Reexamining cluster radioactivity in trans-lead nuclei with consideration of specific density distributions in daughter nuclei and clusters

NASA Astrophysics Data System (ADS)

Qian, Yibin; Ren, Zhongzhou; Ni, Dongdong

2016-08-01

We further investigate the cluster emission from heavy nuclei beyond the lead region in the framework of the preformed cluster model. The refined cluster-core potential is constructed by the double-folding integral of the density distributions of the daughter nucleus and the emitted cluster, where the radius or the diffuseness parameter in the Fermi density distribution formula is determined according to the available experimental data on the charge radii and the neutron skin thickness. The Schrödinger equation of the cluster-daughter relative motion is then solved within the outgoing Coulomb wave-function boundary conditions to obtain the decay width. It is found that the present decay width of cluster emitters is clearly enhanced as compared to that in the previous case, which involved the fixed parametrization for the density distributions of daughter nuclei and clusters. Among the whole procedure, the nuclear deformation of clusters is also introduced into the calculations, and the degree of its influence on the final decay half-life is checked to some extent. Moreover, the effect from the bubble density distribution of clusters on the final decay width is carefully discussed by using the central depressed distribution.

Structure and Stability of GeAu{sub n}, n = 1-10 clusters: A Density Functional Study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Priyanka,; Dharamvir, Keya; Sharma, Hitesh

2011-12-12

The structures of Germanium doped gold clusters GeAu{sub n} (n = 1-10) have been investigated using ab initio calculations based on density functional theory (DFT). We have obtained ground state geometries of GeAu{sub n} clusters and have it compared with Silicon doped gold clusters and pure gold clusters. The ground state geometries of the GeAu{sub n} clusters show patterns similar to silicon doped gold clusters except for n = 5, 6 and 9. The introduction of germanium atom increases the binding energy of gold clusters. The binding energy per atom of germanium doped cluster is smaller than the corresponding siliconmore » doped gold cluster. The HUMO-LOMO gap for Au{sub n}Ge clusters have been found to vary between 0.46 eV-2.09 eV. The mullikan charge analysis indicates that charge of order of 0.1e always transfers from germanium atom to gold atom.« less

Computational Investigation of the Geometrical and Electronic Structures of VGen-/0 (n = 1-4) Clusters by Density Functional Theory and Multiconfigurational CASSCF/CASPT2 Method.

PubMed

Tran, Van Tan; Nguyen, Minh Thao; Tran, Quoc Tri

2017-10-12

Density functional theory and the multiconfigurational CASSCF/CASPT2 method have been employed to study the low-lying states of VGe n -/0 (n = 1-4) clusters. For VGe -/0 and VGe 2 -/0 clusters, the relative energies and geometrical structures of the low-lying states are reported at the CASSCF/CASPT2 level. For the VGe 3 -/0 and VGe 4 -/0 clusters, the computational results show that due to the large contribution of the Hartree-Fock exact exchange, the hybrid B3LYP, B3PW91, and PBE0 functionals overestimate the energies of the high-spin states as compared to the pure GGA BP86 and PBE functionals and the CASPT2 method. On the basis of the pure GGA BP86 and PBE functionals and the CASSCF/CASPT2 results, the ground states of anionic and neutral clusters are defined, the relative energies of the excited states are computed, and the electron detachment energies of the anionic clusters are evaluated. The computational results are employed to give new assignments for all features in the photoelectron spectra of VGe 3 - and VGe 4 - clusters.

Density-based clustering analyses to identify heterogeneous cellular sub-populations

NASA Astrophysics Data System (ADS)

Heaster, Tiffany M.; Walsh, Alex J.; Landman, Bennett A.; Skala, Melissa C.

2017-02-01

Autofluorescence microscopy of NAD(P)H and FAD provides functional metabolic measurements at the single-cell level. Here, density-based clustering algorithms were applied to metabolic autofluorescence measurements to identify cell-level heterogeneity in tumor cell cultures. The performance of the density-based clustering algorithm, DENCLUE, was tested in samples with known heterogeneity (co-cultures of breast carcinoma lines). DENCLUE was found to better represent the distribution of cell clusters compared to Gaussian mixture modeling. Overall, DENCLUE is a promising approach to quantify cell-level heterogeneity, and could be used to understand single cell population dynamics in cancer progression and treatment.

Density functional theory and surface reactivity study of bimetallic AgnYm (n+m = 10) clusters

NASA Astrophysics Data System (ADS)

Hussain, Riaz; Hussain, Abdullah Ijaz; Chatha, Shahzad Ali Shahid; Hussain, Riaz; Hanif, Usman; Ayub, Khurshid

2018-06-01

Density functional theory calculations have been performed on pure silver (Agn), yttrium (Ym) and bimetallic silver yttrium clusters AgnYm (n + m = 2-10) for reactivity descriptors in order to realize sites for nucleophilic and electrophilic attack. The reactivity descriptors of the clusters, studied as a function of cluster size and shape, reveal the presence of different type of reactive sites in a cluster. The size and shape of the pure silver, yttrium and bimetallic silver yttrium cluster (n = 2-10) strongly influences the number and position of active sites for an electrophilic and/or nucleophilic attack. The trends of reactivities through reactivity descriptors are confirmed through comparison with experimental data for CO binding with silver clusters. Moreover, the adsorption of CO on bimetallic silver yttrium clusters is also evaluated. The trends of binding energies support the reactivity descriptors values. Doping of pure cluster with the other element also influence the hardness, softness and chemical reactivity of the clusters. The softness increases as we increase the number of silver atoms in the cluster, whereas the hardness decreases. The chemical reactivity increases with silver doping whereas it decreases by increasing yttrium concentration. Silver atoms are nucleophilic in small clusters but changed to electrophilic in large clusters.

On the accuracy of density-functional theory exchange-correlation functionals for H bonds in small water clusters: Benchmarks approaching the complete basis set limit

NASA Astrophysics Data System (ADS)

Santra, Biswajit; Michaelides, Angelos; Scheffler, Matthias

2007-11-01

The ability of several density-functional theory (DFT) exchange-correlation functionals to describe hydrogen bonds in small water clusters (dimer to pentamer) in their global minimum energy structures is evaluated with reference to second order Møller-Plesset perturbation theory (MP2). Errors from basis set incompleteness have been minimized in both the MP2 reference data and the DFT calculations, thus enabling a consistent systematic evaluation of the true performance of the tested functionals. Among all the functionals considered, the hybrid X3LYP and PBE0 functionals offer the best performance and among the nonhybrid generalized gradient approximation functionals, mPWLYP and PBE1W perform best. The popular BLYP and B3LYP functionals consistently underbind and PBE and PW91 display rather variable performance with cluster size.

On the accuracy of density-functional theory exchange-correlation functionals for H bonds in small water clusters: benchmarks approaching the complete basis set limit.

PubMed

Santra, Biswajit; Michaelides, Angelos; Scheffler, Matthias

2007-11-14

The ability of several density-functional theory (DFT) exchange-correlation functionals to describe hydrogen bonds in small water clusters (dimer to pentamer) in their global minimum energy structures is evaluated with reference to second order Moller-Plesset perturbation theory (MP2). Errors from basis set incompleteness have been minimized in both the MP2 reference data and the DFT calculations, thus enabling a consistent systematic evaluation of the true performance of the tested functionals. Among all the functionals considered, the hybrid X3LYP and PBE0 functionals offer the best performance and among the nonhybrid generalized gradient approximation functionals, mPWLYP and PBE1W perform best. The popular BLYP and B3LYP functionals consistently underbind and PBE and PW91 display rather variable performance with cluster size.

Analysis of the Structures and Properties of (GaSb)n (n = 4-9) Clusters through Density Functional Theory.

PubMed

Lu, Qi Liang; Luo, Qi Quan; Huang, Shou Guo; Li, Yi De; Wan, Jian Guo

2016-07-07

An optimization strategy combining global semiempirical quantum mechanical search with all-electron density functional theory was adopted to determine the lowest energy structure of (GaSb)n clusters up to n = 9. The growth pattern of the clusters differed from those of previously reported group III-V binary clusters. A cagelike configuration was found for cluster sizes n ≤ 7. The structure of (GaSb)6 deviated from that of other III-V clusters. Competition existed between core-shell and hollow cage structures of (GaSb)7. Novel noncagelike structures were energetically preferred over the cages for the (GaSb)8 and (GaSb)9 clusters. Electronic properties, such as vertical ionization potential, adiabatic electron affinities, HOMO-LUMO gaps, and average on-site charges on Ga or Sb atoms, as well as binding energies, were computed.

Source clustering in the Hi-GAL survey determined using a minimum spanning tree method

NASA Astrophysics Data System (ADS)

Beuret, M.; Billot, N.; Cambrésy, L.; Eden, D. J.; Elia, D.; Molinari, S.; Pezzuto, S.; Schisano, E.

2017-01-01

Aims: The aims are to investigate the clustering of the far-infrared sources from the Herschel infrared Galactic Plane Survey (Hi-GAL) in the Galactic longitude range of -71 to 67 deg. These clumps, and their spatial distribution, are an imprint of the original conditions within a molecular cloud. This will produce a catalogue of over-densities. Methods: The minimum spanning tree (MST) method was used to identify the over-densities in two dimensions. The catalogue was further refined by folding in heliocentric distances, resulting in more reliable over-densities, which are cluster candidates. Results: We found 1633 over-densities with more than ten members. Of these, 496 are defined as cluster candidates because of the reliability of the distances, with a further 1137 potential cluster candidates. The spatial distributions of the cluster candidates are different in the first and fourth quadrants, with all clusters following the spiral structure of the Milky Way. The cluster candidates are fractal. The clump mass functions of the clustered and isolated are statistically indistinguishable from each other and are consistent with Kroupa's initial mass function. Hi-GAL is a key-project of the Herschel Space Observatory survey (Pilbratt et al. 2010) and uses the PACS (Poglitsch et al. 2010) and SPIRE (Griffin et al. 2010) cameras in parallel mode.The catalogues of cluster candidates and potential clusters are only available at the CDS via anonymous ftp to http://cdsarc.u-strasbg.fr (http://130.79.128.5) or via http://cdsarc.u-strasbg.fr/viz-bin/qcat?J/A+A/597/A114

From Head to Sword: The Clustering Properties of Stars in Orion

NASA Astrophysics Data System (ADS)

Gomez, Mercedes; Lada, Charles J.

1998-04-01

We investigate the structure in the spatial distributions of optically selected samples of young stars in the Head (lambda Orionis) and in the Sword (Orion A) regions of the constellation of Orion with the aid of stellar surface density maps and the two-point angular correlation function. The distributions of young stars in both regions are found to be nonrandom and highly clustered. Stellar surface density maps reveal three distinct clusters in the lambda Ori region. The two-point correlation function displays significant features at angular scales that correspond to the radii and separations of the three clusters identified in the surface density maps. Most young stars in the lambda Ori region (~80%) are presently found within these three clusters, consistent with the idea that the majority of young stars in this region were formed in dense protostellar clusters that have significantly expanded since their formation. Over a scale of ~0.05d-0.5d the correlation function is well described by a single power law that increases smoothly with decreasing angular scale. This suggests that, within the clusters, the stars either are themselves hierarchically clustered or have a volume density distribution that falls steeply with radius. The relative lack of Hα emission-line stars in the one cluster in this region that contains OB stars suggests a timescale for emission-line activity of less than 4 Myr around late-type stars in the cluster and may indicate that the lifetimes of protoplanetary disks around young stellar objects are reduced in clusters containing O stars. The spatial distribution of young stars in the Orion A region is considerably more complex. The angular correlation function of the OB stars (which are mostly foreground to the Orion A molecular cloud) is very similar to that of the Hα stars (which are located mostly within the molecular cloud) and significantly different from that of the young stars in the lambda Ori region. This suggests that, although spatially separated, both populations in the Orion A region may have originated from a similar fragmentation process. Stellar surface density maps and modeling of the angular correlation function suggest that somewhat less than half of the OB and Hα stars in the Orion A cloud are presently within well-defined stellar clusters. Although all the OB stars could have originated in rich clusters, a significant fraction of the Hα stars appear to have formed outside such clusters in a more spatially dispersed manner. The close similarity of the angular correlation functions of the OB and Hα stars toward the molecular cloud, in conjunction with the earlier indications of a relatively high star formation rate and high gas pressure in this cloud, is consistent with the idea that older, foreground OB stars triggered the current episode of star formation in the Orion A cloud. One of the OB clusters (Upper Sword) that is foreground to the cloud does not appear to be associated with any of the clusterings of emission-line stars, again suggesting a timescale (<4 Myr) for emission-line activity and disk lifetimes around late-type stars born in OB clusters.

The Structure and Stability of Bn(+) Clusters

NASA Technical Reports Server (NTRS)

Ricca, Alessandra; Bauschlicher, Charles W., Jr.; Langhoff, Stephen R. (Technical Monitor)

1995-01-01

The geometries of B+n clusters for n less than 14 have been optimized using density functional theory with the B3LYP functional. The most stable structure for each cluster is planar or quasi-planar. The B3LYP fragmentation energies are calibrated using coupled cluster theory. Overall, our corrected fragmentation energies are in reasonable agreement with experiment. Our results are compared with previous theoretical results.

A density functional theory study on the structural and electronic properties of PbxSbySez (x + y + z = 2, 3) clusters

NASA Astrophysics Data System (ADS)

Peköz, Rengi˙n; Erkoç, Şaki˙r

2018-01-01

The structural and electronic properties of neutral ternary PbxSbySez clusters (x + y + z = 2, 3) in their ground states have been explored by means of density functional theory calculations. The geometric structures and binding energies are systematically explored and for the most stable configurations of each cluster type vibrational frequencies, charges on atoms, energy difference between highest occupied and lowest unoccupied molecular orbitals, and the possible dissociations channels have been analyzed. Depending on being binary or ternary cluster and composition, the most energetic structures have singlet, doublet or triplet ground states, and trimers prefer to form isosceles, equilateral or scalene triangle structure.

Dispersion- and Exchange-Corrected Density Functional Theory for Sodium Ion Hydration.

PubMed

Soniat, Marielle; Rogers, David M; Rempe, Susan B

2015-07-14

A challenge in density functional theory is developing functionals that simultaneously describe intermolecular electron correlation and electron delocalization. Recent exchange-correlation functionals address those two issues by adding corrections important at long ranges: an atom-centered pairwise dispersion term to account for correlation and a modified long-range component of the electron exchange term to correct for delocalization. Here we investigate how those corrections influence the accuracy of binding free energy predictions for sodium-water clusters. We find that the dual-corrected ωB97X-D functional gives cluster binding energies closest to high-level ab initio methods (CCSD(T)). Binding energy decomposition shows that the ωB97X-D functional predicts the smallest ion-water (pairwise) interaction energy and larger multibody contributions for a four-water cluster than most other functionals - a trend consistent with CCSD(T) results. Also, ωB97X-D produces the smallest amounts of charge transfer and the least polarizable waters of the density functionals studied, which mimics the lower polarizability of CCSD. When compared with experimental binding free energies, however, the exchange-corrected CAM-B3LYP functional performs best (error <1 kcal/mol), possibly because of its parametrization to experimental formation enthalpies. For clusters containing more than four waters, "split-shell" coordination must be considered to obtain accurate free energies in comparison with experiment.

Searching for the missing baryons in clusters

PubMed Central

Rasheed, Bilhuda; Bahcall, Neta; Bode, Paul

2011-01-01

Observations of clusters of galaxies suggest that they contain fewer baryons (gas plus stars) than the cosmic baryon fraction. This “missing baryon” puzzle is especially surprising for the most massive clusters, which are expected to be representative of the cosmic matter content of the universe (baryons and dark matter). Here we show that the baryons may not actually be missing from clusters, but rather are extended to larger radii than typically observed. The baryon deficiency is typically observed in the central regions of clusters (∼0.5 the virial radius). However, the observed gas-density profile is significantly shallower than the mass-density profile, implying that the gas is more extended than the mass and that the gas fraction increases with radius. We use the observed density profiles of gas and mass in clusters to extrapolate the measured baryon fraction as a function of radius and as a function of cluster mass. We find that the baryon fraction reaches the cosmic value near the virial radius for all groups and clusters above . This suggests that the baryons are not missing, they are simply located in cluster outskirts. Heating processes (such as shock-heating of the intracluster gas, supernovae, and Active Galactic Nuclei feedback) likely contribute to this expanded distribution. Upcoming observations should be able to detect these baryons. PMID:21321229

The cluster model of a hot dense vapor

NASA Astrophysics Data System (ADS)

Zhukhovitskii, D. I.

2015-04-01

We explore thermodynamic properties of a vapor in the range of state parameters where the contribution to thermodynamic functions from bound states of atoms (clusters) dominates over the interaction between the components of the vapor in free states. The clusters are assumed to be light and sufficiently "hot" for the number of bonds to be minimized. We use the technique of calculation of the cluster partition function for the cluster with a minimum number of interatomic bonds to calculate the caloric properties (heat capacity and velocity of sound) for an ideal mixture of the lightest clusters. The problem proves to be exactly solvable and resulting formulas are functions solely of the equilibrium constant of the dimer formation. These formulas ensure a satisfactory correlation with the reference data for the vapors of cesium, mercury, and argon up to moderate densities in both the sub- and supercritical regions. For cesium, we extend the model to the densities close to the critical one by inclusion of the clusters of arbitrary size. Knowledge of the cluster composition of the cesium vapor makes it possible to treat nonequilibrium phenomena such as nucleation of the supersaturated vapor, for which the effect of the cluster structural transition is likely to be significant.

Density-functional theory study of the geometries, stabilities, and electronic properties of Au n Rb (n = 1-10) clusters: comparison with pure gold clusters

NASA Astrophysics Data System (ADS)

Hu, Yan-Fei; Jiang, Gang; Meng, Da-Qiao

2012-01-01

The density functional method with the relativistic effective core potential has been employed to investigate systematically the geometric structures, relative stabilities, growth-pattern behavior, and electronic properties of small bimetallic Au n Rb (n = 1-10) and pure gold Au n (n ≤ 11) clusters. For the geometric structures of the Au n Rb (n = 1-10) clusters, the dominant growth pattern is for a Rb-substituted Au n +1 cluster or one Au atom capped on a Au n -1Rb cluster, and the turnover point from a two-dimensional to a three-dimensional structure occurs at n = 4. Moreover, the stability of the ground-state structures of these clusters has been examined via an analysis of the average atomic binding energies, fragmentation energies, and the second-order difference of energies as a function of cluster size. The results exhibit a pronounced even-odd alternation phenomenon. The same pronounced even-odd alternations are found for the HOMO-LUMO gap, VIPs, VEAs, and the chemical hardness. In addition, about one electron charge transfers from the Au n host to the Rb atom in each corresponding Au n Rb cluster.

Structural and electronic properties of U{sub n}O{sub m} (n=1-3,m=1-3n) clusters: A theoretical study using screened hybrid density functional theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Yu; Liu, Haitao; Zhang, Ping, E-mail: zhang-ping@iapcm.ac.cn

The structural and electronic properties of small uranium oxide clusters U{sub n}O{sub m} (n=1-3, m=1-3n) are systematically studied within the screened hybrid density functional theory. It is found that the formation of U–O–U bondings and isolated U–O bonds are energetically more stable than U–U bondings. As a result, no uranium cores are observed. Through fragmentation studies, we find that the U{sub n}O{sub m} clusters with the m/n ratio between 2 and 2.5 are very stable, hinting that UO{sub 2+x} hyperoxides are energetically stable. Electronically, we find that the O-2p states always distribute in the deep energy range, and the U-5fmore » states always distribute at the two sides of the Fermi level. The U-6d states mainly hybridize with the U-5f states in U-rich clusters, while hybridizing with O-2p states in O-rich clusters. Our work is the first one on the screened hybrid density functional theory level studying the atomic and electronic properties of the actinide oxide clusters.« less

Rhodium clustering process on defective (8,0) SWCNT: Analysis of chemical and physical properties using density functional theory

NASA Astrophysics Data System (ADS)

Ambrusi, Ruben E.; Luna, C. Romina; Sandoval, Mario G.; Bechthold, Pablo; Pronsato, M. Estela; Juan, Alfredo

2017-12-01

The Spin-polarized density functional theory is used to study the effect of a single vacancy in a (8,0) single-walled carbon nanotube (SWCNT) on the Rh clustering process. The vacancy is considered oxygenated and non-oxygenated and, in each case, different Rhn cluster sizes (n = 1-4) are taken into account. For the analysis of these systems some physical and chemical properties are calculated, such as binding energy (Eb), work function (WF), magnetic moment, charge transfer, bond length, band gap (Eg), and density of state (DOS). From this analysis it can be concluded that: a single Rh atom and Rh2 dimer are adsorbed on vacancy without oxygen, whereas Rh3 and Rh4 clusters prefer to be adsorbed on oxygenated vacancy. In all cases, Rh adsorption induces a magnetic moment. When the Rh atom and Rh2 dimer are bonded to the defective SWCNT, it has been found that they show a semiconductor behavior that could be interesting to use in the spintronic area. In the case of Rh3 and Rh4 clusters our results show a metallic behavior suggesting that these systems are good candidates for nanotube contact.

Are trinuclear superhalogens promising candidates for building blocks of novel magnetic materials? A theoretical prospect from combined broken-symmetry density functional theory and ab initio study.

PubMed

Yu, Yang; Li, Chen; Yin, Bing; Li, Jian-Li; Huang, Yuan-He; Wen, Zhen-Yi; Jiang, Zhen-Yi

2013-08-07

The structures, relative stabilities, vertical electron detachment energies, and magnetic properties of a series of trinuclear clusters are explored via combined broken-symmetry density functional theory and ab initio study. Several exchange-correlation functionals are utilized to investigate the effects of different halogen elements and central atoms on the properties of the clusters. These clusters are shown to possess stronger superhalogen properties than previously reported dinuclear superhalogens. The calculated exchange coupling constants indicate the antiferromagnetic coupling between the transition metal ions. Spin density analysis demonstrates the importance of spin delocalization in determining the strengths of various couplings. Spin frustration is shown to occur in some of the trinuclear superhalogens. The coexistence of strong superhalogen properties and spin frustration implies the possibility of trinuclear superhalogens working as the building block of new materials of novel magnetic properties.

Why do ultrasoft repulsive particles cluster and crystallize? Analytical results from density-functional theory.

PubMed

Likos, Christos N; Mladek, Bianca M; Gottwald, Dieter; Kahl, Gerhard

2007-06-14

We demonstrate the accuracy of the hypernetted chain closure and of the mean-field approximation for the calculation of the fluid-state properties of systems interacting by means of bounded and positive pair potentials with oscillating Fourier transforms. Subsequently, we prove the validity of a bilinear, random-phase density functional for arbitrary inhomogeneous phases of the same systems. On the basis of this functional, we calculate analytically the freezing parameters of the latter. We demonstrate explicitly that the stable crystals feature a lattice constant that is independent of density and whose value is dictated by the position of the negative minimum of the Fourier transform of the pair potential. This property is equivalent with the existence of clusters, whose population scales proportionally to the density. We establish that regardless of the form of the interaction potential and of the location on the freezing line, all cluster crystals have a universal Lindemann ratio Lf=0.189 at freezing. We further make an explicit link between the aforementioned density functional and the harmonic theory of crystals. This allows us to establish an equivalence between the emergence of clusters and the existence of negative Fourier components of the interaction potential. Finally, we make a connection between the class of models at hand and the system of infinite-dimensional hard spheres, when the limits of interaction steepness and space dimension are both taken to infinity in a particularly described fashion.

Relation between the Dynamics of Glassy Clusters and Characteristic Features of their Energy Landscape

NASA Astrophysics Data System (ADS)

De, Sandip; Schaefer, Bastian; Sadeghi, Ali; Sicher, Michael; Kanhere, D. G.; Goedecker, Stefan

2014-02-01

Based on a recently introduced metric for measuring distances between configurations, we introduce distance-energy (DE) plots to characterize the potential energy surface of clusters. Producing such plots is computationally feasible on the density functional level since it requires only a few hundred stable low energy configurations including the global minimum. By using standard criteria based on disconnectivity graphs and the dynamics of Lennard-Jones clusters, we show that the DE plots convey the necessary information about the character of the potential energy surface and allow us to distinguish between glassy and nonglassy systems. We then apply this analysis to real clusters at the density functional theory level and show that both glassy and nonglassy clusters can be found in simulations. It turns out that among our investigated clusters only those can be synthesized experimentally which exhibit a nonglassy landscape.

Large-Scale Structure Studies with the REFLEX Cluster Survey

NASA Astrophysics Data System (ADS)

Schuecker, P.; Bohringer, H.; Guzzo, L.; Collins, C.; Neumann, D. M.; Schindler, S.; Voges, W.

1998-12-01

First preliminary results of the ROSAT ESO Flux-Limited X-Ray (REFLEX) Cluster Survey are described. The survey covers 13,924 square degrees of the southern hemisphere. The present sample consists of about 470 rich clusters (1/3 non Abell/ACO clusters) with X-ray fluxes S >= 3.0 times 10^{-12} erg s^{-1} cm^{-2} (0.1-2.4 keV) and redshifts z <= 0.3. In contrast to other low-redshift surveys, the cumulative flux-number counts have an almost Euclidean slope. Comoving cluster number densities are found to be almost redshift-independent throughout the total survey volume. The X-ray luminosity function is well described by a Schechter function. The power spectrum of the number density fluctuations could be measured on scales up to 400 h^{-1} Mpc. A deeper survey with about 800 galaxy clusters in the same area is in progress.

Onset of carbon-carbon bonding in the Nb(5)C(y) (y = 0-6) clusters: a threshold photo-ionisation and density functional theory study.

PubMed

Dryza, Viktoras; Gascooke, Jason R; Buntine, Mark A; Metha, Gregory F

2009-02-21

We have used photo-ionisation efficiency spectroscopy to determine the ionisation potentials (IPs) of the niobium-carbide clusters, Nb(5)C(y) (y = 0-6). Of these clusters Nb(5)C(2) and Nb(5)C(3) exhibit the lowest IPs. Complementary density functional theory calculations have been performed to locate the lowest energy isomers for each cluster. By comparing the experimental IPs with those calculated for candidate isomers, the structures of the Nb(5)C(y) clusters observed in the experiment are inferred. For all these structures, the underlying Nb(5) cluster has either a "prolate" or "oblate" trigonal bipyramid geometry. Both Nb(5)C(5) and Nb(5)C(6) are shown to contain carbon-carbon bonding in the form of one and two molecular C(2) units, respectively.

A note on the accuracy of KS-DFT densities

NASA Astrophysics Data System (ADS)

Ranasinghe, Duminda S.; Perera, Ajith; Bartlett, Rodney J.

2017-11-01

The accuracy of the density of wave function methods and Kohn-Sham (KS) density functionals is studied using moments of the density, ⟨rn ⟩ =∫ ρ (r )rnd τ =∫0∞4 π r2ρ (r ) rnd r ,where n =-1 ,-2,0,1,2 ,and 3 provides information about the short- and long-range behavior of the density. Coupled cluster (CC) singles, doubles, and perturbative triples (CCSD(T)) is considered as the reference density. Three test sets are considered: boron through neon neutral atoms, two and four electron cations, and 3d transition metals. The total density and valence only density are distinguished by dropping appropriate core orbitals. Among density functionals tested, CAMQTP00 and ωB97x show the least deviation for boron through neon neutral atoms. They also show accurate eigenvalues for the HOMO indicating that they should have a more correct long-range behavior for the density. For transition metals, some density functional approximations outperform some wave function methods, suggesting that the KS determinant could be a better starting point for some kinds of correlated calculations. By using generalized many-body perturbation theory (MBPT), the convergence of second-, third-, and fourth-order KS-MBPT for the density is addressed as it converges to the infinite-order coupled cluster result. For the transition metal test set, the deviations in the KS density functional theory methods depend on the amount of exact exchange the functional uses. Functionals with exact exchange close to 25% show smaller deviations from the CCSD(T) density.

Magnetism, structures and stabilities of cluster assembled TM@Si nanotubes (TM = Cr, Mn and Fe): a density functional study.

PubMed

Dhaka, Kapil; Bandyopadhyay, Debashis

2016-08-02

The present study reports transition metal (TM = Cr, Mn and Fe) doped silicon nanotubes with tunable band structures and magnetic properties by careful selection of cluster assemblies as building blocks using the first-principles density functional theory. We found that the transition metal doping and in addition, the hydrogen termination process can stabilize the pure silicon nanoclusters or cluster assemblies and then it could be extended as magnetic nanotubes with finite magnetic moments. Study of the band structures and density of states (DOS) of different empty and TM doped nanotubes (Type 1 to Type 4) show that these nanotubes are useful as metals, semiconductors, semi-metals and half-metals. These designer magnetic materials could be useful in spintronics and magnetic devices of nanoscale order.

Studying the varied shapes of gold clusters by an elegant optimization algorithm that hybridizes the density functional tight-binding theory and the density functional theory

NASA Astrophysics Data System (ADS)

Yen, Tsung-Wen; Lim, Thong-Leng; Yoon, Tiem-Leong; Lai, S. K.

2017-11-01

We combined a new parametrized density functional tight-binding (DFTB) theory (Fihey et al. 2015) with an unbiased modified basin hopping (MBH) optimization algorithm (Yen and Lai 2015) and applied it to calculate the lowest energy structures of Au clusters. From the calculated topologies and their conformational changes, we find that this DFTB/MBH method is a necessary procedure for a systematic study of the structural development of Au clusters but is somewhat insufficient for a quantitative study. As a result, we propose an extended hybridized algorithm. This improved algorithm proceeds in two steps. In the first step, the DFTB theory is employed to calculate the total energy of the cluster and this step (through running DFTB/MBH optimization for given Monte-Carlo steps) is meant to efficiently bring the Au cluster near to the region of the lowest energy minimum since the cluster as a whole has explicitly considered the interactions of valence electrons with ions, albeit semi-quantitatively. Then, in the second succeeding step, the energy-minimum searching process will continue with a skilledly replacement of the energy function calculated by the DFTB theory in the first step by one calculated in the full density functional theory (DFT). In these subsequent calculations, we couple the DFT energy also with the MBH strategy and proceed with the DFT/MBH optimization until the lowest energy value is found. We checked that this extended hybridized algorithm successfully predicts the twisted pyramidal structure for the Au40 cluster and correctly confirms also the linear shape of C8 which our previous DFTB/MBH method failed to do so. Perhaps more remarkable is the topological growth of Aun: it changes from a planar (n =3-11) → an oblate-like cage (n =12-15) → a hollow-shape cage (n =16-18) and finally a pyramidal-like cage (n =19, 20). These varied forms of the cluster's shapes are consistent with those reported in the literature.

Why do gallium clusters have a higher melting point than the bulk?

PubMed

Chacko, S; Joshi, Kavita; Kanhere, D G; Blundell, S A

2004-04-02

Density functional molecular dynamical simulations have been performed on Ga17 and Ga13 clusters to understand the recently observed higher-than-bulk melting temperatures in small gallium clusters [Phys. Rev. Lett. 91, 215508 (2003)

Low density, resorcinol-formaldehyde aerogels

DOEpatents

Pekala, Richard W.

1991-01-01

The polycondensation of resorcinol with formaldehyde under alkaline conditions results in the formation of surface functionalized polymer "Clusters". The covalent crosslinking of these "clusters" produces gels which when processed under supercritical conditions, produce low density, organic aerogels (density.ltoreq.100 mg/cc; cell size .ltoreq.0.1 microns). The aerogels are transparent, dark red in color and consist of interconnected colloidal-like particles with diameters of about 100.circle.. These aerogels may be further carbonized to form low density carbon foams with cell size of about 0.1 micron.

Low density, resorcinol-formaldehyde aerogels

DOEpatents

Pekala, Richard W.

1989-01-01

The polycondensation of resorcinol with formaldehyde under alkaline conditions results in the formation of surface functionalized polymer "clusters". The covalent crosslinking of these "clusters" produces gels which when processed under supercritical conditions, produce low density, organic aerogels (density .ltoreq.100 mg/cc; cell size .ltoreq.0.1 microns). The aerogels are transparent, dark red in color and consist of interconnected colloidal-like particles with diameters of about 100 .ANG.. These aerogels may be further carbonized to form low density carbon foams with cell size of about 0.1 micron.

Low density, resorcinol-formaldehyde aerogels

DOEpatents

Pekala, R.W.

1989-10-10

The polycondensation of resorcinol with formaldehyde under alkaline conditions results in the formation of surface functionalized polymer clusters. The covalent crosslinking of these clusters produces gels which when processed under supercritical conditions, produce low density, organic aerogels (density [<=]100 mg/cc; cell size [<=]0.1 microns). The aerogels are transparent, dark red in color and consist of interconnected colloidal-like particles with diameters of about 100 [angstrom]. These aerogels may be further carbonized to form low density carbon foams with cell size of about 0.1 micron.

Threshold photoionization and density functional theory studies of bimetallic-carbide nanocrystals and fragments: Ta3ZrC(y) (y = 0-4).

PubMed

Dryza, V; Metha, G F

2009-06-28

Gas-phase bimetallic tantalum-zirconium-carbide clusters are generated using a constructed double ablation cluster source. The Ta(3)ZrC(y) (y = 0-4) clusters are examined by photoionization efficiency spectroscopy to extract experimental ionization energies (IEs). The IE trend for the Ta(3)ZrC(y) cluster series is reasonably similar to that of the Ta(4)C(y) cluster series [V. Dryza et al., J. Phys. Chem. A 109, 11180 (2005)], although the IE reductions upon carbon addition are greater for the former. Complementary density functional theory calculations are performed for the various isomers constructed by attaching carbon atoms to the different faces of the tetrahedral Ta(3)Zr cluster. The good agreement between the experimental IE trend and that calculated for these isomers support a 2x2x2 face centered cubic nanocrystal structure for Ta(4)ZrC(4) and nanocrystal fragment structures for the smaller clusters.

Density functional study on structure and stability of bimetallic AuNZn (N<=6) clusters and their cations

NASA Astrophysics Data System (ADS)

Tanaka, Hiromasa; Neukermans, Sven; Janssens, Ewald; Silverans, Roger E.; Lievens, Peter

2003-10-01

A systematic study on the structure and stability of zinc doped gold clusters has been performed by density functional theory calculations. All the lowest-energy isomers found have a planar structure and resemble pure gold clusters in shape. Stable isomers tend to equally delocalize valence s electrons of the constituent atoms over the entire structure and maximize the number of Au-Zn bonds in the structure. This is because the Au-Zn bond is stronger than the Au-Au bond and gives an extra σ-bonding interaction by the overlap between vacant Zn 4p and valence Au 6s(5d) orbitals. No three-dimensional isomers were found for Au5Zn+ and Au4Zn clusters containing six delocalized valence electrons. This result reflects that these clusters have a magic number of delocalized electrons for two-dimensional systems. Calculated vertical ionization energies and dissociation energies as a function of the cluster size show odd-even behavior, in agreement with recent mass spectrometric observations [Tanaka et al., J. Am. Chem. Soc. 125, 2862 (2003)].

Course 4: Density Functional Theory, Methods, Techniques, and Applications

NASA Astrophysics Data System (ADS)

Chrétien, S.; Salahub, D. R.

Contents 1 Introduction 2 Density functional theory 2.1 Hohenberg and Kohn theorems 2.2 Levy's constrained search 2.3 Kohn-Sham method 3 Density matrices and pair correlation functions 4 Adiabatic connection or coupling strength integration 5 Comparing and constrasting KS-DFT and HF-CI 6 Preparing new functionals 7 Approximate exchange and correlation functionals 7.1 The Local Spin Density Approximation (LSDA) 7.2 Gradient Expansion Approximation (GEA) 7.3 Generalized Gradient Approximation (GGA) 7.4 meta-Generalized Gradient Approximation (meta-GGA) 7.5 Hybrid functionals 7.6 The Optimized Effective Potential method (OEP) 7.7 Comparison between various approximate functionals 8 LAP correlation functional 9 Solving the Kohn-Sham equations 9.1 The Kohn-Sham orbitals 9.2 Coulomb potential 9.3 Exchange-correlation potential 9.4 Core potential 9.5 Other choices and sources of error 9.6 Functionality 10 Applications 10.1 Ab initio molecular dynamics for an alanine dipeptide model 10.2 Transition metal clusters: The ecstasy, and the agony... 10.3 The conversion of acetylene to benzene on Fe clusters 11 Conclusions

The cluster model of a hot dense vapor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhukhovitskii, D. I., E-mail: dmr@ihed.ras.ru

2015-04-28

We explore thermodynamic properties of a vapor in the range of state parameters where the contribution to thermodynamic functions from bound states of atoms (clusters) dominates over the interaction between the components of the vapor in free states. The clusters are assumed to be light and sufficiently “hot” for the number of bonds to be minimized. We use the technique of calculation of the cluster partition function for the cluster with a minimum number of interatomic bonds to calculate the caloric properties (heat capacity and velocity of sound) for an ideal mixture of the lightest clusters. The problem proves tomore » be exactly solvable and resulting formulas are functions solely of the equilibrium constant of the dimer formation. These formulas ensure a satisfactory correlation with the reference data for the vapors of cesium, mercury, and argon up to moderate densities in both the sub- and supercritical regions. For cesium, we extend the model to the densities close to the critical one by inclusion of the clusters of arbitrary size. Knowledge of the cluster composition of the cesium vapor makes it possible to treat nonequilibrium phenomena such as nucleation of the supersaturated vapor, for which the effect of the cluster structural transition is likely to be significant.« less

Density functional study of the structural, electronic, and magnetic properties of Mo n and Mo n S ( n = 1 - 10) clusters

NASA Astrophysics Data System (ADS)

Ziane, M.; Amitouche, F.; Bouarab, S.; Vega, A.

2017-12-01

Structural and electronic properties of pure molybdenum Mo n and molybdenum-sulfide Mo n S ( n = 1 - 10) clusters were investigated in the framework of the density functional theory within the generalized gradient approximation to exchange and correlation with the aim of addressing how doping with a single S atom affects the geometries, magnetic properties, and reactivity of pure molybdenum clusters. These clusters exhibit a less marked tendency to dimerization than their isoelectronic Cr counterparts despite sharing their half-filled valence shell configuration. Doping with a single S impurity is enough to change the structure of the host molybdenum cluster to a large extent, as well as to modify the bonding pattern, the magnetic state and the magnetic moment distribution in the Mo host. Vertical ionization potentials and electron affinities are calculated to determine global reactivity indicators like the electronegativity and the chemical hardness. The results are discussed in terms of the thermodynamical and relative stabilities, charge transfer effects, and spin-polarized densities of electronic states.

Stable isomers and electronic, vibrational, and optical properties of WS2 nano-clusters: A first-principles study

NASA Astrophysics Data System (ADS)

Hafizi, Roohollah; Hashemifar, S. Javad; Alaei, Mojtaba; Jangrouei, MohammadReza; Akbarzadeh, Hadi

2016-12-01

In this paper, we employ an evolutionary algorithm along with the full-potential density functional theory (DFT) computations to perform a comprehensive search for the stable structures of stoichiometric (WS2)n nano-clusters (n = 1 - 9), within three different exchange-correlation functionals. Our results suggest that n = 5 and 8 are possible candidates for the low temperature magic sizes of WS2 nano-clusters while at temperatures above 500 Kelvin, n = 7 exhibits a comparable relative stability with n = 8. The electronic properties and energy gap of the lowest energy isomers were computed within several schemes, including semilocal Perdew-Burke-Ernzerhof and Becke-Lee-Yang-Parr functionals, hybrid B3LYP functional, many body based DFT+GW approach, ΔSCF method, and time dependent DFT calculations. Vibrational spectra of the lowest lying isomers, computed by the force constant method, are used to address IR spectra and thermal free energy of the clusters. Time dependent density functional calculation in a real time domain is applied to determine the full absorption spectra and optical gap of the lowest energy isomers of the WS2 nano-clusters.

A density functional global optimisation study of neutral 8-atom Cu-Ag and Cu-Au clusters

NASA Astrophysics Data System (ADS)

Heard, Christopher J.; Johnston, Roy L.

2013-02-01

The effect of doping on the energetics and dimensionality of eight atom coinage metal subnanometre particles is fully resolved using a genetic algorithm in tandem with on the fly density functional theory calculations to determine the global minima (GM) for Cu n Ag(8- n) and Cu n Au(8- n) clusters. Comparisons are made to previous ab initio work on mono- and bimetallic clusters, with excellent agreement found. Charge transfer and geometric arguments are considered to rationalise the stability of the particular permutational isomers found. An interesting transition between three dimensional and two dimensional GM structures is observed for copper-gold clusters, which is sharper and appears earlier in the doping series than is known for gold-silver particles.

Excitons in Potassium Bromide: A Study using Embedded Time-dependent Density Functional Theory and Equation-of-Motion Coupled Cluster Methods

DOE Office of Scientific and Technical Information (OSTI.GOV)

Govind, Niranjan; Sushko, Petr V.; Hess, Wayne P.

2009-03-05

We present a study of the electronic excitations in insulating materials using an embedded- cluster method. The excited states of the embedded cluster are studied systematically using time-dependent density functional theory (TDDFT) and high-level equation-of-motion coupled cluster (EOMCC) methods. In particular, we have used EOMCC models with singles and doubles (EOMCCSD) and two approaches which account for the e®ect of triply excited con¯gurations in non-iterative and iterative fashions. We present calculations of the lowest surface excitations of the well-studied potassium bromide (KBr) system and compare our results with experiment. The bulk-surface exciton shift is also calculated at the TDDFT levelmore » and compared with experiment.« less

Onset of carbon-carbon bonding in Ta(5)C(y) (y = 0-6) clusters: a threshold photoionization and density functional theory study.

PubMed

Dryza, Viktoras; Alvino, Jason F; Metha, Gregory F

2010-04-01

We have used photoionization efficiency spectroscopy to determine ionization energies (IEs) of the gas-phase tantalum-carbide clusters Ta(5)C(y) (y = 0-6). The structures of the clusters observed in the experiment are assigned by comparing the experimental IEs with those of candidate isomers, calculated by density functional theory. Two competing geometries of the underlying Ta(5) cluster are found to be present in the assigned Ta(5)C(y) structures; either a "prolate" or "distorted oblate" trigonal bipyramid geometry. The onset of carbon-carbon bonding in the Ta(5)C(y) series is proposed to occur at y = 6, with the structure of Ta(5)C(6) containing two molecular C(2) units.

Assessment of the Density Functional Tight Binding Method for Protic Ionic Liquids

PubMed Central

2015-01-01

Density functional tight binding (DFTB), which is ∼100–1000 times faster than full density functional theory (DFT), has been used to simulate the structure and properties of protic ionic liquid (IL) ions, clusters of ions and the bulk liquid. Proton affinities for a wide range of IL cations and anions determined using DFTB generally reproduce G3B3 values to within 5–10 kcal/mol. The structures and thermodynamic stabilities of n-alkyl ammonium nitrate clusters (up to 450 quantum chemical atoms) predicted with DFTB are in excellent agreement with those determined using DFT. The IL bulk structure simulated using DFTB with periodic boundary conditions is in excellent agreement with published neutron diffraction data. PMID:25328497

Thermodynamically accessible titanium clusters TiN, N = 2-32.

PubMed

Lazauskas, Tomas; Sokol, Alexey A; Buckeridge, John; Catlow, C Richard A; Escher, Susanne G E T; Farrow, Matthew R; Mora-Fonz, David; Blum, Volker W; Phaahla, Tshegofatso M; Chauke, Hasani R; Ngoepe, Phuti E; Woodley, Scott M

2018-05-10

We have performed a genetic algorithm search on the tight-binding interatomic potential energy surface (PES) for small TiN (N = 2-32) clusters. The low energy candidate clusters were further refined using density functional theory (DFT) calculations with the PBEsol exchange-correlation functional and evaluated with the PBEsol0 hybrid functional. The resulting clusters were analysed in terms of their structural features, growth mechanism and surface area. The results suggest a growth mechanism that is based on forming coordination centres by interpenetrating icosahedra, icositetrahedra and Frank-Kasper polyhedra. We identify centres of coordination, which act as centres of bulk nucleation in medium sized clusters and determine the morphological features of the cluster.

Cluster perturbation theory for calculation of electronic properties of ensembles of metal nanoclusters

NASA Astrophysics Data System (ADS)

Zhumagulov, Yaroslav V.; Krasavin, Andrey V.; Kashurnikov, Vladimir A.

2018-05-01

The method is developed for calculation of electronic properties of an ensemble of metal nanoclusters with the use of cluster perturbation theory. This method is applied to the system of gold nanoclusters. The Greens function of single nanocluster is obtained by ab initio calculations within the framework of the density functional theory, and then is used in Dyson equation to group nanoclusters together and to compute the Greens function as well as the electron density of states of the whole ensemble. The transition from insulator state of a single nanocluster to metallic state of bulk gold is observed.

Local density variation of gold nanoparticles in aquatic environments

NASA Astrophysics Data System (ADS)

Hosseinzadeh, F.; Shirazian, F.; Shahsavari, R.; Khoei, A. R.

2016-10-01

Gold (Au) nanoparticles are widely used in diagnosing cancer, imaging, and identification of therapeutic methods due to their particular quantum characteristics. This research presents different types of aqueous models and potentials used in TIP3P, to study the effect of the particle size and density of Au clusters in aquatic environments; so it can be useful to facilitate future investigation of the interaction of proteins with Au nanoparticles. The EAM potential is used to model the structure of gold clusters. It is observed that in the systems with identical gold/water density and different cluster radii, gold particles are distributed in aqueous environment almost identically. Thus, Au particles have identical local densities, and the root mean square displacement (RMSD) increases with a constant slope. However in systems with constant cluster radii and different gold/water densities, Au particle dispersion increases with density; as a result, the local density decreases and the RMSD increases with a larger slope. In such systems, the larger densities result in more blunted second peaks in gold-gold radial distribution functions, owing to more intermixing of the clusters and less FCC crystalline features at longer range, a mechanism that is mediated by the competing effects of gold-water and gold-gold interactions.

Nucleation and growth of Ag on Sb-terminated Ge( 1 0 0 )

NASA Astrophysics Data System (ADS)

Chan, L. H.; Altman, E. I.

2002-06-01

The effect of Sb on Ag growth on Ge(1 0 0) was characterized using scanning tunneling microscopy, low energy electron diffraction, and Auger electron spectroscopy. Silver was found to immediately form three-dimensional clusters on the Sb-covered surface over the entire temperature range studied (320-570 K), thus the growth was Volmer-Weber. Regardless of the deposition conditions, there was no evidence that Sb segregated to the Ag surface, despite Sb having a lower surface tension than either Ag or Ge. The failure of Sb to segregate to the surface could be understood in terms of the much stronger interaction between Sb and Ge versus Ag and Ge creating a driving force to maintain an Sb-Ge interface. Silver nucleation on Sb/Ge(1 0 0) was characterized by measuring the Ag cluster density as a function of deposition rate. The results revealed that the cluster density was nearly independent of the deposition rate below 420 K, indicating that heterogeneous nucleation at defects in the Sb-terminated surface competed with homogeneous nucleation. At higher temperatures, the defects were less effective in trapping diffusing Ag atoms and the dependence of the cluster density on deposition rate suggested a critical size of at least two. For temperatures above 420 K, the Ag diffusion barrier plus the dissociation energy of the critical cluster was estimated by measuring the cluster density as a function of temperature; the results suggested a value of 0.84±0.1 eV which is significantly higher than values reported for Ag nucleation on Sb-free surfaces. In comparison to the bare Ge surface, Ag formed a higher density of smaller, lower clusters when Sb was present. Below 420 K the higher cluster density could be attributed to nucleation at defects in the Sb layer while at higher temperatures the high diffusion barrier restricted the cluster size and density. Although Sb does not act as a surfactant in this system since it does not continuously float to the surface and the growth is not layer-by-layer, adding Sb was found to be useful in limiting the Ag cluster size and height which led to smoother, more continuous Ag films and in preventing the formation of metastable Ag-Ge surface alloys.

Psi4 1.1: An Open-Source Electronic Structure Program Emphasizing Automation, Advanced Libraries, and Interoperability.

PubMed

Parrish, Robert M; Burns, Lori A; Smith, Daniel G A; Simmonett, Andrew C; DePrince, A Eugene; Hohenstein, Edward G; Bozkaya, Uğur; Sokolov, Alexander Yu; Di Remigio, Roberto; Richard, Ryan M; Gonthier, Jérôme F; James, Andrew M; McAlexander, Harley R; Kumar, Ashutosh; Saitow, Masaaki; Wang, Xiao; Pritchard, Benjamin P; Verma, Prakash; Schaefer, Henry F; Patkowski, Konrad; King, Rollin A; Valeev, Edward F; Evangelista, Francesco A; Turney, Justin M; Crawford, T Daniel; Sherrill, C David

2017-07-11

Psi4 is an ab initio electronic structure program providing methods such as Hartree-Fock, density functional theory, configuration interaction, and coupled-cluster theory. The 1.1 release represents a major update meant to automate complex tasks, such as geometry optimization using complete-basis-set extrapolation or focal-point methods. Conversion of the top-level code to a Python module means that Psi4 can now be used in complex workflows alongside other Python tools. Several new features have been added with the aid of libraries providing easy access to techniques such as density fitting, Cholesky decomposition, and Laplace denominators. The build system has been completely rewritten to simplify interoperability with independent, reusable software components for quantum chemistry. Finally, a wide range of new theoretical methods and analyses have been added to the code base, including functional-group and open-shell symmetry adapted perturbation theory, density-fitted coupled cluster with frozen natural orbitals, orbital-optimized perturbation and coupled-cluster methods (e.g., OO-MP2 and OO-LCCD), density-fitted multiconfigurational self-consistent field, density cumulant functional theory, algebraic-diagrammatic construction excited states, improvements to the geometry optimizer, and the "X2C" approach to relativistic corrections, among many other improvements.

A density functional study of second-row dicarbides C2X (X = Na-Cl) with carbon monosulfide molecule: molecular structure and bonding mechanism

NASA Astrophysics Data System (ADS)

Parida, Saroj K.; Sahu, Sridhar

2018-05-01

In present work, a systematic study regarding molecular structure, and bonding mechanism of carbon monosulfide (CS) on second-row dicarbides C2X with (X = Na-Cl) has been investigated within the framework of density functional theory (DFT). In presence of carbon monosulfide molecule, the structures of C2Na, C2Mg, C2Al, and C2Si are found be changed from cyclic to linear, whereas geometries of C2P, C2S, and C2Cl clusters are almost remain unchanged. Interestingly, the bare carbon monosulfide molecule is attached with carbon site of bare C2X clusters rather than the second-row elements (X = Na-Cl). Furthermore, the nature of bonding in C2XCS clusters has been studiedthrough Bader's topological analysis of the electron charge density distribution ρ(r), Laplacian ∇2 ρ(r) and total energy density H BCP at the bond critical points (BCPs) of the clusters within the framework of the atoms in molecules theory (AIM). In C2XCS clusters, electron density at the bond critical point ρ(r) > 0.30 a.u. with negative values of Laplacian ∇2 ρ(r) indicates shared-kind of interactions between both the carbon atoms of C2X and CS molecule. In addition, we also analyze IR spectra that could assist for the experimental detection.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schuetrumpf, Bastian; Zhang, Chunli; Nazarewicz, Witold

Nuclear density functional theory is the tool of choice in describing properties of complex nuclei and intricate phases of bulk nucleonic matter. It is a microscopic approach based on an energy density functional representing the nuclear interaction. An attractive feature of nuclear DFT is that it can be applied to both finite nuclei and pasta phases appearing in the inner crust of neutron stars. While nuclear pasta clusters in a neutron star can be easily characterized through their density distributions, the level of clustering of nucleons in a nucleus can often be difficult to assess. To this end, we usemore » the concept of nucleon localization. We demonstrate that the localization measure provides us with fingerprints of clusters in light and heavy nuclei, including fissioning systems. Furthermore we investigate the rod-like pasta phase using twist-averaged boundary conditions, which enable calculations in finite volumes accessible by state of the art DFT solvers.« less

Methanol clusters (CH3OH)n: putative global minimum-energy structures from model potentials and dispersion-corrected density functional theory.

PubMed

Kazachenko, Sergey; Bulusu, Satya; Thakkar, Ajit J

2013-06-14

Putative global minima are reported for methanol clusters (CH3OH)n with n ≤ 15. The predictions are based on global optimization of three intermolecular potential energy models followed by local optimization and single-point energy calculations using two variants of dispersion-corrected density functional theory. Recurring structural motifs include folded and/or twisted rings, folded rings with a short branch, and stacked rings. Many of the larger structures are stabilized by weak C-H···O bonds.

Cool Core Bias in Sunyaev-Zel’dovich Galaxy Cluster Surveys

DOE PAGES

Lin, Henry W.; McDonald, Michael; Benson, Bradford; ...

2015-03-18

Sunyaev-Zeldovich (SZ) surveys find massive clusters of galaxies by measuring the inverse Compton scattering of cosmic microwave background off of intra-cluster gas. The cluster selection function from such surveys is expected to be nearly independent of redshift and cluster astrophysics. In this work, we estimate the effect on the observed SZ signal of centrally-peaked gas density profiles (cool cores) and radio emission from the brightest cluster galaxy (BCG) by creating mock observations of a sample of clusters that span the observed range of classical cooling rates and radio luminosities. For each cluster, we make simulated SZ observations by the Southmore » Pole Telescope and characterize the cluster selection function, but note that our results are broadly applicable to other SZ surveys. We find that the inclusion of a cool core can cause a change in the measured SPT significance of a cluster between 0.01%–10% at z > 0.3, increasing with cuspiness of the cool core and angular size on the sky of the cluster (i.e., decreasing redshift, increasing mass). We provide quantitative estimates of the bias in the SZ signal as a function of a gas density cuspiness parameter, redshift, mass, and the 1.4 GHz radio luminosity of the central AGN. Based on this work, we estimate that, for the Phoenix cluster (one of the strongest cool cores known), the presence of a cool core is biasing the SZ significance high by ~6%. The ubiquity of radio galaxies at the centers of cool core clusters will offset the cool core bias to varying degrees« less

Probing the structural and electronic properties of cationic rubidium-gold clusters: [AunRb]+ (n = 1-10)

NASA Astrophysics Data System (ADS)

Zhao, Ya-Ru; Zhang, Hai-Rong; Qian, Yu; Duan, Xu-Chao; Hu, Yan-Fei

2016-03-01

Density functional theory has been applied to study the geometric structures, relative stabilities, and electronic properties of cationic [AunRb]+ and Aun + 1+ (n = 1-10) clusters. For the lowest energy structures of [AunRb]+ clusters, the planar to three-dimensional transformation is found to occur at cluster size n = 4 and the Rb atoms prefer being located at the most highly coordinated position. The trends of the averaged atomic binding energies, fragmentation energies, second-order difference of energies, and energy gaps show pronounced even-odd alternations. It indicated that the clusters containing odd number of atoms maintain greater stability than the clusters in the vicinity. In particular, the [Au6Rb]+ clusters are the most stable isomer for [AunRb]+ clusters in the region of n = 1-10. The charges in [AunRb]+ clusters transfer from the Rb atoms to Aun host. Density of states revealed that the Au-5d, Au-5p, and Rb-4p orbitals hardly participated in bonding. In addition, it is found that the most favourable channel of the [AunRb]+ clusters is Rb+ cation ejection. The electronic localisation function (ELF) analysis of the [AunRb]+ clusters shown that strong interactions are not revealed in this study.

Magnetic behavior of Si-Ge bond in SixGe4-x nano-clusters

NASA Astrophysics Data System (ADS)

Nahali, Masoud; Mehri, Ali

2018-06-01

The structure of SixGe4-x nano-clusters were optimized by MPW1B95 level of theory using MG3S and SDB-aug-cc-PVTZ basis set. The agreement of the calculated ionization and dissociation energies with experimental values validates the reported structures of nano-clusters and justifies the use of hybrid meta density functional method. Since the Si-Si bond is stronger than Si-Ge and Ge-Ge bonds, the Si-Si, Si-Ge, and Ge-Ge diagonal bonds determine the precedence of the stability in these nano-clusters. The hybrid meta density functional calculations were carried out to investigate the adsorption of CO on all possible SixGe4-x nano-clusters. It was found that the silicon atom generally makes a stronger bond with CO than germanium and thereby preferentially affects the shape of structures having higher multiplicity. In Si-Ge structures with higher spin more than 95% of spins accumulate on positions with less bonds to other atoms of the cluster. Through CO adsorption on these clusters bridge structures are made that behave as spin bridge which conduct the spin from the nano-cluster surface to the adsorbate atoms. A better understanding of bridged structures was achieved upon introducing the 'spin bridge' concept. Based on exhaustive spin density analysis, it was found that the reason for the extra negative charge on oxygen in the bridged structures is the relocation of spin from the surface through the bridge.

Reexamine structures and relative stability of medium-sized silicon clusters: Low-lying endohedral fullerene-like clusters Si 30-Si 38

NASA Astrophysics Data System (ADS)

Yoo, Soohaeng; Shao, Nan; Zeng, X. C.

2009-10-01

We report improved results of lowest-lying silicon clusters Si 30-Si 38. A large population of low-energy clusters are collected from previous searches by several research groups and the binding energies of these clusters are computed using density-functional theory (DFT) methods. Best candidates (isomers with high binding energies) are identified from the screening calculations. Additional constrained search is then performed for the best candidates using the basin-hopping method combined with DFT geometry optimization. The obtained low-lying clusters are classified according to binding energies computed using either the Perdew-Burke-Ernzerhof (PBE) functional or the Becke exchange and Lee-Yang-Parr correlation (BLYP) functional. We propose to rank low-lying clusters according to the mean PBE/BLYP binding energies in view that the PBE functional tends to give greater binding energies for more compact clusters whereas the BLYP functional tends to give greater binding energies for less compact clusters or clusters composed of small-sized magic-number clusters. Except for Si 30, the new search confirms again that medium-size silicon clusters Si 31-Si 38 constructed with proper fullerene cage motifs are most promising to be the lowest-energy structures.

Probing the structural evolution and bonding properties of PtnC2-/0 (n = 1-7) clusters by density functional calculations

NASA Astrophysics Data System (ADS)

Lu, Sheng-Jie

2018-05-01

We present a theoretical investigation on the structural evolution and bonding properties of PtnC2-/0 (n = 1-7) clusters using density functional theoretical calculations. The results showed that both anionic and neutral PtnC2 (n = 1-7) clusters primarily adopt 2D planar chain-shaped or ring-based structures. The two C atoms directly interact with each other to form a Csbnd C bond for n = 1-3, while the two C atoms are separated by the Pt atoms for n = 4-7, except for neutral Pt5C2. Pt4C2- anion and Pt4C2 neutral both show σ plus π double delocalized bonding patterns.

Lattice and Valence Electronic Structures of Crystalline Octahedral Molybdenum Halide Clusters-Based Compounds, Cs2[Mo6X14] (X = Cl, Br, I), Studied by Density Functional Theory Calculations.

PubMed

Saito, Norio; Cordier, Stéphane; Lemoine, Pierric; Ohsawa, Takeo; Wada, Yoshiki; Grasset, Fabien; Cross, Jeffrey S; Ohashi, Naoki

2017-06-05

The electronic and crystal structures of Cs 2 [Mo 6 X 14 ] (X = Cl, Br, I) cluster-based compounds were investigated by density functional theory (DFT) simulations and experimental methods such as powder X-ray diffraction, ultraviolet-visible spectroscopy, and X-ray photoemission spectroscopy (XPS). The experimentally determined lattice parameters were in good agreement with theoretically optimized ones, indicating the usefulness of DFT calculations for the structural investigation of these clusters. The calculated band gaps of these compounds reproduced those experimentally determined by UV-vis reflectance within an error of a few tenths of an eV. Core-level XPS and effective charge analyses indicated bonding states of the halogens changed according to their sites. The XPS valence spectra were fairly well reproduced by simulations based on the projected electron density of states weighted with cross sections of Al K α , suggesting that DFT calculations can predict the electronic properties of metal-cluster-based crystals with good accuracy.

Reactions of mixed silver-gold cluster cations AgmAun+ (m+n=4,5,6) with CO: Radiative association kinetics and density functional theory computations

NASA Astrophysics Data System (ADS)

Neumaier, Marco; Weigend, Florian; Hampe, Oliver; Kappes, Manfred M.

2006-09-01

Near thermal energy reactive collisions of small mixed metal cluster cations AgmAun+ (m +n=4, 5, and 6) with carbon monoxide have been studied in the room temperature Penning trap of a Fourier transform ion-cyclotron-resonance mass spectrometer as a function of cluster size and composition. The tetrameric species AgAu3+ and Ag2Au2+ are found to react dissociatively by way of Au or Ag atom loss, respectively, to form the cluster carbonyl AgAu2CO+. In contrast, measurements on a selection of pentamers and hexamers show that CO is added with absolute rate constants that decrease with increasing silver content. Experimentally determined absolute rate constants for CO adsorption were analyzed using the radiative association kinetics model to obtain cluster cation-CO binding energies ranging from 0.77to1.09eV. High-level ab initio density functional theory (DFT) computations identifying the lowest-energy cluster isomers and the respective CO adsorption energies are in good agreement with the experimental findings clearly showing that CO binds in a "head-on" fashion to a gold atom in the mixed clusters. DFT exploration of reaction pathways in the case of Ag2Au2+ suggests that exoergicities are high enough to access the minimum energy products for all reactive clusters probed.

Investigation of dislocation cluster evolution during directional solidification of multicrystalline silicon

NASA Astrophysics Data System (ADS)

Oriwol, Daniel; Trempa, Matthias; Sylla, Lamine; Leipner, Hartmut S.

2017-04-01

Dislocation clusters are the main crystal defects in multicrystalline silicon and are detrimental for solar cell efficiency. They were formed during the silicon ingot casting due to the relaxation of strain energy. The evolution of the dislocation clusters was studied by means of automated analysing tools of the standard wafer and cell production giving information about the cluster development as a function of the ingot height. Due to the observation of the whole wafer surface the point of view is of macroscopic nature. It was found that the dislocations tend to build clusters of high density which usually expand in diameter as a function of ingot height. According to their structure the dislocation clusters can be divided into light and dense clusters. The appearance of both types shows a clear dependence on the orientation of the grain growth direction. Additionally, a process of annihilation of dislocation clusters during the crystallization has been observed. To complement the macroscopic description, the dislocation clusters were also investigates by TEM. It is shown that the dislocations within the subgrain boundaries are closely arranged. Distances of 40-30 nm were found. These results lead to the conclusion that the dislocation density within the cluster structure is impossible to quantify by means of etch pit counting.

Geometrical, electronic, and magnetic properties of CunFe (n=1-12) clusters: A density functional study

NASA Astrophysics Data System (ADS)

Ling, Wang; Dong, Die; Shi-Jian, Wang; Zheng-Quan, Zhao

2015-01-01

The geometrical, electronic, and magnetic properties of small CunFe (n=1-12) clusters have been investigated by using density functional method B3LYP and LanL2DZ basis set. The structural search reveals that Fe atoms in low-energy CunFe isomers tend to occupy the position with the maximum coordination number. The ground state CunFe clusters possess planar structure for n=2-5 and three-dimensional (3D) structure for n=6-12. The electronic properties of CunFe clusters are analyzed through the averaged binding energy, the second-order energy difference and HOMO-LUMO energy gap. It is found that the magic numbers of stability are 1, 3, 7 and 9 for the ground state CunFe clusters. The energy gap of Fe-encapsulated cage clusters is smaller than that of other configurations. The Cu5Fe and Cu7Fe clusters have a very large energy gap (>2.4 eV). The vertical ionization potential (VIP), electron affinity (EA) and photoelectron spectra are also calculated and simulated theoretically for all the ground-state clusters. The magnetic moment analyses for the ground-state CunFe clusters show that Fe atom can enhance the magnetic moment of the host cluster and carries most of the total magnetic moment.

A Comparison of Young Star Properties with Local Galactic Environment for LEGUS/LITTLE THINGS Dwarf Irregular Galaxies

NASA Astrophysics Data System (ADS)

Hunter, Deidre A.; Adamo, Angela; Elmegreen, Bruce G.; Gallardo, Samavarti; Lee, Janice C.; Cook, David O.; Thilker, David; Kayitesi, Bridget; Kim, Hwihyun; Kahre, Lauren; Ubeda, Leonardo; Bright, Stacey N.; Ryon, Jenna E.; Calzetti, Daniela; Tosi, Monica; Grasha, Kathryn; Messa, Matteo; Fumagalli, Michele; Dale, Daniel A.; Sabbi, Elena; Cignoni, Michele; Smith, Linda J.; Gouliermis, Dimitrios M.; Grebel, Eva K.; Aloisi, Alessandra; Whitmore, Bradley C.; Chandar, Rupali; Johnson, Kelsey E.

2018-07-01

We have explored the role environmental factors play in determining characteristics of young stellar objects in nearby dwarf irregular and blue compact dwarf galaxies. Star clusters are characterized by concentrations, masses, and formation rates; OB associations by mass and mass surface density; O stars by their numbers and near-ultraviolet absolute magnitudes; and H II regions by Hα surface brightnesses. These characteristics are compared to surrounding galactic pressure, stellar mass density, H I surface density, and star formation rate (SFR) surface density. We find no trend of cluster characteristics with environmental properties, implying that larger-scale effects are more important in determining cluster characteristics or that rapid dynamical evolution erases any memory of the initial conditions. On the other hand, the most massive OB associations are found at higher pressure and H I surface density, and there is a trend of higher H II region Hα surface brightness with higher pressure, suggesting that a higher concentration of massive stars and gas is found preferentially in regions of higher pressure. At low pressures we find massive stars but not bound clusters and OB associations. We do not find evidence for an increase of cluster formation efficiency as a function of SFR density. However, there is an increase in the ratio of the number of clusters to the number of O stars with increasing pressure, perhaps reflecting an increase in clustering properties with SFR.

Low density, resorcinol-formaldehyde aerogels

DOEpatents

Pekala, R.W.

1988-05-26

The polycondensation of resorcinol with formaldehyde under alkaline conditions results in the formation of surface functionalized polymer ''clusters''. The covalent crosslinking of these ''clusters'' produces gels which when processed under supercritical conditions, produce low density, organic aerogels (density less than or equal to100 mg/cc; cell size less than or equal to0.1 microns). The aerogels are transparent,dark red in color and consist of interconnected colloidal-like particles with diameters of about 100 A/degree/. These aerogels may be further carbonized to form low density carbon foams with cell size of about 0.1 micron. 1 fig., 1 tab.

Role of size, composition and substrate in controlling the reactivity of α(0001)-Al2O3 supported AgnAum (n + m = 2 - 4) alloy clusters for CO-oxidation: A comprehensive density functional study

NASA Astrophysics Data System (ADS)

Singh, Akansha; Majumder, Chiranjib; Sen, Prasenjit

2018-03-01

Catalytic efficiency of gas phase and alumina-supported bimetallic AgnAum (n + m = 2 - 4) alloy clusters is studied using density functional methods As a pre-requite, adsorption of O2 and CO molecules, and co-adsorption of both molecules on these clusters are studied in detail. O2 and CO are co-adsorbed on nearby sites on the gas phase tetramer clusters Ag2Au2 and Ag3Au. But their catalytic efficiency is hindered by large barriers (1.55 eV and 1.44 eV, respectively) to the breaking of Osbnd O bond. Among the deposited clusters, Ag2Au and AgAu2 have O2 and CO co-adsorbed on nearby locations. Of these two, Ag2Au has a lower kinetic barrier for subsequent CO2 formation. Thus Ag2Au looks the most promising candidate.

Determination of the structures of small gold clusters on stepped magnesia by density functional calculations.

PubMed

Damianos, Konstantina; Ferrando, Riccardo

2012-02-21

The structural modifications of small supported gold clusters caused by realistic surface defects (steps) in the MgO(001) support are investigated by computational methods. The most stable gold cluster structures on a stepped MgO(001) surface are searched for in the size range up to 24 Au atoms, and locally optimized by density-functional calculations. Several structural motifs are found within energy differences of 1 eV: inclined leaflets, arched leaflets, pyramidal hollow cages and compact structures. We show that the interaction with the step clearly modifies the structures with respect to adsorption on the flat defect-free surface. We find that leaflet structures clearly dominate for smaller sizes. These leaflets are either inclined and quasi-horizontal, or arched, at variance with the case of the flat surface in which vertical leaflets prevail. With increasing cluster size pyramidal hollow cages begin to compete against leaflet structures. Cage structures become more and more favourable as size increases. The only exception is size 20, at which the tetrahedron is found as the most stable isomer. This tetrahedron is however quite distorted. The comparison of two different exchange-correlation functionals (Perdew-Burke-Ernzerhof and local density approximation) show the same qualitative trends. This journal is © The Royal Society of Chemistry 2012

Evidence for top-heavy stellar initial mass functions with increasing density and decreasing metallicity

NASA Astrophysics Data System (ADS)

Marks, Michael; Kroupa, Pavel; Dabringhausen, Jörg; Pawlowski, Marcel S.

2012-05-01

Residual-gas expulsion after cluster formation has recently been shown to leave an imprint in the low-mass present-day stellar mass function (PDMF) which allowed the estimation of birth conditions of some Galactic globular clusters (GCs) such as mass, radius and star formation efficiency. We show that in order to explain their characteristics (masses, radii, metallicity and PDMF) their stellar initial mass function (IMF) must have been top heavy. It is found that the IMF is required to become more top heavy the lower the cluster metallicity and the larger the pre-GC cloud-core density are. The deduced trends are in qualitative agreement with theoretical expectation. The results are consistent with estimates of the shape of the high-mass end of the IMF in the Arches cluster, Westerlund 1, R136 and NGC 3603, as well as with the IMF independently constrained for ultra-compact dwarf galaxies (UCDs). The latter suggests that GCs and UCDs might have formed along the same channel or that UCDs formed via mergers of GCs. A Fundamental Plane is found which describes the variation of the IMF with density and metallicity of the pre-GC cloud cores. The implications for the evolution of galaxies and chemical enrichment over cosmological times are expected to be major.

Combination of Wavefunction and Density Functional Approximations for Describing Electronic Correlation

NASA Astrophysics Data System (ADS)

Garza, Alejandro J.

Perhaps the most important approximations to the electronic structure problem in quantum chemistry are those based on coupled cluster and density functional theories. Coupled cluster theory has been called the ``gold standard'' of quantum chemistry due to the high accuracy that it achieves for weakly correlated systems. Kohn-Sham density functionals based on semilocal approximations are, without a doubt, the most widely used methods in chemistry and material science because of their high accuracy/cost ratio. The root of the success of coupled cluster and density functionals is their ability to efficiently describe the dynamic part of the electron correlation. However, both traditional coupled cluster and density functional approximations may fail catastrophically when substantial static correlation is present. This severely limits the applicability of these methods to a plethora of important chemical and physical problems such as, e.g., the description of bond breaking, transition states, transition metal-, lanthanide- and actinide-containing compounds, and superconductivity. In an attempt to tackle this problem, nonstandard (single-reference) coupled cluster-based techniques that aim to describe static correlation have been recently developed: pair coupled cluster doubles (pCCD) and singlet-paired coupled cluster doubles (CCD0). The ability to describe static correlation in pCCD and CCD0 comes, however, at the expense of important amounts of dynamic correlation so that the high accuracy of standard coupled cluster becomes unattainable. Thus, the reliable and efficient description of static and dynamic correlation in a simultaneous manner remains an open problem for quantum chemistry and many-body theory in general. In this thesis, different ways to combine pCCD and CCD0 with density functionals in order to describe static and dynamic correlation simultaneously (and efficiently) are explored. The combination of wavefunction and density functional methods has a long history in quantum chemistry (practical implementations have appeared in the literature since the 1970s). However, this kind of techniques have not achieved widespread use due to problems such as double counting of correlation and the symmetry dilemma--the fact that wavefunction methods respect the symmetries of Hamiltonian, while modern functionals are designed to work with broken symmetry densities. Here, particular mathematical features of pCCD and CCD0 are exploited to avoid these problems in an efficient manner. The two resulting families of approximations, denoted as pCCD+DFT and CCD0+DFT, are shown to be able to describe static and dynamic correlation in standard benchmark calculations. Furthermore, it is also shown that CCD0+DFT lends itself to combination with correlation from the direct random phase approximation (dRPA). Inclusion of dRPA in the long-range via the technique of range-separation allows for the description of dispersion correlation, the remaining part of the correlation. Thus, when combined with the dRPA, CCD0+DFT can account for all three-types of electron correlation that are necessary to accurately describe molecular systems. Lastly, applications of CCD0+DFT to actinide chemistry are considered in this work. The accuracy of CCD0+DFT for predicting equilibrium geometries and vibrational frequencies of actinide molecules and ions is assessed and compared to that of well-established quantum chemical methods. For this purpose, the f0 actinyl series (UO2 2+, NpO 23+, PuO24+, the isoelectronic NUN, and Thorium (ThO, ThO2+) and Nobelium (NoO, NoO2) oxides are studied. It is shown that the CCD0+DFT description of these species agrees with available experimental data and is comparable with the results given by the highest-level calculations that are possible for such heavy compounds while being, at least, an order of magnitude lower in computational cost.

Dispersion correction derived from first principles for density functional theory and Hartree-Fock theory.

PubMed

Guidez, Emilie B; Gordon, Mark S

2015-03-12

The modeling of dispersion interactions in density functional theory (DFT) is commonly performed using an energy correction that involves empirically fitted parameters for all atom pairs of the system investigated. In this study, the first-principles-derived dispersion energy from the effective fragment potential (EFP) method is implemented for the density functional theory (DFT-D(EFP)) and Hartree-Fock (HF-D(EFP)) energies. Overall, DFT-D(EFP) performs similarly to the semiempirical DFT-D corrections for the test cases investigated in this work. HF-D(EFP) tends to underestimate binding energies and overestimate intermolecular equilibrium distances, relative to coupled cluster theory, most likely due to incomplete accounting for electron correlation. Overall, this first-principles dispersion correction yields results that are in good agreement with coupled-cluster calculations at a low computational cost.

Multiconfiguration pair-density functional theory investigation of the electronic spectrum of MnO4-

NASA Astrophysics Data System (ADS)

Sharma, Prachi; Truhlar, Donald G.; Gagliardi, Laura

2018-03-01

The electronic spectrum of permanganate ions contains various highly multiconfigurational ligand-to-metal charge transfer states and is notorious for being one of the most challenging systems to be treated by quantum-chemical methods. Here we studied the lowest nine vertical excitation energies using restricted active space second-order perturbation theory (RASPT2) and multiconfiguration pair-density functional theory (MC-PDFT) to test and compare these two theories in computing such a challenging spectrum. The results are compared to literature data, including time-dependent density functional theory, completely renormalized equation-of-motion couple-cluster theory with single and double excitations, symmetry-adapted-cluster configuration interaction, and experimental spectra in the gas phase and solution. Our results show that MC-PDFT accurately predicts the spectrum at a significantly reduced cost as compared to RASPT2.

Multiconfiguration pair-density functional theory investigation of the electronic spectrum of MnO4.

PubMed

Sharma, Prachi; Truhlar, Donald G; Gagliardi, Laura

2018-03-28

The electronic spectrum of permanganate ions contains various highly multiconfigurational ligand-to-metal charge transfer states and is notorious for being one of the most challenging systems to be treated by quantum-chemical methods. Here we studied the lowest nine vertical excitation energies using restricted active space second-order perturbation theory (RASPT2) and multiconfiguration pair-density functional theory (MC-PDFT) to test and compare these two theories in computing such a challenging spectrum. The results are compared to literature data, including time-dependent density functional theory, completely renormalized equation-of-motion couple-cluster theory with single and double excitations, symmetry-adapted-cluster configuration interaction, and experimental spectra in the gas phase and solution. Our results show that MC-PDFT accurately predicts the spectrum at a significantly reduced cost as compared to RASPT2.

Comparing ab initio density-functional and wave function theories: the impact of correlation on the electronic density and the role of the correlation potential.

PubMed

Grabowski, Ireneusz; Teale, Andrew M; Śmiga, Szymon; Bartlett, Rodney J

2011-09-21

The framework of ab initio density-functional theory (DFT) has been introduced as a way to provide a seamless connection between the Kohn-Sham (KS) formulation of DFT and wave-function based ab initio approaches [R. J. Bartlett, I. Grabowski, S. Hirata, and S. Ivanov, J. Chem. Phys. 122, 034104 (2005)]. Recently, an analysis of the impact of dynamical correlation effects on the density of the neon atom was presented [K. Jankowski, K. Nowakowski, I. Grabowski, and J. Wasilewski, J. Chem. Phys. 130, 164102 (2009)], contrasting the behaviour for a variety of standard density functionals with that of ab initio approaches based on second-order Møller-Plesset (MP2) and coupled cluster theories at the singles-doubles (CCSD) and singles-doubles perturbative triples [CCSD(T)] levels. In the present work, we consider ab initio density functionals based on second-order many-body perturbation theory and coupled cluster perturbation theory in a similar manner, for a range of small atomic and molecular systems. For comparison, we also consider results obtained from MP2, CCSD, and CCSD(T) calculations. In addition to this density based analysis, we determine the KS correlation potentials corresponding to these densities and compare them with those obtained for a range of ab initio density functionals via the optimized effective potential method. The correlation energies, densities, and potentials calculated using ab initio DFT display a similar systematic behaviour to those derived from electronic densities calculated using ab initio wave function theories. In contrast, typical explicit density functionals for the correlation energy, such as VWN5 and LYP, do not show behaviour consistent with this picture of dynamical correlation, although they may provide some degree of correction for already erroneous explicitly density-dependent exchange-only functionals. The results presented here using orbital dependent ab initio density functionals show that they provide a treatment of exchange and correlation contributions within the KS framework that is more consistent with traditional ab initio wave function based methods.

Fermi liquid, clustering, and structure factor in dilute warm nuclear matter

NASA Astrophysics Data System (ADS)

Röpke, G.; Voskresensky, D. N.; Kryukov, I. A.; Blaschke, D.

2018-02-01

Properties of nuclear systems at subsaturation densities can be obtained from different approaches. We demonstrate the use of the density autocorrelation function which is related to the isothermal compressibility and, after integration, to the equation of state. This way we connect the Landau Fermi liquid theory well elaborated in nuclear physics with the approaches to dilute nuclear matter describing cluster formation. A quantum statistical approach is presented, based on the cluster decomposition of the polarization function. The fundamental quantity to be calculated is the dynamic structure factor. Comparing with the Landau Fermi liquid theory which is reproduced in lowest approximation, the account of bound state formation and continuum correlations gives the correct low-density result as described by the second virial coefficient and by the mass action law (nuclear statistical equilibrium). Going to higher densities, the inclusion of medium effects is more involved compared with other quantum statistical approaches, but the relation to the Landau Fermi liquid theory gives a promising approach to describe not only thermodynamic but also collective excitations and non-equilibrium properties of nuclear systems in a wide region of the phase diagram.

Structural, electronic, and magnetic properties of Y(n)O (n=2-14) clusters: Density functional study.

PubMed

Yang, Zhi; Xiong, Shi-Jie

2008-09-28

The geometries stability, electronic properties, and magnetism of Y(n)O clusters up to n=14 are systematically studied with density functional theory. In the lowest-energy structures of Y(n)O clusters, the equilibrium site of the oxygen atom gradually moves from an outer site of the cluster, via a surface site, and finally, to an interior site as the number of the Y atoms increases from 2 to 14. Starting from n=12, the O atom falls into the center of the cluster with the Y atoms forming the outer frame. The results show that clusters with n=2, 4, 8, and 12 are more stable than their respective neighbors, and that the total magnetic moments of Y(n)O clusters are all quite small except Y(12)O cluster. The lowest-energy structure of Y(12)O cluster is a perfect icosahedron with a large magnetic moment 6mu(B). In addition, we find that the total magnetic moments are quenched for n=2, 6, and 8 due to the closed-shell electronic configuration. The calculated ionization potentials and electron affinities are in good agreement with the experimental results, which imply that the present theoretical treatments are satisfactory.

Probing the structural evolution of ruthenium doped germanium clusters: Photoelectron spectroscopy and density functional theory calculations

PubMed Central

Jin, Yuanyuan; Lu, Shengjie; Hermann, Andreas; Kuang, Xiaoyu; Zhang, Chuanzhao; Lu, Cheng; Xu, Hongguang; Zheng, Weijun

2016-01-01

We present a combined experimental and theoretical study of ruthenium doped germanium clusters, RuGen− (n = 3–12), and their corresponding neutral species. Photoelectron spectra of RuGen− clusters are measured at 266 nm. The vertical detachment energies (VDEs) and adiabatic detachment energies (ADEs) are obtained. Unbiased CALYPSO structure searches confirm the low-lying structures of anionic and neutral ruthenium doped germanium clusters in the size range of 3 ≤ n ≤ 12. Subsequent geometry optimizations using density functional theory (DFT) at PW91/LANL2DZ level are carried out to determine the relative stability and electronic properties of ruthenium doped germanium clusters. It is found that most of the anionic and neutral clusters have very similar global features. Although the global minimum structures of the anionic and neutral clusters are different, their respective geometries are observed as the low-lying isomers in either case. In addition, for n > 8, the Ru atom in RuGen−/0 clusters is absorbed endohedrally in the Ge cage. The theoretically predicted vertical and adiabatic detachment energies are in good agreement with the experimental measurements. The excellent agreement between DFT calculations and experiment enables a comprehensive evaluation of the geometrical and electronic structures of ruthenium doped germanium clusters. PMID:27439955

Volume shift and charge instability of simple-metal clusters

NASA Astrophysics Data System (ADS)

Brajczewska, M.; Vieira, A.; Fiolhais, C.; Perdew, J. P.

1996-12-01

Experiment indicates that small clusters show changes (mostly contractions) of the bond lengths with respect to bulk values. We use the stabilized jellium model to study the self-expansion and self-compression of spherical clusters (neutral or ionized) of simple metals. Results from Kohn - Sham density functional theory are presented for small clusters of Al and Na, including negatively-charged ones. We also examine the stability of clusters with respect to charging.

Cluster formation in precompound nuclei in the time-dependent framework

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schuetrumpf, B.; Nazarewicz, W.

Background: Modern applications of nuclear time-dependent density functional theory (TDDFT) are often capable of providing quantitative description of heavy ion reactions. However, the structures of precompound (preequilibrium, prefission) states produced in heavy ion reactions are difficult to assess theoretically in TDDFT as the single-particle density alone is a weak indicator of shell structure and cluster states. Purpose: We employ the time-dependent nucleon localization function (NLF) to reveal the structure of precompound states in nuclear reactions involving light and medium-mass ions. We primarily focus on spin saturated systems with N = Z . Furthermore, we study reactions with oxygen and carbonmore » ions, for which some experimental evidence for α clustering in precompound states exists. Method: We utilize the symmetry-free TDDFT approach with the Skyrme energy density functional UNEDF1 and compute the time-dependent NLFs to describe 16O + 16O, 40Ca + 16O, 40Ca + 40Ca , and 16,18O + 12C collisions at energies above the Coulomb barrier. Results: We show that NLFs reveal a variety of time-dependent modes involving cluster structures. For instance, the 16O + 16O collision results in a vibrational mode of a quasimolecular α - 12 C - 12 C- α state. For heavier ions, a variety of cluster configurations are predicted. For the collision of 16,18O + 12C, we showed that the precompound system has a tendency to form α clusters. This result supports the experimental findings that the presence of cluster structures in the projectile and target nuclei gives rise to strong entrance channel effects and enhanced α emission. Conclusion: The time-dependent nucleon localization measure is a very good indicator of cluster structures in complex precompound states formed in heavy-ion fusion reactions. Finally, the localization reveals the presence of collective vibrations involving cluster structures, which dominate the initial dynamics of the fusing system.« less

Cluster formation in precompound nuclei in the time-dependent framework

DOE PAGES

Schuetrumpf, B.; Nazarewicz, W.

2017-12-15

Background: Modern applications of nuclear time-dependent density functional theory (TDDFT) are often capable of providing quantitative description of heavy ion reactions. However, the structures of precompound (preequilibrium, prefission) states produced in heavy ion reactions are difficult to assess theoretically in TDDFT as the single-particle density alone is a weak indicator of shell structure and cluster states. Purpose: We employ the time-dependent nucleon localization function (NLF) to reveal the structure of precompound states in nuclear reactions involving light and medium-mass ions. We primarily focus on spin saturated systems with N = Z . Furthermore, we study reactions with oxygen and carbonmore » ions, for which some experimental evidence for α clustering in precompound states exists. Method: We utilize the symmetry-free TDDFT approach with the Skyrme energy density functional UNEDF1 and compute the time-dependent NLFs to describe 16O + 16O, 40Ca + 16O, 40Ca + 40Ca , and 16,18O + 12C collisions at energies above the Coulomb barrier. Results: We show that NLFs reveal a variety of time-dependent modes involving cluster structures. For instance, the 16O + 16O collision results in a vibrational mode of a quasimolecular α - 12 C - 12 C- α state. For heavier ions, a variety of cluster configurations are predicted. For the collision of 16,18O + 12C, we showed that the precompound system has a tendency to form α clusters. This result supports the experimental findings that the presence of cluster structures in the projectile and target nuclei gives rise to strong entrance channel effects and enhanced α emission. Conclusion: The time-dependent nucleon localization measure is a very good indicator of cluster structures in complex precompound states formed in heavy-ion fusion reactions. Finally, the localization reveals the presence of collective vibrations involving cluster structures, which dominate the initial dynamics of the fusing system.« less

Cluster formation in precompound nuclei in the time-dependent framework

NASA Astrophysics Data System (ADS)

Schuetrumpf, B.; Nazarewicz, W.

2017-12-01

Background: Modern applications of nuclear time-dependent density functional theory (TDDFT) are often capable of providing quantitative description of heavy ion reactions. However, the structures of precompound (preequilibrium, prefission) states produced in heavy ion reactions are difficult to assess theoretically in TDDFT as the single-particle density alone is a weak indicator of shell structure and cluster states. Purpose: We employ the time-dependent nucleon localization function (NLF) to reveal the structure of precompound states in nuclear reactions involving light and medium-mass ions. We primarily focus on spin saturated systems with N =Z . Furthermore, we study reactions with oxygen and carbon ions, for which some experimental evidence for α clustering in precompound states exists. Method: We utilize the symmetry-free TDDFT approach with the Skyrme energy density functional UNEDF1 and compute the time-dependent NLFs to describe 16O + 16O,40Ca + 16O, 40Ca + 40Ca, and O,1816 + 12C collisions at energies above the Coulomb barrier. Results: We show that NLFs reveal a variety of time-dependent modes involving cluster structures. For instance, the 16O + 16O collision results in a vibrational mode of a quasimolecular α - 12C - 12C-α state. For heavier ions, a variety of cluster configurations are predicted. For the collision of O,1816 + 12C, we showed that the precompound system has a tendency to form α clusters. This result supports the experimental findings that the presence of cluster structures in the projectile and target nuclei gives rise to strong entrance channel effects and enhanced α emission. Conclusion: The time-dependent nucleon localization measure is a very good indicator of cluster structures in complex precompound states formed in heavy-ion fusion reactions. The localization reveals the presence of collective vibrations involving cluster structures, which dominate the initial dynamics of the fusing system.

Density-functional theory applied to d- and f-electron systems

NASA Astrophysics Data System (ADS)

Wu, Xueyuan

Density functional theory (DFT) has been applied to study the electronic and geometric structures of prototype d- and f-electron systems. For the d-electron system, all electron DFT with gradient corrections to the exchange and correlation functionals has been used to investigate the properties of small neutral and cationic vanadium clusters. Results are in good agreement with available experimental and other theoretical data. For the f-electron system, a hybrid DFT, namely, B3LYP (Becke's 3-parameter hybrid functional using the correlation functional of Lee, Yang and Parr) with relativistic effective core potentials and cluster models has been applied to investigate the nature of chemical bonding of both the bulk and the surfaces of plutonium monoxide and dioxide. Using periodic models, the electronic and geometric structures of PuO2 and its (110) surface, as well as water adsorption on this surface have also been investigated using DFT in both local density approximation (LDA) and generalized gradient approximation (GGA) formalisms.

Benchmark CCSD(T) and DFT study of binding energies in Be7 - 12: in search of reliable DFT functional for beryllium clusters

NASA Astrophysics Data System (ADS)

Labanc, Daniel; Šulka, Martin; Pitoňák, Michal; Černušák, Ivan; Urban, Miroslav; Neogrády, Pavel

2018-05-01

We present a computational study of the stability of small homonuclear beryllium clusters Be7 - 12 in singlet electronic states. Our predictions are based on highly correlated CCSD(T) coupled cluster calculations. Basis set convergence towards the complete basis set limit as well as the role of the 1s core electron correlation are carefully examined. Our CCSD(T) data for binding energies of Be7 - 12 clusters serve as a benchmark for performance assessment of several density functional theory (DFT) methods frequently used in beryllium cluster chemistry. We observe that, from Be10 clusters on, the deviation from CCSD(T) benchmarks is stable with respect to size, and fluctuating within 0.02 eV error bar for most examined functionals. This opens up the possibility of scaling the DFT binding energies for large Be clusters using CCSD(T) benchmark values for smaller clusters. We also tried to find analogies between the performance of DFT functionals for Be clusters and for the valence-isoelectronic Mg clusters investigated recently in Truhlar's group. We conclude that it is difficult to find DFT functionals that perform reasonably well for both beryllium and magnesium clusters. Out of 12 functionals examined, only the M06-2X functional gives reasonably accurate and balanced binding energies for both Be and Mg clusters.

Cluster-lensing: A Python Package for Galaxy Clusters and Miscentering

NASA Astrophysics Data System (ADS)

Ford, Jes; VanderPlas, Jake

2016-12-01

We describe a new open source package for calculating properties of galaxy clusters, including Navarro, Frenk, and White halo profiles with and without the effects of cluster miscentering. This pure-Python package, cluster-lensing, provides well-documented and easy-to-use classes and functions for calculating cluster scaling relations, including mass-richness and mass-concentration relations from the literature, as well as the surface mass density {{Σ }}(R) and differential surface mass density {{Δ }}{{Σ }}(R) profiles, probed by weak lensing magnification and shear. Galaxy cluster miscentering is especially a concern for stacked weak lensing shear studies of galaxy clusters, where offsets between the assumed and the true underlying matter distribution can lead to a significant bias in the mass estimates if not accounted for. This software has been developed and released in a public GitHub repository, and is licensed under the permissive MIT license. The cluster-lensing package is archived on Zenodo. Full documentation, source code, and installation instructions are available at http://jesford.github.io/cluster-lensing/.

From clusters to bulk: A relativistic density functional investigation on a series of gold clusters Aun, n=6,…,147

NASA Astrophysics Data System (ADS)

Häberlen, Oliver D.; Chung, Sai-Cheong; Stener, Mauro; Rösch, Notker

1997-03-01

A series of gold clusters spanning the size range from Au6 through Au147 (with diameters from 0.7 to 1.7 nm) in icosahedral, octahedral, and cuboctahedral structure has been theoretically investigated by means of a scalar relativistic all-electron density functional method. One of the main objectives of this work was to analyze the convergence of cluster properties toward the corresponding bulk metal values and to compare the results obtained for the local density approximation (LDA) to those for a generalized gradient approximation (GGA) to the exchange-correlation functional. The average gold-gold distance in the clusters increases with their nuclearity and correlates essentially linearly with the average coordination number in the clusters. An extrapolation to the bulk coordination of 12 yields a gold-gold distance of 289 pm in LDA, very close to the experimental bulk value of 288 pm, while the extrapolated GGA gold-gold distance is 297 pm. The cluster cohesive energy varies linearly with the inverse of the calculated cluster radius, indicating that the surface-to-volume ratio is the primary determinant of the convergence of this quantity toward bulk. The extrapolated LDA binding energy per atom, 4.7 eV, overestimates the experimental bulk value of 3.8 eV, while the GGA value, 3.2 eV, underestimates the experiment by almost the same amount. The calculated ionization potentials and electron affinities of the clusters may be related to the metallic droplet model, although deviations due to the electronic shell structure are noticeable. The GGA extrapolation to bulk values yields 4.8 and 4.9 eV for the ionization potential and the electron affinity, respectively, remarkably close to the experimental polycrystalline work function of bulk gold, 5.1 eV. Gold 4f core level binding energies were calculated for sites with bulk coordination and for different surface sites. The core level shifts for the surface sites are all positive and distinguish among the corner, edge, and face-centered sites; sites in the first subsurface layer show still small positive shifts.

The study of structures and properties of PdnHm(n=1-10, m=1,2) clusters by density functional theory

NASA Astrophysics Data System (ADS)

Wen, Jun-Qing; Chen, Guo-Xiang; Zhang, Jian-Min; Wu, Hua

2018-04-01

The geometrical evolution, local relative stability, magnetism and charge transfer characteristics of PdnHm(n = 1-10, m = 1,2) have been systematically calculated by using density functional theory. The studied results show that the most stable geometries of PdnH and PdnH2 (n = 1-10) can be got by doping one or two H atoms on the sides of Pdn clusters except Pd6H and Pd6H2. It is found that doping one or two H atoms on Pdn clusters cannot change the basic framework of Pdn. The analysis of stability shows that Pd2H, Pd4H, Pd7H, Pd2H2, Pd4H2 and Pd7H2 clusters have higher local relative stability than neighboring clusters. The analysis of magnetic properties demonstrates that absorption of hydrogen atoms decreases the average atomic magnetic moments compared with pure Pdn clusters. More charges transfer from H atoms to Pd atoms for Pd6H and Pd6H2 clusters, demonstrating the adsorption of hydrogen atoms change from side adsorption to surface adsorption.

SU-G-TeP3-14: Three-Dimensional Cluster Model in Inhomogeneous Dose Distribution

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wei, J; Penagaricano, J; Narayanasamy, G

2016-06-15

Purpose: We aim to investigate 3D cluster formation in inhomogeneous dose distribution to search for new models predicting radiation tissue damage and further leading to new optimization paradigm for radiotherapy planning. Methods: The aggregation of higher dose in the organ at risk (OAR) than a preset threshold was chosen as the cluster whose connectivity dictates the cluster structure. Upon the selection of the dose threshold, the fractional density defined as the fraction of voxels in the organ eligible to be part of the cluster was determined according to the dose volume histogram (DVH). A Monte Carlo method was implemented tomore » establish a case pertinent to the corresponding DVH. Ones and zeros were randomly assigned to each OAR voxel with the sampling probability equal to the fractional density. Ten thousand samples were randomly generated to ensure a sufficient number of cluster sets. A recursive cluster searching algorithm was developed to analyze the cluster with various connectivity choices like 1-, 2-, and 3-connectivity. The mean size of the largest cluster (MSLC) from the Monte Carlo samples was taken to be a function of the fractional density. Various OARs from clinical plans were included in the study. Results: Intensive Monte Carlo study demonstrates the inverse relationship between the MSLC and the cluster connectivity as anticipated and the cluster size does not change with fractional density linearly regardless of the connectivity types. An initially-slow-increase to exponential growth transition of the MSLC from low to high density was observed. The cluster sizes were found to vary within a large range and are relatively independent of the OARs. Conclusion: The Monte Carlo study revealed that the cluster size could serve as a suitable index of the tissue damage (percolation cluster) and the clinical outcome of the same DVH might be potentially different.« less

The Impact of Alcohol Outlet Density on the Geographic Clustering of Underage Drinking Behaviors within Census Tracts

PubMed Central

Reboussin, Beth A.; Song, Eun-Young; Wolfson, Mark

2011-01-01

Background The regulation of alcohol outlet density has been considered as a potential means of reducing alcohol consumption and related harms among underage youth. Whereas prior studies have examined whether alcohol outlet density was associated with an individual’s alcohol consumption and related harms, this study examines whether it is related to the co-occurrence, or clustering, of these behaviors within geographic areas, specifically census tracts. Methods The Enforcing Underage Drinking Laws Randomized Community Trial provided cross-sectional telephone survey data in 2006 and 2007 from 10,754 youth aged 14–20 from 5 states residing in 1556 census tracts. The alternating logistic regression approach was used to estimate pairwise odds ratios between responses from youth residing in the same census tract and to model them as a function of alcohol outlet density. Results Riding with a drinking driver, making an alcohol purchase attempt and making a successful alcohol purchase attempt clustered significantly within census tracts with the highest off-premise alcohol outlet density while frequent drinking clustered within census tracts with the greatest on-premise density. Driving after drinking and experiencing non-violent alcohol-related consequences clustered marginally within census tracts with the greatest on-premise and off-premise alcohol outlet density, respectively. Conclusions Although youth primarily receive alcohol from social sources, commercial alcohol access is geographically concentrated within census tracts with the greatest off-premise outlet density. A potentially greater concern is the clustering of more frequent drinking and drinking and driving within census tracts with the greatest on-premise outlet density which may necessitate alternative census tract level initiatives to reduce these potentially harmful behaviors. PMID:21463343

Measuring the stellar luminosity function and spatial density profile of the inner 0.5 pc of the Milky Way nuclear star cluster

NASA Astrophysics Data System (ADS)

Do, Tuan; Ghez, Andrea; Lu, Jessica R.; Morris, Mark R.; Yelda, Sylvana; Martinez, Gregory D.; Peter, Annika H. G.; Wright, Shelley; Bullock, James; Kaplinghat, Manoj; Matthews, K.

2012-07-01

We report on measurements of the luminosity function of early (young) and late-type (old) stars in the central 0.5 pc of the Milky Way nuclear star cluster as well as the density profiles of both components. The young (~ 6 Myr) and old stars (> 1 Gyr) in this region provide different physical probes of the environment around a supermassive black hole; the luminosity function of the young stars offers us a way to measure the initial mass function from star formation in an extreme environment, while the density profile of the old stars offers us a probe of the dynamical interaction of a star cluster with a massive black hole. The two stellar populations are separated through a near-infrared spectroscopic survey using the integral-field spectrograph OSIRIS on Keck II behind the laser guide star adaptive optics system. This spectroscopic survey is able to separate early-type (young) and late-type (old) stars with a completeness of 50% at K' = 15.5. We describe our method of completeness correction using a combination of star planting simulations and Bayesian inference. The completeness corrected luminosity function of the early-type stars contains significantly more young stars at faint magnitudes compared to previous surveys with similar depth. In addition, by using proper motion and radial velocity measurements along with anisotropic spherical Jeans modeling of the cluster, it is possible to measure the spatial density profile of the old stars, which has been difficult to constrain with number counts alone. The most probable model shows that the spatial density profile, n(r) propto r-γ, to be shallow with γ = 0.4 ± 0.2, which is much flatter than the dynamically relaxed case of γ = 3/2 to 7/4, but does rule out a 'hole' in the distribution of old stars. We show, for the first time, that the spatial density profile, the black hole mass, and velocity anisotropy can be fit simultaneously to obtain a black hole mass that is consistent with that derived from individual orbits of stars at distances < 1000 AU from the Galactic center.

A Geometric and Electrostatic Study of the [4Fe-4S] Cluster of Adenosine-5´-Phosphosulfate Reductase from Broken Symmetry Density Functional Calculations and Extended X-ray Absorption Fine Structure Spectroscopy

PubMed Central

Bhave, Devayani P.; Han, Wen-Ge; Pazicni, Samuel; Penner-Hahn, James E.; Carroll, Kate S.; Noodleman, Louis

2011-01-01

Adenosine-5’-phosphosulfate reductase (APSR) is an iron-sulfur protein that catalyses the reduction of adenosine-5’-phosphosulfate (APS) to sulfite. APSR coordinates to a [4Fe-4S] cluster via a conserved CC-X~80-CXXC motif and the cluster is essential for catalysis. Despite extensive functional, structural and spectroscopic studies, the exact role of the iron-sulfur cluster in APS reduction remains unknown. To gain an understanding into the role of the cluster, density functional theory (DFT) analysis and extended X-ray fine structure spectroscopy (EXAFS) have been performed to reveal insights into the coordination, geometry and electrostatics of the [4Fe-4S] cluster. XANES data confirms that the cluster is in the [4Fe-4S]2+ state in both native and substrate-bound APSR while EXAFS data recorded at ~0.1 Å resolution indicates that there is no significant change in the structure of the [4Fe-4S] cluster between the native and substrate-bound forms of the protein. On the other hand, DFT calculations provide an insight into the subtle differences between the geometry of the cluster in the native and APS-bound forms of APSR. A comparison between models with and without the tandem cysteine pair coordination of the cluster suggests a role for the unique coordination in facilitating a compact geometric structure and ‘fine-tuning’ the electronic structure to prevent reduction of the cluster. Further, calculations using models in which residue Lys144 is mutated to Ala confirm the finding that Lys144 serves as a crucial link in the interactions involving the [4Fe-4S] cluster and APS. PMID:21678934

Two-component density functional theory calculations of positron lifetimes for small vacancy clusters in silicon

NASA Astrophysics Data System (ADS)

Makhov, D. V.; Lewis, Laurent J.

2005-05-01

The positron lifetimes for various vacancy clusters in silicon are calculated within the framework of the two-component electron-positron density functional theory. The effect of the trapped positron on the electron density and on the relaxation of the structure is investigated. Our calculations show that, contrary to the usual assumption, the positron-induced forces do not compensate in general for electronic inward forces. Thus, geometry optimization is required in order to determine positron lifetime accurately. For the monovacancy and the divacancy, the results of our calculations are in good agreement with the experimental positron lifetimes, suggesting that this approach gives good estimates of positron lifetimes for larger vacancy clusters, required for their correct identification with positron annihilation spectroscopy. As an application, our calculations show that fourfold trivacancies and symmetric fourfold tetravacancies have positron lifetimes similar to monovacancies and divacancies, respectively, and can thus be confused in the interpretation of positron annihilation experiments.

The correlation function for density perturbations in an expanding universe. II - Nonlinear theory

NASA Technical Reports Server (NTRS)

Mcclelland, J.; Silk, J.

1977-01-01

A formalism is developed to find the two-point and higher-order correlation functions for a given distribution of sizes and shapes of perturbations which are randomly placed in three-dimensional space. The perturbations are described by two parameters such as central density and size, and the two-point correlation function is explicitly related to the luminosity function of groups and clusters of galaxies

An X-ray Luminous, Distant (z=0.78) Cluster of Galaxies

NASA Technical Reports Server (NTRS)

Donahue, Megan

2001-01-01

This granted funded ASCA studies of the most X-ray luminous clusters of galaxies in the Extended Medium Sensitivity Survey. These studies leveraged further observations with Chandra and sparked a new collaboration between the PI and John Carlstrom's Sunyaev-Zel'dovich team. The major scientific results due largely or in part from these observations: the first z=0.5-0.8 cluster temperature function, constraints on cluster evolution which showed definitively that the density of the universe divided by the critical density, Omega-m, could not be 1.0, constraints on cluster evolution limiting Omega_m to 0.2-0.5, independent of lambda, the first detections of intracluster iron in a z>0.6 cluster of galaxies. These results are independent of the supernova and cosmological microwave background results, and provide independent constraint on cosmological parameters.

Cluster redshifts in five suspected superclusters

NASA Technical Reports Server (NTRS)

Ciardullo, R.; Ford, H.; Harms, R.

1985-01-01

Redshift surveys for rich superclusters were carried out in five regions of the sky containing surface-density enhancements of Abell clusters. While several superclusters are identified, projection effects dominate each field, and no system contains more than five rich clusters. Two systems are found to be especially interesting. The first, field 0136 10, is shown to contain a superposition of at least four distinct superclusters, with the richest system possessing a small velocity dispersion. The second system, 2206 - 22, though a region of exceedingly high Abell cluster surface density, appears to be a remarkable superposition of 23 rich clusters almost uniformly distributed in redshift space between 0.08 and 0.24. The new redshifts significantly increase the three-dimensional information available for the distance class 5 and 6 Abell clusters and allow the spatial correlation function around rich superclusters to be estimated.

Effect of functionalization of boron nitride flakes by main group metal clusters on their optoelectronic properties

NASA Astrophysics Data System (ADS)

Chakraborty, Debdutta; Chattaraj, Pratim Kumar

2017-10-01

The possibility of functionalizing boron nitride flakes (BNFs) with some selected main group metal clusters, viz. OLi4, NLi5, CLi6, BLI7 and Al12Be, has been analyzed with the aid of density functional theory (DFT) based computations. Thermochemical as well as energetic considerations suggest that all the metal clusters interact with the BNF moiety in a favorable fashion. As a result of functionalization, the static (first) hyperpolarizability (β ) values of the metal cluster supported BNF moieties increase quite significantly as compared to that in the case of pristine BNF. Time dependent DFT analysis reveals that the metal clusters can lower the transition energies associated with the dominant electronic transitions quite significantly thereby enabling the metal cluster supported BNF moieties to exhibit significant non-linear optical activity. Moreover, the studied systems demonstrate broad band absorption capability spanning the UV-visible as well as infra-red domains. Energy decomposition analysis reveals that the electrostatic interactions principally stabilize the metal cluster supported BNF moieties.

Effect of functionalization of boron nitride flakes by main group metal clusters on their optoelectronic properties.

PubMed

Chakraborty, Debdutta; Chattaraj, Pratim Kumar

2017-10-25

The possibility of functionalizing boron nitride flakes (BNFs) with some selected main group metal clusters, viz. OLi 4 , NLi 5 , CLi 6 , BLI 7 and Al 12 Be, has been analyzed with the aid of density functional theory (DFT) based computations. Thermochemical as well as energetic considerations suggest that all the metal clusters interact with the BNF moiety in a favorable fashion. As a result of functionalization, the static (first) hyperpolarizability ([Formula: see text]) values of the metal cluster supported BNF moieties increase quite significantly as compared to that in the case of pristine BNF. Time dependent DFT analysis reveals that the metal clusters can lower the transition energies associated with the dominant electronic transitions quite significantly thereby enabling the metal cluster supported BNF moieties to exhibit significant non-linear optical activity. Moreover, the studied systems demonstrate broad band absorption capability spanning the UV-visible as well as infra-red domains. Energy decomposition analysis reveals that the electrostatic interactions principally stabilize the metal cluster supported BNF moieties.

The kinematics of dense clusters of galaxies. II - The distribution of velocity dispersions

NASA Technical Reports Server (NTRS)

Zabludoff, Ann I.; Geller, Margaret J.; Huchra, John P.; Ramella, Massimo

1993-01-01

From the survey of 31 Abell R above 1 cluster fields within z of 0.02-0.05, we extract 25 dense clusters with velocity dispersions omicron above 300 km/s and with number densities exceeding the mean for the Great Wall of galaxies by one deviation. From the CfA Redshift Survey (in preparation), we obtain an approximately volume-limited catalog of 31 groups with velocity dispersions above 100 km/s and with the same number density limit. We combine these well-defined samples to obtain the distribution of cluster velocity dispersions. The group sample enables us to correct for incompleteness in the Abell catalog at low velocity dispersions. The clusters from the Abell cluster fields populate the high dispersion tail. For systems with velocity dispersions above 700 km/s, approximately the median for R = 1 clusters, the group and cluster abundances are consistent. The combined distribution is consistent with cluster X-ray temperature functions.

The Richness Dependence of Galaxy Cluster Correlations: Results From A Redshift Survey Of Rich APM Clusters

NASA Technical Reports Server (NTRS)

Croft, R. A. C.; Dalton, G. B.; Efstathiou, G.; Sutherland, W. J.; Maddox, S. J.

1997-01-01

We analyze the spatial clustering properties of a new catalog of very rich galaxy clusters selected from the APM Galaxy Survey. These clusters are of comparable richness and space density to Abell Richness Class greater than or equal to 1 clusters, but selected using an objective algorithm from a catalog demonstrably free of artificial inhomogeneities. Evaluation of the two-point correlation function xi(sub cc)(r) for the full sample and for richer subsamples reveals that the correlation amplitude is consistent with that measured for lower richness APM clusters and X-ray selected clusters. We apply a maximum likelihood estimator to find the best fitting slope and amplitude of a power law fit to x(sub cc)(r), and to estimate the correlation length r(sub 0) (the value of r at which xi(sub cc)(r) is equal to unity). For clusters with a mean space density of 1.6 x 10(exp -6) h(exp 3) MpC(exp -3) (equivalent to the space density of Abell Richness greater than or equal to 2 clusters), we find r(sub 0) = 21.3(+11.1/-9.3) h(exp -1) Mpc (95% confidence limits). This is consistent with the weak richness dependence of xi(sub cc)(r) expected in Gaussian models of structure formation. In particular, the amplitude of xi(sub cc)(r) at all richnesses matches that of xi(sub cc)(r) for clusters selected in N-Body simulations of a low density Cold Dark Matter model.

The impact of baryons on massive galaxy clusters: halo structure and cluster mass estimates

NASA Astrophysics Data System (ADS)

Henson, Monique A.; Barnes, David J.; Kay, Scott T.; McCarthy, Ian G.; Schaye, Joop

2017-03-01

We use the BAHAMAS (BAryons and HAloes of MAssive Systems) and MACSIS (MAssive ClusterS and Intercluster Structures) hydrodynamic simulations to quantify the impact of baryons on the mass distribution and dynamics of massive galaxy clusters, as well as the bias in X-ray and weak lensing mass estimates. These simulations use the subgrid physics models calibrated in the BAHAMAS project, which include feedback from both supernovae and active galactic nuclei. They form a cluster population covering almost two orders of magnitude in mass, with more than 3500 clusters with masses greater than 1014 M⊙ at z = 0. We start by characterizing the clusters in terms of their spin, shape and density profile, before considering the bias in both weak lensing and hydrostatic mass estimates. Whilst including baryonic effects leads to more spherical, centrally concentrated clusters, the median weak lensing mass bias is unaffected by the presence of baryons. In both the dark matter only and hydrodynamic simulations, the weak lensing measurements underestimate cluster masses by ≈10 per cent for clusters with M200 ≤ 1015 M⊙ and this bias tends to zero at higher masses. We also consider the hydrostatic bias when using both the true density and temperature profiles, and those derived from X-ray spectroscopy. When using spectroscopic temperatures and densities, the hydrostatic bias decreases as a function of mass, leading to a bias of ≈40 per cent for clusters with M500 ≥ 1015 M⊙. This is due to the presence of cooler gas in the cluster outskirts. Using mass weighted temperatures and the true density profile reduces this bias to 5-15 per cent.

Segregation formation, thermal and electronic properties of ternary cubic CdZnTe clusters: MD simulations and DFT calculations

NASA Astrophysics Data System (ADS)

Kurban, Mustafa; Erkoç, Şakir

2017-04-01

Surface and core formation, thermal and electronic properties of ternary cubic CdZnTe clusters are investigated by using classical molecular dynamics (MD) simulations and density functional theory (DFT) calculations. In this work, MD simulations of the CdZnTe clusters are performed by means of LAMMPS by using bond order potential (BOP). MD simulations are carried out at different temperatures to study the segregation phenomena of Cd, Zn and Te atoms, and deviation of clusters and heat capacity. After that, using optimized geometries obtained, excess charge on atoms, dipole moments, highest occupied molecular orbitals, lowest unoccupied molecular orbitals, HOMO-LUMO gaps (Eg) , total energies, spin density and the density of states (DOS) have been calculated with DFT. Simulation results such as heat capacity and segregation formation are compared with experimental bulk and theoretical results.

A comprehensive study of large-scale structures in the GOODS-SOUTH field up to z ˜ 2.5

NASA Astrophysics Data System (ADS)

Salimbeni, S.; Castellano, M.; Pentericci, L.; Trevese, D.; Fiore, F.; Grazian, A.; Fontana, A.; Giallongo, E.; Boutsia, K.; Cristiani, S.; de Santis, C.; Gallozzi, S.; Menci, N.; Nonino, M.; Paris, D.; Santini, P.; Vanzella, E.

2009-07-01

Aims: The aim of the present paper is to identify and study the properties and galactic content of groups and clusters in the GOODS-South field up to z˜ 2.5, and to analyse the physical properties of galaxies as a continuous function of environmental density up to high redshift. Methods: We used the deep (z850˜ 26), multi-wavelength GOODS-MUSIC catalogue, which has a 15% of spectroscopic redshifts and accurate photometric redshifts for the remaining fraction. On these data, we applied a (2+1)D algorithm, previously developed by our group, that provides an adaptive estimate of the 3D density field. We supported our analysis with simulations to evaluate the purity and the completeness of the cluster catalogue produced by our algorithm. Results: We find several high-density peaks embedded in larger structures in the redshift range 0.4-2.5. From the analysis of their physical properties (mass profile, M200, σ_v, L_X, U-B vs. B diagram), we find that most of them are groups of galaxies, while two are poor clusters with masses a few times 1014~M_⊙. For these two clusters we find from the Chandra 2Ms data an X-ray emission significantly lower than expected from their optical properties, suggesting that the two clusters are either not virialised or are gas poor. We find that the slope of the colour magnitude relation, for these groups and clusters, is constant at least up to z ˜ 1. We also analyse the dependence on environment of galaxy colours, luminosities, stellar masses, ages, and star formations. We find that galaxies in high-density regions are, on average, more luminous and massive than field galaxies up to z ˜ 2. The fraction of red galaxies increases with luminosity and with density up to z˜ 1.2. At higher z this dependence on density disappears. The variation of galaxy properties as a function of redshift and density suggests that a significant change occurs at z ˜ 1.5-2.

Description of plasmon-like band in silver clusters: the importance of the long-range Hartree-Fock exchange in time-dependent density-functional theory simulations.

PubMed

Rabilloud, Franck

2014-10-14

Absorption spectra of Ag20 and Ag55(q) (q = +1, -3) nanoclusters are investigated in the framework of the time-dependent density functional theory in order to analyse the role of the d electrons in plasmon-like band of silver clusters. The description of the plasmon-like band from calculations using density functionals containing an amount of Hartree-Fock exchange at long range, namely, hybrid and range-separated hybrid (RSH) density functionals, is in good agreement with the classical interpretation of the plasmon-like structure as a collective excitation of valence s-electrons. In contrast, using local or semi-local exchange functionals (generalized gradient approximations (GGAs) or meta-GGAs) leads to a strong overestimation of the role of d electrons in the plasmon-like band. The semi-local asymptotically corrected model potentials also describe the plasmon as mainly associated to d electrons, though calculated spectra are in fairly good agreement with those calculated using the RSH scheme. Our analysis shows that a portion of non-local exchange modifies the description of the plasmon-like band.

VizieR Online Data Catalog: Structure of young stellar clusters. II. (Kuhn+, 2015)

NASA Astrophysics Data System (ADS)

Kuhn, M. A.; Getman, K. V.; Feigelson, E. D.

2015-07-01

We investigate the intrinsic stellar populations (estimated total numbers of OB and pre-main-sequence stars down to 0.1Mȯ) that are present in 17 massive star-forming regions (MSFRs) surveyed by the MYStIX project. The study is based on the catalog of >31000 MYStIX Probable Complex Members with both disk-bearing and disk-free populations, compensating for extinction, nebulosity, and crowding effects. Correction for observational sensitivities is made using the X-ray luminosity function and the near-infrared initial mass function --a correction that is often not made by infrared surveys of young stars. The resulting maps of the projected structure of the young stellar populations, in units of intrinsic stellar surface density, allow direct comparison between different regions. Several regions have multiple dense clumps, similar in size and density to the Orion Nebula Cluster. The highest projected density of ~34000 stars/pc2 is found in the core of the RCW 38 cluster. Histograms of surface density show different ranges of values in different regions, supporting the conclusion of Bressert et al. (B10; 2010MNRAS.409L..54B) that no universal surface-density threshold can distinguish between clustered and distributed star formation. However, a large component of the young stellar population of MSFRs resides in dense environments of 200-10000 stars/pc2 (including within the nearby Orion molecular clouds), and we find that there is no evidence for the B10 conclusion that such dense regions form an extreme "tail" of the distribution. Tables of intrinsic populations for these regions are used in our companion study of young cluster properties and evolution. (3 data files).

Molecular properties via a subsystem density functional theory formulation: a common framework for electronic embedding.

PubMed

Höfener, Sebastian; Gomes, André Severo Pereira; Visscher, Lucas

2012-01-28

In this article, we present a consistent derivation of a density functional theory (DFT) based embedding method which encompasses wave-function theory-in-DFT (WFT-in-DFT) and the DFT-based subsystem formulation of response theory (DFT-in-DFT) by Neugebauer [J. Neugebauer, J. Chem. Phys. 131, 084104 (2009)] as special cases. This formulation, which is based on the time-averaged quasi-energy formalism, makes use of the variation Lagrangian techniques to allow the use of non-variational (in particular: coupled cluster) wave-function-based methods. We show how, in the time-independent limit, we naturally obtain expressions for the ground-state DFT-in-DFT and WFT-in-DFT embedding via a local potential. We furthermore provide working equations for the special case in which coupled cluster theory is used to obtain the density and excitation energies of the active subsystem. A sample application is given to demonstrate the method. © 2012 American Institute of Physics

Multiconfiguration Pair-Density Functional Theory Is Free From Delocalization Error.

PubMed

Bao, Junwei Lucas; Wang, Ying; He, Xiao; Gagliardi, Laura; Truhlar, Donald G

2017-11-16

Delocalization error has been singled out by Yang and co-workers as the dominant error in Kohn-Sham density functional theory (KS-DFT) with conventional approximate functionals. In this Letter, by computing the vertical first ionization energy for well separated He clusters, we show that multiconfiguration pair-density functional theory (MC-PDFT) is free from delocalization error. To put MC-PDFT in perspective, we also compare it with some Kohn-Sham density functionals, including both traditional and modern functionals. Whereas large delocalization errors are almost universal in KS-DFT (the only exception being the very recent corrected functionals of Yang and co-workers), delocalization error is removed by MC-PDFT, which bodes well for its future as a step forward from KS-DFT.

Tantalum induced butterfly-like clusters on Si (111)-7 × 7 surface: STM/STS study at low coverage

NASA Astrophysics Data System (ADS)

Shukrynau, Pavel; Mutombo, Pingo; Švec, Martin; Hietschold, Michael; Cháb, Vladimír

2012-02-01

The adsorption of the small amounts of tantalum on Si (111)-7 × 7 reconstructed surface is investigated systematically using scanning tunneling microscopy and tunneling spectroscopy combined with first-principles density functional theory calculations. We find out that the moderate annealing of the Ta covered surface results in the formation of clusters of the butterfly-like shape. The clusters are sporadically distributed over the surface and their density is metal coverage dependent. Filled and empty state STM images of the clusters differ strongly suggesting the existence of covalent bonds within the cluster. Tunneling spectroscopy measurements reveal small energy gap, showing semiconductor-like behavior of the constituent atoms. The cluster model based on experimental images and theoretical calculations has been proposed and discussed. Presented results show that Ta joins the family of adsorbates, that are known to form magic clusters on Si (111)-7 × 7, but its magic cluster has the structural and electronic properties that are different from those reported before.

Spatial structure and electronic spectrum of TiSi{/n -} clusters ( n = 6-18)

NASA Astrophysics Data System (ADS)

Borshch, N. A.; Pereslavtseva, N. S.; Kurganskii, S. I.

2014-10-01

Results from optimizing the spatial structure and calculated electronic spectra of anion clusters TiSi{/n -} ( n = 6-18) are presented. Calculations are performed within the density functional theory. Spatial structures of clusters detected experimentally are established by comparing the calculated and experimental data. It is shown that prismatic and fullerene-like structures are the ones most energetically favorable for clusters TiSi{/n -}. It is concluded that these structures are basic when building clusters with close numbers of silicon atoms.

Statistical mechanics of high-density bond percolation

NASA Astrophysics Data System (ADS)

Timonin, P. N.

2018-05-01

High-density (HD) percolation describes the percolation of specific κ -clusters, which are the compact sets of sites each connected to κ nearest filled sites at least. It takes place in the classical patterns of independently distributed sites or bonds in which the ordinary percolation transition also exists. Hence, the study of series of κ -type HD percolations amounts to the description of classical clusters' structure for which κ -clusters constitute κ -cores nested one into another. Such data are needed for description of a number of physical, biological, and information properties of complex systems on random lattices, graphs, and networks. They range from magnetic properties of semiconductor alloys to anomalies in supercooled water and clustering in biological and social networks. Here we present the statistical mechanics approach to study HD bond percolation on an arbitrary graph. It is shown that the generating function for κ -clusters' size distribution can be obtained from the partition function of the specific q -state Potts-Ising model in the q →1 limit. Using this approach we find exact κ -clusters' size distributions for the Bethe lattice and Erdos-Renyi graph. The application of the method to Euclidean lattices is also discussed.

Growth and properties of silicon heterostructures with buried nanosize Mg2Si clusters

NASA Astrophysics Data System (ADS)

Galkin, N. G.; Galkin, K. N.

2005-06-01

The technology of solid-phase growth of nanosize islands of magnesium suicide on Si (111) 7x7 with narrow distributions of lateral size and height (60 - 80 and 5 - 7 nanometers, respectively) and density of up to 2x 109 sm-2 is proposed. A 20-50 nm thick Si layer has been grown upon these islands. Basing on the data of AES, EELS, AFM and JR spectroscopy, a conclusion is made that the Mg2Si islands remain in depth of the Si layer. The suggestion is made that sizes, density and crystal structure of the buried magnesium suicide clusters preserves. It is shown, that the system of three as-grown layers of buried clusters has smoother surface than the one layer system. The contribution of the Mg2Si clusters into the dielectric function is observed at the energy 0.8-1.2 eV, it is maximal if the clusters are localized on the silicon surface. It is shown, that with increase of the number of Mg2Si cluster layers their contribution increases into the effective number of electrons per a unit cell and effective dielectric function of the sample.

Communication: Biological applications of coupled-cluster frozen-density embedding

NASA Astrophysics Data System (ADS)

Heuser, Johannes; Höfener, Sebastian

2018-04-01

We report the implementation of the Laplace-transform scaled opposite-spin (LT-SOS) resolution-of-the-identity second-order approximate coupled-cluster singles and doubles (RICC2) combined with frozen-density embedding for excitation energies and molecular properties. In the present work, we furthermore employ the Hartree-Fock density for the interaction energy leading to a simplified Lagrangian which is linear in the Lagrangian multipliers. This approximation has the key advantage of a decoupling of the coupled-cluster amplitude and multipliers, leading also to a significant reduction in computation time. Using the new simplified Lagrangian in combination with efficient wavefunction models such as RICC2 or LT-SOS-RICC2 and density-functional theory (DFT) for the environment molecules (CC2-in-DFT) enables the efficient study of biological applications such as the rhodopsin and visual cone pigments using ab initio methods as routine applications.

Study of Nb2O(y) (y = 2-5) anion and neutral clusters using anion photoelectron spectroscopy and density functional theory calculations.

PubMed

Mann, Jennifer E; Waller, Sarah E; Rothgeb, David W; Jarrold, Caroline Chick

2011-09-14

A study combining anion photoelectron spectroscopy and density functional theory calculations on the transition metal suboxide series, Nb(2)O(y)(-) (y = 2-5), is described. Photoelectron spectra of the clusters are obtained, and Franck-Condon simulations using calculated anion and neutral structures and frequencies are used to evaluate the calculations and assign transitions observed in the spectra. The spectra, several of which exhibit partially resolved vibrational structure, show an increase in electron affinity with increasing cluster oxidation state. Hole-burning experiments suggest that the photoelectron spectra of both Nb(2)O(2)(-) and Nb(2)O(3)(-) have contributions from more than one structural isomer. Reasonable agreement between experiment and computational results is found among all oxides. © 2011 American Institute of Physics

Density functional theory study on the metal-support interaction between a Au9 cluster and an anatase TiO2(001) surface.

PubMed

Jiang, Zong-You; Zhao, Zong-Yan

2017-08-23

Noble metals supported on TiO 2 surfaces have shown extraordinary photocatalytic properties in many important processes such as hydrogenation, water splitting, degradation of hazards, and so on. Using density functional theory calculations, this work has systematically investigated the microstructure and electronic structure of three different Au 9 isomers loaded on anatase TiO 2 (001) surface. The calculated results show that the interaction between the Au 9 cluster and the TiO 2 support is closely related to the adsorption site and the stability of the Au 9 cluster in the gas phase. The adsorption energy of the 2D configuration is larger than that of the 3D configuration of the Au 9 cluster, owing to the stronger interactions between more adsorption sites. The stable adsorption site for Au 9 clusters deposited on the anatase TiO 2 (001) surface tends to be the O 2c -O 2c hollow site. The presentation of the MIGS of the Au 9 cluster, the disappearance of surface states of the TiO 2 (001) surface, and the shifting of the Fermi level from the top of the valence band to the bottom of the conduction band suggest strong interactions between the Au 9 clusters and the TiO 2 (001) surface. Importantly, the electron transfer from the Au 9 clusters to the TiO 2 support occurs mainly through Au-O 2c interactions, which are mainly localized at the contact layer of the Au 9 clusters. These conclusions are useful to understand various physical and chemical properties of noble metal clusters loaded onto an oxide surface, and helpful to design novel metal/semiconductor functional composite materials and devices.

The ACS Survey of Galactic Globular Clusters. VIII. Effects of Environment on Globular Cluster Global Mass Functions

NASA Astrophysics Data System (ADS)

Paust, Nathaniel E. Q.; Reid, I. Neill; Piotto, Giampaolo; Aparicio, Antonio; Anderson, Jay; Sarajedini, Ata; Bedin, Luigi R.; Chaboyer, Brian; Dotter, Aaron; Hempel, Maren; Majewski, Steven; Marín-Franch, A.; Milone, Antonino; Rosenberg, Alfred; Siegel, Michael

2010-02-01

We have used observations obtained as part of the Hubble Space Telescope/ACS Survey of Galactic Globular Clusters to construct global present-day mass functions for 17 globular clusters utilizing multi-mass King models to extrapolate from our observations to the global cluster behavior. The global present-day mass functions for these clusters are well matched by power laws from the turnoff, ≈0.8 M sun, to 0.2-0.3 M sun on the lower main sequence. The slopes of those power-law fits, α, have been correlated with an extensive set of intrinsic and extrinsic cluster properties to investigate which parameters may influence the form of the present-day mass function. We do not confirm previous suggestions of correlations between α and either metallicity or Galactic location. However, we do find a strong statistical correlation with the related parameters central surface brightness, μ V , and inferred central density, ρ0. The correlation is such that clusters with denser cores (stronger binding energy) tend to have steeper mass functions (a higher proportion of low-mass stars), suggesting that dynamical evolution due to external interactions may have played a key role in determining α. Thus, the present-day mass function may owe more to nurture than to nature. Detailed modeling of external dynamical effects is therefore a requisite for determining the initial mass function for Galactic globular clusters.

Efficient Organometallic Spin Filter between Single-Wall Carbon Nanotube or Graphene Electrodes

NASA Astrophysics Data System (ADS)

Koleini, Mohammad; Paulsson, Magnus; Brandbyge, Mads

2007-05-01

We present a theoretical study of spin transport in a class of molecular systems consisting of an organometallic benzene-vanadium cluster placed in between graphene or single-wall carbon-nanotube-model contacts. Ab initio modeling is performed by combining spin density functional theory and nonequilibrium Green’s function techniques. We consider weak and strong cluster-contact bonds. Depending on the bonding we find from 73% (strong bonds) up to 99% (weak bonds) spin polarization of the electron transmission, and enhanced polarization with increased cluster length.

Distant Massive Clusters and Cosmology

NASA Technical Reports Server (NTRS)

Donahue, Megan

1999-01-01

We present a status report of our X-ray study and analysis of a complete sample of distant (z=0.5-0.8), X-ray luminous clusters of galaxies. We have obtained ASCA and ROSAT observations of the five brightest Extended Medium Sensitivity (EMSS) clusters with z > 0.5. We have constructed an observed temperature function for these clusters, and measured iron abundances for all of these clusters. We have developed an analytic expression for the behavior of the mass-temperature relation in a low-density universe. We use this mass-temperature relation together with a Press-Schechter-based model to derive the expected temperature function for different values of Omega-M. We combine this analysis with the observed temperature functions at redshifts from 0 - 0.8 to derive maximum likelihood estimates for the value of Omega-M. We report preliminary results of this analysis.

Al7CX (X=Li-Cs) clusters: Stability and the prospect for cluster materials

NASA Astrophysics Data System (ADS)

Ashman, C.; Khanna, S. N.; Pederson, M. R.; Kortus, J.

2000-12-01

Al7C clusters, recently found to have a high-electron affinity and exceptional stability, are shown to form ionic molecules when combined with alkali-metal atoms. Our studies, based on an ab initio gradient-corrected density-functional scheme, show that Al7CX (X=Li-Cs) clusters have a very low-electron affinity and a high-ionization potential. When combined, the two- and four-atom composite clusters of Al7CLi units leave the Al7C clusters almost intact. Preliminary studies indicate that Al7CLi may be suitable to form cluster-based materials.

Effects of cosmic string velocities and the origin of globular clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin, Ling; Yamanouchi, Shoma; Brandenberger, Robert, E-mail: ling.lin2@mail.mcgill.ca, E-mail: shoma.yamanouchi@mail.mcgill.ca, E-mail: rhb@physics.mcgill.ca

2015-12-01

With the hypothesis that cosmic string loops act as seeds for globular clusters in mind, we study the role that velocities of these strings will play in determining the mass distribution of globular clusters. Loops with high enough velocities will not form compact and roughly spherical objects and can hence not be the seeds for globular clusters. We compute the expected number density and mass function of globular clusters as a function of both the string tension and the peak loop velocity, and compare the results with the observational data on the mass distribution of globular clusters in our Milkymore » Way. We determine the critical peak string loop velocity above which the agreement between the string loop model for the origin of globular clusters (neglecting loop velocities) and observational data is lost.« less

Star Cluster Formation in Cosmological Simulations. I. Properties of Young Clusters

NASA Astrophysics Data System (ADS)

Li, Hui; Gnedin, Oleg Y.; Gnedin, Nickolay Y.; Meng, Xi; Semenov, Vadim A.; Kravtsov, Andrey V.

2017-01-01

We present a new implementation of star formation in cosmological simulations by considering star clusters as a unit of star formation. Cluster particles grow in mass over several million years at the rate determined by local gas properties, with high time resolution. The particle growth is terminated by its own energy and momentum feedback on the interstellar medium. We test this implementation for Milky Way-sized galaxies at high redshift by comparing the properties of model clusters with observations of young star clusters. We find that the cluster initial mass function is best described by a Schechter function rather than a single power law. In agreement with observations, at low masses the logarithmic slope is α ≈ 1.8{--}2, while the cutoff at high mass scales with the star formation rate (SFR). A related trend is a positive correlation between the surface density of the SFR and fraction of stars contained in massive clusters. Both trends indicate that the formation of massive star clusters is preferred during bursts of star formation. These bursts are often associated with major-merger events. We also find that the median timescale for cluster formation ranges from 0.5 to 4 Myr and decreases systematically with increasing star formation efficiency. Local variations in the gas density and cluster accretion rate naturally lead to the scatter of the overall formation efficiency by an order of magnitude, even when the instantaneous efficiency is kept constant. Comparison of the formation timescale with the observed age spread of young star clusters provides an additional important constraint on the modeling of star formation and feedback schemes.

Magic Numbers in Small Iron Clusters: A First-Principles Study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kim, Eunja; Mohrland, Andrew B.; Weck, Philippe F.

2014-10-03

We perform ab initio spin-polarized density functional calculations of Fen aggregates with n ≤ 17 atoms to reveal the origin of the observed magic numbers, which indicate particularly high stability of clusters with 7, 13 and 15 atoms. Our results clarify the controversy regarding the ground state geometry of clusters such as Fe5and indicate that magnetism plays an important role in determining the stability and magic numbers in small iron clusters.

Density Functional Investigation of the Inclusion of Gold Clusters on a CH 3 S Self-Assembled Lattice on Au(111)

DOE PAGES

Allen, Darnel J.; Archibald, Wayne E.; Harper, John A.; ...

2016-01-01

We employ first-principles density functional theoretical calculations to address the inclusion of gold (Au) clusters in a well-packed CH 3 S self-assembled lattice. We compute CH 3 S adsorption energies to quantify the energetic stability of the self-assembly and gold adsorption and dissolution energies to characterize the structural stability of a series of Au clusters adsorbed at the SAM-Au interface. Our results indicate that the inclusion of Au clusters with less than four Au atoms in the SAM-Au interface enhances the binding of CH 3 S species. In contrast, larger Au clusters destabilize the self-assembly. We attribute this effect tomore » the low-coordinated gold atoms in the cluster. For small clusters, these low-coordinated sites have significantly different electronic properties compared to larger islands, which makes the binding with the self-assembly energetically more favorable. Our results further indicate that Au clusters in the SAM-Au interface are thermodynamically unstable and they will tend to dissolve, producing Au adatoms incorporated in the self-assembly in the form of CH 3 S-Au-SCH 3 species. This is due to the strong S-Au bond which stabilizes single Au adatoms in the self-assembly. Our results provide solid insight into the impact of adatom islands at the CH 3 S-Au interface.« less

Density-Functional Theory with Dispersion-Correcting Potentials for Methane: Bridging the Efficiency and Accuracy Gap between High-Level Wave Function and Classical Molecular Mechanics Methods.

PubMed

Torres, Edmanuel; DiLabio, Gino A

2013-08-13

Large clusters of noncovalently bonded molecules can only be efficiently modeled by classical mechanics simulations. One prominent challenge associated with this approach is obtaining force-field parameters that accurately describe noncovalent interactions. High-level correlated wave function methods, such as CCSD(T), are capable of correctly predicting noncovalent interactions, and are widely used to produce reference data. However, high-level correlated methods are generally too computationally costly to generate the critical reference data required for good force-field parameter development. In this work we present an approach to generate Lennard-Jones force-field parameters to accurately account for noncovalent interactions. We propose the use of a computational step that is intermediate to CCSD(T) and classical molecular mechanics, that can bridge the accuracy and computational efficiency gap between them, and demonstrate the efficacy of our approach with methane clusters. On the basis of CCSD(T)-level binding energy data for a small set of methane clusters, we develop methane-specific, atom-centered, dispersion-correcting potentials (DCPs) for use with the PBE0 density-functional and 6-31+G(d,p) basis sets. We then use the PBE0-DCP approach to compute a detailed map of the interaction forces associated with the removal of a single methane molecule from a cluster of eight methane molecules and use this map to optimize the Lennard-Jones parameters for methane. The quality of the binding energies obtained by the Lennard-Jones parameters we obtained is assessed on a set of methane clusters containing from 2 to 40 molecules. Our Lennard-Jones parameters, used in combination with the intramolecular parameters of the CHARMM force field, are found to closely reproduce the results of our dispersion-corrected density-functional calculations. The approach outlined can be used to develop Lennard-Jones parameters for any kind of molecular system.

Geometric, electronic, and bonding properties of AuNM (N = 1-7, M = Ni, Pd, Pt) clusters.

PubMed

Yuan, D W; Wang, Yang; Zeng, Zhi

2005-03-15

Employing first-principles methods, based on density functional theory, we report the ground state geometric and electronic structures of gold clusters doped with platinum group atoms, Au(N)M (N = 1-7, M = Ni, Pd, Pt). The stability and electronic properties of Ni-doped gold clusters are similar to that of pure gold clusters with an enhancement of bond strength. Due to the strong d-d or s-d interplay between impurities and gold atoms originating in the relativistic effects and unique properties of dopant delocalized s-electrons in Pd- and Pt-doped gold clusters, the dopant atoms markedly change the geometric and electronic properties of gold clusters, and stronger bond energies are found in Pt-doped clusters. The Mulliken populations analysis of impurities and detailed decompositions of bond energies as well as a variety of density of states of the most stable dopant gold clusters are given to understand the different effects of individual dopant atom on bonding and electronic properties of dopant gold clusters. From the electronic properties of dopant gold clusters, the different chemical reactivity toward O(2), CO, or NO molecule is predicted in transition metal-doped gold clusters compared to pure gold clusters.

Valence and charge-transfer optical properties for some SinCm (m, n ≤ 12) clusters: Comparing TD-DFT, complete-basis-limit EOMCC, and benchmarks from spectroscopy

NASA Astrophysics Data System (ADS)

Lutz, Jesse J.; Duan, Xiaofeng F.; Ranasinghe, Duminda S.; Jin, Yifan; Margraf, Johannes T.; Perera, Ajith; Burggraf, Larry W.; Bartlett, Rodney J.

2018-05-01

Accurate optical characterization of the closo-Si12C12 molecule is important to guide experimental efforts toward the synthesis of nano-wires, cyclic nano-arrays, and related array structures, which are anticipated to be robust and efficient exciton materials for opto-electronic devices. Working toward calibrated methods for the description of closo-Si12C12 oligomers, various electronic structure approaches are evaluated for their ability to reproduce measured optical transitions of the SiC2, Si2Cn (n = 1-3), and Si3Cn (n = 1, 2) clusters reported earlier by Steglich and Maier [Astrophys. J. 801, 119 (2015)]. Complete-basis-limit equation-of-motion coupled-cluster (EOMCC) results are presented and a comparison is made between perturbative and renormalized non-iterative triples corrections. The effect of adding a renormalized correction for quadruples is also tested. Benchmark test sets derived from both measurement and high-level EOMCC calculations are then used to evaluate the performance of a variety of density functionals within the time-dependent density functional theory (TD-DFT) framework. The best-performing functionals are subsequently applied to predict valence TD-DFT excitation energies for the lowest-energy isomers of SinC and Sin-1C7-n (n = 4-6). TD-DFT approaches are then applied to the SinCn (n = 4-12) clusters and unique spectroscopic signatures of closo-Si12C12 are discussed. Finally, various long-range corrected density functionals, including those from the CAM-QTP family, are applied to a charge-transfer excitation in a cyclic (Si4C4)4 oligomer. Approaches for gauging the extent of charge-transfer character are also tested and EOMCC results are used to benchmark functionals and make recommendations.

Constrained variation in Jastrow method at high density

DOE Office of Scientific and Technical Information (OSTI.GOV)

Owen, J.C.; Bishop, R.F.; Irvine, J.M.

1976-11-01

A method is derived for constraining the correlation function in a Jastrow variational calculation which permits the truncation of the cluster expansion after two-body terms, and which permits exact minimization of the two-body cluster by functional variation. This method is compared with one previously proposed by Pandharipande and is found to be superior both theoretically and practically. The method is tested both on liquid /sup 3/He, by using the Lennard--Jones potential, and on the model system of neutrons treated as Boltzmann particles (''homework'' problem). Good agreement is found both with experiment and with other calculations involving the explicit evaluation ofmore » higher-order terms in the cluster expansion. The method is then applied to a more realistic model of a neutron gas up to a density of 4 neutrons per F/sup 3/, and is found to give ground-state energies considerably lower than those of Pandharipande. (AIP)« less

The cluster Ir4 and its interaction with a hydrogen impurity. A density functional study.

PubMed

Bussai, Chuenchit; Krüger, Sven; Vayssilov, Georgi N; Rösch, Notker

2005-07-07

To contribute to the understanding of how iridium particles act as catalysts for hydrogenation and dehydrogenation of hydrocarbons, we have determined structures and binding energies of various isomers of Ir(4) as well as HIr(4) on the basis of relativistic density functional theory. The most stable isomer of Ir(4) showed a square planar structure with eight unpaired electrons. The tetrahedral structure, experimentally suggested for supported species, was calculated 49 kJ mol(-1) less stable. Hydrogen coordinates preferentially to a single Ir center of the planar cluster with a binding energy of up to 88 kJ mol(-1) with respect to the atom in the H(2) molecule. Terminal interaction of hydrogen with an Ir(4) tetrahedron causes the cluster to open to a butterfly structure. We calculated terminal binding of hydrogen at different Ir(4) isomers to be more stable than bridge coordination, at variance with earlier studies.

Application of Time-Dependent Density Functional and Natural Bond Orbital Theories to the UV-vis Absorption Spectra of Some Phenolic Compounds.

PubMed

Marković, Svetlana; Tošović, Jelena

2015-09-03

The UV-vis properties of 22 natural phenolic compounds, comprising anthraquinones, neoflavonoids, and flavonoids were systematically examined. The time-dependent density functional theory (TDDFT) approach in combination with the B3LYP, B3LYP-D2, B3P86, and M06-2X functionals was used to simulate the UV-vis spectra of the investigated compounds. It was shown that all methods exhibit very good (B3LYP slightly better) performance in reproducing the examined UV-vis spectra. However, the shapes of the Kohn-Sham molecular orbitals (MOs) involved in electronic transitions were misleading in constructing the MO correlation diagrams. To provide better understanding of redistribution of electron density upon excitation, the natural bond orbital (NBO) analysis was applied. Bearing in mind the spatial and energetic separations, as well as the character of the π bonding, lone pair, and π* antibonding natural localized molecular orbitals (NLMOs), the "NLMO clusters" were constructed. NLMO cluster should be understood as a part of a molecule characterized with distinguished electron density. It was shown that all absorption bands including all electronic transitions need to be inspected to fully understand the UV-vis spectrum of a certain compound, and, thus, to learn more about its UV-vis light absorption. Our investigation showed that the TDDFT and NBO theories are complementary, as the results from the two approaches can be combined to interpret the UV-vis spectra. Agreement between the predictions of the TDDFT approach and those based on the NLMO clusters is excellent in the case of major electronic transitions and long wavelengths. It should be emphasized that the approach for investigation of UV-vis light absorption based on the NLMO clusters is applied for the first time.

Analyzing coastal environments by means of functional data analysis

NASA Astrophysics Data System (ADS)

Sierra, Carlos; Flor-Blanco, Germán; Ordoñez, Celestino; Flor, Germán; Gallego, José R.

2017-07-01

Here we used Functional Data Analysis (FDA) to examine particle-size distributions (PSDs) in a beach/shallow marine sedimentary environment in Gijón Bay (NW Spain). The work involved both Functional Principal Components Analysis (FPCA) and Functional Cluster Analysis (FCA). The grainsize of the sand samples was characterized by means of laser dispersion spectroscopy. Within this framework, FPCA was used as a dimension reduction technique to explore and uncover patterns in grain-size frequency curves. This procedure proved useful to describe variability in the structure of the data set. Moreover, an alternative approach, FCA, was applied to identify clusters and to interpret their spatial distribution. Results obtained with this latter technique were compared with those obtained by means of two vector approaches that combine PCA with CA (Cluster Analysis). The first method, the point density function (PDF), was employed after adapting a log-normal distribution to each PSD and resuming each of the density functions by its mean, sorting, skewness and kurtosis. The second applied a centered-log-ratio (clr) to the original data. PCA was then applied to the transformed data, and finally CA to the retained principal component scores. The study revealed functional data analysis, specifically FPCA and FCA, as a suitable alternative with considerable advantages over traditional vector analysis techniques in sedimentary geology studies.

Equilibrium stellar systems with spindle singularities

NASA Technical Reports Server (NTRS)

Shapiro, Stuart L.; Teukolsky, Saul A.

1992-01-01

Equilibrium sequences of axisymmetric Newtonian clusters that tend toward singular states are constructed. The distribution functions are chosen to be of the form f = f(E, Jz). The numerical method then determines the density and gravitational potential self-consistently to satisfy Poisson's equation. For the prolate models, spindle singularities arise from the depletion of angular momentum near the symmetry axis. While the resulting density enhancement is confined to the region near the axis, the influence of the spindle extends much further out through its tidal gravitational field. Centrally condensed prolate clusters may contain strong-field regions even though the spindle mass is small and the mean cluster eccentricity is not extreme. While the calculations performed here are entirely Newtonian, the issue of singularities is an important topic in general relativity. Equilibrium solutions for relativistic star clusters can provide a testing ground for exploring this issue. The methods used in this paper for building nonspherical clusters can be extended to relativistic systems.

Probing the Structures and Electronic Properties of Dual-Phosphorus-Doped Gold Cluster Anions (AunP-2, n = 1–8): A Density functional Theory Investigation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Kang-Ming; Huang, Teng; Liu, Yi-Rong

2015-07-29

The geometries of gold clusters doped with two phosphorus atoms, (AunP-2, n = 1–8) were investigated using density functional theory (DFT) methods. Various two-dimensional (2D) and three-dimensional (3D) structures of the doped clusters were studied. The results indicate that the structures of dual-phosphorus-doped gold clusters exhibit large differences from those of pure gold clusters with small cluster sizes. In our study, as for Au6P-2, two cis–trans isomers were found. The global minimum of Au8P-2 presents a similar configuration to that of Au-20, a pyramid-shaped unit, and the potential novel optical and catalytic properties of this structure warrant further attention. Themore » higher stability of AunP-2 clusters relative to Au-n+2 (n = 1–8) clusters was verified based on various energy parameters, and the results indicate that the phosphorus atom can improve the stabilities of the gold clusters. We then explored the evolutionary path of (n = 1–8) clusters. We found that AunP-2 clusters exhibit the 2D–3D structural transition at n = 6, which is much clearer and faster than that of pure gold clusters and single-phosphorus-doped clusters. The electronic properties of AunP-2 (n = 1–8) were then investigated. The photoelectron spectra provide additional fundamental information on the structures and molecular orbitals shed light on the evolution of AunP-2 (n = 1–8). Natural bond orbital (NBO) described the charge distribution in stabilizing structures and revealed the strong relativistic effects of the gold atoms.« less

Density functional theory study of small X-doped Mg(n) (X = Fe, Co, Ni, n = 1-9) bimetallic clusters: equilibrium structures, stabilities, electronic and magnetic properties.

PubMed

Kong, Fanjie; Hu, Yanfei

2014-03-01

The geometries, stabilities, and electronic and magnetic properties of Mg(n) X (X = Fe, Co, Ni, n = 1-9) clusters were investigated systematically within the framework of the gradient-corrected density functional theory. The results show that the Mg(n)Fe, Mg(n)Co, and Mg(n)Ni clusters have similar geometric structures and that the X atom in Mg(n)X clusters prefers to be endohedrally doped. The average atomic binding energies, fragmentation energies, second-order differences in energy, and HOMO-LUMO gaps show that Mg₄X (X = Fe, Co, Ni) clusters possess relatively high stability. Natural population analysis was performed and the results showed that the 3s and 4s electrons always transfer to the 3d and 4p orbitals in the bonding atoms, and that electrons also transfer from the Mg atoms to the doped atoms (Fe, Co, Ni). In addition, the spin magnetic moments were analyzed and compared. Several clusters, such as Mg₁,₂,₃,₄,₅,₆,₈,₉Fe, Mg₁,₂,₄,₅,₆,₈,₉Co, and Mg₁,₂,₅,₆,₇,₉Ni, present high magnetic moments (4 μ(B), 3 μ(B), and 2 μ(B), respectively).

The young star cluster population of M51 with LEGUS - II. Testing environmental dependences

NASA Astrophysics Data System (ADS)

Messa, Matteo; Adamo, A.; Calzetti, D.; Reina-Campos, M.; Colombo, D.; Schinnerer, E.; Chandar, R.; Dale, D. A.; Gouliermis, D. A.; Grasha, K.; Grebel, E. K.; Elmegreen, B. G.; Fumagalli, M.; Johnson, K. E.; Kruijssen, J. M. D.; Östlin, G.; Shabani, F.; Smith, L. J.; Whitmore, B. C.

2018-06-01

It has recently been established that the properties of young star clusters (YSCs) can vary as a function of the galactic environment in which they are found. We use the cluster catalogue produced by the Legacy Extragalactic UV Survey (LEGUS) collaboration to investigate cluster properties in the spiral galaxy M51. We analyse the cluster population as a function of galactocentric distance and in arm and inter-arm regions. The cluster mass function exhibits a similar shape at all radial bins, described by a power law with a slope close to -2 and an exponential truncation around 105 M⊙. While the mass functions of the YSCs in the spiral arm and inter-arm regions have similar truncation masses, the inter-arm region mass function has a significantly steeper slope than the one in the arm region, a trend that is also observed in the giant molecular cloud mass function and predicted by simulations. The age distribution of clusters is dependent on the region considered, and is consistent with rapid disruption only in dense regions, while little disruption is observed at large galactocentric distances and in the inter-arm region. The fraction of stars forming in clusters does not show radial variations, despite the drop in the H2 surface density measured as a function of galactocentric distance. We suggest that the higher disruption rate observed in the inner part of the galaxy is likely at the origin of the observed flat cluster formation efficiency radial profile.

Structure, reactivity, and electronic properties of V-doped Co clusters

NASA Astrophysics Data System (ADS)

Datta, Soumendu; Kabir, Mukul; Saha-Dasgupta, Tanusri; Mookerjee, Abhijit

2009-08-01

Structures and physicochemical properties of V-doped Co13 clusters have been studied in detail using density-functional-theory-based first-principles method. We have found anomalous variation in stability of the doped clusters with increasing V concentration, which has been nicely demonstrated in terms of energetics and electronic properties of the clusters. Our study explains the nonmonotonic variation in reactivity of Co13-mVm clusters toward H2 molecules as reported experimentally [Nonose , J. Phys. Chem. 94, 2744 (1990)]. Moreover, it provides useful insight into the cluster geometry and chemically active sites on the cluster surface, which can help to design better catalytic processes.

Hole localization in Fe2O3 from density functional theory and wave-function-based methods

NASA Astrophysics Data System (ADS)

Ansari, Narjes; Ulman, Kanchan; Camellone, Matteo Farnesi; Seriani, Nicola; Gebauer, Ralph; Piccinin, Simone

2017-08-01

Hematite (α -Fe2O3 ) is a promising photocatalyst material for water splitting, where photoinduced holes lead to the oxidation of water and the release of molecular oxygen. In this work, we investigate the properties of holes in hematite using density functional theory (DFT) calculations with hybrid functionals. We find that holes form small polarons and, depending on the fraction of exact exchange included in the PBE0 functional, the site where the holes localize changes from Fe to O. We find this result to be independent of the size and structure of the system: small Fe2O3 clusters with tetrahedral coordination, larger clusters with octahedral coordination, Fe2O3 (001) surfaces in contact with water, and bulk Fe2O3 display a very similar behavior in terms of hole localization as a function of the fraction of exact exchange. We then use wave-function-based methods such as coupled cluster with single and double excitations and Møller-Plesset second-order perturbation theory applied on a cluster model of Fe2O3 to shed light on which of the two solutions is correct. We find that these high-level quantum chemistry methods suggest holes in hematite are localized on oxygen atoms. We also explore the use of the DFT +U approach as a computationally convenient way to overcome the known limitations of generalized gradient approximation functionals and recover a gap in line with experiments and hole localization on oxygen in agreement with quantum chemistry methods.

Measuring the Mass Distribution in Z is Approximately 0.2 Cluster Lenses with XMM, HST and CFHT

NASA Technical Reports Server (NTRS)

2004-01-01

Being the most massive gravitationally bound objects in the Universe, clusters of galaxies are prime targets for studies of structure formation and evolution. Specifically the comoving space density of virialized clusters of a given mass (or X-ray temperature), but also the frequency and degree of substructure, as well as the shape of the cluster mass profile are quantities whose current values and evolution as a function of lookback time can provide important constraints on the cosmological and physical parameters of structure formation theories. The project funded by NASA grant NAG 5-10041 intended to take such studies to a new level by combining observations of a well-selected cluster sample by three state-of-the-art telescopes: HST, to accurately measure the mass distribution in the cluster core (approx. 0.5 h(sup -1)(sub 50) Mpc) via strong gravitational lensing; CFHT, to measure the large scale mass distribution out to approx. 3 Mpc via weak lensing; and XMM, to measure the gas density and temperature distribution accurately on intermediate scales < 1.5 Mpc. XMM plays a pivotal role in this context as the calibration of X-ray mass measurements through accurate, spatially resolved X-ray temperature measurements (particularly in the cosmologically most sensitive range of kT> 5 keV) is central to the questions outlined above. This set of observations promised to yield the best cluster mass measurements obtained so far for a representative sample, thus allowing us to: 1) Measure the high-mass end of the local cluster mass function; 2) Test predictions of a universal cluster mass profile; 3) calibrate the mass-temperature and temperature-luminosity relations for clusters and the scatter around these relations, which is vital for studies of cluster evolution using the X-ray temperature and X-ray luminosity functions.

Cosmological constraints from Chandra observations of galaxy clusters.

PubMed

Allen, Steven W

2002-09-15

Chandra observations of rich, relaxed galaxy clusters allow the properties of the X-ray gas and the total gravitating mass to be determined precisely. Here, we present results for a sample of the most X-ray luminous, dynamically relaxed clusters known. We show that the Chandra data and independent gravitational lensing studies provide consistent answers on the mass distributions in the clusters. The mass profiles exhibit a form in good agreement with the predictions from numerical simulations. Combining Chandra results on the X-ray gas mass fractions in the clusters with independent measurements of the Hubble constant and the mean baryonic matter density in the Universe, we obtain a tight constraint on the mean total matter density of the Universe, Omega(m), and an interesting constraint on the cosmological constant, Omega(Lambda). We also describe the 'virial relations' linking the masses, X-ray temperatures and luminosities of galaxy clusters. These relations provide a key step in linking the observed number density and spatial distribution of clusters to the predictions from cosmological models. The Chandra data confirm the presence of a systematic offset of ca. 40% between the normalization of the observed mass-temperature relation and the predictions from standard simulations. This finding leads to a significant revision of the best-fit value of sigma(8) inferred from the observed temperature and luminosity functions of clusters.

Photoelectron Spectroscopy and Density Functional Theory Studies of Iron Sulfur (FeS)m- (m = 2-8) Cluster Anions: Coexisting Multiple Spin States.

PubMed

Yin, Shi; Bernstein, Elliot R

2017-10-05

Iron sulfur cluster anions (FeS) m - (m = 2-8) are studied by photoelectron spectroscopy (PES) at 3.492 eV (355 nm) and 4.661 eV (266 nm) photon energies, and by density functional theory (DFT) calculations. The most probable structures and ground state spin multiplicities for (FeS) m - (m = 2-8) clusters are tentatively assigned through a comparison of their theoretical and experiment first vertical detachment energy (VDE) values. Many spin states lie within 0.5 eV of the ground spin state for the larger (FeS) m - (m ≥ 4) clusters. Theoretical VDEs of these low lying spin states are in good agreement with the experimental VDE values. Therefore, multiple spin states of each of these iron sulfur cluster anions probably coexist under the current experimental conditions. Such available multiple spin states must be considered when evaluating the properties and behavior of these iron sulfur clusters in real chemical and biological systems. The experimental first VDEs of (FeS) m - (m = 1-8) clusters are observed to change with the cluster size (number m). The first VDE trends noted can be related to the different properties of the highest singly occupied molecular orbitals (NBO, HSOMOs) of each cluster anion. The changing nature of the NBO/HSOMO of these (FeS) m - (m = 1-8) clusters from a p orbital on S, to a d orbital on Fe, and to an Fe-Fe bonding orbital is probably responsible for the observed increasing trend for their first VDEs with respect to m.

A density functional theory for colloids with two multiple bonding associating sites.

PubMed

Haghmoradi, Amin; Wang, Le; Chapman, Walter G

2016-06-22

Wertheim's multi-density formalism is extended for patchy colloidal fluids with two multiple bonding patches. The theory is developed as a density functional theory to predict the properties of an associating inhomogeneous fluid. The equation of state developed for this fluid depends on the size of the patch, and includes formation of cyclic, branched and linear clusters of associated species. The theory predicts the density profile and the fractions of colloids in different bonding states versus the distance from one wall as a function of bulk density and temperature. The predictions from our theory are compared with previous results for a confined fluid with four single bonding association sites. Also, comparison between the present theory and Monte Carlo simulation indicates a good agreement.

Formation of young massive clusters from turbulent molecular clouds

NASA Astrophysics Data System (ADS)

Fujii, Michiko; Portegies Zwart, Simon

2015-08-01

We simulate the formation and evolution of young star clusters using smoothed-particle hydrodynamics (SPH) and direct N-body methods. We start by performing SPH simulations of the giant molecular cloud with a turbulent velocity field, a mass of 10^4 to 10^6 M_sun, and a density between 17 and 1700 cm^-3. We continue the SPH simulations for a free-fall time scale, and analyze the resulting structure of the collapsed cloud. We subsequently replace a density-selected subset of SPH particles with stars. As a consequence, the local star formation efficiency exceeds 30 per cent, whereas globally only a few per cent of the gas is converted to stars. The stellar distribution is very clumpy with typically a dozen bound conglomerates that consist of 100 to 10000 stars. We continue to evolve the stars dynamically using the collisional N-body method, which accurately treats all pairwise interactions, stellar collisions and stellar evolution. We analyze the results of the N-body simulations at 2 Myr and 10 Myr. From dense massive molecular clouds, massive clusters grow via hierarchical merging of smaller clusters. The shape of the cluster mass function that originates from an individual molecular cloud is consistent with a Schechter function with a power-law slope of beta = -1.73 at 2 Myr and beta = -1.67 at 10 Myr, which fits to observed cluster mass function of the Carina region. The superposition of mass functions have a power-law slope of < -2, which fits the observed mass function of star clusters in the Milky Way, M31 and M83. We further find that the mass of the most massive cluster formed in a single molecular cloud with a mass of M_g scales with 6.1 M_g^0.51 which also agrees with recent observation in M51. The molecular clouds which can form massive clusters are much denser than those typical in the Milky Way. The velocity dispersion of such molecular clouds reaches 20 km/s and it is consistent with the relative velocity of the molecular clouds observed near NGC 3603 and Westerlund 2, for which a triggered star formation by cloud-cloud collisions is suggested.

Structural and magnetic properties of FeGen-/0 (n = 3-12) clusters: Mass-selected anion photoelectron spectroscopy and density functional theory calculations

NASA Astrophysics Data System (ADS)

Deng, Xiao-Jiao; Kong, Xiang-Yu; Liang, Xiaoqing; Yang, Bin; Xu, Hong-Guang; Xu, Xi-Ling; Feng, Gang; Zheng, Wei-Jun

2017-12-01

The structural, electronic, and magnetic properties of FeGen-/0 (n = 3-12) clusters were investigated by using anion photoelectron spectroscopy in combination with density functional theory calculations. For both anionic and neutral FeGen (n = 3-12) clusters with n ≤ 7, the dominant structures are exohedral. The FeGe8-/0 clusters have half-encapsulated boat-shaped structures, and the opening of the boat-shaped structure is gradually covered by the additional Ge atoms to form Gen cage from n = 9 to 11. The structures of FeGe10-/0 can be viewed as two Ge atoms symmetrically capping the opening of the boat-shaped structure of FeGe8, and those of FeGe12-/0 are distorted hexagonal prisms with the Fe atom at the center. Natural population analysis shows that there is an electron transfer from the Ge atoms to the Fe atom at n = 8-12. The total magnetic moment of FeGen-/0 and local magnetic moment of the Fe atom have not been quenched.

Star cluster formation in cosmological simulations. I. Properties of young clusters

DOE PAGES

Li, Hui; Gnedin, Oleg Y.; Gnedin, Nickolay Y.; ...

2017-01-03

We present a new implementation of star formation in cosmological simulations by considering star clusters as a unit of star formation. Cluster particles grow in mass over several million years at the rate determined by local gas properties, with high time resolution. The particle growth is terminated by its own energy and momentum feedback on the interstellar medium. We test this implementation for Milky Way-sized galaxies at high redshift by comparing the properties of model clusters with observations of young star clusters. We find that the cluster initial mass function is best described by a Schechter function rather than a single power law. In agreement with observations, at low masses the logarithmic slope ismore » $$\\alpha \\approx 1.8\\mbox{–}2$$, while the cutoff at high mass scales with the star formation rate (SFR). A related trend is a positive correlation between the surface density of the SFR and fraction of stars contained in massive clusters. Both trends indicate that the formation of massive star clusters is preferred during bursts of star formation. These bursts are often associated with major-merger events. We also find that the median timescale for cluster formation ranges from 0.5 to 4 Myr and decreases systematically with increasing star formation efficiency. Local variations in the gas density and cluster accretion rate naturally lead to the scatter of the overall formation efficiency by an order of magnitude, even when the instantaneous efficiency is kept constant. As a result, comparison of the formation timescale with the observed age spread of young star clusters provides an additional important constraint on the modeling of star formation and feedback schemes.« less

Structural and electronic properties of Aun-xPtx (n = 2-14; x ⩽ n) clusters: The density functional theory investigation

NASA Astrophysics Data System (ADS)

Yuan, H. K.; Kuang, A. L.; Tian, C. L.; Chen, H.

2014-03-01

The structural evolutions and electronic properties of bimetallic Aun-xPtx (n = 2-14; x ⩽ n) clusters are investigated by using the density functional theory (DFT) with the generalized gradient approximation (GGA). The monatomic doping Aun-1Pt clusters are emphasized and compared with the corresponding pristine Aun clusters. The results reveal that the planar configurations are favored for both Aun-1Pt and Aun clusters with size up to n = 13, and the former often employ the substitution patterns based on the structures of the latter. The most stable clusters are Au6 and Au6Pt, which adopt regular planar triangle (D3h) and hexagon-ring (D6h) structures and can be regarded as the preferential building units in designing large clusters. For Pt-rich bimetallic clusters, their structures can be obtained from the substitution of Pt atoms by Au atoms from the Ptn structures, where Pt atoms assemble together and occupy the center yet Au atoms prefer the apex positions showing a segregation effect. With respect to pristine Au clusters, AunPt clusters exhibit somewhat weaker and less pronounced odd-even oscillations in the highest occupied and lowest unoccupied molecular-orbital gaps (HOMO-LUMO gap), electron affinity (EA), and ionization potential (IP) due to the partially released electron pairing effect. The analyses of electronic structure indicate that Pt atoms in AuPt clusters would delocalize their one 6s and one 5d electrons to contribute the electronic shell closure. The sp-d hybridizations as well as the d-d interactions between the host Au and dopant Pt atoms result in the enhanced stabilities of AuPt clusters.

Star cluster formation in cosmological simulations. I. Properties of young clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Hui; Gnedin, Oleg Y.; Gnedin, Nickolay Y.

We present a new implementation of star formation in cosmological simulations by considering star clusters as a unit of star formation. Cluster particles grow in mass over several million years at the rate determined by local gas properties, with high time resolution. The particle growth is terminated by its own energy and momentum feedback on the interstellar medium. We test this implementation for Milky Way-sized galaxies at high redshift by comparing the properties of model clusters with observations of young star clusters. We find that the cluster initial mass function is best described by a Schechter function rather than a single power law. In agreement with observations, at low masses the logarithmic slope ismore » $$\\alpha \\approx 1.8\\mbox{–}2$$, while the cutoff at high mass scales with the star formation rate (SFR). A related trend is a positive correlation between the surface density of the SFR and fraction of stars contained in massive clusters. Both trends indicate that the formation of massive star clusters is preferred during bursts of star formation. These bursts are often associated with major-merger events. We also find that the median timescale for cluster formation ranges from 0.5 to 4 Myr and decreases systematically with increasing star formation efficiency. Local variations in the gas density and cluster accretion rate naturally lead to the scatter of the overall formation efficiency by an order of magnitude, even when the instantaneous efficiency is kept constant. As a result, comparison of the formation timescale with the observed age spread of young star clusters provides an additional important constraint on the modeling of star formation and feedback schemes.« less

A catalogue of masses, structural parameters and velocity dispersion profiles of 112 Milky Way globular clusters

NASA Astrophysics Data System (ADS)

Baumgardt, H.; Hilker, M.

2018-05-01

We have determined masses, stellar mass functions and structural parameters of 112 Milky Way globular clusters by fitting a large set of N-body simulations to their velocity dispersion and surface density profiles. The velocity dispersion profiles were calculated based on a combination of more than 15,000 high-precision radial velocities which we derived from archival ESO/VLT and Keck spectra together with ˜20, 000 published radial velocities from the literature. Our fits also include the stellar mass functions of the globular clusters, which are available for 47 clusters in our sample, allowing us to self-consistently take the effects of mass segregation and ongoing cluster dissolution into account. We confirm the strong correlation between the global mass functions of globular clusters and their relaxation times recently found by Sollima & Baumgardt (2017). We also find a correlation of the escape velocity from the centre of a globular cluster and the fraction of first generation stars (FG) in the cluster recently derived for 57 globular clusters by Milone et al. (2017), but no correlation between the FG star fraction and the global mass function of a globular cluster. This could indicate that the ability of a globular cluster to keep the wind ejecta from the polluting star(s) is the crucial parameter determining the presence and fraction of second generation stars and not its later dynamical mass loss.

SOTXTSTREAM: Density-based self-organizing clustering of text streams.

PubMed

Bryant, Avory C; Cios, Krzysztof J

2017-01-01

A streaming data clustering algorithm is presented building upon the density-based self-organizing stream clustering algorithm SOSTREAM. Many density-based clustering algorithms are limited by their inability to identify clusters with heterogeneous density. SOSTREAM addresses this limitation through the use of local (nearest neighbor-based) density determinations. Additionally, many stream clustering algorithms use a two-phase clustering approach. In the first phase, a micro-clustering solution is maintained online, while in the second phase, the micro-clustering solution is clustered offline to produce a macro solution. By performing self-organization techniques on micro-clusters in the online phase, SOSTREAM is able to maintain a macro clustering solution in a single phase. Leveraging concepts from SOSTREAM, a new density-based self-organizing text stream clustering algorithm, SOTXTSTREAM, is presented that addresses several shortcomings of SOSTREAM. Gains in clustering performance of this new algorithm are demonstrated on several real-world text stream datasets.

Enhanced momentum feedback from clustered supernovae

NASA Astrophysics Data System (ADS)

Gentry, Eric S.; Krumholz, Mark R.; Dekel, Avishai; Madau, Piero

2017-02-01

Young stars typically form in star clusters, so the supernovae (SNe) they produce are clustered in space and time. This clustering of SNe may alter the momentum per SN deposited in the interstellar medium (ISM) by affecting the local ISM density, which in turn affects the cooling rate. We study the effect of multiple SNe using idealized 1D hydrodynamic simulations which explore a large parameter space of the number of SNe, and the background gas density and metallicity. The results are provided as a table and an analytic fitting formula. We find that for clusters with up to ˜100 SNe, the asymptotic momentum scales superlinearly with the number of SNe, resulting in a momentum per SN which can be an order of magnitude larger than for a single SN, with a maximum efficiency for clusters with 10-100 SNe. We argue that additional physical processes not included in our simulations - self-gravity, breakout from a galactic disc, and galactic shear - can slightly reduce the momentum enhancement from clustering, but the average momentum per SN still remains a factor of 4 larger than the isolated SN value when averaged over a realistic cluster mass function for a star-forming galaxy. We conclude with a discussion of the possible role of mixing between hot and cold gas, induced by multidimensional instabilities or pre-existing density variations, as a limiting factor in the build-up of momentum by clustered SNe, and suggest future numerical experiments to explore these effects.

Fundamental Theory of Crystal Decomposition

DTIC Science & Technology

1991-05-01

rather than combine them as is often the case in a computation based on the density functional method.4 In the Case of a cluster embedded in a...classical lattice, special care needs to be taken to ensure that mathematical consistency is achieved between the cluster and the embedding lattice. This has...localizing potential or KKLP. Simulation of a large crystallite or an infinite lattice containing a point defect represented by a cluster and a

Ligand Effects in Aluminum Cluster based Energetic Materials

DTIC Science & Technology

2017-09-01

was recently reported and the effect of their increased steric bulk is discussed here. Experimental results and density functional theory (DFT...analysis show that these clusters are enthalpically more stable than the Cp* variant, due primarily to non -covalent interactions (NCIs) across ligand...C5Me4iPr), two clusters similar to Al4Cp*4, was recently reported and the effect of their increased steric bulk is discussed here. Experimental

Smallest fullerene-like silicon cage stabilized by a V(2) unit.

PubMed

Xu, Hong-Guang; Kong, Xiang-Yu; Deng, Xiao-Jiao; Zhang, Zeng-Guang; Zheng, Wei-Jun

2014-01-14

We conducted a combined anion photoelectron spectroscopy and density functional theory study on V2Si20 cluster. Our results show that the V2Si20 cluster has an elongated dodecahedron cage structure with a V2 unit encapsulated inside the cage. It is the smallest fullerene-like silicon cage and can be used as building block to make cluster-assembled materials, such as pearl-chain style nanowires.

Smallest fullerene-like silicon cage stabilized by a V2 unit

NASA Astrophysics Data System (ADS)

Xu, Hong-Guang; Kong, Xiang-Yu; Deng, Xiao-Jiao; Zhang, Zeng-Guang; Zheng, Wei-Jun

2014-01-01

We conducted a combined anion photoelectron spectroscopy and density functional theory study on V2Si20 cluster. Our results show that the V2Si20 cluster has an elongated dodecahedron cage structure with a V2 unit encapsulated inside the cage. It is the smallest fullerene-like silicon cage and can be used as building block to make cluster-assembled materials, such as pearl-chain style nanowires.

Exact hierarchical clustering in one dimension. [in universe

NASA Technical Reports Server (NTRS)

Williams, B. G.; Heavens, A. F.; Peacock, J. A.; Shandarin, S. F.

1991-01-01

The present adhesion model-based one-dimensional simulations of gravitational clustering have yielded bound-object catalogs applicable in tests of analytical approaches to cosmological structure formation. Attention is given to Press-Schechter (1974) type functions, as well as to their density peak-theory modifications and the two-point correlation function estimated from peak theory. The extent to which individual collapsed-object locations can be predicted by linear theory is significant only for objects of near-characteristic nonlinear mass.

Stellar age spreads in clusters as imprints of cluster-parent clump densities

DOE Office of Scientific and Technical Information (OSTI.GOV)

Parmentier, G.; Grebel, E. K.; Pfalzner, S.

2014-08-20

It has recently been suggested that high-density star clusters have stellar age distributions much narrower than that of the Orion Nebula Cluster, indicating a possible trend of narrower age distributions for denser clusters. We show this effect to likely arise from star formation being faster in gas with a higher density. We model the star formation history of molecular clumps in equilibrium by associating a star formation efficiency per free-fall time, ε{sub ff}, to their volume density profile. We focus on the case of isothermal spheres and we obtain the evolution with time of their star formation rate. Our modelmore » predicts a steady decline of the star formation rate, which we quantify with its half-life time, namely, the time needed for the star formation rate to drop to half its initial value. Given the uncertainties affecting the star formation efficiency per free-fall time, we consider two distinct values: ε{sub ff} = 0.1 and ε{sub ff} = 0.01. When ε{sub ff} = 0.1, the half-life time is of the order of the clump free-fall time, τ{sub ff}. As a result, the age distributions of stars formed in high-density clumps have smaller full-widths at half-maximum than those of stars formed in low-density clumps. When the star formation efficiency per free-fall time is 0.01, the half-life time is 10 times longer, i.e., 10 clump free-fall times. We explore what happens if the duration of star formation is shorter than 10τ{sub ff}, that is, if the half-life time of the star formation rate cannot be defined. There, we build on the invariance of the shape of the young cluster mass function to show that an anti-correlation between the clump density and the duration of star formation is expected. We therefore conclude that, regardless of whether the duration of star formation is longer than the star formation rate half-life time, denser molecular clumps yield narrower star age distributions in clusters. Published densities and stellar age spreads of young clusters and star-forming regions actually suggest that the timescale for star formation is of order 1-4τ{sub ff}. We also discuss how the age bin size and uncertainties in stellar ages affect our results. We conclude that there is no need to invoke the existence of multiple cluster formation mechanisms to explain the observed range of stellar age spreads in clusters.« less

Exploring N-Rich Phases in Li(x)N(y) Clusters for Hydrogen Storage at Nanoscale.

PubMed

Bhattacharya, Amrita; Bhattacharya, Saswata

2015-09-17

We have performed cascade genetic algorithm and ab initio atomistic thermodynamics under the framework of first-principles-based hybrid density functional theory to study the (meta-)stability of a wide range of Li(x)N(y) clusters. We found that hybrid xc-functional is essential to address this problem as a local/semilocal functional simply fails even to predict a qualitative prediction. Most importantly, we find that though in bulk lithium nitride, the Li-rich phase, that is, Li3N, is the stable stoichiometry; in small Li(x)N(y) clusters, N-rich phases are more stable at thermodynamic equilibrium. We further show that these N-rich clusters are promising hydrogen storage material because of their easy adsorption and desorption ability at respectively low (≤300 K) and moderately high temperature (≥600 K).

Actinide chemistry using singlet-paired coupled cluster and its combinations with density functionals

NASA Astrophysics Data System (ADS)

Garza, Alejandro J.; Sousa Alencar, Ana G.; Scuseria, Gustavo E.

2015-12-01

Singlet-paired coupled cluster doubles (CCD0) is a simplification of CCD that relinquishes a fraction of dynamic correlation in order to be able to describe static correlation. Combinations of CCD0 with density functionals that recover specifically the dynamic correlation missing in the former have also been developed recently. Here, we assess the accuracy of CCD0 and CCD0+DFT (and variants of these using Brueckner orbitals) as compared to well-established quantum chemical methods for describing ground-state properties of singlet actinide molecules. The f0 actinyl series (UO22+, NpO23+, PuO24+), the isoelectronic NUN, and thorium (ThO, ThO2+) and nobelium (NoO, NoO2) oxides are studied.

Theoretical Analysis of Optical Absorption and Emission in Mixed Noble Metal Nanoclusters.

PubMed

Day, Paul N; Pachter, Ruth; Nguyen, Kiet A

2018-04-26

In this work, we studied theoretically two hybrid gold-silver clusters, which were reported to have dual-band emission, using density functional theory (DFT) and linear and quadratic response time-dependent DFT (TDDFT). Hybrid functionals were found to successfully predict absorption and emission, although explanation of the NIR emission from the larger cluster (cluster 1) requires significant vibrational excitation in the final state. For the smaller cluster (cluster 2), the Δ H(0-0) value calculated for the T1 → S0 transition, using the PBE0 functional, is in good agreement with the measured NIR emission, and the calculated T2 → S0 value is in fair agreement with the measured visible emission. The calculated T1 → S0 phosphorescence Δ H(0-0) for cluster 1 is close to the measured visible emission energy. In order for the calculated phosphorescence for cluster 1 to agree with the intense NIR emission reported experimentally, the vibrational energy of the final state (S0) is required to be about 0.7 eV greater than the zero-point vibrational energy.

Theoretical study on the spectroscopic properties of CO3(*-).nH2O clusters: extrapolation to bulk.

PubMed

Pathak, Arup K; Mukherjee, Tulsi; Maity, Dilip K

2008-10-24

Vertical detachment energies (VDE) and UV/Vis absorption spectra of hydrated carbonate radical anion clusters, CO(3)(*-).nH(2)O (n=1-8), are determined by means of ab initio electronic structure theory. The VDE values of the hydrated clusters are calculated with second-order Moller-Plesset perturbation (MP2) and coupled cluster theory using the 6-311++G(d,p) set of basis functions. The bulk VDE value of an aqueous carbonate radical anion solution is predicted to be 10.6 eV from the calculated weighted average VDE values of the CO(3)(*-).nH(2)O clusters. UV/Vis absorption spectra of the hydrated clusters are calculated by means of time-dependent density functional theory using the Becke three-parameter nonlocal exchange and the Lee-Yang-Parr nonlocal correlation functional (B3LYP). The simulated UV/Vis spectrum of the CO(3)(*-).8H(2)O cluster is in excellent agreement with the reported experimental spectrum for CO(3)(*-) (aq), obtained based on pulse radiolysis experiments.

Fragment-based 13C nuclear magnetic resonance chemical shift predictions in molecular crystals: An alternative to planewave methods

NASA Astrophysics Data System (ADS)

Hartman, Joshua D.; Monaco, Stephen; Schatschneider, Bohdan; Beran, Gregory J. O.

2015-09-01

We assess the quality of fragment-based ab initio isotropic 13C chemical shift predictions for a collection of 25 molecular crystals with eight different density functionals. We explore the relative performance of cluster, two-body fragment, combined cluster/fragment, and the planewave gauge-including projector augmented wave (GIPAW) models relative to experiment. When electrostatic embedding is employed to capture many-body polarization effects, the simple and computationally inexpensive two-body fragment model predicts both isotropic 13C chemical shifts and the chemical shielding tensors as well as both cluster models and the GIPAW approach. Unlike the GIPAW approach, hybrid density functionals can be used readily in a fragment model, and all four hybrid functionals tested here (PBE0, B3LYP, B3PW91, and B97-2) predict chemical shifts in noticeably better agreement with experiment than the four generalized gradient approximation (GGA) functionals considered (PBE, OPBE, BLYP, and BP86). A set of recommended linear regression parameters for mapping between calculated chemical shieldings and observed chemical shifts are provided based on these benchmark calculations. Statistical cross-validation procedures are used to demonstrate the robustness of these fits.

Fragment-based (13)C nuclear magnetic resonance chemical shift predictions in molecular crystals: An alternative to planewave methods.

PubMed

Hartman, Joshua D; Monaco, Stephen; Schatschneider, Bohdan; Beran, Gregory J O

2015-09-14

We assess the quality of fragment-based ab initio isotropic (13)C chemical shift predictions for a collection of 25 molecular crystals with eight different density functionals. We explore the relative performance of cluster, two-body fragment, combined cluster/fragment, and the planewave gauge-including projector augmented wave (GIPAW) models relative to experiment. When electrostatic embedding is employed to capture many-body polarization effects, the simple and computationally inexpensive two-body fragment model predicts both isotropic (13)C chemical shifts and the chemical shielding tensors as well as both cluster models and the GIPAW approach. Unlike the GIPAW approach, hybrid density functionals can be used readily in a fragment model, and all four hybrid functionals tested here (PBE0, B3LYP, B3PW91, and B97-2) predict chemical shifts in noticeably better agreement with experiment than the four generalized gradient approximation (GGA) functionals considered (PBE, OPBE, BLYP, and BP86). A set of recommended linear regression parameters for mapping between calculated chemical shieldings and observed chemical shifts are provided based on these benchmark calculations. Statistical cross-validation procedures are used to demonstrate the robustness of these fits.

Combining density functional and incremental post-Hartree-Fock approaches for van der Waals dominated adsorbate-surface interactions: Ag{sub 2}/graphene

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lara-Castells, María Pilar de, E-mail: Pilar.deLara.Castells@csic.es; Mitrushchenkov, Alexander O.; Stoll, Hermann

2015-09-14

A combined density functional (DFT) and incremental post-Hartree-Fock (post-HF) approach, proven earlier to calculate He-surface potential energy surfaces [de Lara-Castells et al., J. Chem. Phys. 141, 151102 (2014)], is applied to describe the van der Waals dominated Ag{sub 2}/graphene interaction. It extends the dispersionless density functional theory developed by Pernal et al. [Phys. Rev. Lett. 103, 263201 (2009)] by including periodic boundary conditions while the dispersion is parametrized via the method of increments [H. Stoll, J. Chem. Phys. 97, 8449 (1992)]. Starting with the elementary cluster unit of the target surface (benzene), continuing through the realistic cluster model (coronene), andmore » ending with the periodic model of the extended system, modern ab initio methodologies for intermolecular interactions as well as state-of-the-art van der Waals-corrected density functional-based approaches are put together both to assess the accuracy of the composite scheme and to better characterize the Ag{sub 2}/graphene interaction. The present work illustrates how the combination of DFT and post-HF perspectives may be efficient to design simple and reliable ab initio-based schemes in extended systems for surface science applications.« less

Structural, electronic, vibrational and optical properties of Bin clusters

NASA Astrophysics Data System (ADS)

Liang, Dan; Shen, Wanting; Zhang, Chunfang; Lu, Pengfei; Wang, Shumin

2017-10-01

The neutral, anionic and cationic bismuth clusters with the size n up to 14 are investigated by using B3LYP functional within the regime of density functional theory and the LAN2DZ basis set. By analysis of the geometries of the Bin (n = 2-14) clusters, where cationic and anionic bismuth clusters are largely similar to those of neutral ones, a periodic effect by adding units with one to four atoms into smaller cluster to form larger cluster is drawn for the stable structures of bismuth clusters. An even-odd alteration is shown for the properties of the clusters, such as the calculated binding energies and dissociation energies, as well as frontier orbital energies, electron affinities, ionization energies. All the properties indicate that the Bi4 cluster is the most possible existence in bismuth-containing materials, which supports the most recent experiment. The orbital compositions, infrared and Raman activities and the ultraviolet absorption of the most possible tetramer bismuth cluster are given in detail to reveal the periodic tendency of adding bismuth atoms and the stability of tetramer bismuth cluster.

High reactivity of nanosized niobium oxide cluster cations in methane activation: A comparison with vanadium oxides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ding, Xun-Lei, E-mail: dingxl@ncepu.edu.cn, E-mail: chemzyx@iccas.ac.cn; Wang, Dan; Wu, Xiao-Nan

2015-09-28

The reactions between methane and niobium oxide cluster cations were studied and compared to those employing vanadium oxides. Hydrogen atom abstraction (HAA) reactions were identified over stoichiometric (Nb{sub 2}O{sub 5}){sub N}{sup +} clusters for N as large as 14 with a time-of-flight mass spectrometer. The reactivity of (Nb{sub 2}O{sub 5}){sub N}{sup +} clusters decreases as the N increases, and it is higher than that of (V {sub 2}O{sub 5}){sub N}{sup +} for N ≥ 4. Theoretical studies were conducted on (Nb{sub 2}O{sub 5}){sub N}{sup +} (N = 2–6) by density functional calculations. HAA reactions on these clusters are all favorablemore » thermodynamically and kinetically. The difference of the reactivity with respect to the cluster size and metal type (Nb vs V) was attributed to thermodynamics, kinetics, the electron capture ability, and the distribution of the unpaired spin density. Nanosized Nb oxide clusters show higher HAA reactivity than V oxides, indicating that niobia may serve as promising catalysts for practical methane conversion.« less

Studies of the evolution of the x ray emission of clusters of galaxies

NASA Technical Reports Server (NTRS)

Henry, J. Patrick

1990-01-01

The x ray luminosity function of clusters of galaxies was determined at different cosmic epoches using data from the Einstein Observatory Extended Medium Survey. The sample consisted of 67 x ray selected clusters that were grouped into three redshift shells. Evolution was detected in the x ray properties of clusters. The present volume density of high luminosity clusters was found to be greater than it was in the past. This result is the first convincing evidence for evolution in the x ray properties of clusters. Investigations into the constraints provided by these data on various Cold Dark Matter models are underway.

New Constraints on Dark Energy from the ObservedGrowth of the Most X-ray Luminous Galaxy Clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mantz, A.; Allen, S.W.; Ebeling, H.

We present constraints on the mean matter density, {Omega}{sub m}, normalization of the density fluctuation power spectrum, {sigma}{sub 8}, and dark energy equation of state parameter, w, obtained from the X-ray luminosity function of the Massive Cluster Survey (MACS) in combination with the local BCS and REFLEX galaxy cluster samples. Our analysis incorporates the mass function predictions of Jenkins et al. (2001), a mass-luminosity relation calibrated using the data of Reiprich and Bohringer (2002), and standard priors on the Hubble constant, H{sub 0}, and mean baryon density, {Omega}{sub b} h{sup 2}. We find {Omega}{sub m}=0.27 {sup +0.06} {sub -0.05} andmore » {sigma}{sub 8}=0.77 {sup +0.07} {sub -0.06} for a spatially flat, cosmological constant model, and {Omega}{sub m}=0.28 {sup +0.08} {sub -0.06}, {sigma}{sub 8}=0.75 {+-} 0.08 and w=-0.97 {sup +0.20} {sub -0.19} for a flat, constant-w model. Our findings constitute the first precise determination of the dark energy equation of state from measurements of the growth of cosmic structure in galaxy clusters. The consistency of our result with w=-1 lends strong additional support to the cosmological constant model. The constraints are insensitive to uncertainties at the 10-20 percent level in the mass function and in the redshift evolution o the mass-luminosity relation; the constraint on dark energy is additionally robust against our choice of priors and known X-ray observational biases affecting the mass-luminosity relation. Our results compare favorably with those from recent analyses of type Ia supernovae, cosmic microwave background anisotropies, the X-ray gas mass fraction of relaxed galaxy clusters and cosmic shear. A simplified combination of the luminosity function data with supernova, cosmic microwave background and cluster gas fraction data using importance sampling yields the improved constraints {Omega}{sub m}=0.263 {+-} 0.014, {sigma}{sub 8}=0.79 {+-} 0.02 and w=-1.00 +- 0.05.« less

Adsorption and Desorption of Hydrogen by Gas-Phase Palladium Clusters Revealed by In Situ Thermal Desorption Spectroscopy.

PubMed

Takenouchi, Masato; Kudoh, Satoshi; Miyajima, Ken; Mafuné, Fumitaka

2015-07-02

Adsorption and desorption of hydrogen by gas-phase Pd clusters, Pdn(+), were investigated by thermal desorption spectroscopy (TDS) experiments and density functional theory (DFT) calculations. The desorption processes were examined by heating the clusters that had adsorbed hydrogen at room temperature. The clusters remaining after heating were monitored by mass spectrometry as a function of temperature up to 1000 K, and the temperature-programmed desorption (TPD) curve was obtained for each Pdn(+). It was found that hydrogen molecules were released from the clusters into the gas phase with increasing temperature until bare Pdn(+) was formed. The threshold energy for desorption, estimated from the TPD curve, was compared to the desorption energy calculated by using DFT, indicating that smaller Pdn(+) clusters (n ≤ 6) tended to have weakly adsorbed hydrogen molecules, whereas larger Pdn(+) clusters (n ≥ 7) had dissociatively adsorbed hydrogen atoms on the surface. Highly likely, the nonmetallic nature of the small Pd clusters prevents hydrogen molecule from adsorbing dissociatively on the surface.

Direct construction of mesoscopic models from microscopic simulations

NASA Astrophysics Data System (ADS)

Lei, Huan; Caswell, Bruce; Karniadakis, George Em

2010-02-01

Starting from microscopic molecular-dynamics (MD) simulations of constrained Lennard-Jones (LJ) clusters (with constant radius of gyration Rg ), we construct two mesoscopic models [Langevin dynamics and dissipative particle dynamics (DPD)] by coarse graining the LJ clusters into single particles. Both static and dynamic properties of the coarse-grained models are investigated and compared with the MD results. The effective mean force field is computed as a function of the intercluster distance, and the corresponding potential scales linearly with the number of particles per cluster and the temperature. We verify that the mean force field can reproduce the equation of state of the atomistic systems within a wide density range but the radial distribution function only within the dilute and the semidilute regime. The friction force coefficients for both models are computed directly from the time-correlation function of the random force field of the microscopic system. For high density or a large cluster size the friction force is overestimated and the diffusivity underestimated due to the omission of many-body effects as a result of the assumed pairwise form of the coarse-grained force field. When the many-body effect is not as pronounced (e.g., smaller Rg or semidilute system), the DPD model can reproduce the dynamic properties of the MD system.

Hydration of copper(II): new insights from density functional theory and the COSMO solvation model.

PubMed

Bryantsev, Vyacheslav S; Diallo, Mamadou S; van Duin, Adri C T; Goddard, William A

2008-09-25

The hydrated structure of the Cu(II) ion has been a subject of ongoing debate in the literature. In this article, we use density functional theory (B3LYP) and the COSMO continuum solvent model to characterize the structure and stability of [Cu(H2O)n](2+) clusters as a function of coordination number (4, 5, and 6) and cluster size (n = 4-18). We find that the most thermodynamically favored Cu(II) complexes in the gas phase have a very open four-coordinate structure. They are formed from a stable square-planar [Cu(H2O)8](2+) core stabilized by an unpaired electron in the Cu(II) ion d(x(2)-y(2)) orbital. This is consistent with cluster geometries suggested by recent mass-spectrometric experiments. In the aqueous phase, we find that the more compact five-coordinate square-pyramidal geometry is more stable than either the four-coordinate or six-coordinate clusters in agreement with recent combined EXAFS and XANES studies of aqueous solutions of Cu(II). However, a small energetic difference (approximately 1.4 kcal/mol) between the five- and six-coordinate models with two full hydration shells around the metal ion suggests that both forms may coexist in solution.

DEMARCATE: Density-based magnetic resonance image clustering for assessing tumor heterogeneity in cancer.

PubMed

Saha, Abhijoy; Banerjee, Sayantan; Kurtek, Sebastian; Narang, Shivali; Lee, Joonsang; Rao, Ganesh; Martinez, Juan; Bharath, Karthik; Rao, Arvind U K; Baladandayuthapani, Veerabhadran

2016-01-01

Tumor heterogeneity is a crucial area of cancer research wherein inter- and intra-tumor differences are investigated to assess and monitor disease development and progression, especially in cancer. The proliferation of imaging and linked genomic data has enabled us to evaluate tumor heterogeneity on multiple levels. In this work, we examine magnetic resonance imaging (MRI) in patients with brain cancer to assess image-based tumor heterogeneity. Standard approaches to this problem use scalar summary measures (e.g., intensity-based histogram statistics) that do not adequately capture the complete and finer scale information in the voxel-level data. In this paper, we introduce a novel technique, DEMARCATE (DEnsity-based MAgnetic Resonance image Clustering for Assessing Tumor hEterogeneity) to explore the entire tumor heterogeneity density profiles (THDPs) obtained from the full tumor voxel space. THDPs are smoothed representations of the probability density function of the tumor images. We develop tools for analyzing such objects under the Fisher-Rao Riemannian framework that allows us to construct metrics for THDP comparisons across patients, which can be used in conjunction with standard clustering approaches. Our analyses of The Cancer Genome Atlas (TCGA) based Glioblastoma dataset reveal two significant clusters of patients with marked differences in tumor morphology, genomic characteristics and prognostic clinical outcomes. In addition, we see enrichment of image-based clusters with known molecular subtypes of glioblastoma multiforme, which further validates our representation of tumor heterogeneity and subsequent clustering techniques.

The correlation function for density perturbations in an expanding universe. III The three-point and predictions of the four-point and higher order correlation functions

NASA Technical Reports Server (NTRS)

Mcclelland, J.; Silk, J.

1978-01-01

Higher-order correlation functions for the large-scale distribution of galaxies in space are investigated. It is demonstrated that the three-point correlation function observed by Peebles and Groth (1975) is not consistent with a distribution of perturbations that at present are randomly distributed in space. The two-point correlation function is shown to be independent of how the perturbations are distributed spatially, and a model of clustered perturbations is developed which incorporates a nonuniform perturbation distribution and which explains the three-point correlation function. A model with hierarchical perturbations incorporating the same nonuniform distribution is also constructed; it is found that this model also explains the three-point correlation function, but predicts different results for the four-point and higher-order correlation functions than does the model with clustered perturbations. It is suggested that the model of hierarchical perturbations might be explained by the single assumption of having density fluctuations or discrete objects all of the same mass randomly placed at some initial epoch.

Comparative study of cluster Ag17Cu2 by instantaneous normal mode analysis and by isothermal Brownian-type molecular dynamics simulation.

PubMed

Tang, Ping-Han; Wu, Ten-Ming; Yen, Tsung-Wen; Lai, S K; Hsu, P J

2011-09-07

We perform isothermal Brownian-type molecular dynamics simulations to obtain the velocity autocorrelation function and its time Fourier-transformed power spectral density for the metallic cluster Ag(17)Cu(2). The temperature dependences of these dynamical quantities from T = 0 to 1500 K were examined and across this temperature range the cluster melting temperature T(m), which we define to be the principal maximum position of the specific heat is determined. The instantaneous normal mode analysis is then used to dissect the cluster dynamics by calculating the vibrational instantaneous normal mode density of states and hence its frequency integrated value I(j) which is an ensemble average of all vibrational projection operators for the jth atom in the cluster. In addition to comparing the results with simulation data, we look more closely at the entities I(j) of all atoms using the point group symmetry and diagnose their temperature variations. We find that I(j) exhibit features that may be used to deduce T(m), which turns out to agree very well with those inferred from the power spectral density and specific heat. © 2011 American Institute of Physics

Percolation of the site random-cluster model by Monte Carlo method

NASA Astrophysics Data System (ADS)

Wang, Songsong; Zhang, Wanzhou; Ding, Chengxiang

2015-08-01

We propose a site random-cluster model by introducing an additional cluster weight in the partition function of the traditional site percolation. To simulate the model on a square lattice, we combine the color-assignation and the Swendsen-Wang methods to design a highly efficient cluster algorithm with a small critical slowing-down phenomenon. To verify whether or not it is consistent with the bond random-cluster model, we measure several quantities, such as the wrapping probability Re, the percolating cluster density P∞, and the magnetic susceptibility per site χp, as well as two exponents, such as the thermal exponent yt and the fractal dimension yh of the percolating cluster. We find that for different exponents of cluster weight q =1.5 , 2, 2.5 , 3, 3.5 , and 4, the numerical estimation of the exponents yt and yh are consistent with the theoretical values. The universalities of the site random-cluster model and the bond random-cluster model are completely identical. For larger values of q , we find obvious signatures of the first-order percolation transition by the histograms and the hysteresis loops of percolating cluster density and the energy per site. Our results are helpful for the understanding of the percolation of traditional statistical models.

Spatio-Temporal Characteristics of Resident Trip Based on Poi and OD Data of Float CAR in Beijing

NASA Astrophysics Data System (ADS)

Mou, N.; Li, J.; Zhang, L.; Liu, W.; Xu, Y.

2017-09-01

Due to the influence of the urban inherent regional functional distribution, the daily activities of the residents presented some spatio-temporal patterns (periodic patterns, gathering patterns, etc.). In order to further understand the spatial and temporal characteristics of urban residents, this paper research takes the taxi trajectory data of Beijing as a sample data and studies the spatio-temporal characteristics of the residents' activities on the weekdays. At first, according to the characteristics of the taxi trajectory data distributed along the road network, it takes the Voronoi generated by the road nodes as the research unit. This paper proposes a hybrid clustering method - based on grid density, which is used to cluster the OD (origin and destination) data of taxi at different times. Then combining with the POI data of Beijing, this research calculated the density of the POI data in the clustering results, and analyzed the relationship between the activities of residents in different periods and the functional types of the region. The final results showed that the residents were mainly commuting on weekdays. And it found that the distribution of travel density showed a concentric circle of the characteristics, focusing on residential areas and work areas. The results of cluster analysis and POI analysis showed that the residents' travel had experienced the process of "spatial relative dispersion - spatial aggregation - spatial relative dispersion" in one day.

A 3D particle Monte Carlo approach to studying nucleation

NASA Astrophysics Data System (ADS)

Köhn, Christoph; Enghoff, Martin Bødker; Svensmark, Henrik

2018-06-01

The nucleation of sulphuric acid molecules plays a key role in the formation of aerosols. We here present a three dimensional particle Monte Carlo model to study the growth of sulphuric acid clusters as well as its dependence on the ambient temperature and the initial particle density. We initiate a swarm of sulphuric acid-water clusters with a size of 0.329 nm with densities between 107 and 108 cm-3 at temperatures between 200 and 300 K and a relative humidity of 50%. After every time step, we update the position of particles as a function of size-dependent diffusion coefficients. If two particles encounter, we merge them and add their volumes and masses. Inversely, we check after every time step whether a polymer evaporates liberating a molecule. We present the spatial distribution as well as the size distribution calculated from individual clusters. We also calculate the nucleation rate of clusters with a radius of 0.85 nm as a function of time, initial particle density and temperature. The nucleation rates obtained from the presented model agree well with experimentally obtained values and those of a numerical model which serves as a benchmark of our code. In contrast to previous nucleation models, we here present for the first time a code capable of tracing individual particles and thus of capturing the physics related to the discrete nature of particles.

Noble gas cluster ions

NASA Astrophysics Data System (ADS)

Kaya, Yunus; Kalkan, Yalçin; Veenhof, Rob

2018-02-01

In this work, a reaction mechanism of formation of noble gas (Ng) cluster ions has been theoretically investigated in detail. The kinetic studies of formation of Xe+Xe cluster in Xe, Ar+Ar cluster ions in Ar, and Ne+Ne cluster ions in Ne have been made as theoretically. The optimized structures in the ground state were calculated using the density functional theory (DFT) by the B3LYP method combined with the Stuttgart/Dresden effective core potential basis set (SDD). In addition, we calculated the rate constants of all cluster formations. The results are 1.15 × 10-31, 3.58 × 10-31, 0.23 × 10-31cm6/s, respectively for Neon, Argon, Xenon cluster ions.

Structural and magnetic evolution of bimetallic MnAu clusters driven by asymmetric atomic migration.

PubMed

Wei, Xiaohui; Zhou, Rulong; Lefebvre, Williams; He, Kai; Le Roy, Damien; Skomski, Ralph; Li, Xingzhong; Shield, Jeffrey E; Kramer, Matthew J; Chen, Shuang; Zeng, Xiao Cheng; Sellmyer, David J

2014-03-12

The nanoscale structural, compositional, and magnetic properties are examined for annealed MnAu nanoclusters. The MnAu clusters order into the L1(0) structure, and monotonic size-dependences develop for the composition and lattice parameters, which are well reproduced by our density functional theory calculations. Simultaneously, Mn diffusion forms 5 Å nanoshells on larger clusters inducing significant magnetization in an otherwise antiferromagnetic system. The differing atomic mobilities yield new cluster nanostructures that can be employed generally to create novel physical properties.

Ultra-small rhenium clusters supported on graphene.

PubMed

Miramontes, Orlando; Bonafé, Franco; Santiago, Ulises; Larios-Rodriguez, Eduardo; Velázquez-Salazar, Jesús J; Mariscal, Marcelo M; Yacaman, Miguel José

2015-03-28

The adsorption of very small rhenium clusters (2-13 atoms) supported on graphene was studied by high-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM). The atomic structure of the clusters was fully resolved with the aid of density functional theory calculations and STEM simulations. It was found that octahedral and tetrahedral structures work as seeds to obtain more complex morphologies. Finally, a detailed analysis of the electronic structure suggested that a higher catalytic effect can be expected in Re clusters when adsorbed on graphene than in isolated ones.

Ultra-small rhenium clusters supported on graphene

PubMed Central

Miramontes, Orlando; Bonafé, Franco; Santiago, Ulises; Larios-Rodriguez, Eduardo; Velázquez-Salazar, Jesús J.; Mariscal, Marcelo M.; Yacaman, Miguel José

2015-01-01

The adsorption of very small rhenium clusters (2 – 13 atoms) supported on graphene was studied with high annular dark field - scanning transmission electron microscopy (HAADF-STEM). The atomic structure of the clusters was fully resolved with the aid of density functional calculations and STEM simulations. It was found that octahedral and tetrahedral structures work as seeds to obtain more complex morphologies. Finally, a detailed analysis of the electronic structure suggested that a higher catalytic effect can be expected in Re clusters when adsorbed on graphene than in isolated ones. PMID:25721176

Density Functional Approach to Superfluid Phonon in Inner Crust of Neutron Stars

NASA Astrophysics Data System (ADS)

Inakura, Tsunenori; Matsuo, Masayuki

We investigate superfluid phonon emerging in inner crust of neutron stars by means of the nuclear density functional theory. Adopting the Wigner-Seitz approximation and a single spherical cell, we describe low-lying collective excitation with the dipole multipolarity. It is found that the superfluid phonon standing on the low-density neutron superfluid does not penetrate into the interior of the nuclear cluster. This suggests that the coupling between the superfluid phonon and the lattice phonon could be weak, and it may affect the thermal conductivity of inner crust.

On the linearity of tracer bias around voids

NASA Astrophysics Data System (ADS)

Pollina, Giorgia; Hamaus, Nico; Dolag, Klaus; Weller, Jochen; Baldi, Marco; Moscardini, Lauro

2017-07-01

The large-scale structure of the Universe can be observed only via luminous tracers of the dark matter. However, the clustering statistics of tracers are biased and depend on various properties, such as their host-halo mass and assembly history. On very large scales, this tracer bias results in a constant offset in the clustering amplitude, known as linear bias. Towards smaller non-linear scales, this is no longer the case and tracer bias becomes a complicated function of scale and time. We focus on tracer bias centred on cosmic voids, I.e. depressions of the density field that spatially dominate the Universe. We consider three types of tracers: galaxies, galaxy clusters and active galactic nuclei, extracted from the hydrodynamical simulation Magneticum Pathfinder. In contrast to common clustering statistics that focus on auto-correlations of tracers, we find that void-tracer cross-correlations are successfully described by a linear bias relation. The tracer-density profile of voids can thus be related to their matter-density profile by a single number. We show that it coincides with the linear tracer bias extracted from the large-scale auto-correlation function and expectations from theory, if sufficiently large voids are considered. For smaller voids we observe a shift towards higher values. This has important consequences on cosmological parameter inference, as the problem of unknown tracer bias is alleviated up to a constant number. The smallest scales in existing data sets become accessible to simpler models, providing numerous modes of the density field that have been disregarded so far, but may help to further reduce statistical errors in constraining cosmology.

Cluster-cluster clustering

NASA Technical Reports Server (NTRS)

Barnes, J.; Dekel, A.; Efstathiou, G.; Frenk, C. S.

1985-01-01

The cluster correlation function xi sub c(r) is compared with the particle correlation function, xi(r) in cosmological N-body simulations with a wide range of initial conditions. The experiments include scale-free initial conditions, pancake models with a coherence length in the initial density field, and hybrid models. Three N-body techniques and two cluster-finding algorithms are used. In scale-free models with white noise initial conditions, xi sub c and xi are essentially identical. In scale-free models with more power on large scales, it is found that the amplitude of xi sub c increases with cluster richness; in this case the clusters give a biased estimate of the particle correlations. In the pancake and hybrid models (with n = 0 or 1), xi sub c is steeper than xi, but the cluster correlation length exceeds that of the points by less than a factor of 2, independent of cluster richness. Thus the high amplitude of xi sub c found in studies of rich clusters of galaxies is inconsistent with white noise and pancake models and may indicate a primordial fluctuation spectrum with substantial power on large scales.

Field-theoretical approach to a dense polymer with an ideal binary mixture of clustering centers.

PubMed

Fantoni, Riccardo; Müller-Nedebock, Kristian K

2011-07-01

We propose a field-theoretical approach to a polymer system immersed in an ideal mixture of clustering centers. The system contains several species of these clustering centers with different functionality, each of which connects a fixed number segments of the chain to each other. The field theory is solved using the saddle point approximation and evaluated for dense polymer melts using the random phase approximation. We find a short-ranged effective intersegment interaction with strength dependent on the average segment density and discuss the structure factor within this approximation. We also determine the fractions of linkers of the different functionalities.

Redshift-space distortions with the halo occupation distribution - II. Analytic model

NASA Astrophysics Data System (ADS)

Tinker, Jeremy L.

2007-01-01

We present an analytic model for the galaxy two-point correlation function in redshift space. The cosmological parameters of the model are the matter density Ωm, power spectrum normalization σ8, and velocity bias of galaxies αv, circumventing the linear theory distortion parameter β and eliminating nuisance parameters for non-linearities. The model is constructed within the framework of the halo occupation distribution (HOD), which quantifies galaxy bias on linear and non-linear scales. We model one-halo pairwise velocities by assuming that satellite galaxy velocities follow a Gaussian distribution with dispersion proportional to the virial dispersion of the host halo. Two-halo velocity statistics are a combination of virial motions and host halo motions. The velocity distribution function (DF) of halo pairs is a complex function with skewness and kurtosis that vary substantially with scale. Using a series of collisionless N-body simulations, we demonstrate that the shape of the velocity DF is determined primarily by the distribution of local densities around a halo pair, and at fixed density the velocity DF is close to Gaussian and nearly independent of halo mass. We calibrate a model for the conditional probability function of densities around halo pairs on these simulations. With this model, the full shape of the halo velocity DF can be accurately calculated as a function of halo mass, radial separation, angle and cosmology. The HOD approach to redshift-space distortions utilizes clustering data from linear to non-linear scales to break the standard degeneracies inherent in previous models of redshift-space clustering. The parameters of the occupation function are well constrained by real-space clustering alone, separating constraints on bias and cosmology. We demonstrate the ability of the model to separately constrain Ωm,σ8 and αv in models that are constructed to have the same value of β at large scales as well as the same finger-of-god distortions at small scales.

Smallest fullerene-like silicon cage stabilized by a V{sub 2} unit

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Hong-Guang, E-mail: xuhong@iccas.ac.cn, E-mail: zhengwj@iccas.ac.cn; Kong, Xiang-Yu; Deng, Xiao-Jiao

We conducted a combined anion photoelectron spectroscopy and density functional theory study on V{sub 2}Si{sub 20} cluster. Our results show that the V{sub 2}Si{sub 20} cluster has an elongated dodecahedron cage structure with a V{sub 2} unit encapsulated inside the cage. It is the smallest fullerene-like silicon cage and can be used as building block to make cluster-assembled materials, such as pearl-chain style nanowires.

Computational study on the molecular structures and photoelectron spectra of bimetallic oxide clusters MW2O9(-/0) (M=V, Nb, Ta).

PubMed

Chen, Wen-Jie; Zhang, Chang-Fu; Zhang, Xian-Hui; Zhang, Yong-Fan; Huang, Xin

2013-05-15

Density functional theory (DFT) and coupled cluster theory (CCSD(T)) calculations are carried out to investigate the electronic and structural properties of a series of bimetallic oxide clusters MW2O9(-/0) (M=V, Nb, Ta). Generalized Koopmans' theorem is applied to predict the vertical detachment energies (VDEs) and simulate the photoelectron spectra (PES). Theoretical calculations at the B3LYP level yield singlet and doublet ground states for the bimetallic anionic and neutral clusters, respectively. All the clusters present the six-membered ring structures with different symmetries, except that the TaW2O9(-) cluster shows a chained style with a penta-coordinated tantalum atom. Spin density analyses reveal oxygen radical species in all neutral clusters, consistent with their structural characteristics. Moreover, additional calculations are performed to study the oxidation reaction of CO molecule with the W3O9(+) cation and the isoelectronic VW2O9 cluster, and results indicate that the introduction of vanadium at tungsten site can efficiently improve the oxidation reactivity. Copyright © 2013 Elsevier B.V. All rights reserved.

Effect of palladium doping on the stability and fragmentation patterns of cationic gold clusters

NASA Astrophysics Data System (ADS)

Ferrari, P.; Hussein, H. A.; Heard, C. J.; Vanbuel, J.; Johnston, R. L.; Lievens, P.; Janssens, E.

2018-05-01

We analyze in detail how the interplay between electronic structure and cluster geometry determines the stability and the fragmentation channels of single Pd-doped cationic Au clusters, PdA uN-1+ (N =2 -20 ). For this purpose, a combination of photofragmentation experiments and density functional theory calculations was employed. A remarkable agreement between the experiment and the calculations is obtained. Pd doping is found to modify the structure of the Au clusters, in particular altering the two-dimensional to three-dimensional transition size, with direct consequences on the stability of the clusters. Analysis of the electronic density of states of the clusters shows that depending on cluster size, Pd delocalizes one 4 d electron, giving an enhanced stability to PdA u6 + , or remains with all 4 d10 electrons localized, closing an electronic shell in PdA u9 + . Furthermore, it is observed that for most clusters, Au evaporation is the lowest-energy decay channel, although for some sizes Pd evaporation competes. In particular, PdA u7 + and PdA u9 + decay by Pd evaporation due to the high stability of the A u7 + and A u9 + fragmentation products.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Goudfrooij, Paul, E-mail: goudfroo@stsci.edu

We study mass functions of globular clusters derived from Hubble Space Telescope/Advanced Camera for Surveys images of the early-type merger remnant galaxy NGC 1316, which hosts a significant population of metal-rich globular clusters of intermediate age ({approx}3 Gyr). For the old, metal-poor ({sup b}lue{sup )} clusters, the peak mass of the mass function M{sub p} increases with internal half-mass density {rho}{sub h} as M{sub p}{proportional_to}{rho}{sub h}{sup 0.44}, whereas it stays approximately constant with galactocentric distance R{sub gal}. The mass functions of these clusters are consistent with a simple scenario in which they formed with a Schechter initial mass function andmore » evolved subsequently by internal two-body relaxation. For the intermediate-age population of metal-rich ({sup r}ed{sup )} clusters, the faint end of the previously reported power-law luminosity function of the clusters with R{sub gal} > 9 kpc is due to many of those clusters having radii larger than the theoretical maximum value imposed by the tidal field of NGC 1316 at their R{sub gal}. This renders disruption by two-body relaxation ineffective. Only a few such diffuse clusters are found in the inner regions of NGC 1316. Completeness tests indicate that this is a physical effect. Using comparisons with star clusters in other galaxies and cluster disruption calculations using published models, we hypothesize that most red clusters in the low-{rho}{sub h} tail of the initial distribution have already been destroyed in the inner regions of NGC 1316 by tidal shocking, and that several remaining low-{rho}{sub h} clusters will evolve dynamically to become similar to 'faint fuzzies' that exist in several lenticular galaxies. Finally, we discuss the nature of diffuse red clusters in early-type galaxies.« less

Study of MoNbO(y) (y = 2-5) anion and neutral clusters using photoelectron spectroscopy and density functional theory calculations: impact of spin contamination on single point calculations.

PubMed

Waller, Sarah E; Mann, Jennifer E; Rothgeb, David W; Jarrold, Caroline C

2012-10-04

Results of a study combining anion photoelectron spectroscopy and density functional theory calculations on the heteronuclear MoNbO(y)(-) (y = 2-5) transition metal suboxide cluster series are reported and analyzed. The photoelectron spectra, which exhibit broad electronic bands with partially resolved vibrational structure, were compared to spectral simulations generated from calculated spectroscopic parameters for all computationally determined energetically competitive structures. Although computational results on the less oxidized clusters could not be satisfactorily reconciled with experimental spectra, possibly because of heavy spin contamination found in a large portion of the computational results, the results suggest that (1) neutral cluster electron affinity is a strong indicator of whether O-atoms are bound in M-O-M bridge positions or M═O terminal positions, (2) MoNbO(y) anions and neutrals have structures that can be described as intermediate with respect to the unary (homonuclear) Mo(2)O(y) and Nb(2)O(y) clusters, and (3) structures in which O-atoms preferentially bind to the Nb center are slightly more stable than alternative structures. Several challenges associated with the calculations are considered, including spin contamination, which appears to cause spurious single point calculations used to determine vertical detachment energies.

Structures and Spectroscopic Properties of F-(H2O) n with n = 1-10 Clusters from a Global Search Based On Density Functional Theory.

PubMed

Shi, Ruili; Wang, Pengju; Tang, Lingli; Huang, Xiaoming; Chen, Yonggang; Su, Yan; Zhao, Jijun

2018-04-05

Using a genetic algorithm incorporated in density functional theory, we explore the ground state structures of fluoride anion-water clusters F - (H 2 O) n with n = 1-10. The F - (H 2 O) n clusters prefer structures in which the F - anion remains at the surface of the structure and coordinates with four water molecules, as the F - (H 2 O) n clusters have strong F - -H 2 O interactions as well as strong hydrogen bonds between H 2 O molecules. The strong interaction between the F - anion and adjacent H 2 O molecule leads to a longer O-H distance in the adjacent molecule than in an individual water molecule. The simulated infrared (IR) spectra of the F - (H 2 O) 1-5 clusters obtained via second-order vibrational perturbation theory (VPT2) and including anharmonic effects reproduce the experimental results quite well. The strong interaction between the F - anion and water molecules results in a large redshift (600-2300 cm -1 ) of the adjacent O-H stretching mode. Natural bond orbital (NBO) analysis of the lowest-energy structures of the F - (H 2 O) 1-10 clusters illustrates that charge transfer from the lone pair electron orbital of F - to the antibonding orbital of the adjacent O-H is mainly responsible for the strong interaction between the F - anion and water molecules, which leads to distinctly different geometric and vibrational properties compared with neutral water clusters.

Tuning optical properties of magic number cluster (SiO2)4O2H4 by substitutional bonding with gold atoms.

PubMed

Cai, Xiulong; Zhang, Peng; Ma, Liuxue; Zhang, Wenxian; Ning, Xijing; Zhao, Li; Zhuang, Jun

2009-04-30

By bonding gold atoms to the magic number cluster (SiO(2))(4)O(2)H(4), two groups of Au-adsorbed shell-like clusters Au(n)(SiO(2))(4)O(2)H(4-n) (n = 1-4) and Au(n)(SiO(2))(4)O(2) (n = 5-8) were obtained, and their spectral properties were studied. The ground-state structures of these clusters were optimized by density functional theory, and the results show that in despite of the different numbers and types of the adsorbed Au atoms, the cluster core (SiO(2))(4)O(2) of T(d) point-group symmetry keeps almost unchanged. The absorption spectra were obtained by time-dependent density functional theory. From one group to the other, an extension of absorption wavelength from the UV-visible to the NIR region was observed, and in each group the absorption strengths vary linearly with the number of Au atoms. These features indicate their advantages for exploring novel materials with easily controlled tunable optical properties. Furthermore, due to the weak electronic charge transfer between the Au atoms, the clusters containing Au(2) dimers, especially Au(8)(SiO(2))(4)O(2), absorb strongly NIR light at 900 approximately 1200 nm. Such strong absorption suggests potential applications of these shell-like clusters in tumor cells thermal therapy, like the gold-coated silica nanoshells with larger sizes.

Combined Mössbauer spectroscopic, multi-edge X-ray absorption spectroscopic, and density functional theoretical study of the radical SAM enzyme spore photoproduct lyase.

PubMed

Silver, Sunshine C; Gardenghi, David J; Naik, Sunil G; Shepard, Eric M; Huynh, Boi Hanh; Szilagyi, Robert K; Broderick, Joan B

2014-03-01

Spore photoproduct lyase (SPL), a member of the radical S-adenosyl-L-methionine (SAM) superfamily, catalyzes the direct reversal of the spore photoproduct, a thymine dimer specific to bacterial spores, to two thymines. SPL requires SAM and a redox-active [4Fe-4S] cluster for catalysis. Mössbauer analysis of anaerobically purified SPL indicates the presence of a mixture of cluster states with the majority (40 %) as [2Fe-2S](2+) clusters and a smaller amount (15 %) as [4Fe-4S](2+) clusters. On reduction, the cluster content changes to primarily (60 %) [4Fe-4S](+). The speciation information from Mössbauer data allowed us to deconvolute iron and sulfur K-edge X-ray absorption spectra to uncover electronic (X-ray absorption near-edge structure, XANES) and geometric (extended X-ray absorption fine structure, EXAFS) structural features of the Fe-S clusters, and their interactions with SAM. The iron K-edge EXAFS data provide evidence for elongation of a [2Fe-2S] rhomb of the [4Fe-4S] cluster on binding SAM on the basis of an Fe···Fe scatterer at 3.0 Å. The XANES spectra of reduced SPL in the absence and presence of SAM overlay one another, indicating that SAM is not undergoing reductive cleavage. The X-ray absorption spectroscopy data for SPL samples and data for model complexes from the literature allowed the deconvolution of contributions from [2Fe-2S] and [4Fe-4S] clusters to the sulfur K-edge XANES spectra. The analysis of pre-edge features revealed electronic changes in the Fe-S clusters as a function of the presence of SAM. The spectroscopic findings were further corroborated by density functional theory calculations that provided insights into structural and electronic perturbations that can be correlated by considering the role of SAM as a catalyst or substrate.

Impact of Sampling Density on the Extent of HIV Clustering

PubMed Central

Novitsky, Vlad; Moyo, Sikhulile; Lei, Quanhong; DeGruttola, Victor

2014-01-01

Abstract Identifying and monitoring HIV clusters could be useful in tracking the leading edge of HIV transmission in epidemics. Currently, greater specificity in the definition of HIV clusters is needed to reduce confusion in the interpretation of HIV clustering results. We address sampling density as one of the key aspects of HIV cluster analysis. The proportion of viral sequences in clusters was estimated at sampling densities from 1.0% to 70%. A set of 1,248 HIV-1C env gp120 V1C5 sequences from a single community in Botswana was utilized in simulation studies. Matching numbers of HIV-1C V1C5 sequences from the LANL HIV Database were used as comparators. HIV clusters were identified by phylogenetic inference under bootstrapped maximum likelihood and pairwise distance cut-offs. Sampling density below 10% was associated with stochastic HIV clustering with broad confidence intervals. HIV clustering increased linearly at sampling density >10%, and was accompanied by narrowing confidence intervals. Patterns of HIV clustering were similar at bootstrap thresholds 0.7 to 1.0, but the extent of HIV clustering decreased with higher bootstrap thresholds. The origin of sampling (local concentrated vs. scattered global) had a substantial impact on HIV clustering at sampling densities ≥10%. Pairwise distances at 10% were estimated as a threshold for cluster analysis of HIV-1 V1C5 sequences. The node bootstrap support distribution provided additional evidence for 10% sampling density as the threshold for HIV cluster analysis. The detectability of HIV clusters is substantially affected by sampling density. A minimal genotyping density of 10% and sampling density of 50–70% are suggested for HIV-1 V1C5 cluster analysis. PMID:25275430

Hyperfine coupling constants of the nitrogen and phosphorus atoms: A challenge for exact-exchange density-functional and post-Hartree-Fock methods

NASA Astrophysics Data System (ADS)

Kaupp, Martin; Arbuznikov, Alexei V.; Heßelmann, Andreas; Görling, Andreas

2010-05-01

The isotropic hyperfine coupling constants of the free N(S4) and P(S4) atoms have been evaluated with high-level post-Hartree-Fock and density-functional methods. The phosphorus hyperfine coupling presents a significant challenge to both types of methods. With large basis sets, MP2 and coupled-cluster singles and doubles calculations give much too small values for the phosphorus atom. Triple excitations are needed in coupled-cluster calculations to achieve reasonable agreement with experiment. None of the standard density functionals reproduce even the correct sign of this hyperfine coupling. Similarly, the computed hyperfine couplings depend crucially on the self-consistent treatment in exact-exchange density-functional theory within the optimized effective potential (OEP) method. Well-balanced auxiliary and orbital basis sets are needed for basis-expansion exact-exchange-only OEP approaches to come close to Hartree-Fock or numerical OEP data. Results from the localized Hartree-Fock and Krieger-Li-Iafrate approximations deviate notably from exact OEP data in spite of very similar total energies. Of the functionals tested, only full exact-exchange methods augmented by a correlation functional gave at least the correct sign of the P(S4) hyperfine coupling but with too low absolute values. The subtle interplay between the spin-polarization contributions of the different core shells has been analyzed, and the influence of even very small changes in the exchange-correlation potential could be identified.

Structure and stability of clusters of β-alanine in the gas phase: importance of the nature of intermolecular interactions.

PubMed

Piekarski, Dariusz Grzegorz; Díaz-Tendero, Sergio

2017-02-15

We present a theoretical study of neutral clusters of β-alanine molecules in the gas phase, (β-ala) n n ≤ 5. Classical molecular dynamics simulations carried out with different internal excitation energies provide information on the clusters formation and their thermal decomposition limits. We also present an assessment study performed with different families of density functionals using the dimer, (β-ala) 2 , as a benchmark system. The M06-2X functional provides the best agreement in geometries and relative energies in comparison with the reference values computed with the MP2 and CCSD(T) methods. The structure, stability, dissociation energies and vertical ionization potentials of the studied clusters have been investigated using this functional in combination with the 6-311++G(d,p) basis set. An exhaustive analysis of intermolecular interactions is also presented. These results provide new insights into the stability, interaction nature and formation mechanisms of clusters of amino acids in the gas phase.

Cosmology with EMSS Clusters of Galaxies

NASA Technical Reports Server (NTRS)

Donahue, Megan; Voit, G. Mark

1999-01-01

We use ASCA observations of the Extended Medium Sensitivity Survey sample of clusters of galaxies to construct the first z = 0.5 - 0.8 cluster temperature function. This distant cluster temperature function, when compared to local z approximately 0 and to a similar moderate redshift (z = 0.3 - 0.4) temperature function strongly constrains the matter density of the universe. Best fits to the distributions of temperatures and redshifts of these cluster samples results in Omega(sub M) = 0.45 +/- 0.1 if Lambda = 0 and Omega = 0.27 +/- 0.1 if Lambda + Omega(sub M) = 1. The uncertainties are 1sigma statistical. We examine the systematics of our approach and find that systematics, stemming mainly from model assumptions and not measurement errors, are about the same size as the statistical uncertainty +/- 0.1. In this poster proceedings, we clarify the issue of a8 as reported in our paper Donahue & Voit (1999), since this was a matter of discussion at the meeting.

Density functional study of structural and electronic properties of bimetallic silver-gold clusters: Comparison with pure gold and silver clusters

NASA Astrophysics Data System (ADS)

Bonacic-Koutecky, Vlasta; Burda, Jaroslav; Mitric, Roland; Ge, Maofa; Zampella, Giuseppe; Fantucci, Piercarlo

2002-08-01

Bimetallic silver-gold clusters offer an excellent opportunity to study changes in metallic versus "ionic" properties involving charge transfer as a function of the size and the composition, particularly when compared to pure silver and gold clusters. We have determined structures, ionization potentials, and vertical detachment energies for neutral and charged bimetallic AgmAun 3[less-than-or-equal](m+n)[less-than-or-equal]5 clusters. Calculated VDE values compare well with available experimental data. In the stable structures of these clusters Au atoms assume positions which favor the charge transfer from Ag atoms. Heteronuclear bonding is usually preferred to homonuclear bonding in clusters with equal numbers of hetero atoms. In fact, stable structures of neutral Ag2Au2, Ag3Au3, and Ag4Au4 clusters are characterized by the maximum number of hetero bonds and peripheral positions of Au atoms. Bimetallic tetramer as well as hexamer are planar and have common structural properties with corresponding one-component systems, while Ag4Au4 and Ag8 have 3D forms in contrast to Au8 which assumes planar structure. At the density functional level of theory we have shown that this is due to participation of d electrons in bonding of pure Aun clusters while s electrons dominate bonding in pure Agm as well as in bimetallic clusters. In fact, Aun clusters remain planar for larger sizes than Agm and AgnAun clusters. Segregation between two components in bimetallic systems is not favorable, as shown in the example of Ag5Au5 cluster. We have found that the structures of bimetallic clusters with 20 atoms Ag10Au10 and Ag12Au8 are characterized by negatively charged Au subunits embedded in Ag environment. In the latter case, the shape of Au8 is related to a pentagonal bipyramid capped by one atom and contains three exposed negatively charged Au atoms. They might be suitable for activating reactions relevant to catalysis. According to our findings the charge transfer in bimetallic clusters is responsible for formation of negatively charged gold subunits which are expected to be reactive, a situation similar to that of gold clusters supported on metal oxides.

Self-consistent calculations for the electronic structure of a vacancy in copper. A solution of the embedding problem

NASA Astrophysics Data System (ADS)

Zeller, R.; Braspenning, P. J.

1982-06-01

The charge density and the local density of states for a vacancy in Cu and for the first shell of Cu neighbours are calculated by the KKR-Green's function technique. The muffin-tin potentials for the vacancy and the neighbour shell atoms are determined self-consistently in the local density approximation of density functional theory. By the use of the proper host Green's function the embedding of this cluster of 13 perturbed muffin-tins into the infinite array of bulk Cu muffin-tin potentials is described rigorously, thus representing a solution of the embedding problem. The calculations demonstrate a rather large charge transfer of 1.1 electrons from the first neighbour shell to the vacancy.

Valence and charge-transfer optical properties for some SinCm (m, n ≤ 12) clusters: Comparing TD-DFT, complete-basis-limit EOMCC, and benchmarks from spectroscopy.

PubMed

Lutz, Jesse J; Duan, Xiaofeng F; Ranasinghe, Duminda S; Jin, Yifan; Margraf, Johannes T; Perera, Ajith; Burggraf, Larry W; Bartlett, Rodney J

2018-05-07

Accurate optical characterization of the closo-Si 12 C 12 molecule is important to guide experimental efforts toward the synthesis of nano-wires, cyclic nano-arrays, and related array structures, which are anticipated to be robust and efficient exciton materials for opto-electronic devices. Working toward calibrated methods for the description of closo-Si 12 C 12 oligomers, various electronic structure approaches are evaluated for their ability to reproduce measured optical transitions of the SiC 2 , Si 2 C n (n = 1-3), and Si 3 C n (n = 1, 2) clusters reported earlier by Steglich and Maier [Astrophys. J. 801, 119 (2015)]. Complete-basis-limit equation-of-motion coupled-cluster (EOMCC) results are presented and a comparison is made between perturbative and renormalized non-iterative triples corrections. The effect of adding a renormalized correction for quadruples is also tested. Benchmark test sets derived from both measurement and high-level EOMCC calculations are then used to evaluate the performance of a variety of density functionals within the time-dependent density functional theory (TD-DFT) framework. The best-performing functionals are subsequently applied to predict valence TD-DFT excitation energies for the lowest-energy isomers of Si n C and Si n-1 C 7-n (n = 4-6). TD-DFT approaches are then applied to the Si n C n (n = 4-12) clusters and unique spectroscopic signatures of closo-Si 12 C 12 are discussed. Finally, various long-range corrected density functionals, including those from the CAM-QTP family, are applied to a charge-transfer excitation in a cyclic (Si 4 C 4 ) 4 oligomer. Approaches for gauging the extent of charge-transfer character are also tested and EOMCC results are used to benchmark functionals and make recommendations.

Cluster kinetics model of particle separation in vibrated granular media.

PubMed

McCoy, Benjamin J; Madras, Giridhar

2006-01-01

We model the Brazil-nut effect (BNE) by hypothesizing that granules form clusters that fragment and aggregate. This provides a heterogeneous medium in which the immersed intruder particle rises (BNE) or sinks (reverse BNE) according to relative convection currents and buoyant and drag forces. A simple relationship proposed for viscous drag in terms of the vibrational intensity and the particle to grain density ratio allows simulation of published experimental data for rise and sink times as functions of particle radius, initial depth of the particle, and particle-grain density ratio. The proposed model correctly describes the experimentally observed maximum in risetime.

A scan statistic for binary outcome based on hypergeometric probability model, with an application to detecting spatial clusters of Japanese encephalitis.

PubMed

Zhao, Xing; Zhou, Xiao-Hua; Feng, Zijian; Guo, Pengfei; He, Hongyan; Zhang, Tao; Duan, Lei; Li, Xiaosong

2013-01-01

As a useful tool for geographical cluster detection of events, the spatial scan statistic is widely applied in many fields and plays an increasingly important role. The classic version of the spatial scan statistic for the binary outcome is developed by Kulldorff, based on the Bernoulli or the Poisson probability model. In this paper, we apply the Hypergeometric probability model to construct the likelihood function under the null hypothesis. Compared with existing methods, the likelihood function under the null hypothesis is an alternative and indirect method to identify the potential cluster, and the test statistic is the extreme value of the likelihood function. Similar with Kulldorff's methods, we adopt Monte Carlo test for the test of significance. Both methods are applied for detecting spatial clusters of Japanese encephalitis in Sichuan province, China, in 2009, and the detected clusters are identical. Through a simulation to independent benchmark data, it is indicated that the test statistic based on the Hypergeometric model outweighs Kulldorff's statistics for clusters of high population density or large size; otherwise Kulldorff's statistics are superior.

Stability and migration of large oxygen clusters in UO(2+x): density functional theory calculations.

PubMed

Andersson, D A; Espinosa-Faller, F J; Uberuaga, B P; Conradson, S D

2012-06-21

Using ab initio molecular dynamics simulations and nudged elastic band calculations we examine the finite temperature stability, transition pathways, and migration mechanisms of large oxygen clusters in UO(2+x). Here we specifically consider the recently proposed split quad-interstitial and cuboctahedral oxygen clusters. It is shown that isolated cuboctahedral clusters may transform into more stable configurations that are closely linked to the split quad-interstitial. The split quad-interstitial is stable with respect to single interstitials occupying the empty octahedral holes of the UO(2) lattice. In order to better understand discrepancies between theory and experiments, the simulated atomic pair distribution functions for the split quad-interstitial structures are analyzed with respect to the distribution function for U(4)O(9) previously obtained from neutron diffraction data. Our nudged elastic band calculations suggest that the split quad-interstitial may migrate by translating one of its constituent di-interstitial clusters via a barrier that is lower than the corresponding barrier for individual interstitials, but higher than the barrier for the most stable di-interstitial cluster.

A multi-scale study of the adsorption of lanthanum on the (110) surface of tungsten

NASA Astrophysics Data System (ADS)

Samin, Adib J.; Zhang, Jinsuo

2016-07-01

In this study, we utilize a multi-scale approach to studying lanthanum adsorption on the (110) plane of tungsten. The energy of the system is described from density functional theory calculations within the framework of the cluster expansion method. It is found that including two-body figures up to the sixth nearest neighbor yielded a reasonable agreement with density functional theory calculations as evidenced by the reported cross validation score. The results indicate that the interaction between the adsorbate atoms in the adlayer is important and cannot be ignored. The parameterized cluster expansion expression is used in a lattice gas Monte Carlo simulation in the grand canonical ensemble at 773 K and the adsorption isotherm is recorded. Implications of the obtained results for the pyroprocessing application are discussed.

Patching the Exchange-Correlation Potential in Density Functional Theory.

PubMed

Huang, Chen

2016-05-10

A method for directly patching exchange-correlation (XC) potentials in materials is derived. The electron density of a system is partitioned into subsystem densities by dividing its Kohn-Sham (KS) potential among the subsystems. Inside each subsystem, its projected KS potential is required to become the total system's KS potential. This requirement, together with the nearsightedness principle of electronic matters, ensures that the electronic structures inside subsystems can be good approximations to the total system's electronic structure. The nearsightedness principle also ensures that subsystem densities could be well localized in their regions, making it possible to use high-level methods to invert the XC potentials for subsystem densities. Two XC patching methods are developed. In the local XC patching method, the total system's XC potential is improved in the cluster region. We show that the coupling between a cluster and its environment is important for achieving a fast convergence of the electronic structure in the cluster region. In the global XC patching method, we discuss how to patch the subsystem XC potentials to construct the XC potential in the total system, aiming to scale up high-level quantum mechanics simulations of materials. Proof-of-principle examples are given.

Role of environmental and antibiotic stress on Staphylococcus epidermidis biofilm microstructure.

PubMed

Stewart, Elizabeth J; Satorius, Ashley E; Younger, John G; Solomon, Michael J

2013-06-11

Cellular clustering and separation of Staphylococcus epidermidis surface adherent biofilms were found to depend significantly on both antibiotic and environmental stress present during growth under steady flow. Image analysis techniques common to colloidal science were applied to image volumes acquired with high-resolution confocal laser scanning microscopy to extract spatial positions of individual bacteria in volumes of size ~30 × 30 × 15 μm(3). The local number density, cluster distribution, and radial distribution function were determined at each condition by analyzing the statistics of the bacterial spatial positions. Environmental stressors of high osmotic pressure (776 mM NaCl) and sublethal antibiotic dose (1.9 μg/mL vancomycin) decreased the average bacterial local number density 10-fold. Device-associated bacterial biofilms are frequently exposed to these environmental and antibiotic stressors while undergoing flow in the bloodstream. Characteristic density phenotypes associated with low, medium, and high local number densities were identified in unstressed S. epidermidis biofilms, while stressed biofilms contained medium- and low-density phenotypes. All biofilms exhibited clustering at length scales commensurate with cell division (~1.0 μm). However, density phenotypes differed in cellular connectivity at the scale of ~6 μm. On this scale, nearly all cells in the high- and medium-density phenotypes were connected into a single cluster with a structure characteristic of a densely packed disordered fluid. However, in the low-density phenotype, the number of clusters was greater, equal to 4% of the total number of cells, and structures were fractal in nature with d(f) =1.7 ± 0.1. The work advances the understanding of biofilm growth, informs the development of predictive models of transport and mechanical properties of biofilms, and provides a method for quantifying the kinetics of bacterial surface colonization as well as biofilm fracture and fragmentation.

First principles study of neutral and anionic (medium-size) aluminum nitride clusters: AlnNn, n=7-16.

PubMed

Costales, Aurora; Blanco, M A; Francisco, E; Pendas, A Martín; Pandey, Ravindra

2006-03-09

We report the results of a theoretical study of AlnNn (n=7-16) clusters that is based on density functional theory. We will focus on the evolution of structural and electronic properties with the cluster size in the stoichiometric AlN clusters considered. The results reveal that the structural and electronic properties tend to evolve toward their respective bulk limits. The rate of evolution is, however, slow due to the hollow globular shape exhibited by the clusters, which introduces large surface effects that dominate the properties studied. We will also discuss the changes induced upon addition of an extra electron to the respective neutral clusters.

Trapping of Li(+) Ions by [ThFn](4-n) Clusters Leading to Oscillating Maxwell-Stefan Diffusivity in the Molten Salt LiF-ThF4.

PubMed

Chakraborty, Brahmananda; Kidwai, Sharif; Ramaniah, Lavanya M

2016-08-18

A molten salt mixture of lithium fluoride and thorium fluoride (LiF-ThF4) serves as a fuel as well as a coolant in the most sophisticated molten salt reactor (MSR). Here, we report for the first time dynamic correlations, Onsager coefficients, Maxwell-Stefan (MS) diffusivities, and the concentration dependence of density and enthalpy of the molten salt mixture LiF-ThF4 at 1200 K in the composition range of 2-45% ThF4 and also at eutectic composition in the temperature range of 1123-1600 K using Green-Kubo formalism and equilibrium molecular dynamics simulations. We have observed an interesting oscillating pattern for the MS diffusivity for the cation-cation pair, in which ĐLi-Th oscillates between positive and negative values with the amplitude of the oscillation reducing as the system becomes rich in ThF4. Through the velocity autocorrelation function, vibrational density of states, radial distribution function analysis, and structural snapshots, we establish an interplay between the local structure and multicomponent dynamics and predict that formation of negatively charged [ThFn](4-n) clusters at a higher ThF4 mole % makes positively charged Li(+) ions oscillate between different clusters, with their range of motion reducing as the number of [ThFn](4-n) clusters increases, and finally Li(+) ions almost get trapped at a higher ThF4% when the electrostatic force on Li(+) exerted by various surrounding clusters gets balanced. Although reports on variations of density and enthalpy with temperature exist in the literature, for the first time we report variations of the density and enthalpy of LiF-ThF4 with the concentration of ThF4 (mole %) and fit them with the square root function of ThF4 concentration, which will be very useful for experimentalists to obtain data over a range of concentrations from fitting the formula for design purposes. The formation of [ThFn](4-n) clusters and the reduction in the diffusivity of the ions at a higher ThF4% may limit the percentage of ThF4 that can be used in the MSR to optimize the neutron economy.

C 60 as a chemical Faraday cage for three ferromagnetic Fe atoms

NASA Astrophysics Data System (ADS)

Gao, Guohua; Kang, Hong Seok

2008-09-01

Based on calculations using density functional theory, we show that C 60 can act as a chemical Faraday cage in which a highly magnetic metal cluster with a high chemical reactivity can be encapsulated. As an example, we find that C 60 can encapsulate a Fe 3 cluster, while it is much less likely to encapsulate a Fe 2 cluster. Spin multiplicity (=9) of the Fe 3@C 60 is very high, being comparable to that (=11) of a free Fe 3 cluster. Geometrically, the triangular plane of the cluster is perpendicular to a S6 axis of the fullerene.

Low oxidation state aluminum-containing cluster anions: Cp{sup ∗}Al{sub n}H{sup −}, n = 1–3

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Xinxing; Ganteför, Gerd; Bowen, Kit, E-mail: AKandalam@wcupa.edu, E-mail: kbowen@jhu.edu

Three new, low oxidation state, aluminum-containing cluster anions, Cp*Al{sub n}H{sup −}, n = 1–3, were prepared via reactions between aluminum hydride cluster anions, Al{sub n}H{sub m}{sup −}, and Cp*H ligands. These were characterized by mass spectrometry, anion photoelectron spectroscopy, and density functional theory based calculations. Agreement between the experimentally and theoretically determined vertical detachment energies and adiabatic detachment energies validated the computed geometrical structures. Reactions between aluminum hydride cluster anions and ligands provide a new avenue for discovering low oxidation state, ligated aluminum clusters.

High–frequency cluster radio galaxies: Luminosity functions and implications for SZE–selected cluster samples

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gupta, Nikhel; Saro, A.; Mohr, J. J.

We study the overdensity of point sources in the direction of X-ray-selected galaxy clusters from the meta-catalogue of X-ray-detected clusters of galaxies (MCXC; < z > = 0.14) at South Pole Telescope (SPT) and Sydney University Molonglo Sky Survey (SUMSS) frequencies. Flux densities at 95, 150 and 220 GHz are extracted from the 2500 deg 2 SPT-SZ survey maps at the locations of SUMSS sources, producing a multifrequency catalogue of radio galaxies. In the direction of massive galaxy clusters, the radio galaxy flux densities at 95 and 150 GHz are biased low by the cluster Sunyaev–Zel’dovich Effect (SZE) signal, whichmore » is negative at these frequencies. We employ a cluster SZE model to remove the expected flux bias and then study these corrected source catalogues. We find that the high-frequency radio galaxies are centrally concentrated within the clusters and that their luminosity functions (LFs) exhibit amplitudes that are characteristically an order of magnitude lower than the cluster LF at 843 MHz. We use the 150 GHz LF to estimate the impact of cluster radio galaxies on an SPT-SZ like survey. The radio galaxy flux typically produces a small bias on the SZE signal and has negligible impact on the observed scatter in the SZE mass–observable relation. If we assume there is no redshift evolution in the radio galaxy LF then 1.8 ± 0.7 per cent of the clusters with detection significance ξ ≥ 4.5 would be lost from the sample. As a result, allowing for redshift evolution of the form (1 + z) 2.5 increases the incompleteness to 5.6 ± 1.0 per cent. Improved constraints on the evolution of the cluster radio galaxy LF require a larger cluster sample extending to higher redshift.« less

High–frequency cluster radio galaxies: Luminosity functions and implications for SZE–selected cluster samples

DOE PAGES

Gupta, Nikhel; Saro, A.; Mohr, J. J.; ...

2017-01-15

We study the overdensity of point sources in the direction of X-ray-selected galaxy clusters from the meta-catalogue of X-ray-detected clusters of galaxies (MCXC; < z > = 0.14) at South Pole Telescope (SPT) and Sydney University Molonglo Sky Survey (SUMSS) frequencies. Flux densities at 95, 150 and 220 GHz are extracted from the 2500 deg 2 SPT-SZ survey maps at the locations of SUMSS sources, producing a multifrequency catalogue of radio galaxies. In the direction of massive galaxy clusters, the radio galaxy flux densities at 95 and 150 GHz are biased low by the cluster Sunyaev–Zel’dovich Effect (SZE) signal, whichmore » is negative at these frequencies. We employ a cluster SZE model to remove the expected flux bias and then study these corrected source catalogues. We find that the high-frequency radio galaxies are centrally concentrated within the clusters and that their luminosity functions (LFs) exhibit amplitudes that are characteristically an order of magnitude lower than the cluster LF at 843 MHz. We use the 150 GHz LF to estimate the impact of cluster radio galaxies on an SPT-SZ like survey. The radio galaxy flux typically produces a small bias on the SZE signal and has negligible impact on the observed scatter in the SZE mass–observable relation. If we assume there is no redshift evolution in the radio galaxy LF then 1.8 ± 0.7 per cent of the clusters with detection significance ξ ≥ 4.5 would be lost from the sample. As a result, allowing for redshift evolution of the form (1 + z) 2.5 increases the incompleteness to 5.6 ± 1.0 per cent. Improved constraints on the evolution of the cluster radio galaxy LF require a larger cluster sample extending to higher redshift.« less

Probing structure, thermochemistry, electron affinity, and magnetic moment of thulium-doped silicon clusters TmSi n (n = 3-10) and their anions with density functional theory.

PubMed

Huang, Xintao; Yang, Jucai

2017-12-26

The most stable structures and electronic properties of TmSi n (n = 3-10) clusters and their anions have been probed by using the ABCluster global search technique combined with the PBE, TPSSh, and B3LYP density functional methods. The results revealed that the most stable structures of neutral TmSi n and their anions can be regarded as substituting a Si atom of the ground state structure of Si n + 1 with a Tm atom. The reliable AEAs, VDEs and simulated PES of TmSi n (n = 3-10) are presented. Calculations of HOMO-LUMO gap revealed that introducing Tm atom to Si cluster can improve photochemical reactivity of the cluster. The NPA analyses indicated that the 4f electron of Tm atom in TmSi n (n = 3-10) and their anions do not participate in bonding. The total magnetic moments of TmSi n are mainly provided by the 4f electrons of Tm atom. The dissociation energy of Tm atom from the most stable structure of TmSi n and their anions has been calculated to examine relative stability.

Study of MoVO(y) (y = 2-5) anion and neutral clusters using anion photoelectron spectroscopy and density functional theory calculations.

PubMed

Mann, Jennifer E; Rothgeb, David W; Waller, Sarah E; Jarrold, Caroline Chick

2010-10-28

The vibrationally resolved anion photoelectron (PE) spectra of MoVO(y)(-) (y = 2 - 5) metal suboxide clusters are presented and analyzed in the context of density functional theory (DFT) calculations. The electronically congested spectra reflect an increase in cluster electron affinity with increasing oxidation state. Ion beam hole-burning results reveal the features in the PE spectra of MoVO(2)(-) and MoVO(4)(-) are a result of only one anion isomer, while at least two isomers contribute to electronic structure observed in the PE spectrum of MoVO(3)(-). Spectral features of the binary systems are compared to their pure analogs, Mo(2)O(y) and V(2)O(y). An attempt to characterize the anion and neutral electronic and molecular structures is made by comparison with results from DFT calculations. However, reconciliation between the cluster spectra and the calculated spectroscopic parameters is not as straightforward as in previous studies on similar systems (Yoder, B. L.; Maze, J. T.; Raghavachari, K.; Jarrold, C. C. J. Chem. Phys. 2005, 122, 094313 and Mayhall, N. J.; Rothgeb, D. W.; Hossain, E.; Raghavachari, K.; Jarrold, C. C. J. Chem. Phys. 2009, 130, 124313).

Methanol clusters (CH3OH)n, n = 3-6 in external electric fields: density functional theory approach.

PubMed

Rai, Dhurba; Kulkarni, Anant D; Gejji, Shridhar P; Pathak, Rajeev K

2011-07-14

Structural evolution of cyclic and branched-cyclic methanol clusters containing three to six molecules, under the influence of externally applied uniform static electric field is studied within the density functional theory. Akin to the situation for water clusters, the electric field is seen to stretch the intermolecular hydrogen bonds, and eventually break the H-bonded network at certain characteristic threshold field values of field strength in the range 0.009-0.016 a.u., yielding linear or branched structures with a lower energy. These structural transitions are characterized by an abrupt increase in the electric dipole moment riding over its otherwise steady nonlinear increase with the applied field. The field tends to rupture the H-bonded structure; consequently, the number of hydrogen bonds decreases with increasing field strength. Vibrational spectra analyzed for fields applied perpendicular to the cyclic ring structures bring out the shifts in the OH ring vibrations (blueshift) and the CO stretch vibrations (redshift). For a given field strength, the blueshifts increase with the number of molecules in the ring and are found to be generally larger than those in the corresponding water cluster counterparts.

Hypernetted-chain-like closure of Ornstein-Zernike equation in multibody dissipative particle dynamics

NASA Astrophysics Data System (ADS)

Mo, Chao-jie; Qin, Li-zi; Yang, Li-jun

2017-10-01

We have derived a hypernetted-chain-like (HNC-like) approximate closure of the Ornstein-Zernike equation for multibody dissipative particle dynamics (MDPD) system in which the classic closures are not directly practicable. We first point out that the Percus's method is applicable to MDPD system in which particles interact with a density-dependent potential. And then an HNC-like closure is derived using Percus's idea and the saddle-point approximation of particle free energy. This HNC-like closure is compared with results of previous researchers, and in many cases, it demonstrates better agreement with computer simulation results. The HNC-like closure is used to predict the cluster crystallization in MDPD. We determine whether the cluster crystallization will happen in a system utilizing the widely applicable Hansen-Verlet freezing criterion and by observing the radial distribution function. The conclusions drawn from the results of the HNC-like closure are in agreement with computer simulation results. We evaluate different weight functions to determine whether they are prone to cluster crystallization. A new effective density-dependent pairwise potential is also proposed to help to explain the tendency to cluster crystallization of MDPD systems.

Improving hot region prediction by parameter optimization of density clustering in PPI.

PubMed

Hu, Jing; Zhang, Xiaolong

2016-11-01

This paper proposed an optimized algorithm which combines density clustering of parameter selection with feature-based classification for hot region prediction. First, all the residues are classified by SVM to remove non-hot spot residues, then density clustering of parameter selection is used to find hot regions. In the density clustering, this paper studies how to select input parameters. There are two parameters radius and density in density-based incremental clustering. We firstly fix density and enumerate radius to find a pair of parameters which leads to maximum number of clusters, and then we fix radius and enumerate density to find another pair of parameters which leads to maximum number of clusters. Experiment results show that the proposed method using both two pairs of parameters provides better prediction performance than the other method, and compare these two predictive results, the result by fixing radius and enumerating density have slightly higher prediction accuracy than that by fixing density and enumerating radius. Copyright © 2016. Published by Elsevier Inc.

Lithium cluster anions: photoelectron spectroscopy and ab initio calculations.

PubMed

Alexandrova, Anastassia N; Boldyrev, Alexander I; Li, Xiang; Sarkas, Harry W; Hendricks, Jay H; Arnold, Susan T; Bowen, Kit H

2011-01-28

Structural and energetic properties of small, deceptively simple anionic clusters of lithium, Li(n)(-), n = 3-7, were determined using a combination of anion photoelectron spectroscopy and ab initio calculations. The most stable isomers of each of these anions, the ones most likely to contribute to the photoelectron spectra, were found using the gradient embedded genetic algorithm program. Subsequently, state-of-the-art ab initio techniques, including time-dependent density functional theory, coupled cluster, and multireference configurational interactions methods, were employed to interpret the experimental spectra.

Predictive coupled-cluster isomer orderings for some Si{sub n}C{sub m} (m, n ≤ 12) clusters: A pragmatic comparison between DFT and complete basis limit coupled-cluster benchmarks

DOE Office of Scientific and Technical Information (OSTI.GOV)

Byrd, Jason N., E-mail: byrd.jason@ensco.com; ENSCO, Inc., 4849 North Wickham Road, Melbourne, Florida 32940; Lutz, Jesse J., E-mail: jesse.lutz.ctr@afit.edu

The accurate determination of the preferred Si{sub 12}C{sub 12} isomer is important to guide experimental efforts directed towards synthesizing SiC nano-wires and related polymer structures which are anticipated to be highly efficient exciton materials for the opto-electronic devices. In order to definitively identify preferred isomeric structures for silicon carbon nano-clusters, highly accurate geometries, energies, and harmonic zero point energies have been computed using coupled-cluster theory with systematic extrapolation to the complete basis limit for set of silicon carbon clusters ranging in size from SiC{sub 3} to Si{sub 12}C{sub 12}. It is found that post-MBPT(2) correlation energy plays a significant rolemore » in obtaining converged relative isomer energies, suggesting that predictions using low rung density functional methods will not have adequate accuracy. Utilizing the best composite coupled-cluster energy that is still computationally feasible, entailing a 3-4 SCF and coupled-cluster theory with singles and doubles extrapolation with triple-ζ (T) correlation, the closo Si{sub 12}C{sub 12} isomer is identified to be the preferred isomer in the support of previous calculations [X. F. Duan and L. W. Burggraf, J. Chem. Phys. 142, 034303 (2015)]. Additionally we have investigated more pragmatic approaches to obtaining accurate silicon carbide isomer energies, including the use of frozen natural orbital coupled-cluster theory and several rungs of standard and double-hybrid density functional theory. Frozen natural orbitals as a way to compute post-MBPT(2) correlation energy are found to be an excellent balance between efficiency and accuracy.« less

Constraints on the Energy Content of the Universe from a Combination of Galaxy Cluster Observables

NASA Technical Reports Server (NTRS)

Molnar, Sandor M.; Haiman, Zoltan; Birkinshaw, Mark; Mushotzky, Richard F.

2003-01-01

We demonstrate that constraints on cosmological parameters from the distribution of clusters as a function of redshift (dN/dz) are complementary to accurate angular diameter distance (D(sub A)) measurements to clusters, and their combination significantly tightens constraints on the energy density content of the Universe. The number counts can be obtained from X-ray and/or SZ (Sunyaev-Ze'dovich effect) surveys, and the angular diameter distances can be determined from deep observations of the intra-cluster gas using their thermal bremsstrahlung X-ray emission and the SZ effect. We combine constraints from simulated cluster number counts expected from a 12 deg(sup 2) SZ cluster survey and constraints from simulated angular diameter distance measurements based on the X-ray/SZ method assuming a statistical accuracy of 10% in the angular diameter distance determination of 100 clusters with redshifts less than 1.5. We find that Omega(sub m), can be determined within about 25%, Omega(sub lambda) within 20% and w within 16%. We show that combined dN/dz+(sub lambda) constraints can be used to constrain the different energy densities in the Universe even in the presence of a few percent redshift dependent systematic error in D(sub lambda). We also address the question of how best to select clusters of galaxies for accurate diameter distance determinations. We show that the joint dN/dz+ D(lambda) constraints on cosmological parameters for a fixed target accuracy in the energy density parameters are optimized by selecting clusters with redshift upper cut-offs in the range 0.55 approx. less than 1. Subject headings: cosmological parameters - cosmology: theory - galaxies:clusters: general

Electronic and magnetic properties of small rhodium clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Soon, Yee Yeen; Yoon, Tiem Leong; Lim, Thong Leng

2015-04-24

We report a theoretical study of the electronic and magnetic properties of rhodium-atomic clusters. The lowest energy structures at the semi-empirical level of rhodium clusters are first obtained from a novel global-minimum search algorithm, known as PTMBHGA, where Gupta potential is used to describe the atomic interaction among the rhodium atoms. The structures are then re-optimized at the density functional theory (DFT) level with exchange-correlation energy approximated by Perdew-Burke-Ernzerhof generalized gradient approximation. For the purpose of calculating the magnetic moment of a given cluster, we calculate the optimized structure as a function of the spin multiplicity within the DFT framework.more » The resultant magnetic moments with the lowest energies so obtained allow us to work out the magnetic moment as a function of cluster size. Rhodium atomic clusters are found to display a unique variation in the magnetic moment as the cluster size varies. However, Rh{sub 4} and Rh{sub 6} are found to be nonmagnetic. Electronic structures of the magnetic ground-state structures are also investigated within the DFT framework. The results are compared against those based on different theoretical approaches available in the literature.« less

In situ study of heavy ion irradiation response of immiscible Cu/Fe multilayers

DOE PAGES

Chen, Youxing; Li, Nan; Bufford, Daniel Charles; ...

2016-04-09

By providing active defect sinks that capture and annihilate radiation induced defect clusters immiscible metallic multilayers with incoherent interfaces can effectively reduce defect density in ion irradiated metals. Although it is anticipated that defect density within the layers should vary as a function of distance to the layer interface, there is, to date, little in situ TEM evidence to validate this hypothesis. In our study monolithic Cu films and Cu/Fe multilayers with individual layer thickness, h, of 100 and 5 nm were subjected to in situ Cu ion irradiation at room temperature to nominally 1 displacement-per-atom inside a transmission electronmore » microscope. Rapid formation and propagation of defect clusters were observed in monolithic Cu, whereas fewer defects with smaller dimensions were generated in Cu/Fe multilayers with smaller h. Moreover, in situ video shows that the cumulative defect density in Cu/Fe 100 nm multilayers indeed varies, as a function of distance to the layer interfaces, supporting a long postulated hypothesis.« less

Quantum chemical study of small AlnBm clusters: Structure and physical properties

NASA Astrophysics Data System (ADS)

Loukhovitski, Boris I.; Sharipov, Alexander S.; Starik, Alexander M.

2017-08-01

The structure and physical properties, including rotational constants, characteristic vibrational temperatures, collision diameter, dipole moment, static polarizability, the energy gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO), and formation enthalpy of the different isomeric forms of AlnBm clusters with n + m ⩽ 7 are studied using density functional theory. The search of the structure of isomers has been carried employing multistep hierarchical algorithm. Temperature dependencies of thermodynamic functions, such as enthalpy, entropy, and specific heat capacity, have been determined both for the individual isomers and for the ensembles with equilibrium and frozen compositions for the each class of clusters taking into account the anharmonicity of cluster vibrations and the contribution of their excited electronic states. The prospects of the application of small AlnBm clusters as the components of energetic materials are also considered.

Fragment-based {sup 13}C nuclear magnetic resonance chemical shift predictions in molecular crystals: An alternative to planewave methods

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hartman, Joshua D.; Beran, Gregory J. O., E-mail: gregory.beran@ucr.edu; Monaco, Stephen

2015-09-14

We assess the quality of fragment-based ab initio isotropic {sup 13}C chemical shift predictions for a collection of 25 molecular crystals with eight different density functionals. We explore the relative performance of cluster, two-body fragment, combined cluster/fragment, and the planewave gauge-including projector augmented wave (GIPAW) models relative to experiment. When electrostatic embedding is employed to capture many-body polarization effects, the simple and computationally inexpensive two-body fragment model predicts both isotropic {sup 13}C chemical shifts and the chemical shielding tensors as well as both cluster models and the GIPAW approach. Unlike the GIPAW approach, hybrid density functionals can be used readilymore » in a fragment model, and all four hybrid functionals tested here (PBE0, B3LYP, B3PW91, and B97-2) predict chemical shifts in noticeably better agreement with experiment than the four generalized gradient approximation (GGA) functionals considered (PBE, OPBE, BLYP, and BP86). A set of recommended linear regression parameters for mapping between calculated chemical shieldings and observed chemical shifts are provided based on these benchmark calculations. Statistical cross-validation procedures are used to demonstrate the robustness of these fits.« less

Final Technical Report for DE-SC0001878 [Theory and Simulation of Defects in Oxide Materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chelikowsky, James R.

2014-04-14

We explored a wide variety of oxide materials and related problems, including materials at the nanoscale and generic problems associated with oxide materials such as the development of more efficient computational tools to examine these materials. We developed and implemented methods to understand the optical and structural properties of oxides. For ground state properties, our work is predominantly based on pseudopotentials and density functional theory (DFT), including new functionals and going beyond the local density approximation (LDA): LDA+U. To study excited state properties (quasiparticle and optical excitations), we use time dependent density functional theory, the GW approach, and GW plusmore » Bethe-Salpeter equation (GW-BSE) methods based on a many-body Green function approaches. Our work focused on the structural, electronic, optical and magnetic properties of defects (such as oxygen vacancies) in hafnium oxide, titanium oxide (both bulk and clusters) and related materials. We calculated the quasiparticle defect states and charge transition levels of oxygen vacancies in monoclinic hafnia. we presented a milestone G0W0 study of two of the crystalline phases of dye-sensitized TiO{sub 2} clusters. We employed hybrid density functional theory to examine the electronic structure of sexithiophene/ZnO interfaces. To identify the possible effect of epitaxial strain on stabilization of the ferromagnetic state of LaCoO{sub 3} (LCO), we compare the total energy of the magnetic and nonmagnetic states of the strained theoretical bulk structure.« less

Percolation analyses of observed and simulated galaxy clustering

NASA Astrophysics Data System (ADS)

Bhavsar, S. P.; Barrow, J. D.

1983-11-01

A percolation cluster analysis is performed on equivalent regions of the CFA redshift survey of galaxies and the 4000 body simulations of gravitational clustering made by Aarseth, Gott and Turner (1979). The observed and simulated percolation properties are compared and, unlike correlation and multiplicity function analyses, favour high density (Omega = 1) models with n = - 1 initial data. The present results show that the three-dimensional data are consistent with the degree of filamentary structure present in isothermal models of galaxy formation at the level of percolation analysis. It is also found that the percolation structure of the CFA data is a function of depth. Percolation structure does not appear to be a sensitive probe of intrinsic filamentary structure.

Computational identification of developmental enhancers:conservation and function of transcription factor binding-site clustersin drosophila melanogaster and drosophila psedoobscura

DOE Office of Scientific and Technical Information (OSTI.GOV)

Berman, Benjamin P.; Pfeiffer, Barret D.; Laverty, Todd R.

2004-08-06

The identification of sequences that control transcription in metazoans is a major goal of genome analysis. In a previous study, we demonstrated that searching for clusters of predicted transcription factor binding sites could discover active regulatory sequences, and identified 37 regions of the Drosophila melanogaster genome with high densities of predicted binding sites for five transcription factors involved in anterior-posterior embryonic patterning. Nine of these clusters overlapped known enhancers. Here, we report the results of in vivo functional analysis of 27 remaining clusters. We generated transgenic flies carrying each cluster attached to a basal promoter and reporter gene, and assayedmore » embryos for reporter gene expression. Six clusters are enhancers of adjacent genes: giant, fushi tarazu, odd-skipped, nubbin, squeeze and pdm2; three drive expression in patterns unrelated to those of neighboring genes; the remaining 18 do not appear to have enhancer activity. We used the Drosophila pseudoobscura genome to compare patterns of evolution in and around the 15 positive and 18 false-positive predictions. Although conservation of primary sequence cannot distinguish true from false positives, conservation of binding-site clustering accurately discriminates functional binding-site clusters from those with no function. We incorporated conservation of binding-site clustering into a new genome-wide enhancer screen, and predict several hundred new regulatory sequences, including 85 adjacent to genes with embryonic patterns. Measuring conservation of sequence features closely linked to function--such as binding-site clustering--makes better use of comparative sequence data than commonly used methods that examine only sequence identity.« less

Performance Assessment of Kernel Density Clustering for Gene Expression Profile Data

PubMed Central

Zeng, Beiyan; Chen, Yiping P.; Smith, Oscar H.

2003-01-01

Kernel density smoothing techniques have been used in classification or supervised learning of gene expression profile (GEP) data, but their applications to clustering or unsupervised learning of those data have not been explored and assessed. Here we report a kernel density clustering method for analysing GEP data and compare its performance with the three most widely-used clustering methods: hierarchical clustering, K-means clustering, and multivariate mixture model-based clustering. Using several methods to measure agreement, between-cluster isolation, and withincluster coherence, such as the Adjusted Rand Index, the Pseudo F test, the r2 test, and the profile plot, we have assessed the effectiveness of kernel density clustering for recovering clusters, and its robustness against noise on clustering both simulated and real GEP data. Our results show that the kernel density clustering method has excellent performance in recovering clusters from simulated data and in grouping large real expression profile data sets into compact and well-isolated clusters, and that it is the most robust clustering method for analysing noisy expression profile data compared to the other three methods assessed. PMID:18629292

A first-principles study of the influence of helium atoms on the optical response of small silver clusters.

PubMed

Pereiro, M; Baldomir, D; Arias, J E

2011-02-28

Optical excitation spectra of Ag(n) and Ag(n)@He(60) (n = 2, 8) clusters are investigated in the framework of the time-dependent density functional theory (TDDFT) within the linear response regime. We have performed the ab initio calculations for two different exact exchange functionals (GGA-exact and LDA-exact). The computed spectra of Ag(n)@He(60) clusters with the GGA-exact functional accounting for exchange-correlation effects are found to be generally in a relatively good agreement with the experiment. A strategy is proposed to obtain the ground-state structures of the Ag(n)@He(60) clusters and in the initial process of the geometry optimization, the He environment is simulated with buckyballs. A redshift of the silver clusters spectra is observed in the He environment with respect to the ones of bare silver clusters. This observation is discussed and explained in terms of a contraction of the Ag-He bonding length and a consequent confinement of the s valence electrons in silver clusters. Likewise, the Mie-Gans predictions combined with our TDDFT calculations also show that the dielectric effect produced by the He matrix is considerably less important in explaining the redshifting observed in the optical spectra of Ag(n)@He(60) clusters.

Application of adaptive cluster sampling to low-density populations of freshwater mussels

USGS Publications Warehouse

Smith, D.R.; Villella, R.F.; Lemarie, D.P.

2003-01-01

Freshwater mussels appear to be promising candidates for adaptive cluster sampling because they are benthic macroinvertebrates that cluster spatially and are frequently found at low densities. We applied adaptive cluster sampling to estimate density of freshwater mussels at 24 sites along the Cacapon River, WV, where a preliminary timed search indicated that mussels were present at low density. Adaptive cluster sampling increased yield of individual mussels and detection of uncommon species; however, it did not improve precision of density estimates. Because finding uncommon species, collecting individuals of those species, and estimating their densities are important conservation activities, additional research is warranted on application of adaptive cluster sampling to freshwater mussels. However, at this time we do not recommend routine application of adaptive cluster sampling to freshwater mussel populations. The ultimate, and currently unanswered, question is how to tell when adaptive cluster sampling should be used, i.e., when is a population sufficiently rare and clustered for adaptive cluster sampling to be efficient and practical? A cost-effective procedure needs to be developed to identify biological populations for which adaptive cluster sampling is appropriate.

Self-consistent Green's function embedding for advanced electronic structure methods based on a dynamical mean-field concept

NASA Astrophysics Data System (ADS)

Chibani, Wael; Ren, Xinguo; Scheffler, Matthias; Rinke, Patrick

2016-04-01

We present an embedding scheme for periodic systems that facilitates the treatment of the physically important part (here a unit cell or a supercell) with advanced electronic structure methods, that are computationally too expensive for periodic systems. The rest of the periodic system is treated with computationally less demanding approaches, e.g., Kohn-Sham density-functional theory, in a self-consistent manner. Our scheme is based on the concept of dynamical mean-field theory formulated in terms of Green's functions. Our real-space dynamical mean-field embedding scheme features two nested Dyson equations, one for the embedded cluster and another for the periodic surrounding. The total energy is computed from the resulting Green's functions. The performance of our scheme is demonstrated by treating the embedded region with hybrid functionals and many-body perturbation theory in the GW approach for simple bulk systems. The total energy and the density of states converge rapidly with respect to the computational parameters and approach their bulk limit with increasing cluster (i.e., computational supercell) size.

Cosmology and astrophysics from relaxed galaxy clusters - III. Thermodynamic profiles and scaling relations

NASA Astrophysics Data System (ADS)

Mantz, A. B.; Allen, S. W.; Morris, R. G.; Schmidt, R. W.

2016-03-01

This is the third in a series of papers studying the astrophysics and cosmology of massive, dynamically relaxed galaxy clusters. Our sample comprises 40 clusters identified as being dynamically relaxed and hot (I.e. massive) in Papers I and II of this series. Here we consider the thermodynamics of the intracluster medium, in particular the profiles of density, temperature and related quantities, as well as integrated measurements of gas mass, average temperature, total luminosity and centre-excluded luminosity. We fit power-law scaling relations of each of these quantities as a function of redshift and cluster mass, which can be measured precisely and with minimal bias for these relaxed clusters using hydrostatic arguments. For the thermodynamic profiles, we jointly model the density and temperature and their intrinsic scatter as a function of radius, thus also capturing the behaviour of the gas pressure and entropy. For the integrated quantities, we also jointly fit a multidimensional intrinsic covariance. Our results reinforce the view that simple hydrodynamical models provide a good description of relaxed clusters outside their centres, but that additional heating and cooling processes are important in the inner regions (radii r ≲ 0.5 r2500 ≈ 0.15 r500). The thermodynamic profiles remain regular, with small intrinsic scatter, down to the smallest radii where deprojection is straightforward (˜20 kpc); within this radius, even the most relaxed systems show clear departures from spherical symmetry. Our results suggest that heating and cooling are continuously regulated in a tight feedback loop, allowing the cluster atmosphere to remain stratified on these scales.

A multi-scale study of the adsorption of lanthanum on the (110) surface of tungsten

DOE Office of Scientific and Technical Information (OSTI.GOV)

Samin, Adib J.; Zhang, Jinsuo

In this study, we utilize a multi-scale approach to studying lanthanum adsorption on the (110) plane of tungsten. The energy of the system is described from density functional theory calculations within the framework of the cluster expansion method. It is found that including two-body figures up to the sixth nearest neighbor yielded a reasonable agreement with density functional theory calculations as evidenced by the reported cross validation score. The results indicate that the interaction between the adsorbate atoms in the adlayer is important and cannot be ignored. The parameterized cluster expansion expression is used in a lattice gas Monte Carlomore » simulation in the grand canonical ensemble at 773 K and the adsorption isotherm is recorded. Implications of the obtained results for the pyroprocessing application are discussed.« less

Density functional theory meta-GGA + U study of water incorporation in the metal-organic framework material Cu-BTC.

PubMed

Cockayne, Eric; Nelson, Eric B

2015-07-14

Water absorption in the metal-organic framework (MOF) material Cu-BTC, up to a concentration of 3.5 H2O per Cu ion, is studied via density functional theory at the meta-GGA + U level. The stable arrangements of water molecules show chains of hydrogen-bonded water molecules and a tendency to form closed cages at high concentration. Water clusters are stabilized primarily by a combination of water-water hydrogen bonding and Cu-water oxygen interactions. Stability is further enhanced by van der Waals interactions, electric field enhancement of water-water bonding, and hydrogen bonding of water to framework oxygens. We hypothesize that the tendency to form such stable clusters explains the particularly strong affinity of water to Cu-BTC and related MOFs with exposed metal sites.

Photoelectron spectroscopy and density functional calculations of CunBO2(OH)- (n = 1,2) clusters

NASA Astrophysics Data System (ADS)

Feng, Yuan; Hou, Gao-Lei; Xu, Hong-Guang; Zhang, Zeng-Guang; Zheng, Wei-Jun

2012-08-01

CunBO2(OH)- (n = 1, 2) clusters were studied by anion photoelectron spectroscopy and density functional calculations. From the experimental photoelectron spectra, the adiabatic detachment energy (ADE) and vertical detachment energy (VDE) of CuBO2(OH)- are determined to be 4.00 ± 0.08 and 4.26 ± 0.08 eV, and those of Cu2BO2(OH)- to be 2.30 ± 0.08 and 2.58 ± 0.08 eV. The structures of CunBO2(OH)- and their corresponding neutrals are assigned by comparison between theoretical calculations and experimental measurements. Both experiment and theory show that CuBO2(OH) can be viewed as a superhalogen, thus, confirmed that OH can behave like a halogen atom to participate in superhalogen formation.

Ion distribution in quaternary-ammonium-functionalized aromatic polymers: effects on the ionic clustering and conductivity of anion-exchange membranes.

PubMed

Weiber, E Annika; Jannasch, Patric

2014-09-01

A series of copoly(arylene ether sulfone)s that have precisely two, three, or four quaternary ammonium (QA) groups clustered directly on single phenylene rings along the backbone are studied as anion-exchange membranes. The copolymers are synthesized by condensation polymerizations that involve either di-, tri-, or tetramethylhydroquinone followed by virtually complete benzylic bromination using N-bromosuccinimide and quaternization with trimethylamine. This synthetic strategy allows excellent control and systematic variation of the local density and distribution of QA groups along the backbone. Small-angle X-ray scattering of these copolymers shows extensive ionic clustering, promoted by an increasing density of QA on the single phenylene rings. At an ion-exchange capacity (IEC) of 2.1 meq g(-1), the water uptake decreases with the increasing local density of QA groups. Moreover, at moderate IECs at 20 °C, the Br(-) conductivity of the densely functionalized copolymers is higher than a corresponding randomly functionalized polymer, despite the significantly higher water uptake of the latter. Thus, the location of multiple cations on single aromatic rings in the polymers facilitates the formation of a distinct percolating hydrophilic phase domain with a high ionic concentration to promote efficient anion transport, despite probable limitations by reduced ion dissociation. These findings imply a viable strategy to improve the performance of alkaline membrane fuel cells. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Density-induced suppression of the {alpha}-particle condensate in nuclear matter and the structure of {alpha}-cluster states in nuclei

DOE Office of Scientific and Technical Information (OSTI.GOV)

Funaki, Y.; Horiuchi, H.; International Institute for Advanced Studies, Kizugawa 619-0225

2008-06-15

At low densities, with decreasing temperatures, in symmetric nuclear matter {alpha} particles are formed, which eventually give raise to a quantum condensate with four-nucleon {alpha}-like correlations (quartetting). Starting with a model of {alpha} matter, where undistorted {alpha} particles interact via an effective interaction such as the Ali-Bodmer potential, the suppression of the condensate fraction at zero temperature with increasing density is considered. Using a Jastrow-Feenberg approach, it is found that the condensate fraction vanishes near saturation density. Additionally, the modification of the internal state of the {alpha} particle due to medium effects will further reduce the condensate. In finite systems,more » an enhancement of the S-state wave function of the center-of-mass orbital of {alpha}-particle motion is considered as the correspondence to the condensate. Wave functions have been constructed for self-conjugate 4n nuclei that describe the condensate state but are fully antisymmetrized on the nucleonic level. These condensate-like cluster wave functions have been successfully applied to describe properties of low-density states near the n{alpha} threshold. Comparison with orthogonality condition model calculations in {sup 12}C and {sup 16}O shows strong enhancement of the occupation of the S-state center-of-mass orbital of the {alpha} particles. This enhancement is decreasing if the baryon density increases, similar to the density-induced suppression of the condensate fraction in {alpha} matter. The ground states of {sup 12}C and {sup 16}O show no enhancement at all, thus a quartetting condensate cannot be formed at saturation densities.« less

Collective transport for active matter run-and-tumble disk systems on a traveling-wave substrate

DOE PAGES

Sándor, Csand; Libál, Andras; Reichhardt, Charles; ...

2017-01-17

Here, we examine numerically the transport of an assembly of active run-and-tumble disks interacting with a traveling-wave substrate. We show that as a function of substrate strength, wave speed, disk activity, and disk density, a variety of dynamical phases arise that are correlated with the structure and net flux of disks. We find that there is a sharp transition into a state in which the disks are only partially coupled to the substrate and form a phase-separated cluster state. This transition is associated with a drop in the net disk flux, and it can occur as a function of themore » substrate speed, maximum substrate force, disk run time, and disk density. Since variation of the disk activity parameters produces different disk drift rates for a fixed traveling-wave speed on the substrate, the system we consider could be used as an efficient method for active matter species separation. Within the cluster phase, we find that in some regimes the motion of the cluster center of mass is in the opposite direction to that of the traveling wave, while when the maximum substrate force is increased, the cluster drifts in the direction of the traveling wave. This suggests that swarming or clustering motion can serve as a method by which an active system can collectively move against an external drift.« less

VLT photometry in the Antlia cluster: the giant ellipticals NGC3258 and NGC3268 and their globular cluster systems

NASA Astrophysics Data System (ADS)

Bassino, Lilia P.; Richtler, Tom; Dirsch, Boris

2008-05-01

We present a deep Very Large Telescope (VLT) photometry in the regions surrounding the two dominant galaxies of the Antlia cluster, the giant ellipticals NGC3258 and NGC3268. We construct the luminosity functions of their globular cluster systems (GCSs) and determine their distances through the turn-over magnitudes. These distances are in good agreement with those obtained by the SBF method. There is some, but not conclusive, evidence that the distance to NGC3268 is larger by several Mpc. The GCSs colour distributions are bimodal but the brightest globular clusters (GCs) show a unimodal distribution with an intermediate colour peak. The radial distributions of both GCSs are well fitted by de Vaucouleurs laws up to 5arcmin. Red GCs present a steeper radial density profile than the blue GCs, and follow closely the galaxies' brightness profiles. Total GC populations are estimated to be about 6000 +/- 150GCs in NGC3258 and NGC4750 +/- 150GCs in NGC3268. We discuss the possible existence of GCs in a field located between the two giant galaxies (intracluster GCs). Their luminosity functions and number densities are consistent with the two GCSs overlapping in projection. Based on observations carried out at the European Southern Observatory, Paranal (Chile). Programme 71.B-0122(A). E-mail: lbassino@fcaglp.unlp.edu.ar (LPB); tom@mobydick.cfm.udec.cl (TR); borischacabuco@yahoo.co.uk (BD)

Conformational Properties, Spectroscopy and Structure of ISATIN-(WATER)_{n=1-3} Clusters

NASA Astrophysics Data System (ADS)

Singh, Milind K.; Upadhya, D. M.; Singh, Vipin B.

2009-06-01

The structure, stability and vibrational characteristics of Isatin-(Water)_n clusters with n=1=3 have been investigated using second order Moller-Plesset (MP2) perturbation tehory and Density Functional Theory (with B3LYP) methods employing the basis set 6-31+G(d). The vertical excitation energies for these complexes have been also computed using the time-dependent density functional theory. The three stable conformational isomers, each for Isatin-(Water)_1 and Isatin-(Water)_2 clusters were obtained. It is shown that in the most stable isomer of Isatin-(Water)_1 cluster hydrogen bond between amide hydrogen and oxygen of water is found stronger as compared to the H-bond in Indole-(Water)_1 cluster. For a particular position of complexation of water, between the carbonyl oxygen's, results an unusual increase in the dipole moment due to an electronic charge displacement from the N atom to the C atom of the neighboring carbonyl bond. This causes a large separation between the effective charges forming the dipole. The complexes involving this position of water are expected to show a small charge transfer character. The experimentally observed electronic absorption peaks are reasonably reproduced by the TD-DFT calculations and it is found that the longest wavelength absorption peak of isatin at 406 nm is significantly red shifted after addition of a water molecule.

Collective transport for active matter run-and-tumble disk systems on a traveling-wave substrate

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sándor, Csand; Libál, Andras; Reichhardt, Charles

Here, we examine numerically the transport of an assembly of active run-and-tumble disks interacting with a traveling-wave substrate. We show that as a function of substrate strength, wave speed, disk activity, and disk density, a variety of dynamical phases arise that are correlated with the structure and net flux of disks. We find that there is a sharp transition into a state in which the disks are only partially coupled to the substrate and form a phase-separated cluster state. This transition is associated with a drop in the net disk flux, and it can occur as a function of themore » substrate speed, maximum substrate force, disk run time, and disk density. Since variation of the disk activity parameters produces different disk drift rates for a fixed traveling-wave speed on the substrate, the system we consider could be used as an efficient method for active matter species separation. Within the cluster phase, we find that in some regimes the motion of the cluster center of mass is in the opposite direction to that of the traveling wave, while when the maximum substrate force is increased, the cluster drifts in the direction of the traveling wave. This suggests that swarming or clustering motion can serve as a method by which an active system can collectively move against an external drift.« less

The insignificant evolution of the richness-mass relation of galaxy clusters

NASA Astrophysics Data System (ADS)

Andreon, S.; Congdon, P.

2014-08-01

We analysed the richness-mass scaling of 23 very massive clusters at 0.15 < z < 0.55 with homogenously measured weak-lensing masses and richnesses within a fixed aperture of 0.5 Mpc radius. We found that the richness-mass scaling is very tight (the scatter is <0.09 dex with 90% probability) and independent of cluster evolutionary status and morphology. This implies a close association between infall and evolution of dark matter and galaxies in the central region of clusters. We also found that the evolution of the richness-mass intercept is minor at most, and, given the minor mass evolution across the studied redshift range, the richness evolution of individual massive clusters also turns out to be very small. Finally, it was paramount to account for the cluster mass function and the selection function. Ignoring them would lead to larger biases than the (otherwise quoted) errors. Our study benefits from: a) weak-lensing masses instead of proxy-based masses thereby removing the ambiguity between a real trend and one induced by an accounted evolution of the used mass proxy; b) the use of projected masses that simplify the statistical analysis thereby not requiring consideration of the unknown covariance induced by the cluster orientation/triaxiality; c) the use of aperture masses as they are free of the pseudo-evolution of mass definitions anchored to the evolving density of the Universe; d) a proper accounting of the sample selection function and of the Malmquist-like effect induced by the cluster mass function; e) cosmological simulations for the computation of the cluster mass function, its evolution, and the mass growth of each individual cluster.

Flow over gravel beds with clusters

NASA Astrophysics Data System (ADS)

Little, M.; Venditti, J. G.

2014-12-01

The structure of a gravel bed has been shown to alter the entrainment threshold. Structures such as clusters, reticulate stone cells and other discrete structures lock grains together, making it more difficult for them to be mobilized. These structures also generate form drag, reducing the shear stress available for mobilization. Form drag over gravel beds is often assumed to be negligible, but this assumption is not well supported. Here, we explore how cluster density and arrangement affect flow resistance and the flow structure over a fixed gravel bed in a flume experiment. Cluster density was varied from 6 to 68.3 clusters per square meter which corresponds to areal bed coverages of 2 to 17%. We used regular, irregular and random arrangements of the clusters. Our results show that flow resistance over a planar gravel bed initially declines, then increases with flow depth. The addition of clusters increases flow resistance, but the effect is dependent on cluster density, flow depth and arrangement. At the highest density, clusters can increase flow resistance as by as much as 8 times when compared to flat planar bed with no grain-related form drag. Spatially resolved observations of flow over the clusters indicate that a well-defined wake forms in the lee of each cluster. At low cluster density, the wakes are isolated and weak. As cluster density increases, the wakes become stronger. At the highest density, the wakes interact and the within cluster flow field detaches from the overlying flow. This generates a distinct shear layer at the height of the clusters. In spite of this change in the flow field at high density, our results suggest that flow resistance simply increases with cluster density. Our results suggest that the form drag associated with a gravel bed can be substantial and that it depends on the arrangement of the grains on the bed.

A Fast Density-Based Clustering Algorithm for Real-Time Internet of Things Stream

PubMed Central

Ying Wah, Teh

2014-01-01

Data streams are continuously generated over time from Internet of Things (IoT) devices. The faster all of this data is analyzed, its hidden trends and patterns discovered, and new strategies created, the faster action can be taken, creating greater value for organizations. Density-based method is a prominent class in clustering data streams. It has the ability to detect arbitrary shape clusters, to handle outlier, and it does not need the number of clusters in advance. Therefore, density-based clustering algorithm is a proper choice for clustering IoT streams. Recently, several density-based algorithms have been proposed for clustering data streams. However, density-based clustering in limited time is still a challenging issue. In this paper, we propose a density-based clustering algorithm for IoT streams. The method has fast processing time to be applicable in real-time application of IoT devices. Experimental results show that the proposed approach obtains high quality results with low computation time on real and synthetic datasets. PMID:25110753

A fast density-based clustering algorithm for real-time Internet of Things stream.

PubMed

Amini, Amineh; Saboohi, Hadi; Wah, Teh Ying; Herawan, Tutut

2014-01-01

Data streams are continuously generated over time from Internet of Things (IoT) devices. The faster all of this data is analyzed, its hidden trends and patterns discovered, and new strategies created, the faster action can be taken, creating greater value for organizations. Density-based method is a prominent class in clustering data streams. It has the ability to detect arbitrary shape clusters, to handle outlier, and it does not need the number of clusters in advance. Therefore, density-based clustering algorithm is a proper choice for clustering IoT streams. Recently, several density-based algorithms have been proposed for clustering data streams. However, density-based clustering in limited time is still a challenging issue. In this paper, we propose a density-based clustering algorithm for IoT streams. The method has fast processing time to be applicable in real-time application of IoT devices. Experimental results show that the proposed approach obtains high quality results with low computation time on real and synthetic datasets.

From cluster structures to nuclear molecules: The role of nodal structure of the single-particle wave functions

NASA Astrophysics Data System (ADS)

Afanasjev, A. V.; Abusara, H.

2018-02-01

The nodal structure of the density distributions of the single-particle states occupied in rod-shaped, hyper- and megadeformed structures of nonrotating and rotating N ˜Z nuclei has been investigated in detail. The single-particle states with the Nilsson quantum numbers of the [N N 0 ]1 /2 (with N from 0 to 5) and [N ,N -1 ,1 ]Ω (with N from 1 to 3 and Ω =1 /2 , 3/2) types are considered. These states are building blocks of extremely deformed shapes in the nuclei with mass numbers A ≤50 . Because of (near) axial symmetry and large elongation of such structures, the wave functions of the single-particle states occupied are dominated by a single basis state in cylindrical basis. This basis state defines the nodal structure of the single-particle density distribution. The nodal structure of the single-particle density distributions allows us to understand in a relatively simple way the necessary conditions for α clusterization and the suppression of the α clusterization with the increase of mass number. It also explains in a natural way the coexistence of ellipsoidal mean-field-type structures and nuclear molecules at similar excitation energies and the features of particle-hole excitations connecting these two types of the structures. Our analysis of the nodal structure of the single-particle density distributions does not support the existence of quantum liquid phase for the deformations and nuclei under study.

Structural transition of (InSb)n clusters at n = 6-10

NASA Astrophysics Data System (ADS)

Lu, Qi Liang; Luo, Qi Quan; Huang, Shou Guo; Li, Yi De

2016-10-01

An optimization strategy combining global semi-empirical quantum mechanical search with all-electron density functional theory was adopted to determine the lowest energy structure of (InSb)n clusters with n = 6-10. A new structural growth pattern of the clusters was observed. The lowest energy structures of (InSb)6 and (InSb)8 were different from that of previously reported results. Competition existed between core-shell and cage-like structures of (InSb)8. The structural transition of (InSb)n clusters occurred at size n = 8-9. For (InSb)9 and (InSb)10 clusters, core-shell structure were more energetically favorable than the cage. The corresponding electronic properties were investigated.

Electronic structure and optical properties of the thiolate-protected Au28(SMe)20 cluster.

PubMed

Knoppe, Stefan; Malola, Sami; Lehtovaara, Lauri; Bürgi, Thomas; Häkkinen, Hannu

2013-10-10

The recently reported crystal structure of the Au28(TBBT)20 cluster (TBBT: p-tert-butylbenzenethiolate) is analyzed with (time-dependent) density functional theory (TD-DFT). Bader charge analysis reveals a novel trimeric Au3(SR)4 binding motif. The cluster can be formulated as Au14(Au2(SR)3)4(Au3(SR)4)2. The electronic structure of the Au14(6+) core and the ligand-protected cluster were analyzed, and their stability can be explained by formation of distorted eight-electron superatoms. Optical absorption and circular dichroism (CD) spectra were calculated and compared to the experiment. Assignment of handedness of the intrinsically chiral cluster is possible.

Competition between surface chemisorption and cage formation in Fe12O12 clusters

NASA Astrophysics Data System (ADS)

Gutsev, G. L.; Weatherford, C. A.; Jena, P.; Johnson, E.; Ramachandran, B. R.

2013-01-01

The electronic and geometrical structures of the clusters composed of 12 iron and 12 oxygen atoms are obtained using all-electron density functional theory. It is found that the states with geometrical structures corresponding to oxygen chemisorbed on the ground-state Fe12 cluster surface (Fe12O12) are close in total energy to the states whose geometrical configurations are hollow cages (FeO)12. The lowest total energy state is the ferrimagnetic triplet state of Fe12O12. A ferrimagnetic nonet state of (FeO)12 is only marginally higher in total energy. The clusters are rich in nearly degenerate isomers. Oxygen adsorption dramatically quenches the spin of Fe12 clusters.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Henzler, Katja; Fetisov, Evgenii O.; Galib, Mirza

We will present a description of nucleation phenomena in the condensed phase that takes into account non-ideal solution effects associated with cluster-cluster interaction. To do this we employ aggregation-volume bias Monte Carlo simulation, making the estimation of free-energy of large pre-critical clusters of sizes 10-20 tractable. We will compare and contrast empirical potential and electronic structure (e.g. Density functional theory) based descriptions of molecular interaction associated with the nucleation of CaCO3, highlighting free-energy trends and qualitative differences in populations of pre-critical clusters as a function of supersaturation. The influence of how the precise local interaction influences the non-ideal solution behaviormore » on the nucleation and growth processes will be highlighted. This research was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences.« less

Transitioning NWChem to the Next Generation of Manycore Machines

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bylaska, Eric J.; Apra, Edoardo; Kowalski, Karol

The NorthWest Chemistry (NWChem) modeling software is a popular molecular chemistry simulation software that was designed from the start to work on massively parallel processing supercomputers[6, 28, 49]. It contains an umbrella of modules that today includes Self Consistent Field (SCF), second order Mller-Plesset perturbation theory (MP2), Coupled Cluster, multi-conguration selfconsistent eld (MCSCF), selected conguration interaction (CI), tensor contraction engine (TCE) many body methods, density functional theory (DFT), time-dependent density functional theory (TDDFT), real time time-dependent density functional theory, pseudopotential plane-wave density functional theory (PSPW), band structure (BAND), ab initio molecular dynamics, Car-Parrinello molecular dynamics, classical molecular dynamics (MD), QM/MM,more » AIMD/MM, GIAO NMR, COSMO, COSMO-SMD, and RISM solvation models, free energy simulations, reaction path optimization, parallel in time, among other capabilities[ 22]. Moreover new capabilities continue to be added with each new release.« less

Clustering the Orion B giant molecular cloud based on its molecular emission.

PubMed

Bron, Emeric; Daudon, Chloé; Pety, Jérôme; Levrier, François; Gerin, Maryvonne; Gratier, Pierre; Orkisz, Jan H; Guzman, Viviana; Bardeau, Sébastien; Goicoechea, Javier R; Liszt, Harvey; Öberg, Karin; Peretto, Nicolas; Sievers, Albrecht; Tremblin, Pascal

2018-02-01

Previous attempts at segmenting molecular line maps of molecular clouds have focused on using position-position-velocity data cubes of a single molecular line to separate the spatial components of the cloud. In contrast, wide field spectral imaging over a large spectral bandwidth in the (sub)mm domain now allows one to combine multiple molecular tracers to understand the different physical and chemical phases that constitute giant molecular clouds (GMCs). We aim at using multiple tracers (sensitive to different physical processes and conditions) to segment a molecular cloud into physically/chemically similar regions (rather than spatially connected components), thus disentangling the different physical/chemical phases present in the cloud. We use a machine learning clustering method, namely the Meanshift algorithm, to cluster pixels with similar molecular emission, ignoring spatial information. Clusters are defined around each maximum of the multidimensional Probability Density Function (PDF) of the line integrated intensities. Simple radiative transfer models were used to interpret the astrophysical information uncovered by the clustering analysis. A clustering analysis based only on the J = 1 - 0 lines of three isotopologues of CO proves suffcient to reveal distinct density/column density regimes ( n H ~ 100 cm -3 , ~ 500 cm -3 , and > 1000 cm -3 ), closely related to the usual definitions of diffuse, translucent and high-column-density regions. Adding two UV-sensitive tracers, the J = 1 - 0 line of HCO + and the N = 1 - 0 line of CN, allows us to distinguish two clearly distinct chemical regimes, characteristic of UV-illuminated and UV-shielded gas. The UV-illuminated regime shows overbright HCO + and CN emission, which we relate to a photochemical enrichment effect. We also find a tail of high CN/HCO + intensity ratio in UV-illuminated regions. Finer distinctions in density classes ( n H ~ 7 × 10 3 cm -3 ~ 4 × 10 4 cm -3 ) for the densest regions are also identified, likely related to the higher critical density of the CN and HCO + (1 - 0) lines. These distinctions are only possible because the high-density regions are spatially resolved. Molecules are versatile tracers of GMCs because their line intensities bear the signature of the physics and chemistry at play in the gas. The association of simultaneous multi-line, wide-field mapping and powerful machine learning methods such as the Meanshift clustering algorithm reveals how to decode the complex information available in these molecular tracers.

Electronic effects on melting: Comparison of aluminum cluster anions and cations

NASA Astrophysics Data System (ADS)

Starace, Anne K.; Neal, Colleen M.; Cao, Baopeng; Jarrold, Martin F.; Aguado, Andrés; López, José M.

2009-07-01

Heat capacities have been measured as a function of temperature for aluminum cluster anions with 35-70 atoms. Melting temperatures and latent heats are determined from peaks in the heat capacities; cohesive energies are obtained for solid clusters from the latent heats and dissociation energies determined for liquid clusters. The melting temperatures, latent heats, and cohesive energies for the aluminum cluster anions are compared to previous measurements for the corresponding cations. Density functional theory calculations have been performed to identify the global minimum energy geometries for the cluster anions. The lowest energy geometries fall into four main families: distorted decahedral fragments, fcc fragments, fcc fragments with stacking faults, and "disordered" roughly spherical structures. The comparison of the cohesive energies for the lowest energy geometries with the measured values allows us to interpret the size variation in the latent heats. Both geometric and electronic shell closings contribute to the variations in the cohesive energies (and latent heats), but structural changes appear to be mainly responsible for the large variations in the melting temperatures with cluster size. The significant charge dependence of the latent heats found for some cluster sizes indicates that the electronic structure can change substantially when the cluster melts.

Combinations of coupled cluster, density functionals, and the random phase approximation for describing static and dynamic correlation, and van der Waals interactions

NASA Astrophysics Data System (ADS)

Garza, Alejandro J.; Bulik, Ireneusz W.; Alencar, Ana G. Sousa; Sun, Jianwei; Perdew, John P.; Scuseria, Gustavo E.

2016-04-01

Contrary to standard coupled cluster doubles (CCD) and Brueckner doubles (BD), singlet-paired analogues of CCD and BD (denoted here as CCD0 and BD0) do not break down when static correlation is present, but neglect substantial amounts of dynamic correlation. In fact, CCD0 and BD0 do not account for any contributions from multielectron excitations involving only same-spin electrons at all. We exploit this feature to add - without introducing double counting, self-interaction, or increase in cost - the missing correlation to these methods via meta-GGA (generalised gradient approximation) density functionals (Tao-Perdew-Staroverov-Scuseria and strongly constrained and appropriately normed). Furthermore, we improve upon these CCD0+DFT blends by invoking range separation: the short- and long-range correlations absent in CCD0/BD0 are evaluated with density functional theory and the direct random phase approximation, respectively. This corrects the description of long-range van der Waals forces. Comprehensive benchmarking shows that the combinations presented here are very accurate for weakly correlated systems, while also providing a reasonable description of strongly correlated problems without resorting to symmetry breaking.

Tidal radii of the globular clusters M 5, M 12, M 13, M 15, M 53, NGC 5053 and NGC 5466 from automated star counts.

NASA Astrophysics Data System (ADS)

Lehmann, I.; Scholz, R.-D.

1997-04-01

We present new tidal radii for seven Galactic globular clusters using the method of automated star counts on Schmidt plates of the Tautenburg, Palomar and UK telescopes. The plates were fully scanned with the APM system in Cambridge (UK). Special account was given to a reliable background subtraction and the correction of crowding effects in the central cluster region. For the latter we used a new kind of crowding correction based on a statistical approach to the distribution of stellar images and the luminosity function of the cluster stars in the uncrowded area. The star counts were correlated with surface brightness profiles of different authors to obtain complete projected density profiles of the globular clusters. Fitting an empirical density law (King 1962) we derived the following structural parameters: tidal radius r_t_, core radius r_c_ and concentration parameter c. In the cases of NGC 5466, M 5, M 12, M 13 and M 15 we found an indication for a tidal tail around these objects (cf. Grillmair et al. 1995).

VizieR Online Data Catalog: Tidal radii of 7 globular clusters (Lehmann+ 1997)

NASA Astrophysics Data System (ADS)

Lehmann, I.; Scholz, R.-D.

1998-02-01

We present new tidal radii for seven Galactic globular clusters using the method of automated star counts on Schmidt plates of the Tautenburg, Palomar and UK telescopes. The plates were fully scanned with the APM system in Cambridge (UK). Special account was given to a reliable background subtraction and the correction of crowding effects in the central cluster region. For the latter we used a new kind of crowding correction based on a statistical approach to the distribution of stellar images and the luminosity function of the cluster stars in the uncrowded area. The star counts were correlated with surface brightness profiles of different authors to obtain complete projected density profiles of the globular clusters. Fitting an empirical density law (King 1962AJ.....67..471K) we derived the following structural parameters: tidal radius rt, core radius rc and concentration parameter c. In the cases of NGC 5466, M 5, M 12, M 13 and M 15 we found an indication for a tidal tail around these objects (cf. Grillmair et al., 1995AJ....109.2553G). (1 data file).

Impact-parameter dependence of the energy loss of fast molecular clusters in hydrogen

NASA Astrophysics Data System (ADS)

Fadanelli, R. C.; Grande, P. L.; Schiwietz, G.

2008-03-01

The electronic energy loss of molecular clusters as a function of impact parameter is far less understood than atomic energy losses. For instance, there are no analytical expressions for the energy loss as a function of impact parameter for cluster ions. In this work, we describe two procedures to evaluate the combined energy loss of molecules: Ab initio calculations within the semiclassical approximation and the coupled-channels method using atomic orbitals; and simplified models for the electronic cluster energy loss as a function of the impact parameter, namely the molecular perturbative convolution approximation (MPCA, an extension of the corresponding atomic model PCA) and the molecular unitary convolution approximation (MUCA, a molecular extension of the previous unitary convolution approximation UCA). In this work, an improved ansatz for MPCA is proposed, extending its validity for very compact clusters. For the simplified models, the physical inputs are the oscillators strengths of the target atoms and the target-electron density. The results from these models applied to an atomic hydrogen target yield remarkable agreement with their corresponding ab initio counterparts for different angles between cluster axis and velocity direction at specific energies of 150 and 300 keV/u.

The hELENa project - I. Stellar populations of early-type galaxies linked with local environment and galaxy mass

NASA Astrophysics Data System (ADS)

Sybilska, A.; Lisker, T.; Kuntschner, H.; Vazdekis, A.; van de Ven, G.; Peletier, R.; Falcón-Barroso, J.; Vijayaraghavan, R.; Janz, J.

2017-09-01

We present the first in a series of papers in The role of Environment in shaping Low-mass Early-type Nearby galaxies (hELENa) project. In this paper, we combine our sample of 20 low-mass early types (dEs) with 258 massive early types (ETGs) from the ATLAS3D survey - all observed with the SAURON integral field unit - to investigate early-type galaxies' stellar population scaling relations and the dependence of the population properties on local environment, extended to the low-σ regime of dEs. The ages in our sample show more scatter at lower σ values, indicative of less massive galaxies being affected by the environment to a higher degree. The shape of the age-σ relations for cluster versus non-cluster galaxies suggests that cluster environment speeds up the placing of galaxies on the red sequence. While the scaling relations are tighter for cluster than for the field/group objects, we find no evidence for a difference in average population characteristics of the two samples. We investigate the properties of our sample in the Virgo cluster as a function of number density (rather than simple clustrocentric distance) and find that dE ages correlate with the local density such that galaxies in regions of lower density are younger, likely because they are later arrivals to the cluster or have experienced less pre-processing in groups, and consequently used up their gas reservoir more recently. Overall, dE properties correlate more strongly with density than those of massive ETGs, which was expected as less massive galaxies are more susceptible to external influences.

Use of density functional theory method to calculate structures of neutral carbon clusters C{sub n} (3 ≤ n ≤ 24) and study their variability of structural forms

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yen, T. W.; Lai, S. K., E-mail: sklai@coll.phy.ncu.edu.tw

2015-02-28

In this work, we present modifications to the well-known basin hopping (BH) optimization algorithm [D. J. Wales and J. P. Doye, J. Phys. Chem. A 101, 5111 (1997)] by incorporating in it the unique and specific nature of interactions among valence electrons and ions in carbon atoms through calculating the cluster’s total energy by the density functional tight-binding (DFTB) theory, using it to find the lowest energy structures of carbon clusters and, from these optimized atomic and electronic structures, studying their varied forms of topological transitions, which include a linear chain, a monocyclic to a polycyclic ring, and a fullerene/cage-likemore » geometry. In this modified BH (MBH) algorithm, we define a spatial volume within which the cluster’s lowest energy structure is to be searched, and introduce in addition a cut-and-splice genetic operator to increase the searching performance of the energy minimum than the original BH technique. The present MBH/DFTB algorithm is, therefore, characteristically distinguishable from the original BH technique commonly applied to nonmetallic and metallic clusters, technically more thorough and natural in describing the intricate couplings between valence electrons and ions in a carbon cluster, and thus theoretically sound in putting these two charged components on an equal footing. The proposed modified minimization algorithm should be more appropriate, accurate, and precise in the description of a carbon cluster. We evaluate the present algorithm, its energy-minimum searching in particular, by its optimization robustness. Specifically, we first check the MBH/DFTB technique for two representative carbon clusters of larger size, i.e., C{sub 60} and C{sub 72} against the popular cut-and-splice approach [D. M. Deaven and K. M. Ho, Phys. Rev. Lett. 75, 288 (1995)] that normally is combined with the genetic algorithm method for finding the cluster’s energy minimum, before employing it to investigate carbon clusters in the size range C{sub 3}-C{sub 24} studying their topological transitions. An effort was also made to compare our MBH/DFTB and its re-optimized results carried out by full density functional theory (DFT) calculations with some early DFT-based studies.« less

Order statistics applied to the most massive and most distant galaxy clusters

NASA Astrophysics Data System (ADS)

Waizmann, J.-C.; Ettori, S.; Bartelmann, M.

2013-06-01

In this work, we present an analytic framework for calculating the individual and joint distributions of the nth most massive or nth highest redshift galaxy cluster for a given survey characteristic allowing us to formulate Λ cold dark matter (ΛCDM) exclusion criteria. We show that the cumulative distribution functions steepen with increasing order, giving them a higher constraining power with respect to the extreme value statistics. Additionally, we find that the order statistics in mass (being dominated by clusters at lower redshifts) is sensitive to the matter density and the normalization of the matter fluctuations, whereas the order statistics in redshift is particularly sensitive to the geometric evolution of the Universe. For a fixed cosmology, both order statistics are efficient probes of the functional shape of the mass function at the high-mass end. To allow a quick assessment of both order statistics, we provide fits as a function of the survey area that allow percentile estimation with an accuracy better than 2 per cent. Furthermore, we discuss the joint distributions in the two-dimensional case and find that for the combination of the largest and the second largest observation, it is most likely to find them to be realized with similar values with a broadly peaked distribution. When combining the largest observation with higher orders, it is more likely to find a larger gap between the observations and when combining higher orders in general, the joint probability density function peaks more strongly. Having introduced the theory, we apply the order statistical analysis to the Southpole Telescope (SPT) massive cluster sample and metacatalogue of X-ray detected clusters of galaxies catalogue and find that the 10 most massive clusters in the sample are consistent with ΛCDM and the Tinker mass function. For the order statistics in redshift, we find a discrepancy between the data and the theoretical distributions, which could in principle indicate a deviation from the standard cosmology. However, we attribute this deviation to the uncertainty in the modelling of the SPT survey selection function. In turn, by assuming the ΛCDM reference cosmology, order statistics can also be utilized for consistency checks of the completeness of the observed sample and of the modelling of the survey selection function.

Divergent electronic structures of isoelectronic metalloclusters: tungsten(II) halides and rhenium(III) chalcogenide halides.

PubMed

Gray, Thomas G

2009-03-02

Same but different: DFT calculations on hexanuclear tungsten(II) halide clusters [W(6)X(8)X'(6)](2-) (X, X'=Cl, Br, I) indicate a breakdown in the isoelectronic analogy between themselves and the isostructural rhenium(III) chalcogenide clusters [Re(6)S(8)X(6)](4-) (see figure).The hexanuclear tungsten(II) halide clusters and the sulfido-halide clusters of rhenium(III) are subsets of a broad system of 24-electron metal-metal bonded assemblies that share a common structure. Tungsten(II) halide clusters and rhenium(III) sulfide clusters luminesce from triplet excited states upon ultraviolet or visible excitation; emission from both cluster series has been extensively characterized elsewhere. Reported here are density-functional theory studies of the nine permutations of [W(6)X(8)X'(6)](2-) (X, X'=Cl, Br, I). Ground-state properties including geometries, harmonic vibrational frequencies, and orbital energy-level diagrams, have been calculated. Comparison is made to the sulfide clusters of rhenium(III), of which [Re(6)S(8)Cl(6)](4-) is representative. [W(6)X(8)X'(6)](2-) and [Re(6)S(8)Cl(6)](4-) possess disparate electronic structures owing to the greater covalency of the metal-sulfur bond and hence of the [Re(6)S(8)](2+) core. Low-lying virtual orbitals are raised in energy in [Re(6)S(8)Cl(6)](4-) with the result that the LUMO+7 (or LUMO+8 in some cases) of tungsten(II) halide clusters is the LUMO of [Re(6)S(8)Cl(6)](4-) species. An inversion of the HOMO and HOMO-1 between the two cluster series also occurs. Time-dependent density-functional calculations using asymptotically correct functionals do not recapture the experimentally observed periodic trend in [W(6)X(14)](2-) luminescence (E(em) increasing in the order [W(6)Cl(14)](2-) < [W(6)Br(14)](2-) < [W(6)I(14)](2-)), predicting instead that emission energies decrease with incorporation of the heavier halides. This circumstance is either a gross failure of the time-dependent formalism of DFT or it indicates extensive multistate emission in [W(6)X(8)X'(6)](2-) clusters. The inapplicability of isoelectronic analogies between clusters of Group 6 and Group 7 is emphasized.

Structural, electronic and magnetic properties of Ti n Mo ( n = 1 - 7) clusters

NASA Astrophysics Data System (ADS)

Zhang, Ge; Zhai, Zhongyuan; Sheng, Yong

2017-04-01

The ground state structures of TinMo and Tin+1 (n = 1 - 7) clusters and their structural, electronic and magnetic properties are investigated with the density functional method at B3LYP/LanL2DZ level. One Mo atom substituted Tin+1 structure is the dominant growth pattern, and the TinMo clusters exhibit enhanced structural stabilities according to the averaged binding energies. The electronic properties are also discussed by investigating chemical hardness and HOMO-LUMO energy gap. The results reveal that Ti3Mo and Ti5Mo keep higher chemical stabilities when compared with the other clusters. For all the studied clusters, the Mo atoms always get electrons from Ti atoms and present negative charges. Moreover, the doping of Mo in the bare titanium clusters can alter the magnetic moments of them. Ti3Mo and Ti5Mo show relatively large total magnetic moments, which may be related to the presence of exchange splitting behavior in their densities of states. Supplementary material in the form of one pdf file available from the Journal web page at http://https://doi.org/10.1140/epjd/e2017-70589-8

The adsorption of Run (n = 1-4) on γ-Al2O3 Surface: A DFT study

NASA Astrophysics Data System (ADS)

Liu, Zhe; Guo, Yafei; Chen, Yu; Shen, Rong

2018-05-01

The density functional theory (DFT) was adopted to study the adsorption and growth of Run (n = 1-4) clusters on γ-Al2O3 surface, which is of great significances for the design of many important catalysts, especially for carbon dioxide methanation. It is found that both the Rusbnd Ru bond length and adsorption energy Eads of Ru clusters with the surface increase with the Run clusters increasing. The growth ability of the supported Run cluster is weaker than the gas phase Run clusters through comparing their respective growth process, which ascribes to the stabilization of γ-Al2O3 support. An interesting discovery is that the basin structure was supposed to be the most favorable adsorption geometry for Run clusters. Additionally, the distances between Ru atoms in the adsorbed clusters are longer than that in their isolated counterparts. Bader charge analysis was conducted for the most stable configurations of Run (n = 1-4) clusters on γ-Al2O3 surface as well. And the results suggest that Run (n = 1-4) clusters serve as the electron donators. The result of projected density of states (PDOS) shows that strong adsorption of Ru atom on the γ-Al2O3 surface correlates with strong interaction between d orbital of Ru atom and p orbital of Al or O atom of the Al2O3 support.

First principles study of structural, electronic and magnetic properties of SnGe n (0, ±1) ( n = 1–17) clusters

NASA Astrophysics Data System (ADS)

Djaadi, Soumaia; Eddine Aiadi, Kamal; Mahtout, Sofiane

2018-04-01

The structures, relative stability and magnetic properties of pure Ge n +1, neutral cationic and anionic SnGe n (n = 1–17) clusters have been investigated by using the first principles density functional theory implemented in SIESTA packages. We find that with the increasing of cluster size, the Ge n +1 and SnGe n (0, ±1) clusters tend to adopt compact structures. It has been also found that the Sn atom occupied a peripheral position for SnGe n clusters when n < 12 and occupied a core position for n > 12. The structural and electronic properties such as optimized geometries, fragmentation energy, binding energy per atom, HOMO–LUMO gaps and second-order differences in energy of the pure Ge n +1 and SnGe n clusters in their ground state are calculated and analyzed. All isomers of neutral SnGe n clusters are generally nonmagnetic except for n = 1 and 4, where the total spin magnetic moments is 2μ b. The total (DOS) and partial density of states of these clusters have been calculated to understand the origin of peculiar magnetic properties. The cluster size dependence of vertical ionization potentials, vertical electronic affinities, chemical hardness, adiabatic electron affinities and adiabatic ionization potentials have been calculated and discussed.

The Correlation Function of Galaxy Clusters and Detection of Baryon Acoustic Oscillations

NASA Astrophysics Data System (ADS)

Hong, T.; Han, J. L.; Wen, Z. L.; Sun, L.; Zhan, H.

2012-04-01

We calculate the correlation function of 13,904 galaxy clusters of z <= 0.4 selected from the cluster catalog of Wen et al. The correlation function can be fitted with a power-law model ξ(r) = (r/R 0)-γ on the scales of 10 h -1 Mpc <= r <= 50 h -1 Mpc, with a larger correlation length of R 0 = 18.84 ± 0.27 h -1 Mpc for clusters with a richness of R >= 15 and a smaller length of R 0 = 16.15 ± 0.13 h -1 Mpc for clusters with a richness of R >= 5. The power-law index of γ = 2.1 is found to be almost the same for all cluster subsamples. A pronounced baryon acoustic oscillations (BAO) peak is detected at r ~ 110 h -1 Mpc with a significance of ~1.9σ. By analyzing the correlation function in the range of 20 h -1 Mpc <= r <= 200 h -1 Mpc, we find that the constraints on distance parameters are Dv (zm = 0.276) = 1077 ± 55(1σ) Mpc and h = 0.73 ± 0.039(1σ), which are consistent with the cosmology derived from Wilkinson Microwave Anisotropy Probe (WMAP) seven-year data. However, the BAO signal from the cluster sample is stronger than expected and leads to a rather low matter density Ω m h 2 = 0.093 ± 0.0077(1σ), which deviates from the WMAP7 result by more than 3σ. The correlation function of the GMBCG cluster sample is also calculated and our detection of the BAO feature is confirmed.

Density-based clustering of small peptide conformations sampled from a molecular dynamics simulation.

PubMed

Kim, Minkyoung; Choi, Seung-Hoon; Kim, Junhyoung; Choi, Kihang; Shin, Jae-Min; Kang, Sang-Kee; Choi, Yun-Jaie; Jung, Dong Hyun

2009-11-01

This study describes the application of a density-based algorithm to clustering small peptide conformations after a molecular dynamics simulation. We propose a clustering method for small peptide conformations that enables adjacent clusters to be separated more clearly on the basis of neighbor density. Neighbor density means the number of neighboring conformations, so if a conformation has too few neighboring conformations, then it is considered as noise or an outlier and is excluded from the list of cluster members. With this approach, we can easily identify clusters in which the members are densely crowded in the conformational space, and we can safely avoid misclustering individual clusters linked by noise or outliers. Consideration of neighbor density significantly improves the efficiency of clustering of small peptide conformations sampled from molecular dynamics simulations and can be used for predicting peptide structures.

Probing Leader Cells in Endothelial Collective Migration by Plasma Lithography Geometric Confinement

PubMed Central

Yang, Yongliang; Jamilpour, Nima; Yao, Baoyin; Dean, Zachary S.; Riahi, Reza; Wong, Pak Kin

2016-01-01

When blood vessels are injured, leader cells emerge in the endothelium to heal the wound and restore the vasculature integrity. The characteristics of leader cells during endothelial collective migration under diverse physiological conditions, however, are poorly understood. Here we investigate the regulation and function of endothelial leader cells by plasma lithography geometric confinement generated. Endothelial leader cells display an aggressive phenotype, connect to follower cells via peripheral actin cables and discontinuous adherens junctions, and lead migrating clusters near the leading edge. Time-lapse microscopy, immunostaining, and particle image velocimetry reveal that the density of leader cells and the speed of migrating clusters are tightly regulated in a wide range of geometric patterns. By challenging the cells with converging, diverging and competing patterns, we show that the density of leader cells correlates with the size and coherence of the migrating clusters. Collectively, our data provide evidence that leader cells control endothelial collective migration by regualting the migrating clusters. PMID:26936382

Engineering Redox Potential of Lithium Clusters for Electrode Material in Lithium-Ion Batteries

DOE PAGES

Kushwaha, Anoop Kumar; Sahoo, Mihir Ranjan; Nanda, Jagjit; ...

2017-07-01

Low negative electrode potential and high reactivity makes lithium (Li) ideal candidate for obtaining highest possible energy density among other materials. Here, we show a novel route with which the overall electrode potential could significantly be enhanced through selection of cluster size. In using first principles density functional theory and continuum dielectric model, we studied free energy and redox potential as well as investigated relative stability of Li n (n ≤ 8) clusters in both gas phase and solution. We found that Li 3 has the lowest negative redox potential (thereby highest overall electrode potential) suggesting that cluster based approachmore » could provide a novel way of engineering the next generation battery technology. The microscopic origin of Li 3 cluster’s superior performance is related to two major factors: gas phase ionization and difference between solvation free energy for neutral and positive ion. Taken together, our study provides insight into the engineering of redox potential in battery and could stimulate further work in this direction.« less

Engineering Redox Potential of Lithium Clusters for Electrode Material in Lithium-Ion Batteries

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kushwaha, Anoop Kumar; Sahoo, Mihir Ranjan; Nanda, Jagjit

Low negative electrode potential and high reactivity makes lithium (Li) ideal candidate for obtaining highest possible energy density among other materials. Here, we show a novel route with which the overall electrode potential could significantly be enhanced through selection of cluster size. In using first principles density functional theory and continuum dielectric model, we studied free energy and redox potential as well as investigated relative stability of Li n (n ≤ 8) clusters in both gas phase and solution. We found that Li 3 has the lowest negative redox potential (thereby highest overall electrode potential) suggesting that cluster based approachmore » could provide a novel way of engineering the next generation battery technology. The microscopic origin of Li 3 cluster’s superior performance is related to two major factors: gas phase ionization and difference between solvation free energy for neutral and positive ion. Taken together, our study provides insight into the engineering of redox potential in battery and could stimulate further work in this direction.« less

Probing Leader Cells in Endothelial Collective Migration by Plasma Lithography Geometric Confinement.

PubMed

Yang, Yongliang; Jamilpour, Nima; Yao, Baoyin; Dean, Zachary S; Riahi, Reza; Wong, Pak Kin

2016-03-03

When blood vessels are injured, leader cells emerge in the endothelium to heal the wound and restore the vasculature integrity. The characteristics of leader cells during endothelial collective migration under diverse physiological conditions, however, are poorly understood. Here we investigate the regulation and function of endothelial leader cells by plasma lithography geometric confinement generated. Endothelial leader cells display an aggressive phenotype, connect to follower cells via peripheral actin cables and discontinuous adherens junctions, and lead migrating clusters near the leading edge. Time-lapse microscopy, immunostaining, and particle image velocimetry reveal that the density of leader cells and the speed of migrating clusters are tightly regulated in a wide range of geometric patterns. By challenging the cells with converging, diverging and competing patterns, we show that the density of leader cells correlates with the size and coherence of the migrating clusters. Collectively, our data provide evidence that leader cells control endothelial collective migration by regualting the migrating clusters.

Carbon X-ray absorption spectra of fluoroethenes and acetone: A study at the coupled cluster, density functional, and static-exchange levels of theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fransson, Thomas; Norman, Patrick; Coriani, Sonia

2013-03-28

Near carbon K-edge X-ray absorption fine structure spectra of a series of fluorine-substituted ethenes and acetone have been studied using coupled cluster and density functional theory (DFT) polarization propagator methods, as well as the static-exchange (STEX) approach. With the complex polarization propagator (CPP) implemented in coupled cluster theory, relaxation effects following the excitation of core electrons are accounted for in terms of electron correlation, enabling a systematic convergence of these effects with respect to electron excitations in the cluster operator. Coupled cluster results have been used as benchmarks for the assessment of propagator methods in DFT as well as themore » state-specific static-exchange approach. Calculations on ethene and 1,1-difluoroethene illustrate the possibility of using nonrelativistic coupled cluster singles and doubles (CCSD) with additional effects of electron correlation and relativity added as scalar shifts in energetics. It has been demonstrated that CPP spectra obtained with coupled cluster singles and approximate doubles (CC2), CCSD, and DFT (with a Coulomb attenuated exchange-correlation functional) yield excellent predictions of chemical shifts for vinylfluoride, 1,1-difluoroethene, trifluoroethene, as well as good spectral features for acetone in the case of CCSD and DFT. Following this, CPP-DFT is considered to be a viable option for the calculation of X-ray absorption spectra of larger {pi}-conjugated systems, and CC2 is deemed applicable for chemical shifts but not for studies of fine structure features. The CCSD method as well as the more approximate CC2 method are shown to yield spectral features relating to {pi}*-resonances in good agreement with experiment, not only for the aforementioned molecules but also for ethene, cis-1,2-difluoroethene, and tetrafluoroethene. The STEX approach is shown to underestimate {pi}*-peak separations due to spectral compressions, a characteristic which is inherent to this method.« less

Carbon X-ray absorption spectra of fluoroethenes and acetone: a study at the coupled cluster, density functional, and static-exchange levels of theory.

PubMed

Fransson, Thomas; Coriani, Sonia; Christiansen, Ove; Norman, Patrick

2013-03-28

Near carbon K-edge X-ray absorption fine structure spectra of a series of fluorine-substituted ethenes and acetone have been studied using coupled cluster and density functional theory (DFT) polarization propagator methods, as well as the static-exchange (STEX) approach. With the complex polarization propagator (CPP) implemented in coupled cluster theory, relaxation effects following the excitation of core electrons are accounted for in terms of electron correlation, enabling a systematic convergence of these effects with respect to electron excitations in the cluster operator. Coupled cluster results have been used as benchmarks for the assessment of propagator methods in DFT as well as the state-specific static-exchange approach. Calculations on ethene and 1,1-difluoroethene illustrate the possibility of using nonrelativistic coupled cluster singles and doubles (CCSD) with additional effects of electron correlation and relativity added as scalar shifts in energetics. It has been demonstrated that CPP spectra obtained with coupled cluster singles and approximate doubles (CC2), CCSD, and DFT (with a Coulomb attenuated exchange-correlation functional) yield excellent predictions of chemical shifts for vinylfluoride, 1,1-difluoroethene, trifluoroethene, as well as good spectral features for acetone in the case of CCSD and DFT. Following this, CPP-DFT is considered to be a viable option for the calculation of X-ray absorption spectra of larger π-conjugated systems, and CC2 is deemed applicable for chemical shifts but not for studies of fine structure features. The CCSD method as well as the more approximate CC2 method are shown to yield spectral features relating to π∗-resonances in good agreement with experiment, not only for the aforementioned molecules but also for ethene, cis-1,2-difluoroethene, and tetrafluoroethene. The STEX approach is shown to underestimate π∗-peak separations due to spectral compressions, a characteristic which is inherent to this method.

Density-functional study of the structures and properties of holmium-doped silicon clusters HoSi n (n = 3-9) and their anions.

PubMed

Hou, Liyuan; Yang, Jucai; Liu, Yuming

2017-04-01

The structures and properties of Ho-doped Si clusters, including their adiabatic electron affinities (AEAs), simulated photoelectron spectra (PESs), stabilities, magnetic moments, and charge-transfer characteristics, were systematically investigated using four density-functional methods. The results show that the double-hybrid functional (which includes an MP2 correlation component) can accurately predict the ground-state structure and properties of Ho-doped Si clusters. The ground-state structures of HoSi n (n = 3-9) are sextuplet electronic states. The structures of these Ho-doped Si clusters (aside from HoSi 7 ) are substitutional. The ground-state structures of HoSi n - are quintuplet electronic states. Their predicted AEAs are in excellent agreement with the experimental ones. The mean absolute error in the theoretical AEAs of HoSi n (n = 4-9) is only 0.04 eV. The simulated PESs for HoSi n - (n = 5-9) are in good agreement with the experimental PESs. Based on its simulated PES and theoretical AEA, we reassigned the experimental PES of HoSi 4 - and obtained an experimental AEA of 2.2 ± 0.1 eV. The dissociation energies of Ho from HoSi n and HoSi n - (n = 3-9) were evaluated to test the relative stabilities of the clusters. HOMO-LUMO gap analysis indicated that doping the Si clusters with the rare-earth metal atom significantly increases their photochemical reactivity. Natural population analysis showed that the magnetic moments of HoSi n (n = 3-9) and their anions derive mainly from the Ho atom. It was also found that the magnetic moments of Ho in the HoSi n clusters are larger than the magnetic moment of an isolated Ho atom.

Computational investigation on the structures and electronic properties of the nanosized rhenium clusters

DOE PAGES

Zhao, Run -Ning; Chen, Rui; Yuan, Yan -Hong; ...

2017-08-10

Here, the stable equilibrium geometries, relative stabilities, and electronic and magnetic characteristics of Re n (n = 2–16) clusters were investigated by density functional theory method. The calculated fragmentation energies and second-order differences of energies exhibited interestingly that the stabilities of Re n (n = 2–16) clusters show a dramatic odd-even alternative behavior of the cluster size n: with the even-numbered Ren clusters being obviously more stable than their neighboring odd-numbered Re n clusters (beside n = 11). Simultaneously, the calculated HOMO-LUMO gaps of Re n (n = 6–16) display an oscillatory feature at large-sized Ren clusters. From the calculatedmore » magnetic moments and growth behaviors of Rhenium clusters, the magnetic Re 6 unit can be seen as the building block for the novel magnetic cluster-assembled nanomaterial. Such calculated results are in good agreement with the available experimental measurements.« less

Computational investigation on the structures and electronic properties of the nanosized rhenium clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhao, Run -Ning; Chen, Rui; Yuan, Yan -Hong

Here, the stable equilibrium geometries, relative stabilities, and electronic and magnetic characteristics of Re n (n = 2–16) clusters were investigated by density functional theory method. The calculated fragmentation energies and second-order differences of energies exhibited interestingly that the stabilities of Re n (n = 2–16) clusters show a dramatic odd-even alternative behavior of the cluster size n: with the even-numbered Ren clusters being obviously more stable than their neighboring odd-numbered Re n clusters (beside n = 11). Simultaneously, the calculated HOMO-LUMO gaps of Re n (n = 6–16) display an oscillatory feature at large-sized Ren clusters. From the calculatedmore » magnetic moments and growth behaviors of Rhenium clusters, the magnetic Re 6 unit can be seen as the building block for the novel magnetic cluster-assembled nanomaterial. Such calculated results are in good agreement with the available experimental measurements.« less

X-ray absorption in insulators with non-Hermitian real-time time-dependent density functional theory.

PubMed

Fernando, Ranelka G; Balhoff, Mary C; Lopata, Kenneth

2015-02-10

Non-Hermitian real-time time-dependent density functional theory was used to compute the Si L-edge X-ray absorption spectrum of α-quartz using an embedded finite cluster model and atom-centered basis sets. Using tuned range-separated functionals and molecular orbital-based imaginary absorbing potentials, the excited states spanning the pre-edge to ∼20 eV above the ionization edge were obtained in good agreement with experimental data. This approach is generalizable to TDDFT studies of core-level spectroscopy and dynamics in a wide range of materials.

Evaluation of B3LYP, X3LYP, and M06-Class Density Functionals for Predicting the Binding Energies of Neutral, Protonated, and Deprotonated Water Clusters.

PubMed

Bryantsev, Vyacheslav S; Diallo, Mamadou S; van Duin, Adri C T; Goddard, William A

2009-04-14

In this paper we assess the accuracy of the B3LYP, X3LYP, and newly developed M06-L, M06-2X, and M06 functionals to predict the binding energies of neutral and charged water clusters including (H2O)n, n = 2-8, 20), H3O(+)(H2O)n, n = 1-6, and OH(-)(H2O)n, n = 1-6. We also compare the predicted energies of two ion hydration and neutralization reactions on the basis of the calculated binding energies. In all cases, we use as benchmarks calculated binding energies of water clusters extrapolated to the complete basis set limit of the second-order Møller-Plesset perturbation theory with the effects of higher order correlation estimated at the coupled-cluster theory with single, double, and perturbative triple excitations in the aug-cc-pVDZ basis set. We rank the accuracy of the functionals on the basis of the mean unsigned error (MUE) between calculated benchmark and density functional theory energies. The corresponding MUE (kcal/mol) for each functional is listed in parentheses. We find that M06-L (0.73) and M06 (0.84) give the most accurate binding energies using very extended basis sets such as aug-cc-pV5Z. For more affordable basis sets, the best methods for predicting the binding energies of water clusters are M06-L/aug-cc-pVTZ (1.24), B3LYP/6-311++G(2d,2p) (1.29), and M06/aug-cc-PVTZ (1.33). M06-L/aug-cc-pVTZ also gives more accurate energies for the neutralization reactions (1.38), whereas B3LYP/6-311++G(2d,2p) gives more accurate energies for the ion hydration reactions (1.69).

Theoretical prediction of novel ultrafine nanowires formed by Si12C12 cage-like clusters

NASA Astrophysics Data System (ADS)

Yong, Yongliang; Song, Bin; He, Pimo

2014-02-01

Using density functional theory calculations, we predict that novel SiC ultrafine nanowires can be produced via the coalescence of stable Si12C12 clusters. For the isolated Si12C12 clusters, we find that the cage-like structure with a distinct segregation between Si and C atoms is energetically more favourable than the fullerene-like structure with alternating Si-C bonds. Via the coalescence of Si12C12 clusters, three novel stable nanowires have been characterised. The band structure reveals that these nanowires are semiconductors with narrow gap, indicating that they may be used as infrared detectors and thermoelectrics.

Molecular oxygen adsorption and dissociation on Au12M clusters with M = Cu, Ag or Ir

NASA Astrophysics Data System (ADS)

Jiménez-Díaz, Laura M.; Pérez, Luis A.

2018-03-01

In this work, we present a density functional theory study of the structural and electronic properties of isolated neutral clusters of the type Au12M, with M = Cu, Ag, or Ir. On the other hand, there is experimental evidence that gold-silver, gold-copper and gold-iridium nanoparticles have an enhanced catalytic activity for the CO oxidation reaction. In order to address these phenomena, we also performed density functional calculations of the adsorption and dissociation of O2 on these nanoparticles. Moreover, to understand the effects of Cu, Ag, and Ir impurity atoms on the dissociation of O2, we also analyze this reaction in the corresponding pure gold cluster. The results indicate that the substitution of one gold atom in a Au13 cluster by Ag, Cu or Ir diminishes the activation energy barrier for the O2 dissociation by nearly 1 eV. This energy barrier is similar for Au12Ag and Au12Cu, whereas for Au12Ir is even lower. These results suggest that the addition of other transition metal atoms to gold nanoclusters can enhance their catalytic activity towards the CO oxidation reaction, independently of the effect that the substrate could have on supported nanoclusters.

GDPC: Gravitation-based Density Peaks Clustering algorithm

NASA Astrophysics Data System (ADS)

Jiang, Jianhua; Hao, Dehao; Chen, Yujun; Parmar, Milan; Li, Keqin

2018-07-01

The Density Peaks Clustering algorithm, which we refer to as DPC, is a novel and efficient density-based clustering approach, and it is published in Science in 2014. The DPC has advantages of discovering clusters with varying sizes and varying densities, but has some limitations of detecting the number of clusters and identifying anomalies. We develop an enhanced algorithm with an alternative decision graph based on gravitation theory and nearby distance to identify centroids and anomalies accurately. We apply our method to some UCI and synthetic data sets. We report comparative clustering performances using F-Measure and 2-dimensional vision. We also compare our method to other clustering algorithms, such as K-Means, Affinity Propagation (AP) and DPC. We present F-Measure scores and clustering accuracies of our GDPC algorithm compared to K-Means, AP and DPC on different data sets. We show that the GDPC has the superior performance in its capability of: (1) detecting the number of clusters obviously; (2) aggregating clusters with varying sizes, varying densities efficiently; (3) identifying anomalies accurately.

Calibrating First-Order Strong Lensing Mass Estimates in Clusters of Galaxies

NASA Astrophysics Data System (ADS)

Reed, Brendan; Remolian, Juan; Sharon, Keren; Li, Nan; SPT Clusters Cooperation

2018-01-01

We investigate methods to reduce the statistical and systematic errors inherent to using the Einstein Radius as a first-order mass estimate in strong lensing galaxy clusters. By finding an empirical universal calibration function, we aim to enable a first-order mass estimate of large cluster data sets in a fraction of the time and effort of full-scale strong lensing mass modeling. We use 74 simulated cluster data from the Argonne National Laboratory in a lens redshift slice of [0.159, 0.667] with various source redshifts in the range of [1.23, 2.69]. From the simulated density maps, we calculate the exact mass enclosed within the Einstein Radius. We find that the mass inferred from the Einstein Radius alone produces an error width of ~39% with respect to the true mass. We explore an array of polynomial and exponential correction functions with dependence on cluster redshift and projected radii of the lensed images, aiming to reduce the statistical and systematic uncertainty. We find that the error on the the mass inferred from the Einstein Radius can be reduced significantly by using a universal correction function. Our study has implications for current and future large galaxy cluster surveys aiming to measure cluster mass, and the mass-concentration relation.

Diffuse Optical Light in Galaxy Clusters. II. Correlations with Cluster Properties

NASA Astrophysics Data System (ADS)

Krick, J. E.; Bernstein, R. A.

2007-08-01

We have measured the flux, profile, color, and substructure in the diffuse intracluster light (ICL) in a sample of 10 galaxy clusters with a range of mass, morphology, redshift, and density. Deep, wide-field observations for this project were made in two bands at the 1 m Swope and 2.5 m du Pont telescopes at Las Campanas Observatory. Careful attention in reduction and analysis was paid to the illumination correction, background subtraction, point-spread function determination, and galaxy subtraction. ICL flux is detected in both bands in all 10 clusters ranging from 7.6×1010 to 7.0×1011 h-170 Lsolar in r and 1.4×1010 to 1.2×1011 h-170 Lsolar in the B band. These fluxes account for 6%-22% of the total cluster light within one-quarter of the virial radius in r and 4%-21% in the B band. Average ICL B-r colors range from 1.5 to 2.8 mag when k- and evolution corrected to the present epoch. In several clusters we also detect ICL in group environments near the cluster center and up to 1 h-170 Mpc distant from the cluster center. Our sample, having been selected from the Abell sample, is incomplete in that it does not include high-redshift clusters with low density, low flux, or low mass, and it does not include low-redshift clusters with high flux, high mass, or high density. This bias makes it difficult to interpret correlations between ICL flux and cluster properties. Despite this selection bias, we do find that the presence of a cD galaxy corresponds to both centrally concentrated galaxy profiles and centrally concentrated ICL profiles. This is consistent with ICL either forming from galaxy interactions at the center or forming at earlier times in groups and later combining in the center.

Computational identification of developmental enhancers:conservation and function of transcription factor binding-site clustersin drosophila melanogaster and drosophila psedoobscura

DOE Office of Scientific and Technical Information (OSTI.GOV)

Berman, Benjamin P.; Pfeiffer, Barret D.; Laverty, Todd R.

2004-08-06

Background The identification of sequences that control transcription in metazoans is a major goal of genome analysis. In a previous study, we demonstrated that searching for clusters of predicted transcription factor binding sites could discover active regulatory sequences, and identified 37 regions of the Drosophila melanogaster genome with high densities of predicted binding sites for five transcription factors involved in anterior-posterior embryonic patterning. Nine of these clusters overlapped known enhancers. Here, we report the results of in vivo functional analysis of 27 remaining clusters. Results We generated transgenic flies carrying each cluster attached to a basal promoter and reporter gene,more » and assayed embryos for reporter gene expression. Six clusters are enhancers of adjacent genes: giant, fushi tarazu, odd-skipped, nubbin, squeeze and pdm2; three drive expression in patterns unrelated to those of neighboring genes; the remaining 18 do not appear to have enhancer activity. We used the Drosophila pseudoobscura genome to compare patterns of evolution in and around the 15 positive and 18 false-positive predictions. Although conservation of primary sequence cannot distinguish true from false positives, conservation of binding-site clustering accurately discriminates functional binding-site clusters from those with no function. We incorporated conservation of binding-site clustering into a new genome-wide enhancer screen, and predict several hundred new regulatory sequences, including 85 adjacent to genes with embryonic patterns. Conclusions Measuring conservation of sequence features closely linked to function - such as binding-site clustering - makes better use of comparative sequence data than commonly used methods that examine only sequence identity.« less

The MUSIC of CLASH: Predictions on the Concentration-Mass Relation

NASA Astrophysics Data System (ADS)

Meneghetti, M.; Rasia, E.; Vega, J.; Merten, J.; Postman, M.; Yepes, G.; Sembolini, F.; Donahue, M.; Ettori, S.; Umetsu, K.; Balestra, I.; Bartelmann, M.; Benítez, N.; Biviano, A.; Bouwens, R.; Bradley, L.; Broadhurst, T.; Coe, D.; Czakon, N.; De Petris, M.; Ford, H.; Giocoli, C.; Gottlöber, S.; Grillo, C.; Infante, L.; Jouvel, S.; Kelson, D.; Koekemoer, A.; Lahav, O.; Lemze, D.; Medezinski, E.; Melchior, P.; Mercurio, A.; Molino, A.; Moscardini, L.; Monna, A.; Moustakas, J.; Moustakas, L. A.; Nonino, M.; Rhodes, J.; Rosati, P.; Sayers, J.; Seitz, S.; Zheng, W.; Zitrin, A.

2014-12-01

We present an analysis of the MUSIC-2 N-body/hydrodynamical simulations aimed at estimating the expected concentration-mass relation for the CLASH (Cluster Lensing and Supernova Survey with Hubble) cluster sample. We study nearly 1,400 halos simulated at high spatial and mass resolution. We study the shape of both their density and surface-density profiles and fit them with a variety of radial functions, including the Navarro-Frenk-White (NFW), the generalized NFW, and the Einasto density profiles. We derive concentrations and masses from these fits. We produce simulated Chandra observations of the halos, and we use them to identify objects resembling the X-ray morphologies and masses of the clusters in the CLASH X-ray-selected sample. We also derive a concentration-mass relation for strong-lensing clusters. We find that the sample of simulated halos that resembles the X-ray morphology of the CLASH clusters is composed mainly of relaxed halos, but it also contains a significant fraction of unrelaxed systems. For such a heterogeneous sample we measure an average two-dimensional concentration that is ~11% higher than is found for the full sample of simulated halos. After accounting for projection and selection effects, the average NFW concentrations of CLASH clusters are expected to be intermediate between those predicted in three dimensions for relaxed and super-relaxed halos. Matching the simulations to the individual CLASH clusters on the basis of the X-ray morphology, we expect that the NFW concentrations recovered from the lensing analysis of the CLASH clusters are in the range [3-6], with an average value of 3.87 and a standard deviation of 0.61.

The music of clash: predictions on the concentration-mass relation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meneghetti, M.; Rasia, E.; Vega, J.

We present an analysis of the MUSIC-2 N-body/hydrodynamical simulations aimed at estimating the expected concentration-mass relation for the CLASH (Cluster Lensing and Supernova Survey with Hubble) cluster sample. We study nearly 1,400 halos simulated at high spatial and mass resolution. We study the shape of both their density and surface-density profiles and fit them with a variety of radial functions, including the Navarro-Frenk-White (NFW), the generalized NFW, and the Einasto density profiles. We derive concentrations and masses from these fits. We produce simulated Chandra observations of the halos, and we use them to identify objects resembling the X-ray morphologies andmore » masses of the clusters in the CLASH X-ray-selected sample. We also derive a concentration-mass relation for strong-lensing clusters. We find that the sample of simulated halos that resembles the X-ray morphology of the CLASH clusters is composed mainly of relaxed halos, but it also contains a significant fraction of unrelaxed systems. For such a heterogeneous sample we measure an average two-dimensional concentration that is ∼11% higher than is found for the full sample of simulated halos. After accounting for projection and selection effects, the average NFW concentrations of CLASH clusters are expected to be intermediate between those predicted in three dimensions for relaxed and super-relaxed halos. Matching the simulations to the individual CLASH clusters on the basis of the X-ray morphology, we expect that the NFW concentrations recovered from the lensing analysis of the CLASH clusters are in the range [3-6], with an average value of 3.87 and a standard deviation of 0.61.« less

An improved initialization center k-means clustering algorithm based on distance and density

NASA Astrophysics Data System (ADS)

Duan, Yanling; Liu, Qun; Xia, Shuyin

2018-04-01

Aiming at the problem of the random initial clustering center of k means algorithm that the clustering results are influenced by outlier data sample and are unstable in multiple clustering, a method of central point initialization method based on larger distance and higher density is proposed. The reciprocal of the weighted average of distance is used to represent the sample density, and the data sample with the larger distance and the higher density are selected as the initial clustering centers to optimize the clustering results. Then, a clustering evaluation method based on distance and density is designed to verify the feasibility of the algorithm and the practicality, the experimental results on UCI data sets show that the algorithm has a certain stability and practicality.

Star cluster formation in a turbulent molecular cloud self-regulated by photoionization feedback

NASA Astrophysics Data System (ADS)

Gavagnin, Elena; Bleuler, Andreas; Rosdahl, Joakim; Teyssier, Romain

2017-12-01

Most stars in the Galaxy are believed to be formed within star clusters from collapsing molecular clouds. However, the complete process of star formation, from the parent cloud to a gas-free star cluster, is still poorly understood. We perform radiation-hydrodynamical simulations of the collapse of a turbulent molecular cloud using the RAMSES-RT code. Stars are modelled using sink particles, from which we self-consistently follow the propagation of the ionizing radiation. We study how different feedback models affect the gas expulsion from the cloud and how they shape the final properties of the emerging star cluster. We find that the star formation efficiency is lower for stronger feedback models. Feedback also changes the high-mass end of the stellar mass function. Stronger feedback also allows the establishment of a lower density star cluster, which can maintain a virial or sub-virial state. In the absence of feedback, the star formation efficiency is very high, as well as the final stellar density. As a result, high-energy close encounters make the cluster evaporate quickly. Other indicators, such as mass segregation, statistics of multiple systems and escaping stars confirm this picture. Observations of young star clusters are in best agreement with our strong feedback simulation.

Detection of protein complex from protein-protein interaction network using Markov clustering

NASA Astrophysics Data System (ADS)

Ochieng, P. J.; Kusuma, W. A.; Haryanto, T.

2017-05-01

Detection of complexes, or groups of functionally related proteins, is an important challenge while analysing biological networks. However, existing algorithms to identify protein complexes are insufficient when applied to dense networks of experimentally derived interaction data. Therefore, we introduced a graph clustering method based on Markov clustering algorithm to identify protein complex within highly interconnected protein-protein interaction networks. Protein-protein interaction network was first constructed to develop geometrical network, the network was then partitioned using Markov clustering to detect protein complexes. The interest of the proposed method was illustrated by its application to Human Proteins associated to type II diabetes mellitus. Flow simulation of MCL algorithm was initially performed and topological properties of the resultant network were analysed for detection of the protein complex. The results indicated the proposed method successfully detect an overall of 34 complexes with 11 complexes consisting of overlapping modules and 20 non-overlapping modules. The major complex consisted of 102 proteins and 521 interactions with cluster modularity and density of 0.745 and 0.101 respectively. The comparison analysis revealed MCL out perform AP, MCODE and SCPS algorithms with high clustering coefficient (0.751) network density and modularity index (0.630). This demonstrated MCL was the most reliable and efficient graph clustering algorithm for detection of protein complexes from PPI networks.

Effects of stomata clustering on leaf gas exchange.

PubMed

Lehmann, Peter; Or, Dani

2015-09-01

A general theoretical framework for quantifying the stomatal clustering effects on leaf gaseous diffusive conductance was developed and tested. The theory accounts for stomatal spacing and interactions among 'gaseous concentration shells'. The theory was tested using the unique measurements of Dow et al. (2014) that have shown lower leaf diffusive conductance for a genotype of Arabidopsis thaliana with clustered stomata relative to uniformly distributed stomata of similar size and density. The model accounts for gaseous diffusion: through stomatal pores; via concentration shells forming at pore apertures that vary with stomata spacing and are thus altered by clustering; and across the adjacent air boundary layer. Analytical approximations were derived and validated using a numerical model for 3D diffusion equation. Stomata clustering increases the interactions among concentration shells resulting in larger diffusive resistance that may reduce fluxes by 5-15%. A similar reduction in conductance was found for clusters formed by networks of veins. The study resolves ambiguities found in the literature concerning stomata end-corrections and stomatal shape, and provides a new stomata density threshold for diffusive interactions of overlapping vapor shells. The predicted reduction in gaseous exchange due to clustering, suggests that guard cell function is impaired, limiting stomatal aperture opening. © 2015 The Authors. New Phytologist © 2015 New Phytologist Trust.

Assessing the performance of dispersionless and dispersion-accounting methods: helium interaction with cluster models of the TiO2(110) surface.

PubMed

de Lara-Castells, María Pilar; Stoll, Hermann; Mitrushchenkov, Alexander O

2014-08-21

As a prototypical dispersion-dominated physisorption problem, we analyze here the performance of dispersionless and dispersion-accounting methodologies on the helium interaction with cluster models of the TiO2(110) surface. A special focus has been given to the dispersionless density functional dlDF and the dlDF+Das construction for the total interaction energy (K. Pernal, R. Podeswa, K. Patkowski, and K. Szalewicz, Phys. Rev. Lett. 2009, 109, 263201), where Das is an effective interatomic pairwise functional form for the dispersion. Likewise, the performance of symmetry-adapted perturbation theory (SAPT) method is evaluated, where the interacting monomers are described by density functional theory (DFT) with the dlDF, PBE, and PBE0 functionals. Our benchmarks include CCSD(T)-F12b calculations and comparative analysis on the nuclear bound states supported by the He-cluster potentials. Moreover, intra- and intermonomer correlation contributions to the physisorption interaction are analyzed through the method of increments (H. Stoll, J. Chem. Phys. 1992, 97, 8449) at the CCSD(T) level of theory. This method is further applied in conjunction with a partitioning of the Hartree-Fock interaction energy to estimate individual interaction energy components, comparing them with those obtained using the different SAPT(DFT) approaches. The cluster size evolution of dispersionless and dispersion-accounting energy components is then discussed, revealing the reduced role of the dispersionless interaction and intramonomer correlation when the extended nature of the surface is better accounted for. On the contrary, both post-Hartree-Fock and SAPT(DFT) results clearly demonstrate the high-transferability character of the effective pairwise dispersion interaction whatever the cluster model is. Our contribution also illustrates how the method of increments can be used as a valuable tool not only to achieve the accuracy of CCSD(T) calculations using large cluster models but also to evaluate the performance of SAPT(DFT) methods for the physically well-defined contributions to the total interaction energy. Overall, our work indicates the excellent performance of a dlDF+Das approach in which the parameters are optimized using the smallest cluster model of the target surface to treat van der Waals adsorbate-surface interactions.

The XXL Survey. II. The bright cluster sample: catalogue and luminosity function

NASA Astrophysics Data System (ADS)

Pacaud, F.; Clerc, N.; Giles, P. A.; Adami, C.; Sadibekova, T.; Pierre, M.; Maughan, B. J.; Lieu, M.; Le Fèvre, J. P.; Alis, S.; Altieri, B.; Ardila, F.; Baldry, I.; Benoist, C.; Birkinshaw, M.; Chiappetti, L.; Démoclès, J.; Eckert, D.; Evrard, A. E.; Faccioli, L.; Gastaldello, F.; Guennou, L.; Horellou, C.; Iovino, A.; Koulouridis, E.; Le Brun, V.; Lidman, C.; Liske, J.; Maurogordato, S.; Menanteau, F.; Owers, M.; Poggianti, B.; Pomarède, D.; Pompei, E.; Ponman, T. J.; Rapetti, D.; Reiprich, T. H.; Smith, G. P.; Tuffs, R.; Valageas, P.; Valtchanov, I.; Willis, J. P.; Ziparo, F.

2016-06-01

Context. The XXL Survey is the largest survey carried out by the XMM-Newton satellite and covers a total area of 50 square degrees distributed over two fields. It primarily aims at investigating the large-scale structures of the Universe using the distribution of galaxy clusters and active galactic nuclei as tracers of the matter distribution. The survey will ultimately uncover several hundreds of galaxy clusters out to a redshift of ~2 at a sensitivity of ~10-14 erg s-1 cm-2 in the [0.5-2] keV band. Aims: This article presents the XXL bright cluster sample, a subsample of 100 galaxy clusters selected from the full XXL catalogue by setting a lower limit of 3 × 10-14 erg s-1 cm-2 on the source flux within a 1' aperture. Methods: The selection function was estimated using a mixture of Monte Carlo simulations and analytical recipes that closely reproduce the source selection process. An extensive spectroscopic follow-up provided redshifts for 97 of the 100 clusters. We derived accurate X-ray parameters for all the sources. Scaling relations were self-consistently derived from the same sample in other publications of the series. On this basis, we study the number density, luminosity function, and spatial distribution of the sample. Results: The bright cluster sample consists of systems with masses between M500 = 7 × 1013 and 3 × 1014 M⊙, mostly located between z = 0.1 and 0.5. The observed sky density of clusters is slightly below the predictions from the WMAP9 model, and significantly below the prediction from the Planck 2015 cosmology. In general, within the current uncertainties of the cluster mass calibration, models with higher values of σ8 and/or ΩM appear more difficult to accommodate. We provide tight constraints on the cluster differential luminosity function and find no hint of evolution out to z ~ 1. We also find strong evidence for the presence of large-scale structures in the XXL bright cluster sample and identify five new superclusters. Based on observations obtained with XMM-Newton, an ESA science mission with instruments and contributions directly funded by ESA Member States and NASA. Based on observations made with ESO Telescopes at the La Silla and Paranal Observatories under programme ID 089.A-0666 and LP191.A-0268.The Master Catalogue is available at the CDS via anonymous ftp to http://cdsarc.u-strasbg.fr (http://130.79.128.5) or via http://cdsarc.u-strasbg.fr/viz-bin/qcat?J/A+A/592/A2

Evaluation of optical and electronic properties of silicon nano-agglomerates embedded in SRO: applying density functional theory

PubMed Central

2014-01-01

In systems in atomic scale and nanoscale such as clusters or agglomerates constituted by particles from a few to less than 100 atoms, quantum confinement effects are very important. Their optical and electronic properties are often dependent on the size of the systems and the way in which the atoms in these clusters are bonded. Generally, these nanostructures display optical and electronic properties significantly different to those found in corresponding bulk materials. Silicon agglomerates embedded in silicon rich oxide (SRO) films have optical properties, which have been reported to be directly dependent on silicon nanocrystal size. Furthermore, the room temperature photoluminescence (PL) of SRO has repeatedly generated a huge interest due to its possible applications in optoelectronic devices. However, a plausible emission mechanism has not been widely accepted in the scientific community. In this work, we present a short review about the experimental results on silicon nanoclusters in SRO considering different techniques of growth. We focus mainly on their size, Raman spectra, and photoluminescence spectra. With this as background, we employed the density functional theory with a functional B3LYP and a basis set 6-31G* to calculate the optical and electronic properties of clusters of silicon (constituted by 15 to 20 silicon atoms). With the theoretical calculation of the structural and optical properties of silicon clusters, it is possible to evaluate the contribution of silicon agglomerates in the luminescent emission mechanism, experimentally found in thin SRO films. PMID:25276105

The Cosmological Dependence of Galaxy Cluster Morphologies

NASA Astrophysics Data System (ADS)

Crone, Mary Margaret

1995-01-01

Measuring the density of the universe has been a fundamental problem in cosmology ever since the "Big Bang" model was developed over sixty years ago. In this simple and successful model, the age and eventual fate of the universe are determined by its density, its rate of expansion, and the value of a universal "cosmological constant". Analytic models suggest that many properties of galaxy clusters are sensitive to cosmological parameters. In this thesis, I use N-body simulations to examine cluster density profiles, abundances, and degree of subclustering to test the feasibility of using them as cosmological tests. The dependence on both cosmology and initial density field is examined, using a grid of cosmologies and scale-free initial power spectra P(k)~ k n. Einstein-deSitter ( Omegao=1), open ( Omegao=0.2 and 0.1) and flat, low density (Omegao=0.2, lambdao=0.8) models are studied, with initial spectral indices n=-2, -1 and 0. Of particular interest are the results for cluster profiles and substructure. The average density profiles are well fit by a power law p(r)~ r ^{-alpha} for radii where the local density contrast is between 100 and 3000. There is a clear trend toward steeper slopes with both increasing n and decreasing Omegao, with profile slopes in the open models consistently higher than Omega=1 values for the range of n examined. The amount of substructure in each model is quantified and explained in terms of cluster merger histories and the behavior of substructure statistics. The statistic which best distinguishes models is a very simple measure of deviations from symmetry in the projected mass distribution --the "Center-of-Mass Shift" as a function of overdensity. Some statistics which are quite sensitive to substructure perform relatively poorly as cosmological indicators. Density profiles and the Center-of-Mass test are both well-suited for comparison with weak lensing data and galaxy distributions. Such data are currently being collected and should be available within the next few years. At that time the predictions described here can be used to set useful cosmological constraints.

Density-dependent clustering: I. Pulling back the curtains on motions of the BAO peak

NASA Astrophysics Data System (ADS)

Neyrinck, Mark C.; Szapudi, István; McCullagh, Nuala; Szalay, Alexander S.; Falck, Bridget; Wang, Jie

2018-05-01

The most common statistic used to analyze large-scale structure surveys is the correlation function, or power spectrum. Here, we show how `slicing' the correlation function on local density brings sensitivity to interesting non-Gaussian features in the large-scale structure, such as the expansion or contraction of baryon acoustic oscillations (BAO) according to the local density. The sliced correlation function measures the large-scale flows that smear out the BAO, instead of just correcting them as reconstruction algorithms do. Thus, we expect the sliced correlation function to be useful in constraining the growth factor, and modified gravity theories that involve the local density. Out of the studied cases, we find that the run of the BAO peak location with density is best revealed when slicing on a ˜40 h-1 Mpc filtered density. But slicing on a ˜100 h-1 Mpc filtered density may be most useful in distinguishing between underdense and overdense regions, whose BAO peaks are separated by a substantial ˜5 h-1 Mpc at z = 0. We also introduce `curtain plots' showing how local densities drive particle motions toward or away from each other over the course of an N-body simulation.

FT-ICR mass spectrometric and density functional theory studies of sulfate prenucleation clusters

NASA Astrophysics Data System (ADS)

Lemke, K. H.

2012-12-01

Recent mass spectrometric1 and relaxation spectroscopic studies2 of metal sulfate salts have demonstrated that aqueous clusters play an important role in sulfate prenucleation processes. While such studies provide evidence that that ion clusters are nucleation relevant species, ultra-high resolution mass spectrumetry, in particular, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR/MS) can provide additional valuable information about the molecular composition and stability of individual ion clusters. Prompted by the above studies, our group has begun a systematic survey of metal sulfate clusters using FT-ICR mass spectrometry. Here, I report stoichiometries, structures and thermodynamic properties of calcium sulfate ion clusters, both "dry" and microsolvated, using electrospray ionization FT-ICR mass spectrometry in combination with semi-empirical methods and M062X/aug-cc-PVXZ level density functional theory calculations. In electrosprayed dilute aqueous solutions of CaSO4 (1-20mM), droplet desolvation results in the formation of stable doubly-charged clusters of [Ca(CaSO4)m(H2O)n]+2 (m≤10 & n≤9) as well as larger quadruply-charged ion clusters [Ca2(CaSO4)m(H2O)n]+4 with m≤23 and n≤10, demonstrating considerable sulfate nucleation potential in undersaturated electrolyte solutions. An attempt was also made to assess the extent of ion cluster aggregation in solution prior to electrospray ionization by measuring ion mass spectra at different solution concentrations. In brief, an increase in calcium sulfate concentration from 1-10mM results in a continuous increase in polynuclear ion cluster species, while smaller clusters, for instance, Ca[CaSO4]+2 and corresponding hydrated forms, become increasingly less abundant. Building on semi-empirical methods, M062X calculations have been applied to predict calcium sulfate cluster geometries, both "dry" and microsolvated, as well as the size-dependent evolution of clustering and hydration energies. 1Schoeder et al. (2011) J.Am.Chem.Soc., 133, 2444; 2Chen et al. (2005) J.Sol.Chem., 34, 1045;

Theoretical prediction of a new stable structure of Au28(SR)20 cluster

NASA Astrophysics Data System (ADS)

Sun, Xiangxiang; Wang, Pu; Xiong, Lin; Pei, Yong

2018-07-01

A new stable structure of Au28(SR)20 cluster is predicted, which has the same gold core as two known structures but different Au-S framework. The new Au28(SR)20 cluster is proposed to be a key link in the evolution of Au22(SR)18, Au34(SR)22 and Au40(SR)24 clusters. The four clusters belong to a homogenous Au16+6N(SR)16+2N series (N = 1-4). The relative stabilities of the new Au28 isomer structure were confirmed by density functional theory calculations including dispersion corrections (DFT-D). It is found that upon protection of certain SR ligands, the new isomer structure has lower or comparable energies to two known cluster structures.

Low-end mass function of the Quintuplet cluster

NASA Astrophysics Data System (ADS)

Shin, Jihye; Kim, Sungsoo S.

2016-08-01

The Quintuplet and Arches clusters, which were formed in the harsh environment of the Galactic Centre (GC) a few million years ago, have been excellent targets for studying the effects of a star-forming environment on the initial mass function (IMF). In order to estimate the shape of the low-end IMF of the Arches cluster, Shin & Kim devised a novel photometric method that utilizes pixel intensity histograms (PIHs) of the observed images. Here, we apply the PIH method to the Quintuplet cluster and estimate the shape of its low-end IMF below the magnitude of completeness limit as set by conventional photometry. We found that the low-end IMF of the Quintuplet is consistent with that found for the Arches cluster-Kroupa MF, with a significant number of low-mass stars below 1 M⊙. We conclude that the most likely IMFs of the Quintuplet and the Arches clusters are not too different from the IMFs found in the Galactic disc. We also find that the observed PIHs and stellar number density profiles of both clusters are best reproduced when the clusters are assumed to be at three-dimensional distances of approximately 100 pc from the GC.

Perspective: Size selected clusters for catalysis and electrochemistry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Halder, Avik; Curtiss, Larry A.; Fortunelli, Alessandro

We report that size-selected clusters containing a handful of atoms may possess noble catalytic properties different from nano-sized or bulk catalysts. Size- and composition-selected clusters can also serve as models of the catalytic active site, where an addition or removal of a single atom can have a dramatic effect on their activity and selectivity. In this Perspective, we provide an overview of studies performed under both ultra-high vacuum and realistic reaction conditions aimed at the interrogation, characterization and understanding of the performance of supported size-selected clusters in heterogeneous and electrochemical reactions, which address the effects of cluster size, cluster composition,more » cluster-support interactions and reaction conditions, the key parameters for the understanding and control of catalyst functionality. Computational modelling based on density functional theory sampling of local minima and energy barriers or ab initio Molecular Dynamics simulations is an integral part of this research by providing fundamental understanding of the catalytic processes at the atomic level, as well as by predicting new materials compositions which can be validated in experiments. Lastly, we discuss approaches which aim at the scale up of the production of well-defined clusters for use in real world applications.« less

Perspective: Size selected clusters for catalysis and electrochemistry

DOE PAGES

Halder, Avik; Curtiss, Larry A.; Fortunelli, Alessandro; ...

2018-03-15

We report that size-selected clusters containing a handful of atoms may possess noble catalytic properties different from nano-sized or bulk catalysts. Size- and composition-selected clusters can also serve as models of the catalytic active site, where an addition or removal of a single atom can have a dramatic effect on their activity and selectivity. In this Perspective, we provide an overview of studies performed under both ultra-high vacuum and realistic reaction conditions aimed at the interrogation, characterization and understanding of the performance of supported size-selected clusters in heterogeneous and electrochemical reactions, which address the effects of cluster size, cluster composition,more » cluster-support interactions and reaction conditions, the key parameters for the understanding and control of catalyst functionality. Computational modelling based on density functional theory sampling of local minima and energy barriers or ab initio Molecular Dynamics simulations is an integral part of this research by providing fundamental understanding of the catalytic processes at the atomic level, as well as by predicting new materials compositions which can be validated in experiments. Lastly, we discuss approaches which aim at the scale up of the production of well-defined clusters for use in real world applications.« less

Perspective: Size selected clusters for catalysis and electrochemistry

NASA Astrophysics Data System (ADS)

Halder, Avik; Curtiss, Larry A.; Fortunelli, Alessandro; Vajda, Stefan

2018-03-01

Size-selected clusters containing a handful of atoms may possess noble catalytic properties different from nano-sized or bulk catalysts. Size- and composition-selected clusters can also serve as models of the catalytic active site, where an addition or removal of a single atom can have a dramatic effect on their activity and selectivity. In this perspective, we provide an overview of studies performed under both ultra-high vacuum and realistic reaction conditions aimed at the interrogation, characterization, and understanding of the performance of supported size-selected clusters in heterogeneous and electrochemical reactions, which address the effects of cluster size, cluster composition, cluster-support interactions, and reaction conditions, the key parameters for the understanding and control of catalyst functionality. Computational modeling based on density functional theory sampling of local minima and energy barriers or ab initio molecular dynamics simulations is an integral part of this research by providing fundamental understanding of the catalytic processes at the atomic level, as well as by predicting new materials compositions which can be validated in experiments. Finally, we discuss approaches which aim at the scale up of the production of well-defined clusters for use in real world applications.

A Self-Adaptive Fuzzy c-Means Algorithm for Determining the Optimal Number of Clusters

PubMed Central

Wang, Zhihao; Yi, Jing

2016-01-01

For the shortcoming of fuzzy c-means algorithm (FCM) needing to know the number of clusters in advance, this paper proposed a new self-adaptive method to determine the optimal number of clusters. Firstly, a density-based algorithm was put forward. The algorithm, according to the characteristics of the dataset, automatically determined the possible maximum number of clusters instead of using the empirical rule n and obtained the optimal initial cluster centroids, improving the limitation of FCM that randomly selected cluster centroids lead the convergence result to the local minimum. Secondly, this paper, by introducing a penalty function, proposed a new fuzzy clustering validity index based on fuzzy compactness and separation, which ensured that when the number of clusters verged on that of objects in the dataset, the value of clustering validity index did not monotonically decrease and was close to zero, so that the optimal number of clusters lost robustness and decision function. Then, based on these studies, a self-adaptive FCM algorithm was put forward to estimate the optimal number of clusters by the iterative trial-and-error process. At last, experiments were done on the UCI, KDD Cup 1999, and synthetic datasets, which showed that the method not only effectively determined the optimal number of clusters, but also reduced the iteration of FCM with the stable clustering result. PMID:28042291

STAR FORMATION AND SUPERCLUSTER ENVIRONMENT OF 107 NEARBY GALAXY CLUSTERS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cohen, Seth A.; Hickox, Ryan C.; Wegner, Gary A.

We analyze the relationship between star formation (SF), substructure, and supercluster environment in a sample of 107 nearby galaxy clusters using data from the Sloan Digital Sky Survey. Previous works have investigated the relationships between SF and cluster substructure, and cluster substructure and supercluster environment, but definitive conclusions relating all three of these variables has remained elusive. We find an inverse relationship between cluster SF fraction ( f {sub SF}) and supercluster environment density, calculated using the Galaxy luminosity density field at a smoothing length of 8 h {sup −1} Mpc (D8). The slope of f {sub SF} versus D8more » is −0.008 ± 0.002. The f {sub SF} of clusters located in low-density large-scale environments, 0.244 ± 0.011, is higher than for clusters located in high-density supercluster cores, 0.202 ± 0.014. We also divide superclusters, according to their morphology, into filament- and spider-type systems. The inverse relationship between cluster f {sub SF} and large-scale density is dominated by filament- rather than spider-type superclusters. In high-density cores of superclusters, we find a higher f {sub SF} in spider-type superclusters, 0.229 ± 0.016, than in filament-type superclusters, 0.166 ± 0.019. Using principal component analysis, we confirm these results and the direct correlation between cluster substructure and SF. These results indicate that cluster SF is affected by both the dynamical age of the cluster (younger systems exhibit higher amounts of SF); the large-scale density of the supercluster environment (high-density core regions exhibit lower amounts of SF); and supercluster morphology (spider-type superclusters exhibit higher amounts of SF at high densities).« less

Stability and minimum size of colloidal clusters on a liquid-air interface.

PubMed

Pergamenshchik, V M

2012-02-01

A vertical force applied to each of two colloids, trapped at a liquid-air interface, induces their logarithmic pairwise attraction. I recently showed [Phys. Rev. E 79, 011407 (2009)] that in clusters of size R much larger than the capillary length λ, the attraction changes to that of a power law and is much stronger due to a many-body effect, and I derived two equations that describe the equilibrium coarse-grained meniscus profile and colloid density in such clusters. In this paper, this theory is shown also to describe small clusters with R≪ λ provided the number N of colloids therein is sufficiently large. An analytical solution for a small circular cluster with an arbitrary short-range power-law pairwise repulsion is found. The energy of a cluster is obtained as a function of its radius R and colloid number N. As in large clusters, the attraction force and energy universally scale with the distance L between colloids as L(-3) and L(-2), respectively, for any repulsion forces. The states of an equilibrium cluster, predicted by the theory, are shown to be stable with respect to small perturbations of the meniscus profile and colloid density. The minimum number of colloids in a circular cluster, which sustains the thermal motion, is estimated. For standard parameters, it can be very modest, e.g., in the range 20-200, which is in line with experimental findings on reversible clusterization on a liquid-air interface. © 2012 American Physical Society

X-ray clusters in a cold dark matter + lambda universe: A direct, large-scale, high-resolution, hydrodynamic simulation

NASA Technical Reports Server (NTRS)

Cen, Renyue; Ostriker, Jeremiah P.

1994-01-01

A new, three-dimensional, shock-capturing, hydrodynamic code is utilized to determine the distribution of hot gas in a cold dark matter (CDM) + lambda model universe. Periodic boundary conditions are assumed: a box with size 85/h Mpc, having cell size 0.31/h Mpc, is followed in a simulation with 270(exp 3) = 10(exp 7.3) cells. We adopt omega = 0.45, lambda = 0.55, h identically equal to H/100 km/s/Mpc = 0.6, and then, from the cosmic background explorer (COBE) and light element nucleosynthesis, sigma(sub 8) = 0.77, omega(sub b) = 0.043. We identify the X-ray emitting clusters in the simulation box, compute the luminosity function at several wavelength bands, the temperature function and estimated sizes, as well as the evolution of these quantities with redshift. This open model succeeds in matching local observations of clusters in contrast to the standard omega = 1, CDM model, which fails. It predicts an order of magnitude decline in the number density of bright (h nu = 2-10 keV) clusters from z = 0 to z = 2 in contrast to a slight increase in the number density for standard omega = 1, CDM model. This COBE-normalized CDM + lambda model produces approximately the same number of X-ray clusters having L(sub x) greater than 10(exp 43) erg/s as observed. The background radiation field at 1 keV due to clusters is approximately the observed background which, after correction for numerical effects, again indicates that the model is consistent with observations.

Lattice density functional theory for confined Ising fluids: comparison between different functional approximations in slit pore

NASA Astrophysics Data System (ADS)

Chen, Xueqian; Feng, Wei; Liu, Honglai; Hu, Ying

2016-09-01

In this paper, Lafuente and Cuesta's cluster density functional theory (CDFT) and lattice mean field approximation (LMFA) are formulated and compared within the framework of lattice density functional theory (LDFT). As a comparison, an LDFT based on our previous work on nonrandom correction to LMFA is also developed, where local density approximation is adopted on the correction. The numerical results of density distributions of an Ising fluid confined in a slit pore obtained from Monte Carlo simulation are used to check these functional approximations. Due to rational treatment on the coupling between site-excluding entropic effect and contact-attracting enthalpic effect by CDFT with Bethe-Peierls approximation (named as BPA-CDFT for short), the improvement of BPA-CDFT beyond LMFA is checked as expected. And it is interesting that our LDFT has a comparative accuracy with BPA-CDFT. Apparent differences between the profiles such as solvation force, excess adsorption quantity and interfacial tension from LMFA and non-LMFAs are found in our calculations. We also discuss some possible theoretical extensions of BPA-CDFT.

IR + VUV double resonance spectroscopy and extended density functional theory studies of ketone solvation by alcohol: 2-butanone·(methanol)n, n = 1-4 clusters.

PubMed

Shin, Joong-Won; Bernstein, Elliot R

2017-09-28

Infrared plus vacuum ultraviolet (IR + VUV) photoionization vibrational spectroscopy of 2-butanone/methanol clusters [MEK·(MeOH) n , n = 1-4] is performed to explore structures associated with hydrogen bonding of MeOH molecules to the carbonyl functional group of the ketone. IR spectra and X3LYP/6-31++G(d,p) calculations show that multiple isomers of MEK·(MeOH) n are generated in the molecular beam as a result of several hydrogen bonding sites available to the clusters throughout the size range investigated. Isomer interconversion involving solvating MeOH rearrangement should probably occur for n = 1 and 2. The mode energy for a hydrogen bonded OH stretching transition gradually redshifts as the cluster size increases. Calculations suggest that the n = 3 cluster isomers adopt structures in which the MEK molecule is inserted into the cyclic MeOH hydrogen bond network. In larger structures, the cyclic network may be preserved.

Identifying Few-Molecule Water Clusters with High Precision on Au(111) Surface.

PubMed

Dong, Anning; Yan, Lei; Sun, Lihuan; Yan, Shichao; Shan, Xinyan; Guo, Yang; Meng, Sheng; Lu, Xinghua

2018-06-01

Revealing the nature of a hydrogen-bond network in water structures is one of the imperative objectives of science. With the use of a low-temperature scanning tunneling microscope, water clusters on a Au(111) surface were directly imaged with molecular resolution by a functionalized tip. The internal structures of the water clusters as well as the geometry variations with the increase of size were identified. In contrast to a buckled water hexamer predicted by previous theoretical calculations, our results present deterministic evidence for a flat configuration of water hexamers on Au(111), corroborated by density functional theory calculations with properly implemented van der Waals corrections. The consistency between the experimental observations and improved theoretical calculations not only renders the internal structures of absorbed water clusters unambiguously, but also directly manifests the crucial role of van der Waals interactions in constructing water-solid interfaces.

Deducing the Milky Way's Massive Cluster Population

NASA Astrophysics Data System (ADS)

Hanson, M. M.; Popescu, B.; Larsen, S. S.; Ivanov, V. D.

2010-11-01

Recent near-infrared surveys of the galactic plane have been used to identify new massive cluster candidates. Follow up study indicates about half are not true, gravitationally-bound clusters. These false positives are created by high density fields of unassociated stars, often due to a sight-line of reduced extinction. What is not so easy to estimate is the number of false negatives, clusters which exist but are not currently being detected by our surveys. In order to derive critical characteristics of the Milky Way's massive cluster population, such as cluster mass function and cluster lifetimes, one must be able to estimate the characteristics of these false negatives. Our group has taken on the daunting task of attempting such an estimate by first creating the stellar cluster imaging simulation program, MASSCLEAN. I will present our preliminary models and methods for deriving the biases of current searches.

The Role of Large-Scale Structure and Assembly in the Quenching of Star Formation in Cluster Galaxies at z 0.2

NASA Astrophysics Data System (ADS)

Moran, Sean; Smith, G.; Haines, C.; Egami, E.; Hardegree-Ullman, E.; Heckman, T.

2010-01-01

We present results from LoCuSS, the Local Cluster Substructure Survey, on the distribution and abundance of cluster galaxies showing signatures of recently quenched star formation, within a sample of 15 z 0.2 clusters. Combining LoCuSS' wide-field UV through NIR photometry with weak-lensing derived mass maps for these clusters, we identify passive galaxies that have undergone recent quenching via both rapid (100Myr) and slow (1Gyr) mechanisms. By studying their abundance in a statistically significant sample of z 0.2 clusters, we explore how the effectiveness of environmental quenching of star formation varies as a function of the level of cluster substructure, in addition to global cluster characteristics such as mass or X-ray luminosity and temperature, with the aim of understanding the role that pre-processing of galaxies within groups and filaments plays in the overall buildup of the morphology-density and SFR-density relations. We find that clusters with large levels of substructure indicative of recent assembly or cluster-cluster mergers host a higher fraction of galaxies with signs of recent ram-pressure stripping by the hot intra-cluster gas. In addition, we find that the fraction of post-starburst galaxies increases with cluster mass (M500), but fractions of optically-selected AGN and GALEX-defined "Green Valley" galaxies show the opposite trend, being most abundant in rather low-mass clusters. These trends suggest a picture where quenching of star formation occurs most vigorously in actively assembling structures, with comparatively little activity in the most massive structures where most of the nearby large-scale structure has already been accreted and Virialized into the main cluster body.

Density-Aware Clustering Based on Aggregated Heat Kernel and Its Transformation

DOE PAGES

Huang, Hao; Yoo, Shinjae; Yu, Dantong; ...

2015-06-01

Current spectral clustering algorithms suffer from the sensitivity to existing noise, and parameter scaling, and may not be aware of different density distributions across clusters. If these problems are left untreated, the consequent clustering results cannot accurately represent true data patterns, in particular, for complex real world datasets with heterogeneous densities. This paper aims to solve these problems by proposing a diffusion-based Aggregated Heat Kernel (AHK) to improve the clustering stability, and a Local Density Affinity Transformation (LDAT) to correct the bias originating from different cluster densities. AHK statistically\\ models the heat diffusion traces along the entire time scale, somore » it ensures robustness during clustering process, while LDAT probabilistically reveals local density of each instance and suppresses the local density bias in the affinity matrix. Our proposed framework integrates these two techniques systematically. As a result, not only does it provide an advanced noise-resisting and density-aware spectral mapping to the original dataset, but also demonstrates the stability during the processing of tuning the scaling parameter (which usually controls the range of neighborhood). Furthermore, our framework works well with the majority of similarity kernels, which ensures its applicability to many types of data and problem domains. The systematic experiments on different applications show that our proposed algorithms outperform state-of-the-art clustering algorithms for the data with heterogeneous density distributions, and achieve robust clustering performance with respect to tuning the scaling parameter and handling various levels and types of noise.« less

The Very Small Scale Clustering of SDSS-II and SDSS-III Galaxies

NASA Astrophysics Data System (ADS)

Piscionere, Jennifer

2015-01-01

We measure the angular clustering of galaxies from the Sloan Digital Sky Survey Data Release 7 in order to probe the spatial distribution of satellite galaxies within their dark matter halos. Specifically, we measure the angular correlation function on very small scales (7 - 320‧‧) in a range of luminosity threshold samples (absolute r-band magnitudes of -18 up to -21) that are constructed from the subset of SDSS that has been spectroscopically observed more than once (the so-called plate overlap region). We choose to measure angular clustering in this reduced survey footprint in order to minimize the effects of fiber collision incompleteness, which are otherwise substantial on these small scales. We model our clustering measurements using a fully numerical halo model that populates dark matter halos in N-body simulations to create realistic mock galaxy catalogs. The model has free parameters that specify both the number and spatial distribution of galaxies within their host halos. We adopt a flexible density profile for the spatial distribution of satellite galaxies that is similar to the dark matter Navarro-Frenk-White (NFW) profile, except that the inner slope is allowed to vary. We find that the angular clustering of our most luminous samples (Mr < -20 and -21) suggests that luminous satellite galaxies have substantially steeper inner density profiles than NFW. Lower luminosity samples are less constraining, however, and are consistent with satellite galaxies having shallow density profiles. Our results confirm the findings of Watson et al. (2012) while using different clustering measurements and modeling methodology. With the new SDSS-III Baryon Oscillation Spectroscopic Survey (BOSS; Dawson et al., 2013), we can measure how the same class of galaxy evolves over time. The BOSS CMASS sample is of roughly constant stellar mass and number density out to z ˜ 0.6. The clustering of these samples appears to evolve very little with redshift, and each of the samples exhibit flattening of wp at roughly the same comoving distance of 100kpc.

High Level ab initio Predictions of the Energetics of mCO2•(H2O)n (n = 1-3, m = 1-12) Clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thanthiriwatte, Sahan; Duke, Jessica R.; Jackson, Virgil E.

Electronic structure calculations at the correlated molecular orbital theory and density functional theory levels have been used to generate a reliable set of clustering energies for up to three water molecules in carbon dioxide clusters up to n = 12. The structures and energetics are dominated by Lewis acid-base interactions with hydrogen bonding interactions playing a lesser energetic role. The actual binding energies are somewhat larger than might be expected. The correlated molecular orbital MP2 method and density functional theory with the ωB97X exchange-correlation functional provide good results for the energetics of the clusters but the B3LYP and ωB97X-D functionalsmore » do not. Seven CO2 molecules form the first solvent shell about a single H2O with four CO2 molecules interacting with the H2O via Lewis acid-base interactions, two CO2 interacting with the H2O by hydrogen bonds, and the seventh CO2 completing the shell. The Lewis acid-base and weak hydrogen bond interactions between the water molecules and the CO2 molecules are strong enough to disrupt the trimer ring configuration for as few as seven CO2 molecules. Calculated 13C NMR chemical shifts for mCO2•(H2O)n show little change with respect to the number of H2O or CO2 molecules in the cluster. The O-H stretching frequencies do exhibit shifts that can provide information about the interactions between water and CO2 molecules.« less

BH-DFTB/DFT calculations for iron clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aktürk, Abdurrahman; Sebetci, Ali, E-mail: asebetci@mevlana.edu.tr

2016-05-15

We present a study on the structural, electronic, and magnetic properties of Fe{sub n}(n  =  2  −  20) clusters by performing density functional tight binding (DFTB) calculations within a basin hopping (BH) global optimization search followed by density functional theory (DFT) investigations. The structures, total energies and total spin magnetic moments are calculated and compared with previously reported theoretical and experimental results. Two basis sets SDD with ECP and 6-31G** are employed in the DFT calculations together with BLYP GGA exchange-correlation functional. The results indicate that the offered BH-DFTB/DFT strategy collects all the global minima of which different minima havemore » been reported in the previous studies by different groups. Small Fe clusters have three kinds of packing; icosahedral (Fe{sub 9−13}), centered hexagonal antiprism (Fe{sub 14−17}, Fe{sub 20}), and truncated decahedral (Fe{sub 17(2)}, Fe{sub 18−19}). It is obtained in a qualitative agreement with the time of flight mass spectra that the magic numbers for the small Fe clusters are 7, 13, 15, and 19 and with the collision induced dissociation experiments that the sizes 6, 7, 13, 15, and 19 are thermodynamically more stable than their neighboring sizes. The spin magnetic moment per atom of Fe{sub n}(n = 2 − 20) clusters is between 2.4 and 3.6 μ{sub B} for the most of the sizes. The antiferromagnetic coupling between the central and the surface atoms of the Fe{sub 13} icosahedron, which have already been reported by experimental and theoretical studies, is verified by our calculations as well. The quantitative disagreements between the calculations and measurements of the magnetic moments of the individual sizes are still to be resolved.« less

The clustering of galaxies in the SDSS-III Baryon Oscillation Spectroscopic Survey: effect of smoothing of density field on reconstruction and anisotropic BAO analysis

NASA Astrophysics Data System (ADS)

Vargas-Magaña, Mariana; Ho, Shirley; Fromenteau, Sebastien.; Cuesta, Antonio. J.

2017-05-01

The reconstruction algorithm introduced by Eisenstein et al., which is widely used in clustering analysis, is based on the inference of the first-order Lagrangian displacement field from the Gaussian smoothed galaxy density field in redshift space. The smoothing scale applied to the density field affects the inferred displacement field that is used to move the galaxies, and partially erases the non-linear evolution of the density field. In this article, we explore this crucial step in the reconstruction algorithm. We study the performance of the reconstruction technique using two metrics: first, we study the performance using the anisotropic clustering, extending previous studies focused on isotropic clustering; secondly, we study its effect on the displacement field. We find that smoothing has a strong effect in the quadrupole of the correlation function and affects the accuracy and precision with which we can measure DA(z) and H(z). We find that the optimal smoothing scale to use in the reconstruction algorithm applied to Baryonic Oscillations Spectroscopic Survey-Constant (stellar) MASS (CMASS) is between 5 and 10 h-1 Mpc. Varying from the `usual' 15-5 h-1 Mpc shows ˜0.3 per cent variations in DA(z) and ˜0.4 per cent H(z) and uncertainties are also reduced by 40 per cent and 30 per cent, respectively. We also find that the accuracy of velocity field reconstruction depends strongly on the smoothing scale used for the density field. We measure the bias and uncertainties associated with different choices of smoothing length.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ben-Naim, Eli; Krapivsky, Paul

Here we generalize the ordinary aggregation process to allow for choice. In ordinary aggregation, two random clusters merge and form a larger aggregate. In our implementation of choice, a target cluster and two candidate clusters are randomly selected and the target cluster merges with the larger of the two candidate clusters.We study the long-time asymptotic behavior and find that as in ordinary aggregation, the size density adheres to the standard scaling form. However, aggregation with choice exhibits a number of different features. First, the density of the smallest clusters exhibits anomalous scaling. Second, both the small-size and the large-size tailsmore » of the density are overpopulated, at the expense of the density of moderate-size clusters. Finally, we also study the complementary case where the smaller candidate cluster participates in the aggregation process and find an abundance of moderate clusters at the expense of small and large clusters. Additionally, we investigate aggregation processes with choice among multiple candidate clusters and a symmetric implementation where the choice is between two pairs of clusters.« less

Note: The performance of new density functionals for a recent blind test of non-covalent interactions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mardirossian, Narbe; Head-Gordon, Martin

Benchmark datasets of non-covalent interactions are essential for assessing the performance of density functionals and other quantum chemistry approaches. In a recent blind test, Taylor et al. benchmarked 14 methods on a new dataset consisting of 10 dimer potential energy curves calculated using coupled cluster with singles, doubles, and perturbative triples (CCSD(T)) at the complete basis set (CBS) limit (80 data points in total). Finally, the dataset is particularly interesting because compressed, near-equilibrium, and stretched regions of the potential energy surface are extensively sampled.

Note: The performance of new density functionals for a recent blind test of non-covalent interactions

DOE PAGES

Mardirossian, Narbe; Head-Gordon, Martin

2016-11-09

Benchmark datasets of non-covalent interactions are essential for assessing the performance of density functionals and other quantum chemistry approaches. In a recent blind test, Taylor et al. benchmarked 14 methods on a new dataset consisting of 10 dimer potential energy curves calculated using coupled cluster with singles, doubles, and perturbative triples (CCSD(T)) at the complete basis set (CBS) limit (80 data points in total). Finally, the dataset is particularly interesting because compressed, near-equilibrium, and stretched regions of the potential energy surface are extensively sampled.

Smallest fullerene-like clusters in two-probe device junctions: first principle study

NASA Astrophysics Data System (ADS)

Kaur, Milanpreet; Sawhney, Ravinder Singh; Engles, Derick

2017-07-01

First principle calculations based on density functional theory are realised to investigate the electron transport of the smallest fullerene-like clusters as two-probe junction devices. The junction devices are constructed by mechanically controlled break junction techniques to ensure the maximum stability of the Be20, B20 and N20 cluster molecular junctions. We investigate the density of states, transmission spectrum, molecular orbitals, current and differential conductance characteristics at discrete bias voltages to gain insight about the various transport phenomena occurring in these nano-junctions. The results show that B20 molecule when stringed to gold electrodes works as an ideal nano-device similar to the pure C20 device and is more symmetric in its characteristic nature. However, in N20 molecular device, the conduction is negligible due to the higher atomic interactions within N20 molecule, despite the fact that it is constructed with penta-valent atoms.

Visualizing Time-Varying Distribution Data in EOS Application

NASA Technical Reports Server (NTRS)

Shen, Han-Wei

2004-01-01

In this research, we have developed several novel visualization methods for spatial probability density function data. Our focus has been on 2D spatial datasets, where each pixel is a random variable, and has multiple samples which are the results of experiments on that random variable. We developed novel clustering algorithms as a means to reduce the information contained in these datasets; and investigated different ways of interpreting and clustering the data.

Applied anatomic site study of palatal anchorage implants using cone beam computed tomography.

PubMed

Lai, Ren-fa; Zou, Hui; Kong, Wei-dong; Lin, Wei

2010-06-01

The purpose of this study was to conduct quantitative research on bone height and bone mineral density of palatal implant sites for implantation, and to provide reference sites for safe and stable palatal implants. Three-dimensional reformatting images were reconstructed by cone beam computed tomography (CBCT) in 34 patients, aged 18 to 35 years, using EZ Implant software. Bone height was measured at 20 sites of interest on the palate. Bone mineral density was measured at the 10 sites with the highest implantation rate, classified using K-mean cluster analysis based on bone height and bone mineral density. According to the cluster analysis, 10 sites were classified into three clusters. Significant differences in bone height and bone mineral density were detected between these three clusters (P<0.05). The greatest bone height was obtained in cluster 2, followed by cluster 1 and cluster 3. The highest bone mineral density was found in cluster 3, followed by cluster 1 and cluster 2. CBCT plays an important role in pre-surgical treatment planning. CBCT is helpful in identifying safe and stable implantation sites for palatal anchorage.

Diagrammatic analysis of correlations in polymer fluids: Cluster diagrams via Edwards' field theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Morse, David C.

2006-10-15

Edwards' functional integral approach to the statistical mechanics of polymer liquids is amenable to a diagrammatic analysis in which free energies and correlation functions are expanded as infinite sums of Feynman diagrams. This analysis is shown to lead naturally to a perturbative cluster expansion that is closely related to the Mayer cluster expansion developed for molecular liquids by Chandler and co-workers. Expansion of the functional integral representation of the grand-canonical partition function yields a perturbation theory in which all quantities of interest are expressed as functionals of a monomer-monomer pair potential, as functionals of intramolecular correlation functions of non-interacting molecules,more » and as functions of molecular activities. In different variants of the theory, the pair potential may be either a bare or a screened potential. A series of topological reductions yields a renormalized diagrammatic expansion in which collective correlation functions are instead expressed diagrammatically as functionals of the true single-molecule correlation functions in the interacting fluid, and as functions of molecular number density. Similar renormalized expansions are also obtained for a collective Ornstein-Zernicke direct correlation function, and for intramolecular correlation functions. A concise discussion is given of the corresponding Mayer cluster expansion, and of the relationship between the Mayer and perturbative cluster expansions for liquids of flexible molecules. The application of the perturbative cluster expansion to coarse-grained models of dense multi-component polymer liquids is discussed, and a justification is given for the use of a loop expansion. As an example, the formalism is used to derive a new expression for the wave-number dependent direct correlation function and recover known expressions for the intramolecular two-point correlation function to first-order in a renormalized loop expansion for coarse-grained models of binary homopolymer blends and diblock copolymer melts.« less

CO2 adsorption on gas-phase Cu4-xPtx (x = 0-4) clusters: a DFT study.

PubMed

Gálvez-González, Luis E; Juárez-Sánchez, J Octavio; Pacheco-Contreras, Rafael; Garzón, Ignacio L; Paz-Borbón, Lauro Oliver; Posada-Amarillas, Alvaro

2018-06-13

Transition and noble metal clusters have proven to be critical novel materials, potentially offering major advantages over conventional catalysts in a range of value-added catalytic processess such as carbon dioxide transformation to methanol. In this work, a systematic computational study of CO2 adsorption on gas-phase Cu4-xPtx (x = 0-4) clusters is performed. An exhaustive potential energy surface exploration is initially performed using our recent density functional theory basin-hopping global optimization implementation. Ground-state and low-lying energy isomers are identified for Cu4-xPtx clusters. Secondly, a CO2 molecule adsorption process is analyzed on the ground-state Cu4-xPtx configurations, as a function of cluster composition. Our results show that the gas-phase linear CO2 molecule is deformed upon adsorption, with its bend angle varying from about 132° to 139°. Cu4-xPtx cluster geometries remain unchanged after CO2 adsorption, with the exception of Cu3Pt1 and Pt4 clusters. For these particular cases, a structural conversion between the ground-state geometry and the corresponding first isomer configurations is found to be assisted by the CO2 adsorption. For all clusters, the energy barriers between the ground-state and first isomer structures are explored. Our calculated CO2 adsorption energies are found to be larger for Pt-rich clusters, exhibiting a volcano-type plot. The overall effect of a hybrid functional including dispersion forces is also discussed.

Extracting Galaxy Cluster Gas Inhomogeneity from X-Ray Surface Brightness: A Statistical Approach and Application to Abell 3667

NASA Astrophysics Data System (ADS)

Kawahara, Hajime; Reese, Erik D.; Kitayama, Tetsu; Sasaki, Shin; Suto, Yasushi

2008-11-01

Our previous analysis indicates that small-scale fluctuations in the intracluster medium (ICM) from cosmological hydrodynamic simulations follow the lognormal probability density function. In order to test the lognormal nature of the ICM directly against X-ray observations of galaxy clusters, we develop a method of extracting statistical information about the three-dimensional properties of the fluctuations from the two-dimensional X-ray surface brightness. We first create a set of synthetic clusters with lognormal fluctuations around their mean profile given by spherical isothermal β-models, later considering polytropic temperature profiles as well. Performing mock observations of these synthetic clusters, we find that the resulting X-ray surface brightness fluctuations also follow the lognormal distribution fairly well. Systematic analysis of the synthetic clusters provides an empirical relation between the three-dimensional density fluctuations and the two-dimensional X-ray surface brightness. We analyze Chandra observations of the galaxy cluster Abell 3667, and find that its X-ray surface brightness fluctuations follow the lognormal distribution. While the lognormal model was originally motivated by cosmological hydrodynamic simulations, this is the first observational confirmation of the lognormal signature in a real cluster. Finally we check the synthetic cluster results against clusters from cosmological hydrodynamic simulations. As a result of the complex structure exhibited by simulated clusters, the empirical relation between the two- and three-dimensional fluctuation properties calibrated with synthetic clusters when applied to simulated clusters shows large scatter. Nevertheless we are able to reproduce the true value of the fluctuation amplitude of simulated clusters within a factor of 2 from their two-dimensional X-ray surface brightness alone. Our current methodology combined with existing observational data is useful in describing and inferring the statistical properties of the three-dimensional inhomogeneity in galaxy clusters.

On-top density functionals for the short-range dynamic correlation between electrons of opposite and parallel spin

NASA Astrophysics Data System (ADS)

Hollett, Joshua W.; Pegoretti, Nicholas

2018-04-01

Separate, one-parameter, on-top density functionals are derived for the short-range dynamic correlation between opposite and parallel-spin electrons, in which the electron-electron cusp is represented by an exponential function. The combination of both functionals is referred to as the Opposite-spin exponential-cusp and Fermi-hole correction (OF) functional. The two parameters of the OF functional are set by fitting the ionization energies and electron affinities, of the atoms He to Ar, predicted by ROHF in combination with the OF functional to the experimental values. For ionization energies, the overall performance of ROHF-OF is better than completely renormalized coupled-cluster [CR-CC(2,3)] and better than, or as good as, conventional density functional methods. For electron affinities, the overall performance of ROHF-OF is less impressive. However, for both ionization energies and electron affinities of third row atoms, the mean absolute error of ROHF-OF is only 3 kJ mol-1.

The Ursa Major cluster of galaxies - III. Optical observations of dwarf galaxies and the luminosity function down to MR=-11

NASA Astrophysics Data System (ADS)

Trentham, Neil; Tully, R. Brent; Verheijen, Marc A. W.

2001-07-01

Results are presented of a deep optical survey of the Ursa Major cluster, a spiral-rich cluster of galaxies at a distance of 18.6Mpc which contains about 30 per cent of the light but only 5 per cent of the mass of the nearby Virgo cluster. Fields around known cluster members and a pattern of blind fields along the major and minor axes of the cluster were studied with mosaic CCD cameras on the Canada-France-Hawaii Telescope. The dynamical crossing time for the Ursa Major cluster is only slightly less than a Hubble time. Most galaxies in the local Universe exist in similar moderate-density environments. The Ursa Major cluster is therefore a good place to study the statistical properties of dwarf galaxies, since this structure is at an evolutionary stage representative of typical environments, yet has enough galaxies that reasonable counting statistics can be accumulated. The main observational results of our survey are as follows. (i) The galaxy luminosity function is flat, with a logarithmic slope α=-1.1 for -17

Insight from first principles into the stability and magnetism of alkali-metal superoxide nanoclusters

NASA Astrophysics Data System (ADS)

Arcelus, Oier; Suaud, Nicolas; Katcho, Nebil A.; Carrasco, Javier

2017-05-01

Alkali-metal superoxides are gaining increasing interest as 2p magnetic materials for information and energy storage. Despite significant research efforts on bulk materials, gaps in our knowledge of the electronic and magnetic properties at the nanoscale still remain. Here, we focused on the role that structural details play in determining stability, electronic structure, and magnetic couplings of (MO2)n (M = Li, Na, and K, with n = 2-8) clusters. Using first-principles density functional theory based on the Perdew-Burke-Ernzerhof and Heyd-Scuseria-Ernzerhof functionals, we examined the effect of atomic structure on the relative stability of different polymorphs within each investigated cluster size. We found that small clusters prefer to form planar-ring structures, whereas non-planar geometries become more stable when increasing the cluster size. However, the crossover point depends on the nature of the alkali metal. Our analysis revealed that electrostatic interactions govern the highly ionic M-O2 bonding and ultimately control the relative stability between 2-D and 3-D geometries. In addition, we analyzed the weak magnetic couplings between superoxide molecules in (NaO2)4 clusters comparing model Hamiltonian methods based on Wannier function projections onto πg states with wave function-based multi-reference calculations.

Subsystem real-time time dependent density functional theory.

PubMed

Krishtal, Alisa; Ceresoli, Davide; Pavanello, Michele

2015-04-21

We present the extension of Frozen Density Embedding (FDE) formulation of subsystem Density Functional Theory (DFT) to real-time Time Dependent Density Functional Theory (rt-TDDFT). FDE is a DFT-in-DFT embedding method that allows to partition a larger Kohn-Sham system into a set of smaller, coupled Kohn-Sham systems. Additional to the computational advantage, FDE provides physical insight into the properties of embedded systems and the coupling interactions between them. The extension to rt-TDDFT is done straightforwardly by evolving the Kohn-Sham subsystems in time simultaneously, while updating the embedding potential between the systems at every time step. Two main applications are presented: the explicit excitation energy transfer in real time between subsystems is demonstrated for the case of the Na4 cluster and the effect of the embedding on optical spectra of coupled chromophores. In particular, the importance of including the full dynamic response in the embedding potential is demonstrated.

Galaxies at the Extremes: Ultradiffuse Galaxies in the Virgo Cluster

NASA Astrophysics Data System (ADS)

Mihos, Chris

2017-08-01

The ultradiffuse galaxies (UDGs) recently discovered in massive galaxy clusters presents both challenges and opportunities for our understanding of galaxy evolution in dense clusters. Such large, low density galaxies should be most vulnerable to gravitational destruction within the cluster environment. Thus their presence in cluster cores argues either that they must be stabilized by massive dark halos or else be short-lived objects undergoing rapid transformation, perhaps leading to the formation of ultracompact dwarf galaxies (UCDs) if their destruction leaves only a compact nucleus behind. We propose deep imaging of four Virgo Cluster UDGs to probe their local environment within Virgo via accurate tip of the red giant branch (TRGB) distances. With a distance precision of 1 Mpc, we will accurately place the objects in the Virgo core, cluster outskirts, or intervening field. When coupled with our extant kinematic data, we can determine whether they are infalling objects or instead have already passed through the cluster core. We will also compare their compact nuclei to Virgo UCDs, and study their globular cluster (GC) populations in detail. Probing three magnitudes beyond the turnover in the GC luminosity function, we will construct larger and cleaner GC samples than possible with ground-based imaging, using the total mass and radial extent of the globular cluster systems to estimate the dark halo mass and tidal radius for each UDG. The new information provided by HST about the local environment and intrinsic properties of these Virgo UDGs will be used in conjunction with simulation data to study cluster-driven evolution and transformation of low density galaxies.

A DFT study on surface-enhanced Raman spectroscopy of aromatic dithiol derivatives adsorbed on gold nanojunctions

NASA Astrophysics Data System (ADS)

You, Tingting; Lang, Xiufeng; Huang, Anping; Yin, Penggang

2018-01-01

A computational study on aromatic dithiol derivatives (HS-Ar-X-Ar-SH, X = O, S, Se, NH, CH2, Ndbnd N, CHdbnd CH, Ctbnd C) interacting with gold cluster(s) was presented to investigate the chemical enhancement mechanism related to surface-enhanced Raman spectroscopy (SERS) for molecular junctions. Density functional theory (DFT) were performed on derivatives molecules as well as their single-end-linked (SEL) or double-end-linked (DEL) complexes for geometric, spectra, electronic and excitation properties, leading to discussions on dominant factor during SERS process. The resulted enhancement factors of SEL and DEL complexes exhibited specific dependency on linking atom or functional group between two phenyls, which was in accordance with the variation of polarizabilities and molecule-cluster transition energy.

First principles calculations for interaction of tyrosine with (ZnO)3 cluster

NASA Astrophysics Data System (ADS)

Singh, Satvinder; Singh, Gurinder; Kaura, Aman; Tripathi, S. K.

2018-04-01

First Principles Calculations have been performed to study interactions of Phenol ring of Tyrosine (C6H5OH) with (ZnO)3 atomic cluster. All the calculations have been performed under the Density Functional Theory (DFT) framework. Structural and electronic properties of (ZnO)3/C6H5OH have been studied. Gaussian basis set approach has been adopted for the calculations. A ring type most stable (ZnO)3 atomic cluster has been modeled, analyzed and used for the calculations. The compatibility of the results with previous studies has been presented here.

Remarkable Second-Order Optical Nonlinearity of Nano-Sized Au Cluster: A TDDFT Study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Kechen; Li, Jun; Lin, Chensheng

2004-04-21

The dipole polarizability, static first hyperpolarizability, and UV-vis spectrum of the recently identified nano-sized tetrahedral cluster of Au have been investigated by using time-dependent density functional response theory. We have discovered that the Au cluster possesses remarkably large molecular second-order optical nonlinearity with the first hyperpolarizabilty (xyz) calculated to be 14.3 x 10 electrostatic unit (esu). The analysis of the low-energy absorption band suggests that the charge transfer from the edged gold atoms to the vertex ones plays the key role in nonlinear optical (NLO) response of Au.

On the statistics of proto-cluster candidates detected in the Planck all-sky survey

NASA Astrophysics Data System (ADS)

Negrello, M.; Gonzalez-Nuevo, J.; De Zotti, G.; Bonato, M.; Cai, Z.-Y.; Clements, D.; Danese, L.; Dole, H.; Greenslade, J.; Lapi, A.; Montier, L.

2017-09-01

Observational investigations of the abundance of massive precursors of local galaxy clusters ('proto-clusters') allow us to test the growth of density perturbations, to constrain cosmological parameters that control it, to test the theory of non-linear collapse and how the galaxy formation takes place in dense environments. The Planck collaboration has recently published a catalogue of ≳2000 cold extragalactic sub-millimeter sources, I.e. with colours indicative of z ≳ 2, almost all of which appear to be overdensities of star-forming galaxies. They are thus considered as proto-cluster candidates. Their number densities (or their flux densities) are far in excess of expectations from the standard scenario for the evolution of large-scale structure. Simulations based on a physically motivated galaxy evolution model show that essentially all cold peaks brighter than S545GHz = 500 mJy found in Planck maps after having removed the Galactic dust emission can be interpreted as positive Poisson fluctuations of the number of high-z dusty proto-clusters within the same Planck beam, rather then being individual clumps of physically bound galaxies. This conclusion does not change if an empirical fit to the luminosity function of dusty galaxies is used instead of the physical model. The simulations accurately reproduce the statistic of the Planck detections and yield distributions of sizes and ellipticities in qualitative agreement with observations. The redshift distribution of the brightest proto-clusters contributing to the cold peaks has a broad maximum at 1.5 ≤ z ≤ 3. Therefore follow-up of Planck proto-cluster candidates will provide key information on the high-z evolution of large scale structure.

Novel density-based and hierarchical density-based clustering algorithms for uncertain data.

PubMed

Zhang, Xianchao; Liu, Han; Zhang, Xiaotong

2017-09-01

Uncertain data has posed a great challenge to traditional clustering algorithms. Recently, several algorithms have been proposed for clustering uncertain data, and among them density-based techniques seem promising for handling data uncertainty. However, some issues like losing uncertain information, high time complexity and nonadaptive threshold have not been addressed well in the previous density-based algorithm FDBSCAN and hierarchical density-based algorithm FOPTICS. In this paper, we firstly propose a novel density-based algorithm PDBSCAN, which improves the previous FDBSCAN from the following aspects: (1) it employs a more accurate method to compute the probability that the distance between two uncertain objects is less than or equal to a boundary value, instead of the sampling-based method in FDBSCAN; (2) it introduces new definitions of probability neighborhood, support degree, core object probability, direct reachability probability, thus reducing the complexity and solving the issue of nonadaptive threshold (for core object judgement) in FDBSCAN. Then, we modify the algorithm PDBSCAN to an improved version (PDBSCANi), by using a better cluster assignment strategy to ensure that every object will be assigned to the most appropriate cluster, thus solving the issue of nonadaptive threshold (for direct density reachability judgement) in FDBSCAN. Furthermore, as PDBSCAN and PDBSCANi have difficulties for clustering uncertain data with non-uniform cluster density, we propose a novel hierarchical density-based algorithm POPTICS by extending the definitions of PDBSCAN, adding new definitions of fuzzy core distance and fuzzy reachability distance, and employing a new clustering framework. POPTICS can reveal the cluster structures of the datasets with different local densities in different regions better than PDBSCAN and PDBSCANi, and it addresses the issues in FOPTICS. Experimental results demonstrate the superiority of our proposed algorithms over the existing algorithms in accuracy and efficiency. Copyright © 2017 Elsevier Ltd. All rights reserved.

Conjugate-gradient optimization method for orbital-free density functional calculations.

PubMed

Jiang, Hong; Yang, Weitao

2004-08-01

Orbital-free density functional theory as an extension of traditional Thomas-Fermi theory has attracted a lot of interest in the past decade because of developments in both more accurate kinetic energy functionals and highly efficient numerical methodology. In this paper, we developed a conjugate-gradient method for the numerical solution of spin-dependent extended Thomas-Fermi equation by incorporating techniques previously used in Kohn-Sham calculations. The key ingredient of the method is an approximate line-search scheme and a collective treatment of two spin densities in the case of spin-dependent extended Thomas-Fermi problem. Test calculations for a quartic two-dimensional quantum dot system and a three-dimensional sodium cluster Na216 with a local pseudopotential demonstrate that the method is accurate and efficient. (c) 2004 American Institute of Physics.

Ultra-small Ag clusters in zeolite A4: Antibacterial and thermochromic applications

NASA Astrophysics Data System (ADS)

Horta-Fraijo, P.; Cortez-Valadez, M.; Flores-Lopez, N. S.; Britto Hurtado, R.; Vargas-Ortiz, R. A.; Perez-Rodriguez, A.; Flores-Acosta, M.

2018-03-01

The physical and chemical properties of metal clusters depend on their atomic structure, therefore, it is important to determine the lowest-energy structures of the clusters in order to understand and utilize their properties. In this work, we use the Density Functional Theory (DFT) at the generalized gradient approximation level Becke's three-parameter and the gradient corrected functional of Lee, Yang and Puar (B3LYP) in combination with the basis set LANL2DZ (the effective core potentials and associated double-zeta valence) to determine some of the structural, electronic and vibrational properties of the planar silver clusters (Agn clusters n = 2-24). Additionally, the study reports the experimental synthesis of small silver clusters in synthetic zeolite A4. The synthesis was possible using the ion exchange method with some precursors like silver nitrate (AgNO3) and synthetic zeolite A4. The silver clusters in zeolite powder underwent thermal treatment at 450 °C to release the remaining water or humidity on it. The morphology of the particles was determined by Transmission Electron microscopy. The nanomaterials obtained show thermochromic properties. The structural parameters were correlated theoretically and experimentally.

Abnormal characteristics of binary molecular clusters in DMSO–ethanol mixtures under external electric fields

NASA Astrophysics Data System (ADS)

Wu, Zhiyan; Huang, Kama

2018-05-01

For the nonlinearly phenomena on the dielectric properties of dimethyl sulfoxide (DMSO)-ethanol mixtures under a low intensity microwave field, we propose a conjecture that there exist some abnormal molecular clusters. To interpret the mechanism of abnormal phenomena and confirm our conjecture about the existence of abnormal molecular clusters, an in-depth investigation about the structure evolutions of (DMSO)m(C2H5OH)n (m = 0-4; n = 0-4; m + n ≤ 4) molecular clusters induced by external electric fields has been given by using density functional theory. The results show that there exist some binary molecular clusters with large cluster radii in mixtures, and some of them are unstable under exposure of electric fields. It implies that the existence of certain abnormal molecular clusters in DMSO-ethanol mixtures results in their abnormality of dielectric properties.

Structural study of gold clusters.

PubMed

Xiao, Li; Tollberg, Bethany; Hu, Xiankui; Wang, Lichang

2006-03-21

Density functional theory (DFT) calculations were carried out to study gold clusters of up to 55 atoms. Between the linear and zigzag monoatomic Au nanowires, the zigzag nanowires were found to be more stable. Furthermore, the linear Au nanowires of up to 2 nm are formed by slightly stretched Au dimers. These suggest that a substantial Peierls distortion exists in those structures. Planar geometries of Au clusters were found to be the global minima till the cluster size of 13. A quantitative correlation is provided between various properties of Au clusters and the structure and size. The relative stability of selected clusters was also estimated by the Sutton-Chen potential, and the result disagrees with that obtained from the DFT calculations. This suggests that a modification of the Sutton-Chen potential has to be made, such as obtaining new parameters, in order to use it to search the global minima for bigger Au clusters.

A model for sputtering from solid surfaces bombarded by energetic clusters

NASA Astrophysics Data System (ADS)

Benguerba, Messaoud

2018-04-01

A model is developed to explain and predict the sputtering from solid surfaces bombarded by energetic clusters, on the basis of shock wave generated at the impact of cluster. Under the shock compression the temperature increases causing the vaporization of material that requires an internal energy behind the shock, at least, of about twice the cohesive energy of target. The sputtering is treated as a gas of vaporized particles from a hemispherical volume behind the shock front. The sputter yield per cluster atoms is given as a universal function depending on the ratio of target to cluster atomic density and the ratio of cluster velocity to the velocity calculated on the basis of an internal energy equals about twice cohesive energy. The predictions of the model for self sputter yield of copper, gold, tungsten and of silver bombarded by C60 clusters agree well, with the corresponding data simulated by molecular dynamics.

Clustering the Orion B giant molecular cloud based on its molecular emission

PubMed Central

Bron, Emeric; Daudon, Chloé; Pety, Jérôme; Levrier, François; Gerin, Maryvonne; Gratier, Pierre; Orkisz, Jan H.; Guzman, Viviana; Bardeau, Sébastien; Goicoechea, Javier R.; Liszt, Harvey; Öberg, Karin; Peretto, Nicolas; Sievers, Albrecht; Tremblin, Pascal

2017-01-01

Context Previous attempts at segmenting molecular line maps of molecular clouds have focused on using position-position-velocity data cubes of a single molecular line to separate the spatial components of the cloud. In contrast, wide field spectral imaging over a large spectral bandwidth in the (sub)mm domain now allows one to combine multiple molecular tracers to understand the different physical and chemical phases that constitute giant molecular clouds (GMCs). Aims We aim at using multiple tracers (sensitive to different physical processes and conditions) to segment a molecular cloud into physically/chemically similar regions (rather than spatially connected components), thus disentangling the different physical/chemical phases present in the cloud. Methods We use a machine learning clustering method, namely the Meanshift algorithm, to cluster pixels with similar molecular emission, ignoring spatial information. Clusters are defined around each maximum of the multidimensional Probability Density Function (PDF) of the line integrated intensities. Simple radiative transfer models were used to interpret the astrophysical information uncovered by the clustering analysis. Results A clustering analysis based only on the J = 1 – 0 lines of three isotopologues of CO proves suffcient to reveal distinct density/column density regimes (nH ~ 100 cm−3, ~ 500 cm−3, and > 1000 cm−3), closely related to the usual definitions of diffuse, translucent and high-column-density regions. Adding two UV-sensitive tracers, the J = 1 − 0 line of HCO+ and the N = 1 − 0 line of CN, allows us to distinguish two clearly distinct chemical regimes, characteristic of UV-illuminated and UV-shielded gas. The UV-illuminated regime shows overbright HCO+ and CN emission, which we relate to a photochemical enrichment effect. We also find a tail of high CN/HCO+ intensity ratio in UV-illuminated regions. Finer distinctions in density classes (nH ~ 7 × 103 cm−3 ~ 4 × 104 cm−3) for the densest regions are also identified, likely related to the higher critical density of the CN and HCO+ (1 – 0) lines. These distinctions are only possible because the high-density regions are spatially resolved. Conclusions Molecules are versatile tracers of GMCs because their line intensities bear the signature of the physics and chemistry at play in the gas. The association of simultaneous multi-line, wide-field mapping and powerful machine learning methods such as the Meanshift clustering algorithm reveals how to decode the complex information available in these molecular tracers. PMID:29456256

Dynamic Harris current sheet thickness from Cluster current density and plasma measurements

NASA Technical Reports Server (NTRS)

Thompson, S. M.; Kivelson, M. G.; Khurana, K. K.; McPherron, R. L.; Weygand, J. M.; Balogh, A.; Reme, H.; Kistler, L. M.

2005-01-01

We use the first accurate measurements of current densities in the plasma sheet to calculate the half-thickness and position of the current sheet as a function of time. Our technique assumes a Harris current sheet model, which is parameterized by lobe magnetic field B(o), current sheet half-thickness h, and current sheet position z(sub o). Cluster measurements of magnetic field, current density, and plasma pressure are used to infer the three parameters as a function of time. We find that most long timescale (6-12 hours) current sheet crossings observed by Cluster cannot be described by a static Harris current sheet with a single set of parameters B(sub o), h, and z(sub o). Noting the presence of high-frequency fluctuations that appear to be superimposed on lower frequency variations, we average over running 6-min intervals and use the smoothed data to infer the parameters h(t) and z(sub o)(t), constrained by the pressure balance lobe magnetic field B(sub o)(t). Whereas this approach has been used in previous studies, the spatial gnuhen& now provided by the Cluster magnetometers were unavailable or not well constrained in earlier studies. We place the calculated hdf&cknessa in a magnetospheric context by examining the change in thickness with substorm phase for three case study events and 21 events in a superposed epoch analysis. We find that the inferred half-thickness in many cases reflects the nominal changes experienced by the plasma sheet during substorms (i.e., thinning during growth phase, thickening following substorm onset). We conclude with an analysis of the relative contribution of (Delta)B(sub z)/(Delta)X to the cross-tail current density during substorms. We find that (Delta)B(sub z)/(Delta)X can contribute a significant portion of the cross-tail c m n t around substorm onset.

The JCMT Gould Belt Survey: Dense Core Clusters in Orion B

NASA Astrophysics Data System (ADS)

Kirk, H.; Johnstone, D.; Di Francesco, J.; Lane, J.; Buckle, J.; Berry, D. S.; Broekhoven-Fiene, H.; Currie, M. J.; Fich, M.; Hatchell, J.; Jenness, T.; Mottram, J. C.; Nutter, D.; Pattle, K.; Pineda, J. E.; Quinn, C.; Salji, C.; Tisi, S.; Hogerheijde, M. R.; Ward-Thompson, D.; The JCMT Gould Belt Survey Team

2016-04-01

The James Clerk Maxwell Telescope Gould Belt Legacy Survey obtained SCUBA-2 observations of dense cores within three sub-regions of Orion B: LDN 1622, NGC 2023/2024, and NGC 2068/2071, all of which contain clusters of cores. We present an analysis of the clustering properties of these cores, including the two-point correlation function and Cartwright’s Q parameter. We identify individual clusters of dense cores across all three regions using a minimal spanning tree technique, and find that in each cluster, the most massive cores tend to be centrally located. We also apply the independent M-Σ technique and find a strong correlation between core mass and the local surface density of cores. These two lines of evidence jointly suggest that some amount of mass segregation in clusters has happened already at the dense core stage.

Theoretical Prediction of Si 2–Si 33 Absorption Spectra

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhao, Li -Zhen; Lu, Wen -Cai; Qin, Wei

Here, the optical absorption spectra of Si 2–Si 33 clusters were systematically studied by a time-dependent density functional theory approach. The calculations revealed that the absorption spectrum becomes significantly broad with increasing cluster size, stretching from ultraviolet to the infrared region. The absorption spectra are closely related to the structural motifs. With increasing cluster size, the absorption intensity of cage structures gradually increases, but the absorption curves of the prolate and the Y-shaped structures are very sensitive to cluster size. If the transition energy reaches ~12 eV, it is noted that all the clusters have remarkable absorption in deep ultravioletmore » region of 100–200 nm, and the maximum absorption intensity is ~100 times that in the visible region. Further, the optical responses to doping in the Si clusters were studied.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yu, Chongqi; Harbich, Wolfgang; Sementa, Luca

Ligand-protected Au clusters are non-bleaching fluorescence markers in bio- and medical applications. We show that their fluorescence is an intrinsic property of the Au cluster itself. We find a very intense and sharp fluorescence peak located at λ =739.2 nm (1.68 eV) for Au20 clusters in a Ne matrix held at 6 K. The fluorescence reflects the HOMO-LUMO diabatic bandgap of the cluster. The cluster shows a very rich absorption fine structure reminiscent of well defined molecule-like quantum levels. These levels are resolved since Au20 has only one stable isomer (tetrahedral), therefore our sample is mono-disperse in cluster size andmore » conformation. Density-functional theory (DFT) and time-dependent DFT calculations clarify the nature of optical absorptionand predict both main absorption peaks and intrinsic fluorescence in good agreement with experiment.« less

Theoretical Prediction of Si 2–Si 33 Absorption Spectra

DOE PAGES

Zhao, Li -Zhen; Lu, Wen -Cai; Qin, Wei; ...

2017-07-07

Here, the optical absorption spectra of Si 2–Si 33 clusters were systematically studied by a time-dependent density functional theory approach. The calculations revealed that the absorption spectrum becomes significantly broad with increasing cluster size, stretching from ultraviolet to the infrared region. The absorption spectra are closely related to the structural motifs. With increasing cluster size, the absorption intensity of cage structures gradually increases, but the absorption curves of the prolate and the Y-shaped structures are very sensitive to cluster size. If the transition energy reaches ~12 eV, it is noted that all the clusters have remarkable absorption in deep ultravioletmore » region of 100–200 nm, and the maximum absorption intensity is ~100 times that in the visible region. Further, the optical responses to doping in the Si clusters were studied.« less

Ab initio structures and polarizabilities of sodium clusters

NASA Astrophysics Data System (ADS)

Kronik, Leeor; Vasiliev, Igor; Jain, Manish; Chelikowsky, James R.

2001-09-01

We present quantitative ab initio calculations for Na cluster structures and polarizabilities, for all cluster sizes up to 20 atoms. Our calculations are performed by combining an ab initio core-corrected pseudopotential and a gradient-corrected density functional within a real space approach. We find the cluster bonding to be very floppy and catalog a host of low-energy quasi-degenerate isomers for all second-decade clusters. The existence of these isomers results in a band of polarizability values for each cluster size even at zero temperature. This eliminates any finer structure in the polarizability curve. We further show that the experimental polarizability values are consistently underestimated by calculations at zero temperature. By computing the effects of structure expansion and distortion due to a finite temperature we arrive at a quantitative agreement between theory and experiment.

Structure and vibrational spectra of low-energy silicon clusters

NASA Astrophysics Data System (ADS)

Sieck, A.; Porezag, D.; Frauenheim, Th.; Pederson, M. R.; Jackson, K.

1997-12-01

We have identified low-energy structures of silicon clusters with 9 to 14 atoms using a nonorthogonal tight-binding method (TB) based on density-functional theory (DF). We have further investigated the resulting structures with an accurate all-electron first-principles technique. The results for cohesive energies, cluster geometries, and highest occupied to lowest unoccupied molecular orbital (HOMO-LUMO) gaps show an overall good agreement between DF-TB and self-consistent-field (SCF) DF theory. For Si9 and Si14, we have found equilibrium structures, whereas for Si11, Si12, and Si13, we present clusters with energies close to that of the corresponding ground-state structure recently proposed in the literature. The bonding scheme of clusters in this size range is different from the bulk tetrahedral symmetry. The most stable structures, characterized by low energies and large HOMO-LUMO gaps, have similar common subunits. To aid in their experimental identification, we have computed the full vibrational spectra of the structures, along with the Raman activities, IR intensities, and static polarizabilities, using SCF-DF theory within the local-density approximation (LDA). This method has already been successfully applied to the determination of Raman and IR spectra of silicon clusters with 3-8, 10, 13, 20, and 21 atoms.

Estimating metallicities with isochrone fits to photometric data of open clusters

NASA Astrophysics Data System (ADS)

Monteiro, H.; Oliveira, A. F.; Dias, W. S.; Caetano, T. C.

2014-10-01

The metallicity is a critical parameter that affects the correct determination of stellar cluster's fundamental characteristics and has important implications in Galactic and Stellar evolution research. Fewer than 10% of the 2174 currently catalogued open clusters have their metallicity determined in the literature. In this work we present a method for estimating the metallicity of open clusters via non-subjective isochrone fitting using the cross-entropy global optimization algorithm applied to UBV photometric data. The free parameters distance, reddening, age, and metallicity are simultaneously determined by the fitting method. The fitting procedure uses weights for the observational data based on the estimation of membership likelihood for each star, which considers the observational magnitude limit, the density profile of stars as a function of radius from the center of the cluster, and the density of stars in multi-dimensional magnitude space. We present results of [Fe/H] for well-studied open clusters based on distinct UBV data sets. The [Fe/H] values obtained in the ten cases for which spectroscopic determinations were available in the literature agree, indicating that our method provides a good alternative to estimating [Fe/H] by using an objective isochrone fitting. Our results show that the typical precision is about 0.1 dex.

[Density functional theory studies on structure and spectrum of Cu3 Ti cluster].

PubMed

Wei, Yong-Hui; Cheng, Jian-Bo; Zhao, Bing; Lombardi, John R

2008-07-01

Bulk intermetallic Ti-Cu compounds have been found to possess special properties, including increased hardness, as well as displaying enhanced sound absorption and e shape memory. Since only one Raman progression is observed, there is not sufficient information to determine the structure of TiCu3. The different structures and vibrational frequencies of the Cu3 Ti cluster were studied by means of the density functional theory with SVWN5, B3LYP and BPW91 methods at basis sets of lanl2dz, 6-31g, 6-311g, 6-311g(d), 6-311 +/- g(2df) and 6-311 +/- g(3d2f). The calculated results show that the ground state of the Cu3 Ti cluster is a e-type structure with the C2v point group symmetry, and the bond lengths and vibrational frequencies of Cu3 T are considerably dependent on the variation of basis sets. We observed only a single Raman progression in approximately 300 cm(-1). This progression is most likely the totally symmetric stretch. The computed and observed Raman spectra were also compared with each other.

Application of B{sub 12}N{sub 12} and B{sub 12}P{sub 12} as two fullerene-like semiconductors for adsorption of halomethane: Density functional theory study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rad, Ali Shokuhi, E-mail: a.shokuhi@gmail.com

We examined and discussed the interaction of two halomethanes (mono-chloromethane (MCM), and mono-fluoromethane (MFM)) with B{sub 12}N{sub 12} and B{sub 12}P{sub 12} fullerene-like nanocages as semiconductor based on density functional theory (DFT). We calculated adsorption energies and followed the changes in the electronic structure of semiconductors upon adsorption of MCM and MFM. We found that the adsorption on the B{sub 12}N{sub 12} nano-cluster is energetically more favorable compared to B{sub 12}P{sub 12} nano-cluster. Also for both systems we found higher values of adsorption energy for MFM than for MCM. We found that upon adsorption of above-mentioned species on these twomore » fullerene-like semiconductors, the HOMO–LUMO distributions and also the gap energy for each system did not change significantly, which correspond to the physisorption process. As a result, B{sub 12}N{sub 12} is a more appropriate nano-cluster to be used as a selective sensor for halomethanes, especially for MFM.« less

The neutron skin thickness in nuclei with clustering at low densities

NASA Astrophysics Data System (ADS)

Nooraihan, A.; Usmani, Q. N.; Sauli, Z.; Anwar, K.

2016-11-01

This study concentrates on searching for a dependable, fully microscopic theory to find out new behaviours and understand their consequences for theoretical pictures. The models for nuclear structure are tested, refined and developed by acquiring new data [1][2][3]. This data is useful for astrophysical calculations and predictions. In density functional theories, including the ETF theory, the equation of state (EOS) of symmetric nuclear matter (SNM), is an important measure. Empirically, we receive information about quantities relating to SNM, all these measures are thoroughly tested. In the absence of any unswerving knowledge below this density we shall take that energy still rises up to some density, neglecting possible small fluctuations, as the density is brought down. Our discussion at the moment is without the Coulomb forces applicable only for the hypothetical nuclear matter; they are added finally to correctly portray the actual picture in nuclei. Our approach in this study is macroscopic. This work concludes that the neutron skin thickness in nuclei is found to reduce significantly, for the reason of clustering.

Probing Metal Cluster and Metal Oxide Cluster Interactions with Organo-Sulfur and Organo-Phosphorous Molecules using Mass Spectrometry and Anion PES

DTIC Science & Technology

2002-10-30

atomic anions and methanol: Anion photoelectron spectroscopy and density functional theory calculations on HNiCO-, PdCO - and PtCO-,” Bappaditya...HNiC2H, Ni(C2H)2, PdCO , PdCN, PdC2H, PtCO, PtCN, PtC2H), they are not included in this report, but can be found in the papers cited above. PE

Kinetics of Aggregation with Choice

DOE PAGES

Ben-Naim, Eli; Krapivsky, Paul

2016-12-01

Here we generalize the ordinary aggregation process to allow for choice. In ordinary aggregation, two random clusters merge and form a larger aggregate. In our implementation of choice, a target cluster and two candidate clusters are randomly selected and the target cluster merges with the larger of the two candidate clusters.We study the long-time asymptotic behavior and find that as in ordinary aggregation, the size density adheres to the standard scaling form. However, aggregation with choice exhibits a number of different features. First, the density of the smallest clusters exhibits anomalous scaling. Second, both the small-size and the large-size tailsmore » of the density are overpopulated, at the expense of the density of moderate-size clusters. Finally, we also study the complementary case where the smaller candidate cluster participates in the aggregation process and find an abundance of moderate clusters at the expense of small and large clusters. Additionally, we investigate aggregation processes with choice among multiple candidate clusters and a symmetric implementation where the choice is between two pairs of clusters.« less

Photoelectron spectroscopy and density functional theory study of TiAlO(y) (-) (y=1-3) and TiAl(2)O(y) (-) (y=2-3) clusters.

PubMed

Zhang, Zeng-Guang; Xu, Hong-Guang; Zhao, Yuchao; Zheng, Weijun

2010-10-21

Small titanium-aluminum oxide clusters, TiAlO(y) (-) (y=1-3) and TiAl(2)O(y) (-) (y=2-3), were studied by using anion photoelectron spectroscopy. The adiabatic detachment energies of TiAlO(y) (-) (y=1-3) were estimated to be 1.11±0.05, 1.70±0.08, and 2.47±0.08eV based on their photoelectron spectra; those of TiAl(2)O(2) (-) and TiAl(2)O(3) (-) were estimated to be 1.17±0.08 and 2.2±0.1eV, respectively. The structures of these clusters were determined by comparison of density functional calculations with the experimental results. The structure of TiAlO(-) is nearly linear with the O atom in the middle. That of TiAlO(2) (-) is a kite-shaped structure. TiAlO(3) (-) has a kite-shaped TiAlO(2) unit with the third O atom attaching to the Ti atom. TiAl(2)O(2) (-) has two nearly degenerate Al-O-Ti-O-Al chain structures that can be considered as cis and trans forms. TiAl(2)O(3) (-) has two low-lying isomers, kite structure and book structure. The structures of these clusters indicate that the Ti atom tends to bind to more O atoms.

Transitioning NWChem to the Next Generation of Manycore Machines

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bylaska, Eric J.; Apra, E; Kowalski, Karol

The NorthWest chemistry (NWChem) modeling software is a popular molecular chemistry simulation software that was designed from the start to work on massively parallel processing supercomputers [1-3]. It contains an umbrella of modules that today includes self-consistent eld (SCF), second order Møller-Plesset perturbation theory (MP2), coupled cluster (CC), multiconguration self-consistent eld (MCSCF), selected conguration interaction (CI), tensor contraction engine (TCE) many body methods, density functional theory (DFT), time-dependent density functional theory (TDDFT), real-time time-dependent density functional theory, pseudopotential plane-wave density functional theory (PSPW), band structure (BAND), ab initio molecular dynamics (AIMD), Car-Parrinello molecular dynamics (MD), classical MD, hybrid quantum mechanicsmore » molecular mechanics (QM/MM), hybrid ab initio molecular dynamics molecular mechanics (AIMD/MM), gauge independent atomic orbital nuclear magnetic resonance (GIAO NMR), conductor like screening solvation model (COSMO), conductor-like screening solvation model based on density (COSMO-SMD), and reference interaction site model (RISM) solvation models, free energy simulations, reaction path optimization, parallel in time, among other capabilities [4]. Moreover, new capabilities continue to be added with each new release.« less

Optimization of self-interstitial clusters in 3C-SiC with genetic algorithm

NASA Astrophysics Data System (ADS)

Ko, Hyunseok; Kaczmarowski, Amy; Szlufarska, Izabela; Morgan, Dane

2017-08-01

Under irradiation, SiC develops damage commonly referred to as black spot defects, which are speculated to be self-interstitial atom clusters. To understand the evolution of these defect clusters and their impacts (e.g., through radiation induced swelling) on the performance of SiC in nuclear applications, it is important to identify the cluster composition, structure, and shape. In this work the genetic algorithm code StructOpt was utilized to identify groundstate cluster structures in 3C-SiC. The genetic algorithm was used to explore clusters of up to ∼30 interstitials of C-only, Si-only, and Si-C mixtures embedded in the SiC lattice. We performed the structure search using Hamiltonians from both density functional theory and empirical potentials. The thermodynamic stability of clusters was investigated in terms of their composition (with a focus on Si-only, C-only, and stoichiometric) and shape (spherical vs. planar), as a function of the cluster size (n). Our results suggest that large Si-only clusters are likely unstable, and clusters are predominantly C-only for n ≤ 10 and stoichiometric for n > 10. The results imply that there is an evolution of the shape of the most stable clusters, where small clusters are stable in more spherical geometries while larger clusters are stable in more planar configurations. We also provide an estimated energy vs. size relationship, E(n), for use in future analysis.

Compressive Sensing Cluster Expansion Studies of Lithium Intercalation and Phase Transformation in MoS2 for Energy Storage

NASA Astrophysics Data System (ADS)

Liu, Chi-Ping; Zhou, Fei; Ozolins, Vidvuds; University of California, Los Angeles Collaboration; Lawrence livermore national laboratory Collaboration

2015-03-01

Bulk molybdenum disulfide (MoS2) is a good electrode material candidate for energy storage applications, such as lithium ion batteries and supercapacitors due to its high theoretical energy and power density. First-principles density-functional theory (DFT) calculations combined with cluster expansion are an effective method to study thermodynamic and kinetic properties of electrode materials. In order to construct accurate models for cluster expansion, it is important to effectively choose clusters with significant contributions. In this work, we employ a compressive sensing based technique to select relevant clusters in order to build an accurate Hamiltonian for cluster expansion, enabling the study of Li intercalation in MoS2. We find that the 2H MoS2 structure is only stable at low Li content while 1T MoS2 is the preferred phase at high Li content. The results show that the 2H MoS2 phase transforms into the disordered 1T phase and the disordered 1T structure remains after the first Li insertion/deinsertion cycle suggesting that disordered 1T MoS2 is stable even at dilute Li content. This work also highlights that cluster expansion treated with compressive sensing is an effective and powerful tool for model construction and can be applied to advanced battery and supercapacitor electrode materials.

Relativistic coupled-cluster calculations of the 173Yb nuclear quadrupole coupling constant for the YbF molecule

NASA Astrophysics Data System (ADS)

Pašteka, L. F.; Mawhorter, R. J.; Schwerdtfeger, P.

2016-04-01

We report calculations on the q(Yb) electric field gradient (EFG) for the X2Σ+ and A2Π1/2 electronic states of the ytterbium monofluoride (YbF) molecule at the molecular mean-field Dirac-Coulomb-Gaunt as well as scalar-relativistic coupled-cluster levels of theory using large uncontracted basis sets. Vibrational contributions are included in the final results. Our estimated nuclear quadrupole coupling constants of -3386(78) MHz and -2083(153) MHz for the X2Σ+ and A2Π1/2 states of 173YbF are in stark contrast to the only available experimental results (-2050(170) MHz and -1090(160) MHz) respectively, where the only similarity is the difference between the two values. Perturbative triple contributions in the coupled cluster treatment are significant and point towards the necessity to go to higher order in the coupled-cluster treatment in future calculations. We also present density functional calculations which show rather large variations for the Yb EFG with different functionals used; the best result was obtained using the CAM-B3LYP* functional.

Object Kinetic Monte Carlo Simulations of Radiation Damage In Bulk Tungsten

NASA Astrophysics Data System (ADS)

Nandipati, Giridhar; Setyawan, Wahyu; Heinisch, Howard; Roche, Kenneth; Kurtz, Richard; Wirth, Brian

2015-11-01

Results are presented for the evolution of radiation damage in bulk tungsten investigated using the object KMC simulation tool, KSOME, as a function of dose, dose rate and primary knock-on atom (PKA) energies in the range of 10 to 100 keV, at temperatures of 300, 1025 and 2050 K. At 300 K, the number density of vacancies changes minimally with dose rate while the number density of vacancy clusters slightly decreases with dose rate indicating that larger clusters are formed at higher dose rates. Although the average vacancy cluster size increases slightly, the vast majority exists as mono-vacancies. At 1025 K void lattice formation was observed at all dose rates for cascades below 60 keV and at lower dose rates for higher PKA energies. After the appearance of initial features of the void lattice, vacancy cluster density increased minimally while the average vacancy cluster size increases rapidly with dose. At 2050 K, no accumulation of defects was observed over a broad range of dose rates for all PKA energies studied in this work. Further comparisons of results of irradiation simulations at various dose rates and PKA spectra, representative of the High Flux Isotope Reactor and future fusion relevant irradiation facilities will be discussed. The U.S. Department of Energy, Office of Fusion Energy Sciences (FES) and Office of Advanced Scientific Computing Research (ASCR) has supported this study through the SciDAC-3 program.

An X-Ray Flux-Limited Sample of Galaxy Clusters: Physical Properties and Cosmological Implications

NASA Astrophysics Data System (ADS)

Reiprich, Thomas H.

2001-07-01

An X-ray selected and X-ray flux-limited sample comprising the 63 X-ray brightest galaxy clusters in the sky (excluding the galactic band, called HIFLUGCS) has been constructed based on the ROSAT All-Sky Survey. The flux limit has been set at 2x10^-11 erg/s/cm^2 in the energy band 0.1-2.4 keV. It has been shown that a high completeness is indicated by several tests. Due to the high flux limit this sample can be used for a variety of applications requiring a statistical cluster sample without any corrections to the effective survey volume. Mainly high quality pointed observations have been used to determine fluxes and physical cluster parameters. It has been shown that a tight correlation exists between the X-ray luminosity and the gravitational mass using HIFLUGCS and an extended sample of 106 galaxy clusters. The relation and its scatter have been quantified using different fitting methods. A comparison to theoretical and numerical predictions shows an overall agreement. This relation may be directly applied in large X-ray cluster surveys or dark matter simulations for conversions between X-ray luminosity and gravitating mass. Data from the performance verification phase of the recently launched X-ray satellite observatory XMM-Newton on the galaxy cluster Abell 1835 has been analyzed, in order to test the assumption of isothermality of the cluster gas in the outer parts applied throughout the work. It has been found that the measured outer temperature profile is consistent with being isothermal. In the inner regions a clear drop of the temperature by a factor of two has been found. Physical properties of the cluster sample have been studied by analyzing relations between different cluster parameters. The overall properties are well understood but in detail deviations from simple expectations have been found. It has been found that the gas mass fraction (fgas) does not vary as a function of intracluster gas temperature. For galaxy groups (kTx < 2 keV), however, a steep drop of fgas has been observed. No clear trend of a variation of the shape of the surface brightness profile, i.e. beta, has been observed as a function of temperature. The Lx-Tx relation has been found to be steeper than expected from simple self similar models, as has been found by previous authors. But no clear deviations from a power law shape down to kTx = 0.7 keV have been found. The Mt-Tx relation found here is steeper than expected from self similar models and its normalization is lower compared to hydrodynamic simulations, in agreement with previous findings. Suggested scenarios to account for these deviations, including heating and cooling processes, and observational difficulties have been described. It appears that a blend of different effects, possibly including a variation of mean formation redshift with system mass, is needed to account for the observations presented here. Using HIFLUGCS the gravitational mass function has been determined for the mass interval 3.5x10^13 < M200 < 5.2x10^15 h50^-1 Msun. Comparison with Press-Schechter mass functions has yielded tight constraints on the mean matter density in the universe and the amplitude of density fluctuations. The large covered mass range has allowed to put constraints on the parameters individually. Specifically it has been found that OmegaM = 0.12^{+0.06}_{-0.04} and sigma8 = 0.96^{+0.15}_{-0.12} (90% c.l. statistical uncertainty). This result is consistent with two more estimates of OmegaM obtained in this work using different methods. The mean intracluster gas fraction of the 106 clusters in the extended sample combined with predictions from the theory of nucleosynthesis indicates OmegaM < 0.34. The cluster mass to light ratio multiplied by the mean luminosity density implies OmegaM 0.15. Various tests for systematic uncertainties have been performed, including comparison of the Press-Schechter mass function with the most recent results from large N-body simulations, yielding deviations smaller than the statistical uncertainties. For comparison the best fit OmegaM values for fixed sigma8 values have been determined yielding the relation sigma8 = 0.43OmegaM^-0.38. The mass function has been integrated to obtain the fraction of the total gravitating mass in the universe contained in galaxy clusters. Normalized to the critical density it has been found that Omega_Cluster = 0.012^{+0.003}_{-0.004} for cluster masses larger than 6.4^{+0.7}_{-0.6}x10^13 h50^-1 Msun. With the value for OmegaM determined here this implies that about 90% of the mass in the universe resides outside virialized cluster regions. Similarly it has been found that the fraction of the total gravitating mass which is contained in the intracluster gas, Omega_b,Cluster = 0.0015^{+0.0002}_{-0.0001} h50^-1.5 for gas masses larger than 6.9^{+1.4}_{-1.5}x10^12 h50^{-5/2}Msun, is very small.

The Herschel Virgo Cluster Survey - XVI. A cluster inventory

NASA Astrophysics Data System (ADS)

Davies, J. I.; Bianchi, S.; Baes, M.; Bendo, G. J.; Clemens, M.; De Looze, I.; di Serego Alighieri, S.; Fritz, J.; Fuller, C.; Pappalardo, C.; Hughes, T. M.; Madden, S.; Smith, M. W. L.; Verstappen, J.; Vlahakis, C.

2014-03-01

Herschel far-infrared (FIR) observations are used to construct Virgo cluster galaxy luminosity functions and to show that the cluster lacks the very bright and the numerous faint sources detected in field galaxy surveys. The FIR spectral energy distributions are fitted to obtain dust masses and temperatures and the dust mass function. The cluster is overdense in dust by about a factor of 100 compared to the field. The same emissivity (β)-temperature relation applies for different galaxies as that found for different regions of M31. We use optical and H I data to show that Virgo is overdense in stars and atomic gas by about a factor of 100 and 20, respectively. Metallicity values are used to measure the mass of metals in the gas phase. The mean metallicity is ˜0.7 solar, and ˜50 per cent of the metals are in the dust. For the cluster as a whole, the mass density of stars in galaxies is eight times that of the gas and the gas mass density is 130 times that of the metals. We use our data to consider the chemical evolution of the individual galaxies, inferring that the measured variations in the effective yield are due to galaxies having different ages, being affected to varying degrees by gas loss. Four galaxy scaling relations are considered: mass-metallicity, mass-velocity, mass-star formation rate and mass-radius - we suggest that initial galaxy mass is the prime driver of a galaxy's ultimate destiny. Finally, we use X-ray observations and galaxy dynamics to assess the dark and baryonic matter content compared to the cosmological model.

The devil is in the tails: the role of globular cluster mass evolution on stream properties

NASA Astrophysics Data System (ADS)

Balbinot, Eduardo; Gieles, Mark

2018-02-01

We present a study of the effects of collisional dynamics on the formation and detectability of cold tidal streams. A semi-analytical model for the evolution of the stellar mass function was implemented and coupled to a fast stellar stream simulation code, as well as the synthetic cluster evolution code EMACSS for the mass evolution as a function of a globular cluster orbit. We find that the increase in the average mass of the escaping stars for clusters close to dissolution has a major effect on the observable stream surface density. As an example, we show that Palomar 5 would have undetectable streams (in an SDSS-like survey) if it was currently three times more massive, despite the fact that a more massive cluster loses stars at a higher rate. This bias due to the preferential escape of low-mass stars is an alternative explanation for the absence of tails near massive clusters, than a dark matter halo associated with the cluster. We explore the orbits of a large sample of Milky Way globular clusters and derive their initial masses and remaining mass fraction. Using properties of known tidal tails, we explore regions of parameter space that favour the detectability of a stream. A list of high-probability candidates is discussed.

Nonlinear dynamics of the cellular-automaton ``game of Life''

NASA Astrophysics Data System (ADS)

Garcia, J. B. C.; Gomes, M. A. F.; Jyh, T. I.; Ren, T. I.; Sales, T. R. M.

1993-11-01

A statistical analysis of the ``game of Life'' due to Conway [Berlekamp, Conway, and Guy, Winning Ways for Your Mathematical Plays (Academic, New York, 1982), Vol. 2] is reported. The results are based on extensive computer simulations starting with uncorrelated distributions of live sites at t=0. The number n(s,t) of clusters of s live sites at time t, the mean cluster size s¯(t), and the diversity of sizes among other statistical functions are obtained. The dependence of the statistical functions with the initial density of live sites is examined. Several scaling relations as well as static and dynamic critical exponents are found.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yu, Kuang; Libisch, Florian; Carter, Emily A., E-mail: eac@princeton.edu

We report a new implementation of the density functional embedding theory (DFET) in the VASP code, using the projector-augmented-wave (PAW) formalism. Newly developed algorithms allow us to efficiently perform optimized effective potential optimizations within PAW. The new algorithm generates robust and physically correct embedding potentials, as we verified using several test systems including a covalently bound molecule, a metal surface, and bulk semiconductors. We show that with the resulting embedding potential, embedded cluster models can reproduce the electronic structure of point defects in bulk semiconductors, thereby demonstrating the validity of DFET in semiconductors for the first time. Compared to ourmore » previous version, the new implementation of DFET within VASP affords use of all features of VASP (e.g., a systematic PAW library, a wide selection of functionals, a more flexible choice of U correction formalisms, and faster computational speed) with DFET. Furthermore, our results are fairly robust with respect to both plane-wave and Gaussian type orbital basis sets in the embedded cluster calculations. This suggests that the density functional embedding method is potentially an accurate and efficient way to study properties of isolated defects in semiconductors.« less

Arsenic interactions with a fullerene-like BN cage in the vacuum and aqueous phase.

PubMed

Beheshtian, Javad; Peyghan, Ali Ahmadi; Bagheri, Zargham

2013-02-01

Adsorption of arsenic ions, As (III and V), on the surface of fullerene-like B(12)N(12) cage has been explored in vacuum and aqueous phase using density functional theory in terms of Gibbs free energies, enthalpies, geometry, and density of state analysis. It was found that these ions can be strongly chemisorbed on the surface of the cluster in both vacuum and aqueous phase, resulting in significant changes in its electronic properties so that the cluster transforms from a semi-insulator to a semiconductor. The solvent significantly affects the geometry parameters and electronic properties of the As/B(12)N(12) complexes and the interaction between components is considerably weaker in the aqueous phase than that in the vacuum.

Molecular dynamics simulation of liquid structure for undercooled Zr-Nb alloys assisted with electrostatic levitation experiments

NASA Astrophysics Data System (ADS)

Yang, S. J.; Hu, L.; Wang, L.; Wei, B.

2018-06-01

The liquid structures of undercooled Zr90Nb10, Zr70Nb30 and Zr50Nb50 alloys were studied by molecular dynamics simulation combined with electrostatic levitation experiments. The densities of three alloys were measured by electrostatic levitation to modify the Zr-Nb potential functions by adjusting parameters in potential functions. In simulation, the atomic packing in Zr-Nb alloys was more ordered at lower temperatures. The Voronoi tessellation analyses indicated Nb-centered clusters were easier to form than Zr-centered clusters although the Nb content was less than 50%. The partial pair distribution functions showed that the interactions among Zr atoms are quite different to that among Nb atoms.

Current Density Functional Theory Using Meta-Generalized Gradient Exchange-Correlation Functionals.

PubMed

Furness, James W; Verbeke, Joachim; Tellgren, Erik I; Stopkowicz, Stella; Ekström, Ulf; Helgaker, Trygve; Teale, Andrew M

2015-09-08

We present the self-consistent implementation of current-dependent (hybrid) meta-generalized gradient approximation (mGGA) density functionals using London atomic orbitals. A previously proposed generalized kinetic energy density is utilized to implement mGGAs in the framework of Kohn-Sham current density functional theory (KS-CDFT). A unique feature of the nonperturbative implementation of these functionals is the ability to seamlessly explore a wide range of magnetic fields up to 1 au (∼235 kT) in strength. CDFT functionals based on the TPSS and B98 forms are investigated, and their performance is assessed by comparison with accurate coupled-cluster singles, doubles, and perturbative triples (CCSD(T)) data. In the weak field regime, magnetic properties such as magnetizabilities and nuclear magnetic resonance shielding constants show modest but systematic improvements over generalized gradient approximations (GGA). However, in the strong field regime, the mGGA-based forms lead to a significantly improved description of the recently proposed perpendicular paramagnetic bonding mechanism, comparing well with CCSD(T) data. In contrast to functionals based on the vorticity, these forms are found to be numerically stable, and their accuracy at high field suggests that the extension of mGGAs to CDFT via the generalized kinetic energy density should provide a useful starting point for further development of CDFT approximations.

Diagrams for the Free Energy and Density Weight Factors of the Ising Models.

DTIC Science & Technology

1983-01-01

sum to zero . The associated R. A. Farrell, T. Morita, and P. H. E. Meijer, "Cluster Expan- also, "_ ratum: New Generating Functions and Results for the...given for the cubic lattices. We employ a theorem that states that a certain sum of diagrams is zero in order to obtain the density-dependent weight...these diagrams are given for the cubic lattices. We employ a theorem that states that a certain sum of diagrams is zero in order to obtain the density

Time-dependent density functional theory description of total photoabsorption cross sections

NASA Astrophysics Data System (ADS)

Tenorio, Bruno Nunes Cabral; Nascimento, Marco Antonio Chaer; Rocha, Alexandre Braga

2018-02-01

The time-dependent version of the density functional theory (TDDFT) has been used to calculate the total photoabsorption cross section of a number of molecules, namely, benzene, pyridine, furan, pyrrole, thiophene, phenol, naphthalene, and anthracene. The discrete electronic pseudo-spectra, obtained in a L2 basis set calculation were used in an analytic continuation procedure to obtain the photoabsorption cross sections. The ammonia molecule was chosen as a model system to compare the results obtained with TDDFT to those obtained with the linear response coupled cluster approach in order to make a link with our previous work and establish benchmarks.

First-principles study on stability, and growth strategies of small AlnZr (n=1-9) clusters

NASA Astrophysics Data System (ADS)

Li, Zhi; Zhou, Zhonghao; Wang, Hongbin; Li, Shengli; Zhao, Zhen

2016-09-01

The geometries, relative stability as well as growth strategies of the AlnZr (n=1-9) clusters are investigated with spin polarized density functional theory: BLYP. The results reveal that the AlnZr clusters are more likely to form the dense accumulation structures than the AlN (N=1-10) clusters. The average binding energies of AlnZr are higher than those of AlN clusters. The AlnZr (n=3, 5, and 7) clusters are more stable than others by the differences of the total binding energies. Mülliken population analysis for the AlnZr clusters shows that the electron's adsorption ability of Zr is slightly lower than that of Al except for AlZr cluster. Local peaks of the HOMO-LUMO gap curve are found at n=3, 5, and 7. The reaction energies of AlnZr are higher, which means that AlnZr clusters are easier to react with Al clusters. Zr atom preferential reacts with Al2 cluster. Local peaks of the magnetic dipole moments are found at n=2, 5, and 8.

The separate and combined effects of baryon physics and neutrino free streaming on large-scale structure

NASA Astrophysics Data System (ADS)

Mummery, Benjamin O.; McCarthy, Ian G.; Bird, Simeon; Schaye, Joop

2017-10-01

We use the cosmo-OWLS and bahamas suites of cosmological hydrodynamical simulations to explore the separate and combined effects of baryon physics (particularly feedback from active galactic nuclei, AGN) and free streaming of massive neutrinos on large-scale structure. We focus on five diagnostics: (I) the halo mass function, (II) halo mass density profiles, (III) the halo mass-concentration relation, (IV) the clustering of haloes and (v) the clustering of matter, and we explore the extent to which the effects of baryon physics and neutrino free streaming can be treated independently. Consistent with previous studies, we find that both AGN feedback and neutrino free streaming suppress the total matter power spectrum, although their scale and redshift dependences differ significantly. The inclusion of AGN feedback can significantly reduce the masses of groups and clusters, and increase their scale radii. These effects lead to a decrease in the amplitude of the mass-concentration relation and an increase in the halo autocorrelation function at fixed mass. Neutrinos also lower the masses of groups and clusters while having no significant effect on the shape of their density profiles (thus also affecting the mass-concentration relation and halo clustering in a qualitatively similar way to feedback). We show that, with only a small number of exceptions, the combined effects of baryon physics and neutrino free streaming on all five diagnostics can be estimated to typically better than a few per cent accuracy by treating these processes independently (I.e. by multiplying their separate effects).

Effect of Rubber Polarity on Cluster Formation in Rubbers Cross-Linked with Diels–Alder Chemistry

PubMed Central

2017-01-01

Diels–Alder chemistry has been used for the thermoreversible cross-linking of furan-functionalized ethylene/propylene (EPM) and ethylene/vinyl acetate (EVM) rubbers. Both furan-functionalized elastomers were successfully cross-linked with bismaleimide to yield products with a similar cross-link density. NMR relaxometry and SAXS measurements both show that the apolar EPM-g-furan precursor contains phase-separated polar clusters and that cross-linking with polar bismaleimide occurs in these clusters. The heterogeneously cross-linked network of EPM-g-furan contrasts with the homogeneous network in the polar EVM-g-furan. The heterogeneous character of the cross-links in EPM-g-furan results in a relatively high Young’s modulus, whereas the more uniform cross-linking in EVM-g-furan results in a higher tensile strength and elongation at break. PMID:29213149

Traveling-cluster approximation for uncorrelated amorphous systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sen, A.K.; Mills, R.; Kaplan, T.

1984-11-15

We have developed a formalism for including cluster effects in the one-electron Green's function for a positionally disordered (liquid or amorphous) system without any correlation among the scattering sites. This method is an extension of the technique known as the traveling-cluster approximation (TCA) originally obtained and applied to a substitutional alloy by Mills and Ratanavararaksa. We have also proved the appropriate fixed-point theorem, which guarantees, for a bounded local potential, that the self-consistent equations always converge upon iteration to a unique, Herglotz solution. To our knowledge, this is the only analytic theory for considering cluster effects. Furthermore, we have performedmore » some computer calculations in the pair TCA, for the model case of delta-function potentials on a one-dimensional random chain. These results have been compared with ''exact calculations'' (which, in principle, take into account all cluster effects) and with the coherent-potential approximation (CPA), which is the single-site TCA. The density of states for the pair TCA clearly shows some improvement over the CPA and yet, apparently, the pair approximation distorts some of the features of the exact results.« less

Copper cluster size effect in methanol synthesis from CO 2

DOE PAGES

Yang, Bing; Liu, Cong; Halder, Avik; ...

2017-05-08

Here, size-selected Cu n catalysts ( n = 3, 4, 20) were synthesized on Al 2O 3 thin films using mass-selected cluster deposition. A systematic study of size and support effects was carried out for CO 2 hydrogenation at atmospheric pressure using a combination of in situ grazing incidence X-ray absorption spectroscopy, catalytic activity measurement, and first-principles calculations. The catalytic activity for methanol synthesis is found to strongly vary as a function of the cluster size; the Cu 4/Al 2O 3 catalyst shows the highest turnover rate for CH 3OH production. With only one atom less than Cu 4, Cumore » 3 showed less than 50% activity. Density functional theory calculations predict that the activities of the gas-phase Cu clusters increase as the cluster size decreases; however, the stronger charge transfer interaction with Al 2O 3 support for Cu 3 than for Cu 4 leads to remarkably reduced binding strength between the adsorbed intermediates and supported Cu 3, which subsequently results in a less favorable energetic pathway to transform carbon dioxide to methanol.« less

Optical properties of hybrid spherical nanoclusters containing quantum emitters and metallic nanoparticles

NASA Astrophysics Data System (ADS)

Yannopapas, V.; Paspalakis, E.

2018-05-01

We study theoretically the optical response of a hybrid spherical cluster containing quantum emitters and metallic nanoparticles. The quantum emitters are modeled as two-level quantum systems whose dielectric function is obtained via a density matrix approach wherein the modified spontaneous emission decay rate at the position of each quantum emitter is calculated via the electromagnetic Green's tensor. The problem of light scattering off the hybrid cluster is solved by employing the coupled-dipole method. We find, in particular, that the presence of the quantum emitters in the cluster, even in small fractions, can significantly alter the absorption and extinction spectra of the sole cluster of the metallic nanoparticles, where the corresponding electromagnetic modes can have a weak plexcitonic character under suitable conditions.

Dewetting and spreading transitions for active matter on random pinning substrates.

PubMed

Sándor, Cs; Libál, A; Reichhardt, C; Olson Reichhardt, C J

2017-05-28

We show that sterically interacting self-propelled disks in the presence of random pinning substrates exhibit transitions among a variety of different states. In particular, from a phase separated cluster state, the disks can spread out and homogeneously cover the substrate in what can be viewed as an example of an active matter wetting transition. We map the location of this transition as a function of activity, disk density, and substrate strength, and we also identify other phases including a cluster state, coexistence between a cluster and a labyrinth wetted phase, and a pinned liquid. Convenient measures of these phases include the cluster size, which dips at the wetting-dewetting transition, and the fraction of sixfold coordinated particles, which drops when dewetting occurs.

Primordial binary populations in low-density star clusters as seen by Chandra: globular clusters versus old open clusters

NASA Astrophysics Data System (ADS)

van den Berg, Maureen C.

2015-08-01

The binaries in the core of a star cluster are the energy source that prevents the cluster from experiencing core collapse. To model the dynamical evolution of a cluster, it is important to have constraints on the primordial binary content. X-ray observations of old star clusters are very efficient in detecting the close interacting binaries among the cluster members. The X-ray sources in star clusters are a mix of binaries that were dynamically formed and primordial binaries. In massive, dense star clusters, dynamical encounters play an important role in shaping the properties and numbers of the binaries. In contrast, in the low-density clusters the impact of dynamical encounters is presumed to be very small, and the close binaries detected in X-rays represent a primordial population. The lowest density globular clusters have current masses and central densities similar to those of the oldest open clusters in our Milky Way. I will discuss the results of studies with the Chandra X-ray Observatory that have nevertheless revealed a clear dichotomy: far fewer (if any at all) X-ray sources are detected in the central regions of the low-density globular clusters compared to the number of secure cluster members that have been detected in old open clusters (above a limiting X-ray luminosity of typically 4e30 erg/s). The low stellar encounter rates imply that dynamical destruction of binaries can be ignored at present, therefore an explanation must be sought elsewhere. I will discuss several factors that can shed light on the implied differences between the primordial close binary populations in the two types of star clusters.

Wobbled electronic properties of lithium clusters: Deterministic approach through first principles

NASA Astrophysics Data System (ADS)

Kushwaha, Anoop Kumar; Nayak, Saroj Kumar

2018-03-01

The innate tendency to form dendritic growth promoted through cluster formation leading to the failure of a Li-ion battery system have drawn significant attention of the researchers towards the effective destabilization of the cluster growth through selective implementation of electrolytic media such as acetonitrile (MeCN). In the present work, using first principles density functional theory and continuum dielectric model, we have investigated the origin of oscillatory nature of binding energy per atom of Lin (n ≤ 8) under the influence of MeCN. In the gas phase, we found that static mean polarizability is strongly correlated with binding energy and shows oscillatory nature with cluster size due to the open shell of Lin cluster. However, in acetonitrile medium, the binding energy has been correlated with electrostatic Lin -MeCN interaction and it has been found that both of them possess wobbled behavior characterized by the cluster size.

Reactions of sulfur dioxide with neutral vanadium oxide clusters in the gas phase. I. Density functional theory study.

PubMed

Jakubikova, Elena; Bernstein, Elliot R

2007-12-27

Thermodynamics of reactions of vanadium oxide clusters with SO2 are studied at the BPW91/LANL2DZ level of theory. BPW91/LANL2DZ is insufficient to properly describe relative V-O and S-O bond strengths of vanadium and sulfur oxides. Calibration of theoretical results with experimental data is necessary to compute reliable enthalpy changes for reactions between VxOy and SO2. Theoretical results indicate SO2 to SO conversion occurs for oxygen-deficient clusters and SO2 to SO3 conversion occurs for oxygen-rich clusters. Stable intermediate structures of VOy (y = 1 - 4) clusters with SO2 are also obtained at the BPW91/TZVP level of theory. Some possible mechanisms for SO3 formation and catalyst regeneration for condensed-phase systems are suggested. These results are in agreement with, and complement, gas-phase experimental studies of neutral vanadium oxide clusters.

Young star clusters in circumnuclear starburst rings

NASA Astrophysics Data System (ADS)

de Grijs, Richard; Ma, Chao; Jia, Siyao; Ho, Luis C.; Anders, Peter

2017-03-01

We analyse the cluster luminosity functions (CLFs) of the youngest star clusters in two galaxies exhibiting prominent circumnuclear starburst rings. We focus specifically on NGC 1512 and NGC 6951, for which we have access to Hα data that allow us to unambiguously identify the youngest sample clusters. To place our results on a firm statistical footing, we first explore in detail a number of important technical issues affecting the process from converting the observational data into the spectral energy distributions of the objects in our final catalogues. The CLFs of the young clusters in both galaxies exhibit approximate power-law behaviour down to the 90 per cent observational completeness limits, thus showing that star cluster formation in the violent environments of starburst rings appears to proceed similarly as that elsewhere in the local Universe. We discuss this result in the context of the density of the interstellar medium in our starburst-ring galaxies.

Equilibrium geometries, electronic and magnetic properties of small AunNi- (n = 1-9) clusters

NASA Astrophysics Data System (ADS)

Tang, Cui-Ming; Chen, Xiao-Xu; Yang, Xiang-Dong

2014-05-01

Geometrical, electronic and magnetic properties of small AunNi- (n = 1-9) clusters have been investigated based on density functional theory (DFT) at PW91P86 level. An extensive structural search shows that the relative stable structures of AunNi- (n = 1-9) clusters adopt 2D structure for n = 1-5, 7 and 3D structure for n = 6, 8-9. And the substitution of a Ni atom for an Au atom in the Au-n+1 cluster obviously changes the structure of the host cluster. Moreover, an odd-even alternation phenomenon has been found for HOMO-LUMO energy gaps, indicating that the relative stable structures of the AunNi- clusters with odd-numbered gold atoms have a higher relative stability. Finally, the natural population analysis (NPA) and the vertical detachment energies (VDE) are studied, respectively. The theoretical values of VDE are reported for the first time to our best knowledge.

Formation of prismatic loops from C15 Laves phase interstitial clusters in body-centered cubic iron

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Yongfeng; Bai, Xian-Ming; Tonks, Michael R.

2015-03-01

This Letter reports the transition of C15 phase self-interstitial clusters to loops in body-centered-cubic Iron. Molecular dynamics simulations are performed to evaluate the relative stabilities of difference interstitial cluster configurations including C15 phase structure and <100> and <111>/2 loops. Within a certain size range, C15 cluster are found more stable than loops, and the relative stabilities are reversed beyond that range. In accordance to the crossover in relative stabilities, C15 clusters may grow by absorbing individual interstitials at small sizes and transitions into loops eventually. The transition takes place by nucleation and reaction of <111>/2 loop segments. These observations explainmore » the absence of C15 phase interstitial clusters predicted by density-functional-theory calculations in previous experimental observations. More importantly, the current results provide a new formation mechanism of <100> loops which requires no interaction of loops.« less

A new solution-adaptive grid generation method for transonic airfoil flow calculations

NASA Technical Reports Server (NTRS)

Nakamura, S.; Holst, T. L.

1981-01-01

The clustering algorithm is controlled by a second-order, ordinary differential equation which uses the airfoil surface density gradient as a forcing function. The solution to this differential equation produces a surface grid distribution which is automatically clustered in regions with large gradients. The interior grid points are established from this surface distribution by using an interpolation scheme which is fast and retains the desirable properties of the original grid generated from the standard elliptic equation approach.

Cloud Structure of Galactic OB Cluster-forming Regions from Combining Ground- and Space-based Bolometric Observations

NASA Astrophysics Data System (ADS)

Lin, Yuxin; Liu, Hauyu Baobab; Li, Di; Zhang, Zhi-Yu; Ginsburg, Adam; Pineda, Jaime E.; Qian, Lei; Galván-Madrid, Roberto; McLeod, Anna Faye; Rosolowsky, Erik; Dale, James E.; Immer, Katharina; Koch, Eric; Longmore, Steve; Walker, Daniel; Testi, Leonardo

2016-09-01

We have developed an iterative procedure to systematically combine the millimeter and submillimeter images of OB cluster-forming molecular clouds, which were taken by ground-based (CSO, JCMT, APEX, and IRAM-30 m) and space telescopes (Herschel and Planck). For the seven luminous (L\\gt {10}6 L ⊙) Galactic OB cluster-forming molecular clouds selected for our analyses, namely W49A, W43-Main, W43-South, W33, G10.6-0.4, G10.2-0.3, and G10.3-0.1, we have performed single-component, modified blackbody fits to each pixel of the combined (sub)millimeter images, and the Herschel PACS and SPIRE images at shorter wavelengths. The ˜10″ resolution dust column density and temperature maps of these sources revealed dramatically different morphologies, indicating very different modes of OB cluster-formation, or parent molecular cloud structures in different evolutionary stages. The molecular clouds W49A, W33, and G10.6-0.4 show centrally concentrated massive molecular clumps that are connected with approximately radially orientated molecular gas filaments. The W43-Main and W43-South molecular cloud complexes, which are located at the intersection of the Galactic near 3 kpc (or Scutum) arm and the Galactic bar, show a widely scattered distribution of dense molecular clumps/cores over the observed ˜10 pc spatial scale. The relatively evolved sources G10.2-0.3 and G10.3-0.1 appear to be affected by stellar feedback, and show a complicated cloud morphology embedded with abundant dense molecular clumps/cores. We find that with the high angular resolution we achieved, our visual classification of cloud morphology can be linked to the systematically derived statistical quantities (I.e., the enclosed mass profile, the column density probability distribution function (N-PDF), the two-point correlation function of column density, and the probability distribution function of clump/core separations). In particular, the massive molecular gas clumps located at the center of G10.6-0.4 and W49A, which contribute to a considerable fraction of their overall cloud masses, may be special OB cluster-forming environments as a direct consequence of global cloud collapse. These centralized massive molecular gas clumps also uniquely occupy much higher column densities than what is determined by the overall fit of power-law N-PDF. We have made efforts to archive the derived statistical quantities of individual target sources, to permit comparisons with theoretical frameworks, numerical simulations, and other observations in the future.

Density functional theory study of ethylene partial oxidation on Ag 7 clusters

NASA Astrophysics Data System (ADS)

Yu, Hua-Gen

2006-11-01

The partial oxidation reaction of ethylene on neutral and anionic Ag 7 clusters has been studied using the BPW91 hybrid DFT method with the Stuttgart RSC97 relativistic pseudopotential for the 28-electron ionic core of Ag. The atomic oxygen reaction mechanism is mainly addressed. Results show that the reaction occurs via a stable oxametallacycle intermediate ( AgOCH4p, p = 0 or -1), but it involves small reaction barriers along the reaction path. The ZPE-corrected barrier heights are obtained as 0.7-6.5 kcal/mole. In addition, the structure and anionic effects of Ag 7 clusters are also discussed.

Advances in stellar evolution; Proceedings of the Workshop on Stellar Ecology, Marciana Marina, Italy, June 23-29, 1996

NASA Astrophysics Data System (ADS)

Rood, R. T.; Renzini, A.

1997-01-01

The present volume on stellar evolution discusses fundamentals of stellar evolution and star clusters, variable stars, AGB stars and planetary nebulae, white dwarfs, binary star evolution, and stars in galaxies. Attention is given to the stellar population in the Galactic bulge, a photometric study of NGC 458, and HST observations of high-density globular clusters. Other topics addressed include the Cepheid instability strip in external galaxies, Hyades cluster white dwarfs and the initial-final mass relation, element diffusion in novae, mass function of the stars in the solar neighborhood, synthetic spectral indices for elliptical galaxies, and stars at the Galactic center.

Electronic structures of Al-Si clusters and the magic number structure Al8Si4

NASA Astrophysics Data System (ADS)

Du, Ning; Su, Mingzhi; Chen, Hongshan

2018-02-01

The low-energy structures of Al8Sim (m = 1-6) have been determined by using the genetic algorithm combined with density functional theory and the Second-order Moller-Plesset perturbation theory (MP2) models. The results show that the close-packed structures are preferable in energy for Al-Si clusters and in most cases there exist a few isomers with close energies. The valence molecular orbitals, the orbital level structures and the electron localisation function (ELF) consistently demonstrate that the electronic structures of Al-Si clusters can be described by the jellium model. Al8Si4 corresponds to a magic number structure with pronounced stability and large energy gap; the 40 valence electrons form closed 1S21P61D102S21F142P6 shells. The ELF attractors also suggest weak covalent Si-Si, Si-Al and Al-Al bonding, and doping Si in aluminium clusters promotes the covalent interaction between Al atoms.

On the extended stellar structure around NGC 288

NASA Astrophysics Data System (ADS)

Piatti, Andrés E.

2018-01-01

We report on observational evidence of an extra-tidal clumpy structure around NGC 288 from homogeneous coverage of a large area with the Panoramic Survey Telescope and Rapid Response System (Pan-STARRS) PS1 data base. The extra-tidal star population has been disentangled from that of the Milky Way (MW) field by using a cleaning technique that successfully reproduces the stellar density, luminosity function and colour distributions of MW field stars. We have produced the cluster stellar density radial profile and a stellar density map from independent approaches, and we found the results to be in excellent agreement - the feature extends up to 3.5 times further than the cluster tidal radius. Previous works based on shallower photometric data sets have speculated on the existence of several long tidal tails, similar to that found in Pal 5. The present outcome shows that NGC 288 could hardly have such tails, but it favours the notion that the use of interactions with the MW tidal field has been a relatively inefficient process for stripping stars off the cluster. These results point to the need for a renewed overall study of the external regions of Galactic globular clusters (GGCs) in order to reliably characterize them. It will then be possible to investigate whether there is any connection between detected tidal tails, extra-tidal stellar populations and extended diffuse halo-like structures, and the dynamical histories of GGCs in the Galaxy.

Globular cluster ages determined from the Oosterhoff period-metallicity effect using oxygen-enhanced isochrones. III

NASA Astrophysics Data System (ADS)

Sandage, Allan

1993-08-01

The new brighter calibration of absolute luminosities of RR Lyrae stars by about 0.25 mag as a function of metallicity via the Oosterhoff period effect gives a revised age of the Galactic globular cluster system as 14 Gyr when used with the oxygen-enhanced main-sequence termination models of Bergbush and VandenBerg (1992). There is no correlation of cluster age with metallicity. The presence or absence of age differences between any two clusters is neither proof nor disproof of the Eggen-Lynden Bell-Sandage model of the formation of the Galaxy by collapse. If there were different density regimes within the initial density fluctuation that was the protogalaxy, then there has been a hierarchy of collapse times for the various parts of the present Galaxy. The age of the universe is 15 Gyr, based on the age of the Galaxy at 14 Gyr, to which 1 Gyr is added for the gestation time of the galaxies. The ratio of this age to the inverse Hubble constant with H(0) about 45 km/s Mpc, based on a recent concordant determination using supernovae of type Ia, is close to the critical value of 2/3 required if the deceleration is caused by a mean density just equal to that needed for closure. For the first time, these new data give the possibility that Omega = 1 from this timing test.

Topology of Large-Scale Structure by Galaxy Type: Hydrodynamic Simulations

NASA Astrophysics Data System (ADS)

Gott, J. Richard, III; Cen, Renyue; Ostriker, Jeremiah P.

1996-07-01

The topology of large-scale structure is studied as a function of galaxy type using the genus statistic. In hydrodynamical cosmological cold dark matter simulations, galaxies form on caustic surfaces (Zeldovich pancakes) and then slowly drain onto filaments and clusters. The earliest forming galaxies in the simulations (defined as "ellipticals") are thus seen at the present epoch preferentially in clusters (tending toward a meatball topology), while the latest forming galaxies (defined as "spirals") are seen currently in a spongelike topology. The topology is measured by the genus (number of "doughnut" holes minus number of isolated regions) of the smoothed density-contour surfaces. The measured genus curve for all galaxies as a function of density obeys approximately the theoretical curve expected for random- phase initial conditions, but the early-forming elliptical galaxies show a shift toward a meatball topology relative to the late-forming spirals. Simulations using standard biasing schemes fail to show such an effect. Large observational samples separated by galaxy type could be used to test for this effect.

Bonding and vibrations of CO molecules adsorbed at transition metal impurity sites on the MgO (001) surface. A density functional model cluster study

NASA Astrophysics Data System (ADS)

Neyman, K. M.; Rösch, N.

1993-11-01

First principles density functional cluster investigations of adsorption at the (001) surface of pure and doped magnesium oxide are carried out to characterize and compare the interaction of CO molecules with main group (Mg 2+) and d metal (Co 2+, Ni 2+, Cu 2+) surface cationic centers of the ionic substrate. The geometry of the adsorption complexes, the binding mechanism and spectroscopic manifestations of the surface species are analyzed. Special attention is payed to vibrational frequencies and intensities. The calculations qualitatively reproduce observed trends in the adsorption-induced frequency shifts for the series of the surface aggregates Mg 5cCO→Ni 5cCO→CO 5cCO and the corresponding change of the infrared intensities of the CO vibrational mode. For the transition metal impurity sites these results are rationalized in terms of a small, but notable Md πCOπ interaction.

Investigation on the neutral and anionic BxAlyH2 (x + y = 7, 8, 9) clusters using density functional theory combined with photoelectron spectroscopy.

PubMed

Ding, Li-Ping; Shao, Peng; Lu, Cheng; Zhang, Fang-Hui; Ding, Lei; Yuan, Tao Li

2016-08-17

The structure and bonding nature of neutral and negatively charged BxAlyH2 (x + y = 7, 8, 9) clusters are investigated with the aid of previously published experimental photoelectron spectra combined with the present density functional theory calculations. The comparison between the experimental photoelectron spectra and theoretical simulated spectra helps to identify the ground state structures. The accuracy of the obtained ground state structures is further verified by calculating their adiabatic electron affinities and vertical detachment energies and comparing them against available experimental data. The results show that the structures of BxAlyH2 transform from three-dimensional to planar structures as the number of boron atoms increases. Moreover, boron atoms tend to bind together forming Bn units. The hydrogen atoms prefer to bind with boron atoms rather than aluminum atoms. The analyses of the molecular orbital on the ground state structures further support the abovementioned results.

Deep and wide photometry of two open clusters NGC 1245 and NGC 2506: dynamical evolution and halo

NASA Astrophysics Data System (ADS)

Lee, S. H.; Kang, Y.-W.; Ann, H. B.

2013-06-01

We studied the structure of two old open clusters, NGC 1245 and NGC 2506, from a wide and deep VI photometry data acquired using the CFH12K CCD camera at Canada-France-Hawaii Telescope. We devised a new method for assigning cluster membership probability to individual stars using both spatial positions and positions in the colour-magnitude diagram. From analyses of the luminosity functions at several cluster-centric radii and the radial surface density profiles derived from stars with different luminosity ranges, we found that the two clusters are dynamically relaxed to drive significant mass segregation and evaporation of some fraction of low-mass stars. There seems to be a signature of tidal tail in NGC 1245 but the signal is too low to be confirmed.

Photoelectron Angular Distributions of Transition Metal Dioxide Anions - a joint experimental and theoretical study

NASA Astrophysics Data System (ADS)

Iordanov, Ivan; Gunaratne, Dasitha; Harmon, Christopher; Sofo, Jorge; Castleman, A. W., Jr.

2012-02-01

Angular-resolved photoelectron spectroscopy (PES) studies of the MO2- (M=Ti, Zr, Hf, Co, Rh) clusters are presented for the first time along with theoretical calculations of their properties. We confirm previously reported non-angular PES results for the vertical detachment energies (VDE), vibrational energies and geometric structures of these clusters and further explore the effect of the 'lanthanide contraction' on the MO2- clusters by comparing the electronic spectra of 4d and 5d transition metal dioxides. Angular-resolved PES provides the angular momentum contributions to the HOMO of these clusters and we use theoretical calculations to examine the HOMO and compare to our experimental results. First-principles calculations are done using both density functional theory (DFT) and the coupled-cluster, singles, doubles and triples (CCSD(T)) methods.

A search for novae in M 31 globular clusters

NASA Astrophysics Data System (ADS)

Ciardullo, Robin; Tamblyn, Peter; Phillips, A. C.

1990-10-01

By combining a local sky-fitting algorithm with a Fourier point-spread-function matching technique, nova outbursts have been searched for inside 54 of the globular clusters contained on the Ciardullo et al. (1987 and 1990) H-alpha survey frames of M 31. Over a mean effective survey time of about 2.0 years, no cluster exhibited a magnitude increase indicative of a nova explosion. If the cataclysmic variables (CVs) contained within globular clusters are similar to those found in the field, then these data imply that the overdensity of CVs within globulars is at least several times less than that of the high-luminosity X-ray sources. If tidal capture is responsible for the high density of hard binaries within globulars, then the probability of capturing condensed objects inside globular clusters may depend strongly on the mass of the remnant.

STABILITY OF SMALL SELF-INTERSTITIAL CLUSTERS IN TUNGSTEN

DOE Office of Scientific and Technical Information (OSTI.GOV)

Setyawan, Wahyu; Nandipati, Giridhar; Kurtz, Richard J.

2015-12-31

Density functional theory was employed to explore the stability of interstitial clusters in W up to size seven. For each cluster size, the most stable configuration consists of parallel dumbbells. For clusters larger than size three, parallel dumbbells prefer to form in a multilayer fashion, instead of a planar structure. For size-7 clusters, the most stable configuration is a complete octahedron. The binding energy of a [111] dumbbell to the most stable cluster increases with cluster size, namely 2.49, 3.68, 4.76, 4.82, 5.47, and 6.85 eV for clusters of size 1, 2, 3, 4, 5, and 6, respectively. For amore » size-2 cluster, collinear dumbbells are still repulsive at the maximum allowable distance of 13.8 Å (the fifth neighbor along [111]). On the other hand, parallel dumbbells are strongly bound together. Two parallel dumbbells in which the axis-to-axis distance is within a cylindrical radius of 5.2 Å still exhibit a considerable binding of 0.28 eV. The most stable cluster in each size will be used to explore interactions with transmutation products.« less

Galaxy Clusters

NASA Astrophysics Data System (ADS)

Miller, Christopher J. Miller

2012-03-01

There are many examples of clustering in astronomy. Stars in our own galaxy are often seen as being gravitationally bound into tight globular or open clusters. The Solar System's Trojan asteroids cluster at the gravitational Langrangian in front of Jupiter’s orbit. On the largest of scales, we find gravitationally bound clusters of galaxies, the Virgo cluster (in the constellation of Virgo at a distance of ˜50 million light years) being a prime nearby example. The Virgo cluster subtends an angle of nearly 8◦ on the sky and is known to contain over a thousand member galaxies. Galaxy clusters play an important role in our understanding of theUniverse. Clusters exist at peaks in the three-dimensional large-scale matter density field. Their sky (2D) locations are easy to detect in astronomical imaging data and their mean galaxy redshifts (redshift is related to the third spatial dimension: distance) are often better (spectroscopically) and cheaper (photometrically) when compared with the entire galaxy population in large sky surveys. Photometric redshift (z) [Photometric techniques use the broad band filter magnitudes of a galaxy to estimate the redshift. Spectroscopic techniques use the galaxy spectra and emission/absorption line features to measure the redshift] determinations of galaxies within clusters are accurate to better than delta_z = 0.05 [7] and when studied as a cluster population, the central galaxies form a line in color-magnitude space (called the the E/S0 ridgeline and visible in Figure 16.3) that contains galaxies with similar stellar populations [15]. The shape of this E/S0 ridgeline enables astronomers to measure the cluster redshift to within delta_z = 0.01 [23]. The most accurate cluster redshift determinations come from spectroscopy of the member galaxies, where only a fraction of the members need to be spectroscopically observed [25,42] to get an accurate redshift to the whole system. If light traces mass in the Universe, then the locations of galaxy clusters will be at locations of the peaks in the true underlying (mostly) dark matter density field. Kaiser (1984) [19] called this the high-peak model, which we demonstrate in Figure 16.1. We show a two-dimensional representation of a density field created by summing plane-waves with a predetermined power and with random wave-vector directions. In the left panel, we plot only the largest modes, where we see the density peaks (black) and valleys (white) in the combined field. In the right panel, we allow for smaller modes. You can see that the highest density peaks in the left panel contain smaller-scale, but still high-density peaks. These are the locations of future galaxy clusters. The bottom panel shows just these cluster-scale peaks. As you can see, the peaks themselves are clustered, and instead of just one large high-density peak in the original density field (see the left panel), the smaller modes show that six peaks are "born" within the broader, underlying large-scale density modes. This exemplifies the "bias" or amplified structure that is traced by galaxy clusters [19]. Clusters are rare, easy to find, and their member galaxies provide good distance estimates. In combination with their amplified clustering signal described above, galaxy clusters are considered an efficient and precise tracer of the large-scale matter density field in the Universe. Galaxy clusters can also be used to measure the baryon content of the Universe [43]. They can be used to identify gravitational lenses [38] and map the distribution of matter in clusters. The number and spatial distribution of galaxy clusters can be used to constrain cosmological parameters, like the fraction of the energy density in the Universe due to matter (Omega_matter) or the variation in the density field on fixed physical scales (sigma_8) [26,33]. The individual clusters act as “Island Universes” and as such are laboratories here we can study the evolution of the properties of the cluster, like the hot, gaseous intra-cluster medium or shapes, colors, and star-formation histories of the member galaxies [17].

Interaction of benzene thiol and thiolate with small gold clusters.

PubMed

Letardi, Sara; Cleri, Fabrizio

2004-06-01

We studied the interaction between benzene thiol and thiolate molecules, and gold clusters made of 1 to 3 atoms, by means of ab initio density functional theory in the local density approximation. We find that the thiolate is energetically more stable than the thiol, however the process of detachment of H from the thiol appears to be possibly mediated by the intermediate step of H chemisorption on Au. Cleavage of the S-H bond is accompanied by a 90 degrees rotation of the molecule around the S-Au bond, showing a strong steric specificity. Such a rotation is induced by the relative energy shift of the S atom p orbitals with respect to the benzene pi ring and the Au d orbitals. By analyzing the correlation of the bond energy, bond lengths, and HOMO-LUMO gap with the number of S-Au bonds, we find that the thiolate S atom appears to prefer a low-coordination condition on Au clusters. (c) 2004 American Institute of Physics.

X-ray clusters from a high-resolution hydrodynamic PPM simulation of the cold dark matter universe

NASA Technical Reports Server (NTRS)

Bryan, Greg L.; Cen, Renyue; Norman, Michael L.; Ostriker, Jermemiah P.; Stone, James M.

1994-01-01

A new three-dimensional hydrodynamic code based on the piecewise parabolic method (PPM) is utilized to compute the distribution of hot gas in the standard Cosmic Background Explorer (COBE)-normalized cold dark matter (CDM) universe. Utilizing periodic boundary conditions, a box with size 85 h(exp-1) Mpc, having cell size 0.31 h(exp-1) Mpc, is followed in a simulation with 270(exp 3)=10(exp 7.3) cells. Adopting standard parameters determined from COBE and light-element nucleosynthesis, Sigma(sub 8)=1.05, Omega(sub b)=0.06, we find the X-ray-emitting clusters, compute the luminosity function at several wavelengths, the temperature distribution, and estimated sizes, as well as the evolution of these quantities with redshift. The results, which are compared with those obtained in the preceding paper (Kang et al. 1994a), may be used in conjuction with ROSAT and other observational data sets. Overall, the results of the two computations are qualitatively very similar with regard to the trends of cluster properties, i.e., how the number density, radius, and temeprature depend on luminosity and redshift. The total luminosity from clusters is approximately a factor of 2 higher using the PPM code (as compared to the 'total variation diminishing' (TVD) code used in the previous paper) with the number of bright clusters higher by a similar factor. The primary conclusions of the prior paper, with regard to the power spectrum of the primeval density perturbations, are strengthened: the standard CDM model, normalized to the COBE microwave detection, predicts too many bright X-ray emitting clusters, by a factor probably in excess of 5. The comparison between observations and theoretical predictions for the evolution of cluster properties, luminosity functions, and size and temperature distributions should provide an important discriminator among competing scenarios for the development of structure in the universe.

Experimental and theoretical study of the reactions between neutral vanadium oxide clusters and ethane, ethylene, and acetylene.

PubMed

Dong, Feng; Heinbuch, Scott; Xie, Yan; Rocca, Jorge J; Bernstein, Elliot R; Wang, Zhe-Chen; Deng, Ke; He, Sheng-Gui

2008-02-13

Reactions of neutral vanadium oxide clusters with small hydrocarbons, namely C2H6, C2H4, and C2H2, are investigated by experiment and density functional theory (DFT) calculations. Single photon ionization through extreme ultraviolet (EUV, 46.9 nm, 26.5 eV) and vacuum ultraviolet (VUV, 118 nm, 10.5 eV) lasers is used to detect neutral cluster distributions and reaction products. The most stable vanadium oxide clusters VO2, V2O5, V3O7, V4O10, etc. tend to associate with C2H4 generating products V(m)O(n)C2H4. Oxygen-rich clusters VO3(V2O5)(n=0,1,2...), (e.g., VO3, V3O8, and V5O13) react with C2H4 molecules to cause a cleavage of the C=C bond of C2H4 to produce (V2O5)(n)VO2CH2 clusters. For the reactions of vanadium oxide clusters (V(m)O(n)) with C2H2 molecules, V(m)O(n)C2H2 are assigned as the major products of the association reactions. Additionally, a dehydration reaction for VO3 + C2H2 to produce VO2C2 is also identified. C2H6 molecules are quite stable toward reaction with neutral vanadium oxide clusters. Density functional theory calculations are employed to investigate association reactions for V2O5 + C2H(x). The observed relative reactivity of C2 hydrocarbons toward neutral vanadium oxide clusters is well interpreted by using the DFT calculated binding energies. DFT calculations of the pathways for VO3+C2H4 and VO3+C2H2 reaction systems indicate that the reactions VO3+C2H4 --> VO2CH2 + H2CO and VO3+C2H2 --> VO2C2 + H2O are thermodynamically favorable and overall barrierless at room temperature, in good agreement with the experimental observations.

Study on the electronic structure of Al12N12 and Al12P12 fullerene-like nano-clusters upon adsorption of CH3F and CH3Cl

NASA Astrophysics Data System (ADS)

Shokuhi Rad, A.; Zareyee, D.; Pouralijan Foukolaei, V.; Kamyab Moghadas, B.; Peyravi, M.

2016-11-01

We study the interaction of two mono-halomethanes (CH3F and CH3Cl) on Al12N12 and Al12P12 fullerene-like nano-clusters based on density functional theory (DFT). We search on fully optimised adsorbed systems by theoretical investigation considering binding energies, total density of states, natural bond orbital (NBO) charges, and molecular electrostatic potential. We found that the direction of electron transfer is from halomethane to nano-cluster for all systems, indicating p-type semiconductor property of the mentioned nano-clusters. The interaction energy of halomethanes on nano-clusters is evaluated with dispersion corrected (wB97XD) and non-corrected (B3LYP) methods in order to estimate the dispersion effects. The binding energies are found in order of Al12N12-CH3F > Al12N12-CH3Cl > Al12P12-CH3F > Al12P12-CH3Cl with the values of -102.7, -83.7, -64.2, and -48.9 kJ mol-1 based on wB97XD, respectively. We found significant changes in the location of HOMO as well as LUMO of nano-clusters upon adsorption of the above-mentioned molecules. As a result, we suggest the suitability of Al12N12 nano-cluster as a strong adsorbent for practical applications.

Clustering the Orion B giant molecular cloud based on its molecular emission

NASA Astrophysics Data System (ADS)

Bron, Emeric; Daudon, Chloé; Pety, Jérôme; Levrier, François; Gerin, Maryvonne; Gratier, Pierre; Orkisz, Jan H.; Guzman, Viviana; Bardeau, Sébastien; Goicoechea, Javier R.; Liszt, Harvey; Öberg, Karin; Peretto, Nicolas; Sievers, Albrecht; Tremblin, Pascal

2018-02-01

Context. Previous attempts at segmenting molecular line maps of molecular clouds have focused on using position-position-velocity data cubes of a single molecular line to separate the spatial components of the cloud. In contrast, wide field spectral imaging over a large spectral bandwidth in the (sub)mm domain now allows one to combine multiple molecular tracers to understand the different physical and chemical phases that constitute giant molecular clouds (GMCs). Aims: We aim at using multiple tracers (sensitive to different physical processes and conditions) to segment a molecular cloud into physically/chemically similar regions (rather than spatially connected components), thus disentangling the different physical/chemical phases present in the cloud. Methods: We use a machine learning clustering method, namely the Meanshift algorithm, to cluster pixels with similar molecular emission, ignoring spatial information. Clusters are defined around each maximum of the multidimensional probability density function (PDF) of the line integrated intensities. Simple radiative transfer models were used to interpret the astrophysical information uncovered by the clustering analysis. Results: A clustering analysis based only on the J = 1-0 lines of three isotopologues of CO proves sufficient to reveal distinct density/column density regimes (nH 100 cm-3, 500 cm-3, and >1000 cm-3), closely related to the usual definitions of diffuse, translucent and high-column-density regions. Adding two UV-sensitive tracers, the J = 1-0 line of HCO+ and the N = 1-0 line of CN, allows us to distinguish two clearly distinct chemical regimes, characteristic of UV-illuminated and UV-shielded gas. The UV-illuminated regime shows overbright HCO+ and CN emission, which we relate to a photochemical enrichment effect. We also find a tail of high CN/HCO+ intensity ratio in UV-illuminated regions. Finer distinctions in density classes (nH 7 × 103 cm-3, 4 × 104 cm-3) for the densest regions are also identified, likely related to the higher critical density of the CN and HCO+ (1-0) lines. These distinctions are only possible because the high-density regions are spatially resolved. Conclusions: Molecules are versatile tracers of GMCs because their line intensities bear the signature of the physics and chemistry at play in the gas. The association of simultaneous multi-line, wide-field mapping and powerful machine learning methods such as the Meanshift clustering algorithm reveals how to decode the complex information available in these molecular tracers. Data products associated with this paper are available at the CDS via anonymous ftp to http://cdsarc.u-strasbg.fr (http://130.79.128.5) or via http://cdsarc.u-strasbg.fr/viz-bin/qcat?J/A+A/610/A12 and at http://www.iram.fr/ pety/ORION-B

Chemistry and Processing of Nanostructured Materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fox, G A; Baumann, T F; Hope-Weeks, L J

2002-01-18

Nanostructured materials can be formed through the sol-gel polymerization of inorganic or organic monomer systems. For example, a two step polymerization of tetramethoxysilane (TMOS) was developed such that silica aerogels with densities as low as 3 kg/m{sup 3} ({approx} two times the density of air) could be achieved. Organic aerogels based upon resorcinol-formaldehyde and melamine-formaldehyde can also be prepared using the sol-gel process. Materials of this type have received significant attention at LLNL due to their ultrafine cell sizes, continuous porosity, high surface area and low mass density. For both types of aerogels, sol-gel polymerization depends upon the transformation ofmore » these monomers into nanometer-sized clusters followed by cross-linking into a 3-dimensional gel network. While sol-gel chemistry provides the opportunity to synthesize new material compositions, it suffers from the inability to separate the process of cluster formation from gelation. This limitation results in structural deficiencies in the gel that impact the physical properties of the aerogel, xerogel or nanocomposite. In order to control the properties of the resultant gel, one should be able to regulate the formation of the clusters and their subsequent cross-linking. Towards this goal, we are utilizing dendrimer chemistry to separate the cluster formation from the gelation so that new nanostructured materials can be produced. Dendrimers are three-dimensional, highly branched macromolecules that are prepared in such a way that their size, shape and surface functionality are readily controlled. The dendrimers will be used as pre-formed clusters of known size that can be cross-linked to form an ordered gel network.« less

Dark Energy and Key Physical Parameters of Clusters of Galaxies

NASA Astrophysics Data System (ADS)

Chernin, A. D.; Bisnovatyi-Kogan, G. S.

We discuss the physics of clusters of galaxies embedded in the cosmic dark energy background and show that 1) the halo cut-off radius of a cluster like the Virgo cluster is practically, if not exactly, equal to the zero-gravity radius at which the dark matter gravity is balanced by the dark energy antigravity; 2) the halo averaged density is equal to two densities of dark energy; 3) the halo edge (cut-off) density is the dark energy density with a numerical factor of the unity order slightly depending on the halo profile.

Preparing transition-metal clusters in known structural forms: the mass-analyzed threshold ionization spectrum of V3.

PubMed

Ford, Mark S; Mackenzie, Stuart R

2005-08-22

The first results are presented of a new experiment designed both to generate and characterize spectroscopically individual isomers of transition-metal cluster cations. As a proof of concept the one-photon mass-analyzed threshold ionization (MATI) spectrum of V3 has been recorded in the region of 44,000-45,000 cm-1. This study extends the range of a previous zero-kinetic-energy (ZEKE) photoelectron study of Yang et al. [Chem. Phys. Lett. 231, 177 (1994)] with which the current results are compared. The MATI spectra reported here exhibit surprisingly high resolution (0.2 cm-1) for this technique despite the use of large discrimination and extraction fields. Analysis of the rotational profile of the origin band allows assignment of the V3 ground state as and the V3+ ground state as , both with D3h geometry, in agreement with the density-functional theory study of the V3 ZEKE spectrum by Calaminici et al. [J. Chem. Phys. 114, 4036 (2001)]. There is also some evidence in the spectrum of transitions to the low-lying excited state of the ion. The vibrational structure observed in the MATI spectrum is, however, significantly different to and less extensive than that predicted in the density-functional theory study. Possible reasons for the discrepancies are discussed and an alternative assignment is proposed which results in revised values for the vibrational wave numbers of both the neutral and ionic states. These studies demonstrate the efficient generation of cluster ions in known structural (isomeric) forms and pave the way for the study of cluster reactivity as a function of geometrical structure.

Ceria nanoclusters on graphene/Ru(0001): A new model catalyst system

DOE PAGES

Novotny, Z.; Netzer, F. P.; Dohnalek, Z.

2016-03-22

In this study, the growth of ceria nanoclusters on single-layer graphene on Ru(0001) has been examined, with a view towards fabricating a stable system for model catalysis studies. The surface morphology and cluster distribution as a function of oxide coverage and substrate temperature has been monitored by scanning tunneling microscopy (STM), whereas the chemical composition of the cluster deposits has been determined by Auger electron spectroscopy (AES). The ceria nanoparticles are of the CeO 2(111)-type and are anchored at the intrinsic defects of the graphene surface, resulting in a variation of the cluster densities across the macroscopic sample surface. Themore » ceria clusters on graphene display a remarkable stability against reduction in ultrahigh vacuum up to 900 K, but some sintering of clusters is observed for temperatures > 450 K. The evolution of the cluster size distribution suggests that the sintering proceeds via a Smoluchowski ripening mechanism, i.e. diffusion and aggregation of entire clusters.« less

Neutral and charged gallium clusters: structures, physical properties and implications for the melting features

NASA Astrophysics Data System (ADS)

Núñez, Sara; López, José M.; Aguado, Andrés

2012-09-01

We report the putative Global Minimum (GM) structures and electronic properties of GaN+, GaN and GaN- clusters with N = 13-37 atoms, obtained from first-principles density functional theory structural optimizations. The calculations include spin polarization and employ an exchange-correlation functional which accounts for van der Waals dispersion interactions (vdW-DFT). We find a wide diversity of structural motifs within the located GM, including decahedral, polyicosahedral, polytetrahedral and layered structures. The GM structures are also extremely sensitive to the number of electrons in the cluster, so that the structures of neutral and charged clusters differ for most sizes. The main magic numbers (clusters with an enhanced stability) are identified and interpreted in terms of electronic and geometric shell closings. The theoretical results are consistent with experimental abundance mass spectra of GaN+ and with photoelectron spectra of GaN-. The size dependence of the latent heats of melting, the shape of the heat capacity peaks, and the temperature dependence of the collision cross-sections, all measured for GaN+ clusters, are properly interpreted in terms of the calculated cohesive energies, spectra of configurational excitations, and cluster shapes, respectively. The transition from ``non-melter'' to ``magic-melter'' behaviour, experimentally observed between Ga30+ and Ga31+, is traced back to a strong geometry change. Finally, the higher-than-bulk melting temperatures of gallium clusters are correlated with a more typically metallic behaviour of the clusters as compared to the bulk, contrary to previous theoretical claims.We report the putative Global Minimum (GM) structures and electronic properties of GaN+, GaN and GaN- clusters with N = 13-37 atoms, obtained from first-principles density functional theory structural optimizations. The calculations include spin polarization and employ an exchange-correlation functional which accounts for van der Waals dispersion interactions (vdW-DFT). We find a wide diversity of structural motifs within the located GM, including decahedral, polyicosahedral, polytetrahedral and layered structures. The GM structures are also extremely sensitive to the number of electrons in the cluster, so that the structures of neutral and charged clusters differ for most sizes. The main magic numbers (clusters with an enhanced stability) are identified and interpreted in terms of electronic and geometric shell closings. The theoretical results are consistent with experimental abundance mass spectra of GaN+ and with photoelectron spectra of GaN-. The size dependence of the latent heats of melting, the shape of the heat capacity peaks, and the temperature dependence of the collision cross-sections, all measured for GaN+ clusters, are properly interpreted in terms of the calculated cohesive energies, spectra of configurational excitations, and cluster shapes, respectively. The transition from ``non-melter'' to ``magic-melter'' behaviour, experimentally observed between Ga30+ and Ga31+, is traced back to a strong geometry change. Finally, the higher-than-bulk melting temperatures of gallium clusters are correlated with a more typically metallic behaviour of the clusters as compared to the bulk, contrary to previous theoretical claims. Electronic supplementary information (ESI) available: Atomic coordinates (in xyz format and Å units) and point group symmetries for the global minimum structures reported in this paper. See DOI: 10.1039/c2nr31222k

Radiation hydrodynamics of super star cluster formation

NASA Astrophysics Data System (ADS)

Tsang, Benny Tsz Ho; Milos Milosavljevic

2018-01-01

Throughout the history of the Universe, the nuclei of super star clusters represent the most active sites for star formation. The high densities of massive stars within the clusters produce intense radiation that imparts both energy and momentum on the surrounding star-forming gas. Theoretical claims based on idealized geometries have claimed the dominant role of radiation pressure in controlling the star formation activity within the clusters. In order for cluster formation simulations to be reliable, numerical schemes have to be able to model accurately the radiation flows through the gas clumps at the cluster nuclei with high density contrasts. With a hybrid Monte Carlo radiation transport module we developed, we performed 3D radiation hydrodynamical simulations of super star cluster formation in turbulent clouds. Furthermore, our Monte Carlo radiation treatment provides a native capability to produce synthetic observations, which allows us to predict observational indicators and to inform future observations. We found that radiation pressure has definite, but minor effects on limiting the gas supply for star formation, and the final mass of the most massive cluster is about one million solar masses. The ineffective forcing was due to the density variations inside the clusters, i.e. radiation takes the paths of low densities and avoids forcing on dense clumps. Compared to a radiation-free control run, we further found that the presence of radiation amplifies the density variations. The core of the resulting cluster has a high stellar density, about the threshold required for stellar collisions and merging. The very massive star that form from the stellar merging could continue to gain mass from the surrounding gas reservoir that is gravitationally confined by the deep potential of the cluster, seeding the potential formation of a massive black hole.

High-Order Ca(II)-Chloro Complexes in Mixed CaCl2-LiCl Aqueous Solution: Insights from Density Functional Theory and Molecular Dynamics Simulations.

PubMed

Wang, Yu-Lin; Wang, Ying; Yi, Hai-Bo

2016-07-21

In this study, the structural characteristics of high-coordinated Ca-Cl complexes present in mixed CaCl2-LiCl aqueous solution were investigated using density functional theory (DFT) and molecular dynamics (MD) simulations. The DFT results show that [CaClx](2-x) (x = 4-6) clusters are quite unstable in the gas phase, but these clusters become metastable when hydration is considered. The MD simulations show that high-coordinated Ca-chloro complexes are possible transient species that exist for up to nanoseconds in concentrated (11.10 mol·kg(-1)) Cl(-) solution at 273 and 298 K. As the temperature increases to 423 K, these high-coordinated structures tend to disassociate and convert into smaller clusters and single free ions. The presence of high-order Ca-Cl species in concentrated LiCl solution can be attributed to their enhanced hydration shell and the inadequate hydration of ions. The probability of the [CaClx](2-x)aq (x = 4-6) species being present in concentrated LiCl solution decreases greatly with increasing temperature, which also indicates that the formation of the high-coordinated Ca-Cl structure is related to its hydration characteristics.

Probing the Initial Mass Function in Extended Ultraviolet (XUV) Disks

NASA Astrophysics Data System (ADS)

Koda, Jin

2012-01-01

"The GALEX UV satellite discovered tantalizing evidence of star formation (SF) far beyond the optical edge of galactic disks (i.e. extended UV disk, or XUV disk). This discovery provides a new opportunity for studying SF in the exceedingly low-density environment (˜1/10 of typical SF density), spurring intense debate on the universality of the initial mass function (IMF) in such exceptional environments. Our pilot S-Cam study of M83’s XUV disk led to support for the universal IMF at least in M83 (Koda et al. 2012). We propose an expansion of the pilot study, observing 6 XUV disks in NA656(Hα), B, I, and R-band with S-Cam. In conjunction with GALEX UV bands, these images will reveal the presence of O stars (Hα; NA656-R) and O&B stars (UV) in stellar clusters -thus, constraining the high-mass end of the IMF. The multi-broadband images will enable us to determine the masses of the clusters with much improved accuracy (previously, relied only on R). The proposed observations will not only increase the statistical significance of our previous result, but also enable us to analyze the stochastic effect of IMF sampling in very low-mass clusters (10^{2+3} M_sun) - the regime about which there is much ongoing debate."

An all-electron density functional theory study of the structure and properties of the neutral and singly charged M12 and M13 clusters: M = Sc-Zn.

PubMed

Gutsev, G L; Weatherford, C W; Belay, K G; Ramachandran, B R; Jena, P

2013-04-28

The electronic and geometrical structures of the M12 and M13 clusters where M = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, and Zn along with their singly negatively and positively charged ions are studied using all-electron density functional theory within the generalized gradient approximation. The geometries corresponding to the lowest total energy states of singly and negatively charged ions of V13, Mn12, Co12, Ni13, Cu13, Zn12, and Zn13 are found to be different from the geometries of the corresponding neutral parents. The computed ionization energies of the neutrals, vertical electron detachment energies from the anions, and energies required to remove a single atom from the M13 and M13(+) clusters are in good agreement with experiment. The change in a total spin magnetic moment of the cation or anion with respect to a total spin magnetic moment of the corresponding neutral is consistent with the one-electron model in most cases, i.e., they differ by ±1.0 μ(B). Exceptions are found only for Sc12(-), Ti12(+), Mn12(-), Mn12(+), Fe12(-), Fe13(+), and Co12(+).

O2 adsorbed on Ptn clusters: Structure and optical absorption

NASA Astrophysics Data System (ADS)

Wang, Ruiying; Zhao, Liang; Jia, Jianfeng; Wu, Hai-Shun

2018-03-01

The interaction of O2 with Ptn and the optical absorption properties of PtnO2 were explored under the framework of density functional theory. The Ptn (n= 2, 4, 6, 9, 10, 14, 18, 22, and 27) clusters were selected, which were reported as magnetic number Ptn clusters in reference (V. Kumar and Y. Kawazoe, Phys. Rev. B 77(20), 205418 (2008)). The single Pt atom was also considered. The longest O2 bonds were found for Pt27O2, Pt6O2 and Pt14O2, while PtO2 and Pt2O2 have the shortest O2 bonds. This result showed that the single Pt atom was not preferred for O2 activation. The O2 bond length was closely related to the electron transfer from Ptn to O2. The optical absorptions of PtnO2 were investigated with time-dependent density functional theory method. A new term of charge transfer strength was defined to estimate the further electron transfer from Ptn to O2 caused by the optical absorption in the visible light range. Our calculations showed that with the increasing n, the further electron transfer from Ptn to O2 caused by optical absorption will become very weak.

Mapping the genome of meta-generalized gradient approximation density functionals: The search for B97M-V

NASA Astrophysics Data System (ADS)

Mardirossian, Narbe; Head-Gordon, Martin

2015-02-01

A meta-generalized gradient approximation density functional paired with the VV10 nonlocal correlation functional is presented. The functional form is selected from more than 1010 choices carved out of a functional space of almost 1040 possibilities. Raw data come from training a vast number of candidate functional forms on a comprehensive training set of 1095 data points and testing the resulting fits on a comprehensive primary test set of 1153 data points. Functional forms are ranked based on their ability to reproduce the data in both the training and primary test sets with minimum empiricism, and filtered based on a set of physical constraints and an often-overlooked condition of satisfactory numerical precision with medium-sized integration grids. The resulting optimal functional form has 4 linear exchange parameters, 4 linear same-spin correlation parameters, and 4 linear opposite-spin correlation parameters, for a total of 12 fitted parameters. The final density functional, B97M-V, is further assessed on a secondary test set of 212 data points, applied to several large systems including the coronene dimer and water clusters, tested for the accurate prediction of intramolecular and intermolecular geometries, verified to have a readily attainable basis set limit, and checked for grid sensitivity. Compared to existing density functionals, B97M-V is remarkably accurate for non-bonded interactions and very satisfactory for thermochemical quantities such as atomization energies, but inherits the demonstrable limitations of existing local density functionals for barrier heights.

A theoretical study of the reaction of Ti+ with ethane

NASA Astrophysics Data System (ADS)

Moc, Jerzy; Fedorov, Dmitri G.; Gordon, Mark S.

2000-06-01

The doublet and quartet potential energy surfaces for the Ti++C2H6→TiC2H4++H2 and Ti++C2H6→TiCH2++CH4 reactions are studied using density functional theory (DFT) with the B3LYP functional and ab initio coupled cluster CCSD(T) methods with high quality basis sets. Structures have been optimized at the DFT level and the minima connected to each transition state (TS) by following the intrinsic reaction coordinate (IRC). Relative energies are calculated both at the DFT and coupled-cluster levels of theory. The relevant parts of the potential energy surface, especially key transition states, are also studied using multireference wave functions with the final energetics obtained with multireference second-order perturbation theory.

Genarris: Random generation of molecular crystal structures and fast screening with a Harris approximation

NASA Astrophysics Data System (ADS)

Li, Xiayue; Curtis, Farren S.; Rose, Timothy; Schober, Christoph; Vazquez-Mayagoitia, Alvaro; Reuter, Karsten; Oberhofer, Harald; Marom, Noa

2018-06-01

We present Genarris, a Python package that performs configuration space screening for molecular crystals of rigid molecules by random sampling with physical constraints. For fast energy evaluations, Genarris employs a Harris approximation, whereby the total density of a molecular crystal is constructed via superposition of single molecule densities. Dispersion-inclusive density functional theory is then used for the Harris density without performing a self-consistency cycle. Genarris uses machine learning for clustering, based on a relative coordinate descriptor developed specifically for molecular crystals, which is shown to be robust in identifying packing motif similarity. In addition to random structure generation, Genarris offers three workflows based on different sequences of successive clustering and selection steps: the "Rigorous" workflow is an exhaustive exploration of the potential energy landscape, the "Energy" workflow produces a set of low energy structures, and the "Diverse" workflow produces a maximally diverse set of structures. The latter is recommended for generating initial populations for genetic algorithms. Here, the implementation of Genarris is reported and its application is demonstrated for three test cases.

Quadratic canonical transformation theory and higher order density matrices.

PubMed

Neuscamman, Eric; Yanai, Takeshi; Chan, Garnet Kin-Lic

2009-03-28

Canonical transformation (CT) theory provides a rigorously size-extensive description of dynamic correlation in multireference systems, with an accuracy superior to and cost scaling lower than complete active space second order perturbation theory. Here we expand our previous theory by investigating (i) a commutator approximation that is applied at quadratic, as opposed to linear, order in the effective Hamiltonian, and (ii) incorporation of the three-body reduced density matrix in the operator and density matrix decompositions. The quadratic commutator approximation improves CT's accuracy when used with a single-determinant reference, repairing the previous formal disadvantage of the single-reference linear CT theory relative to singles and doubles coupled cluster theory. Calculations on the BH and HF binding curves confirm this improvement. In multireference systems, the three-body reduced density matrix increases the overall accuracy of the CT theory. Tests on the H(2)O and N(2) binding curves yield results highly competitive with expensive state-of-the-art multireference methods, such as the multireference Davidson-corrected configuration interaction (MRCI+Q), averaged coupled pair functional, and averaged quadratic coupled cluster theories.

Analyzing the errors of DFT approximations for compressed water systems

NASA Astrophysics Data System (ADS)

Alfè, D.; Bartók, A. P.; Csányi, G.; Gillan, M. J.

2014-07-01

We report an extensive study of the errors of density functional theory (DFT) approximations for compressed water systems. The approximations studied are based on the widely used PBE and BLYP exchange-correlation functionals, and we characterize their errors before and after correction for 1- and 2-body errors, the corrections being performed using the methods of Gaussian approximation potentials. The errors of the uncorrected and corrected approximations are investigated for two related types of water system: first, the compressed liquid at temperature 420 K and density 1.245 g/cm3 where the experimental pressure is 15 kilobars; second, thermal samples of compressed water clusters from the trimer to the 27-mer. For the liquid, we report four first-principles molecular dynamics simulations, two generated with the uncorrected PBE and BLYP approximations and a further two with their 1- and 2-body corrected counterparts. The errors of the simulations are characterized by comparing with experimental data for the pressure, with neutron-diffraction data for the three radial distribution functions, and with quantum Monte Carlo (QMC) benchmarks for the energies of sets of configurations of the liquid in periodic boundary conditions. The DFT errors of the configuration samples of compressed water clusters are computed using QMC benchmarks. We find that the 2-body and beyond-2-body errors in the liquid are closely related to similar errors exhibited by the clusters. For both the liquid and the clusters, beyond-2-body errors of DFT make a substantial contribution to the overall errors, so that correction for 1- and 2-body errors does not suffice to give a satisfactory description. For BLYP, a recent representation of 3-body energies due to Medders, Babin, and Paesani [J. Chem. Theory Comput. 9, 1103 (2013)] gives a reasonably good way of correcting for beyond-2-body errors, after which the remaining errors are typically 0.5 mEh ≃ 15 meV/monomer for the liquid and the clusters.

Analyzing the errors of DFT approximations for compressed water systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alfè, D.; London Centre for Nanotechnology, UCL, London WC1H 0AH; Thomas Young Centre, UCL, London WC1H 0AH

We report an extensive study of the errors of density functional theory (DFT) approximations for compressed water systems. The approximations studied are based on the widely used PBE and BLYP exchange-correlation functionals, and we characterize their errors before and after correction for 1- and 2-body errors, the corrections being performed using the methods of Gaussian approximation potentials. The errors of the uncorrected and corrected approximations are investigated for two related types of water system: first, the compressed liquid at temperature 420 K and density 1.245 g/cm{sup 3} where the experimental pressure is 15 kilobars; second, thermal samples of compressed watermore » clusters from the trimer to the 27-mer. For the liquid, we report four first-principles molecular dynamics simulations, two generated with the uncorrected PBE and BLYP approximations and a further two with their 1- and 2-body corrected counterparts. The errors of the simulations are characterized by comparing with experimental data for the pressure, with neutron-diffraction data for the three radial distribution functions, and with quantum Monte Carlo (QMC) benchmarks for the energies of sets of configurations of the liquid in periodic boundary conditions. The DFT errors of the configuration samples of compressed water clusters are computed using QMC benchmarks. We find that the 2-body and beyond-2-body errors in the liquid are closely related to similar errors exhibited by the clusters. For both the liquid and the clusters, beyond-2-body errors of DFT make a substantial contribution to the overall errors, so that correction for 1- and 2-body errors does not suffice to give a satisfactory description. For BLYP, a recent representation of 3-body energies due to Medders, Babin, and Paesani [J. Chem. Theory Comput. 9, 1103 (2013)] gives a reasonably good way of correcting for beyond-2-body errors, after which the remaining errors are typically 0.5 mE{sub h} ≃ 15 meV/monomer for the liquid and the clusters.« less

The Excursion Set Theory of Halo Mass Functions, Halo Clustering, and Halo Growth

NASA Astrophysics Data System (ADS)

Zentner, Andrew R.

I review the excursion set theory with particular attention toward applications to cold dark matter halo formation and growth, halo abundance, and halo clustering. After a brief introduction to notation and conventions, I begin by recounting the heuristic argument leading to the mass function of bound objects given by Press and Schechter. I then review the more formal derivation of the Press-Schechter halo mass function that makes use of excursion sets of the density field. The excursion set formalism is powerful and can be applied to numerous other problems. I review the excursion set formalism for describing both halo clustering and bias and the properties of void regions. As one of the most enduring legacies of the excursion set approach and one of its most common applications, I spend considerable time reviewing the excursion set theory of halo growth. This section of the review culminates with the description of two Monte Carlo methods for generating ensembles of halo mass accretion histories. In the last section, I emphasize that the standard excursion set approach is the result of several simplifying assumptions. Dropping these assumptions can lead to more faithful predictions and open excursion set theory to new applications. One such assumption is that the height of the barriers that define collapsed objects is a constant function of scale. I illustrate the implementation of the excursion set approach for barriers of arbitrary shape. One such application is the now well-known improvement of the excursion set mass function derived from the "moving" barrier for ellipsoidal collapse. I also emphasize that the statement that halo accretion histories are independent of halo environment in the excursion set approach is not a general prediction of the theory. It is a simplifying assumption. I review the method for constructing correlated random walks of the density field in the more general case. I construct a simple toy model to illustrate that excursion set theory (with a constant barrier height) makes a simple and general prediction for the relation between halo accretion histories and the large-scale environments of halos: regions of high density preferentially contain late-forming halos and conversely for regions of low density. I conclude with a brief discussion of the importance of this prediction relative to recent numerical studies of the environmental dependence of halo properties.

Scaffold Architecture Controls Insulinoma Clustering, Viability, and Insulin Production

PubMed Central

Blackstone, Britani N.; Palmer, Andre F.; Rilo, Horacio R.

2014-01-01

Recently, in vitro diagnostic tools have shifted focus toward personalized medicine by incorporating patient cells into traditional test beds. These cell-based platforms commonly utilize two-dimensional substrates that lack the ability to support three-dimensional cell structures seen in vivo. As monolayer cell cultures have previously been shown to function differently than cells in vivo, the results of such in vitro tests may not accurately reflect cell response in vivo. It is therefore of interest to determine the relationships between substrate architecture, cell structure, and cell function in 3D cell-based platforms. To investigate the effect of substrate architecture on insulinoma organization and function, insulinomas were seeded onto 2D gelatin substrates and 3D fibrous gelatin scaffolds with three distinct fiber diameters and fiber densities. Cell viability and clustering was assessed at culture days 3, 5, and 7 with baseline insulin secretion and glucose-stimulated insulin production measured at day 7. Small, closely spaced gelatin fibers promoted the formation of large, rounded insulinoma clusters, whereas monolayer organization and large fibers prevented cell clustering and reduced glucose-stimulated insulin production. Taken together, these data show that scaffold properties can be used to control the organization and function of insulin-producing cells and may be useful as a 3D test bed for diabetes drug development. PMID:24410263

Interactions of small platinum clusters with the TiC(001) surface

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mao, Jianjun; Li, Shasha; Chu, Xingli

2015-11-14

Density functional theory calculations are used to elucidate the interactions of small platinum clusters (Pt{sub n}, n = 1–5) with the TiC(001) surface. The results are analyzed in terms of geometric, energetic, and electronic properties. It is found that a single Pt atom prefers to be adsorbed at the C-top site, while a Pt{sub 2} cluster prefers dimerization and a Pt{sub 3} cluster forms a linear structure on the TiC(001). As for the Pt{sub 4} cluster, the three-dimensional distorted tetrahedral structure and the two-dimensional square structure almost have equal stability. In contrast with the two-dimensional isolated Pt{sub 5} cluster, the adsorbed Pt{submore » 5} cluster prefers a three-dimensional structure on TiC(001). Substantial charge transfer takes place from TiC(001) surface to the adsorbed Pt{sub n} clusters, resulting in the negatively charged Pt{sub n} clusters. At last, the d-band centers of the absorbed Pt atoms and their implications in the catalytic activity are discussed.« less

Magnetic behavior in Cr{sub 2}@Ge{sub n} (1≤n≤12) clusters: A density functional investigation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dhaka, Kapil, E-mail: kapil.dhaka@pilani.bits-pilani.ac.in; Trivedi, Ravi, E-mail: kapil.dhaka@pilani.bits-pilani.ac.in; Bandyopadhyay, Debashis, E-mail: kapil.dhaka@pilani.bits-pilani.ac.in

2014-04-24

With a goal to produce magnetic moment in Cr{sub 2} Doped Ge{sub n} clusters which will be useful for practical applications, we have considered the structure and magnetic properties of Pure Germanium clusters and substitutionally doped it with Cr dimer to produce Cr{sub 2}@Ge{sub n} clusters. As the first step of calculation, geometrical optimizations of the nanoclusters have been done. These optimized geometries have been used in calculate the average binding energy per atom (BE), HOMO-LUMO gap and hence the relative stability of the clusters. These parameters have been demonstrated as structural and electronic properties of the clusters. Gap betweenmore » highest occupied molecular orbital and lowest unoccupied molecular orbital indicate cluster to be a potential motif for generating magnetic cluster assembled materials. Based on these values a comparative study on different sized clusters has been done in order to understand the origin of structures, electronic and magnetic properties of Cr{sub 2}@Ge{sub n} nanoclusters.« less

Galaxy Clustering Around Nearby Luminous Quasars

NASA Technical Reports Server (NTRS)

Fisher, Karl B.; Bahcall, John N.; Kirhakos, Sofia; Schneider, Donald P.

1996-01-01

We examine the clustering of galaxies around a sample of 20 luminous low redshift (z approx. less than 0.30) quasars observed with the Wide Field Camera-2 on the Hubble Space Telescope (HST). The HST resolution makes possible galaxy identification brighter than V = 24.5 and as close as 1 min or 2 min to the quasar. We find a significant enhancement of galaxies within a projected separation of approx. less than 100 1/h kpc of the quasars. If we model the QSO/galaxy correlation function as a power law with a slope given by the galaxy/galaxy correlation function, we find that the ratio of the QSO/galaxy to galaxy/galaxy correlation functions is 3.8 +/- 0.8. The galaxy counts within r less than 15 1/h kpc of the quasars are too high for the density profile to have an appreciable core radius (approx. greater than 100 1/h kpc). Our results reinforce the idea that low redshift quasars are located preferentially in groups of 10-20 galaxies rather than in rich clusters. We see no significant difference in the clustering amplitudes derived from radio-loud and radio-quiet subsamples.

Change of Brain Functional Connectivity in Patients With Spinal Cord Injury: Graph Theory Based Approach.

PubMed

Min, Yu-Sun; Chang, Yongmin; Park, Jang Woo; Lee, Jong-Min; Cha, Jungho; Yang, Jin-Ju; Kim, Chul-Hyun; Hwang, Jong-Moon; Yoo, Ji-Na; Jung, Tae-Du

2015-06-01

To investigate the global functional reorganization of the brain following spinal cord injury with graph theory based approach by creating whole brain functional connectivity networks from resting state-functional magnetic resonance imaging (rs-fMRI), characterizing the reorganization of these networks using graph theoretical metrics and to compare these metrics between patients with spinal cord injury (SCI) and age-matched controls. Twenty patients with incomplete cervical SCI (14 males, 6 females; age, 55±14.1 years) and 20 healthy subjects (10 males, 10 females; age, 52.9±13.6 years) participated in this study. To analyze the characteristics of the whole brain network constructed with functional connectivity using rs-fMRI, graph theoretical measures were calculated including clustering coefficient, characteristic path length, global efficiency and small-worldness. Clustering coefficient, global efficiency and small-worldness did not show any difference between controls and SCIs in all density ranges. The normalized characteristic path length to random network was higher in SCI patients than in controls and reached statistical significance at 12%-13% of density (p<0.05, uncorrected). The graph theoretical approach in brain functional connectivity might be helpful to reveal the information processing after SCI. These findings imply that patients with SCI can build on preserved competent brain control. Further analyses, such as topological rearrangement and hub region identification, will be needed for better understanding of neuroplasticity in patients with SCI.

Embedded-cluster calculations in a numeric atomic orbital density-functional theory framework.

PubMed

Berger, Daniel; Logsdail, Andrew J; Oberhofer, Harald; Farrow, Matthew R; Catlow, C Richard A; Sherwood, Paul; Sokol, Alexey A; Blum, Volker; Reuter, Karsten

2014-07-14

We integrate the all-electron electronic structure code FHI-aims into the general ChemShell package for solid-state embedding quantum and molecular mechanical (QM/MM) calculations. A major undertaking in this integration is the implementation of pseudopotential functionality into FHI-aims to describe cations at the QM/MM boundary through effective core potentials and therewith prevent spurious overpolarization of the electronic density. Based on numeric atomic orbital basis sets, FHI-aims offers particularly efficient access to exact exchange and second order perturbation theory, rendering the established QM/MM setup an ideal tool for hybrid and double-hybrid level density functional theory calculations of solid systems. We illustrate this capability by calculating the reduction potential of Fe in the Fe-substituted ZSM-5 zeolitic framework and the reaction energy profile for (photo-)catalytic water oxidation at TiO2(110).

Embedded-cluster calculations in a numeric atomic orbital density-functional theory framework

DOE Office of Scientific and Technical Information (OSTI.GOV)

Berger, Daniel, E-mail: daniel.berger@ch.tum.de; Oberhofer, Harald; Reuter, Karsten

2014-07-14

We integrate the all-electron electronic structure code FHI-aims into the general ChemShell package for solid-state embedding quantum and molecular mechanical (QM/MM) calculations. A major undertaking in this integration is the implementation of pseudopotential functionality into FHI-aims to describe cations at the QM/MM boundary through effective core potentials and therewith prevent spurious overpolarization of the electronic density. Based on numeric atomic orbital basis sets, FHI-aims offers particularly efficient access to exact exchange and second order perturbation theory, rendering the established QM/MM setup an ideal tool for hybrid and double-hybrid level density functional theory calculations of solid systems. We illustrate this capabilitymore » by calculating the reduction potential of Fe in the Fe-substituted ZSM-5 zeolitic framework and the reaction energy profile for (photo-)catalytic water oxidation at TiO{sub 2}(110)« less

Searching for a 4 α linear-chain structure in excited states of 16O with covariant density functional theory

NASA Astrophysics Data System (ADS)

Yao, J. M.; Itagaki, N.; Meng, J.

2014-11-01

A study of the 4 α linear-chain structure in high-lying collective excitation states of 16O with covariant density functional theory is presented. The low-spin states are obtained by configuration mixing of particle-number and angular-momentum projected quadrupole deformed mean-field states with the generator coordinate method. The high-spin states are determined by cranking calculations. These two calculations are based on the same energy density functional PC-PK1. We have found a rotational band at low spin with the dominant intrinsic configuration considered to be the one whereby 4 α clusters stay along a common axis. The strongly deformed rod shape also appears in the high-spin region with the angular momentum 13 ℏ to18 ℏ ; however, whether the state is a pure 4 α linear chain is less obvious than for the low-spin states.

Dielectric function for doped graphene layer with barium titanate

NASA Astrophysics Data System (ADS)

Martinez Ramos, Manuel; Garces Garcia, Eric; Magana, Fernado; Vazquez Fonseca, Gerardo Jorge

2015-03-01

The aim of our study is to calculate the dielectric function for a system formed with a graphene layer doped with barium titanate. Density functional theory, within the local density approximation, plane-waves and pseudopotentials scheme as implemented in Quantum Espresso suite of programs was used. We considered 128 carbon atoms with a barium titanate cluster of 11 molecules as unit cell with periodic conditions. The geometry optimization is achieved. Optimization of structural configuration is performed by relaxation of all atomic positions to minimize their total energies. Band structure, density of states and linear optical response (the imaginary part of dielectric tensor) were calculated. We thank Dirección General de Asuntos del Personal Académico de la Universidad Nacional Autónoma de México, partial financial support by Grant IN-106514 and we also thank Miztli Super-Computing center the technical assistance.

Atomically resolved structure of ligand-protected Au{sub 9} clusters on TiO{sub 2} nanosheets using aberration-corrected STEM

DOE Office of Scientific and Technical Information (OSTI.GOV)

Al Qahtani, Hassan S.; Andersson, Gunther G., E-mail: gunther.andersson@flinders.edu.au, E-mail: nakayama.tomonobu@nims.go.jp; Kimoto, Koji

2016-03-21

Triphenylphosphine ligand-protected Au{sub 9} clusters deposited onto titania nanosheets show three different atomic configurations as observed by scanning transmission electron microscopy. The configurations observed are a 3-dimensional structure, corresponding to the previously proposed Au{sub 9} core of the clusters, and two pseudo-2-dimensional (pseudo-2D) structures, newly found by this work. With the help of density functional theory (DFT) calculations, the observed pseudo-2D structures are attributed to the low energy, de-ligated structures formed through interaction with the substrate. The combination of scanning transmission electron microscopy with DFT calculations thus allows identifying whether or not the deposited Au{sub 9} clusters have been de-ligatedmore » in the deposition process.« less

First-Principles Study of Structural, Electronic and Magnetic Properties of Metal-Centered Tetrahexahedral V15+ Cluster

PubMed Central

Ren, Hongjiang; Huang, Xinwei; Li, Shuna

2017-01-01

The V-centered bicapped hexagonal antiprism structure (A), as the most stable geometry of the cationic V15+ cluster, is determined by using infrared multiple photo dissociation (IR-MPD) in combination with density functional theory computations. It is found that the A structure can be stabilized by 18 delocalized 3c-2e σ-bonds on outer V3 triangles of the bicapped hexagonal antiprism surface and 12 delocalized 4c-2e σ-bonds on inner trigonal pyramidal V4 moiety, and the features are related to the strong p-d hybridization of the cluster. The total magnetic moments on the cluster are predicted to be 2.0 µB, which come mainly from the central vanadium atom. PMID:28665337

Clustering of amines and hydrazines in atmospheric nucleation

NASA Astrophysics Data System (ADS)

Li, Siyang; Qu, Kun; Zhao, Hailiang; Ding, Lei; Du, Lin

2016-06-01

It has been proved that the presence of amines in the atmosphere can enhance aerosol formation. Hydrazine (HD) and its substituted derivatives, monomethylhydrazine (MMH) and unsymmetrical dimethylhydrazine (UDMH), which are organic derivatives of amine and ammonia, are common trace atmospheric species that may contribute to the growth of nucleation clusters. The structures of the hydrazine and amine clusters containing one or two common nucleation molecules (ammonia, water, methanol and sulfuric acid) have been optimized using density functional theory (DFT) methods. The clusters growth mechanism has been explored from the thermochemistry by calculating the Gibbs free energies of adding an ammonia, water, methanol or sulfuric acid molecule step by step at room temperature, respectively. The results show that hydrazine and its derivatives could enhance heteromolecular homogeneous nucleation in the earth's atmosphere.

Low-symmetry structures of Au32Z (Z = +1, 0, -1) clusters.

PubMed

Jalbout, Abraham F; Contreras-Torres, Flavio F; Pérez, Luis A; Garzón, Ignacio L

2008-01-24

In this work, we have explored new stable structures of the Au32Z (Z = +1, 0, -1) clusters. Theoretical calculations using density functional theory within the generalized-gradient approximation were performed. Our results show that, in the anion state (Au32-), low-symmetry (disordered) structures are preferred over the caged fullerene-like isomer. In addition, the cationic cluster (Au32+) also exhibits a disordered low-symmetry structure as its lowest energy configuration, but it is much closer in energy to the fullerene-like isomer. These results, obtained at T = 0 K, indicate that disordered structures for the Au32- and Au32+ clusters may be detected not only at room temperature, as was experimentally verified for the Au32- one, but also at much lower temperatures.

Wavelet analysis of particle density functions in nucleus-nucleus interactions

NASA Astrophysics Data System (ADS)

Manna, S. K.; Haldar, P. K.; Mali, P.; Mukhopadhyay, A.; Singh, G.

A continuous wavelet analysis is performed for pattern recognition of the pseudorapidity density profile of singly charged particles produced in 16O+Ag/Br and 32S+Ag/Br interactions, each at an incident energy of 200 GeV per nucleon in the laboratory system. The experiments are compared with a model prediction based on the ultra-relativistic quantum molecular dynamics (UrQMD). To eliminate the contribution coming from known source(s) of particle cluster formation like Bose-Einstein correlation (BEC), the UrQMD output is modified by “an algorithm that mimics the BEC as an after burner.” We observe that for both interactions particle clusters are found at same pseudorapidity locations at all scales. However, the cluster locations in the 16O+Ag/Br interaction are different from those found in the 32S+Ag/Br interaction. Significant differences between experiments and simulations are revealed in the wavelet pseudorapidity spectra that can be interpreted as the preferred pseudorapidity values and/or scales of the pseudorapidity interval at which clusters of particles are formed. The observed discrepancy between experiment and corresponding simulation should therefore be interpreted in terms of some kind of nontrivial dynamics of multiparticle production.

LoCuSS: connecting the dominance and shape of brightest cluster galaxies with the assembly history of massive clusters

NASA Astrophysics Data System (ADS)

Smith, Graham P.; Khosroshahi, Habib G.; Dariush, A.; Sanderson, A. J. R.; Ponman, T. J.; Stott, J. P.; Haines, C. P.; Egami, E.; Stark, D. P.

2010-11-01

We study the luminosity gap, Δm12, between the first- and second-ranked galaxies in a sample of 59 massive (~1015Msolar) galaxy clusters, using data from the Hale Telescope, the Hubble Space Telescope, Chandra and Spitzer. We find that the Δm12 distribution, p(Δm12), is a declining function of Δm12 to which we fitted a straight line: p(Δm12) ~ -(0.13 +/- 0.02)Δm12. The fraction of clusters with `large' luminosity gaps is p(Δm12 >= 1) = 0.37 +/- 0.08, which represents a 3σ excess over that obtained from Monte Carlo simulations of a Schechter function that matches the mean cluster galaxy luminosity function. We also identify four clusters with `extreme' luminosity gaps, Δm12 >= 2, giving a fraction of . More generally, large luminosity gap clusters are relatively homogeneous, with elliptical/discy brightest cluster galaxies (BCGs), cuspy gas density profiles (i.e. strong cool cores), high concentrations and low substructure fractions. In contrast, small luminosity gap clusters are heterogeneous, spanning the full range of boxy/elliptical/discy BCG morphologies, the full range of cool core strengths and dark matter concentrations, and have large substructure fractions. Taken together, these results imply that the amplitude of the luminosity gap is a function of both the formation epoch and the recent infall history of the cluster. `BCG dominance' is therefore a phase that a cluster may evolve through and is not an evolutionary `cul-de-sac'. We also compare our results with semi-analytic model predictions based on the Millennium Simulation. None of the models is able to reproduce all of the observational results on Δm12, underlining the inability of the current generation of models to match the empirical properties of BCGs. We identify the strength of active galactic nucleus feedback and the efficiency with which cluster galaxies are replenished after they merge with the BCG in each model as possible causes of these discrepancies.

Linear and quadratic static response functions and structure functions in Yukawa liquids.

PubMed

Magyar, Péter; Donkó, Zoltán; Kalman, Gabor J; Golden, Kenneth I

2014-08-01

We compute linear and quadratic static density response functions of three-dimensional Yukawa liquids by applying an external perturbation potential in molecular dynamics simulations. The response functions are also obtained from the equilibrium fluctuations (static structure factors) in the system via the fluctuation-dissipation theorems. The good agreement of the quadratic response functions, obtained in the two different ways, confirms the quadratic fluctuation-dissipation theorem. We also find that the three-point structure function may be factorizable into two-point structure functions, leading to a cluster representation of the equilibrium triplet correlation function.

Computational chemistry of modified [MFe3S4] and [M2Fe2S4] clusters: assessment of trends in electronic structure and properties.

PubMed

Jensen, Kasper P; Ooi, Bee-Lean; Christensen, Hans E M

2008-12-18

The aim of this work is to understand the molecular evolution of iron-sulfur clusters in terms of electronic structure and function. Metal-substituted models of biological [Fe(4)S(4)] clusters in oxidation states [M(x)Fe(4-x)S(4)](3+/2+/1+) have been studied by density functional theory (M = Cr, Mn, Fe, Co, Ni, Cu, Zn, and Pd, with x = 1 or 2). Most of these clusters have not been characterized before. For those that have been characterized experimentally, very good agreement is obtained, implying that also the predicted structures and properties of new clusters are accurate. Mean absolute errors are 0.024 A for bond lengths ([Fe(4)S(4)], [NiFe(3)S(4)], [CoFe(3)S(4)]) and 0.09 V for shifts in reduction potentials relative to the [Fe(4)S(4)] cluster. All structures form cuboidal geometries similar to the all-iron clusters, except the Pd-substituted clusters, which instead form highly distorted trigonal and tetragonal local sites in compromised, pseudocuboidal geometries. In contrast to other electron-transfer sites, cytochromes, blue copper proteins, and smaller iron-sulfur clusters, we find that the [Fe(4)S(4)] clusters are very insensitive to metal substitution, displaying quite small changes in reorganization energies and reduction potentials upon substitution. Thus, the [Fe(4)S(4)] clusters have an evolutionary advantage in being robust to pollution from other metals, still retaining function. We analyze in detail the electronic structure of individual clusters and rationalize spin couplings and redox activity. Often, several configurations are very close in energy, implying possible use as spin-crossover systems, and spin states are predicted accurately in all but one case ([CuFe(3)S(4)]). The results are anticipated to be helpful in defining new molecular systems with catalytic and magnetic properties.

Cosmological Constraints from Galaxy Clustering and the Mass-to-number Ratio of Galaxy Clusters

NASA Astrophysics Data System (ADS)

Tinker, Jeremy L.; Sheldon, Erin S.; Wechsler, Risa H.; Becker, Matthew R.; Rozo, Eduardo; Zu, Ying; Weinberg, David H.; Zehavi, Idit; Blanton, Michael R.; Busha, Michael T.; Koester, Benjamin P.

2012-01-01

We place constraints on the average density (Ω m ) and clustering amplitude (σ8) of matter using a combination of two measurements from the Sloan Digital Sky Survey: the galaxy two-point correlation function, wp (rp ), and the mass-to-galaxy-number ratio within galaxy clusters, M/N, analogous to cluster M/L ratios. Our wp (rp ) measurements are obtained from DR7 while the sample of clusters is the maxBCG sample, with cluster masses derived from weak gravitational lensing. We construct nonlinear galaxy bias models using the Halo Occupation Distribution (HOD) to fit both wp (rp ) and M/N for different cosmological parameters. HOD models that match the same two-point clustering predict different numbers of galaxies in massive halos when Ω m or σ8 is varied, thereby breaking the degeneracy between cosmology and bias. We demonstrate that this technique yields constraints that are consistent and competitive with current results from cluster abundance studies, without the use of abundance information. Using wp (rp ) and M/N alone, we find Ω0.5 m σ8 = 0.465 ± 0.026, with individual constraints of Ω m = 0.29 ± 0.03 and σ8 = 0.85 ± 0.06. Combined with current cosmic microwave background data, these constraints are Ω m = 0.290 ± 0.016 and σ8 = 0.826 ± 0.020. All errors are 1σ. The systematic uncertainties that the M/N technique are most sensitive to are the amplitude of the bias function of dark matter halos and the possibility of redshift evolution between the SDSS Main sample and the maxBCG cluster sample. Our derived constraints are insensitive to the current level of uncertainties in the halo mass function and in the mass-richness relation of clusters and its scatter, making the M/N technique complementary to cluster abundances as a method for constraining cosmology with future galaxy surveys.

Electronic structure investigation of neutral titanium oxide molecules TixOy

NASA Astrophysics Data System (ADS)

Jeong, K. S.; Chang, Ch; Sedlmayr, E.; Sülzle, D.

2000-09-01

Electronic and structural properties of energetically low-lying isomers of isolated TixOy (x = 1-6, y = 1-12) molecular systems have been investigated by density functional theoretical methods. A variety of stationary points are thoroughly characterized. We report total cluster energies, equilibrium geometries and harmonic vibrational wavenumbers.

Barrierless Reactions with Loose Transition States Govern the Yields and Lifetimes of Organic Nitrates Derived from Isoprene

EPA Science Inventory

The chemical reaction mechanism of NO addition to two β and δ isoprene hydroxy–peroxy radical isomers is examined in detail using density functional theory, coupled cluster methods, and the energy resolved master equation formalism to provide estimates of rate co...

Bug Distribution and Pattern Classification.

ERIC Educational Resources Information Center

Tatsuoka, Kikumi K.; Tatsuoka, Maurice M.

The study examines the rule space model, a probabilistic model capable of measuring cognitive skill acquisition and of diagnosing erroneous rules of operation in a procedural domain. The model involves two important components: (1) determination of a set of bug distributions (bug density functions representing clusters around the rules); and (2)…

DENSITY FUNCTIONAL THEORY (DFT) AND MICROCALORIMETRIC INVESTIGATIONS OF CO ADSORPTION ON PT CLUSTERS. (R825370C056)

EPA Science Inventory

The perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Concl...

DENSITY FUNCTIONAL THEORY (DFT) STUDIES OF C1 AND C2 HYDROCARBONS SPECIES ON PT CLUSTERS. (R825370C056)

EPA Science Inventory

The perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Concl...

Site specific interaction between ZnO nanoparticles and tyrosine: A density functional theory study

NASA Astrophysics Data System (ADS)

Singh, Satvinder; Singh, Janpreet; Singh, Baljinder; Singh, Gurinder; Kaura, Aman; Tripathi, S. K.

2018-05-01

First Principles Calculations have been performed on ZnO/Tyrosine atomic complex to study site specific interaction of Tyrosine and ZnO nanoparticles. Calculated results shows that -COOH group present in Tyrosine is energetically more favorable than -NH2 group. Interactions show ionic bonding between ZnO and Tyrosine. All the calculations have been performed under the Density Functional Theory (DFT) framework. Structural and electronic properties of (ZnO)3/Tyrosine complex have been studied. Gaussian basis set approach has been adopted for the calculations. A ring type most stable (ZnO)3 atomic cluster has been modeled, analyzed and used for the calculations.

Application of Density Functional Theory to Systems Containing Metal Atoms

NASA Technical Reports Server (NTRS)

Bauschlicher, Charles W., Jr.

2006-01-01

The accuracy of density functional theory (DFT) for problems involving metal atoms is considered. The DFT results are compared with experiment as well as results obtained using the coupled cluster approach. The comparisons include geometries, frequencies, and bond energies. The systems considered include MO2, M(OH)+n, MNO+, and MCO+2. The DFT works well for frequencies and geometries, even in case with symmetry breaking; however, some examples have been found where the symmetry breaking is quite severe and the DFT methods do not work well. The calculation of bond energies is more difficult and examples of successes as well as failures of DFT will be given.

Bonding reactivity descriptor from conceptual density functional theory and its applications to elucidate bonding formation

NASA Astrophysics Data System (ADS)

Zhou, Pan-Pan; Liu, Shubin; Ayers, Paul W.; Zhang, Rui-Qin

2017-10-01

Condensed-to-atom Fukui functions which reflect the atomic reactivity like the tendency susceptible to either nucleophilic or electrophilic attack demonstrate the bonding trend of an atom in a molecule. Accordingly, Fukui functions based concepts, that is, bonding reactivity descriptors which reveal the bonding properties of molecules in the reaction were put forward and then applied to pericyclic and cluster reactions to confirm their effectiveness and reliability. In terms of the results from the bonding descriptors, a covalent bond can readily be predicted between two atoms with large Fukui functions (i.e., one governs nucleophilic attack while the other one governs electrophilic attack, or both of them govern radical attacks) for pericyclic reactions. For SinOm clusters' reactions, the clusters with a low O atom ratio readily form a bond between two Si atoms with big values of their Fukui functions in which they respectively govern nucleophilic and electrophilic attacks or both govern radical attacks. Also, our results from bonding descriptors show that Si—Si bonds can be formed via the radical mechanism between two Si atoms, and formations of Si—O and O—O bonds are possible when the O content is high. These results conform with experimental findings and can help experimentalists design appropriate clusters to synthesize Si nanowires with high yields. The approach established in this work could be generalized and applied to study reactivity properties for other systems.

Continuum Level Density of a Coupled-Channel System in the Complex Scaling Method

NASA Astrophysics Data System (ADS)

Suzuki, R.; Kruppa, A. T.; Giraud, B. G.; Katō, K.

2008-06-01

We study the continuum level density (CLD) in the formalism of the complex scaling method (CSM) for coupled-channel systems. We apply the formalism to the ^{4}He = [^{3}H + p] + [^3{He} + n] coupled-channel cluster model where there are resonances at low energy. Numerical calculations of the CLD in the CSM with a finite number of L^{2} basis functions are consistent with the exact result calculated from the S-matrix by solving coupled-channel equations. We also study channel densities. In this framework, the extended completeness relation (ECR) plays an important role.

Halo correlations in nonlinear cosmic density fields

NASA Astrophysics Data System (ADS)

Bernardeau, F.; Schaeffer, R.

1999-09-01

The question we address in this paper is the determination of the correlation properties of the dark matter halos appearing in cosmic density fields once they underwent a strongly nonlinear evolution induced by gravitational dynamics. A series of previous works have given indications that kind of non-Gaussian features are induced by nonlinear evolution in term of the high-order correlation functions. Assuming such patterns for the matter field, i.e. that the high-order correlation functions behave as products of two-body correlation functions, we derive the correlation properties of the halos, that are assumed to represent the correlation properties of galaxies or clusters. The hierarchical pattern originally induced by gravity is shown to be conserved for the halos. The strength of their correlations at any order varies, however, but is found to depend only on their internal properties, namely on the parameter x~ m/r(3-gamma ) where m is the mass of the halo, r its size and gamma is the power law index of the two-body correlation function. This internal parameter is seen to be close to the depth of the internal potential well of virialized objects. We were able to derive the explicit form of the generating function of the moments of the halo counts probability distribution function. In particular we show explicitly that, generically, S_P(x)-> P(P-2) in the rare halo limit. Various illustrations of our general results are presented. As a function of the properties of the underlying matter field, we construct the count probabilities for halos and in particular discuss the halo void probability. We evaluate the dependence of the halo mass function on the environment: within clusters, hierarchical clustering implies the higher masses are favored. These properties solely arise from what is a natural bias (ie, naturally induced by gravity) between the observed objects and the unseen matter field, and how it manifests itself depending on which selection effects are imposed.

First-principles investigation of the dissociation and coupling of methane on small copper clusters: Interplay of collision dynamics and geometric and electronic effects

DOE Office of Scientific and Technical Information (OSTI.GOV)

Varghese, Jithin J.; Mushrif, Samir H., E-mail: shmushrif@ntu.edu.sg

Small metal clusters exhibit unique size and morphology dependent catalytic activity. The search for alternate minimum energy pathways and catalysts to transform methane to more useful chemicals and carbon nanomaterials led us to investigate collision induced dissociation of methane on small Cu clusters. We report here for the first time, the free energy barriers for the collision induced activation, dissociation, and coupling of methane on small Cu clusters (Cu{sub n} where n = 2–12) using ab initio molecular dynamics and metadynamics simulations. The collision induced activation of the stretching and bending vibrations of methane significantly reduces the free energy barriermore » for its dissociation. Increase in the cluster size reduces the barrier for dissociation of methane due to the corresponding increase in delocalisation of electron density within the cluster, as demonstrated using the electron localisation function topology analysis. This enables higher probability of favourable alignment of the C–H stretching vibration of methane towards regions of high electron density within the cluster and makes higher number of sites available for the chemisorption of CH{sub 3} and H upon dissociation. These characteristics contribute in lowering the barrier for dissociation of methane. Distortion and reorganisation of cluster geometry due to high temperature collision dynamics disturb electron delocalisation within them and increase the barrier for dissociation. Coupling reactions of CH{sub x} (x = 1–3) species and recombination of H with CH{sub x} have free energy barriers significantly lower than complete dehydrogenation of methane to carbon. Thus, competition favours the former reactions at high hydrogen saturation on the clusters.« less

Dark energy and key physical parameters of clusters of galaxies

NASA Astrophysics Data System (ADS)

Bisnovatyi-Kogan, G. S.; Chernin, A. D.

2012-04-01

We study physics of clusters of galaxies embedded in the cosmic dark energy background. Under the assumption that dark energy is described by the cosmological constant, we show that the dynamical effects of dark energy are strong in clusters like the Virgo cluster. Specifically, the key physical parameters of the dark mater halos in clusters are determined by dark energy: (1) the halo cut-off radius is practically, if not exactly, equal to the zero-gravity radius at which the dark matter gravity is balanced by the dark energy antigravity; (2) the halo averaged density is equal to two densities of dark energy; (3) the halo edge (cut-off) density is the dark energy density with a numerical factor of the unity order slightly depending on the halo profile. The cluster gravitational potential well in which the particles of the dark halo (as well as galaxies and intracluster plasma) move is strongly affected by dark energy: the maximum of the potential is located at the zero-gravity radius of the cluster.

Interaction of size-selected gold nanoclusters with dopamine

NASA Astrophysics Data System (ADS)

Montone, Georgia R.; Hermann, Eric; Kandalam, Anil K.

2016-12-01

We present density functional theory based results on the interaction of size-selected gold nanoclusters, Au10 and Au20, with dopamine molecule. The gold clusters interact strongly with the nitrogen site of dopamine, thereby forming stable gold-dopamine complexes. Our calculations further show that there is no site specificity on the planar Au10 cluster with all the edge gold atoms equally preferred. On the other hand, in the pyramidal Au20 cluster, the vertex metal atom is the most active site. As the size increased from Au10 to Au20, the interaction strength has shown a declining trend. The effect of aqueous environment on the interaction strengths were also studied by solvation model. It is found that the presence of solvent water stabilizes the interaction between the metal cluster and dopamine molecule, even though for Au10 cluster the energy ordering of the isomers changed from that of the gas-phase.

Automating the expert consensus paradigm for robust lung tissue classification

NASA Astrophysics Data System (ADS)

Rajagopalan, Srinivasan; Karwoski, Ronald A.; Raghunath, Sushravya; Bartholmai, Brian J.; Robb, Richard A.

2012-03-01

Clinicians confirm the efficacy of dynamic multidisciplinary interactions in diagnosing Lung disease/wellness from CT scans. However, routine clinical practice cannot readily accomodate such interactions. Current schemes for automating lung tissue classification are based on a single elusive disease differentiating metric; this undermines their reliability in routine diagnosis. We propose a computational workflow that uses a collection (#: 15) of probability density functions (pdf)-based similarity metrics to automatically cluster pattern-specific (#patterns: 5) volumes of interest (#VOI: 976) extracted from the lung CT scans of 14 patients. The resultant clusters are refined for intra-partition compactness and subsequently aggregated into a super cluster using a cluster ensemble technique. The super clusters were validated against the consensus agreement of four clinical experts. The aggregations correlated strongly with expert consensus. By effectively mimicking the expertise of physicians, the proposed workflow could make automation of lung tissue classification a clinical reality.

Influence of silver and copper doping on luminescent properties of zinc-phosphate glasses after x-ray irradiation

NASA Astrophysics Data System (ADS)

Murashov, Alexander A.; Sidorov, Alexander I.; Shakhverdov, Teimur A.; Stolyarchuk, Maxim V.

2017-11-01

It is shown, experimentally, that in silver- and copper-containing zinc-phosphate glasses, metal molecular clusters are formed during the glass synthesis. X-ray irradiation of these glasses led to the considerable increase of its luminescence in visible spectral range. This effect is caused by the transformation of the charged metal molecular clusters into the neutral state. Luminescence and excitation spectra of the glass, doped with silver and copper simultaneously, change significantly in comparison with the spectra of glasses doped with one metal. The reason for this can be the formation of hybrid AgnCum molecular clusters. The computer simulation of the structure and optical properties of such clusters by the time-dependent density functional theory method is presented. It is shown that the optimal luminescent material for photonics application, in comparison with other studied materials, is glass, containing hybrid molecular clusters.

Collaborative Simulation Grid: Multiscale Quantum-Mechanical/Classical Atomistic Simulations on Distributed PC Clusters in the US and Japan

NASA Technical Reports Server (NTRS)

Kikuchi, Hideaki; Kalia, Rajiv; Nakano, Aiichiro; Vashishta, Priya; Iyetomi, Hiroshi; Ogata, Shuji; Kouno, Takahisa; Shimojo, Fuyuki; Tsuruta, Kanji; Saini, Subhash;

Infrared spectroscopic probing of dimethylamine clusters in an Ar matrix.

PubMed

Li, Siyang; Kjaergaard, Henrik G; Du, Lin

2016-02-01

Amines have many atmospheric sources and their clusters play an important role in aerosol nucleation processes. Clusters of a typical amine, dimethylamine (DMA), of different sizes were measured with matrix isolation IR (infrared) and NIR (near infrared) spectroscopy. The NIR vibrations are more separated and therefore it is easier to distinguish different sizes of clusters in this region. The DMA clusters, up to DMA tetramer, have been optimized using density functional methods, and the geometries, binding energies and thermodynamic properties of DMA clusters were obtained. The computed frequencies and intensities of NH-stretching vibrations in the DMA clusters were used to interpret the experimental spectra. We have identified the fundamental transitions of the bonded NH-stretching vibration and the first overtone transitions of the bonded and free NH-stretching vibration in the DMA clusters. Based on the changes in vibrational intensities during the annealing processes, the growth of clusters was clearly observed. The results of annealing processes indicate that DMA molecules tend to form larger clusters with lower energies under matrix temperatures, which is also supported by the calculated reaction energies of cluster formation. Copyright © 2015. Published by Elsevier B.V.

Distribution of neurons in functional areas of the mouse cerebral cortex reveals quantitatively different cortical zones

PubMed Central

Herculano-Houzel, Suzana; Watson, Charles; Paxinos, George

2013-01-01

How are neurons distributed along the cortical surface and across functional areas? Here we use the isotropic fractionator (Herculano-Houzel and Lent, 2005) to analyze the distribution of neurons across the entire isocortex of the mouse, divided into 18 functional areas defined anatomically. We find that the number of neurons underneath a surface area (the N/A ratio) varies 4.5-fold across functional areas and neuronal density varies 3.2-fold. The face area of S1 contains the most neurons, followed by motor cortex and the primary visual cortex. Remarkably, while the distribution of neurons across functional areas does not accompany the distribution of surface area, it mirrors closely the distribution of cortical volumes—with the exception of the visual areas, which hold more neurons than expected for their volume. Across the non-visual cortex, the volume of individual functional areas is a shared linear function of their number of neurons, while in the visual areas, neuronal densities are much higher than in all other areas. In contrast, the 18 functional areas cluster into three different zones according to the relationship between the N/A ratio and cortical thickness and neuronal density: these three clusters can be called visual, sensory, and, possibly, associative. These findings are remarkably similar to those in the human cerebral cortex (Ribeiro et al., 2013) and suggest that, like the human cerebral cortex, the mouse cerebral cortex comprises two zones that differ in how neurons form the cortical volume, and three zones that differ in how neurons are distributed underneath the cortical surface, possibly in relation to local differences in connectivity through the white matter. Our results suggest that beyond the developmental divide into visual and non-visual cortex, functional areas initially share a common distribution of neurons along the parenchyma that become delimited into functional areas according to the pattern of connectivity established later. PMID:24155697

On the mass of dense star clusters in starburst galaxies from spectrophotometry

NASA Astrophysics Data System (ADS)

Fleck, J.-J.; Boily, C. M.; Lançon, A.; Deiters, S.

2006-07-01

The mass of unresolved young star clusters derived from spectrophotometric data may well be off by a factor of 2 or more once the migration of massive stars driven by mass segregation is accounted for. We quantify this effect for a large set of cluster parameters, including variations in the stellar initial mass function (IMF), the intrinsic cluster mass, and mean mass density. Gas-dynamical models coupled with the Cambridge stellar evolution tracks allow us to derive a scheme to recover the real cluster mass given measured half-light radius, one-dimensional velocity dispersion and age. We monitor the evolution with time of the ratio of real to apparent mass through the parameter η. When we compute η for rich star clusters, we find non-monotonic evolution in time when the IMF stretches beyond a critical cut-off mass of 25.5Msolar. We also monitor the rise of colour gradients between the inner and outer volume of clusters: we find trends in time of the stellar IMF power indices overlapping well with those derived for the Large Magellanic Cloud cluster NGC 1818 at an age of 30Myr. We argue that the core region of massive Antennae clusters should have suffered from much segregation despite their low ages. We apply these results to a cluster mass function, and find that the peak of the mass distribution would appear to observers shifted to lower masses by as much as 0.2dex. The star formation rate derived for the cluster population is then underestimated by from 20 to 50 per cent.

Metalloid Aluminum Clusters with Fluorine

DTIC Science & Technology

2016-12-01

molecular dynamics, binding energy , siesta code, density of states, projected density of states 15. NUMBER OF PAGES 69 16. PRICE CODE 17. SECURITY...high energy density compared to explosives, but typically release this energy slowly via diffusion-limited combustion. There is recent interest in using...examine the cluster binding energy and electronic structure. Partial fluorine substitution in a prototypical aluminum-cyclopentadienyl cluster results

Rayleigh Scattering Density Measurements, Cluster Theory, and Nucleation Calculations at Mach 10

NASA Technical Reports Server (NTRS)

Balla, R. Jeffrey; Everhart, Joel L.

2012-01-01

In an exploratory investigation, quantitative unclustered laser Rayleigh scattering measurements of density were performed in the air in the NASA Langley Research Center's 31 in. Mach 10 wind tunnel. A review of 20 previous years of data in supersonic and Mach 6 hypersonic flows is presented where clustered signals typically overwhelmed molecular signals. A review of nucleation theory and accompanying nucleation calculations are also provided to interpret the current observed lack of clustering. Data were acquired at a fixed stagnation temperature near 990Kat five stagnation pressures spanning 2.41 to 10.0 MPa (350 to 1454 psi) using a pulsed argon fluoride excimer laser and double-intensified charge-coupled device camera. Data averaged over 371 images and 210 pixels along a 36.7mmline measured freestream densities that agree with computed isentropic-expansion densities to less than 2% and less than 6% at the highest and lowest densities, respectively. Cluster-free Mach 10 results are compared with previous clustered Mach 6 and condensation-free Mach 14 results. Evidence is presented indicating vibrationally excited oxygen and nitrogen molecules are absorbed as the clusters form, release their excess energy, and inhibit or possibly reverse the clustering process. Implications for delaying clustering and condensation onset in hypersonic and hypervelocity facilities are discussed.

Using Density Functional Theory (DFT) for the Calculation of Atomization Energies

NASA Technical Reports Server (NTRS)

Bauschlicher, Charles W., Jr.; Partridge, Harry; Langhoff, Stephen R. (Technical Monitor)

1995-01-01

The calculation of atomization energies using density functional theory (DFT), using the B3LYP hybrid functional, is reported. The sensitivity of the atomization energy to basis set is studied and compared with the coupled cluster singles and doubles approach with a perturbational estimate of the triples (CCSD(T)). Merging the B3LYP results with the G2(MP2) approach is also considered. It is found that replacing the geometry optimization and calculation of the zero-point energy by the analogous quantities computed using the B3LYP approach reduces the maximum error in the G2(MP2) approach. In addition to the 55 G2 atomization energies, some results for transition metal containing systems will also be presented.

Observational and Numerical Diagnostics of Galaxy Cluster Outer Regions

NASA Technical Reports Server (NTRS)

Eckert, D.; Vazza, F.; Ettori, S.; Molendi, S.; Nagai, D.; Lau, E.; Roncarelli, M.; Rossetti, M.; Snowden, S. L.; Gastaldello, F.

2011-01-01

Aims. We present the analysis of a local (z = 0.04 - 0.2) sample of 31 galaxy clusters with the aim of measuring the density of the X-ray emitting gas in cluster outskirts. We compare our results with numerical simulations to set constraints on the azimuthal symmetry and gas clumping in the outer regions of galaxy clusters. Methods. We exploit the large field-of-view and low instrumental background of ROSAT/PSPC to trace the density of the intracluster gas out to the virial radius. We perform a stacking of the density profiles to detect a signal beyond r(sub 200) and measure the typical density and scatter in cluster outskirts. We also compute the azimuthal scatter of the profiles with respect to the mean value to look for deviations from spherical symmetry. Finally, we compare our average density and scatter profiles with the results of numerical simulations. Results. As opposed to several recent results, we observe a steepening of the density profiles beyond approximately 0.3r(sub 500). Comparing our density profiles with simulations, we find that non-radiative runs predict too steep density profiles, whereas runs including additional physics and/or gas clumping are in better agreement with the observed gas distribution. We note a systematic difference between cool-core and non-cool core clusters beyond approximately 0.3r(sub 200), which we explain by a different distribution of the gas in the two classes. Beyond approximately r(sub 500), galaxy clusters deviate significantly from spherical symmetry, with only little differences between relaxed and disturbed systems. We find good agreement between the observed and predicted scatter profiles, but only when the 1% densest clumps are filtered out in the simulations. Conclusions. The general trend of steepening density around the virial radius indicates that the shallow density profiles found in several recent works were probably obtained along particular directions (e.g., filaments) and are not representative of the typical behavior of clusters. Comparing our results with numerical simulations, we find that non-radiative simulations fail to reproduce the gas distribution, even well outside cluster cores. Therefore, a detailed treatment of gas cooling, star formation, clumping, and AGN feedback is required to construct realistic models of cluster outer regions.

Density functional theory study on the structures, electronic and magnetic properties of the MFe3n‑1O4n (n = 1–3) (M=Mn, Co and Ni) clusters

NASA Astrophysics Data System (ADS)

Li, Zhi; Zhao, Zhen; Wang, Qi; Yin, Xi-tao

2018-04-01

The structures, electronic and magnetic properties of the MFe3n‑1O4n (n = 1–3) (M=Mn, Co and Ni) clusters are obtained by using the GGA-PBE functional. The results found that the CoFe3n‑1O4n (n = 1–3) clusters are more stable than the corresponding NiFe3n‑1O4n and MnFe3n‑1O4n clusters. The NiFe2O4, MnFe5O8 and CoFe5O8 clusters have higher kinetic stability than their neighbors. The average magnetic moments of MFe3n‑1O4n (n = 1–3) (M=Mn, Co and Ni) clusters are successively: NiFe3n‑1O4n > CoFe3n‑1O4n > MnFe3n‑1O4n. For NiFe3n‑1O4n and CoFe3n‑1O4n clusters, the average magnetic moments are decreased with the cluster size increasing while for MnFe3n‑1O4n, the opposite situation is occur. The difference of 3d orbital electrons of M (M=Mn, Co and Ni) atoms influence the magnetic properties of MFe3n‑1O4n clusters.

Ionization energies and electron affinities from a random-phase-approximation many-body Green's-function method including exchange interactions

NASA Astrophysics Data System (ADS)

Heßelmann, Andreas

2017-06-01

A many-body Green's-function method employing an infinite order summation of ring and exchange-ring contributions to the self-energy is presented. The individual correlation and relaxation contributions to the quasiparticle energies are calculated using an iterative scheme which utilizes density fitting of the particle-hole, particle-particle and hole-hole densities. It is shown that the ionization energies and electron affinities of this approach agree better with highly accurate coupled-cluster singles and doubles with perturbative triples energy difference results than those obtained with second-order Green's-function approaches. An analysis of the correlation and relaxation terms of the self-energy for the direct- and exchange-random-phase-approximation (RPA) Green's-function methods shows that the inclusion of exchange interactions leads to a reduction of the two contributions in magnitude. These differences, however, strongly cancel each other when summing the individual terms to the quasiparticle energies. Due to this, the direct- and exchange-RPA methods perform similarly for the description of ionization energies (IPs) and electron affinities (EAs). The coupled-cluster reference IPs and EAs, if corrected to the adiabatic energy differences between the neutral and charged molecules, were shown to be in very good agreement with experimental measurements.

DOE Office of Scientific and Technical Information (OSTI.GOV)

San Fabián, J.; Omar, S.; García de la Vega, J. M., E-mail: garcia.delavega@uam.es

The effect of a fraction of Hartree-Fock exchange on the calculated spin-spin coupling constants involving fluorine through a hydrogen bond is analyzed in detail. Coupling constants calculated using wavefunction methods are revisited in order to get high-level calculations using the same basis set. Accurate MCSCF results are obtained using an additive approach. These constants and their contributions are used as a reference for density functional calculations. Within the density functional theory, the Hartree-Fock exchange functional is split in short- and long-range using a modified version of the Coulomb-attenuating method with the SLYP functional as well as with the original B3LYP.more » Results support the difficulties for calculating hydrogen bond coupling constants using density functional methods when fluorine nuclei are involved. Coupling constants are very sensitive to the Hartree-Fock exchange and it seems that, contrary to other properties, it is important to include this exchange for short-range interactions. Best functionals are tested in two different groups of complexes: those related with anionic clusters of type [F(HF){sub n}]{sup −} and those formed by difluoroacetylene and either one or two hydrogen fluoride molecules.« less

Density functional theory and chromium: Insights from the dimers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Würdemann, Rolf; Kristoffersen, Henrik H.; Moseler, Michael

2015-03-28

The binding in small Cr clusters is re-investigated, where the correct description of the dimer in three charge states is used as criterion to assign the most suitable density functional theory approximation. The difficulty in chromium arises from the subtle interplay between energy gain from hybridization and energetic cost due to exchange between s and d based molecular orbitals. Variations in published bond lengths and binding energies are shown to arise from insufficient numerical representation of electron density and Kohn-Sham wave-functions. The best functional performance is found for gradient corrected (GGA) functionals and meta-GGAs, where we find severe differences betweenmore » functionals from the same family due to the importance of exchange. Only the “best fit” from Bayesian error estimation is able to predict the correct energetics for all three charge states unambiguously. With this knowledge, we predict small bond-lengths to be exclusively present in Cr{sub 2} and Cr{sub 2}{sup −}. Already for the dimer cation, solely long bond-lengths appear, similar to what is found in the trimer and in chromium bulk.« less

Density functional Theory Based Generalized Effective Fragment Potential Method (Postprint)

DTIC Science & Technology

2014-07-01

is acceptable for other applications) leads to induced dipole moments within 10−6 to 10−7 au of the precise values . Thus, the applied field of 10−4...noncovalent interactions. The water-benzene clusters17 and WATER2711 reference values were also ob- tained at the CCSD(T)/CBS level, except for the clusters...with n = 20,42 where MP2/CBS was used. The n-alkane dimers18 benchmark values were CCSD(T)/CBS for ethane to butane and a linear extrapolation method

Lowest-energy cage structures of medium-sized ( ZnO )n clusters with n = 15 - 24

NASA Astrophysics Data System (ADS)

Tang, Lingli; Sai, Linwei; Zhao, Jijun; Qiu, Ruifeng

2015-01-01

Fullerene-like cage structures of medium-sized ( ZnO )n clusters with n = 15 - 24 were generated by spiral algorithm and optimized using density functional theory calculations. Most of these lowest-energy cage structures contain only four-membered and six-membered rings, whereas eight-membered rings were found in the lowest-energy cages of ( ZnO )n (n = 19, 20, 23, 24). Our best cage configurations either reproduce or prevail the previously reported ones. The size-dependent electronic properties were also discussed.

Lowest-energy cage structures of medium-sized (ZnO){sub n} clusters with n = 15 − 24

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tang, Lingli; Sai, Linwei; Zhao, Jijun, E-mail: zhaojj@dlut.edu.cn

2015-01-22

Fullerene-like cage structures of medium-sized (ZnO){sub n} clusters with n = 15 − 24 were generated by spiral algorithm and optimized using density functional theory calculations. Most of these lowest-energy cage structures contain only four-membered and six-membered rings, whereas eight-membered rings were found in the lowest-energy cages of (ZnO){sub n} (n = 19, 20, 23, 24). Our best cage configurations either reproduce or prevail the previously reported ones. The size-dependent electronic properties were also discussed.

LoCuSS: The infall of X-ray groups onto massive clusters

NASA Astrophysics Data System (ADS)

Haines, C. P.; Finoguenov, A.; Smith, G. P.; Babul, A.; Egami, E.; Mazzotta, P.; Okabe, N.; Pereira, M. J.; Bianconi, M.; McGee, S. L.; Ziparo, F.; Campusano, L. E.; Loyola, C.

2018-03-01

Galaxy clusters are expected to form hierarchically in a ΛCDM universe, growing primarily through mergers with lower mass clusters and the continual accretion of group-mass halos. Galaxy clusters assemble late, doubling their masses since z ˜ 0.5, and so the outer regions of clusters should be replete with accreting group-mass systems. We present an XMM-Newton survey to search for X-ray groups in the infall regions of 23 massive galaxy clusters ( ˜ 1015 M⊙) at z ˜ 0.2, identifying 39 X-ray groups that have been spectroscopically confirmed to lie at the cluster redshift. These groups have mass estimates in the range 2 × 1013 - 7 × 1014 M⊙, and group-to-cluster mass ratios as low as 0.02. The comoving number density of X-ray groups in the infall regions is ˜25 × higher than that seen for isolated X-ray groups from the XXL survey. The average mass per cluster contained within these X-ray groups is 2.2 × 1014 M⊙, or 19 ± 5% of the mass within the primary cluster itself. We estimate that ˜1015 M⊙ clusters increase their masses by 16 ± 4% between z = 0.223 and the present day due to the accretion of groups with M200 ≥ 1013.2 M⊙. This represents about half of the expected mass growth rate of clusters at these late epochs. The other half is likely to come from smooth accretion of matter not bound within halos. The mass function of the infalling X-ray groups appears significantly top heavy with respect to that of "field" X-ray systems, consistent with expectations from numerical simulations, and the basic consequences of collapsed massive dark matter halos being biased tracers of the underlying large-scale density distribution.

The rise and fall of star formation in z ~ 0.2 merging galaxy clusters

DOE PAGES

Stroe, Andra; Sobral, David; Dawson, William; ...

2015-04-20

CIZA J2242.8+5301 (‘Sausage’) and 1RXS J0603.3+4213 (‘Toothbrush’) are two low-redshift (z ~ 0.2), massive (~2 × 10 15 M ⊙), post-core passage merging clusters, which host-shock waves traced by diffuse radio emission. To study their star formation properties, we uniformly survey the ‘Sausage’ and ‘Toothbrush’ clusters in broad- and narrow-band filters and select a sample of 201 and 463 line emitters, down to a rest-frame equivalent width (13 Å). Here, we robustly separate between Hα and higher redshift emitters using a combination of optical multiband (B, g, V, r, i, z) and spectroscopic data. We build Hα luminosity functions formore » the entire cluster region, near the shock fronts, and away from the shock fronts and find striking differences between the two clusters. In the dynamically younger, 1 Gyr old ‘Sausage’ cluster we find numerous (59) Hα emitters above a star formation rate (SFR) of 0.17 M ⊙ yr -1 surprisingly located in close proximity to the shock fronts, embedded in very hot intracluster medium plasma. The SFR density for the cluster population is at least at the level of typical galaxies at z ~ 2. Down to the same SFR, the possibly dynamically more evolved ‘Toothbrush’ cluster has only nine Hα galaxies. The cluster Hα galaxies fall on the SFR–stellar mass relation z ~ 0.2 for the field. However, the ‘Sausage’ cluster has an Hα emitter density >20 times that of blank fields. If the shock passes through gas-rich cluster galaxies, the compressed gas could collapse into dense clouds and excite star formation for a few 100 Myr. Finally, this process ultimately leads to a rapid consumption of the molecular gas, accelerating the transformation of gas-rich field spirals into cluster S0s or ellipticals.« less

LoCuSS: The infall of X-ray groups on to massive clusters

NASA Astrophysics Data System (ADS)

Haines, C. P.; Finoguenov, A.; Smith, G. P.; Babul, A.; Egami, E.; Mazzotta, P.; Okabe, N.; Pereira, M. J.; Bianconi, M.; McGee, S. L.; Ziparo, F.; Campusano, L. E.; Loyola, C.

2018-07-01

Galaxy clusters are expected to form hierarchically in a Λ cold dark matter (ΛCDM) universe, growing primarily through mergers with lower mass clusters and the continual accretion of group-mass haloes. Galaxy clusters assemble late, doubling their masses since z ˜ 0.5, and so the outer regions of clusters should be replete with accreting group-mass systems. We present an XMM-Newton survey to search for X-ray groups in the infall regions of 23 massive galaxy clusters ( ˜ 1015 M⊙) at z ˜ 0.2, identifying 39 X-ray groups that have been spectroscopically confirmed to lie at the cluster redshift. These groups have mass estimates in the range 2 × 1013-7 × 1014 M⊙, and group-to-cluster mass ratios as low as 0.02. The comoving number density of X-ray groups in the infall regions is ˜25× higher than that seen for isolated X-ray groups from the XXL survey. The average mass per cluster contained within these X-ray groups is 2.2 × 1014 M⊙, or 19 ± 5 per cent of the mass within the primary cluster itself. We estimate that ˜1015 M⊙ clusters increase their masses by 16 ± 4 per cent between z = 0.223 and the present day due to the accretion of groups with M200 ≥ 1013.2 M⊙. This represents about half of the expected mass growth rate of clusters at these late epochs. The other half is likely to come from smooth accretion of matter not bound within haloes. The mass function of the infalling X-ray groups appears significantly top heavy with respect to that of `field' X-ray systems, consistent with expectations from numerical simulations, and the basic consequences of collapsed massive dark matter haloes being biased tracers of the underlying large-scale density distribution.

Composite polarizability and the construction of an invariant function of refraction and mass density for solutions.

PubMed

Szymański, Krzysztof; Petrache, Horia I

2011-04-14

Re-examination of dynamical ionic polarizabilities in water solutions leads to the formulation of a solution function r(c), which combines the indices of refraction and mass densities of solutions. We show that this function should be independent of ionic concentration if the composite polarizabilities of hydrated solute clusters are constant. Using existing experimental data for a number of aqueous salt and organic solutions, we find that the r(c) function is either constant or varies linearly with concentration, in most cases with negligible slope. We use this function to compare ionic polarizabilities of crystals and aqueous solutions and to highlight how solute polarizabilities at infinite dilution scale with the electronic valence shell of cations and anions. The proposed r(c) function can be used generally to verify the consistency of experimental measurements and of simulation results, and it provides a test of assumptions in current theories of ionic polarizabilities.

Sub-saturation matter in compact stars: Nuclear modelling in the framework of the extended Thomas-Fermi theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aymard, François; Gulminelli, Francesca; Margueron, Jérôme

A recently introduced analytical model for the nuclear density profile [1] is implemented in the Extended Thomas-Fermi (ETF) energy density functional. This allows to (i) shed a new light on the issue of the sign of surface symmetry energy in nuclear mass formulas, as well as to (ii) show the importance of the in-medium corrections to the nuclear cluster energies in thermodynamic conditions relevant for the description of core-collapse supernovae and (proto)-neutron star crust.

Sub-saturation matter in compact stars: Nuclear modelling in the framework of the extended Thomas-Fermi theory

NASA Astrophysics Data System (ADS)

Aymard, François; Gulminelli, Francesca; Margueron, Jérôme

2015-02-01

A recently introduced analytical model for the nuclear density profile [1] is implemented in the Extended Thomas-Fermi (ETF) energy density functional. This allows to (i) shed a new light on the issue of the sign of surface symmetry energy in nuclear mass formulas, as well as to (ii) show the importance of the in-medium corrections to the nuclear cluster energies in thermodynamic conditions relevant for the description of core-collapse supernovae and (proto)-neutron star crust.

OSO-8 X-ray spectra of clusters of galaxies. 1. Observations of twenty clusters: Physical correlations

NASA Technical Reports Server (NTRS)

Mushotzky, R. F.; Serlemitsos, P. J.; Smith, B. W.; Boldt, E. A.; Holt, S. S.

1978-01-01

OSO-8 X-ray spectra from 2 to 20 keV were analyzed for 26 clusters of galaxies. Temperature, emission integrals, iron abundances, and low energy absorption measurements are given. Eight clusters have positive iron emission line detections at the 90% confidence level, and all twenty cluster spectra are consistent with Fe/H=0.000014 by number with the possible exception of Virgo. Physical correlations between X-ray spectral parameters and other cluster properties are examined. It is found that: (1) the X-ray temperature is approximately proportional to the square of the velocity dispersion of the galaxies; (2) the emission integral and therefore the bolometric X-ray luminosity is a strong function of the X-ray temperature; (3) the X-ray temperature and emission integral are better correlated with cluster central galaxy density than with richness; (4) temperature and emission integral are separately correlated with Rood-Sastry type; and (5) the fraction of galaxies which are spirals is correlated with the observed ram pressure in the cluster core.

Quantum-chemical study of the effect of ligands on the structure and properties of gold clusters

NASA Astrophysics Data System (ADS)

Golosnaya, M. N.; Pichugina, D. A.; Oleinichenko, A. V.; Kuz'menko, N. E.

2017-02-01

The structures of [Au4(dpmp)2X2]2+clusters, where X =-C≡CH,-CH3,-SCH3,-F,-Cl,-Br,-I, dpmp is bis((diphenylphosphino)methyl)(phenyl)phosphine, are calculated at the level of density functional theory with the PBE functional and a modified Dirac-Coulomb-Breit Hamiltonian in an all-electron basis set (Λ). Using the example of [Au4(dpmp)2(C≡CC6H5)2]2+, the interatomic distances and bond angles calculated by means of PBE0/LANL2DZ, TPSS/LANL2DZ, TPSSh/LANL2DZ, and PBE/Λ are compared to X-ray crystallography data. It is shown that PBE/Λ yields the most accurate calculation of the geometrical parameters of this cluster. The ligand effect on the electronic stability of a cluster and the stability in reactions of decomposition into different fragments is studied, along with the capability of ligand exchange. Stability is predicted for [Au4(dpmp)2F2]2+ and [Au4(dpmp)2(SCH3)2]2+, while [Au4(dpmp)2I2]2+ cluster is unstable and its decomposes into two identical fragments is supposed.

m-BIRCH: an online clustering approach for computer vision applications

NASA Astrophysics Data System (ADS)

Madan, Siddharth K.; Dana, Kristin J.

2015-03-01

We adapt a classic online clustering algorithm called Balanced Iterative Reducing and Clustering using Hierarchies (BIRCH), to incrementally cluster large datasets of features commonly used in multimedia and computer vision. We call the adapted version modified-BIRCH (m-BIRCH). The algorithm uses only a fraction of the dataset memory to perform clustering, and updates the clustering decisions when new data comes in. Modifications made in m-BIRCH enable data driven parameter selection and effectively handle varying density regions in the feature space. Data driven parameter selection automatically controls the level of coarseness of the data summarization. Effective handling of varying density regions is necessary to well represent the different density regions in data summarization. We use m-BIRCH to cluster 840K color SIFT descriptors, and 60K outlier corrupted grayscale patches. We use the algorithm to cluster datasets consisting of challenging non-convex clustering patterns. Our implementation of the algorithm provides an useful clustering tool and is made publicly available.

Evolution of the Blue and Far-Infrared Galaxy Luminosity Functions

NASA Technical Reports Server (NTRS)

Lonsdale, Carol J.; Chokshi, Arati

1993-01-01

The space density of blue-selected galaxies at moderate redshifts is determined here directly by deriving the luminosity function. Evidence is found for density evolution for moderate luminosity galaxies at a rate of (1+z) exp delta, with a best fit of delta + 4 +/- 2, between the current epoch and Z greater than about 0.1. At M(b) less than -22 evidence is found for about 0.5-1.5 mag of luminosity evolution in addition to the density evolution, corresponding to an evolutionary rate of about (1+z) exp gamma, with gamma = 0.5-2.5, but a redshift of about 0.4. Assuming a steeper faint end slope of alpha = -1.3 similar to that observed in the Virgo cluster, could explain the data with a luminosity evolution rate of gamma = 1-2, without need for any density evolution. Acceptable fits are found by comparing composite density and luminosity evolution models to faint IRAS 60 micron source counts, implying that the blue and far-IR evolutionary rates may be similar.

Theoretical studies on photoelectron and IR spectral properties of Br2.-(H2O)n clusters.

PubMed

Pathak, A K; Mukherjee, T; Maity, D K

2007-07-28

We report vertical detachment energy (VDE) and IR spectra of Br2.-.(H2O)n clusters (n=1-8) based on first principles electronic structure calculations. Cluster structures and IR spectra are calculated at Becke's half-and-half hybrid exchange-correlation functional (BHHLYP) with a triple split valence basis function, 6-311++G(d,p). VDE for the hydrated clusters is calculated based on second order Moller-Plesset perturbation (MP2) theory with the same set of basis function. On full geometry optimization, it is observed that conformers having interwater hydrogen bonding among solvent water molecules are more stable than the structures having double or single hydrogen bonded structures between the anionic solute, Br2.-, and solvent water molecules. Moreover, a conformer having cyclic interwater hydrogen bonded network is predicted to be more stable for each size hydrated cluster. It is also noticed that up to four solvent H2O units can reside around the solute in a cyclic interwater hydrogen bonded network. The excess electron in these hydrated clusters is localized over the solute atoms. Weighted average VDE is calculated for each size (n) cluster based on statistical population of the conformers at 150 K. A linear relationship is obtained for VDE versus (n+3)(-1/3) and bulk VDE of Br2.- aqueous solution is calculated as 10.01 eV at MP2 level of theory. BHHLYP density functional is seen to make a systematic overestimation in VDE values by approximately 0.5 eV compared to MP2 data in all the hydrated clusters. It is observed that hydration increases VDE of bromine dimer anion system by approximately 6.4 eV. Calculated IR spectra show that the formation of Br2.--water clusters induces large shifts from the normal O-H stretching bands of isolated water keeping bending modes rather insensitive. Hydrated clusters, Br2.-.(H2O)n, show characteristic sharp features of O-H stretching bands of water in the small size clusters.

Theoretical studies on photoelectron and IR spectral properties of Br2.-(H2O)n clusters

NASA Astrophysics Data System (ADS)

Pathak, A. K.; Mukherjee, T.; Maity, D. K.

2007-07-01

We report vertical detachment energy (VDE) and IR spectra of Br2•-•(H2O)n clusters (n=1-8) based on first principles electronic structure calculations. Cluster structures and IR spectra are calculated at Becke's half-and-half hybrid exchange-correlation functional (BHHLYP) with a triple split valence basis function, 6-311++G(d,p). VDE for the hydrated clusters is calculated based on second order Moller-Plesset perturbation (MP2) theory with the same set of basis function. On full geometry optimization, it is observed that conformers having interwater hydrogen bonding among solvent water molecules are more stable than the structures having double or single hydrogen bonded structures between the anionic solute, Br2•-, and solvent water molecules. Moreover, a conformer having cyclic interwater hydrogen bonded network is predicted to be more stable for each size hydrated cluster. It is also noticed that up to four solvent H2O units can reside around the solute in a cyclic interwater hydrogen bonded network. The excess electron in these hydrated clusters is localized over the solute atoms. Weighted average VDE is calculated for each size (n) cluster based on statistical population of the conformers at 150K. A linear relationship is obtained for VDE versus (n+3)-1/3 and bulk VDE of Br2•- aqueous solution is calculated as 10.01eV at MP2 level of theory. BHHLYP density functional is seen to make a systematic overestimation in VDE values by ˜0.5eV compared to MP2 data in all the hydrated clusters. It is observed that hydration increases VDE of bromine dimer anion system by ˜6.4eV. Calculated IR spectra show that the formation of Br2•--water clusters induces large shifts from the normal O-H stretching bands of isolated water keeping bending modes rather insensitive. Hydrated clusters, Br2•-•(H2O)n, show characteristic sharp features of O-H stretching bands of water in the small size clusters.

EXPLORING THE VARIABLE SKY WITH LINEAR. II. HALO STRUCTURE AND SUBSTRUCTURE TRACED BY RR LYRAE STARS TO 30 kpc

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sesar, Branimir; Ivezic, Zeljko; Morgan, Dylan M.

We present a sample of {approx}5000 RR Lyrae stars selected from the recalibrated LINEAR data set and detected at heliocentric distances between 5 kpc and 30 kpc over {approx}8000 deg{sup 2} of sky. The coordinates and light curve properties, such as period and Oosterhoff type, are made publicly available. We analyze in detail the light curve properties and Galactic distribution of the subset of {approx}4000 type ab RR Lyrae (RRab) stars, including a search for new halo substructures and the number density distribution as a function of Oosterhoff type. We find evidence for the Oosterhoff dichotomy among field RR Lyraemore » stars, with the ratio of the type II and I subsamples of about 1:4, but with a weaker separation than for globular cluster stars. The wide sky coverage and depth of this sample allow unique constraints for the number density distribution of halo RRab stars as a function of galactocentric distance: it can be described as an oblate ellipsoid with an axis ratio q = 0.63 and with either a single or a double power law with a power-law index in the range -2 to -3. Consistent with previous studies, we find that the Oosterhoff type II subsample has a steeper number density profile than the Oosterhoff type I subsample. Using the group-finding algorithm EnLink, we detected seven candidate halo groups, only one of which is statistically spurious. Three of these groups are near globular clusters (M53/NGC 5053, M3, M13), and one is near a known halo substructure (Virgo Stellar Stream); the remaining three groups do not seem to be near any known halo substructures or globular clusters and seem to have a higher ratio of Oosterhoff type II to Oosterhoff type I RRab stars than what is found in the halo. The extended morphology and the position (outside the tidal radius) of some of the groups near globular clusters are suggestive of tidal streams possibly originating from globular clusters. Spectroscopic follow-up of detected halo groups is encouraged.« less

Exploring the Variable Sky with LINEAR. II. Halo Structure and Substructure Traced by RR Lyrae Stars to 30 kpc

NASA Astrophysics Data System (ADS)

Sesar, Branimir; Ivezić, Željko; Stuart, J. Scott; Morgan, Dylan M.; Becker, Andrew C.; Sharma, Sanjib; Palaversa, Lovro; Jurić, Mario; Wozniak, Przemyslaw; Oluseyi, Hakeem

2013-08-01

We present a sample of ~5000 RR Lyrae stars selected from the recalibrated LINEAR data set and detected at heliocentric distances between 5 kpc and 30 kpc over ~8000 deg2 of sky. The coordinates and light curve properties, such as period and Oosterhoff type, are made publicly available. We analyze in detail the light curve properties and Galactic distribution of the subset of ~4000 type ab RR Lyrae (RRab) stars, including a search for new halo substructures and the number density distribution as a function of Oosterhoff type. We find evidence for the Oosterhoff dichotomy among field RR Lyrae stars, with the ratio of the type II and I subsamples of about 1:4, but with a weaker separation than for globular cluster stars. The wide sky coverage and depth of this sample allow unique constraints for the number density distribution of halo RRab stars as a function of galactocentric distance: it can be described as an oblate ellipsoid with an axis ratio q = 0.63 and with either a single or a double power law with a power-law index in the range -2 to -3. Consistent with previous studies, we find that the Oosterhoff type II subsample has a steeper number density profile than the Oosterhoff type I subsample. Using the group-finding algorithm EnLink, we detected seven candidate halo groups, only one of which is statistically spurious. Three of these groups are near globular clusters (M53/NGC 5053, M3, M13), and one is near a known halo substructure (Virgo Stellar Stream); the remaining three groups do not seem to be near any known halo substructures or globular clusters and seem to have a higher ratio of Oosterhoff type II to Oosterhoff type I RRab stars than what is found in the halo. The extended morphology and the position (outside the tidal radius) of some of the groups near globular clusters are suggestive of tidal streams possibly originating from globular clusters. Spectroscopic follow-up of detected halo groups is encouraged.

Liquid Drop Model for Charged Spherical Metal Clusters

NASA Astrophysics Data System (ADS)

Seidl, M.; Brack, M.

1996-02-01

The average ground-state energy of a charged spherical metal cluster withNatoms andzexcessive valence electrons, i.e., with net chargeQ=-ezand radiusR=rsN1/3, is presented in the liquid drop model (LDM) expansionE(N, z)=avN+asN2/3+acN1/3+a0(z)+a-1(z) N-1/3+O(N-2/3). We derive analytical expressions for the leading LDM coefficientsav,as,ac, and, in particular, for the charge dependence of the further LDM coefficientsa0anda-1, using the jellium model and density functional theory in the local density approximation. We obtain for the ionization energyI(R)=W+α(e2/R)+O(R-2), with the bulk work functionW=[Φ(+∞)-Φ(0)]-eb, given first by Mahan and Schaich in terms of the electrostatic potentialΦand the bulk energy per electroneb, and a new analytical expression for the dimensionless coefficientα. We demonstrate that within classical theoryα={1}/{2} but, in agreement with experimental information,αtends to ∼0.4 if quantum-mechanical contributions are included. In order to test and confirm our analytical expressions, we discuss the numerical results of semiclassical density variational calculations in the extended Thomas-Fermi model.

B80 and B101-103 clusters: Remarkable stability of the core-shell structures established by validated density functionalsa)

NASA Astrophysics Data System (ADS)

Li, Fengyu; Jin, Peng; Jiang, De-en; Wang, Lu; Zhang, Shengbai B.; Zhao, Jijun; Chen, Zhongfang

2012-02-01

Prompted by the very recent claim that the volleyball-shaped B80 fullerene [X. Wang, Phys. Rev. B 82, 153409 (2010), 10.1103/PhysRevB.82.153409] is lower in energy than the B80 buckyball [N. G. Szwacki, A. Sadrzadeh, and B. I. Yakobson, Phys. Rev. Lett. 98, 166804 (2007), 10.1103/PhysRevLett.98.166804] and core-shell structure [J. Zhao, L. Wang, F. Li, and Z. Chen, J. Phys. Chem. A 114, 9969 (2010), 10.1021/jp1018873], and inspired by the most recent finding of another core-shell isomer as the lowest energy B80 isomer [S. De, A. Willand, M. Amsler, P. Pochet, L. Genovese, and S. Goedecher, Phys. Rev. Lett. 106, 225502 (2011), 10.1103/PhysRevLett.106.225502], we carefully evaluated the performance of the density functional methods in the energetics of boron clusters and confirmed that the core-shell construction (stuffed fullerene) is thermodynamically the most favorable structural pattern for B80. Our global minimum search showed that both B101 and B103 also prefer a core-shell structure and that B103 can reach the complete core-shell configuration. We called for great attention to the theoretical community when using density functionals to investigate boron-related nanomaterials.

Imaging the Ultrafast Photoelectron Transfer Process in Alizarin-TiO2.

PubMed

Gomez, Tatiana; Hermann, Gunter; Zarate, Ximena; Pérez-Torres, Jhon Fredy; Tremblay, Jean Christophe

2015-07-30

In this work, we adopt a quantum mechanical approach based on time-dependent density functional theory (TDDFT) to study the optical and electronic properties of alizarin supported on TiO2 nano-crystallites, as a prototypical dye-sensitized solar cell. To ensure proper alignment of the donor (alizarin) and acceptor (TiO2 nano-crystallite) levels, static optical excitation spectra are simulated using time-dependent density functional theory in response. The ultrafast photoelectron transfer from the dye to the cluster is simulated using an explicitly time-dependent, one-electron TDDFT ansatz. The model considers the δ-pulse excitation of a single active electron localized in the dye to the complete set of energetically accessible, delocalized molecular orbitals of the dye/nano-crystallite complex. A set of quantum mechanical tools derived from the transition electronic flux density is introduced to visualize and analyze the process in real time. The evolution of the created wave packet subject to absorbing boundary conditions at the borders of the cluster reveal that, while the electrons of the aromatic rings of alizarin are heavily involved in an ultrafast charge redistribution between the carbonyl groups of the dye molecule, they do not contribute positively to the electron injection and, overall, they delay the process.

Infrared spectroscopy of protonated trimethylamine-(benzene)(n) (n = 1-4) as model clusters of the quaternary ammonium-aromatic ring interaction.

PubMed

Shishido, Ryunosuke; Kawai, Yuki; Fujii, Asuka

2014-09-04

The essence of the molecular recognition of the neurotransmitter acetylcholine has been attributed to the attractive interaction between a quaternary ammonium and aromatic rings. We employed protonated trimethylamine-(benzene)n clusters (n = 1-4) in the gas phase as a model to study the recognition mechanism of acetylcholine at the microscopic level. We applied size-selective infrared spectroscopy to the clusters and observed the NH and CH stretching vibrational regions. We also performed density functional theory calculations of stable structures, charge distributions, and infrared spectra of the clusters. It was shown that the methyl groups of protonated trimethylamine are solvated by benzene one at a time in the n > 1 clusters, and the validity of these clusters as a model system of the acetylcholine recognition was demonstrated. The nature of the interactions between a quaternary ammonium and aromatic rings is discussed on the basis of the observed infrared spectra and the theoretical calculations.

Correlation Functions Quantify Super-Resolution Images and Estimate Apparent Clustering Due to Over-Counting

PubMed Central

Veatch, Sarah L.; Machta, Benjamin B.; Shelby, Sarah A.; Chiang, Ethan N.; Holowka, David A.; Baird, Barbara A.

2012-01-01

We present an analytical method using correlation functions to quantify clustering in super-resolution fluorescence localization images and electron microscopy images of static surfaces in two dimensions. We use this method to quantify how over-counting of labeled molecules contributes to apparent self-clustering and to calculate the effective lateral resolution of an image. This treatment applies to distributions of proteins and lipids in cell membranes, where there is significant interest in using electron microscopy and super-resolution fluorescence localization techniques to probe membrane heterogeneity. When images are quantified using pair auto-correlation functions, the magnitude of apparent clustering arising from over-counting varies inversely with the surface density of labeled molecules and does not depend on the number of times an average molecule is counted. In contrast, we demonstrate that over-counting does not give rise to apparent co-clustering in double label experiments when pair cross-correlation functions are measured. We apply our analytical method to quantify the distribution of the IgE receptor (FcεRI) on the plasma membranes of chemically fixed RBL-2H3 mast cells from images acquired using stochastic optical reconstruction microscopy (STORM/dSTORM) and scanning electron microscopy (SEM). We find that apparent clustering of FcεRI-bound IgE is dominated by over-counting labels on individual complexes when IgE is directly conjugated to organic fluorophores. We verify this observation by measuring pair cross-correlation functions between two distinguishably labeled pools of IgE-FcεRI on the cell surface using both imaging methods. After correcting for over-counting, we observe weak but significant self-clustering of IgE-FcεRI in fluorescence localization measurements, and no residual self-clustering as detected with SEM. We also apply this method to quantify IgE-FcεRI redistribution after deliberate clustering by crosslinking with two distinct trivalent ligands of defined architectures, and we evaluate contributions from both over-counting of labels and redistribution of proteins. PMID:22384026

MEASURING THE LUMINOSITY AND VIRIAL BLACK HOLE MASS DEPENDENCE OF QUASAR–GALAXY CLUSTERING AT z ∼ 0.8

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krolewski, Alex G.; Eisenstein, Daniel J., E-mail: akrolewski@college.harvard.edu

2015-04-10

We study the dependence of quasar clustering on quasar luminosity and black hole mass by measuring the angular overdensity of photometrically selected galaxies imaged by the Wide-field Infrared Survey Explorer (WISE) about z ∼ 0.8 quasars from SDSS. By measuring the quasar–galaxy cross-correlation function and using photometrically selected galaxies, we achieve a higher density of tracer objects and a more sensitive detection of clustering than measurements of the quasar autocorrelation function. We test models of quasar formation and evolution by measuring the luminosity dependence of clustering amplitude. We find a significant overdensity of WISE galaxies about z ∼ 0.8 quasarsmore » at 0.2–6.4 h{sup −1} Mpc in projected comoving separation. We find no appreciable increase in clustering amplitude with quasar luminosity across a decade in luminosity, and a power-law fit between luminosity and clustering amplitude gives an exponent of −0.01 ± 0.06 (1 σ error). We also fail to find a significant relationship between clustering amplitude and black hole mass, although our dynamic range in true mass is suppressed due to the large uncertainties in virial black hole mass estimates. Our results indicate that a small range in host dark matter halo mass maps to a large range in quasar luminosity.« less

Properties of iron sulfide, hydrosulfide, and mixed sulfide/hydrosulfide cluster anions through photoelectron spectroscopy and density functional theory calculations.

PubMed

Yin, Shi; Bernstein, Elliot R

2016-10-21

A new magnetic-bottle time-of-flight photoelectron spectroscopy (PES) apparatus is constructed in our laboratory. The PES spectra of iron sulfide, hydrosulfide, and mixed sulfide/hydrosulfide [FeS m (SH) n - ; m, n = 0-3, 0 < (m + n) ≤ 3] cluster anions, obtained at 2.331 eV (532 nm) and 3.492 eV (355 nm) photon energies, are reported. The electronic structure and bonding properties of these clusters are additionally investigated at different levels of density functional theory. The most probable structures and ground state spin multiplicity for these cluster anions are tentatively assigned by comparing their theoretical first vertical detachment energies (VDEs) with their respective experiment values. The behavior of S and (SH) as ligands in these iron sulfide, hydrosulfide, and mixed sulfide/hydrosulfide cluster anions is investigated and compared. The experimental first VDEs for Fe(SH) 1-3 - cluster anions are lower than those found for their respective FeS 1-3 - cluster anions. The experimental first VDEs for FeS 1-3 - clusters are observed to increase for the first two S atoms bound to Fe - ; however, due to the formation of an S-S bond for the FeS 3 - cluster, its first VDE is found to be ∼0.41 eV lower than the first VDE for the FeS 2 - cluster. The first VDEs of Fe(SH) 1-3 - cluster anions are observed to increase with the increasing numbers of SH groups. The calculated partial charges of the Fe atom for ground state FeS 1-3 - and Fe(SH) 1-3 - clusters are apparently related to and correlated with their determined first VDEs. The higher first VDE is correlated with a higher, more positive partial charge for the Fe atom of these cluster anions. Iron sulfide/hydrosulfide mixed cluster anions are also explored in this work: the first VDE for FeS(SH) - is lower than that for FeS 2 - , but higher than that for Fe(SH) 2 - ; the first VDEs for FeS 2 (SH) - and FeS(SH) 2 - are close to that for FeS 3 - , but higher than that for Fe(SH) 3 - . The first VDEs of general iron sulfide, hydrosulfide, and mixed sulfide/hydrosulfide clusters [FeS m (SH) n - ; m, n = 0-3, 0 < (m + n) ≤ 3] are dependent on three properties of these anions: 1. the partial charge on the Fe atom, 2. disulfide bond formation (S-S) in the cluster, and 3. the number of hydrosulfide ligands in the cluster. The higher the partial charge on the Fe atom of these clusters, the larger the first VDE; however, cluster S-S bonding and more (SH) ligands in the cluster lower the cluster anion first VDE.

Properties of iron sulfide, hydrosulfide, and mixed sulfide/hydrosulfide cluster anions through photoelectron spectroscopy and density functional theory calculations

NASA Astrophysics Data System (ADS)

Yin, Shi; Bernstein, Elliot R.

2016-10-01

A new magnetic-bottle time-of-flight photoelectron spectroscopy (PES) apparatus is constructed in our laboratory. The PES spectra of iron sulfide, hydrosulfide, and mixed sulfide/hydrosulfide [FeSm(SH)n-; m, n = 0-3, 0 < (m + n) ≤ 3] cluster anions, obtained at 2.331 eV (532 nm) and 3.492 eV (355 nm) photon energies, are reported. The electronic structure and bonding properties of these clusters are additionally investigated at different levels of density functional theory. The most probable structures and ground state spin multiplicity for these cluster anions are tentatively assigned by comparing their theoretical first vertical detachment energies (VDEs) with their respective experiment values. The behavior of S and (SH) as ligands in these iron sulfide, hydrosulfide, and mixed sulfide/hydrosulfide cluster anions is investigated and compared. The experimental first VDEs for Fe(SH)1-3- cluster anions are lower than those found for their respective FeS1-3- cluster anions. The experimental first VDEs for FeS1-3- clusters are observed to increase for the first two S atoms bound to Fe-; however, due to the formation of an S-S bond for the FeS3- cluster, its first VDE is found to be ˜0.41 eV lower than the first VDE for the FeS2- cluster. The first VDEs of Fe(SH)1-3- cluster anions are observed to increase with the increasing numbers of SH groups. The calculated partial charges of the Fe atom for ground state FeS1-3- and Fe(SH)1-3- clusters are apparently related to and correlated with their determined first VDEs. The higher first VDE is correlated with a higher, more positive partial charge for the Fe atom of these cluster anions. Iron sulfide/hydrosulfide mixed cluster anions are also explored in this work: the first VDE for FeS(SH)- is lower than that for FeS2-, but higher than that for Fe(SH)2-; the first VDEs for FeS2(SH)- and FeS(SH)2- are close to that for FeS3-, but higher than that for Fe(SH)3-. The first VDEs of general iron sulfide, hydrosulfide, and mixed sulfide/hydrosulfide clusters [FeSm(SH)n-; m, n = 0-3, 0 < (m + n) ≤ 3] are dependent on three properties of these anions: 1. the partial charge on the Fe atom, 2. disulfide bond formation (S-S) in the cluster, and 3. the number of hydrosulfide ligands in the cluster. The higher the partial charge on the Fe atom of these clusters, the larger the first VDE; however, cluster S-S bonding and more (SH) ligands in the cluster lower the cluster anion first VDE.

From the Superatom Model to a Diverse Array of Super-Elements: A Systematic Study of Dopant Influence on the Electronic Structure of Thiolate-Protected Gold Clusters.

PubMed

Schacht, Julia; Gaston, Nicola

2016-10-18

The electronic properties of doped thiolate-protected gold clusters are often referred to as tunable, but their study to date, conducted at different levels of theory, does not allow a systematic evaluation of this claim. Here, using density functional theory, the applicability of the superatomic model to these clusters is critically evaluated, and related to the degree of structural distortion and electronic inhomogeneity in the differently doped clusters, with dopant atoms Pd, Pt, Cu, and Ag. The effect of electron number is systematically evaluated by varying the charge on the overall cluster, and the nominal number of delocalized electrons, employed in the superatomic model, is compared to the numbers obtained from Bader analysis of individual atomic charges. We find that the superatomic model is highly applicable to all of these clusters, and is able to predict and explain the changing electronic structure as a function of charge. However, significant perturbations of the model arise due to doping, due to distortions of the core structure of the Au 13 [RS(AuSR) 2 ] 6 - cluster. In addition, analysis of the electronic structure indicates that the superatomic character is distributed further across the ligand shell in the case of the doped clusters, which may have implications for the self-assembly of these clusters into materials. The prediction of appropriate clusters for such superatomic solids relies critically on such quantitative analysis of the tunability of the electronic structure. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Do Ag{sub n} (up to n = 8) clusters retain their identity on graphite? Insights from first-principles calculations including dispersion interactions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Singh, Akansha; Sen, Prasenjit, E-mail: prasen@hri.res.in; Majumder, Chiranjib

Adsorption of pre-formed Ag{sub n} clusters for n = 1 − 8 on a graphite substrate is studied within the density functional theory employing the vdW-DF2 functional to treat dispersion interactions. Top sites above surface layer carbon atoms turn out to be most favorable for a Ag adatom, in agreement with experimental observations. The same feature is observed for clusters of almost all sizes which have the lowest energies when the Ag atoms are positioned over top sites. Most gas phase isomers retain their structures over the substrate, though a couple of them undergo significant distortions. Energetics of the adsorptionmore » can be understood in terms of a competition between energy cost of disturbing Ag–Ag bonds in the cluster and energy gain from Ag–C interactions at the surface. Ag{sub 3} turns out to be an exceptional candidate in this regard that undergoes significant structural distortion and has only two of the Ag atoms close to surface C atoms in its lowest energy structure.« less

Investigation of the 9B nucleus and its cluster-nucleon correlations

NASA Astrophysics Data System (ADS)

Zhao, Qing; Ren, Zhongzhou; Lyu, Mengjiao; Horiuchi, Hisashi; Funaki, Yasuro; Röpke, Gerd; Schuck, Peter; Tohsaki, Akihiro; Xu, Chang; Yamada, Taiichi; Zhou, Bo

2018-05-01

In order to study the correlations between clusters and nucleons in light nuclei, we formulate a new superposed Tohsaki-Horiuchi-Schuck-Röpke (THSR) wave function which describes both spatially large spreading and cluster-correlated dynamics of valence nucleons. Using this new THSR wave function, the binding energy of 9B is significantly improved in comparison with our previous studies. We calculate the excited states of 9B and obtain an energy spectrum of 9B which is consistent with the experimental results. This includes the prediction of the first 1 /2+ excited state of 9B which is not yet fixed experimentally. We study the proton dynamics in 9B and find that the cluster-proton correlation plays an essential role for the proton dynamics in the ground state of 9B. Furthermore, we discuss the density distribution of the valence proton with special attention to its tail structure. Finally, the resonance nature of excited states of 9B is illustrated comparing root-mean-square radii between the ground and excited states.

Cosmological constraints from galaxy clustering in the presence of massive neutrinos

NASA Astrophysics Data System (ADS)

Zennaro, M.; Bel, J.; Dossett, J.; Carbone, C.; Guzzo, L.

2018-06-01

The clustering ratio is defined as the ratio between the correlation function and the variance of the smoothed overdensity field. In Λ cold dark matter (ΛCDM) cosmologies without massive neutrinos, it has already been proven to be independent of bias and redshift space distortions on a range of linear scales. It therefore can provide us with a direct comparison of predictions (for matter in real space) against measurements (from galaxies in redshift space). In this paper we first extend the applicability of such properties to cosmologies that account for massive neutrinos, by performing tests against simulated data. We then investigate the constraining power of the clustering ratio on cosmological parameters such as the total neutrino mass and the equation of state of dark energy. We analyse the joint posterior distribution of the parameters that satisfy both measurements of the galaxy clustering ratio in the SDSS-DR12, and the angular power spectra of cosmic microwave background temperature and polarization anisotropies measured by the Planck satellite. We find the clustering ratio to be very sensitive to the CDM density parameter, but less sensitive to the total neutrino mass. We also forecast the constraining power the clustering ratio will achieve, predicting the amplitude of its errors with a Euclid-like galaxy survey. First we compute parameter forecasts using the Planck covariance matrix alone, then we add information from the clustering ratio. We find a significant improvement on the constraint of all considered parameters, and in particular an improvement of 40 per cent for the CDM density and 14 per cent for the total neutrino mass.