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At least 1,801 records · Page 100

Constraining Data Mining with Physical Models: Voltage- and Oxygen Pressure-Dependent Transport in Multiferroic Nanostructures

Development of new generation electronic devices requires understanding and controlling the electronic transport in ferroic, magnetic, and optical materials, which is hampered by two factors. First, the complications of working at the nanoscale, where interfaces, grain boundaries, defects, and so forth, dictate the macroscopic characteristics. Second, the convolution of the response signals stemming from the fact that several physical processes may be activated simultaneously. Here, we present a method of solving these challenges via a combination of atomic force microscopy and data mining analysis techniques. Rational selection of the latter allows application of physical constraints and enables direct interpretation of the statistically significant behaviors in the framework of the chosen physical model, thus distilling physical meaning out of raw data. We demonstrate our approach with an example of deconvolution of complex transport behavior in a bismuth ferrite–cobalt ferrite nanocomposite in ambient and ultrahigh vacuum environments. Measured signal is apportioned into four electronic transport patterns, showing different dependence on partial oxygen and water vapor pressure. These patterns are described in terms of Ohmic conductance and Schottky emission models in the light of surface electrochemistry. Finally and furthermore, deep data analysis allows extraction of local dopant concentrations and barrier heights empowering our understanding of the underlying dynamic mechanisms of resistive switching.

36 MATERIALS SCIENCE↗

Single-Polymer–Particle Growth Kinetics with Molecular Catalyst Speciation and Single-Turnover Imaging

The dynamics of the local environments surrounding molecular polymerization catalysts plausibly impact turnover kinetics, but the impact of and nature of such dynamics have previously been obscured by ensemble averaging. With Grubbs’ second generation ruthenium metathesis catalyst and a precipitation polymerization system, studies at the single-particle and -turnover level establish that (1) an inverse correlation exists between rate and duration of single-polymer–particle growth of aggregates, consistent with a local environment density model for the time-variable kinetics; (2) cross-linking additives produced a small, but detectible, reduction in overall monomer incorporation; (3) total ruthenium quantity within the polymer particles (as characterized by energy dispersive X-ray spectroscopy) is differentiable from the quantity that is catalytically active (as characterized by in situ fluorescence microscopy), providing catalyst speciation information; and (4) time-resolved enyne metathesis reactions can be imaged, corresponding to single turnovers at individual molecular catalysts during polymer growth under synthetically relevant conditions. Here, these findings identify and characterize reactivity distributions likely arising from the dynamics of local environments. As such, these data provide reactivity information that is unavailable through traditional ensemble analytical methods that obscure this type of information through averaging.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Influence of Molecular Solvation on the Conformation of Star Polymers

We have used neutron scattering to investigate the influence of concentration on the conformation of a star polymer. By varying the contrast between the solvent and isotopically labeled stars, we obtain the distributions of polymer and solvent within a star polymer from analysis of scattering data. A correlation between the local desolvation and the inward folding of star branches is discovered. From the perspective of thermodynamics, we find an analogy between the mechanism of polymer localization driven by solvent depletion and that of the hydrophobic collapse of polymers in solutions.

Li, Xin↗

X-ray Mapping of Nanoparticle Superlattice Thin Films

We combine grazing-incidence and transmission small-angle X-ray diffraction with electron microscopy studies to characterize the structure of nanoparticle films with long-range order. Transmission diffraction is used to collect in-plane diffraction data from single grains and locally aligned nanoparticle superlattice films. Systematic mapping of samples can be achieved by translating the sample in front of the X-ray beam with a spot size selected to be on the order of superlattice grain features. This allows a statistical determination of superlattice grain size and size distribution over much larger areas than typically accessible with electron microscopy. Transmission X-ray measurements enables spatial mapping of the grain size, orientation, uniformity, strain, or crystal projections and polymorphs. Furthermore, we expand this methodology to binary nanoparticle superlattice and nanorod superlattice films. Our study provides a framework for characterization of nanoparticle superlattices over large areas which complements or expands microstructure information from real-space imaging.

GISAXS↗

Magnetically brightened dark electron-phonon bound states in a van der Waals antiferromagnet

In van der Waals (vdW) materials, strong coupling between different degrees of freedom can hybridize elementary excitations into bound states with mixed character. Correctly identifying the nature and composition of these bound states is key to understanding their ground state properties and excitation spectra. Here, we use ultrafast spectroscopy to reveal bound states of d-orbitals and phonons in 2D vdW antiferromagnet NiPS 3 . These bound states manifest themselves through equally spaced phonon replicas in frequency domain. These states are optically dark above the Néel temperature and become accessible with magnetic order. By launching this phonon and spectrally tracking its amplitude, we establish the electronic origin of bound states as localized d–d excitations. Our data directly yield electron-phonon coupling strength which exceeds the highest known value in 2D systems. These results demonstrate NiPS 3 as a platform to study strong interactions between spins, orbitals and lattice, and open pathways to coherent control of 2D magnets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Addressing the characterisation challenge to understand catalysis in MOFs: the case of nanoscale Cu supported in NU-1000

Here, we explore the dynamic structure and reactivity of Cu species supported on NU-1000. By combining pair distribution function (PDF) analysis and difference envelope density (DED) analysis of in situ synchrotron-based X-ray scattering data, we simultaneously probe the local structure of supported Cu-species, their distribution within NU-1000 and distortions of the NU-1000 lattice under conditions relevant to catalysis and catalyst activation. Our analyses show that atomic layer deposition (ALD) of Cu in NU-1000 (Cu-AIM) leads to the formation of Cu-oxo clusters within the small pores that connect the triangular and hexagonal channels. Exposure of Cu-AIM to a reducing atmosphere at 200 °C produces metallic Cu 0 of two distinct particle sizes: ~4 nm nanoparticles and small sub-nanometer clusters. The size of these nanoparticles appears to be constrained by NU-1000 pore dimensions, with evidence of the sub-nanometer clusters being bound within the triangular channels flanked by pyrene rings. This supported Cu 0 –NU-1000 system is catalytically active for gas-phase ethylene hydrogenation. Exposure of the catalyst to oxidative atmosphere re-oxidises the Cu species to a Cu 2 O cuprite phase. The dynamic restructuring of the system in different chemical environments underscores the importance of probing these systems in situ .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Enhanced Jahn-Teller response induced by low-dose 10 MeV I{sup +} irradiation of La{sub 0.7}Ca{sub 0.3}MnO{sub 3−δ} films

The structural response of pulsed laser deposited La{sub 0.7}Ca{sub 0.3}Mn0{sub 3−δ} films to low-level 10 MeV I{sup +} irradiation is correlated with magnetic and electronic properties. A series of annealed pulsed laser deposited films were subjected to ion irradiation at doses of 0.5–2.0 × 10{sup 13} 10 MeV iodine ions/cm{sup 2}. X-ray diffraction measurements show no measurable increase in the full width at half maximum values of major reflections before and after irradiation. Extended x-ray absorption fine structure analyses (EXAFS), employing both a model independent fitting using expanded cumulants as well as a nonlinear least squares multiple scattering model based on FEFF generated theoretical EXAFS data, were employed to measure local properties relative to the Mn ions. Increasing irradiation doses lead to an unambiguous evolution of MnO{sub 6} octahedra from highly symmetric (i.e., undistorted) to a clear bimodal structure in which the MnO{sub 6} octahedra are measured to undergo a c-axis stretching bearing resemblance to a Jahn-Teller distortion. Concomitantly, the metal to insulator transition temperature decreases more than 270 K and the magnetoresistance increases from 10{sup 2}% to 10{sup 6}%.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Communication: Does a single CH{sub 3}CN molecule attached to Ru(bipy){sub 3}{sup 2+} affect its absorption spectrum?

Tris(bipyridine)ruthenium(II) (Ru(bipy){sub 3}{sup 2+}) is a prototypical transition metal coordination complex whose photophysical properties have attracted considerable attention. A much debated issue is whether the metal-to-ligand charge transfer (MLCT) transition that accounts for the complex’s beautiful red color is fully delocalized across all three bipyridine ligands or located on just one ligand. Here, we show based on gas-phase action spectroscopy that attachment of a single acetonitrile molecule does not change the absorption spectrum from that of the bare ions, which is indicative of a delocalized state. However, the gas-phase spectra of the bare and one solvent molecule complexes are significantly blueshifted relative to that obtained in bulk acetonitrile, which suggests that in solution the polarizability of many solvent molecules working together can localize the MLCT state. Our data clearly show that more than one solvent molecule is needed to break the symmetry of the MLCT excited state and reproduce its solution-phase characteristics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The uncharacterized gene EVE contributes to vessel element dimensions in Populus

The radiation of angiosperms led to the emergence of the vast majority of today’s plant species and all our major food crops. Their extraordinary diversification occurred in conjunction with the evolution of a more efficient vascular system for the transport of water, composed of vessel elements. The physical dimensions of these water-conducting specialized cells have played a critical role in angiosperm evolution; they determine resistance to water flow, influence photosynthesis rate, and contribute to plant stature. However, the genetic factors that determine their dimensions are unclear. Here we show that a previously uncharacterized gene, ENLARGED VESSEL ELEMENT ( EVE ) , contributes to the dimensions of vessel elements in Populus , impacting hydraulic conductivity. Our data suggest that EVE is localized in the plasma membrane and is involved in potassium uptake of differentiating xylem cells during vessel development. In plants, EVE first emerged in streptophyte algae, but expanded dramatically among vessel-containing angiosperms. The phylogeny, structure and composition of EVE indicates that it may have been involved in an ancient horizontal gene-transfer event.

59 BASIC BIOLOGICAL SCIENCES↗

AGN evolution from a galaxy evolution viewpoint

We explore the connections between the evolving galaxy and active galactic nucleus (AGN) populations. We present a simple phenomenological model that links the evolving galaxy mass function and the evolving quasar luminosity function, which makes specific and testable predictions for the distribution of host galaxy masses for AGNs of different luminosities. We show that the ϕ{sup ∗} normalizations of the galaxy mass function and of the AGN luminosity function closely track each other over a wide range of redshifts, implying a constant “duty cycle” of AGN activity. The strong redshift evolution in the AGN L{sup ∗} can be produced by either an evolution in the distribution of Eddington ratios, or in the m{sub bh}/m{sub ∗} mass ratio, or both. To try to break this degeneracy we look at the distribution of AGNs in the Sloan Digital Sky Survey (m{sub bh}, L) plane, showing that an evolving ratio m{sub bh}/m{sub ∗}∝(1+z){sup 2} reproduces the observed data and also reproduces the local relations that connect the black hole population with the host galaxies for both quenched and star-forming populations. We stress that observational studies that compare the masses of black holes in active galaxies at high redshift with those in quiescent galaxies locally will always see much weaker evolution. Evolution of this form would produce, or could be produced by, a redshift-independent m{sub bh}–σ relation and could explain why the local m{sub bh}–σ relation is tighter than m{sub bh}–m{sub *} even if σ is not directly linked to black hole growth. Irrespective of the evolution of m{sub bh}/m{sub *}, the model reproduces both the appearance of “downsizing” and the so-called “sub-Eddington boundary” without any mass-dependence in the evolution of black hole growth rates.

79 ASTRONOMY AND ASTROPHYSICS↗

Cosmological constraints from H ii starburst galaxy apparent magnitude and other cosmological measurements

ABSTRACT We use H ii starburst galaxy apparent magnitude measurements to constrain cosmological parameters in six cosmological models. A joint analysis of H ii galaxy, quasar angular size, baryon acoustic oscillations peak length scale, and Hubble parameter measurements result in relatively model-independent and restrictive estimates of the current values of the non-relativistic matter density parameter $\Omega _{\rm m_0}$ and the Hubble constant H0. These estimates favour a 2.0–3.4σ (depending on cosmological model) lower H0 than what is measured from the local expansion rate. The combined data are consistent with dark energy being a cosmological constant and with flat spatial hypersurfaces, but do not strongly rule out mild dark energy dynamics or slightly non-flat spatial geometries.

79 ASTRONOMY AND ASTROPHYSICS↗

Physical properties of metallic antiferromagneticCaCo1.86As2 single crystals

X-ray powder diffraction (XRD), magnetic susceptibility χ, isothermal magnetization M, heat capacity Cp, and in-plane electrical resistivity ρ measurements as a function of temperature T and magnetic field H are presented for CaCo1.86As2 single crystals. The electronic structure is probed by angle-resolved photoemission spectroscopy (ARPES) measurements of CaCo1.86As2 and by full-potential linearized augmented-plane-wave calculations for the supercell Ca8Co15As16 (CaCo1.88As2). Our XRD crystal structure refinement is consistent with the previous combined refinement of x-ray and neutron powder diffraction data showing a collapsed-tetragonal ThCr2Si2-type structure with 7(1)% vacancies on the Co sites corresponding to the composition CaCo1.86As2 [D. G. Quirinale et al., Phys. Rev. B 88, 174420 (2013)]. The anisotropic χ(T) data are consistent with the magnetic neutron diffraction data of Quirianale et al. that demonstrate the presence of A-type collinear antiferromagnetic order below the Néel temperature TN=52(1) K with the easy axis being the tetragonal c axis. However, no clear evidence from the ρ(T) and Cp(T) data for a magnetic transition at TN is observed. A metallic ground state is demonstrated from the band calculations and the ρ(T), Cp(T), and ARPES data, and spin-polarized calculations indicate a competition between the A-type AFM and FM ground states. The Cp(T) data exhibit a large Sommerfield electronic coefficient reflecting a large density of states at the Fermi energy D(EF) that is enhanced compared with the band structure calculation where the bare D(EF) arises from Co 3d bands. At 1.8 K, the M(H) data for H∥c exhibit a well-defined first-order spin-flop transition at an applied field of 3.5 T. The small ordered moment of ≈0.3μB/Co obtained from the M(H) data at low T, the large exchange enhancement of χ and the lack of a self-consistent interpretation of the χ(T) and M(H,T) data in terms of a local moment Heisenberg model together indicate that the magnetism of CaCo1.86As2 is itinerant.

36 MATERIALS SCIENCE↗

Tools for probing new physics with newly discovered gamma-ray targets

Here, we present a computational tool, TweedleDEE, for empirically modeling diffuse gamma-ray background emission in a 1° region of the sky, using publicly available gamma-ray data off-axis from the region of interest. This background model allows a user to perform a purely data-driven search for anomalous localized sources of gamma-ray emission, including new physics. A major application of this tool would be in searching for dark matter annihilation in newly discovered astrophysical targets. For this purpose, we derive a scaling relation for determining velocity-dependent 𝐽-factors using only the stellar parameters, which can be broadly applied to obtain dark matter constraints from new targets. As an application of these tools, we use TweedleDEE and MADHATv2 to perform the first search for dark matter annihilation in the newly discovered Leo VI dwarf spheroidal galaxy, and present model constraints for a variety of choices of the annihilation channel and velocity dependence of the cross section.

dark matter↗

X-ray scattering based scanning tomography for imaging and structural characterization of cellulose in plants

X-ray and neutron scattering have long been used for structural characterization of cellulose in plants. Due to averaging over the illuminated sample volume, these measurements traditionally overlooked the compositional and morphological heterogeneity within the sample. Here, a scanning tomographic imaging method is described, using contrast derived from the X-ray scattering intensity, for virtually sectioning the sample to reveal its internal structure at a resolution of a few micrometres. This method provides a means for retrieving the local scattering signal that corresponds to any voxel within the virtual section, enabling characterization of the local structure using traditional data-analysis methods. This is accomplished through tomographic reconstruction of the spatial distribution of a handful of mathematical components identified by non-negative matrix factorization from the large dataset of X-ray scattering intensity. Joint analysis of multiple datasets, to find similarity between voxels by clustering of the decomposed data, could help elucidate systematic differences between samples, such as those expected from genetic modifications, chemical treatments or fungal decay. The spatial distribution of the microfibril angle can also be analyzed, based on the tomographically reconstructed scattering intensity as a function of the azimuthal angle.

36 MATERIALS SCIENCE↗

Scalable Asynchronous Domain Decomposition Solvers

We discuss how parallel implementations of linear iterative solvers generally alternate between phases of data exchange and phases of local computation. Increasingly large problem sizes and more heterogeneous compute architectures make load balancing and the design of low latency network interconnects that are able to satisfy the communication requirements of linear solvers very challenging tasks. In particular, global communication patterns such as inner products become increasingly limiting at scale. We explore the use of asynchronous communication based on one-sided Message Passing Interface primitives in the context of domain decomposition solvers. In particular, a scalable asynchronous two-level Schwarz method is presented. We discuss practical issues encountered in the development of a scalable solver and show experimental results obtained on a state-of-the-art supercomputer system that illustrate the benefits of asynchronous solvers in load balanced as well as load imbalanced scenarios. Using the novel method, we can observe speedups of up to four times over its classical synchronous equivalent.

97 MATHEMATICS AND COMPUTING↗

Phoenix Dust Storm (PHX-DUST) Scale: A Cooperatively Developed Dust Storm Scale for Phoenix, Arizona

Using extensive localized meteorological and air quality data for central Arizona from 2010 to 2023, we create a postevent dust storm scale for use by the primary stakeholders in central Arizona for the Phoenix metropolitan area called the Phoenix Dust Storm (PHX-DUST) scale. To ensure usability across a wide spectrum of users, a core concept was to “keep it simple.” The PHX-DUST scale is based on (i) maximum dust concentration for particulate matter (PM10) across the network in micrograms per cubic meter which determines category, e.g., “category 5 (the highest observed category)” and category 4; (ii) the number of network monitors achieving dust concentrations above a threshold of 500 μg m−3 (categorized as “widespread” or “isolated,” as measures of spatial extent); (iii) a duration parameter (which determines “long duration” or “short duration”); and (iv) a measure of wind speed over the affected area (maximum wind gust recorded over the network, which may not be the maximum wind of the storm). Using this index for the 189 dust storms impacting the Phoenix metropolitan area for the period 2010–23, the most severe dust storm occurred on 5 July 2011 and is classified as a “Category 5, Widespread, Long-Duration High-Gust” event. This initial attempt at defining the PHX-DUST scale holds valuable applications for research, education, and applied analyses. It demonstrates that a consortium of interested groups can effectively work to create products benefiting the weather community and general public. Here, the PHX-DUST scale can also serve as a foundational framework for application in other regions where dust storms pose a threat to the well-being of populations, infrastructure, and ecosystems.

Atmosphere↗

Enhanced mesoscale climate projections in TAR and AR5 IPCC scenarios: a case study in a Mediterranean climate (Araucanía Region, south central Chile)

Here, climate change scenarios are computed on a large scale, not accounting for local variations presented in historical data and related to human scale. Based on historical records, we validate a baseline (1962–1990) and correct the bias of A2 and B2 regional projections for the end of twenty-first century (2070–2100) issued from a high resolution dynamical downscaled (using PRECIS mesoscale model, hereinafter DGF-PRECIS) of Hadley GCM from the IPCC 3rd Assessment Report (TAR). This is performed for the Araucanía Region (Chile; 37°–40°S and 71°–74°W) using two different bias correction methodologies. Next, we study high-resolution precipitations to find monthly patterns such as seasonal variations, rainfall months, and the geographical effect on these two scenarios. Finally, we compare the TAR projections with those from the recent Assessment Report 5 (AR5) to find regional precipitation patterns and update the Chilean `projection. To show the effects of climate change projections, we compute the rainfall climatology for the Araucanía Region, including the impact of ENSO cycles (El Niño and La Niña events). The corrected climate projection from the high-resolution dynamical downscaled model of the TAR database (DGF-PRECIS) show annual precipitation decreases: B2 (-19.19 %, -287 ± 42 mm) and A2 (-43.38 %, -655 ± 27.4 mm per year. Furthermore, both projections increase the probability of lower rainfall months (lower than 100 mm per month) to 64.2 and 72.5 % for B2 and A2, respectively.

54 ENVIRONMENTAL SCIENCES↗

Integrating distributed acoustic sensing, borehole 3C geophone array, and surface seismic array data to identify long-period long-duration seismic events during stimulation of a Marcellus Shale gas reservoir

Microseismic monitoring by downhole geophones, surface seismic, fiber-optic distributed acoustic sensing (DAS), and distributed temperature sensing (DTS) observations were made during the hydraulic fracture stimulation of the MIP-3H well in the Marcellus Shale in northern West Virginia. DAS and DTS data measure the fiber strain and temperature, respectively, along a fiber-optic cable cemented behind the casing of the well. The presence of long-period long-duration (LPLD) events is evaluated in the borehole geophones, DAS data, and surface seismic data of one of the MIP-3H stimulated stages. LPLD events are generally overlooked during the conventional processing of microseismic data, but they represent significant nonbrittle deformation produced during hydraulic fracture stimulation. In a single stage that was examined, 160 preexisting fractures and two faults of suboptimal orientation are noted in the image logs. We identified two low-frequency ([Formula: see text]) events of large temporal duration (tens of seconds) by comparing the surface seismic data, borehole geophone data, and DAS amplitude spectra of one of the MIP-3H stages. Spectrograms of DAS traces in time and depth reveal that the first low-frequency event might be an injection noise that has footprints on all DAS channels above the stimulated stage. However, the surface seismic array indicates an LPLD event concurrent with the first low-frequency event on DAS. The second LPLD event on DAS data and surface seismic data is related to a local deformation and does not have footprints on all DAS channels. The interpreted events have duration less than 100 s with frequencies concentrated below 10 Hz, and are accompanied by microseismic events.

Geochemistry & Geophysics↗

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