Cluster Nucleation and Growth from a Highly Supersaturated Adatom Phase: Silver on Magnetite
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catalysis (heterogeneous), hydrogen and fuel cells↗
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Cooperative Cluster Metalation and Ligand Migration in Zirconium Metal–Organic Frameworks
Abstract Cooperative cluster metalation and ligand migration were performed on a Zr‐MOF, leading to the isolation of unique bimetallic MOFs based on decanuclear Zr 6 M 4 (M=Ni, Co) clusters. The M 2+ reacts with the μ 3 ‐OH and terminal H 2 O ligands on an 8‐connected [Zr 6 O 4 (OH) 8 (H 2 O) 4 ] cluster to form a bimetallic [Zr 6 M 4 O 8 (OH) 8 (H 2 O) 8 ] cluster. Along with the metalation of Zr 6 cluster, ligand migration is observed in which a Zr–carboxylate bond dissociates to form a M–carboxylate bond. Single‐crystal to single‐crystal transformation is realized so that snapshots for cooperative cluster metalation and ligand migration processes are captured by successive single‐crystal X‐ray structures. In 3+ was metalated into the same Zr‐MOF which showed excellent catalytic activity in the acetaldehyde cyclotrimerization reaction. This work not only provides a powerful tool to functionalize Zr‐MOFs with other metals, but also structurally elucidates the formation mechanism of the resulting heterometallic MOFs.
Yuan, Shuai↗
Oxygen trapped by rare earth tetrahedral clusters in Nd{sub 4}FeOS{sub 6}: Crystal structure, electronic structure, and magnetic properties
Single crystals of Nd{sub 4}FeOS{sub 6} were grown from an Fe–S eutectic solution. Single crystal X-ray diffraction analysis revealed a Nd{sub 4}MnOSe{sub 6}-type structure (P6{sub 3}mc, a=9.2693(1) Å, c=6.6650(1)Å, V=495.94(1) Å{sup 3}, Z=2), featuring parallel chains of face-sharing [FeS{sub 6×1/2}]{sup 4−} trigonal antiprisms and interlinked [Nd{sub 4}OS{sub 3}]{sup 4+} cubane-like clusters. Oxygen atoms were found to be trapped by Nd{sub 4} clusters in the [Nd{sub 4}OS{sub 3}]{sup 4{sub +}} chains. Structural differences among Nd{sub 4}MnOSe{sub 6}-type Nd{sub 4}FeOS{sub 6} and the related La{sub 3}CuSiS{sub 7}− and Pr{sub 8}CoGa{sub 3}-type structures have been described. Magnetic susceptibility measurements on Nd{sub 4}FeOS{sub 6} suggested the dominance of antiferromagnetic interactions at low temperature, but no magnetic ordering down to 2 K was observed. Spin-polarized electronic structure calculations revealed magnetic frustration with dominant antiferromagnetic interactions. - Graphical abstract: Trapping of oxygen in Nd{sub 4} tetrahedral clusters results in the formation of the Nd{sub 4}MnOSe{sub 6}-type Nd{sub 4}FeOS{sub 6}, in contrast to the La{sub 3}CuSiS{sub 7}-type oxygen-free Nd{sub 4}FeS{sub 7} and related Pr{sub 8}CoGa{sub 3}-type structures. Complex magnetic frustration inhibits magnetic ordering at low temperature. - Highlights: • Single crystals of Nd{sub 4}FeOS{sub 6} were grown using self-flux method. • Oxygen was found trapped by Nd{sub 4} tetrahedral clusters. • Comparison with two closely related structural types were discussed. • Magnetic measurements revealed antiferromagnetic (AFM) interaction. • VASP calculations confirmed strong magnetic frustration in AFM model.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Do Practical Standard Coupled Cluster Calculations Agree Better than Kohn–Sham Calculations with Currently Available Functionals When Compared to the Best Available Experimental Data for Dissociation Energies of Bonds to 3d Transition Metals?
Coupled-cluster (CC) methods have been extensively used as the high-level approach in quantum electronic structure theory to predict various properties of molecules when experimental results are unavailable. It is often assumed that CC methods, if they include at least up to connected-triple-excitation quasiperturbative corrections to a full treatment of single and double excitations (in particular, CCSD(T)), and a very large basis set, are more accurate than Kohn–Sham (KS) density functional theory (DFT). In the present work, we tested and compared the performance of standard CC and KS methods on bond energy calculations of 20 3d transition metal-containing diatomic molecules against the most reliable experimental data available, as collected in a database called 3dMLBE20. It is found that, although the CCSD(T) and higher levels CC methods have mean unsigned deviations from experiment that are smaller than most exchange-correlation functionals for metal–ligand bond energies of transition metals, the improvement is less than one standard deviation of the mean unsigned deviation. Furthermore, on average, almost half of the 42 exchange-correlation functionals that we tested are closer to experiment than CCSD(T) with the same extended basis set for the same molecule. The results show that, when both relativistic and core–valence correlation effects are considered, even the very high-level (expensive) CC method with single, double, triple, and perturbative quadruple cluster operators, namely, CCSDT(2)Q, averaged over 20 bond energies, gives a mean unsigned deviation (MUD(20) = 4.7 kcal/mol when one correlates only valence, 3p, and 3s electrons of transition metals and only valence electrons of ligands, or 4.6 kcal/mol when one correlates all core electrons except for 1s shells of transition metals, S, and Cl); and that is similar to some good xc functionals (e.g., B97-1 (MUD(20) = 4.5 kcal/mol) and PW6B95 (MUD(20) = 4.9 kcal/mol)) when the same basis set is used. We found that, for both coupled cluster calculations and KS calculations, the T1 diagnostics correlate the errors better than either the M diagnostics or the B1 DFT-based diagnostics. The potential use of practical standard CC methods as a benchmark theory is further confounded by the finding that CC and DFT methods usually have different signs of the error. We conclude that the available experimental data do not provide a justification for using conventional single-reference CC theory calculations to validate or test xc functionals for systems involving 3d transition metals.
Environmental Molecular Sciences Laboratory↗
Clusters, molecular layers, and 3D crystals of water on Ni(111)
We examined the growth and stability of ice layers on Ni(111) up to ∼7 molecular layers (ML) thick using scanning tunneling microscopy. At low coverage, films were comprised of ∼1 nm wide two-dimensional (2D) clusters. Only above ∼0.5 ML did patches of continuous 2D layers emerge, coexisting with the clusters until the first ML was complete. The structure of the continuous layer is clearly different from that of the 2D clusters. Subsequently, a second molecular layer grew on top of the first. 3D crystallites started to form only after this 2nd ML was complete. 2D clusters re-appeared when thicker films were partially evaporated, implying that these clusters represent the equilibrium configuration at low coverage. Binding energies and image simulations computed with density functional theory suggest that the 2D clusters are partially dissociated and surrounded by H adatoms. The complete 2D layer contains only intact water molecules because of the lack of favorable binding sites for H atoms. We propose molecular structures for the 2D layer that are composed of the same pentagon-heptagon binding motif and water density observed on Pt(111). The similarity of the water structures on Pt and Ni suggests a general prescription for generating low-energy configurations on close-packed metal substrates.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Microhydrated aromatic cluster cations: Binding motifs of 4-aminobenzonitrile-(H{sub 2}O){sub n} cluster cations with n ≤ 4
Infrared photodissociation (IRPD) spectra of mass-selected 4-aminobenzonitrile-(water){sub n} cluster cations, ABN{sup +}-(H{sub 2}O){sub n} with n ≤ 4, recorded in the N–H and O–H stretch ranges are analyzed by quantum chemical calculations at the M06-2X/aug-cc-pVTZ level to determine the evolution of the initial microhydration process of this bifunctional aromatic cation in its ground electronic state. IRPD spectra of cold clusters tagged with Ar and N{sub 2} display higher resolution and allow for a clear-cut structural assignment. The clusters are generated in an electron impact source, which generates predominantly the most stable isomers. The IRPD spectra are assigned to single isomers for n = 1–3. The preferred cluster growth begins with sequential hydration of the two acidic NH protons of the amino group (n = 1–2), which is followed by attachment of secondary H{sub 2}O ligands hydrogen-bonded to the first-shell ligands (n = 3–4). These symmetric and branched structures are more stable than those with a cyclic H-bonded solvent network. Moreover, in the size range n ≤ 4 the formation of a solvent network stabilized by strong cooperative effects is favored over interior ion hydration which is destabilized by noncooperative effects. The potential of the ABN{sup +}-H{sub 2}O dimer is characterized in detail and supports the cluster growth derived from the IRPD spectra. Although the N–H bonds are destabilized by stepwise microhydration, which is accompanied by increasing charge transfer from ABN{sup +} to the solvent cluster, no proton transfer to the solvent is observed for n ≤ 4.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
A 3.55 keV line from DM →a→γ: predictions for cool-core and non-cool-core clusters
We further study a scenario in which a 3.55 keV X-ray line arises from decay of dark matter to an axion-like particle (ALP), that subsequently converts to a photon in astrophysical magnetic fields. We perform numerical simulations of Gaussian random magnetic fields with radial scaling of the magnetic field magnitude with the electron density, for both cool-core 'Perseus' and non-cool-core 'Coma' electron density profiles. Using these, we quantitatively study the resulting signal strength and morphology for cool-core and non-cool-core clusters. Our study includes the effects of fields of view that cover only the central part of the cluster, the effects of offset pointings on the radial decline of signal strength and the effects of dividing clusters into annuli. We find good agreement with current data and make predictions for future analyses and observations.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Galaxy clustering, photometric redshifts and diagnosis of systematics in the DES Science Verification data
Abstract Not Provided
Astrophysics,ASTRO↗
redMaPPer – III. A detailed comparison of the Planck 2013 and SDSS DR8 redMaPPer cluster catalogues
We compare the Planck Sunyaev–Zeldovich (SZ) cluster sample (PSZ1) to the Sloan Digital Sky Survey (SDSS) redMaPPer catalogue, finding that all Planck clusters within the redMaPPer mask and within the redshift range probed by redMaPPer are contained in the redMaPPer cluster catalogue. These common clusters define a tight scaling relation in the richness-SZ mass (λ–MSZ) plane, with an intrinsic scatter in richness of σλ|MSZ=0.266±0.017. The corresponding intrinsic scatter in true cluster halo mass at fixed richness is ≈21 percent. The regularity of this scaling relation is used to identify failures in both catalogues. The failure rates for redMaPPer and PSZ1 1.2 percent and 14.7 percent, respectively. The PSZ1 failure rates decreases to 9.8 percent after removing incorrect redshifts that were drawn from the literature. We note the failure rates in the PSZ1 from this analysis are specific to the SDSS overlap region, and may not be indicative of failure rates over the full Planck survey. We have further identified five PSZ1 sources that suffer from projection effects (multiple rich systems along the line of sight of the SZ detection) and 17 new high-redshift (z ≳ 0.6) cluster candidates of varying degrees of confidence.
Astrophysics,ASTRO↗
Dark Energy Survey Year 3 results: Cosmology from combined galaxy clustering and lensing validation on cosmological simulations
In this work, we present a validation of the Dark Energy Survey Year 3 (DES Y3) 3×2-point analysis choices by testing them on Buzzard2.0, a new suite of cosmological simulations that is tailored for the testing and validation of combined galaxy clustering and weak-lensing analyses. We show that the buzzard2.0 simulations accurately reproduce many important aspects of the DES Y3 data, including photometric redshift and magnitude distributions, and the relevant set of two-point clustering and weak-lensing statistics. We then show that our model for the 3×2-point data vector is accurate enough to recover the true cosmology in simulated surveys assuming the true redshift distributions for our source and lens samples, demonstrating robustness to uncertainties in the modeling of the nonlinear matter power spectrum, nonlinear galaxy bias, and higher-order lensing corrections. Additionally, we demonstrate for the first time that our photometric redshift calibration methodology, including information from photometry, spectroscopy, clustering cross-correlations, and galaxy–galaxy lensing ratios, is accurate enough to recover the true cosmology in simulated surveys in the presence of realistic photometric redshift uncertainties.
79 ASTRONOMY AND ASTROPHYSICS↗
Wigner SU(4) symmetry, clustering, and the spectrum of $$^{12}$$C
Abstract We present lattice calculations of the low-lying spectrum of $$^{12}$$ 12 C using a simple nucleon–nucleon interaction that is independent of spin and isospin and therefore invariant under Wigner’s SU(4) symmetry. We find strong signals for all excited states up to $$\sim 15$$ ∼ 15 MeV above the ground state, and explore the structure of each state using a large variety of $$\alpha $$ α cluster and harmonic oscillator trial states, projected onto given irreducible representations of the cubic group. We are able to verify earlier findings for the $$\alpha $$ α clustering in the Hoyle state and the second $$2^+$$ 2 + state of $$^{12}$$ 12 C. The success of these calculations to describe the full low-lying energy spectrum using spin-independent interactions suggest that either the spin-orbit interactions are somewhat weak in the $$^{12}$$ 12 C system, or the effects of $$\alpha $$ α clustering are diminishing their influence. This is in agreement with previous findings from ab initio shell model calculations.
Shen, Shihang (ORCID:0000000280516466)↗
Topological cell clustering in the ATLAS calorimeters and its performance in LHC Run 1
The reconstruction of the signal from hadrons and jets emerging from the proton–proton collisions at the Large Hadron Collider (LHC) and entering the ATLAS calorimeters is based on a three-dimensional topological clustering of individual calorimeter cell signals. The cluster formation follows cell signal-significance patterns generated by electromagnetic and hadronic showers. In this, the clustering algorithm implicitly performs a topological noise suppression by removing cells with insignificant signals which are not in close proximity to cells with significant signals. The resulting topological cell clusters have shape and location information, which is exploited to apply a local energy calibration and corrections depending on the nature of the cluster. Lastly, topological cell clustering is established as a well-performing calorimeter signal definition for jet and missing transverse momentum reconstruction in ATLAS.
43 PARTICLE ACCELERATORS↗
Two New Calcium-rich Gap Transients in Group and Cluster Environments
We present the Palomar Transient Factory discoveries and the photometric and spectroscopic observations of PTF11kmb and PTF12bho. We show that both transients have properties consistent with the class of calcium-rich gap transients, specifically lower peak luminosities and rapid evolution compared to ordinary supernovae, and a nebular spectrum dominated by [Ca ii] emission. A striking feature of both transients is their host environments: PTF12bho is an intracluster transient in the Coma Cluster, while PTF11kmb is located in a loose galaxy group, at a physical offset ∼150 kpc from the most likely host galaxy. Deep Subaru imaging of PTF12bho rules out an underlying host system to a limit of M{sub R}>−8.0 mag, while Hubble Space Telescope imaging of PTF11kmb reveals a marginal counterpart that, if real, could be either a background galaxy or a globular cluster. We show that the offset distribution of Ca-rich gap transients is significantly more extreme than that seen for SNe Ia or even short-hard gamma-ray bursts (sGRBs). Thus, if the offsets are caused by a kick, they require higher kick velocities and/or longer merger times than sGRBs. We also show that almost all Ca-rich transients found to date are in group and cluster environments with elliptical host galaxies, indicating a very old progenitor population; the remote locations could partially be explained by these environments having the largest fraction of stars in the intragroup/intracluster light following galaxy–galaxy interactions.
79 ASTRONOMY AND ASTROPHYSICS↗
The SPT-deep Cluster Catalog: Sunyaev–Zel’dovich Selected Clusters from Combined SPT-3G and SPTpol Measurements over 100 Square Degrees
We present a catalog of 500 galaxy cluster candidates in the SPT-Deep field: a 100 deg$^{2}$ field that combines data from the SPT-3G and SPTpol surveys to reach noise levels of 3.0, 2.2, and 9.0 μK-arcmin at 95, 150, and 220 GHz, respectively. Candidates are selected via the thermal Sunyaev–Zel’dovich (SZ) effect with a minimum significance of ξ = 4.0, resulting in a catalog of purity ∼89%. Optical data from the Dark Energy Survey and infrared data from the Spitzer Space Telescope are used to confirm 442 cluster candidates. The clusters span 0.12 < z ≲ 1.8 and 1.0 × 10$^{14}$M$_{⊙}$/h$_{70}$ < M$_{500c}$ < 8.7 × 10$^{14}$M$_{⊙}$/h$_{70}$. The sample’s median redshift is 0.74, and the median mass is 1.7 × 10$^{14}$M$_{⊙}$/h$_{70}$; these are the lowest median mass and highest median redshift of any SZ-selected sample to date. We assess the effect of infrared emission from cluster member galaxies on cluster selection by performing a joint fit to the infrared dust and tSZ signals by combining measurements from SPT and overlapping submillimeter data from Herschel/SPIRE. We find that at high redshift (z > 1), the tSZ signal is reduced by $17.9_{−3.2}^{+3.8}$%$(3.8_{−0.7}^{+0.9}$%$)$ at 150 GHz (95 GHz) due to dust contamination. We repeat our cluster finding method on dust-nulled SPT maps and find the resulting catalog is consistent with the nominal SPT-Deep catalog, suggesting dust contamination does not significantly impact the SPT-Deep selection function; we attribute this lack of bias to the inclusion of the SPT 220 GHz band.
79 ASTRONOMY AND ASTROPHYSICS↗
OSO-8 X-ray spectra of clusters of galaxies. 1. Observations of twenty clusters: Physical correlations
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.
Mushotzky, R. F.↗
A search for X-ray emission from rich clusters, extended halos around clusters, and superclusters
HEAO A-2 X-ray observations of rich clusters, extended halos around clusters, and superclusters are discussed. Concerning the optically richest clusters, results in the 0.2-60 keV energy range show that they appear to be relatively underluminous in X-rays. It is found that X-ray and microwave measurements for some rich clusters and for Abell 576 can be used to meaningfully constrain intracluster gas parameters and H(0); in addition, observations of Abell 576 show its luminosity to be less than earlier estimates. Extended halos around clusters were not detected in the data, and spectral observations of Abell 401 and 2147 reveal that they have typical cluster spectra with iron-line emission, while intensity measurements indicate that supercluster X-ray emission is not required.
Pravdo, S. H.↗
The dynamics of rich clusters of galaxies. II - The Perseus cluster
The dynamics of the Perseus cluster are analyzed using self-consistent equilibrium analytical models. Using existing data in the literature plus new radial velocities reported here, composite surface density and velocity dispersion profiles are derived. These profiles have been compared with dynamical models described by Kent and Gunn (1982). The best fit suggest the presence of a significant degree of anisotropy in the velocity distribution: galaxy orbits are constrained to pass within a radius of seven cluster radii, or 1.3 deg of the cluster center. For Hubble constant = 50, a core radius of 340 kpc 11 arcmin and a mass to visual light ratio M/L = 300 are found. Using these results, X-ray observations of the intracluster medium in Perseus are reanalyzed. A previously noted discrepancy between the observed temperature of the hot gas and the cluster velocity dispersion is reduced but not eliminated. A cooling accretion flow previously deduced to exist in this cluster is shown to extend to only about one-third of the cluster radius.
Kent, S. M.↗