A Partitioned Method for Reduced OrderModel-Finite Element Model (ROM-FEM)and ROM-ROM Couplings with SeparateReduced Bases for Interior and InterfaceVariables
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de Castro, Amy Grace↗
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Beyond Magic Barrels: Digital manufacturing for crystallization, process development and optimization of explosive materials: Part II Resveratrol Exemplar
This SAND report summarizes work supported by an Engineering Sciences Research Foundation (ESRF) Lab Directed Research and Development (LDRD) project entitled “Beyond Magic Barrels: Digital manufacturing for crystallization, process development and optimization of explosive materials.” This SAND report is written in two parts with Part 1 discusses recrystallization of our explosive exemplar and Part 2 summarizing our work with recrystallization of resveratrol. We have studied resveratrol recrystallization with a multiscale approach combining experiments, modeling and simulation. At the single crystal scale, microscopy experiments illuminate crystal time-dependent growth rates using advanced image analysis. Bench scale experiments were carried out to look at growth of multiple particles in a small reactor creating thousands of particles and analyzing the results with microscopy and μCT. For the modeling we combine kinetic Monte Carlo (kMC) models with subscale information from density functional theory (DFT) or molecular dynamics. This work is discussed in Part 1 and can also be found in a paper from the project discussing a coarse-grained kMC model specifically developed for resveratrol. For well-mixed systems, we have population balance equations (PBE) linked with species mass conservation forming a set of ordinary differential equations that can be solved quickly. For more complicated geometries, such as the vat crystallization used throughout the complex, a coupled computational fluid dynamic (CFD)/PBE method was developed to account for gradients in temperature and concentration and differences in crystallization rates throughout the domain. These simulations are more complex and require high performance computing. We present results for two cases: 5% seed fast cool with parameters fit to the well-mixed case and 5% seed slow cool using the same parameters. We show reasonable agreement with experiments though are particles are significantly larger than the experiments.
36 MATERIALS SCIENCE↗
Symmetry Breaking in an Extended-O(2) Model
Motivated by attempts to quantum simulate lattice models with continuous Abelian symmetries using discrete approximations, we consider an extended-O(2) model that differs from the ordinary O(2) model by an explicit symmetry breaking term. Its coupling allows to smoothly interpolate between the O(2) model (zero coupling) and a $q$-state clock model (infinite coupling). In the latter case, a $q$-state clock model can also be defined for non-integer values of $q$. Thus, such a limit can also be considered as an analytic continuation of an ordinary $q$-state clock model to non-integer $q$. The phase diagram of the extended-O(2) model in the infinite coupling limit was established in our previous work, where it was shown that for non-integer $q$, there is a second-order phase transition at low temperature and a crossover at high temperature. In this work, we investigate the model at finite values of the coupling using Monte Carlo and tensor methods. The results may be relevant for configurable Rydberg-atom arrays.
Hostetler, Leon↗
Studying electroweak few-body observables in chiral effective field theory
The use of nuclei to study electroweak probes is becoming increasingly relevant experimentally. The success of dark matter and neutrino experiments strongly depends on the ability to control nuclear effects in order to extract the fundamental parameters associated with external probes. Therefore, reliable theoretical calculations of nuclear structure and reactions, with well-controlled errors, are crucial for the success of experimental efforts. Currently, chiral effective field theory ($\chi$EFT) coupled with {\it ab-initio} methods represents one of the best approaches that fulfills these requirements. To use this approach as a tool for studying fundamental physics, it is essential to validate it against experimental data for which the calculations are well under control, such as the elastic scattering of electrons on nuclei. In this proceeding, I will present recent developments in the fitting of electromagnetic currents derived using $\chi$EFT and the calculation of electromagnetic form factors of light nuclei. The results of these calculations demonstrate the strength of the theory in describing the interaction of nuclei with electromagnetic probes over a broad range of momentum transfers and highlight the robustness of $\chi$EFT for analyzing future experimental data aimed at extracting fundamental parameters.
Gnech, Alex [Old Dominion Univ., Norfolk, VA (Unit↗
A Scaling Study for Incompressible Multispecies Solver in Vertex-CFD
Multispecies incompressible flows occur widely in engineering and environmental applications, such as chemical reactors, fuel cells, ocean mixing, and biomedical systems. However, accurately resolving the complex transport and mixing phenomena associated with multiple interacting species remains computationally challenging, especially for large-scale problems. In this study, we present a robust, high-performance computing--enabled multispecies incompressible Navier–Stokes solver integrated within the Vertex-CFD framework. Our solver employs a fully coupled, implicit, finite element--based formulation that accurately captures the advection, diffusion, and interaction of multiple species in incompressible flows by leveraging the Kokkos library for parallel computing to achieve high computational efficiency. For pressure coupling, the entropically damped artificial compressibility method is utilized. We validated the solver against canonical test cases, including multispecies advection, diffusion, and Bateman systems; the results demonstrate second- and third-order spatial accuracy and consistent convergence. Additionally, we demonstrated the strong and weak scaling study results obtained on the leadership-class high-performance computing system, Frontier at Oak Ridge National Laboratory.
Oz, Furkan [ORNL] (ORCID:0000000265831724)↗
Multibody for Everybody (M4E): A Symbolic Dynamics Modeling Tool with Applications in Simulation, Control, and Optimization
Developing the analytical model of a multibody system is often the initial step in control and optimization. The analytical model (equations of motion) describes a system’s time evolution under specified forcing conditions. Although developing these equations is easy for simple systems, this process becomes more complex for systems composed of multiple bodies. Deriving equations of motion for complex multibody systems requires specialized expertise in multibody dynamics, is time-consuming, and is susceptible to error. To address this issue, this paper presents an open-source, easy-to-use, systematic framework to derive symbolic equations of motion in both Python and MATLAB using the joint coordinate formulation. This formulation results in a set of ordinary differential equations that use the minimum set of coordinates needed to model a system. The symbolic representation provides better insight into the influence of design parameters on system performance, facilitates sensitivity analysis and parameter studies, and supports direct implementation of control and optimization routines. The tool enables numerical simulation for specified parameter sets, is modular for straightforward integration with other tools and libraries, and allows incorporation of hydrodynamics, mooring, and other external forces. The result is a reproducible, extensible pipeline for modeling, simulation, and design of complex multibody systems. The proposed tool is versatile and can be applied to domains such as robotics, control, and design. In addition, we integrated external libraries that provide capabilities for modeling offshore systems such as underwater robots and marine energy converters.
16 TIDAL AND WAVE POWER↗
Mathematical Tools for the Analysis of Periodic and Aperiodic Grid Signals
Numerous sensing techniques and instrumentation are used in determining the state of the electric grid. Coupled with such measurements are the methods and analysis tools used. The parameters of interest result in both periodic and aperiodic signals. An examination of appropriate analysis tools is presented
97 MATHEMATICS AND COMPUTING↗
GEAR-MC and Differential-Operator Methods Applied to Electron-Photon Transport in the Integrated TIGER Series
The sensitivity analysis algorithms that have been developed by the radiation transport community in multiple neutron transport codes, such as MCNP and SCALE, are extensively used by fields such as the nuclear criticality community. However, these techniques have seldom been considered for electron transport applications. In the past, the differential-operator method with the single scatter capability has been implemented in Sandia National Laboratories’ Integrated TIGER Series (ITS) coupled electron-photon transport code. This work is meant to extend the available sensitivity estimation techniques in ITS by implementing an adjoint-based sensitivity method, GEAR-MC, to strengthen its sensitivity analysis capabilities. To ensure the accuracy of this method being extended to coupled electron-photon transport, it is compared against the central-difference and differential-operator methodologies to estimate sensitivity coefficients for an experiment performed by McLaughlin and Hussman. Energy deposition sensitivities were calculated using all three methods, and the comparison between them has provided confidence in the accuracy of the newly implemented method. Unlike the current implementation of the differential-operator method in ITS, the GEAR-MC method was implemented with the option to calculate the energy-dependent energy deposition sensitivities, which are the sensitivity coefficients for energy deposition tallies to energy-dependent cross sections. The energy-dependent cross sections could be the cross sections for the material, elements in the material, or reactions of interest for the element. Further, these sensitivities were compared to the energy-integrated sensitivity coefficients and exhibited a maximum percentage difference of 2.15%.
42 ENGINEERING↗
Nanoporous weakly coordinating anionic frameworks (Final Technical Report)
Under this award, we synthesized and characterized new weakly coordinating, anionic covalent organic frameworks. The motivation was to expand the class of covalent organic frameworks though the introduction of the first weakly coordinating anionic ones. The significance of the weakly coordinating anionic character of these frameworks is associated with the character of the counter (metal) cations in their pores. Those counter-cations, due to the inability to effectively coordinate to the pore walls, have a “naked”, and thus highly electrophilic, Lewis acidic character. Such properties are expected to translate to a number of interesting physical properties that can be potentially used for a range of energy-relevant applications. One of these applications is gas adsorption, separation, and storage. The electrophilic, Lewis acidic character of the counter-cations are expected to strongly bind to gas molecules entering the pores leading to higher gas sorption capacities. Other applications include heterogeneous catalysis, ion exchange, and solid state ion conduction. Within the project we explored a range of chemical blocks, and tested synthesis conditions to polymerize these building blocks to form the target materials. In particular, we focused on materials with group 15 elements like phosphorus in the oxidation state +5 and the coordination number 6, that have a formal -1 charge. The synthesis of such materials is challenging because its success depends on the absence of residual monomeric and oligomeric side-products in the pores, and the absence of significant framework interpenetration. Crystalline forms of these materials require sufficient reversibility of the polymerization reaction (which is difficult to achieve because group 15 elements like P tend to make strong covalent bonds with neighbored elements), as well as suitable polymerization rates that prevent the formation of kinetically controlled products. We had success with the preparation of anionic porous organic frameworks with anionic building blocks containing P(V)O6 octahedra synthesized through Yamamoto coupling reactions. These materials are non-crystalline because of the irreversible nature of the Yamamoto coupling reaction, but show porosity. The porosity and surface area can be significantly increased by co-reaction with electrostatically neutral co-reactants. Very high porosity and surface areas can be achieved when the materials are washed with hydrochloric acid. This method is commonly used to free products from Yamamoto coupling reactions from by-products. Indeed, this method removed by products from the pores of our materials, however it also led to the hydrolysis of the PO6 octahedra to form pending phosphonic acid groups (-PO3H)-groups in the frameworks (PA-POFs) which was actually not desired. Nonetheless, these materials showed high CO2 sorption capacities. In addition, they show extremely high (actually record) sorption capacities for the removal of a range of common micropollutants such as bisphenol A (BPA) and 4-nitrophenol in water. BPA is a wide-spread organic pollutant and a known endocrine disruptor. The maximum adsorption capacity of BPA at equilibrium is found to be as high as 3,366 mg g-1 by Langmuir adsorption model, which is more than 10 times greater than peer materials. The polymer also rapidly removes various other organic micropollutants with more than 90% removal efficiencies. In addition, the PA-POF material can be regenerated at least five times by mild washing using methanol without significant loss in removal efficiency. This is significant advantage over commonly used activated carbon materials (that are in Brita water faucet filters, for example). Comparison studies showed that only materials with the phosphonate groups show extreme sorption although the number of PA group is actually small according to solid state NMR and EDX data. More research would be needed to investigate why this is (a possibility is that the phosphonate groups have a multiplying effect in which a PA-induced initial adsorption leads to the adsorption of much more adsorbate). The extreme sorption capabilities can also be visually seen when colored adsorbates such as 4-nitrophenol are used, as the adsorption of the nitrobenzene leads to the decoloration of the solution. We have produced three short videos that illustrate the sorption capabilities compared to two peer materials (activated carbon from dismantled Brita water filters, and a electrostatically neutral, chemically related, porous organic polymer, respectively).
36 MATERIALS SCIENCE↗
A fourth order sharp immersed method for the incompressible Navier-Stokes equations with stationary and moving boundaries and interfaces
We propose a fourth order Navier-Stokes solver based on the immersed interface method (IIM), for flow problems with stationary and one-way coupled moving boundaries and interfaces. Our algorithm employs a Runge-Kutta-based projection method that maintains high-order temporal accuracy in both velocity and pressure for steady and unsteady velocity boundary conditions. Fourth order spatial accuracy is achieved through a novel fifth order IIM discretization scheme for the advection term, as well as existing high-order interface-corrected finite difference schemes for the other differential operators. Using a set of manufactured flow problems with stationary and moving boundaries, we demonstrate fourth order convergence of velocity and pressure in the infinity norm, both inside the domain and on the immersed boundaries. The solver’s performance is further validated through a range of practical flow simulations, highlighting its efficiency over a second order scheme. Finally, we showcase the ability of our immersed discretization scheme to handle interface-coupled multiphysics problems by solving a conjugate heat transfer problem with multiple immersed solids. Overall, the proposed approach robustly combines the efficiency of high order discretization schemes with the flexibility of immersed discretizations for flow problems with complex, moving boundaries and interfaces.
42 ENGINEERING↗
Unitary coupled-cluster based self-consistent polarization propagator theory: A quadratic unitary coupled-cluster singles and doubles scheme
The development of a quadratic unitary coupled-cluster singles and doubles (qUCCSD) based self-consistent polarization propagator method is reported here. We present a simple strategy for truncating the commutator expansion of the unitary version of coupled-cluster transformed Hamiltonian $\bar{H}$. The qUCCSD method for the electronic ground state includes up to double commutators for the amplitude equations and up to cubic commutators for the energy expression. The qUCCSD excited-state eigenvalue equations include up to double commutators for the singles–singles block of $\bar{H}$, single commutators for the singles–doubles and doubles–singles blocks, and the bare Hamiltonian for the doubles–doubles block. Benchmark qUCCSD calculations of the ground-state properties and excitation energies for representative molecules demonstrate significant improvement of the accuracy and robustness over the previous UCC3 scheme derived using Møller–Plesset perturbation theory.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Nuclear-Electronic Orbital Ehrenfest Dynamics
The recently developed real-time nuclear-electronic orbital (RT-NEO) approach provides an elegant framework for treating electrons and selected nuclei, typically pro- tons, quantum mechanically in nonequilibrium dynamical processes. However, the RT-NEO approach neglects the motion of the other nuclei, preventing a complete de- scription of the coupled nuclear-electronic dynamics and spectroscopy. In this work, we describe the dynamical interaction between the other nuclei and the electron-proton subsystem with the mixed quantum-classical Ehrenfest dynamics method. The NEO- Ehrenfest approach propagates the electrons and quantum protons in a time-dependent variational framework, while the remaining nuclei move classically on the correspond- ing average electron-proton vibronic surface. This approach includes the non-Born- Oppenheimer eects between the electrons and quantum protons with RT-NEO and between the classical nuclei and the electron-proton subsystem with Ehrenfest dynam- ics. Spectral features for vibrational modes involving both quantum and classical nuclei are resolved from the time-dependent dipole moments. Moreover, nuclear quantum ef- fects are included directly in nonadiabatic dynamics simulations. The excited state intramolecular proton transfer in the o-hydroxybenzaldehyde molecule is shown to be faster and to exhibit a larger kinetic isotope eect with NEO-Ehrenfest compared to classical Ehrenfest dynamics. This work shows that the NEO-Ehrenfest method is a powerful tool to study dynamical processes with coupled electronic and nuclear degrees of freedom.
Zhao, Luning↗
Coupled Cluster Theory for Nonadiabatic Dynamics: Nuclear Gradients and Nonadiabatic Couplings in Similarity Constrained Coupled Cluster Theory
Coupled cluster theory is one of the most accurate electronic structure methods for predicting ground and excited state chemistry. However, the presence of numerical artifacts at electronic degeneracies, such as complex energies, has made it difficult to apply the method in nonadiabatic dynamics simulations. While it has already been shown that such numerical artifacts can be fully removed by using similarity constrained coupled cluster (SCC) theory [J. Phys. Chem. Lett. 2017, 8(19), 4801–4807], simulating dynamics requires efficient implementations of gradients and nonadiabatic couplings. Here, we present an implementation of nuclear gradients and nonadiabatic derivative couplings at the similarity constrained coupled cluster singles and doubles (SCCSD) level of theory, thereby making possible nonadiabatic dynamics simulations using a coupled cluster theory that provides a correct description of conical intersections between excited states. We present a few numerical examples that show good agreement with literature values and discuss some limitations of the method.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Synthesis of Sandwich-α-Diimine Ligands via Copper-Mediated Stille Coupling
While sandwich diimines have found use in transition metal catalysis, the general method for their preparation has been lacking. Here, this approach utilizes a copper-mediated Stille-type coupling between aryl stannanes and α-diimines bearing 8-bromonaphthylimino group in commercial-grade N,N-dimethylformamide solvent and employs CuI or thiophene-2-carboxylate to promote the reactions. No other additives or bases are required. Electron-poor, electron-rich, heterocyclic, and hindered aryl stannanes can be employed as coupling reagents. Ligand scaffolds derived from structurally diverse α-diketones can be used.
Catalysts↗
Experimental Quantification of Spin–Phonon Coupling in Molecular Qubits Using Inelastic Neutron Scattering
Electronic spin superposition states enable nanoscale sensing through their sensitivity to the local environment, yet their sensitivity to vibrational motion also limits their coherence times. In molecular spin systems, chemical tunability and atomicscale resolution are accompanied by a dense, thermally accessible phonon spectrum that introduces efficient spin relaxation pathways. Despite extensive theoretical work, there is little experimental consensus on which vibrational energies dominate spin relaxation or how molecular structure controls spin−phonon coupling (SPC). We present a fully experimental method to quantify SPC coefficients by combining temperature-dependent vibrational spectra from inelastic neutron scattering with spin relaxation rates measured by electron paramagnetic resonance. We apply this framework to two model S = 1/2 systems, copper(II) phthalocyanine (CuPc) and copper(II) octaethylporphyrin (CuOEP). Two distinct relaxation regimes emerge: below 40 K, weakly coupled lattice modes below 50 cm −1 dominate, whereas above 40 K, optical phonons above ∼185 cm −1 become thermally populated and drive relaxation with SPC coefficients nearly 3 orders of magnitude larger. Structural distortions in CuOEP that break planar symmetry soften the crystal lattice and enhance anharmonic scattering but also raise the energy of stretching modes at the molecular core where the spins reside. This redistributes vibrational energy toward the molecular periphery and out of plane, ultimately reducing SPC relative to CuPc and enabling room-temperature spin coherence in CuOEP. Although our method does not provide mode-specific SPC coefficients, it quantifies contributions from distinct spectral regions and establishes a broadly applicable, fully experimental link between crystal structure, lattice dynamics, and spin relaxation.
Lohaus, Stefan H. [California Institute of Technol↗
Using Ultrasonics to Optimize the Processing Parameters of Thermoset Polymers [Slides]
Ultrasonics is used as a non-destructive evaluation method to improve our understanding of polymers. Coupling ultrasonics and FTIR can help determine which bonds are more relevant to the mechanical properties of the polymer. Modeling the cure kinetics can determine if the curing process of a sample deviates from the baseline. Cure kinetics influence the final chemical structure of the polymer. This method opens a new pathway to design and adapt polymers for high demanding applications.
36 MATERIALS SCIENCE↗
Neutronics Calculation Advances at Los Alamos: Manhattan Project to Monte Carlo
The history and advances of neutronics calculations at Los Alamos during the Manhattan Project through the present are reviewed. Substantial improvements to neutron diffusion methods and the invention of both the Monte Carlo neutron transport methods in 1947 and deterministic discrete ordinates Sn in 1953 were all made at Los Alamos just after the Manhattan Project. We briefly summarize early simpler and more approximate neutronics methods and then describe the need to better predict neutronics behavior through consideration of theoretical equations, models and algorithms, experimental measurements, and available computing capabilities and their limitations. This paper briefly covers key advances in deterministic methods during the Manhattan Project. These capabilities, coupled with increasing postwar defense needs and the invention of electronic computing with the Electronic Numeric Integrator and Computer, known as ENIAC, and the Mathematical Analyzer Numerical Integrator and Automatic Computer Model, known as MANIAC, led to the creation of Monte Carlo and deterministic discrete ordinates neutronics transport methods. We note the important role that the scientific comradery between the Los Alamos scientists played in the process. This paper briefly covers the early methods, algorithms, computers, and electronic and women pioneers that enabled Monte Carlo to spread to all areas of science. We focus heavily on these early developments and the subsequent creation of the MCNP® code, advances in its associated nuclear data, and its applications to problems of national defense at Los Alamos.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Inverse Volume Scaling of Finite-Size Error in Periodic Coupled Cluster Theory
Coupled cluster theory is one of the most popular post-Hartree-Fock methods for molecular quantum chemistry. The finite-size error of the correlation energy in periodic coupled cluster calculations for three-dimensional insulating systems has been observed to satisfy the inverse volume scaling, even in the absence of any correction schemes. This is surprising, as simpler theories that utilize only a subset of the coupled cluster diagrams exhibit much slower decay of the finite-size error, which scales inversely with the length of the system. In this study, we review the current understanding of finite-size error in quantum chemistry methods for periodic systems. We introduce new tools that elucidate the mechanisms behind this phenomenon in the context of coupled cluster doubles calculations. This reconciles some seemingly paradoxical statements related to finite-size scaling. Our findings also show that singularity subtraction can be a powerful method to effectively reduce finite-size errors in practical quantum chemistry calculations for periodic systems. Published by the American Physical Society 2024
97 MATHEMATICS AND COMPUTING↗