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At least 19 records

Alpha-relaxation by scattering and medium-range atomic correlation in simple liquids

The relaxation dynamics of liquid and glass can be studied by inelastic x-ray or neutron scattering through the intermediate scattering function F(Q, t), where Q is the momentum transfer of scattering. Because of the time-consuming nature of these measurements, F(Q, t) is usually measured only at the first peak of the structure function S(Q), and its principal decay time is referred to as the α-relaxation time τ α . τ α is generally considered to describe the relaxation time of the bulk, which is related to viscosity and is controlled by the atomic cage around an atom. Here, through simulations on metallic liquids, we show that the α-relaxation time determined by scattering experiments does not purely reflect viscosity but is influenced by changes in spatial cooperativity. We also demonstrate that atomic caging is not exerted by the nearest neighbors but involves more cooperative atomic dynamics of the atomic medium-range order.

Glass transitions↗

Medium-range order and compositional correlation in metallic glasses

The compositional atomic ordering in metallic glasses was studied by simulation focusing on the medium-range order (MRO). Many metallic alloy liquids and glasses show MRO characterized by the oscillations in the atomic pair-distribution function (PDF) beyond the first peak, which decay exponentially with distance. To study the effects of the local chemical order on MRO, we examine the compositionally resolved PDF and its MRO for models of various binary metallic alloy glasses. We show that compositional ordering is limited mostly to the nearest-neighbor atoms and the MRO is largely independent of the compositional order. For some elements that strongly repel each other in the alloy, a second MRO periodicity is observed owing to the distinct correlations among them. These results are discussed in light of the idea that the MRO oscillations in the PDF describe the correlations in the atomic density fluctuations, rather than the detailed local atomic structure.

Atomic structure↗

Medium-Range Order, Density Fluctuations, and Activated Relaxation in the Equilibrated Deep Glass Regime

A successful microscopic theory of activated relaxation in metastable supercooled liquids is extended to the equilibrated deep glass regime. Surprisingly, the predicted power-law scaling connections of the dynamic barrier with diverse scalar order parameters (medium-range order correlation length, dimensionless compressibility, shear modulus) remain unchanged up to astronomically long timescales, despite a fundamental crossover of equilibrium thermodynamics and structure near the laboratory kinetic vitrification point. Quantitative tests against experiments on aged to equilibrium glass-forming liquids up to nearly 20 decades in time scale reveal good agreement. This conflicts with the idea of a crossover from super-Arrhenius to literal Arrhenius relaxation around the laboratory glass transition temperature, and supports the robustness of the theoretical idea that ultraslow dynamics is causally related to medium-range structural order. Here, new avenues of experimental and theoretical research in the deep glass regime are suggested.

Amorphous materials↗

Complexity in the medium-range order of gallium as a polyvalent liquid metal

Simplicity in chemical composition does not always translate into simplicity in the structures and dynamics of liquids and solids. Some elementary liquid metals, such as gallium, show unusual behaviors in thermodynamic and transport properties as a result of their complex atomic structure and dynamics. Here, in this work, we study the real-space atomic correlation function of liquid gallium by neutron scattering. In the pair-distribution function, there exist two kinds of medium-range order (MRO), characterized by oscillations beyond the first nearest neighbors. On the other hand, the first neighbor shell shows only one kind of bond. The two types of MRO are strongly overlapping in space and fluctuating in time. We propose that they are the basis for anomalous behavior of liquid gallium. This view challenges the current view that liquid gallium consists of fluctuating metallic and insulating domains. These findings shed light on the interpretation of similar microscopic anomalies observed in other semimetallic liquids.

Hua, Chengyun [Oak Ridge National Laboratory (ORNL↗

Temporal development of the correlation between ozone and potential vorticity in the Arctic in the winters of 1988/1989, 1989/1990, and 1990/1991

Ozone sonde data of the winters 1988/89, 1989/90, and 1990/91 from a group of Arctic stations are used in this study. The ozone mixing ratio on several isentropic surfaces is correlated to the potential vorticity (P). The P is based on the initialized analysis data from the European Center for Medium-Range Weather Forecasts. Similar investigations were made by Lait et al. (Geophys. Res. Lett., 17, 521-524, March Supplement 1990) for the AASE campaign (January and February 1989), showing how the ozone mixing ratio varies with the distance to the edge of the vortex. Their findings are confirmed and extended to the following two winters. Furthermore we have studied the temporal development of the P-ozone correlations during these winters in order to recognize any chemical ozone depletion.

Knudsen, Bjorn↗

Anisotropic structure in a vapor-deposited Pd-based metallic glass

The understanding of the structure of amorphous solids beyond nearest-neighbors has long been sought after. While recent works have demonstrated evidence for medium-range ordering and its importance for the physical properties of glassy systems, few have investigated mesoscopic structural correlations beyond a few nanometers. In this work, combining X-ray nano-diffraction with high-energy X-ray total scattering with a small focus, we have not only found structural anisotropy in a vapor-deposited Pd 77.5 Cu 6 Si 16.5 metallic glass sample which appears to show two distinct and well-defined structures in different directions, but also obtained detailed characterizations of this anisotropic structure in real space. Upon annealing, the sample loses the long-range anisotropy, and at the same time, it appears to densify with a contraction of higher-order coordination shells. In light of recent works, our results may indicate a transition between two structures in the sample with different densities, medium-range ordering, and degrees of anisotropy. We expect these results to be relevant to a larger family of metallic glass systems, where similar discoveries may be made with the use of high-quality, small-focus X-ray beams.

36 MATERIALS SCIENCE↗

Observational Evidence of a Hemispheric-wide Ice-ocean Albedo Feedback Effect on Antarctic Sea-ice Decay

The effect of ice-ocean albedo feedback (a kind of ice-albedo feedback) on sea-ice decay is demonstrated over the Antarctic sea-ice zone from an analysis of satellite-derived hemispheric sea ice concentration and European Centre for Medium-Range Weather Forecasts (ERA-40) atmospheric data for the period 1979-2001. Sea ice concentration in December (time of most active melt) correlates better with the meridional component of the wind-forced ice drift (MID) in November (beginning of the melt season) than the MID in December. This 1 month lagged correlation is observed in most of the Antarctic sea-ice covered ocean. Daily time series of ice , concentration show that the ice concentration anomaly increases toward the time of maximum sea-ice melt. These findings can be explained by the following positive feedback effect: once ice concentration decreases (increases) at the beginning of the melt season, solar heating of the upper ocean through the increased (decreased) open water fraction is enhanced (reduced), leading to (suppressing) a further decrease in ice concentration by the oceanic heat. Results obtained fi-om a simple ice-ocean coupled model also support our interpretation of the observational results. This positive feedback mechanism explains in part the large interannual variability of the sea-ice cover in summer.

Nihashi, Sohey↗

Interannual Sea Level Variations in the Tropical Indian Ocean from Geosat and Shallow Water Simulations

Sea level variations of the Indian Ocean north of 20 deg S are analyzed from Geosat satellite altimeter data over April 1985-September 1989. These variations are compared and interpreted with numerical simulations derived from a reduced gravity model forced by FSU observed winds over the same period. After decomposition into complex empirical orthogonal functions, the low-frequency anomalies are described by the first two modes for observations as well as for simulations. The sums of the two modes contain 34% and 40% of the observed and simulated variances, respectively. Averaged over the basin, the observed and simulated sea level changes are correlated by 0.92 over 1985-1988. The strongest change happens during the El Ninio 1986-1987: between winter 1986 and summer 1987 the basin-averaged sea level rises by approx. 1 cm. These low-frequency variations can partly be explained by changes in the Sverdrup circulation. The southern tropical Indian Ocean between 1O deg and 20 deg S is the domain where those changes are strongest: the averaged sea level rises by approx. 4.5 cm between winter 1986 and winter 1987. There, the signal propagates southwestward across the basin at a speed similar to free Rossby waves. Sensitivity of observed anomalies is examined over 1987-1988, with different orbit ephemeris, tropospheric corrections, and error reduction processes. The uncertainty of the basin-averaged sea level estimates is mostly due to the way the orbit error is reduced and reaches approx. 1 cm. Nonetheless, spatial correlation is good between the various observations and better than between observations and simulations. Sensitivity of simulated anomalies to the wind uncertainty, examined with Former Soviet Union (FSU) and European Center for Medium-Range Weather Forecasting (ECMWF) forcings over 1985-1988, shows that the variance of the simulations driven by ECMWF is 52% smaller, as FSU winds are stronger than ECMWF. Results show that the wind strength also affects the dynamic response of the ocean: anomalies propagate westward across the basin more than twice as fast with FSU than with ECMWF. It is found that the discrepancy is larger between ECMWF and FSU simulations than between observations and FSU simulations.

Perigaud, Claire↗

Real-space atomic dynamics in liquid gallium studied by inelastic neutron scattering

Gallium is a prototypical liquid metal and has gained renewed attention because of its unique properties. Characterizing and elucidating its atomic dynamics remains elusive despite numerous studies, primarily because of the challenges in quantifying atomic-scale dynamics in liquids. Recent developments in inelastic neutron scattering enable us to measure the Van Hove correlation function that describes the real-space motion of liquid atoms. Here, in this work, we use this approach to reveal the dynamics in gallium liquids and find the co-existence of two dynamical medium-range orders (MROs), which have a dynamical behavior distinct from that of the short-range order (SRO). We propose that these MROs are driven by global forces in the form of two density waves, as a direct consequence of the underlying competition between ionic core repulsion and valence electron cohesion. We suggest that the density wave approach is not only applicable to other metallic liquids exhibiting similar structural anomalies, but also offers a promising direction for elucidating the dynamics of complex liquids and glasses by linking electronic-state fluctuations to atomic dynamics.

Hua, Chengyun [Oak Ridge National Laboratory (ORNL↗

Prediction of monthly 700 mb heights using simulated medium-range numerical forecasts

Standardized 700 mb heights at 126 grid points over the Northern Hemisphere during 1948-80 were used to quantify the persistence of the heights from one month to the next (using various antecedent period lengths) and to determine predictive skill for calendar-month 700 mb heights using antecedent and simulated prognostic height information. The calculations showed that optimum period length and its corresponding average pattern correlation vary widely over the course of the year, being largest in summer and winter. The skill of models using simulated prog heights was found to be much superior to those using antecedent heights.

Harnack, R.↗

Exploring Structural Anisotropy in Amorphous Tb-Co via Changes in Medium-Range Ordering

Amorphous thin films grown by magnetron co-sputtering exhibit changes in atomic structure with varying growth and annealing temperatures. Structural variations influence the bulk properties of the films. Scanning nanodiffraction performed in a transmission electron microscope (TEM) is applied to amorphous Tb 17 Co 83 (a-Tb-Co) films deposited over a range of temperatures to measure relative changes in medium-range ordering (MRO). These measurements reveal an increase in MRO with higher growth temperatures and a decrease in MRO with higher annealing temperatures. The trend in MRO indicates a relationship between the growth conditions and local atomic ordering. By tilting select films, the TEM measures variations in the local atomic structure as a function of orientation within the films. The findings support claims that preferential ordering along the growth direction results from temperature-mediated adatom configurations during deposition, and that oriented MRO correlates with increased structural anisotropy, explaining the strong growth-induced perpendicular magnetic anisotropy found in rare earth–transition metal films. Beyond magnetic films, we propose the tilted FEM workflow as a method of extracting anisotropic structural information in a variety of amorphous materials with directionally dependent bulk properties, such as films with inherent bonding asymmetry grown by physical vapor deposition.

36 MATERIALS SCIENCE↗

Diabatic heating rate estimates from European Centre for Medium-Range Weather Forecasts analyses

Vertically integrated diabatic heating rate estimates (H) calculated from 32 months of European Center for Medium-Range Weather Forecasts daily analyses (May 1985-December 1987) are determined as residuals of the thermodynamic equation in pressure coordinates. Values for global, hemispheric, zonal, and grid point H are given as they vary over the time period examined. The distribution of H is compared with previous results and with outgoing longwave radiation (OLR) measurements. The most significant negative correlations between H and OLR occur for (1) tropical and Northern-Hemisphere mid-latitude oceanic areas and (2) zonal and hemispheric mean values for periods less than 90 days. Largest positive correlations are seen in periods greater than 90 days for the Northern Hemispheric mean and continental areas of North Africa, North America, northern Asia, and Antarctica. The physical basis for these relationships is discussed. An interyear comparison between 1986 and 1987 reveals the ENSO signal.

Christy, John R.↗

Evaluating the potential of short-term instrument deployment to improve distributed wind resource assessment

Distributed wind projects, which are connected at the distribution level of an electricity system or in off-grid applications to serve specific or local energy needs, often rely solely on wind resource models to establish wind speed and energy generation expectations. Historically, anemometer loan programs have provided an affordable avenue for more accurate onsite wind resource assessment, and the lowering cost of lidar systems has shown similar advantages for more recent assessments. While a full 12 months of onsite wind measurement is the standard for correcting model-based long-term wind speed estimates for utility-scale wind farms, the time and capital investment involved in gathering onsite measurements must be reconciled with the energy needs and funding opportunities that drive expedient deployment of distributed wind projects. Much literature exists to quantify the performance of correcting long-term wind speed estimates with 1 or more years of observational data, but few studies explore the impacts of correcting with months-long observational periods. This study aims to answer the question of how short you can go in terms of the observational time period needed to make impactful improvements to model-based long-term wind speed estimates. Three algorithms, multivariable linear regression, adaptive regression splines, and regression trees, are evaluated for their skill at correcting long-term wind resource estimates from the European Centre for Medium-Range Weather Forecasts Reanalysis version 5 (ERA5) using months-long periods of observational data from 66 locations across the US. On average, correction with even 1 month of observations provides significant improvement over the baseline ERA5 wind speed estimates and produces median bias magnitudes and relative errors within 0.22 m s −1 and 4 percentage points of the median bias magnitudes and relative errors achieved using the standard 12 months of data for correction. However, in cases when the shortest observational periods (1 to 2 months) used for correction are not well correlated with the overlapping ERA5 reference, the resultant long-term wind speed errors are worse than those produced using ERA5 without correction. Summer months, which are characterized by weaker relative wind speeds and standard deviations for most of the evaluation sites, tend to produce the worst results for long-term correction using months-long observations. The three tested algorithms perform similarly for long-term wind speed bias; however, regression trees perform notably worse than multivariable linear regression and adaptive regression splines in terms of correlation when using 6 months or less of observational data for correction. Translating the analysis to wind energy, median relative errors in the capacity factor are on average within 10 % using 1 month of training. If the observation period used for correction is not well correlated with the reference data, however, misrepresentation of the observed capacity factor can be substantial. The risk associated with poor correlation between the observed and reference datasets decreases with increasing training period length. In the worst-correlation scenarios, the median capacity factor relative errors from using 1, 3, and 6 months are within 47 %, 26 %, and 16 %, respectively.

17 WIND ENERGY↗

Variability of moisture in the upper troposphere as inferred from TOVS satellite observations and the ECMWF model analyses in 1989

Large-scale variability of moisture in the upper troposphere is examined using TIROS (Television Infrared Observation Satellite) Operational Vertical Sounder (TOVS) satellite observations and European Centre for Medium-Range Weather Forecasts (ECMWF) model analyses from 1989 in the latitude band from 40 deg N to 40 S. To compare these dissimilar datasets, upwelling radiances were computed for the 6-7 micrometer water vapor band from the ECMWF temperature and moisture analyses, and these computed radiances were compared to the corresponding TOVS satellite observations. The ECMWF-based radiances reproduce the general locations and seasonal cycle of the TOVS-observed moisture features, particularly after an improved convective parameterization scheme was adopted by ECMWF in May 1989. However, the ECMWF analysis scheme still results in much milder lateral moisture gradients and seasonal contrasts than indicated by the TOVS observations. Seasonally, the upper troposphere in each hemisphere dries in winter and moistens in summer, but there are regions in each hemisphere that run counter to this seasonal trend, apparently depending on continental- and monsoon-scale dynamics. Dynamically, the TOVS-observed regions of significant subtropical dryness are correlated with persistent subsidence indicated by ECMWF 300-mb vertical velocity analyses. The TOVS radiance observations indicate large variations in space and time of the upper-tropospheric moisture field, which are not fully captured by the ECMWF analyses.

Salathe, Eric P., Jr.↗

Principal modes of atmospheric circulation anomalies associated with global angular momentum fluctuations

This paper provides a description of the variability of global atmospheric angular momentum (GAM) and its relationship with principal modes of three-dimensional atmospheric circulation anomalies. The data used are 5-day mean global wind fields from the European Centre for Medium-Range Weather Forecasts initialized dataset for 1980-1989. Significant seasonal variation of GAM is observed with maxima in April and November and a minimum during late July. The amplitude of the annual cycle is largest in the upper troposphere and decreases toward the surface. Although the lower tropospheric contribution to the total angular momentum is relatively small, its annual cycle is out of phase with those of the upper atmosphere and GAM. Also identified is a distinct semiannual component, with double peaks appearing in April and November. This signal is most noticeable in the upper troposphere above the 300-mb level. The principal modes of zonal-mean angular momentum and meridional circulation anomalies and their coupled modes are obtained by using empirical orthogonal function analysis and singular value decomposition. It is shown that the leading modes of the angular momentum and meridional circulation are coupled with each other and are responsible for much of the variability in GAM. The coupled modes represent fluctuations of upper-level subtropical zonal flow, which are linked to the modulation of Hadley circulation intensity in both hemispheres. It is found that GAM is highly correlated with the first eigenvector of upper-level streamfunction anomalies, which consists of a superrotational flow in the tropics and subtropics, except over the central Pacific where a 'blocked' flow with two subtropical anticyclonic circulation cells straddling the equator is found. Much of the blocked flow is due to the establishment of dipole anomalies in the velocity potential with centers over the central Pacific and the Maritime Continent on the interannual time scale. On the intraseasonal time scale, GAM fluctuation is dominated by superrotational flow in the tropics, with the blocked flow present to a much lesser extent. The associated velocity potential anomaly has a weak dipole structure with centers over the Indian Ocean and the eastern Pacific. The implications of the above results on the total angular momentum balance of the earth-atmosphere system are also discussed.

Kang, In-Sik↗

Evaluation of water vapor distribution in general circulation models using satellite observations

This paper presents a comparison of the water vapor distribution obtained from two general circulation models, the European Centre for Medium-Range Weather Forecasts (ECMWF) model and the National Center for Atmospheric Research (NCAR) Community Climate Model (CCM), with satellite observations of total precipitable water (TPW) from Special Sensor Microwave/Imager (SSM/I) and upper tropospheric relative humidity (UTH) from GOES. Overall, both models are successful in capturing the primary features of the observed water vapor distribution and its seasonal variation. For the ECMWF model, however, a systematic moist bias in TPW is noted over well-known stratocumulus regions in the eastern subtropical oceans. Comparison with radiosonde profiles suggests that this problem is attributable to difficulties in modeling the shallowness of the boundary layer and large vertical water vapor gradients which characterize these regions. In comparison, the CCM is more successful in capturing the low values of TPW in the stratocumulus regions, although it tends to exhibit a dry bias over the eastern half of the subtropical oceans and a corresponding moist bias in the western half. The CCM also significantly overestimates the daily variability of the moisture fields in convective regions, suggesting a problem in simulating the temporal nature of moisture transport by deep convection. Comparison of the monthly mean UTH distribution indicates generally larger discrepancies than were noted for TPW owing to the greater influence of large-scale dynamical processes in determining the distribution of UTH. In particular, the ECMWF model exhibits a distinct dry bias along the Intertropical Convergence Zone (ITCZ) and a moist bias over the subtropical descending branches of the Hadley cell, suggesting an underprediction in the strength of the Hadley circulation. The CCM, on the other hand, demonstrates greater discrepancies in UTH than are observed for the ECMWF model, but none that are as clearly correlated with well-known features of the large-scale circulation.

Soden, Brian J.↗

Electron Microscopy Approaches to Unraveling the Structure of Amorphous Materials

Determining atomic structures in crystalline materials—where atoms are arranged in rigid, periodic lattices—has been highly successful using probes such as electrons, X-rays, and neutrons. In contrast, amorphous materials, despite their ubiquity and technological importance, remain far more challenging to characterize with comparable accuracy and precision. This review highlights existing, emerging, and potential (scanning) transmission electron microscopy ((S)TEM) techniques for probing short- and medium-range order in amorphous materials. Approaches ranging from high-resolution (S)TEM imaging and selected electron diffraction pattern to four-dimensional STEM (4D-STEM) based pair distribution function, fluctuation electron microscopy, tomography, ptychography, and spectroscopic methods are discussed, emphasizing their ability to provide complementary insights across multiple length scales—from sub-angstrom local environments to nanometer-scale correlations. Here, we further explore the promise of multimodal and correlative strategies, as well as the growing role of machine learning and physics-informed AI in enabling real-time, quantitative interpretation of complex structural signatures. Together, these advances point toward a future where electron microscopy not only reveals the hidden order in amorphous systems but also establishes robust structure–property relationships, paving the way for materials innovation in disordered matter.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Medium-Range Structural Order as the Driver of Activated Dynamics and Complexity Reduction in Glass-Forming Liquids

Here, we analyze in depth the Elastically Collective Nonlinear Langevin Equation theory of activated dynamics in metastable liquids to establish that the predicted inter-relationships between the alpha relaxation time, local cage and collective elastic barriers, dynamic localization length, and shear modulus are causally related within the theory to the medium range order (MRO) static correlation length. The latter grows exponentially with density for metastable hard sphere fluids and as a nonuniversal inverse power law with temperature for supercooled liquids under isobaric conditions. The physical origin of predicted connections between the alpha time and other metrics of cage order and the thermodynamic inverse dimensionless compressibility is fully established. It is discovered that although kinetic constraints from the real space first coordination shell are important for the alpha time, they are of secondary importance compared to the consequences of the more universal MRO correlations in both the modestly and deeply metastable regimes. This understanding sheds new light on the theoretical basis for, and prior successes of, the predictive mapping of chemically complex thermal liquids to effective hard sphere fluids based on matching their dimensionless compressibilities, a scheme we call “complexity reduction”. In essence, the latter is equivalent to the physical requirement that the thermal liquid MRO correlation equals that of its effective hard sphere analog. The mapping alone is shown to provide a remarkable level of quantitative predictive power for the glass transition temperature T g of 21 molecular and polymer liquids. Predictions for the chemically specific absolute magnitude and growth with cooling of the MRO correlation length are obtained and lie in the window of 2–6 nm at T g . Dynamic heterogeneity, elastic facilitation, and beyond pair structure issues are briefly discussed. Future opportunities to theoretically analyze the equilibrated deep glass regime are outlined.

cancer↗