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DOE OSTI2016

Experimental and Computational Mechanistic Studies Guiding the Rational Design of Molecular Electrocatalysts for Production and Oxidation of Hydrogen

Understanding how to control the movement of protons and electrons is crucial to the design of fast, efficient electrocatalysts for hydrogen production and oxidation based on earth-abundant metals. Our work seeks to elucidate fundamental questions about proton movement. We have demonstrated that incorporating a pendant amine functioning as a proton relay in the second coordination sphere of a metal complex helps proton mobility, resulting in faster and more energy efficient catalysts. Proton transfer reactions are often rate limiting, and are influenced by several factors, such as pKa values, steric effects, hydrogen bonding, and solvation/desolvation of the exogenous base and acid employed. The presence of multiple protonation sites introduces branching points along the catalytic cycle, making less productive pathways accessible, or leading to the formation of stable off-cycle species. Using ligands with only one pendant amine mitigates this problem and results in catalysts with high rates for production of H2. For H2 oxidation catalysts, iron complexes with a high H2 binding affinity were developed. However, the improvement of H2 binding enthalpy resulted in a pKa mismatch between the protonated metal center and the protonated pendant amine, and consequently to rate-limiting intramolecular proton movement. Taken altogether, our results demonstrate the necessity of optimizing the entire catalytic cycle, as the optimization of a specific catalytic step can negatively influence another step, and not necessarily lead to better catalytic performance. We discuss a general procedure, based on thermodynamic arguments, which allows the simultaneous minimization of the free energy change of each catalytic step, yielding a nearly flat free energy surface, with no large barriers due to energy mismatches from either high- or low-energy intermediates. This research was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Pacific Northwest National Laboratory is operated by Battelle for DOE.

hydrogen, catalysis, quantum chemistry, proton tra↗

DOE OSTI2014

Coupled-oscillator theory of dispersion and Casimir-Polder interactions

We address the question of the applicability of the argument theorem (of complex variable theory) to the calculation of two distinct energies: (i) the first-order dispersion interaction energy of two separated oscillators, when one of the oscillators is excited initially and (ii) the Casimir-Polder interaction of a ground-state quantum oscillator near a perfectly conducting plane. We show that the argument theorem can be used to obtain the generally accepted equation for the first-order dispersion interaction energy, which is oscillatory and varies as the inverse power of the separation r of the oscillators for separations much greater than an optical wavelength. However, for such separations, the interaction energy cannot be transformed into an integral over the positive imaginary axis. If the argument theorem is used incorrectly to relate the interaction energy to an integral over the positive imaginary axis, the interaction energy is non-oscillatory and varies as r{sup −4}, a result found by several authors. Rather remarkably, this incorrect expression for the dispersion energy actually corresponds to the nonperturbative Casimir-Polder energy for a ground-state quantum oscillator near a perfectly conducting wall, as we show using the so-called “remarkable formula” for the free energy of an oscillator coupled to a heat bath [G. W. Ford, J. T. Lewis, and R. F. O’Connell, Phys. Rev. Lett. 55, 2273 (1985)]. A derivation of that formula from basic results of statistical mechanics and the independent oscillator model of a heat bath is presented.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2014

On the mass of the local group

We use recent proper motion measurements of the tangential velocity of M31, along with its radial velocity and distance, to derive the likelihood of the sum of halo masses of the Milky Way and M31. This is done using a sample of halo pairs in the Bolshoi cosmological simulation of ΛCDM cosmology selected to match the properties and the environment of the Local Group. The resulting likelihood gives an estimate of the sum of the masses of M {sub MW,} {sub 200c} + M {sub M31,} {sub 200c} = 2.40{sub −1.05}{sup +1.95}×10{sup 12} M{sub ⊙} (90% confidence interval). This estimate is consistent with individual mass estimates for the Milky Way and M31 and is consistent, albeit somewhat on the low side, with the mass estimated using the timing argument. We show that although the timing argument is unbiased on average for all pairs, for pairs constrained to have radial and tangential velocities similar to that of the Local Group the argument overestimates the sum of masses by a factor of 1.6. Using similar technique, we estimate the total dark matter mass enclosed within 1 Mpc from the Local Group barycenter to be M{sub LG}(r<1 Mpc)=4.2{sub −2.0}{sup +3.4}×10{sup 12} M{sub ⊙} (90% confidence interval).

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2013

Universal doomsday: analyzing our prospects for survival

Given a sufficiently large universe, numerous civilizations almost surely exist. Some of these civilizations will be short-lived and die out relatively early in their development, i.e., before having the chance to spread to other planets. Others will be long-lived, potentially colonizing their galaxy and becoming enormous in size. What fraction of civilizations in the universe are long-lived? The ''universal doomsday'' argument states that long-lived civilizations must be rare because if they were not, we should find ourselves living in one. Furthermore, because long-lived civilizations are rare, our civilization's prospects for long-term survival are poor. Here, we develop the formalism required for universal doomsday calculations and show that while the argument has some force, our future is not as gloomy as the traditional doomsday argument would suggest, at least when the number of early existential threats is small.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

Vacuum selection on axionic landscapes

We compute the distribution of minima that are reached dynamically on multi-field axionic landscapes, both numerically and analytically. Such landscapes are well suited for inflationary model building due to the presence of shift symmetries and possible alignment effects (the KNP mechanism). The resulting distribution of dynamically reached minima differs considerably from the naive expectation based on counting all vacua. These differences are more pronounced in the presence of many fields due to dynamical selection effects: while low lying minima are preferred as fields roll down the potential, trajectories are also more likely to get trapped by one of the many nearby minima. We show that common analytic arguments based on random matrix theory in the large D-limit to estimate the distribution of minima are insufficient for quantitative arguments pertaining to the dynamically reached ones. This discrepancy is not restricted to axionic potentials. We provide an empirical expression for the expectation value of such dynamically reached minimas' height and argue that the cosmological constant problem is not alleviated in the absence of anthropic arguments. We further comment on the likelihood of inflation on axionic landscapes in the large D-limit.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Angular correlation between the fission fragment intrinsic spins

The generation of fission fragment (FF) spins and of their relative orbital angular momentum has been debated for more than six decades, and no consensus has been achieved so far. The interpretation of recent experimental results of Wilson et al., has been challenged by several recent theoretical studies, which are not in agreement with one another. According to the interpretation by Wilson et al., the FF spins emerge very long after scission occurrs. Randrup and Vogt, while agreeing that the FF spins are uncorrelated, conclude on the basis of a phenomenological model that these spins are uncorrelated already before scission. Bulgac et al., in a fully microscopic study demonstrate that the primordial FF spin final values are defined before the emission of prompt neutrons and statistical gammas and are strongly correlated with a relative angle between spins close to 2π/3, a result in full agreement with the present independent analysis. The prompt neutrons and statistical gammas carry a significant amount of angular momentum according to the study of Stetcu et al. which can lead to a decorrelation of the FF bandhead spins of the yrast lines measured by Wilson et al., and which also provides arguments why these measured spins are so different from the primordial FF spins evaluated by Bulgac et al.. Here, I show that the unexpected character of the angular correlation between the primordial FF intrinsic spins, recently evaluated by Bulgac et al., which favors FF intrinsic spins pointing predominantly in opposite directions, can be understood by using simple general phase space arguments. The observation by Wilson et al., that the FF spins are uncorrelated follows from both the results of the microscopic calculation of Bulgac et al., and the present analysis of the full correlated probability distribution of the FF spins together with the relative orbital angular momentum of the primordial FFs. These arguments may apply also to heavy-ion collisions and, since there is no use of specifics of the particle interactions, the present results might apply to atomic and molecular systems as well.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Competition between roughness and strength for scale-dependent surfaces

Rocks famously have scale-dependent strength, yet the actual dependence is notoriously hard to measure or incorporate into any theoretical framework. Natural rough surfaces present an opportunity to solve the problem. Surfaces sliding in shear evolve as protrusions collide. These asperities can deform or break, thus creating a new surface shape. In particular, natural surfaces have roughness at all scales as well as scale-dependent strength. Based on a scaling analysis, we have previously suggested that the scale-dependent aspect ratio of steady-state surfaces should be proportional to the scale-dependent shear strain at yield. If true, scale-dependent strength could easily be inferred from natural surfaces. Thus, moving beyond the scaling argument to a rigorous treatment of scale-dependent strength for multiscale rough surfaces in shear is important. However, analytic frameworks for analyzing multiscale problems are challenging, as conventional continuum mechanics typically involves a single value for a material property across scales. Here, in this work, we build on the formalism of Persson (2001) that presents a method to compute contact area for rough surfaces with a prescribed topographic spectrum using a stochastic differential equation. The Persson formalism allows for plastic yield under normal loading of otherwise elastic materials and leaves open the possibility of scale-dependent yield stress. In this study, we pursue this route to develop a theory and numerical results for the yielding of a rough, elastoplastic surface with scale-dependent yield stress. Here, we examine surfaces for which the power spectrum of the topography 𝐶 and yield stress 𝑌 follow power laws as a function of scale 𝜆, such that 𝐶∼𝜆 −𝑚 and 𝑌∼𝜆 −𝑛 , respectively. In this formal treatment of the problem, we focus on surfaces in contact and the resulting yield and do not impose shear. Numerical solutions show that the deviation from the elastic scaling solution is bounded as expected by the prior 1D heuristic scaling argument that anticipates the Hurst exponent as 1−𝑛. We also show that the plasticity is expected to erode the contacts if 𝑚 is lower than 𝑛−3, which corresponds to a Hurst exponent lower than 1−𝑛/2. This result is rigorously sound for 2D, i.e., realistic surfaces, and quantitatively different than the prior scaling argument. The theory now permits a correspondingly quantitative approach to interpreting natural surfaces.

elasticity↗

DOE OSTI2023

Weak gravity conjecture

The weak gravity conjecture holds that in a theory of quantum gravity any gauge force must mediate interactions stronger than gravity for some particles. This statement has surprisingly deep and extensive connections to many different areas of physics and mathematics. Several variations on the basic conjecture have been proposed, including statements that are much stronger but are nonetheless satisfied by all known consistent quantum gravity theories. These related conjectures and the evidence for their validity in the string theory landscape are reviewed. Also reviewed here are a variety of arguments for these conjectures, which tend to fall into two categories: qualitative arguments that claim the conjecture is plausible based on general principles and quantitative arguments for various special cases or analogs of the conjecture. The implications of these conjectures for particle physics, cosmology, general relativity, and mathematics are also outlined. Finally, important directions for future research are highlighted.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2012

Linearization of dose-response curve of the radiochromic film dosimetry system

Purpose: Despite numerous advantages of radiochromic film dosimeter (high spatial resolution, near tissue equivalence, low energy dependence) to measure a relative dose distribution with film, one needs to first measure an absolute dose (following previously established reference dosimetry protocol) and then convert measured absolute dose values into relative doses. In this work, we present result of our efforts to obtain a functional form that would linearize the inherently nonlinear dose-response curve of the radiochromic film dosimetry system. Methods: Functional form [{zeta}= (-1){center_dot}netOD{sup (2/3)}/ln(netOD)] was derived from calibration curves of various previously established radiochromic film dosimetry systems. In order to test the invariance of the proposed functional form with respect to the film model used we tested it with three different GAFCHROMIC Trade-Mark-Sign film models (EBT, EBT2, and EBT3) irradiated to various doses and scanned on a same scanner. For one of the film models (EBT2), we tested the invariance of the functional form to the scanner model used by scanning irradiated film pieces with three different flatbed scanner models (Epson V700, 1680, and 10000XL). To test our hypothesis that the proposed functional argument linearizes the response of the radiochromic film dosimetry system, verification tests have been performed in clinical applications: percent depth dose measurements, IMRT quality assurance (QA), and brachytherapy QA. Results: Obtained R{sup 2} values indicate that the choice of the functional form of the new argument appropriately linearizes the dose response of the radiochromic film dosimetry system we used. The linear behavior was insensitive to both film model and flatbed scanner model used. Measured PDD values using the green channel response of the GAFCHROMIC Trade-Mark-Sign EBT3 film model are well within {+-}2% window of the local relative dose value when compared to the tabulated Cobalt-60 data. It was also found that criteria of 3%/3 mm for an IMRT QA plan and 3%/2 mm for a brachytherapy QA plan are passing 95% gamma function points. Conclusions: In this paper, we demonstrate the use of functional argument to linearize the inherently nonlinear response of a radiochromic film based reference dosimetry system. In this way, relative dosimetry can be conveniently performed using radiochromic film dosimetry system without the need of establishing calibration curve.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2013

Extracting and Applying SV-SV Shear Modes from Vertical Vibrator Data Across Geothermal Prospects Final Report

This 3-year project was terminated at the end of Year 1 because the DOE Geothermal project-evaluation committee decided one Milestone was not met and also concluded that our technology would not be successful. The Review Panel recommended a? no-go? decision be implemented by DOE. The Principal Investigator and his research team disagreed with the conclusions reached by the DOE evaluation committee and wrote a scientifically based rebuttal to the erroneous claims made by the evaluators. We were not told if our arguments were presented to the people who evaluated our work and made the? no-go? decision. Whatever the case regarding the information we supplied in rebuttal, we received an official letter from Laura Merrick, Contracting Officer at the Golden Field Office, dated June 11, 2013 in which we were informed that project funding would cease and instructed us to prepare a final report before September 5, 2013. In spite of the rebuttal arguments we presented to DOE, this official letter repeated the conclusions of the Review Panel that we had already proven to be incorrect. This is the final report that we are expected to deliver. The theme of this report will be another rebuttal of the technical deficiencies claimed by the DOE Geothermal Review Panel about the value and accomplishments of the work we did in Phase 1 of the project. The material in this report will present images made from direct-S modes produced by vertical-force sources using the software and research findings we developed in Phase 1 that the DOE Review Panel said would not be successful. We made these images in great haste when we were informed that DOE Geothermal rejected our rebuttal arguments and still regarded our technical work to be substandard. We thought it was more important to respond quickly rather than to take additional time to create better quality images than what we present in this Final Report.

15 GEOTHERMAL ENERGY↗

DOE OSTI2013

Truchas Reference Manual (V.2.8)

Truchas is executed in serial using a command of the form truchas [-h] [-d[:n ]] [-t] [-o:outdir ] [-r:rstfile ] infile assuming truchas is the name of the executable. The brackets denote optional arguments that are described in Table 1.1. The only required argument is the path to the input file infile . This file name must end with the extension “.inp" (without the quotes). The general format of the input file is described in the next section, and the following chapters describe the various Fortran namelists that go into the input file to describe the problem to be simulated. All of the output files are written to directory whose name is generated from the base name of the input file. For example, if the input file is myprob.inp, the output directory will be named myprob_output. The name of the output directory can be overridden using the -o option. The directory will be created if necessary. The precise manner of executing Truchas in parallel depends on the MPI implementation being used. This may be as simple as prefixing the serial invocation above with “mpirun -np n”, where n is the number of processes. But this varies widely and providing specific instructions is beyond the scope of this document. There is no difference in the Truchas arguments between serial and parallel, however.

36 MATERIALS SCIENCE↗

NASA NTRS1972

Implications of lunar aseismicity.

The aseismicity of the moon has been interpreted by Latham et al. (1970) as an indication that the moon is relatively cold in the interior. An alternative argument is now presented. This argument suggests the reverse conclusion, that the moon is too warm to be seismic. The argument is based on known properties of materials, in particular their modes of failure under shear stress. A tentative conclusion is presented that the moon is largely aseismic because the lunar-therm lies in the stable-sliding field of rock failure. It is too warm, rather than too cold.

Thomsen, L.↗

NASA NTRS1975

Improved upper limit on the photon rest mass

It is shown that application of standard MHD arguments to hydromagnetic waves observed in the Crab Nebula dramatically improves the upper bound on photon rest mass. The standard argument that massive photons are governed by the Phoca field equations is outlined and applied to wisp features (identified as hydromagnetic waves) observed in the Crab. The results imply an upper limit for the photon rest mass of between 3 by 10 to the -54th power and 3 by 10 to the -53rd power gram, which is smaller than the best previous limits by a factor of 10,000 to 100,000. It is noted that although the present limit is probably valid in order of magnitude, some doubt remains since there are inconsistencies in the standard arguments.

Barnes, A.↗

NASA NTRS1993

On Al-26 and other short-lived interstellar radioactivity

Several authors have shown that massive stars exploding at a rate of about three per century can account for a large portion, if not all, of the observed interstellar Al-26. In a separate argument using models of Galactic chemical evolution, Clayton (1984) showed that the Al-26/Al-27 production ratio was not large enough to maintain enough Al-26 in the Galactic disk gas of about 10 exp 10 solar masses having solar composition. We present a resolution of those conflicting arguments. A past history of Galactic infall growing the Galactic disk so dilutes the stable Al-27 concentration that the two approaches can be brought into near agreement. If massive stars dominate the production of Al-26, we suggest that the apparent shortfall of their Al-26/Al-27 yield ratio is to be interpreted as evidence for significant growth of the Galactic disk. We also discuss the implications of these arguments for other extinct radioactivities in meteorites, using I-129 and Sm-146 as examples.

Clayton, Donald D.↗

NASA NTRS2010

A Safety Conundrum Illustrated: Logic, Mathematics, and Science Are Not Enough

In an ideal world, conversations about whether a particular system is safe, or whether a particular method or tool enhances safety, would be emotion-free discussions concentrating on the level of safety required, available evidence, and coherent logical, mathematical, or scientific arguments based on that evidence. In the real world, discussions about safety are often not emotion-free. Political and economic arguments may play a bigger role than logical, mathematical, and scientific arguments, and psychological factors may be as important, or even more important, than purely technical factors. This paper illustrates the conundrum that can result from this clash of the ideal and the real by means of an imagined conversation among a collection of fictional characters representing various types of people who may be participating in a safety discussion.

Holloway, C. M.↗

NASA NTRS2015

AdvoCATE - User Guide

The basic vision of AdvoCATE is to automate the creation, manipulation, and management of large-scale assurance cases based on a formal theory of argument structures. Its main purposes are for creating and manipulating argument structures for safety assurance cases using the Goal Structuring Notation (GSN), and as a test bed and proof-of-concept for the formal theory of argument structures. AdvoCATE is available for Windows 7, Macintosh OSX, and Linux. Eventually, AdvoCATE will serve as a dashboard for safety related information and provide an infrastructure for safety decisions and management.

Safety Case↗

NASA NTRS2013

The Eccentric Behavior of Nearly Frozen Orbits

Frozen orbits are orbits which have only short-period changes in their mean eccentricity and argument of periapse, so that they basically keep a fixed orientation within their plane of motion. Nearly frozen orbits are those whose eccentricity and argument of periapse have values close to those of a frozen orbit. We call them "nearly" frozen because their eccentricity vector (a vector whose polar coordinates are eccentricity and argument of periapse) will stay within a bounded distance from the frozen orbit eccentricity vector, circulating around it over time. For highly inclined orbits around the Earth, this distance is effectively constant over time. Furthermore, frozen orbit eccentricity values are low enough that these orbits are essentially eccentric (i.e., off center) circles, so that nearly frozen orbits around Earth are bounded above and below by frozen orbits.

spacecraft↗

NASA NTRS1961

The Theory of Artificial Satellites in Terms of the Orbital True Longitude

The author's previous theory of the artificial satellite is derived in terms of the. disturbed eccentric anomaly. The present development, in terms of the orbital true longitude, is a substantial improvement over the earlier work in that it leads to the faster convergence for large eccentricities and to a smaller number of terms in the series representing the perturbations. Moreover, each approximation of the radius vector and of the parameters determining the position of the orbit plane is obtained not in the form of a truncated infinite series but in the form of trigonometric polynomials in two arguments. These arguments are the mean true anomaly and the mean argument of the latitude. The present theory, like the previous one, permits the computation of perturbations of any desired order. Thus, any future information about earth's gravitational field can easily be included.

Musen, Peter↗