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DOE OSTI2015

Unusual behavior in magnesium-copper cluster matter produced by helium droplet mediated deposition

We demonstrate the ability to produce core-shell nanoclusters of materials that typically undergo intermetallic reactions using helium droplet mediated deposition. Composite structures of magnesium and copper were produced by sequential condensation of metal vapors inside the 0.4 K helium droplet baths and then gently deposited onto a substrate for analysis. Upon deposition, the individual clusters, with diameters ∼5 nm, form a cluster material which was subsequently characterized using scanning and transmission electron microscopies. Results of this analysis reveal the following about the deposited cluster material: it is in the un-alloyed chemical state, it maintains a stable core-shell 5 nm structure at sub-monolayer quantities, and it aggregates into unreacted structures of ∼75 nm during further deposition. Surprisingly, high angle annular dark field scanning transmission electron microscopy images revealed that the copper appears to displace the magnesium at the core of the composite cluster despite magnesium being the initially condensed species within the droplet. This phenomenon was studied further using preliminary density functional theory which revealed that copper atoms, when added sequentially to magnesium clusters, penetrate into the magnesium cores.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Power Profile Monitoring and Tracking Evolution of System-Wide HPC Workloads

The power & energy demands of HPC machines have grown significantly. Modern exascale HPC systems require tens of megawatts of combined power for computing resources and cooling facilities at full capacity. The current energy trend is not sustainable for future HPC systems, and there is a need to work toward the energy efficiency aspect of HPC performance. Energy awareness of the HPC applications at the job level is essential for running an efficient HPC system. This work aims to develop a pipeline to provide a production-level system-wide overview of the HPC workloads' power profile while handling evolving workloads exhibiting new power trends. We developed an open-set classification model for HPC jobs based on the properties of power profiles to continuously provide a system-wide holistic view of recently completed jobs. The pipeline helps continuously monitor the job-level power usage pattern of HPC and enables us to capture the new trends in applications' power behavior. We employed a comprehensive set of techniques to generate job-level data, custom-designed feature extraction methods to extract critical features from jobs' power profiles, clustering techniques powered by generative modeling, and open-set classification for identifying job profiles into known classes or an unknown set. With extensive evaluations, we demonstrate the effectiveness of each component in our pipeline. We provide an analysis of the resulting clusters that characterize the power profile landscape of the Summit supercomputer from more than 60K jobs executed in a year. The open-set classification classifies the known data sets into known classes with high accuracy and identifies unknown data noints with over 85% accuracy.

Karimi, Ahmad Maroof↗

DOE OSTI2017

CLASH-VLT: constraints on f (R) gravity models with galaxy clusters using lensing and kinematic analyses

We perform a maximum likelihood kinematic analysis of the two dynamically relaxed galaxy clusters MACS J1206.2-0847 at z =0.44 and RXC J2248.7-4431 at z =0.35 to determine the total mass profile in modified gravity models, using a modified version of the MAMPOSSt code of Mamon, Biviano and Bou and apos;e. Our work is based on the kinematic and lensing mass profiles derived using the data from the Cluster Lensing And Supernova survey with Hubble (hereafter CLASH) and the spectroscopic follow-up with the Very Large Telescope (hereafter CLASH-VLT). We assume a spherical Navarro-Frenk-White (NFW hereafter) profile in order to obtain a constraint on the fifth force interaction range λ for models in which the dependence of this parameter on the environment is negligible at the scale considered (i.e. λ= const ) and fixing the fifth force strength to the value predicted in f (R) gravity. We then use information from lensing analysis to put a prior on the other NFW free parameters. In the case of MACSJ 1206 the joint kinematic+lensing analysis leads to an upper limit on the effective interaction range λ≤1.61 mpc at Δχ{sup 2}=2.71 on the marginalized distribution. For RXJ 2248 instead a possible tension with the ΛCDM model appears when adding lensing information, with a lower limit λ≥0.14 mpc at Δχ{sup 2}=2.71. This is consequence of the slight difference between the lensing and kinematic data, appearing in GR for this cluster, that could in principle be explained in terms of modifications of gravity. We discuss the impact of systematics and the limits of our analysis as well as future improvements of the results obtained. This work has interesting implications in view of upcoming and future large imaging and spectroscopic surveys, that will deliver lensing and kinematic mass reconstruction for a large number of galaxy clusters.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Coupling of nTRACER to COBRA-TF for full core high-fidelity analysis of VVERs

The evolution of computing clusters allows the use of high-resolution multi-physics solvers for reactor analysis. Despite the continuous expansion of VVER technology, only one other high-fidelity sub-pin multi-physics core solver is currently developed for safety analysis. To that end the Laboratory of Reactor Physics and Thermal-Hydraulics (LRT) of Paul Scherrer Institut is developing such a tool with the coupling of the neutronic code nTRACER and the sub-channel code COBRA-TF. This work follows the initial steps of the coupling and focuses to the extension of the core solver to full core VVER geometries. The X2 VVER-1000 benchmark is modeled with the novel core solver. The results are compared to the ones of a standalone nTRACER calculation where the feedbacks are provided by a simplified 1D thermal-hydraulic solver. Despite relatively good agreement in power distribution, the limitations of the simplified solver become apparent especially when comparing global temperature profiles. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2020

Dark Energy Survey Year 1 Results: Cosmological constraints from cluster abundances and weak lensing

In this work we perform a joint analysis of the counts and weak lensing signal of redMaPPer clusters selected from the Dark Energy Survey (DES) Year 1 dataset. Our analysis uses the same shear and source photometric redshifts estimates as were used in the DES combined probes analysis. Our analysis results in surprisingly low values for $S_8 =\sigma_8(\Omega_{\rm m}/0.3)^{0.5}= 0.65\pm 0.04$, driven by a low matter density parameter, $\Omega_{\rm m}=0.179^{+0.031}_{-0.038}$, with $\sigma_8-\Omega_{\rm m}$ posteriors in $2.4\sigma$ tension with the DES Y1 3x2pt results, and in $5.6\sigma$ with the Planck CMB analysis. These results include the impact of post-unblinding changes to the analysis, which did not improve the level of consistency with other data sets compared to the results obtained at the unblinding. The fact that multiple cosmological probes (supernovae, baryon acoustic oscillations, cosmic shear, galaxy clustering and CMB anisotropies), and other galaxy cluster analyses all favor significantly higher matter densities suggests the presence of systematic errors in the data or an incomplete modeling of the relevant physics. Cross checks with X-ray and microwave data, as well as independent constraints on the observable--mass relation from SZ selected clusters, suggest that the discrepancy resides in our modeling of the weak lensing signal rather than the cluster abundance. Repeating our analysis using a higher richness threshold ($\lambda \ge 30$) significantly reduces the tension with other probes, and points to one or more richness-dependent effects not captured by our model.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2022

Efficient Clustering of Software Vulnerabilities using Self Organizing Map (SOM)

The common vulnerabilities and exposures (CVE) database was created with a mission to ``identify, define, and catalog publicly disclosed cybersecurity vulnerabilities''. This rich body of information can be used to enable rapid and efficient response to secure and defend cyber operations and protect critical cyber infrastructure. The main goal of this paper is to develop a visual analytics tool to enable deep analysis of CVEs using unsupervised clustering techniques. We enhance our analysis by first mapping CVEs to hierarchical-classes in Common Weakness Enumeration (CWE) using information in the National Vulnerability Database (NVD). Both the mapping and the numerical representation of CVEs are enabled by V2W-BERT, which uses natural language processing of the extensive information in NVD to generate a large tabular database of 137,226 CVE entries from 1999 to 2020, where each CVE is represented by a vector of 768 numerical features. The vectorized data is processed by Self-Organizing Maps (SOM), which is an unsupervised machine learning technique for dimensionality reduction, visual representation and clustering. Using a Torus map of 6417 units, we achieve ~10-fold data compression of ~140k CVEs using SOM. The trained map is further clustered using standard K-means clustering into 138 clusters of CVEs. We conducted a brief investigation of the rich mapping of CVEs to best-matching-units to K-means clusters, as well as CVEs to CWEs. For example, this novel mapping provided insight into the role of CWE-59 and CWE-264 in several CVEs that is otherwise hard to explore in the original data. We conclude that our this novel approach will not only enable deep analysis of the complex relationships between CVEs and CWEs, but also a mechanism to quickly respond to and design mitigation actions for rapidly evolving vulnerabilities that have not been mapped to existing CWEs.

Panchal, Khyati↗

DOE OSTI2014

On the interaction of the PKS B1358–113 radio galaxy with the A1836 cluster

Here we present the analysis of multifrequency data gathered for the Fanaroff-Riley type-II (FR II) radio galaxy PKS B1358-113, hosted in the brightest cluster galaxy in the center of A1836. The galaxy harbors one of the most massive black holes known to date, and our analysis of the acquired optical data reveals that this black hole is only weakly active, with a mass accretion rate M-dot {sub acc}∼2×10{sup −4} M-dot {sub Edd}∼0.02 M{sub ⊙} yr{sup –1}. Based on analysis of new Chandra and XMM-Newton X-ray observations and archival radio data, and assuming the well-established model for the evolution of FR II radio galaxies, we derive the preferred range for the jet kinetic luminosity L {sub j} ∼ (1-6) × 10{sup –3} L {sub Edd} ∼ (0.5-3) × 10{sup 45} erg s{sup –1}. This is above the values implied by various scaling relations proposed for radio sources in galaxy clusters, being instead very close to the maximum jet power allowed for the given accretion rate. We also constrain the radio source lifetime as τ{sub j} ∼ 40-70 Myr, meaning the total amount of deposited jet energy E {sub tot} ∼ (2-8) × 10{sup 60} erg. We argue that approximately half of this energy goes into shock heating of the surrounding thermal gas, and the remaining 50% is deposited into the internal energy of the jet cavity. The detailed analysis of the X-ray data provides indication for the presence of a bow shock driven by the expanding radio lobes into the A1836 cluster environment. We derive the corresponding shock Mach number in the range M{sub sh}∼2--4, which is one of the highest claimed for clusters or groups of galaxies. This, together with the recently growing evidence that powerful FR II radio galaxies may not be uncommon in the centers of clusters at higher redshifts, supports the idea that jet-induced shock heating may indeed play an important role in shaping the properties of clusters, galaxy groups, and galaxies in formation. In this context, we speculate on a possible bias against detecting stronger jet-driven shocks in poorer environments, resulting from inefficient electron heating at the shock front, combined with a relatively long electron-ion temperature equilibration timescale.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

CHEMICAL COMPOSITION OF INTERMEDIATE-MASS STAR MEMBERS OF THE M6 (NGC 6405) OPEN CLUSTER

We present here the first abundance analysis of 44 late B-, A-, and F-type members of the young open cluster M6 (NGC 6405, age about 75 Myr). Low- and medium-resolution spectra, covering the 4500–5840 Å wavelength range, were obtained using the FLAMES/GIRAFFE spectrograph attached to the ESO Very Large Telescopes. We determined the atmospheric parameters using calibrations of the Geneva photometry and by adjusting the H{sub β} profiles to synthetic ones. The abundances of up to 20 chemical elements, from helium to mercury, were derived for 19 late B, 16 A, and 9 F stars by iteratively adjusting synthetic spectra to the observations. We also derived a mean cluster metallicity of [Fe/H] = 0.07 ± 0.03 dex from the iron abundances of the F-type stars. We find that for most chemical elements, the normal late B- and A-type stars exhibit larger star-to-star abundance variations than the F-type stars probably because of the faster rotation of the B and A stars. The abundances of C, O, Mg, Si, and Sc appear to be anticorrelated with that of Fe, while the opposite holds for the abundances of Ca, Ti, Cr, Mn, Ni, Y, and Ba as expected if radiative diffusion is efficient in the envelopes of these stars. In the course of this analysis, we discovered five new peculiar stars: one mild Am, one Am, and one Fm star (HD 318091, CD-32 13109, GSC 07380-01211, CP1), one HgMn star (HD 318126, CP3), and one He-weak P-rich (HD 318101, CP4) star. We also discovered a new spectroscopic binary, most likely a SB2. We performed a detailed modeling of HD 318101, the new He-weak P-rich CP star, using the Montréal stellar evolution code XEVOL which self-consistently treats all particle transport processes. Although the overall abundance pattern of this star is properly reproduced, we find that detailed abundances (in particular the high P excess) resisted modeling attempts even when a range of turbulence profiles and mass-loss rates were considered. Solutions are proposed which are still under investigation.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2017

The clustering of galaxies in the completed SDSS-III Baryon Oscillation Spectroscopic Survey: cosmological analysis of the DR12 galaxy sample

Here we present cosmological results from the final galaxy clustering data set of the Baryon Oscillation Spectroscopic Survey, part of the Sloan Digital Sky Survey III. Our combined galaxy sample comprises 1.2 million massive galaxies over an effective area of 9329 deg 2 and volume of 18.7 Gpc 3 , divided into three partially overlapping redshift slices centred at effective redshifts 0.38, 0.51 and 0.61. We measure the angular diameter distance DM and Hubble parameter H from the baryon acoustic oscillation (BAO) method, in combination with a cosmic microwave background prior on the sound horizon scale, after applying reconstruction to reduce non-linear effects on the BAO feature. Using the anisotropic clustering of the pre-reconstruction density field, we measure the product DMH from the Alcock–Paczynski (AP) effect and the growth of structure, quantified by fσ8(z), from redshift-space distortions (RSD). We combine individual measurements presented in seven companion papers into a set of consensus values and likelihoods, obtaining constraints that are tighter and more robust than those from any one method; in particular, the AP measurement from sub-BAO scales sharpens constraints from post-reconstruction BAOs by breaking degeneracy between DM and H. Combined with Planck 2016 cosmic microwave background measurements, our distance scale measurements simultaneously imply curvature ΩK = 0.0003 ± 0.0026 and a dark energy equation-of-state parameter w = -1.01 ± 0.06, in strong affirmation of the spatially flat cold dark matter (CDM) model with a cosmological constant (ΛCDM). Our RSD measurements of fσ8, at 6 per cent precision, are similarly consistent with this model. When combined with supernova Ia data, we find H0 = 67.3 ± 1.0 km s -1 Mpc -1 even for our most general dark energy model, in tension with some direct measurements. Adding extra relativistic species as a degree of freedom loosens the constraint only slightly, to H0 = 67.8 ± 1.2km s -1 Mpc -1 . Assuming flat ΛCDM, we find Ωm = 0.310 ± 0.005 and H0 = 67.6 ± 0.5 km s -1 Mpc -1 , and we find a 95 per cent upper limit of 0.16 eV c -2 on the neutrino mass sum.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Blinding multiprobe cosmological experiments

ABSTRACT The goal of blinding is to hide an experiment’s critical results – here the inferred cosmological parameters – until all decisions affecting its analysis have been finalized. This is especially important in the current era of precision cosmology, when the results of any new experiment are closely scrutinized for consistency or tension with previous results. In analyses that combine multiple observational probes, like the combination of galaxy clustering and weak lensing in the Dark Energy Survey (DES), it is challenging to blind the results while retaining the ability to check for (in)consistency between different parts of the data. We propose a simple new blinding transformation, which works by modifying the summary statistics that are input to parameter estimation, such as two-point correlation functions. The transformation shifts the measured statistics to new values that are consistent with (blindly) shifted cosmological parameters while preserving internal (in)consistency. We apply the blinding transformation to simulated data for the projected DES Year 3 galaxy clustering and weak lensing analysis, demonstrating that practical blinding is achieved without significant perturbation of internal-consistency checks, as measured here by degradation of the χ2 between the data and best-fitting model. Our blinding method’s performance is expected to improve as experiments evolve to higher precision and accuracy.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2014

Faint X-ray binaries and their optical counterparts in M31

X-ray binaries (XRBs) are probes of both star formation and stellar mass, but more importantly remain one of the only direct tracers of the compact object population. To investigate the XRB population in M31, we utilized all 121 publicly available observations of M31 totalling over 1 Ms from Chandra's ACIS instrument. We studied 83 star clusters in the bulge using the year 1 star cluster catalogue from the Panchromatic Hubble Andromeda Treasury Survey. We found 15 unique star clusters that matched to 17 X-ray point sources within 1'' (3.8 pc). This population is composed predominantly of globular cluster low-mass XRBs, with one previously unidentified star cluster X-ray source. Star clusters that were brighter and more compact preferentially hosted an X-ray source. Specifically, logistic regression showed that the F475W magnitude was the most important predictor followed by the effective radius, while color (F475W–F814W) was not statistically significant. We also completed a matching analysis of 1566 H II regions and found 10 unique matches to 9 X-ray point sources within 3'' (11 pc). The H II regions hosting X-ray point sources were on average more compact than unmatched H II regions, but logistic regression concluded that neither the radius nor Hα luminosity was a significant predictor. Four matches have no previous classification and thus are high-mass XRB candidates. A stacking analysis of both star clusters and H II regions resulted in non-detections, giving typical upper limits of ≈10{sup 32} erg s{sup –1}, which probes the quiescent XRB regime.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2024

Dark energy survey year 3 results: cosmology from galaxy clustering and galaxy–galaxy lensing in harmonic space

We present the joint tomographic analysis of galaxy-galaxy lensing and galaxy clustering in harmonic space (HS), using galaxy catalogues from the first three years of observations by the Dark Energy Survey (DES Y3). We utilize the redMaGiC and MagLim catalogues as lens galaxies and the metacalibration catalogue as source galaxies. The measurements of angular power spectra are performed using the pseudo-$C_\ell$ method, and our theoretical modelling follows the fiducial analyses performed by DES Y3 in configuration space, accounting for galaxy bias, intrinsic alignments, magnification bias, shear magnification bias and photometric redshift uncertainties. We explore different approaches for scale cuts based on non-linear galaxy bias and baryonic effects contamination. Our fiducial covariance matrix is computed analytically, accounting for mask geometry in the Gaussian term, and including non-Gaussian contributions and super-sample covariance terms. To validate our HS pipelines and covariance matrix, we used a suite of 1800 log-normal simulations. We also perform a series of stress tests to gauge the robustness of our HS analysis. In the $\Lambda$CDM model, the clustering amplitude $S_8 =\sigma _8(\Omega _m/0.3)^{0.5}$ is constrained to $S_8 = 0.704\pm 0.029$ and $S_8 = 0.753\pm 0.024$ (68 per cent C.L.) for the redMaGiC and MagLim catalogues, respectively. For the wCDM, the dark energy equation of state is constrained to $w = -1.28 \pm 0.29$ and $w = -1.26^{+0.34}_{-0.27}$, for redMaGiC and MagLim catalogues, respectively. These results are compatible with the corresponding DES Y3 results in configuration space and pave the way for HS analyses using the DES Y6 data.

(cosmology:) cosmological parameters↗

NASA NTRS1994

The metallicity of M4: Accurate spectroscopic fundamental parameters for four giants

High-quality spectra, covering the wavelength range 5480 to 7080 A, have been obtained for four giant stars in the intermediate-metallicity CN-bimodal globular cluster M4 (NGC 6121). We have employed a model atmosphere analysis that is entirely independent from cluster parameters, such as distance, age, and reddening, in order to derive accurate values for the stellar parameters effective temperature, surface gravity, and microturbulence, and for the abundance of iron relative to the Sun, (Fe/H), and of calcium, Ca/H, for each of the four stars. Detailed radiative transfer and statistical equilibrium calculations carried out for iron and calcium suggest that departures from local thermodynamic equilibrium are not significant for the purposes of our analysis. The spectroscopically derived effective temperatures for our program stars are hotter by about 200 K than existing photometric calibrations suggest. We conclude that this is due partly to the uncertain reddening of M4 and to the existing photometric temperature calibration for red giants being too cool by about 100 K. Comparison of our spectroscopic and existing photometric temperatures supports the prognosis of a significant east-west gradient in the reddening across M4. Our derived iron abundances are slightly higher than previous high-resolution studies suggested; the differences are most probably due to the different temperature scale and choice of microturbulent velocities adopted by earlier workers. The resulting value for the metallicity of M4 is (Fe/H )(sub M4) = -1.05 + or - 0.15. Based on this result, we suggest that metallicities derived in previous high-dispersion globular cluster abundance analyses could be too low by 0.2 to 0.3 dex. Our calcium abundances suggest an enhancement of calcium, an alpha element, over iron, relative to the Sun, in M4 of (Ca/H) = 0.23.

Drake, J. J.↗

NASA NTRS1986

The advanced X-ray Astrophysics Facility

The basic characteristics and capabilities of the Advanced X-ray Astrophysics Facility (AXAF) are described. The use of the AXAF to perform mass determinations in galaxies and in cluster of galaxies is discussed. The study of galaxy evolution, the interactions of galaxies with their environment, and the properties of galactic halos with the AXAF is proposed. The application of the facility to cosmological measurements, the estimation of the age of the universe, and the analysis of stars, galaxy clusters, and protogalaxies is examined.

Tananbaum, H.↗

DOE OSTI2023

Cool Cores in Clusters of Galaxies in the Dark Energy Survey

We search for the presence of cool cores in optically selected galaxy clusters from the Dark Energy Survey (DES) and investigate their prevalence as a function of redshift and cluster richness. Clusters were selected from the redMaPPer analysis of three years of DES observations that have archival Chandra X-ray observations, giving a sample of 99 clusters with a redshift range of 0.11 < z < 0.87 and a richness range of 25 < λ < 207. Using the X-ray data, the core temperature was compared to the outer temperature to identify clusters where the core temperature is a factor of 0.7 or less than the outer temperature. We found a cool core fraction of approximately 20% with no significant trend in the cool core fraction with either redshift or richness.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1989

NETRA: A parallel architecture for integrated vision systems. 1: Architecture and organization

Computer vision is regarded as one of the most complex and computationally intensive problems. An integrated vision system (IVS) is considered to be a system that uses vision algorithms from all levels of processing for a high level application (such as object recognition). A model of computation is presented for parallel processing for an IVS. Using the model, desired features and capabilities of a parallel architecture suitable for IVSs are derived. Then a multiprocessor architecture (called NETRA) is presented. This architecture is highly flexible without the use of complex interconnection schemes. The topology of NETRA is recursively defined and hence is easily scalable from small to large systems. Homogeneity of NETRA permits fault tolerance and graceful degradation under faults. It is a recursively defined tree-type hierarchical architecture where each of the leaf nodes consists of a cluster of processors connected with a programmable crossbar with selective broadcast capability to provide for desired flexibility. A qualitative evaluation of NETRA is presented. Then general schemes are described to map parallel algorithms onto NETRA. Algorithms are classified according to their communication requirements for parallel processing. An extensive analysis of inter-cluster communication strategies in NETRA is presented, and parameters affecting performance of parallel algorithms when mapped on NETRA are discussed. Finally, a methodology to evaluate performance of algorithms on NETRA is described.

Choudhary, Alok N.↗

DOE OSTI2024

Molecular dynamics study of interstitial He clusters in nickel

This study presents a molecular dynamics analysis focusing on the behavior of interstitial helium (He) clusters in nickel (Ni), examining their formation, stability, and migration energetics. Consistent with previous research, we found that the binding energies of interstitial helium within a helium cluster are positive and increase with the cluster size, indicating a preference for helium atoms to cluster together. However, our findings also reveal that while the formation energy increases monotonically with cluster size, the increase in binding energy is non-monotonic. Importantly, small He clusters were observed to be thermally unstable at reactor operational temperatures (approximately 600 K), with the He 2 cluster exhibiting instability even at room temperature. With a binding energy of 0.49 eV for a He 4 cluster, we hypothesize that for helium bubbles to form via homogeneous nucleation (i.e., through trap mutation) at reactor operating temperatures, the helium concentration must be high enough to facilitate the formation of helium clusters of at least size 4 or larger. As expected, interstitial helium and small helium clusters are highly mobile. This mobility was observed not only at room temperature but also at temperatures as low as approximately 200 K. Furthermore, the mean squared displacement method has been utilized to determine the migration barriers and the corresponding prefactors for clusters ranging from He 1 to He 6

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2015

Water transport and clustering behavior in homopolymer and graft copolymer polylactide

Polylactide is a bio-based and biodegradable polymer well-known for its renewable origins. Water sorption and clustering behavior in both a homopolymer polylactide and a graft copolymer of polylactide was studied using the quartz crystal microbalance/heat conduction calorimetry (QCM/HCC) technique. The graft copolymer, poly(1,5-cyclooctadiene-co-5-norbornene-2-methanol-graft-D,L-lactide), contained polylactide chains (95 wt.%) grafted onto a hydrophobic rubbery backbone (5 wt.%). Clustering is an important phenomenon in the study of water transport properties in polymers since the presence of water clusters can affect the water diffusivity. The HCC method using the thermal power signals and Van't Hoff's law were both employed to estimate the water sorption enthalpy. Sorption enthalpy of water in both polymers was determined to be approximately -40 kJ/mol for all water activity levels. Zimm-Lundberg analysis showed that water clusters start to form at a water activity of 0.4. The engaged species induced clustering (ENSIC) model was used to curve fit sorption isotherms and showed that the affinity among water molecules is higher than that between water molecules and polymer chains. All the methods used indicate that clustering of water molecules exists in both polymers.

36 MATERIALS SCIENCE↗