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DOE OSTI2023

Structure, Dynamics, and Hydrogen Transport in Amorphous Polymers: An Analysis of the Interplay between Free Volume Element Distribution and Local Segmental Dynamics from Molecular Dynamics Simulations

Polymers are attractive membrane materials owing to their mechanical robustness and relatively inexpensive fabrication. An important indicator of membrane performance are free volume elements (FVE): microporous void spaces created by the inefficient packing of bulky groups along the polymer chain. FVEs tend to degrade over time, as polymer chains reorganize irreversibly. While it is widely accepted that polymer flexibility has an impact on membrane transport properties, the molecular nature of this impact is still not well understood. By the establishment of a correlation between local chain dynamics and the distribution of free volume elements (FVEs), penetrant transport can be regulated more efficiently in amorphous polymer membranes. In this work, we implement all-atom molecular dynamics (MD) simulations to explore the relationship between chain dynamics and free volume in three polymers with different levels of backbone flexibility: polymethylpentene (PMP), polystyrene (PS), and HAB-6FDA thermally rearranged polymer (TRP). We construct these polymers at different temperatures and examine how temperature impacts the FVE distribution and segmental mobility. Our analysis shows that chain segments near FVEs have higher mobility compared with the atoms in the bulk; the extent of this difference increases with chain flexibility. Increasing the chain flexibility by increasing the temperature results in a broader FVE distribution. Rigid polymers such as TRP show the most robust FVE distribution and are not significantly affected by the temperature change. To capture penetrant diffusion through the polymer matrix, hydrogen is inserted and the diffusion is measured at different temperatures; hydrogen mobility is influenced by the FVE structure and overall mobility of polymer chains. Lastly, at low temperatures, hydrogen mobility is influenced by void distribution, while at high temperatures, polymer dynamics dictate hydrogen transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Discrete Adjoint Sensitivity Analysis of Hybrid Dynamical Systems With Switching [Discrete Adjoint Sensitivity Analysis of Hybrid Dynamical Systems]

Sensitivity analysis is an important tool for describing power system dynamic behavior in response to parameter variations. It is a central component in preventive and corrective control applications. The existing approaches for sensitivity calculations, namely, finite-difference and forward sensitivity analysis, require a computational effort that increases linearly with the number of sensitivity parameters. In this paper, we investigate, implement, and test a discrete adjoint sensitivity approach whose computational effort is effectively independent of the number of sensitivity parameters. The proposed approach is highly efficient for calculating sensitivities of larger systems and is consistent, within machine precision, with the function whose sensitivity we are seeking. This is an essential feature for use in optimization applications. Moreover, our approach includes a consistent treatment of systems with switching, such as dc exciters, by deriving and implementing the adjoint jump conditions that arise from state-dependent and time-dependent switchings. The accuracy and the computational efficiency of the proposed approach are demonstrated in comparison with the forward sensitivity analysis approach. In conclusion, this paper focuses primarily on the power system dynamics, but the approach is general and can be applied to hybrid dynamical systems in a broader range of fields.

42 ENGINEERING↗

DOE OSTI2023

Beam Dynamics Challenges in the Muon g-2 Experiment

The muon&s;s anomalous magnetic moment $a_{\mu}$ has hinted at physics beyond the standard model for nearly 20 years. The Muon $g-2$ experiment at Fermilab aims to measure $a_{\mu}$ to 140 parts per billion (ppb) precision. The 460 ppb result from its first data run (Run-1), released in 2021, agreed with the previous 2006 Brookhaven Muon $g-2$ result. The experimental average stands in tension with the standard model theory $a_{\mu}$ prediction by $4.2 \sigma$. The result of Run-2/3 data analysis is set be released in summer 2023, and will improve on the Run-1 precision by a factor of two. With the data collected in all six runs, the experiment is on track to produce a 140 ppb measurement of $a_{\mu}$. If the experiment and theory central values are both unchanged, the tension would exceed $5 \sigma$. The measurement is accomplished by injecting muons into a magnetic storage ring and precisely measuring two observable frequencies: $\omega_a$, the muons&s; anomalous precession frequency, and $\tilde{\omega}&s;_p$, the precession frequency of protons which determines the magnetic field strength experienced by the muons. This thesis presents a selection of muon beam dynamics effects which are critical for reaching the experiment precision goal. A system of detectors assists with the challenging beam injection into the storage ring, and a measurement of the injected beam provides input for simulating the stored beam dynamics. A new method is introduced to reduce a critical systemic caused by time dependence in the stored beam momentum, enabled by a detector which directly profiles the stored beam. Finally the analysis of $\tilde{\omega}&s;_p$, the muon-weighted magnetic field, for the Run-2/3 result is presented. Systematics of $\tilde{\omega}&s;_p$ due to beam effects are evaluated in detail, and shown to be sub-dominant.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2020

Toward large-scale simulation of residual stress and distortion in wire and arc additive manufacturing

In this study, we aim to advance the structural analysis of wire and arc additive manufacturing (WAAM) by considering the thermomechanical features inherent in direct energy deposition. Simulation approaches including the iterative substructure method (ISM), dynamic mesh refining method (DMRM), and graphics processing unit (GPU) based explicit finite element method (FEM) were developed for accelerating additive manufacturing stress analysis that is very time consuming by conventional numerical methods. ISM and DMRM take advantage of the strong nonlinearity phenomenon near the moving heat source by reducing the global iterations and refining the local mesh, respectively. In addition to the use of GPUs, the explicit FEM is accelerated by a time scaling technique based on the inherent strain concept. The residual stress and distortion of two large builds were analyzed, showing very consistent numerical results and good agreement with experiments. Compared with the commercial software Abaqus, the novel approaches reduced the computational cost substantially without compromising accuracy. The GPU code showed the highest computational efficiency (30~70×), while DMRM and ISM had acceleration factors of 9× and 3×, respectively. Finally, such high-fidelity modeling approaches will be very useful for building up a digital twin of WAAM to reduce development time and cost.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Topological Effects in Isolated Poly[ n ]catenanes: Molecular Dynamics Simulations and Rouse Mode Analysis

Poly[n]catenanes are mechanically interlocked polymers consisting of interlocking ring molecules. We report that over the years, researchers have speculated that the permanent topological interactions within the poly[n]catenane backbone could lead to unique dynamical behaviors. To investigate these unusual polymers, molecular dynamics simulations of isolated poly[n]catenanes have been conducted, along with a Rouse mode analysis. Owing to the mechanical bonds within the molecule, the dynamics of poly[n]catenanes at short length scales are significantly slowed and the distribution of relaxation times is broadened; these same behaviors have been observed in melts of linear polymers and are associated with entanglement. Lastly, despite these entanglement-like effects, at large length scales poly[n]catenanes do not relax much slower than isolated linear polymers and are less strongly impacted by increased segmental stiffness.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Pursuing Heteroleptic Ligand Design Principles for Photoactive Fe Complexes with Ultrafast X-ray Emission and Variable-Temperature Optical Spectroscopies

Understanding the key parameters that govern the photophysical and photochemical properties of transition metal complexes is essential for the development of efficient photosensitizers for photocatalytic applications. Achieving this objective necessitates clear and detailed investigations of their electronic excited states, for which time-resolved metal Kβ X-ray emission spectroscopy (XES) has proven highly effective. Here, we present a time-resolved Fe Kβ XES study of a heteroleptic Fe(II) polypyridyl carbene complex, [Fe(phen) 2 (C 4 H 10 N 4 )] 2+ (1; phen = 1,10-phenanthroline), utilizing both the valence-to-core and Kβ mainline spectral regions, complemented by variable-temperature transient optical absorption (VT-TA) spectroscopy. Detailed analysis of the time-resolved Kβ XES data, supported by density functional theory (DFT) calculations and an Eyring analysis of the VT-TA data, reveals parallel excited state relaxation dynamics that support an assignment of the long-lived excited state to a triplet metal-centered state. Placing these results in the context of prior studies of heteroleptic Fe(II) polypyridyl cyanide complexes motivated a series of DFT calculations to investigate the effects of ligand structural flexibility and arrangement. These calculations reinforce the experimentally derived conclusion that constraining structural flexibility with multidentate ligands significantly impacts the excited state relaxation dynamics. Furthermore, our study emphasizes that the arrangement of strong field ligands in heteroleptic complexes substantially affects the energy of Jahn–Teller active triplet metal-centered states in low-spin d 6 metal complexes. Together, these findings provide synthetic design principles for extending metal-to-ligand charge transfer excited state lifetimes of heteroleptic Fe complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Intercomparison of phenological transition dates derived from the PhenoCam Dataset V1.0 and MODIS satellite remote sensing

Phenology is a valuable diagnostic of ecosystem health, and has applications to environmental monitoring and management. Here, we conduct an intercomparison analysis using phenological transition dates derived from near-surface PhenoCam imagery and MODIS satellite remote sensing. We used approximately 600 site-years of data, from 128 camera sites covering a wide range of vegetation types and climate zones. During both “greenness rising” and “greenness falling” transition phases, we found generally good agreement between PhenoCam and MODIS transition dates for agricultural, deciduous forest, and grassland sites, provided that the vegetation in the camera field of view was representative of the broader landscape. The correlation between PhenoCam and MODIS transition dates was poor for evergreen forest sites. We discuss potential reasons (including sub-pixel spatial heterogeneity, flexibility of the transition date extraction method, vegetation index sensitivity in evergreen systems, and PhenoCam geolocation uncertainty) for varying agreement between time series of vegetation indices derived from PhenoCam and MODIS imagery. This analysis increases our confidence in the ability of satellite remote sensing to accurately characterize seasonal dynamics in a range of ecosystems, and provides a basis for interpreting those dynamics in the context of tangible phenological changes occurring on the ground.

47 OTHER INSTRUMENTATION↗

DOE OSTI2019

High-order two-fluid plasma solver for direct numerical simulations of plasma flows with full transport phenomena

The two-fluid plasma equations for a single ion species, with full transport terms, including temperature and magnetic field dependent ion and electron viscous stresses and heat fluxes, frictional drag force, and ohmic heating terms, have been implemented in the CFDNS code and solved by using sixth-order non-dissipative compact finite differences for plasma flows in several different regimes. In order to be able to fully resolve all the dynamically relevant time and length scales, while maintaining computational feasibility, the assumptions of infinite speed of light and negligible electron inertia have been made. Non-dimensional analysis of the two-fluid plasma equations shows that, by varying the characteristic/background number density, length scale, temperature, and magnetic strength, the corresponding Hall, resistive, and ideal magnetohydrodynamic equations can be recovered as limiting cases. The accuracy and robustness of this two-fluid plasma solver in handling plasma flows in different regimes have been validated against four canonical problems: Alfven and whistler dispersion relations, electromagnetic plasma shock, and magnetic reconnection. For all test cases, by using physical dissipation and diffusion, with negligible numerical dissipation/diffusion, fully converged Direct Numerical Simulation (DNS)-like solutions are obtained when the ion Reynolds number based on the grid size is smaller than a threshold value which is about 2.3. For the magnetic reconnection problem, the results show that the magnetic flux saturation time and value converge when the ion and magnetic Reynolds numbers are large enough. Thus, the DNS-like results become relevant to practical problems with much larger Reynolds numbers.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS1972

Time and temperature dependent modulus of pyrrone and polyimide moldings

A method is presented by which the modulus obtained from a stress relaxation test can be used to estimate the modulus which would be obtained from a sonic vibration test. The method was applied to stress relaxation, sonic vibration, and high speed stress-strain data which was obtained on a flexible epoxy. The modulus as measured by the three test methods was identical for identical test times, and a change of test temperature was equivalent to a shift in the logarithmic time scale. An estimate was then made of the dynamic modulus of moldings of two Pyrrones and two polyimides, using stress relaxation data and the method of analysis which was developed for the epoxy. Over the common temperature range (350 to 500 K) in which data from both types of tests were available, the estimated dynamic modulus value differed by only a few percent from the measured value. As a result, it is concluded that, over the 500 to 700 K temperature range, the estimated dynamic modulus values are accurate.

Lander, L. L.↗

NASA NTRS1972

On the determination of optimal costly measurement strategies for linear stochastic systems.

This paper presents the formulation of a class of optimization problems dealing with selecting, at each instant of time, one measurement provided by one out of many sensors. Each measurement has an associated measurement cost. The basic problem is then to select an optimal measurement policy, during a specified observation time interval, so that a weighted combination of prediction accuracy and accumulated observation cost is optimized. The current analysis is limited to the class of linear stochastic dynamic systems and measurement subsystems. The problem of selecting the optimal measurement strategy can be transformed into a deterministic optimal control problem. It is shown that the optimal measurement policy and the associated matched Kalman-type filter can be precomputed.

Athans, M.↗

NASA NTRS1971

Numerical solution of stiff systems of ordinary differential equations with applications to electronic circuits

Systems of ordinary differential equations in which the magnitudes of the eigenvalues (or time constants) vary greatly are commonly called stiff. Such systems of equations arise in nuclear reactor kinetics, the flow of chemically reacting gas, dynamics, control theory, circuit analysis and other fields. The research reported develops an A-stable numerical integration technique for solving stiff systems of ordinary differential equations. The method, which is called the generalized trapezoidal rule, is a modification of the trapezoidal rule. However, the method is computationally more efficient than the trapezoidal rule when the solution of the almost-discontinuous segments is being calculated.

Rosenbaum, J. S.↗

NASA NTRS1987

Issues in modeling and controlling the SCOLE configuration

The parametric study of the in-plane Spacecraft Control Laboratory Experiment (SCOLE) system, the Floquet Stability Analysis, and three dimensional formulations of the SCOLE system dynamics are examined. Control issues are discussed, such as: control of large structures with delayed input in continuous time; control with delayed input in discrete time; control law design for SCOLE using Linear Quadratic Gaussian (LQC)/TRR technique; and optimal torque control for SCOLE slewing maneuvers.

Bainum, Peter M.↗

NASA NTRS1989

On damping mechanisms in beams

A partial differential equation model of a cantilevered beam with a tip mass at its free end is used to study damping in a composite. Four separate damping mechanisms consisting of air damping, strain rate damping, spatial hysteresis and time hysteresis are considered experimentally. Dynamic tests were performed to produce time histories. The time history data is then used along with an approximate model to form a sequence of least squares problems. The solution of the least squares problem yields the estimated damping coefficients. The resulting experimentally determined analytical model is compared with the time histories via numerical simulation of the dynamic response. The procedure suggested here is compared with a standard modal damping ratio model commonly used in experimental modal analysis.

Banks, H. T.↗

NASA NTRS1991

Large Angle Transient Dynamics (LATDYN) user's manual

A computer code for modeling the large angle transient dynamics (LATDYN) of structures was developed to investigate techniques for analyzing flexible deformation and control/structure interaction problems associated with large angular motions of spacecraft. This type of analysis is beyond the routine capability of conventional analytical tools without simplifying assumptions. In some instances, the motion may be sufficiently slow and the spacecraft (or component) sufficiently rigid to simplify analyses of dynamics and controls by making pseudo-static and/or rigid body assumptions. The LATDYN introduces a new approach to the problem by combining finite element structural analysis, multi-body dynamics, and control system analysis in a single tool. It includes a type of finite element that can deform and rotate through large angles at the same time, and which can be connected to other finite elements either rigidly or through mechanical joints. The LATDYN also provides symbolic capabilities for modeling control systems which are interfaced directly with the finite element structural model. Thus, the nonlinear equations representing the structural model are integrated along with the equations representing sensors, processing, and controls as a coupled system.

Abrahamson, A. Louis↗

NASA NTRS1990

Visualization of fluid dynamics at NASA Ames

Some of the hardware and software tools and techniques in use at NASA's numerical aerodynamic simulation facility for the analysis of computational fluid dynamics are described. The visualization process can be illustrated by video tapes and stereo pictures. Although these visualization tools have dramatically improved the ability to conduct research in fluid dynamics, a comparison of the current environment for analysis with an 'ideal' environment illustrates that there are still major improvements that should be made. The most time-consuming task in future analyses of the increasingly complex computer simulations will be the extraction and clear display of the key features. In addition, the interface between the workstation and the scientist should be improved significantly. Current research on techniques for creating these improvements is described.

Watson, V.↗

NASA NTRS1991

On damping mechanisms in beams

Banks, H. T.↗

NASA NTRS1992

New literal approximations for the longitudinal dynamic characteristics of flexible flight vehicles

The goal of the literal approximation method is to obtain simple literal (analytical) approximations for key dynamic characteristics of flexible flight vehicles. A basic question regarding the method is its usefulness as an additional design tool for existing design and simulation procedures. Two aspects of this question are: (1) ease of derivation and use of the literal approximations, and (2) the suitability of one set of literal approximations to describe the dynamics of a large set of significantly different vehicles. These issues are addressed by incorporating symbolic manipulation software into the literal approximation method for the analysis of a fifth order model of the longitudinal dynamics of a flexible flight vehicle. The automated literal approximation generated in this fashion reduces the manual derivation time by an approximate factor of four. A single set of literal approximations is shown to provide adequate approximations for the dynamics of significantly different flight vehicles configurations, such as an aircraft, a missile, and a hypersonic vehicle.

Livneh, Rafael↗

NASA NTRS1994

Multi-dimensional combustor flowfield analyses in gas-gas rocket engine

The objectives of the present research are to improve design capabilities for low thrust rocket engines through understanding of the detailed mixing and combustions processes. Of particular interest is a small gaseous hydrogen-oxygen thruster which is considered as a coordinated part of an on-going experimental program at NASA LeRC. Detailed computational modeling requires the application of the full three-dimensional Navier Stokes equations, coupled with species diffusion equations. The numerical procedure is performed on both time-marching and time-accurate algorithms and using an LU approximate factorization in time, flux split upwinding differencing in space. The emphasis in this paper is focused on using numerical analysis to understand detailed combustor flowfields, including the shear layer dynamics created between fuel film cooling and the core gas in the vicinity on the nearby combustor wall; the integrity and effectiveness of the coolant film; three-dimensional fuel jets injection/mixing/combustion characteristics; and their impacts on global engine performance.

Tsuei, Hsin-Hua↗