scattering, synchrotron x-ray diffraction, specific heat, resistivity and magnetic susceptibility measurements were performed in Sr(Fe1−xCox)2As2 [] single crystals with superconducting critical temperature K and two additional transitions at 132 and 152 K observed in both specific heat and resistivity data. A quasielastic Raman signal with B2g symmetry (tetragonal cell) associated with electronic nematic fluctuations is observed. Crucially, this signal shows maximum intensity at K, marking the nematic transition temperature. X-ray diffraction shows evidence of coexisting orthorhombic and tetragonal domains between and ∼ 152 K, implying that precursor orthorhombic domains emerge over an extended temperature range above . While the height of the quasielastic Raman peak is insensitive to , the temperature-dependence of the average nematic fluctuation rate indicates a slowing down of the nematic fluctuations inside the precursor orthorhombic domains. These results are analogous to those previously reported for the LaFeAsO parent oxypnictide (Kaneko et al 2017 Phys. Rev. B 96 014506). We propose a scenario where the precursor orthorhombic phase may be generated within the electronically disordered regime () as long as the nematic fluctuation rate is sufficiently small in comparison to the optical phonon frequency range. In this regime, the local atomic structure responds adiabatically to the electronic nematic fluctuations, creating a net of orthorhombic clusters that, albeit dynamical for , may be sufficiently dense to sustain long-range phase coherence in a diffraction process up to .

Effects of Confinement and Pressure on the Vibrational Behavior of Nano-Confined Propane

Fluids confined in nanopores exhibit significant deviations in their structure and dynamics from the bulk behavior. Although phase, structural, and diffusive behaviors of confined fluids have been investigated and reported extensively, confinement effects on the vibrational properties are less understood. We study the vibrational behavior of propane confined in 1.5 nm nanopores of MCM-41-S using inelastic neutron scattering (INS) and molecular dynamics (MD) simulations. Vibrational spectra have been obtained from INS data as functions of temperature and pressure. At ambient pressure, a strong quasielastic signal observed in the INS spectrum at 80 K suggests that confined propane remains liquid below the bulk phase melting point of 85 K. The quasielastic signal is heavily suppressed when either the pressure is increased to 1 kbar or the temperature is lowered to 30 K, indicating solidification of pore-confined propane. Confinement in MCM-41-S pores results in a glass-like state of propane that exhibits a relatively featureless low-energy vibrational spectrum compared to that of the bulk crystalline propane. Increasing the pressure to 3 kbar results in hardening of the intermolecular and methyl torsional modes. The INS data are used for estimating the isochoric specific heat of confined propane, which is compared with the specific heat of bulk propane reported in literature. Data from MD simulations are used to calculate the vibrational power spectra that agree qualitatively with the experimental data. Simulation data also suggest a reduction of the structural ordering (positional, orientational, and intramolecular) of propane under confinement.

Propane diffusion in ZSM-5 pores measured by quasielastic neutron scattering under macroscopic flow

Quasielastic neutron scattering (QENS) was used to investigate the diffusion of propane in zeolite ZSM-5 under static and macroscopic flow conditions. The rate of self-diffusion in the adsorbed phase was slightly faster under the flow conditions studied. Control measurements showed that the broadening seen in the quasielastic signal must result from propane condensed in the zeolitic pore and not from gas, either in the bulk or inter-particle voids.

Quasielastic and low-energy inelastic neutron scattering study of HoCrO3 by high resolution time-of-flight neutron spectroscopy

In order to understand the origin of the huge quasielastic magnetic scattering observed previously with a back-scattering neutron spectrometer, we have re-investigated the low energy excitations in HoCrO3 by inelastic neutron scattering in a much wider energy range with time-of-flight neutron spectrometers. The inelastic signals are due to the excitations between the ground state doublet of the Ho ion. The quasielastic signal is due to the fluctuation of the disordered Ho moments. At low temperature the intensity of quasielastic scattering is small. It starts increasing as the temperature increases above 30 K. At the same temperature, the elastic intensity due to Ho moment ordering decreases in a similar way. This observation strengthens the hypothesis that the quasielastic scattering is due the fluctuations of the disordered Ho moments. The time scale of fluctuations has been determine from the quasielastic scattering and was found to vary from about 22 ps at K to about 2.5 ps at K. The stretched exponential line shape indicates a distribution of decay rates at low temperatures.

Long-Range Order in the Dipolar XY Antiferromagnet Er_{2}Sn_{2}O_{7}.

Er_{2}Sn_{2}O_{7} remains a puzzling case among the extensively studied frustrated compounds of the rare-earth pyrochlore family. Indeed, while a first-order transition towards a long-range antiferromagnetic state with the so-called Palmer-Chalker structure is theoretically predicted, it has not yet been observed, leaving the issue as to whether it is a spin-liquid candidate open. We report on neutron scattering and magnetization measurements which evidence a second-order transition towards this Palmer-Chalker ordered state around 108mK. Extreme care was taken to ensure a proper thermalization of the sample, which has proved to be crucial to successfully observe the magnetic Bragg peaks. At the transition, a gap opens in the excitations, superimposed on a strong quasielastic signal. The exchange parameters, refined from a spin-wave analysis in applied magnetic field, confirm that Er_{2}Sn_{2}O_{7} is a realization of the dipolar XY pyrochlore antiferromagnet. The proximity of competing phases and the strong XY anisotropy of the Er^{3+} magnetic moment might be at the origin of enhanced fluctuations, leading to the unexpected nature of the transition, the low ordering temperature, and the observed multiscale dynamics.

Water Mobility in Chalk: A Quasielastic Neutron Scattering Study

Water mobility through porous rock has a role to play in many systems, such as contaminant remediation, CO2 storage, and oil recovery. We used inelastic and quasielastic neutron scattering to describe water dynamics in two different chalk samples that have similar pore volume (ranging from tens of micrometers to a few nanometers) but different water uptake properties. We observed distinct water populations, where the analysis of the quasielastic data shows that after the hydration process most of the water behaves as bulk water. However, the lack of quasielastic signal, together with the observation of a translational mode at 10 meV, imply that in chalk samples that take up less water confinement occurs mostly in the pore volume that is accessible with nitrogen adsorption measurements.

Thermal evolution of magnetic-excitation spectrum of PrB6

The magnetic dynamic response of a PrB6 single crystal has been studied using inelastic neutron scattering in a temperature range of 10–120 K, which is above the temperatures of the phase transitions to the magnetic-ordered state. The study is aimed at revealing peculiarities of the state with a low magnetic moment in a temperature range of 7 K < T ≤ 20 K, which was identified in a number of magnetometric experiments. In addition to a quasielastic signal, a weak-dispersion excitation with an energy of ~1 meV has been detected, which exists at temperatures below 24 K. The results have been analyzed from the viewpoint of the formation of a spatially nonuniform state based on domains with short-range magnetic correlations at temperatures of 10–20 K. Judging by the dispersion of excitations, the character of the correlation is similar to that observed in a state with long-range magnetic order which arises at lower temperatures.

Microscopic dynamics of glycerol: a QENS study

We report on a quasielastic incoherent neutron scattering (QENS) experiment on liquid glycerol. QENS data were collected at the temperature T=380 K and with a resolution (FWHM) R=55μeV. The analysis of the quasielastic signal enables us to draw a consistent picture of the diffusive mechanism on a picosecond time scale and to compare with most recent models for glycerol dynamics. Model selection, performed with the fitting algorithm FABADA, gives us a preliminary description about the motions of the glycerol molecules in its liquid state.

Vibrational dynamics changes of protein hydration water across the dynamic transition

The vibrational dynamics of protein hydration water has been studied by incoherent neutron scattering. Experiments on a sample of fully deuterated maltose binding protein allowed us to single out the hydration water susceptibility. The main inelastic features, corresponding to hydrogen-bond bending, hydrogen-bond stretching and librational excitations, have been followed over a temperature range extending from 50 to 300K. It turns out that the temperature dependence of the hydrogen-bond stretching contribution is quite similar to that of the mean square displacements deduced by the quasielastic signal, thus suggesting a close relationship between the anharmonicity of longitudinal phonon-like motions and the onset of diffusive molecular dynamics. On the other hand, both hydrogen-bond bending and librational excitations show a temperature dependence consistent with a harmonic character over the whole temperature range.

Polymorphism of Paracetamol: A New Understanding of Molecular Flexibility through Local Methyl Dynamics

This study focuses on the interplay of molecular flexibility and hydrogen bonding manifested in the monoclinic (form I) and orthorhombic (form II) polymorphs of paracetamol. By means of incoherent inelastic neutron scattering and density functional theory calculations, the relaxation processes related to the methyl side-group reorientation were analyzed in detail. Our computational study demonstrates the importance of considering quantum effects to explain how methyl reorientations and subtle conformational changes of the molecule are intertwined. Indeed, by analyzing the quasi elastic signal of the neutron data, we were able to show a unique and complex motional flexibility in form II, reflected by a coupling between the methyl and the phenyl reorientation. This is associated with a higher energy barrier of the methyl rotation and a lower Gibbs free energy when compared to form I. We put forward the idea that correlating solubility and molecular flexibility, through the relation between pKa and methyl rotation activation energy, might bring new insights to understanding and predicting drug bioavailability.

Characteristic energy scales in CePdAl

AbstractWe report on inelastic neutron scattering experiments that were carried out on single‐crystalline CePdAl, which is a heavy fermion system with hexagonal crystal structure and is close to an antiferromagnetic quantum critical point. The measurements yield information on the crystalline‐electric‐field (CEF) excitations and quasielastic spin fluctuations. Two excited CEF levels have been detected at ≈240 K and &gt;400 K. A broad quasielastic magnetic signal could be observed, yielding a Kondo temperature TK = 5 K that agrees with the result from thermodynamic measurements.

Magnetic excitations in EuCu2(SixGe1−x)2: from mixed valence towards magnetism

We report the inelastic neutron scattering study of spin dynamics in EuCu2(SixGe1−x)2 (x = 1, 0.9, 0.75, 0.6), performed in a wide temperature range. At x = 1 the magnetic excitation spectrum was found to be represented by the double-peak structure well below the energy range of the Eu3+ spin–orbit (SO) excitation 7F0→7F1, so that at least the high-energy spectral component can be assigned to the renormalized SO transition. Change of the Eu valence towards 2 + with increased temperature and/or Ge concentration results in further renormalization (lowering the energy) and gradual suppression of both inelastic peaks in the spectrum, along with developing sizeable quasielastic signal. The origin of the spectral structure and its evolution is discussed in terms of excitonic model for the mixed valence state.

Dynamics of highly concentrated protein solutions around the denaturing transition

Using both quasi-elastic and fixed-window neutron spectroscopy, we study the dynamics of highly concentrated aqueous protein solutions of bovine serum albumin around the denaturing transition. For the temperature range 280 K < T < 370 K, the total mean-squared displacement 〈u2〉 is recorded. Below and above the denaturing, we observe that 〈u2〉 increases monotonically with T, but at the denaturing transition it decreases strongly. This observation can be rationalized and quantitatively modeled as a transition from a liquid protein solution to a gel-like state. Atomic vibrations, molecular subunit diffusion and, most importantly, diffusion of the entire protein determine 〈u2〉. The latter is strongly hindered due to entanglement and cross-linking of the chains and causes the pronounced decrease of 〈u2〉. Using information from the full quasi-elastic signal, we separate the diffusion contribution from 〈u2〉 and reveal the transition temperature. For the analysis of this separation, we introduce a general concept, which is applicable to other colloid systems exhibiting both center-of-mass and internal dynamics.

Effects of nonmagnetic La impurities on the spin resonance of Ce1−xLaxCoIn5single crystals as seen via inelastic neutron scattering

The influence of La nonmagnetic impurities on the spin dynamics of CeCoIn${}_{5}$ was studied by inelastic neutron scattering. In La-substituted systems, the spin resonance peak (observed at ${\ensuremath{\Omega}}_{\mathrm{res}}=0.55$ meV in the pure system) is shifted to lower energies but the ratio ${\ensuremath{\Omega}}_{\mathrm{res}}/{k}_{B}{T}_{c}$ remains almost unchanged. The excitation broadens up to an energy of 0.3 meV which is equal to the value of the quasielastic signal in the normal state. The evolution of the excitation as a function of La substitution is compared with Ni- and Zn-substituted YBa${}_{2}$Cu${}_{3}$O${}_{7}$.

Interplay of thermal and quantum spin fluctuations in the kagome lattice compound herbertsmithite

We present a Raman spectroscopic investigation of the herbertsmithite ${\text{ZnCu}}_{3}{(\text{OH})}_{6}{\text{Cl}}_{2}$, a realization of a Heisenberg $s=1/2$ antiferromagnet on a perfect kagome lattice. Focusing on its magnetic excitation spectrum we find two components, a high-temperature quasielastic signal and a low temperature, broad maximum. The latter has a linear low-energy slope and extends to high energy. We have investigated the temperature dependence and symmetry properties of both signals. Our data agree with previous calculations and point to a gapless spin liquid ground state.

Dynamic study of N’N-dimethylparanitroaniline encapsulated in silicalite-1 matrix using neutron spin-echo spectroscopy

The present work focuses on the dynamic studies of N'N- dimethyl-paranitroaniline (dmpNA) encapsulated in silicalite zeolite. Quasielastic neutron scattering (QENS) experiments are carried out using neutron spin-echo technique. Polarisation of the scattered neu- tron beam is measured at carefully chosen values of Q =0 .35, 0.9, 1.1 and 1.45u �1 at fixed T = 298K and at fixed Q =0 .9u �1 at 150, 200, 250 and 298K. This gives insight into the motion and the related ac- tivation energy of the guest dmpNA molecule. The quasielastic signal observed in the present system within the time range considered is due to fast local rotational motions of protons of the end methyl groups. The results are in good agreement with the dynamics of methyl group rotations reported in the literature by back-scattering QENS technique.