Fingerprints of hydrogen bonding in the terahertz dynamics of ethanol and water: An inelastic x-ray scattering study.

We used inelastic x-ray scattering methods to measure the terahertz spectrum of density fluctuations of ethanol in both liquid and solid phases. The results of a Bayesian inference-based lineshape analysis with a multiple excitation model and the comparison with a previous similar analysis on water indicate that the different structures induced by hydrogen bonds in ethanol and water have a profound influence on the respective dynamic responses, the latter being characterized by longer living and better resolved high-frequency acoustic excitations. In addition, we compare these findings with those obtained with an alternative approach based on the exponential expansion theory and ensuring sum rules fulfillment, demonstrating that the model's choice directly impacts the number of spectral modes detected.

Ice phonon spectra and Bayes inference: A gateway to a new understanding of terahertz sound propagation in water.

Understanding how molecules engage in collective motions in a liquid where a network of bonds exists has both fundamental and applied relevance. On the one hand, it can elucidate the "ordering" role of long-range correlations and inspire new avenues to control such order to implement sound manipulation. Water represents an ideal investigation case to unfold these general aspects, and, across the decades, it has been the focus of thorough scrutiny. Despite this investigative effort, the spectrum of terahertz density fluctuations of water largely remains a puzzle for condensed matter physicists. To unravel it, we compare previous scattering measurements of water spectra with new ones on ice. Owing to the unique asset of Bayesian inference, we draw a more detailed portrayal of the phonon response of ice. The comparison with the one of liquid water challenges the current understanding of density fluctuations in water, or more in general, of any networked liquid.

Trends and gaps in climate change and health research in North America.

The Intergovernmental Panel on Climate Change (IPCC) 5th Assessment Report (2014) assessed the state of climate change and health knowledge, globally through the Human Health: Impacts, Adaptation, and Co-Benefits Chapter and regionally through chapters, such as the North America Chapter. With IPCC's 6th Assessment Report scheduled to be released in 2021-22, we asked: how has climate change and health research in North America advanced since the IPCC's 5th Assessment Report in 2014? Specifically, we systematically identified and examined trends in the extent, range, and nature of climate-health research conducted in North America. We used a scoping review methodology to systematically identify literature and map publication trends. A search string was used to search five academic databases. Two independent reviewers first screened titles and abstracts, and then the full texts of articles for relevance. Research articles and reviews using systematic methods published since 2013 were eligible for inclusion, and no language restrictions were applied. To be included, articles had to measure and link climatic variables or hazards to health outcomes in North America. Relevant articles were analysed using descriptive statistics to explore publication trends. The number of climate-health articles has significantly increased since the last IPCC Assessment Report. Published research about climate change impacts, heat-related mortality and morbidity, and respiratory illness taking place in urban centres and in the USA continue to dominate the North American climate-health literature, reflected by the high proportion of articles published. Important research gaps on previously neglected climate-sensitive health outcomes, however, are beginning to be filled, including climate change impacts on mental health, nutrition, and foodborne disease. We also observed progress in research that included future projections of climate-health risks; however, projection research is still relatively nascent and under-studied for many climate-sensitive health outcomes in North America, and would benefit from considering social and demographic variables in models. Important research disparities in geographical coverage were noted, including research gaps in Canada and Mexico, and in rural and remote regions. Overall, these publication trends suggest an improved understanding of exposure-response relationships and future projections of climate-health risks for many climate-sensitive health outcomes in North America, which is promising and provides an evidence-base to inform the IPCC 6th Assessment Report. Despite these advancements and considering the urgent policy and practice implications, more research is needed to deepen our understanding of climate-sensitive health outcomes, as well as examine new arising issues that have limited evidence-bases. In particular, transdisciplinary and cross-sector research, that includes the social sciences, examining current and future climate-health adaptation, mitigation, and the adaptation-mitigation nexus should become a top priority for research, given the urgent need for this evidence to inform climate change policies, actions, and interventions.

Investigation of the

This Letter reports a study of the highly debated ^{10}Li structure through the d(^{9}Li,p)^{10}Li one-neutron transfer reaction at 100 MeV. The ^{10}Li energy spectrum is measured up to 4.6 MeV and angular distributions corresponding to different excitation energy regions are reported for the first time. The comparison between data and theoretical predictions, including pairing correlation effects, shows the existence of a p_{1/2} resonance at 0.45±0.03 MeV excitation energy, while no evidence for a significant s-wave contribution close to the threshold energy is observed. Moreover, two high-lying structures are populated at 1.5 and 2.9 MeV. The corresponding angular distributions suggest a significant s_{1/2} partial-wave contribution for the 1.5 MeV structure and a mixing of configurations at higher energy, with the d_{5/2} partial-wave contributing the most to the cross section.

Signatures of the Giant Pairing Vibration in the 14C and 15C atomic nuclei.

Giant resonances are collective excitation modes for many-body systems of fermions governed by a mean field, such as the atomic nuclei. The microscopic origin of such modes is the coherence among elementary particle-hole excitations, where a particle is promoted from an occupied state below the Fermi level (hole) to an empty one above the Fermi level (particle). The same coherence is also predicted for the particle-particle and the hole-hole excitations, because of the basic quantum symmetry between particles and holes. In nuclear physics, the giant modes have been widely reported for the particle-hole sector but, despite several attempts, there is no precedent in the particle-particle and hole-hole ones, thus making questionable the aforementioned symmetry assumption. Here we provide experimental indications of the Giant Pairing Vibration, which is the leading particle-particle giant mode. An immediate implication of it is the validation of the particle-hole symmetry.

Refinement of the experimental dynamic structure factor for liquid para-hydrogen and ortho-deuterium using semi-classical quantum simulation.

The dynamic structure factor of liquid para-hydrogen and ortho-deuterium in corresponding thermodynamic states (T = 20.0 K, n = 21.24 nm(-3)) and (T = 23.0 K, n = 24.61 nm(-3)), respectively, has been computed by both the Feynman-Kleinert linearized path-integral (FK-LPI) and Ring-Polymer Molecular Dynamics (RPMD) methods and compared with Inelastic X Ray Scattering spectra. The combined use of computational and experimental methods enabled us to reduce experimental uncertainties in the determination of the true sample spectrum. Furthermore, the refined experimental spectrum of para-hydrogen and ortho-deuterium is consistently reproduced by both FK-LPI and RPMD results at momentum transfers lower than 12.8 nm(-1). At larger momentum transfers the FK-LPI results agree with experiment much better for ortho-deuterium than for para-hydrogen. More specifically we found that for k ∼ 20.0 nm(-1) para-hydrogen provides a test case for improved approximations to quantum dynamics.

The dispersive behavior of collective excitations in fluids: an experimental test for the generalized collective modes theory.

The predictions of the generalized collective modes (GCM) theory on the non-hydrodynamic dispersion of collective excitations of liquids and supercritical fluids have been tested against previous inelastic x-ray scattering measurements on samples of increasing complexity. We observed a good agreement between experimental results and theoretical predictions within the hypothesis that sound propagation is adiabatic. Overall, the performed comparison provides an experimental validation of GCM predictions and shows that, even in the transition region between the hydrodynamic and the mesoscopic regimes, thermal fluctuations have a minor influence on the dispersion, whose non-hydrodynamic effects are mostly driven by viscoelastic phenomena.

Multiple-wave diffraction in high energy resolution back-reflecting x-ray optics.

We have studied the effects of multiple-wave diffraction in a novel optical scheme recently published by Shvyd'ko et al. utilizing Bragg diffraction of x rays in backscattering geometry from asymmetrically cut crystals for achieving energy resolutions beyond the intrinsic width of the Bragg reflection. By numerical simulations based on dynamic x-ray diffraction and by experimentation involving two-dimensional angular scans of the back-reflecting crystal, multiple-wave diffraction was found to contribute up to several tens percent loss of efficiency but can be avoided without degrading the energy resolution of the original scheme by careful choice of azimuthal orientation of the diffracting crystal surface and by tilting of the crystal perpendicular to the dispersion plane.

Structural and microscopic relaxations in glycerol: an inelastic x-ray scattering study.

The THz dynamics of liquid glycerol has been probed by inelastic x-ray scattering at different pressure spanning the 0.66-3 Kbar range. A comparison with ultrasound absorption results available in literature leads us to identify the presence of two different relaxations, a structural (slow) relaxation and a microscopic (fast) one. Although the former has been already thoroughly studied in glycerol by lower frequency spectroscopic techniques, no hints on the latter are so far available in literature. We observe that the characteristic timescale of this fast relaxation ranges in the sub-picosecond, tends to decrease with increasing the wave-vector and seems rather insensitive to pressure changes. Finally, the timescale and strength of the fast relaxation have a direct link revealing the microscopic, single particle, nature of the involved process.

The single particle dynamics of iodine in the Sachs-Teller regime: an inelastic x-ray scattering study.

The high frequency dynamics of liquid iodine has been investigated by deep inelastic x-ray scattering at exchanged wave-vectors (q) ranging from 2.5 to 15 Å(-1). The experimental data have been analyzed in the frame of the Sachs-Teller theory of the molecular spectrum while accounting for final state corrections to the lineshape. The performed data analysis carries insights on physical quantities as relevant as the mean rototranslational kinetic energy and the mean square Laplacian of the intermolecular potential. In both cases the measured values are consistent with corresponding theoretical expectations.

Pressure dependence of the large-scale structure of water.

We report on small-angle x-ray scattering measurements on liquid water aimed at characterizing the pressure evolution of its large-scale structure. Diffraction profiles have been fitted assuming a Lorentzian dependence on the exchanged momentum. As a result, we observe an anomalous behavior of the diffracted intensity that tends to disappear, increasing either the pressure or the temperature. This effect is discussed in detail and imputed to the ability of hydrostatic pressure to weaken hydrogen bonds.

High frequency dynamics in liquids and supercritical fluids: A comparative inelastic x-ray scattering study.

The microscopic dynamics of four prototype systems (water, ammonia, nitrogen, and neon) across the critical temperature has been investigated by means of high-resolution inelastic x-ray scattering. The experimental line shape has been described using a model based on the memory function formalism. Two main relaxations, the thermal and the structural one, were observed in all the investigated systems. We found that the microscopic mechanism driving the structural relaxation clearly changes, being mainly governed by intermolecular bond rearrangements below the critical temperature and by binary collisions above it. Moreover, we observed that the relative weight of the thermal relaxation systematically increases on approaching the critical temperature, thus allowing for the observation of a transition from an adiabatic to an isothermal regime of sound propagation. Finally, we found the presence of an additional instantaneous relaxation, likely related to the coupling between collective vibrational modes and intramolecular degrees of freedom.

High-frequency dynamics of liquid and supercritical water.

The dynamic structure factor S(Q,omega) of water has been determined by high-resolution inelastic x-ray scattering (IXS) in a momentum (Q) and energy (E) transfer range extending from 2 to 4 nm{-1} and from +/-40meV . IXS spectra have been recorded along an isobaric path (400bar) in a temperature (T) interval ranging from ambient up to supercritical (T>647K) conditions. The experimental data have been described in the frame of the generalized hydrodynamic theory, utilizing a model based on the memory function approach. This model allows identifying the active relaxation processes which affect the time decay of density fluctuations, as well as a direct determination of the Q , T , and density (rho) dependencies of the involved transport parameters. The experimental spectra are well described by considering three different relaxation processes: the thermal, the structural, and the instantaneous one. On approaching supercritical conditions, we observe that the microscopic mechanism responsible for the structural relaxation is no longer related to the making and breaking of intermolecular bonds, but to binary intermolecular collisions.

Structural and collisional relaxations in liquids and supercritical fluids.

The dynamic structure factor S(Q,omega) of both associated (water and ammonia) and simple fluids (nitrogen and neon) has been determined by high-resolution inelastic x-ray scattering in the 2-14 nm(-1) momentum transfer range. A line-shape analysis with a generalized hydrodynamic model was used to study the involved relaxation process and to characterize its strength and time scale. We observe that in the liquid phase such a process is governed by rearrangements of intermolecular bonds, whereas in the supercritical region it assumes a collisional nature.

On the anomalous behaviour of microscopic diffusion of liquid water.

We propose here a new interpretation of recent quasi-elastic neutron scattering (QENS) measurements on water. A line-shape analysis based on a stretched exponential ansatz for the time decay of density fluctuations enabled us to observe an anomalous dependence on the exchanged momentum of relevant relaxation parameters. We discuss this effect and relate it to an a priori uncorrelated anomaly, previously evidenced by diffraction measurements.

Quasielastic neutron scattering investigation of the pressure dependence of molecular motions in liquid water.

We report on a high-resolution, high-statistics, quasielastic neutron scattering (QENS) experiment on liquid water, aimed at accurately measuring the pressure dependence of the single-particle dynamic response function at low wave vector transfers, namely, from 0.26 to 1.32 A(-1). High-pressure QENS data were collected along the T = 268 K isothermal path over the rather extended pressure range of 80 up to 350 MPa, a thermodynamic region so far unexplored by this microscopic technique. The analysis of the measured line shapes enabled us to draw a consistent picture of the wave vector and pressure dependences of the diffusion mechanisms in liquid water, against which the most recent models for water dynamics can be checked. In close similarity with the case of supercooled water, the relaxing-cage model was found to provide a quantitatively more accurate description of the molecular motions and their pressure evolution in liquid water.

High-frequency longitudinal and transverse dynamics in water.

High-resolution, inelastic x-ray scattering measurements of the dynamic structure factor S (Q,omega) of liquid water have been performed for wave vectors Q between 4 and 30 nm(-1) in distinctly different thermodynamic conditions ( T=263-420 K ; at, or close to, ambient pressure and at P=2 kbar ). In agreement with previous inelastic x-ray and neutron studies, the presence of two inelastic contributions (one dispersing with Q and the other almost nondispersive) is confirmed. The study of their temperature and Q dependence provides strong support for a dynamics of liquid water controlled by the structural relaxation process. A viscoelastic analysis of the Q -dispersing mode, associated with the longitudinal dynamics, reveals that the sound velocity undergoes a complete transition from the adiabatic sound velocity ( c(0) ) (viscous limit) to the infinite-frequency sound velocity ( c(infinity) ) (elastic limit). On decreasing Q , as the transition regime is approached from the elastic side, we observe a decrease of the intensity of the second, weakly dispersing feature, which completely disappears when the viscous regime is reached. These findings unambiguously identify the second excitation to be a signature of the transverse dynamics with a longitudinal symmetry component, which becomes visible in S (Q,omega) as soon as the purely viscous regime is left.

Signatures of quantum behavior in the microscopic dynamics of liquid hydrogen and deuterium.

We discuss the microscopic dynamics and structure of liquid hydrogen and deuterium, as probed by inelastic x-ray scattering measurements. Samples are kept in corresponding thermodynamic conditions, at which classical systems are expected to exhibit the same dynamic and static responses. On the contrary, we observe clear differences revealing the onset of quantum deviations, both in the broadening of inelastic excitations and in the position of the first sharp diffraction peak. These features are discussed, compared to path-integral Monte Carlo simulations, and finally associated with the different de Broglie wavelengths of the two isotopes.

Pressure evolution of the high-frequency sound velocity in liquid water.

The high-frequency sound velocity v( infinity ) of liquid water has been determined to densities of 1.37 g/cm(3) by inelastic x-ray scattering. In comparison to the hydrodynamic sound velocity v(0), the increase of v( infinity ) with density is substantially less pronounced, indicating that, at high density, the hydrogen-bond network is decreasingly relevant to the physical properties of liquid water. Furthermore, we observe an anomaly in v( infinity ) at densities around 1.12 g/cm(3), contrasting the smooth density evolution of v(0).

Deep inelastic atomic scattering of x rays in liquid neon.

An inelastic x-ray scattering (IXS) experiment in liquid neon has been performed in the +/-100 meV exchanged energy range and at exchanged wave numbers, q, comprised between 1 and 16 A(-1). At the highest probed q's a deep inelastic scattering regime is reached where the Ne core electrons, after collision with the x rays, recoil almost freely with an effective mass equal to the Ne atomic mass. IXS in this high q regime is here shown to provide quantitative information on the atomic momentum distribution of liquid Ne, thus supplying a complementary technique to neutron scattering. There are several open problems in quantum and classical liquids which can benefit from this complementarity.