Magnetic Excitations of the Classical Spin Liquid MgCr_{2}O_{4}.

We report a comprehensive inelastic neutron-scattering study of the frustrated pyrochlore antiferromagnet MgCr_{2}O_{4} in its cooperative paramagnetic regime. Theoretical modeling yields a microscopic Heisenberg model with exchange interactions up to third-nearest neighbors, which quantitatively explains all of the details of the dynamic magnetic response. Our work demonstrates that the magnetic excitations in paramagnetic MgCr_{2}O_{4} are faithfully represented in the entire Brillouin zone by a theory of magnons propagating in a highly correlated paramagnetic background. Our results also suggest that MgCr_{2}O_{4} is proximate to a spiral spin-liquid phase distinct from the Coulomb phase, which has implications for the magnetostructural phase transition in MgCr_{2}O_{4}.

Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce_{2}Zr_{2}O_{7}.

Neutron scattering measurements on the pyrochlore magnet Ce_{2}Zr_{2}O_{7} reveal an unusual crystal field splitting of its lowest J=5/2 multiplet, such that its ground-state doublet is composed of m_{J}=±3/2, giving these doublets a dipole-octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with θ_{CW}=-0.4(2) K, leading to a naive expectation of an all-in, all-out ordered state at low temperatures. Instead, our low-energy inelastic neutron scattering measurements show a dynamic quantum spin ice state, with suppressed scattering near |Q|=0, and no long-range order at low temperatures. This is consistent with recent theory predicting symmetry-enriched U(1) quantum spin liquids for such DO doublets decorating the pyrochlore lattice. Finally, we show that disorder, especially oxidation of powder samples, is important in Ce_{2}Zr_{2}O_{7} and could play an important role in the low-temperature behavior of this material.

Effect of fine-tuning pore structures on the dynamics of confined water.

Confinement of water in sub-nanometer pores strongly alters its vibrational dynamics from that of bulk water. The effect of confinement can, furthermore, be finely tuned by small changes in the size and symmetry of the confining pore. Using inelastic neutron scattering (INS), we recently studied the dynamics of water confined in the channels of beryl and cordierite in which, at low temperatures, water shows similar behavior, indicating an absence of hydrogen bonds acting on the water molecule and a shallow water potential in the direction perpendicular to the channels. In addition, we observed multiple tunneling modes (between 0.66 and 14.7 meV) in the INS spectra of beryl due to transitions between the split ground-state of the water protons. Here, we present a study of (i) the effect of pressure on the dynamics of water in beryl, (ii) the dynamics of water in beryl containing alkali metals (which results in changing the orientation of the water molecule in the crystal), and (iii) the dynamics of water in cordierite at low energies. We found a shift in the tunneling and vibrational modes of water in beryl to higher energies at 22 kbar relative to 1 bar. No tunneling modes were observed for water in cordierite and type-II water in beryl. Therefore, we conclude that very small differences in the size and structure of the pores and the orientation of the water molecule in these minerals result in changes in the potential of the water protons and drastic changes in the confined water dynamics.

Fast Rotational Diffusion of Water Molecules in a 2D Hydrogen Bond Network at Cryogenic Temperatures.

Individual water molecules or small clusters of water molecules contained within microporous minerals present an extreme case of confinement where the local structure of hydrogen bond networks are dramatically altered from bulk water. In the zinc silicate hemimorphite, the water molecules form a two-dimensional hydrogen bond network with hydroxyl groups in the crystal framework. Here, we present a combined experimental and theoretical study of the structure and dynamics of water molecules within this network. The water molecules undergo a continuous phase transition in their orientational configuration analogous to a two-dimensional Ising model. The incoherent dynamic structure factor reveals two thermally activated relaxation processes, one on a subpicosecond timescale and another on a 10-100 ps timescale, between 70 and 130 K. The slow process is an in-plane reorientation of the water molecule involving the breaking of hydrogen bonds with a framework that, despite the low temperatures involved, is analogous to rotational diffusion of water molecules in the bulk liquid. The fast process is a localized motion of the water molecule with no apparent analogs among known bulk or confined phases of water.

Neutron-scattering evidence for a periodically modulated superconducting phase in the underdoped cuprate La1.905Ba0.095CuO4.

The role of antiferromagnetic spin correlations in high-temperature superconductors remains a matter of debate. We present inelastic neutron-scattering evidence that gapless spin fluctuations coexist with superconductivity in La1.905Ba0.095CuO4. Furthermore, we observe that both the low-energy magnetic spectral weight and the spin incommensurability are enhanced with the onset of superconducting correlations. We propose that the coexistence occurs through intertwining of spatial modulations of the pair wave function and the antiferromagnetic correlations. This proposal is also directly relevant to sufficiently underdoped La(2-x)Sr(x)CuO(4) and YBa(2)Cu(3)O(6+x).

Neutron scattering and neural-network quantum molecular dynamics investigation of the vibrations of ammonia along the solid-to-liquid transition.

Vibrational spectroscopy allows us to understand complex physical and chemical interactions of molecular crystals and liquids such as ammonia, which has recently emerged as a strong hydrogen fuel candidate to support a sustainable society. We report inelastic neutron scattering measurement of vibrational properties of ammonia along the solid-to-liquid phase transition with high enough resolution for direct comparisons to ab-initio simulations. Theoretical analysis reveals the essential role of nuclear quantum effects (NQEs) for correctly describing the intermolecular spectrum as well as high energy intramolecular N-H stretching modes. This is achieved by training neural network models using ab-initio path-integral molecular dynamics (PIMD) simulations, thereby encompassing large spatiotemporal trajectories required to resolve low energy dynamics while retaining NQEs. Our results not only establish the role of NQEs in ammonia but also provide general computational frameworks to study complex molecular systems with NQEs.

Spin pseudogap in Ni-doped SrCuO2.

The S=1/2 spin chain material SrCuO2 doped with 1% S=1 Ni impurities is studied by inelastic neutron scattering. At low temperatures, the spectrum shows a pseudogap Δ≈8 meV, absent in the parent compound, and not related to any structural phase transition. The pseudogap is shown to be a generic feature of quantum spin chains with dilute defects. A simple model based on this idea quantitatively accounts for the experimental data measured in the temperature range from 2 to 300 K, and allows us to represent the momentum-integrated dynamic structure factor in a universal scaling form.

[Cytoflavin in the treatment of patients with chronic abacterial prostatitis and erectile dysfunction].

The problem of chronic prostatitis (CP) and erectile dysfunction (ED) involves not only their high prevalence, but also the insufficient effectiveness of their treatments. In this regard, there is need for administration the pathogenetic drugs with antihypoxic, antioxidant and neuroprotective effects and improving blood flow to the genitals. The study included 60 men with CP associated with ED, aged 22 to 60 years. Patients were randomized into 2 groups of 30 people. Patients of comparison group received baseline therapy (alpha1-adrenoblockers, non-specific anti-inflammatory drugs, digital prostate massage and vacuum phallostimulation). Antibiotics were applied on the basis of their potential effectiveness in chronic abacterial prostatitis. In addition to the above treatment, patients of main group received step-down therapy with cytoflavin (in infusion, then oral administration). Positive dynamics was noted in both groups of patients; however, according to the indicators of the severity of pain and dysuria, as well as quality of life, positive dynamics in the main group of patients was more significant. Similarly, the dynamics of objective criteria for inflammation in the prostate gland was more pronounced when using cytoflavin. After treatment, the rigid phase of erection during vacuum fallotest occurred within 2-3 min from the beginning of the procedure in 16 (53.3%) patients of main group and only in 9 (30%) patients of comparison group. During follow-up examination at 6 months after treatment, stable remission was found in 75% of patients of main group. Thus, the inclusion of cytoflavin in the scheme of complex treatment of patients with abacterial CP associated with ED is pathogenetically justified, makes it more efficient and provides good DFS.

Singlet-triplet excitations in the unconventional spin-Peierls TiOBr compound.

We have performed time-of-flight neutron scattering measurements on powder samples of the unconventional spin-Peierls compound TiOBr using the fine-resolution Fermi chopper spectrometer (SEQUOIA) at the Spallation Neutron Source at Oak Ridge National Laboratory. These measurements reveal two branches of magnetic excitations within the commensurate and incommensurate spin-Peierls phases, which we associate with n=1 and n=2 triplet excitations out of the singlet ground state. These results represent the first direct measurement of the singlet-triplet energy gap in TiOBr, which has a value of E(g)=21.2±1.0 meV.

Simulation of Inelastic Neutron Scattering Spectra Directly from Molecular Dynamics Trajectories.

Inelastic neutron scattering (INS) is a widely used technique to study atomic and molecular vibrations. With the increasing complexity of materials and thus the INS spectra, being able to simulate the spectra from various atomistic models becomes an essential step and also a major bottleneck for INS data analysis. The conventional approach using density functional theory and lattice dynamics often falls short when the materials of interest are complex (e.g., defective, disordered, heterogeneous, amorphous, large-scale), for which molecular dynamics driven by an interatomic force field is a more common approach. In this paper, we demonstrate a method to directly convert molecular dynamics trajectories into simulated INS spectra, including not only fundamental but also higher order excitations. The results are compared with data collected on various representative samples from different neutron spectrometers. This development will open great opportunities by providing the key tool to perform in-depth analysis of INS data and to validate and optimize computer models.

Simulation of Inelastic Neutron Scattering Spectra Using OCLIMAX.

Studying the vibration of atoms is of fundamental importance and can provide critical insight for the understanding of materials behavior, such as structure and phase transition, thermodynamics, and chemical reactions. The atomic vibration can be probed using vibrational spectroscopy with various incident particles such as photons, neutrons, or electrons. A major challenge when applying these techniques is often how to interpret the vibrational spectra and how to make connections to the theory. To this end, methods that can simulate the spectra from atomistic models are highly desired. In this paper, we present a program developed for the simulation of inelastic neutron scattering spectra. It has many new and useful features that were not previously available and will greatly facilitate the analysis and understanding of inelastic neutron scattering data.

Heat capacity of α-AlH(3) and α-AlD(3) at temperatures up to 1000 K.

The densest α modification of AlH(3) and AlD(3) is thermodynamically stable at high hydrogen pressures. At ambient pressure, α-AlH(3) and α-AlD(3) rapidly and irreversibly decompose to Al and H(2) or D(2) gas when heated to about 420 and 520 K, respectively. In the present paper, the heat capacities at constant volume (C(V)) and at constant pressure (C(P)) are calculated for α-AlH(3) and α-AlD(3) at a pressure of 1 atm and temperatures 0-1000 K using the phonon densities of states determined earlier by inelastic neutron scattering at helium temperatures (Kolesnikov et al 2007 Phys. Rev. B 76 064302). The C(P)(T) dependence of AlH(3) is also measured at temperatures 6-30 K and 130-320 K and that of AlD(3) at 130-320 K in order to compensate for the scatter in the literature data and to improve the accuracy of the calculated C(V) and C(P) dependences at low temperatures.

Intermediate-valence state of the Sm and Eu in SmB6 and EuCu2Si2: neutron spectroscopy data and analysis.

Magnetic neutron scattering data for Sm (SmB6, Sm(Y)S) and Eu (EuCu2Si2-x Ge x ) intermediate-valence compounds have been analysed in terms of a generalized model of the intermediate-radius exciton. Special attention is paid to the correlation between the average ion's valence and parameters of the low-energy excitation in the neutron spectra, such as the resonance mode, including its magnetic form factor. Along with specific features of the formation of the intermediate-valence state for Sm and Eu ions, common physical mechanisms have been revealed for systems based on these elements from the middle of the rare-earth series. A consistent description of the existing experimental data has been obtained by using the concept of a loosely bound hole for the Eu f-electron shell in the intermediate-valence state, in analogy with the previously established loosely bound electron model for the Sm ion.

Observation of a dynamic crossover in water confined in double-wall carbon nanotubes.

High-resolution quasielastic neutron scattering spectroscopy was used to measure H2O hydrated double-wall carbon nanotubes (DWNT). The measurements were made at a series of temperatures from 250 K down to 150 K. The relaxing-cage model was used to analyze the quasielastic spectra. We observed clear evidence of a fragile-to-strong dynamic crossover (FSC) at T(L) = 190 K in the confined water. We further show that the mean-square atomic displacement of the hydrogen atoms in water exhibits a sharp change in slope at approximately the same temperature 190 K. Comparing the result with that obtained from the confined water in hydrophilic porous silica material MCM-41, we demonstrate experimentally that water confined in a hydrophobic substrate exhibits a lower dynamic crossover temperature by deltaT(L) approximately = 35 K.

The cold neutron chopper spectrometer at the Spallation Neutron Source-A review of the first 8 years of operation.

The first eight years of operation of the Cold Neutron Chopper Spectrometer (CNCS) at the Spallation Neutron Source in Oak Ridge is being reviewed. The instrument has been part of the facility user program since 2009, and more than 250 individual user experiments have been performed to date. CNCS is an extremely powerful and versatile instrument and offers leading edge performance in terms of beam intensity, energy resolution, and flexibility to trade one for another. Experiments are being routinely performed with the sample at extreme conditions: T ≲ 0.05 K, p ≳ 2 GPa, and B = 8 T can be achieved individually or in combination. In particular, CNCS is in a position to advance the state of the art with inelastic neutron scattering under pressure, and some of the recent accomplishments in this area will be presented in more detail.

Quantum Coherence and Temperature Dependence of the Anomalous State of Nanoconfined Water in Carbon Nanotubes.

X-ray Compton scattering measurements of the electron momentum distribution in water confined in both single-walled and double-walled carbon nanotubes (SWNT and DWNT), as a function of temperature and confinement size are presented here together with earlier measurements of the proton momentum distribution in the same systems using neutron Compton scattering. These studies provide a coherent picture of an anomalous state of water that exists because of nanoconfinement. This state cannot be described by the weakly interacting molecule picture. It has unique transport properties for both protons and water molecules. We suggest that knowledge of the excitation spectrum of this state is needed to understand the enhanced flow of water in cylinders with diameters on the order of 20 Å.

The effect of hydrazine intercalation on the structure and capacitance of 2D titanium carbide (MXene).

Herein we show that hydrazine intercalation into 2D titanium carbide (Ti3C2-based MXene) results in changes in its surface chemistry by decreasing the amounts of fluorine, OH surface groups and intercalated water. It also creates a pillaring effect between Ti3C2Tx layers pre-opening the structure and improving the accessability to active sites. The hydrazine treated material has demonstrated a greatly improved capacitance of 250 F g(-1) in acidic electrolytes with an excellent cycling ability for electrodes as thick as 75 µm.

Spin-orbit coupling control of anisotropy, ground state and frustration in 5d(2) Sr2MgOsO6.

The influence of spin-orbit coupling (SOC) on the physical properties of the 5d(2) system Sr2MgOsO6 is probed via a combination of magnetometry, specific heat measurements, elastic and inelastic neutron scattering, and density functional theory calculations. Although a significant degree of frustration is expected, we find that Sr2MgOsO6 orders in a type I antiferromagnetic structure at the remarkably high temperature of 108 K. The measurements presented allow for the first accurate quantification of the size of the magnetic moment in a 5d(2) system of 0.60(2) µB -a significantly reduced moment from the expected value for such a system. Furthermore, significant anisotropy is identified via a spin excitation gap, and we confirm by first principles calculations that SOC not only provides the magnetocrystalline anisotropy, but also plays a crucial role in determining both the ground state magnetic order and the size of the local moment in this compound. Through comparison to Sr2ScOsO6, it is demonstrated that SOC-induced anisotropy has the ability to relieve frustration in 5d(2) systems relative to their 5d(3) counterparts, providing an explanation of the high TN found in Sr2MgOsO6.

Quantum effects in the dynamics of deeply supercooled water.

Despite its simple chemical structure, water remains one of the most puzzling liquids with many anomalies at low temperatures. Combining neutron scattering and dielectric relaxation spectroscopy, we show that quantum fluctuations are not negligible in deeply supercooled water. Our dielectric measurements reveal the anomalously weak temperature dependence of structural relaxation in vapor-deposited water close to the glass transition temperature T(g)∼136K. We demonstrate that this anomalous behavior can be explained well by quantum effects. These results have significant implications for our understanding of water dynamics.

[Stage-by-stage lavage of the abdominal cavity in the treatment of diffuse suppurative peritonitis]. / Etapnye promyvaniia briushnoi polosti v lechenii rasprostranennogo gnoinogo peritonita.

The article generalizes experience in the treatment of 65 patients with generalized purulent peritonitis at the toxic and terminal stage with the use of active cleansing of the abdominal cavity by step-by-step lavage (1 to 12 times). The authors studied changes of the flora, the indices of immunological and nonspecific reactivity and central hemodynamics, the parameters of water spaces and electrolytes, and the condition of hemostasis from the peak of peritonitis to recovery. The cleansing step-by-step lavages of the abdominal cavity in generalized purulent peritonitis reduce the frequency and intensity of surgical complications, make it possible to avoid generalization of the septic process or its further development, and are, on the whole, an effective method of treatment. They may be considered to be method of choice in patients with polyorganic insufficiency.