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At least 1,513 records · Page 84

Single Molecule Spectroscopy Studies of Acid–Base Chemical Gradients Using Nile Red as a Probe of Local Surface Acidity

Single molecule spectroscopy studies of local acidity along bifunctional acid-base gradients are reported. Gradients are prepared by directional vapor phase diffusion and subsequent reaction of 3-aminopropyl-trimethoxysilane with a uniform silica film. Gradient formation is confirmed by spectroscopic ellipsometry and by static water contact angle measurements. X-ray photoelectron spectroscopy is used to characterize the nitrogen content and degree of nitrogen protonation along the gradient. Nile Red is employed as the probe dye in single molecule spectroscopy studies of these gradients. While Nile Red is well-known for its solvent sensitivity, it is used here, for the first time, to sense the acid/base properties of the film in two-color wide-field fluorescence imaging experiments. The data reveal broad bimodal distributions of Nile Red emission spectra that vary along the gradient direction. The single-molecule results are consistent with solution-phase ensemble acid/base studies of the dye. The former reveal a gradual transition from a surface dominated by basic aminosilane sites at the high-amine end of the gradient to one dominated by acidic silanol sites at the low-amine end. The sub-diffraction-limited spatial resolution afforded by superlocalization of the single molecules reveals spatial correlations in the acid/base properties of the gradient over ~ 200 nm distances. Furthermore, these studies provide data relevant to the use of aminosilane-modified silica in bifunctional, cooperative chemical catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Critical Role of the Interfacial Layer in Associating Polymers with Microphase Separation

Polymers with dynamic (transient) bonds, often called associating polymers, have been attracting significant attention in recent years due to their unique viscoelastic properties, self-healing ability, and recyclability. Nevertheless, understanding the mechanisms and the factors controlling their macroscopic properties remains limited due to the higher complexity introduced by the dynamic bonds. Here in this study, small-angle X-ray scattering (SAXS), broadband dielectric spectroscopy (BDS), and rheology were applied to unravel the structure and dynamics of telechelic associating polymers with different molecular weights. SAXS measurements revealed phase separation of the functional end groups with an average cluster size of ~2–3 nm and the distance between clusters controlled by the chain length. Borrowing the interfacial layer model analysis of BDS data from the polymer nanocomposite field, we demonstrated the presence of an interfacial polymer layer with a thickness of ~0.7–0.9 nm surrounding these clusters. Rheological measurements showed quantitatively that the presence of the interfacial layer significantly alters the viscoelastic behavior of these materials, indicating the crucial role of the interfacial layer in defining the macroscopic mechanical properties of the studied telechelic materials. The presented results emphasize that phase separation of the functional groups in associating polymers leads to very significant changes of the viscoelastic properties, opening a promising avenue in the design of novel functional materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Seasonality and Albedo Dependence of Cloud Radiative Forcing in the Upper Colorado River Basin

Mountains create and enhance their own clouds, which both scatter and absorb shortwave radiation from the sun and absorb and re-emit land surface and atmospheric longwave radiation. However, the impacts of clouds on the surface radiation balance in high elevation snowy mountain terrain are poorly explored. In this study, we use data collected by the SAIL field campaign and partner organizations in the upper elevations (2,880 m.a.s.l) of the Upper Colorado River Basin (UCRB) over a 21-month period from September 2021 to June 2023 to estimate Cloud Radiative Forcing (CRF) in the shortwave, longwave, and the net effect. Longwave warming effects dominate during the winter when snow albedos are high (0.8–0.9) and the background atmospheric precipitable water vapor is low (<0.5 cm), yielding a maximum monthly average net CRF of +34.7 W·m -2 , meaning that clouds increase the net radiation relative to clear skies during this time period. The sign of net CRF switches in the warm season as snow recedes, sun-angles increase, and the North American monsoon arrives, yielding a minimum monthly average net CRF of -47.6 W·m -2 with hourly minima of -600 W·m -2 . The sign of net CRF is typically positive, even at solar noon, when the surface is snow covered, except for a brief period over melting, low-albedo snow (0.5–0.6) impacted by dust impurities. Sensitivity tests elucidate the role of the surface albedo on the net CRF. The results suggest that net CRF will increase in magnitude and lead to a more persistent cooling effect on the surface net radiation budget as the snow cover declines.

54 ENVIRONMENTAL SCIENCES↗

Remote Sensing of Live Fuel Moisture for Wildfires Using SMAP Satellite Observations

Live Fuel Moisture (LFM) is a critical parameter for wildfire risk assessment, traditionally measured by labor-intensive field sampling. However, sampled LFM data are influenced by site-specific factors, such as local vegetation types and plant traits, and are often collected retrospectively after wildfire events, making it difficult to obtain pre-fire data for predictive applications. Here, we evaluate the relationship between LFM and Vegetation Water Content (VWC) and Soil Moisture (SM) retrieved from SMAP L-band brightness temperature using the Maximum Entropy Production (MEP) approach. The MEP-retrieved VWC exhibited strong correlation with in situ measurements of LFM ( r > 0.6) in the Western U.S. The integration of high-resolution vegetation coverage data enhances the detection of sub-grid vegetation heterogeneity. This study demonstrates the operational potential of remote sensing derived VWC as a scalable proxy of LFM, supporting its application in regional assessment of wildfire risk.

Cho, Kyeungwoo [Georgia Institute of Technology, A↗

Auto-generating databases of Yield Strength and Grain Size using ChemDataExtractor

Abstract The emerging field of material-based data science requires information-rich databases to generate useful results which are currently sparse in the stress engineering domain. To this end, this study uses the’materials-aware’ text-mining toolkit, ChemDataExtractor, to auto-generate databases of yield-strength and grain-size values by extracting such information from the literature. The precision of the extracted data is 83.0% for yield strength and 78.8% for grain size. The automatically-extracted data were organised into four databases: a Yield Strength, Grain Size, Engineering-Ready Yield Strength and Combined database. For further validation of the databases, the Combined database was used to plot the Hall-Petch relationship for, the alloy, AZ31, and similar results to the literature were found, demonstrating how one can make use of these automatically-extracted datasets.

36 MATERIALS SCIENCE↗

Quantum annealing algorithms for Boolean tensor networks

Abstract Quantum annealers manufactured by D-Wave Systems, Inc., are computational devices capable of finding high-quality heuristic solutions of NP-hard problems. In this contribution, we explore the potential and effectiveness of such quantum annealers for computing Boolean tensor networks. Tensors offer a natural way to model high-dimensional data commonplace in many scientific fields, and representing a binary tensor as a Boolean tensor network is the task of expressing a tensor containing categorical (i.e., $$\{0, 1\}$$ { 0 , 1 } ) values as a product of low dimensional binary tensors. A Boolean tensor network is computed by Boolean tensor decomposition, and it is usually not exact. The aim of such decomposition is to minimize the given distance measure between the high-dimensional input tensor and the product of lower-dimensional (usually three-dimensional) tensors and matrices representing the tensor network. In this paper, we introduce and analyze three general algorithms for Boolean tensor networks: Tucker, Tensor Train, and Hierarchical Tucker networks. The computation of a Boolean tensor network is reduced to a sequence of Boolean matrix factorizations, which we show can be expressed as a quadratic unconstrained binary optimization problem suitable for solving on a quantum annealer. By using a novel method we introduce called parallel quantum annealing, we demonstrate that Boolean tensor’s with up to millions of elements can be decomposed efficiently using a DWave 2000Q quantum annealer.

97 MATHEMATICS AND COMPUTING↗

Broadband radiometric measurements from GPS satellites reveal summertime Arctic Ocean Albedo decreases more rapidly than sea ice recedes

Abstract New measurements from the Arctic ± 40 days around the summer solstice show reflected sunlight from north of 80°N decreases 20–35%. Arctic sea ice coverage decreases 7–9% over this same time period (as reported by the NSIDC) implying Arctic sea ice albedo decreases in addition to the sea ice receding. Similar Antarctic measurements provide a baseline to which Arctic measurements are compared. The Antarctic reflected sunlight south of 80°S is up to 30% larger than the Arctic reflectance and is symmetric around the solstice implying constant Antarctic reflectivity. Arctic reflected sunlight 20 days after solstice is > 100W/m 2 less than Antarctic reflected sunlight. For perspective, this is enough heat to melt > 1 mm/hour of ice. This finding should be compared with climate models and in reanalysis data sets to further quantify sea ice albedo’s role in Arctic Amplification. The measurements were made with previously unpublished pixelated radiometers on Global Positioning System satellites from 2014 to 2019. The GPS orbits give each radiometer instantaneous and continuous views of 37% of the Earth, two daily full views of the Arctic and Antarctic. Furthermore, the GPS constellation gives full-time full-Earth coverage that may provide data that complements existing limited field of view instruments that provide a less synoptic Earth view.

54 ENVIRONMENTAL SCIENCES↗

A neutron recoil-spectrometer for measuring yield and determining liner areal densities at the Z facility

For this study, a proof-of-principle CR-39 based neutron-recoil-spectrometer was built and fielded on the Z facility. Data from this experiment match indium activation yields within a factor of 2 using simplified instrument response function (IRF) models. The data also demonstrates the need for neutron shielding in order to infer liner areal densities. A new shielded design has been developed. The spectrometer is expected to achieve signal-to-background greater than 2 for the down-scattered neutron signal and greater than 30 for the primary signal.

47 OTHER INSTRUMENTATION↗

Study of structural, transport and magneto-crystalline anisotropy in La 1-x Sr x MnO 3 (0.30 ≤ x ≤ 0.40) perovskite manganites

In this paper we present structural, transport, magnetic and magneto-crystalline anisotropy of La 1–x Sr x MnO 3 (х = 0.30, 0.33, 0.36, and 0.40) synthesized using the solid-state reaction method. The X-ray diffraction pattern of the samples is well indexed to the rhombohedral structure with R 3 - c space group. Lattice parameters and unit cell volume are found to decrease monotonically upon increasing Sr 2+ concentration at La 3+ site. X-ray photoelectron spectroscopy confirms the presence of Mn 4+ and Mn 3+ , the ratio of which (Mn 4+ /Mn 3+ ) increases from 0.44 to 0.64 with increasing Sr 2+ concentration. From the ρ(T) and M(T) data analysis, we find that T MI and M S are larger for x = 0.33 composition, suggesting a weakening of the double-exchange interaction due to competing super-exchange interactions in x = 0.30, 0.36 and 0.40 samples. We calculated MCA constant (K 1 ) by fitting the saturation magnetisation data at a higher magnetic field using the law of approach model, M = M S [1-a/H-b/H 2 ]-χH with K 1 2 = (105/8)bMs 2 and is in the order of 10 5 erg/cm 3 .

36 MATERIALS SCIENCE↗

Does Bayesian model averaging improve polynomial extrapolations? Two toy problems as tests

We assess the accuracy of Bayesian polynomial extrapolations from small parameter values, x, to large values of x. We consider a set of polynomials of fixed order, intended as a proxy for a fixed-order effective field theory (EFT) description of data. We employ Bayesian model averaging (BMA) to combine results from different order polynomials (EFT orders). Our study considers two 'toy problems' where the underlying function used to generate data sets is known. We use Bayesian parameter estimation to extract the polynomial coefficients that describe these data at low x. A 'naturalness' prior is imposed on the coefficients, so that they are $\mathcal{O}(1)$. We BMA different polynomial degrees by weighting each according to its Bayesian evidence and compare the predictive performance of this BMA with that of the individual polynomials. In conclusion, the credibility intervals on the BMA forecast have the stated coverage properties more consistently than does the highest evidence polynomial, though BMA does not necessarily outperform every polynomial.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Dynamical inflection point inflation

Abstract We provide a mechanism to obtain multiple inflection points for the inflaton potential based on the Coleman-Weinberg potential. The key ingredient is the existence of zeros of the inflaton quartic coupling beta function, which can be simply realized by a sign change of a gauge coupling beta function at a massive threshold scale in gauge-Yukawa models. A universal inflaton potential emerges for a wide range of models and can accommodate the observational data in the small-field inflation scenario. While the ratio of tensor over scalar amplitudes is predicted to be small, the running of the scalar spectral index, α s , has branches with both positive and negative values. The positive branch with α s ≳ 0.002 will be tested by the coming cosmic microwave background observations.

Astronomy & Astrophysics↗

Calibration of the underground muon detector of the Pierre Auger Observatory

To obtain direct measurements of the muon content of extensive air showers with energy above 10 16.5 eV, the Pierre Auger Observatory is currently being equipped with an underground muon detector (UMD), consisting of 219 10 m 2 -modules, each segmented into 64 scintillators coupled to silicon photomultipliers (SiPMs). Direct access to the shower muon content allows for the study of both of the composition of primary cosmic rays and of high-energy hadronic interactions in the forward direction. As the muon density can vary between tens of muons per m 2 close to the intersection of the shower axis with the ground to much less than one per m 2 when far away, the necessary broad dynamic range is achieved by the simultaneous implementation of two acquisition modes in the read-out electronics: the binary mode, tuned to count single muons, and the ADC mode, suited to measure a high number of them. In this work, we present the end-to-end calibration of the muon detector modules: first, the SiPMs are calibrated by means of the binary channel, and then, the ADC channel is calibrated using atmospheric muons, detected in parallel to the shower data acquisition. The laboratory and field measurements performed to develop the implementation of the full calibration chain of both binary and ADC channels are presented and discussed. The calibration procedure is reliable to work with the high amount of channels in the UMD, which will be operated continuously, in changing environmental conditions, for several years.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Prospects for future studies using deep imaging: analysis of individual Galactic cirrus filaments

The presence of Galactic cirrus is an obstacle for studying both faint objects in our Galaxy and low surface brightness extragalactic structures. With the aim of studying individual cirrus filaments in Sloan Digital Sky Survey (SDSS) Stripe 82 data, we develop techniques based on machine learning and neural networks that allow one to isolate filaments from foreground and background sources in the entirety of Stripe 82 with a precision similar to that of the human expert. Our photometric study of individual filaments indicates that only those brighter than 26 mag arcsec −2 in the SDSS r band are likely to be identified in SDSS Stripe 82 data by their distinctive colours in the optical bands. We also show a significant impact of data processing (e.g. flat-fielding, masking of bright stars, and sky subtraction) on colour estimation. Analysing the distribution of filaments’ colours with the help of mock simulations, we conclude that most filaments have colours in the following ranges: 0.55 ≤g − r ≤ 0.73 and 0.01 ≤ r − i ≤ 0.33. Our work provides a useful framework for an analysis of all types of low surface brightness features (cirri, tidal tails, stellar streams, etc.) in existing and future deep optical surveys. For practical purposes, we provide the catalogue of dust filaments.

79 ASTRONOMY AND ASTROPHYSICS↗

6⁢𝐻-perovskite dimer lattice with antiferromagnetic interactions: Ba 3⁢ Zn 1−𝑥⁢ Ca 𝑥 ⁢Ru 2 ⁢O 9

Here, we investigate the magnetic behavior of the 6⁢𝐻-perovskite dimer lattice Ba 3 ⁢Zn 1−𝑥 ⁢Ca 𝑥 ⁢Ru 2 ⁢O 9 using analytical theory, density functional theory, inelastic neutron scattering, and modeling of historical magnetization and neutron-scattering data. A dimer mean-field theory built upon classical Luttinger–Tisza analysis generates a phase diagram revealing a transition from a nonmagnetic singlet to a finite-moment ground state as interdimer couplings increase. A (generalized) linear spin-wave theory captures multiplet mixing, excitation gap closing, and fluctuation-induced moment suppression. Density-functional-theory calculations on selected compounds, together with neutron spectroscopy of dilute Ba 3 ⁢Zn⁢(Ru 1−𝑥 ⁢Sb 𝑥 ) 2 ⁢O 9 , confirm the exchange hierarchy, enabling quantification of previously published experiments within this framework. Our results identify three mechanisms for magnetic moment suppression—quantum fluctuations, ligand hybridization, and nonmagnetic-singlet/magnetic-multiplet mixing.

Pajerowski, Daniel M. [Oak Ridge National Laborato↗

Strong-field ionization of water. II. Electronic and nuclear dynamics en route to double ionization

We investigate the role of nuclear motion and strong-field-induced electronic couplings during the double ionization of deuterated water using momentum-resolved coincidence spectroscopy. By examining the three-body dicationic dissociation channel, D$^{+}$/D$^{+}$/O, for both few- and multi-cycle laser pulses, strong evidence for intra-pulse dynamics is observed. The extracted angle- and energy-resolved double ionization yields are compared to classical trajectory simulations of the dissociation dynamics occurring from different electronic states of the dication. In contrast with measurements of single photon double ionization, pronounced departure from the expectations for vertical ionization is observed, even for pulses as short as 10~fs in duration. We outline numerous mechanisms by which the strong laser field can modify the nuclear wavefunction en-route to final states of the dication where molecular fragmentation occurs. Specifically, we consider the possibility of a coordinate-dependence to the strong-field ionization rate, intermediate nuclear motion in monocation states prior to double ionization, and near-resonant laser-induced dipole couplings in the ion. These results highlight the fact that, for small and light molecules such as D$_2$O, a vertical-transition treatment of the ionization dynamics is not sufficient to reproduce the features seen experimentally in the strong field coincidence double-ionization data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Bayesian inference for plasmonic nanometrology

Here, we introduce a Bayesian method for the characterization of plasmonic nanoparticles, which is applicable to both near- and far-field problems. Designed to combine data generated from any photon-plasmon interaction experiment with physically motivated theoretical models, our approach leverages state-of-the-art Markov chain Monte Carlo sampling techniques and returns parameter estimates on nanometric scales. Simulated spectral data sets, describing resonant scattering of photons from ellipsoidal and toroidal nanoparticles, are explored as concrete examples of our approach, with the resulting Bayesian estimates showing excellent agreement with the ground truth, even under conditions of high statistical noise. By incorporating Bayes factors into the method as well, we reveal how model selection can determine which one of competing geometric shapes better explains the observed data. Our comprehensive nanometrology procedure can be tailored to a variety of light-particle interaction models, and its reliance on Bayesian inference furnishes automatic uncertainty quantification. In addition to applicability to a host of plasmonic configurations such as nanoparticle dimers, trimers, and array studies, it is proposed that the presented analysis can be extended to the quantum regime, where nonclassical photon statistics may provide additional insight for inference of scatterer properties.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Spin Seebeck effect near the antiferromagnetic spin-flop transition

In this work, we develop a low-temperature, long-wavelength theory for the interfacial spin Seebeck effect (SSE) in easy-axis antiferromagnets. The field-induced spin-flop (SF) transition of Néel order is associated with a qualitative change in SSE behavior: Below SF, there are two spin carriers with opposite magnetic moments, with the carriers polarized along the field forming a majority magnon band. Above SF, the low-energy, ferromagneticlike mode has magnetic moment opposite the field. This results in a sign change of the SSE across SF, which agrees with recent measurements on Cr 2 O 3 /Pt and Cr 2 O 3 /Ta devices. In our theory, SSE is due to a Néel spin current below SF and a magnetic spin current above SF. Using the ratio of the associated Néel to magnetic spin-mixing conductances as a single constant fitting parameter, we reproduce the field dependence of the experimental data and partially the temperature dependence of the relative SSE jump across SF.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗