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At least 883 records · Page 49

Photodriven Ammonia Synthesis from Manganese Nitrides: Photophysics and Mechanistic Investigations

Ammonia synthesis from N,N,O,O-supported manganese(V) nitrides and 9,10-dihydroacridine using proton-coupled electron transfer and visible light irradiation in the absence of precious metal photocatalysts is described. While the reactivity of the nitride correlated with increased absorption of blue light, excited-state lifetimes determined by transient absorption were on the order of picoseconds. Furthermore, this eliminated excited-state manganese nitrides as responsible for bimolecular N–H bond formation. Spectroscopic measurements on the hydrogen source, dihydroacridine, demonstrated that photooxidation of 9,10-dihydroacridine was necessary for productive ammonia synthesis. Transient absorption and pulse radiolysis data for dihydroacridine provided evidence for the presence of intermediates with weak E–H bonds, including the dihydroacridinium radical cation and both isomers of the monohydroacridine radical, but notably these intermediates were unreactive toward hydrogen atom transfer and net N–H bond formation. Additional optimization of the reaction conditions using higher photon flux resulted in higher rates of the ammonia production from the manganese(V) nitrides due to increased activation of the dihydroacridine.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

EXITE observation of the Galactic center - A new transient?

The balloon-borne Energetic X-ray Imaging Telescope Experiment observed the Galactic center on May 9, 1989. Within the 3.4-deg (FWHM) field of view, imaged with 22-arcmin resolution at 20-250 keV, two sources were detected: the 'Einstein source' (1E1740.7-2942) and a possible second source about 40 deg West (EXS1737.9-2952). This source was detected significantly at both 20-30 keV and 83-111 keV, suggesting a double-backscattered 511 keV line source at 102 keV and a soft excess, perhaps from a black hole candidate undergoing a transient outburst.

Grindlay, J. E.↗

Quantifying spatiotemporal variability in occupant exposure to an indoor airborne contaminant with an uncertain source location

Well-mixed zone models are often employed to compute indoor air quality and occupant exposures. While effective, a potential downside to assuming instantaneous, perfect mixing is underpredicting exposures to high intermittent concentrations within a room. When such cases are of concern, more spatially resolved models, like computational-fluid dynamics methods, are used for some or all of the zones. But, these models have higher computational costs and require more input information. A preferred compromise would be to continue with a multi-zone modeling approach for all rooms, but with a better assessment of the spatial variability within a room. Here to do so, we present a quantitative method for estimating a room's spatiotemporal variability, based on influential room parameters. Our proposed method disaggregates variability into the variability in a room's average concentration, and the spatial variability within the room relative to that average. This enables a detailed assessment of how variability in particular room parameters impacts the uncertain occupant exposures. To demonstrate the utility of this method, we simulate contaminant dispersion for a variety of possible source locations. We compute breathing-zone exposure during the releasing (source is active) and decaying (source is removed) periods. Using CFD methods, we found after a 30 minutes release the average standard deviation in the spatial distribution of exposure was approximately 28% of the source average exposure, whereas variability in the different average exposures was lower, only 10% of the total average. We also find that although uncertainty in the source location leads to variability in the average magnitude of transient exposure, it does not have a particularly large influence on the spatial distribution during the decaying period, or on the average contaminant removal rate. By systematically characterizing a room's average concentration, its variability, and the spatial variability within the room important insights can be gained as to how much uncertainty is introduced into occupant exposure predictions by assuming a uniform in-room contaminant concentration. We discuss how the results of these characterizations can improve our understanding of the uncertainty in occupant exposures relative to well-mixed models.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

An objective inter-comparison of trash mark constellations generated by manual and automated detection methods

Trash marks are unintentional markings observed on printed, scanned, or photocopied documents that result from permanent defects or transient material in office machines and can be used for source attribution of questioned documents. Trash mark examinations have been in use in forensic laboratories for decades, yet the method remains relatively untested and relies on training, experience, and anecdotal information to support its validity. Herein this study generated and harnessed objective data to empirically test one of the foundational theories for assessing the origin of photocopied documents: provided trash marks are present in sufficient quantity and/or quality, no two machines will exhibit a constellation of trash marks that is indistinguishable from another. In this project, objective trash mark location and size data was generated for 50 known photocopiers using both a traditional and a novel, automated method. Inter-machine comparisons were conducted using a novel variant of the Hausdorff distance algorithm to generate a quantitative assessment of how similar or different the 2450 pairs of trash mark constellations were from one another. This study found that each of the machines bearing one or more trash marks exhibited objective differences in their trash mark constellations, ultimately providing support for the tested hypothesis

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Subject-specific modeling framework for particle deposition using computational fluid dynamics

Quantifying particle deposition and dose in the respiratory tract requires a physiologically realistic representation and reproducible computational workflows. However, existing modeling frameworks, such as the International Commission on Radiological Protection (ICRP) compartmental models and the Multiple Path Particle Dosimetry (MPPD) tool, lack detailed deposition profiles and subject-specific capabilities. The combination of advances in computer vision algorithms applied to the respiratory tract and Computational Fluid and Particle Dynamics (CFPD) allows high-fidelity simulations of particle behavior in anatomically accurate geometries derived from individual CT scans. The segmentation, preprocessing, and file preparation task for a CFPD simulation was often time-consuming, and no prior studies to-date have yet presented a fully automated framework. This work presents a fully automated workflow to obtain individualized particle deposition profiles in the human respiratory tract. The pipeline starts with segmenting upper and lower airway geometries using morphological and deep learning-based methods, generating three-dimensional (3D) models from CT imaging data. Next, a series of algorithms are presented to quality check and prepare the 3D geometry for a CFD or CFPD simulation. The preprocessing step includes correcting geometric artifacts, enforcing a physically consistent mesh, and automatically identifying and capping multiple outlets, which is required for CFD/CFPD simulations. These processed models are then input into open-source (OpenFOAM) or commercial (StarCCM+) CFD solvers, where flow and transient particle transport equations — including turbulence and particle–wall interactions are solved under realistic breathing conditions. Finally, the resulting particle deposition profiles can be integrated with Monte Carlo radiation transport codes and state-of-the-art computational phantoms to assess organ-specific absorbed doses in scenarios of radioactive aerosol inhalation. The presented work streamlines respiratory tract segmentation, preprocessing for CFD/CFPD simulations, and integration with dose assessment workflows, reducing manual intervention and improving access to high-fidelity, subject-specific modeling. The high precision in predicted particle deposition and dose distributions can improve personalized treatment strategies in respiratory medicine and refine dose estimates for radiation protection.

AI↗

Optically targeted search for gravitational waves emitted by core-collapse supernovae during the first and second observing runs of advanced LIGO and advanced Virgo

In this work, we present the results from a search for gravitational-wave transients associated with core-collapse supernovae observed within a source distance of approximately 20 Mpc during the first and second observing runs of Advanced LIGO and Advanced Virgo. No significant gravitational-wave candidate was detected. We report the detection efficiencies as a function of the distance for waveforms derived from multidimensional numerical simulations and phenomenological extreme emission models. Furthermore, the sources with neutrino-driven explosions are detectable at the distances approaching 5 kpc, and for magnetorotationally driven explosions the distances are up to 54 kpc. However, waveforms for extreme emission models are detectable up to 28 Mpc. For the first time, the gravitational-wave data enabled us to exclude part of the parameter spaces of two extreme emission models with confidence up to 83%, limited by coincident data coverage. Besides, using ad hoc harmonic signals windowed with Gaussian envelopes, we constrained the gravitational-wave energy emitted during core collapse at the levels of 4.27×10 -4 M ⊙ c 2 and 1.28×10 -1 M ⊙ c 2 for emissions at 235 and 1304 Hz, respectively. These constraints are 2 orders of magnitude more stringent than previously derived in the corresponding analysis using initial LIGO, initial Virgo, and GEO 600 data.

79 ASTRONOMY AND ASTROPHYSICS↗

Removal of correlated background in a high-order harmonic transient absorption spectra with principal component regression

We demonstrate a 40x mean noise power reduction (NPR) in core-to-valence extreme ultraviolet (XUV) femtosecond transient absorption spectroscopy with a high harmonic generation (HHG) light source. An adaptive iteratively reweighted principal component regression (airPCR) is used to analyze and suppress spectrally correlated HHG intensity fluctuations. The technique requires significantly less user input and leads to a higher mean NPR than a previously introduced edge-pixel PCR method that relies on the manual identification of signal-free spectral regions. Both techniques are applied in a time-resolved XUV absorption study of the 2 snp 1 P o ( n ≥ 2) autoionizing Rydberg states of helium, demonstrating sub-10 −3 optical density sensitivity.

Faccialà, Davide (ORCID:0000000250720394)↗

Searches for Ultra-High-Energy Photons at the Pierre Auger Observatory

The Pierre Auger Observatory, which is the largest air-shower experiment in the world, offers unprecedented exposure to neutral particles at the highest energies. Since the start of data collection more than 18 years ago, various searches for ultra-high-energy (UHE, E≳10 17 eV) photons have been performed, either for a diffuse flux of UHE photons, for point sources of UHE photons or for UHE photons associated with transient events such as gravitational wave events. In the present paper, we summarize these searches and review the current results obtained using the wealth of data collected by the Pierre Auger Observatory.

79 ASTRONOMY AND ASTROPHYSICS↗

Numerical coupling of aerosol emissions, dry removal, and turbulent mixing in the E3SM Atmosphere Model version 1 (EAMv1) – Part 1: Dust budget analyses and the impacts of a revised coupling scheme

Abstract. An earlier study evaluating dust life cycle in the Energy Exascale Earth System Model (E3SM) Atmosphere Model version 1 (EAMv1) has revealed that the simulated global mean dust lifetime is substantially shorter when higher vertical resolution is used, primarily due to significant strengthening of dust dry removal in source regions. This paper demonstrates that the sequential splitting of aerosol emissions, dry removal, and turbulent mixing in the model's time integration loop, especially the calculation of dry removal after surface emissions and before turbulent mixing, is the primary reason for the vertical resolution sensitivity reported in that earlier study. Based on this reasoning, we propose a revised numerical process coupling scheme that requires the least amount of code changes, in which the surface emissions are applied before turbulent mixing instead of before dry removal. The revised scheme allows newly emitted particles to be transported aloft by turbulence before being removed from the atmosphere, and hence better resembles the dust life cycle in the real world. Sensitivity experiments show that the revised process coupling substantially weakens dry removal and strengthens vertical mixing in dust source regions. It also strengthens the large-scale transport from source to non-source regions, strengthens dry removal outside the source regions, and strengthens wet removal and activation globally. In transient simulations of the years 2000–2009 conducted using 1∘ horizontal grid spacing, 72 vertical layers, and unchanged tuning parameters of emission strength, the revised process coupling leads to a 40 % increase in the global total dust burden and an increase of dust lifetime from 1.8 to 2.5 d in terms of 10-year averages. Weakened dry removal and increased mixing ratios are also seen for other aerosol species that have substantial surface emissions, although the changes in mixing ratio are considerably smaller for the submicron species than for dust and sea salt. Numerical experiments confirm that the revised coupling scheme significantly reduces the strong and non-physical sensitivities of model results to vertical resolution in the original EAMv1. This provides a motivation for adopting the revised scheme in EAM as well as for further improvements on the simple revision presented in this paper.

54 ENVIRONMENTAL SCIENCES↗

A pulsed xenon megawatt arc plasma source

The exhaust of the source flowing into vacuum was measured by Thomson scattering diagnosis. Mean electron temperatures and densities were found to be 4-8 eV and of order ten to the 13th power cm/3 respectively over the 8 cm exhaust diameter at 30 cm from the source. Large shot to shot variations were noted. After a transient spike passes, these conditions persist during the power time of 125 microsecond. These exhaust conditions are marginal for evaluation of a proposed near resonant charge exchange pumped laser theory.

Michels, C. J.↗

A pulsed xenon megawatt arc plasma source

The exhaust of the source flowing into vacuum was measured by Thomson scattering diagnosis. Mean electron temperatures and densities were found to be 4-8 eV and on the order of 10 trillion per cu cm respectively, over the 8 cm exhaust diameter at 30 cm from the source. Large shot to shot variations were noted. After a transient spike passes, these conditions persist during the power time of 125 microsec. These exhaust conditions are marginal for evaluation of a proposed near resonant charge exchange pumped laser theory.

Michels, C. J.↗

Expansion of an X-ray coronal arch into the outer corona

An asymmetric expanding arch photographed in the inner corona with an X-ray telescope on August 13, 1973, is identified as the source of the mass ejected in a white-light transient in the outer corona. The morphology, angular position, estimated mass, and apparent rate of upward acceleration of the lower coronal arch are similar to those of the arch seen passing through the outer corona. The mass of material removed from the lower corona is estimated to be 2 by 10 to the 15th power g, and the upward motion is consistent with a constant acceleration of 12.5 m/sec per sec between 1.3 and 5 solar radii.

Rust, D. M.↗

Gamma-ray astronomy: Nuclear transition region

This monograph reviews the major theoretical and experimental efforts made during the past 12 years in gamma-ray astronomy over the energy range from 10 keV to about 100 MeV, where nuclear-transition lines are expected. Early attempts to detect celestial gamma rays are recounted, mechanisms of gamma-ray line and continuum production are examined, and formulas giving the various possible differential gamma-ray spectral shapes are provided. Predicted fluxes are discussed for solar gamma rays as well as for gamma emission from supernova remnants, supernovae, neutron stars, flare stars, the galactic core and disk, black holes, and diffuse sources. Gamma-ray interactions with matter are analyzed, particularly the photoelectric effect, Compton scattering from free electrons, and pair production in nuclear fields. Significant results are summarized for observations of gamma rays from the sun as well as from point and extended sources within and beyond the Galaxy, including diffuse fluxes and transient gamma-ray bursts. Factors pertaining to the design of gamma-ray astronomy experiments are considered, especially detector background limitations, gamma-ray production within instruments, and present-day detection methods.

Chupp, E. L.↗

Separation of variables solution for non-linear radiative cooling

A separation of variables solution has been obtained for transient radiative cooling of an absorbing-scattering plane layer. The solution applies after an initial transient period required for adjustment of the temperature and scattering source function distributions. The layer emittance, equal to the instantaneous heat loss divided by the fourth power of the instantaneous mean temperature, becomes constant. This emittance is a function of only the optical thickness of the layer and the scattering albedo; its behavior as a function of these quantities is considerably different than for a layer at constant temperature.

Siegel, Robert↗

The distance to the heliospheric VLF emission region

Two major episodes of heliospheric VLF emissions near 3 kHz have been observed by the Voyager spacecraft in 1983/84 and 1992/3. This higher-frequency component is apparently triggered by solar wind transients with sufficiently large spatial extents and energies to continue to propagate as shocks in the heliosheath. Entrainment of previously unshocked material and changed flow conditions in the heliosheath both tend to slow the shock propagation. The shock evolution is not self-similar. Rather, it is intermediate to two blast-wave similarity solutions in the moving solar wind frame. In one solution the shock moves as time to the 2/3 power and in the other as time to the 4/5 power. Using these models, the shock/Forbush decrease observed at Voyager 2 in September, 1991 and the turn-on of the 1992 emission is consistent with an emission region distance of approximately 130 AU (assuming no additional slowing of the shock in the heliosheath). If the termination shock was at approximately 70 AU when the transient shock collided with it, the true distance to the source region was probably closer to approximately 115 AU.

Mcnutt, R. L., Jr.↗

The Distance to the Heliospheric VLF Emission Region

Two major episodes of heliospheric VLF emissions near 3 kHz have been observed by the Voyager spacecraft in 1983-1984 and 1992-1993. This higher-frequency component is apparently triggered by solar wind transients with sufficiently large spatial extents and energies to continue to propagate as shocks in the heliosheath. Entrainment of previously unshocked material and changed flow conditions in the heliosheath both tend to slow the shock propagation. The shock evolution is not self-similar. Rather, it is intermediate to two blast-wave similarity solutions in the moving solar wind frame. In one solution the shock moves as time to the 2/3 power and in the other as time to the 4/5 power. Using these models, the shock/Forbush decrease observed at Voyager 2 in September, 1991 and the turn-on of the 1992 emission is consistent with an emission region distance of approx. 130 AU (assuming no additional slowing of the shock in the heliosheath). If the termination shock was at approx. 70 AU when the transient shock collided with it, the true distance to the source region was probably closer to approx. 115 AU.

McNutt, R. L., Jr.↗

"X-Ray Transients in Star-Forming Regions" and "Hard X-Ray Emission from X-Ray Bursters"

This grant funded work on the analysis of data obtained with the Burst and Transient Experiment (BATSE) on the Compton Gamma-Ray Observatory. The goal of the work was to search for hard x-ray transients in star forming regions using the all-sky hard x-ray monitoring capability of BATSE. Our initial work lead to the discovery of a hard x-ray transient, GRO J1849-03. Follow-up observations of this source made with the Wide Field Camera on BeppoSAX showed that the source should be identified with the previously known x-ray pulsar GS 1843-02 which itself is identified with the x-ray source X1845-024 originally discovered with the SAS-3 satellite. Our identification of the source and measurement of the outburst recurrence time, lead to the identification of the source as a Be/X-ray binary with a spin period of 94.8 s and an orbital period of 241 days. The funding was used primarily for partial salary and travel support for John Tomsick, then a graduate student at Columbia University. John Tomsick, now Dr. Tomsick, received his Ph.D. from Columbia University in July 1999, based partially on results obtained under this investigation. He is now a postdoctoral research scientist at the University of California, San Diego.

Halpern, Jules P.↗

Lightning and Other Influences On Tropical Tropospheric Ozone: Empirical Studies of Covariation

Tropical and subtropical tropospheric ozone are important radiatively active species, with particularly large effects in the upper third of the troposphere. Temporal variability of O3 has proved difficult to simulate day by day in process models. Thus, individual roles of lightning, biomass burning, and other pollution in providing precursor NO(x), radicals, and chain carriers (CO, hydrocarbons) remain unquantified by simulation, and it is theoretically reasonable that individual roles are magnified by a joint synergy. We use wavelet analysis and Burg-algorithm maximum entropy spectral analyses to describe time-scales and correlation of ozone with proxies for processes controlling its concentration. Our empirical studies link time variations apparent in several datasets: the SHADOZ (Southern Hemisphere Additional Ozonesondes) network stations (Nairobi, Fiji), and auxiliary series with power to explain ozone-determining processes, with some interpretation based on the TTO (Tropical Tropospheric Ozone) product derived from TOMS (the Total Ozone Mapping Spectrometer). The auxiliary series are The OTD/LIS(Optical Transient Detector/Lightning Imaging Sensor) measurements of the lightning NO(x) source, the OLR (Outgoing Longwave Radiation)measurement of high-topped clouds, and standard meteorological variables from the United States NCEP (National Centers for Environmental Prediction) and Data Assimilation Office analyses. Concentrating on equatorial ozone, we compare the statistical evidence on the variability of tropospheric ozone. Important variations occur on approximately two-week, two-month (Madden-Julian Oscillation) and annual scales, and relations with OLR suggest controls associated with continental clouds. Hence we are now using the Lightning Imaging Sensor data set to indicate NO(x) sources. We report initial results defining relative roles of the process mentioned affecting O3 using their covariance properties.

Chatfield, Robert B.↗