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Effects of Natural Variability on the Use of Standard Deviation to Represent Measurement Uncertainties in Atmospheric Composition Studies

Measurement uncertainty is defined as a “non-negative parameter characterizing the dispersion of the quantity values being attributed to a measurand”. It is most common that the uncertainties of GAW hourly measurements, such as greenhouse gas measurements, are reported as standard deviations derived from individual sampling at a higher time resolution (e.g., 1 min). In contrast, the uncertainties of GAW measurements of reactive gases and aerosol properties are reported in percentiles covering the same probability. A quick look at hourly CO 2 data from Cape Grim, Australia yielded some interesting findings: the hourly standard deviation is, on average, more than a factor of 10 higher for the measurements under non-background conditions (over 50% observations), while the difference in average CO 2 amount fraction was less than 2 ppm. The dramatic contrast cannot be explained by the difference in measurement uncertainties, but can largely be attributed the natural variability, or episodic ambient CO 2 variation reflecting changes in meteorological conditions or emissions. These initial findings motivated a more in-depth analysis of the ground-based measurements of trace gases and aerosol properties. This analysis will be using continuous 1 min ground site observations to construct time averaged statistical indicators to evaluate whether the standard deviation is adequate to represent the dispersion, especially under marked influence by natural variability. The suitability of this representation can be determined by examining the difference between the standard deviation and percentiles encompassing the same probability. We will examine time intervals of 1 hour, 3 hours, and 24 hours, with the latter time intervals chosen to match those commonly used in model assessments. We will also investigate how natural variability can alter the probability distribution of the measurands and how adequate the quadrature propagation of uncertainties is under these conditions. The results will include several trace gases (e.g., CO 2 , CO, O 3 , and NO 2 ) with a range of measurement techniques (e.g., PANDORA, in situ), atmospheric lifetimes, and aerosol properties (e.g. scattering coefficient). The findings from this analysis should provide some useful feedback on the best practices for uncertainty reporting.

Measurement Uncertainty↗
DOE OSTI2023

Measurement of the cross-sections of the electroweak and total production of a Zγ pair in association with two jets in pp collisions at s = 13 TeV with the ATLAS detector

This Letter presents the measurement of the fiducial and differential cross-sections of the electroweak production of a Zγ pair in association with two jets. The analysis uses 140 fb –1 of LHC proton–proton collision data taken at $\sqrt{s}$ = 13 TeV recorded by the ATLAS detector during the years 2015–2018. Events with a Z boson candidate decaying into either an e + e – or μ + μ – pair, a photon and two jets are selected. The electroweak component is extracted by requiring a large dijet invariant mass and by using the information about the centrality of the system and is measured with an observed and expected significance well above five standard deviations. The fiducial pp→Zγjj cross-section for the electroweak production is measured to be 3.6 ± 0.5 fb. The total fiducial cross-section that also includes contributions where the jets arise from strong interactions is measured to be $16.8_{–1.8}^{+2.0}$ fb. The results are consistent with the Standard Model predictions. Differential cross-sections are also measured using the same events and are compared with parton-shower Monte Carlo simulations. Good agreement is observed between data and predictions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Observation of triple J/ψ meson production in proton-proton collisions

Protons consist of three valence quarks, two up-quarks and one down-quark, held together by gluons and a sea of quark-antiquark pairs. Collectively, quarks and gluons are referred to as partons. In a proton-proton collision, typically only one parton of each proton undergoes a hard scattering – referred to as single-parton scattering – leaving the remainder of each proton only slightly disturbed. Here, we report the study of double- and triple-parton scatterings through the simultaneous production of three J/ψ mesons, which consist of a charm quark-antiquark pair, in proton-proton collisions recorded with the CMS experiment at the Large Hadron Collider. We observed this process – reconstructed through the decays of J/ψ mesons into pairs of oppositely charged muons – with a statistical significance above five standard deviations. We measured the inclusive fiducial cross-section to be 272$^{+141}_{-104}$(stat) ± 17 (syst)fb, and compared it to theoretical expectations for triple-J/ψ meson production in single-, double- and triple-parton scattering scenarios. Assuming factorization of multiple hard-scattering probabilities in terms of single-parton scattering cross-sections, double- and triple-parton scattering are the dominant contributions for the measured process.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Marcus–Hush–Chidsey kinetics at electrode–electrolyte interfaces

Electrochemical kinetics at electrode–electrolyte interfaces limit the performance of devices including fuel cells and batteries. While the importance of moving beyond Butler–Volmer kinetics and incorporating the effect of electronic density of states of the electrode has been recognized, a unified framework that incorporates these aspects directly into electrochemical performance models is still lacking. In this work, we explicitly account for the density functional theory-calculated density of states numerically in calculating electrochemical reaction rates for a variety of electrode–electrolyte interfaces. We first show the utility of this for two cases related to Li metal electrodeposition and stripping on a Li surface and a Cu surface (anode-free configuration). The deviation in reaction rates is minor for cases with flat densities of states such as Li, but is significant for Cu due to nondispersive d-bands creating large variation. Finally, we consider a semiconducting case of a solid-electrolyte interphase consisting of LiF and Li2CO3 and note the importance of the Fermi level at the interface pinned by the redox reaction occurring there. We identify the asymmetry in reaction rates as a function of discharge/charge naturally within this approach.

Kurchin, Rachel (ORCID:0000000221474809)↗
DOE OSTI2025

Extreme radiation emission regime for electron beams in strong focusing ion channels and undulators

A fundamental comparison between a magnetic undulator and an ion channel, or betatron, radiation from relativistic electrons is presented. While conventional theories nominally range from the undulator (𝐾 <1) to the wiggler (𝐾 >1) regime, they are only applicable for sufficiently large Lorentz factors (𝛾 0 ≫𝐾). They therefore do not account for high 𝐾/𝛾 0 cases, for which we show that particle trajectories and radiation characteristics strongly deviate from the linear predictions in both magnetic undulators and ion channels. This problem arises from the fundamental differences between a magnetostatically and electrostatically induced oscillation. A reformulation of both the ion channel betatron wavelength and amplitude, as well as the same parameters in a magnetic undulator, permits us to compare cases with equivalent oscillation period and amplitude in the two different scenarios. The notable differences in spectral features of the two radiation mechanisms can then be addressed via numerical simulations of single particle as well as full beam dynamics. Additionally, we identify and quantify a novel transverse orbit precession effect in ion channels for particles with initial angular momentum relative to the device axis. This effect, which is significant in cases of strong transverse kinetic energy oscillations, alters both the radiation divergence and the beam emittance. In this paper, we present this new theoretical framework and compare its results with numerical simulation applied to realizable experimental tests of such radiation sources.

Frazzitta, Andrea [University of Rome “La Sapienza↗
DOE OSTI2024

Quantum electrodynamics mediated by a photon with continuous spin

In recent work with Zhou, we studied classical interactions of matter with a “continuous spin” field, whose excitations have zero mass but nonzero spin Casimir (spin scale) ρ . We reported evidence that such theories are a calculable infrared deformation of familiar massless theories including electromagnetism. Building on the aforementioned work, this paper presents rules for computing scattering amplitudes involving charged scalar matter and continuous spin photons with nonzero spin scale. As a concrete example, we compute the pair annihilation and Compton scattering amplitudes in this theory and comment on their physical properties, including unitarity and scaling behavior at small and large ρ . Like the classical physics and soft factors studied in prior work, these amplitudes exhibit “helicity correspondence,” recovering familiar amplitudes at energy scales ≫ ρ , but with calculable deviations that could be experimentally tested. These results bolster the conjecture that continuous spin particles with a very small ρ could mediate long-range forces in nature (e.g., the photon could be a continuous spin particle), and extend the range of physical effects that could be used to test this hypothesis. Published by the American Physical Society 2024

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1977

Photon scattering cross sections of H2 and He measured with synchrotron radiation

Total (elastic + inelastic) differential photon scattering cross sections have been measured for H2 gas and He, using an X-ray beam. Absolute measured cross sections agree with theory within the probable errors. Relative cross sections (normalized to theory at large S) agree to better than one percent with theoretical values calculated from wave functions that include the effect of electron-electron Coulomb correlation, but the data deviate significantly from theoretical independent-particle (e.g., Hartree-Fock) results. The ratios of measured absolute He cross sections to those of H2, at any given S, also agree to better than one percent with theoretical He-to-H2 cross-section ratios computed from correlated wave functions. It appears that photon scattering constitutes a very promising tool for probing electron correlation in light atoms and molecules.

Ice, G. E.↗
NASA NTRS1977

Effects of random phase changes on the formation of synthetic aperture radar imagery

The effects of Gaussian random fluctuation and linear change of the echo phase on the response of the azimuth matched processor of a synthetic aperture radar (airborne or spaceborne for ocean-surface sensing) is analyzed numerically. It is found that the random fluctuation would not alter appreciably the processor response if its standard deviation is less than pi, while its normalized correlation time is larger than 1. If these two bounding conditions are not satisfied, then the sidelobe level becomes relatively large and overshadows the central peak. In the case of linear displacement it is found that the main effect is the spatial displacement of the point scatterer in the image plane.

Elachi, C.↗
NASA NTRS1976

Long-latency evoked potentials to irrelevant, deviant stimuli

Occasional shifts of loudness in a repetitive train of clicks elicited a late-positive wave (P3a) in nonattending subjects which peaked at a mean latency of 258 msec and had a frontocentral scalp distribution; P3a was typically preceded by an 'N2' component at 196 msec. The P3a wave was distinguishable from the longer-latency (378 msec) parietocentrally distributed 'P3b' wave that was evoked by the same stimulus in an actively attending subject, thus confirming the findings of Squires et al. (1975). Infrequently presented single sounds did not produce large or consistent N2-P3a components; the critical condition for the generation of an N2-P3a wave seemed to be that the infrequent sounds represent a deviation (intensity increment or decrement) from a repetitive background. Furthermore, increasing the repetition rate of the background clicks drastically reduced N1-P2 amplitude but had little effect on the amplitude of N2-P3a. This suggests that N2-P3a is not simply a delayed N1-P2 'vertex potential', but rather reflects the operation of a 'mismatch' detector, which registers deviations from an ongoing auditory background.

Snyder, E.↗
NASA NTRS1985

Ellipsoidal geometry in asteroid thermal models - The standard radiometric model

The major consequences of ellipsoidal geometry in an othewise standard radiometric model for asteroids are explored. It is shown that for small deviations from spherical shape a spherical model of the same projected area gives a reasonable aproximation to the thermal flux from an ellipsoidal body. It is suggested that large departures from spherical shape require that some correction be made for geometry. Systematic differences in the radii of asteroids derived radiometrically at 10 and 20 microns may result partly from nonspherical geometry. It is also suggested that extrapolations of the rotational variation of thermal flux from a nonspherical body based solely on the change in cross-sectional area are in error.

Brown, R. H.↗
NASA NTRS2000

Processing and Properties of SiC/MoSi2-SiC Composites Fabricated by Melt Infiltration

Hi-Nicalon SiC fiber reinforced MoSi2-SiC matrix composites (SiC/MoSi2-SiC) have been fabricated by the melt infiltration approach. The composite consists of approximately 60 vol%, 2-D woven BN/SiC coated Hi-Nicalon SiC fibers and approximately 40 vol% MoSi2-SiC matrix. The room temperature tensile properties and thermal conductivity of the SiC/MoSi2-SiC composites were measured and compared with those of the melt infiltrated SiC/SiC composites. The influence oi fiber architecture on tensile properties was also evaluated. Results indicate that the primary modulus, stress corresponding to deviation from linearity, and transverse thermal conductivity values for the SiC/MoSi2-SiC composites are significantly lower than those for the SiC/SiC composites. Microcracking of the matrix due to the large difference in thermal expansion between MoSi2 and SiC appears to be the reason for the lower matrix dominated properties of SiC/MoSi2-SiC composites.

Bhatt, Ramakrishna T.↗
NASA NTRS2003

A Comparison of Latent Heat Fluxes over Global Oceans for Four Flux Products

To improve our understanding of global energy and water cycle variability, and to improve model simulations of climate variations, it is vital to have accurate latent heat fluxes (LHF) over global oceans. Monthly LHF, 10-m wind speed (U10m), 10-m specific humidity (Q10h), and sea-air humidity difference (Qs-Q10m) of GSSTF2 (version 2 Goddard Satellite-based Surface Turbulent Fluxes) over global Oceans during 1992-93 are compared with those of HOAPS (Hamburg Ocean Atmosphere Parameters and Fluxes from Satellite Data), NCEP (NCEP/NCAR reanalysis). The mean differences, standard deviations of differences, and temporal correlation of these monthly variables over global Oceans during 1992-93 between GSSTF2 and each of the three datasets are analyzed. The large-scale patterns of the 2yr-mean fields for these variables are similar among these four datasets, but significant quantitative differences are found. The temporal correlation is higher in the northern extratropics than in the south for all variables, with the contrast being especially large for da Silva as a result of more missing ship data in the south. The da Silva has extremely low temporal correlation and large differences with GSSTF2 for all variables in the southern extratropics, indicating that da Silva hardly produces a realistic variability in these variables. The NCEP has extremely low temporal correlation (0.27) and large spatial variations of differences with GSSTF2 for Qs-Q10m in the tropics, which causes the low correlation for LHF. Over the tropics, the HOAPS LHF is significantly smaller than GSSTF2 by approx. 31% (37 W/sq m), whereas the other two datasets are comparable to GSSTF2. This is because the HOAPS has systematically smaller LHF than GSSTF2 in space, while the other two datasets have very large spatial variations of large positive and negative LHF differences with GSSTF2 to cancel and to produce smaller regional-mean differences. Our analyses suggest that the GSSTF2 latent heat flux, surface air humidity, and winds are likely to be more realistic than the other three flux datasets examined, although those of GSSTF2 are still subject to regional biases.

Chou, Shu-Hsien↗
DOE OSTI2020

Method and apparatus for evaluating superconducting tunnel junction detector noise versus bias voltage

A technique for characterizing the noise behavior of a superconducting tunnel junction (STJ) detector as a function of its applied bias voltage Vb by stepping the STJ's bias voltage across a predetermined range and, at each applied bias, making multiple measurements of the detector's current, calculating their mean and their standard deviation from their mean, and using this standard deviation as a measure of the STJ detector's noise at that applied bias. Because the method is readily executed under computer control, it is particularly useful when large numbers of STJ detectors require biasing, as in STJ detector arrays In a preferred implementation, the STJ is measured under computer control by attaching it to a digital spectrometer comprising a digital x-ray processor (DXP) coupled to a preamplifier that can set the STJ's bias voltage Vb using a digital-to-analog converter (DAC) controlled by the DXP.

Warburton, William K.↗
DOE OSTI2022

Anderson Acceleration for Distributed Training of Deep Learning Models

Anderson acceleration (AA) is an extrapolation technique that has recently gained interest in the deep learning (DL) community to speed-up the sequential training of DL models. However, when performed at large scale, the DL training is exposed to a higher risk of getting trapped into steep local minima of the training loss function, and standard AA does not provide sufficient acceleration to escape from these steep local minima. This results in poor generalizability and makes AA ineffective. To restore AA’s advantage to speed-up the training of DL models on large scale computing platforms, we combine AA with an adaptive moving average procedure that boosts the training to escape from steep local minima. By monitoring the relative standard deviation between consecutive iterations, we also introduce a criterion to automatically assess whether the moving average is needed. We applied the method to the following DL instantiations for image classification: (i) ResNet50 trained on the open-source CIFAR100 dataset and (ii) ResNet50 trained on the open-source ImageNet1k dataset. Numerical results obtained using up to 1,536 NVIDIA V100 GPUs on the OLCF supercomputer Summit showed the stabilizing effect of the moving average on AA for all the problems above.

Lupo Pasini, Massimiliano↗
NASA NTRS1986

Viscous nongeostrophic baroclinic instability

Calculations have been performed of the (linear) stability of a baroclinic flow to three-dimensional perturbations. Both the simple Eady basic state and the rotating Hadley cell of Antar and Fowlis are considered. The independent influences of the Richardson (Ri), thermal Rossby (baroclinicity), Ekman, and Prandtl numbers are examined, as well as the influences of the angle of orientation of the horizontal wave vector and the wavelength. It is shown that if the wavelength is allowed to vary freely, disturbances of the Eady type are preferred (i.e., have greatest growth rate) unless Ri and Ekman numbers are small enough and the thermal Rossby number is large enough. In the latter case, disturbances whose angles of orientation are almost symmetric and whose wavelengths are mesoscale are preferred. If, on the other hand, the wavelength is fixed at a mesoscale size, only the symmetric and almost symmetric modes have growth. By allowing the wave vector orientation to deviate from purely symmetric, it is noted that the region of instability (i.e., critical Ri) is increased, the extent of which is greater for longer wavelength. For Prandtl number = 1, permitting the angle to be nonsymmetric demonstrates the existence of two maxima in growth rate at opposite angles of orientation and with very different energetics. For Prandtl number far enough from one and for large enough dissipation, only one of these two modes has positive growth rates. Growing oscillatory modes were found for some cases.

Miller, T. L.↗
NASA NTRS2015

Implicit Large-Eddy Simulations of Zero-Pressure Gradient, Turbulent Boundary Layer

A set of direct simulations of zero-pressure gradient, turbulent boundary layer flows are conducted using various span widths (62-630 wall units), to document their influence on the generated turbulence. The FDL3DI code that solves compressible Navier-Stokes equations using high-order compact-difference scheme and filter, with the standard recycling/rescaling method of turbulence generation, is used. Results are analyzed at two different Re values (500 and 1,400), and compared with spectral DNS data. They show that a minimum span width is required for the mere initiation of numerical turbulence. Narrower domains ((is) less than 100 w.u.) result in relaminarization. Wider spans ((is) greater than 600 w.u.) are required for the turbulent statistics to match reference DNS. The upper-wall boundary condition for this setup spawns marginal deviations in the mean velocity and Reynolds stress profiles, particularly in the buffer region.

Turblent boundary layer↗
DOE OSTI2021

Anion Exchange Ionomers: Impact of Chemistry on Thin-Film Properties

Ionomer thin-films (i.e., 20–100 nm) on supports serve as model systems to understand ionomer-catalyst interfacial behavior as well as the confinement-driven deviation in properties from bulk membranes. While ionomer thin-films have been examined for proton exchange ionomers, the thin-film properties of anion exchange ionomers (AEIs) remain largely unexplored. More importantly, delineating the convoluted impact of chemistry and confinement on thin-film morphology and hydration is of interest to advancing the field on functional ionic interfaces. In this work, these aspects are studied by using AEIs of different backbones (perfluorinated, aliphatic, and aromatic) and side chains (various lengths, and single versus dual functional groups). Quartz-crystal microbalance and spectroscopic ellipsometry are used to analyze density and coupled with calculated free volume fraction of thin-films to provide insights on their gas transport properties. AEI side-chain's chemical character plays a key role in how confinement modulates hydration (in thin-film versus bulk). Overall, the results elucidate the effects of backbone, side-chain chemistry versus anion/cation type in the confinement-driven changes in thin-film morphology and swelling. This study also provides new insights for tuning AEI transport functionalities at interfaces via chemistry, which can benefit the design and development of electrode-ionomers for alkaline membrane-based energy systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Comparing simulated demand flexibility against actual performance in commercial office buildings

Commercial building energy benchmarking has been used as a mechanism to evaluate energy use of a single building over time, relative to other similar buildings, or to simulations of a reference building conforming to various energy standards. Lack of empirical demand flexibility data and consistent flexibility metrics has limited the ability to compare demand flexibility performance with estimated demand flexibility in buildings. In this study, we collected demand response performance data for a total of 831 demand response events from 192 sites as a first step to build such a building demand flexibility dataset, and propose a standard core data schema to consolidate field data from different sources. We also performed parametric simulations of a control strategy called “global temperature adjustment” using commercial office prototype building models. We then compared the simulated demand flexibility performance against the actual data for offices with global temperature adjustment strategy implemented. During demand response events with an average outside air temperature of 34 °C (range 23 °C–42 °C), the measured demand decrease intensity of the demand flexibility metrics were 6.1 watts per square meter (W/m 2 ), 10.0 W/m 2 , 11.1 W/m 2 , 7.1 W/m 2 , and 4.7 W/m 2 for small, small–medium, medium, medium–large, and large office buildings, respectively. Compared to the measured data in medium- and large-size buildings, the simulated demand decrease intensity was 0.7 W/m 2 (17%) lower on average. The discrepancy between simulated and measured peak demand intensities fell within one standard deviation of the mean measured data. Here, the comparison results validate the credibility of simulations in capturing real building data for assessing the technical potential of building demand flexibility.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗