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DOE OSTI2024

Adaptive finite differencing in high accuracy electronic structure calculations

Abstract A multi-order Adaptive Finite Differencing (AFD) method is developed for the kinetic energy operator in real-space, grid-based electronic structure codes. It uses atomic pseudo orbitals produced by the corresponding pseudopotential codes to optimize the standard finite difference (SFD) operators for improved precision. Results are presented for a variety of test systems and Bravais lattice types, including the well-known Δ test for 71 elements in the periodic table, the Mott insulator NiO, and borax decahydrate, which contains covalent, ionic, and hydrogen bonds. The tests show that an 8th-order AFD operator leads to the same average Δ value as that achieved by plane-wave codes and is typically far more accurate and has a much lower computational cost than a 12th-order SFD operator. The scalability of real-space electronic calculations is demonstrated for a 2016-atom NiO cell, for which the computational time decreases nearly linearly when scaled from 18 to 144 CPU-GPU nodes.

Briggs, E. L. (ORCID:0000000343983492)↗

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 OSTI2021

Fast and robust all-electron density functional theory calculations in solids using orthogonalized enriched finite elements

Here, we present a computationally efficient approach to perform systematically convergent real-space all-electron Kohn-Sham density functional theory calculations for solids using an enriched finite element (FE) basis. The enriched FE basis is constructed by augmenting the classical FE basis with atom-centered numerical basis functions, comprising of atomic solutions to the Kohn-Sham problem. Notably, to improve the conditioning, we orthogonalize the enrichment functions with respect to the classical FE basis, without sacrificing the locality of the resultant basis. In addition to improved conditioning, this orthogonalization procedure also renders the overlap matrix block diagonal, greatly simplifying its inversion. Subsequently, we use a Chebyshev polynomial based filtering technique to efficiently compute the occupied eigenspace in each self-consistent field iteration. We demonstrate the accuracy and efficiency of the proposed approach on periodic unit cells and supercells. The benchmark studies show a staggering 130× speedup of the orthogonalized enriched FE basis over the classical FE basis. We also present a comparison of the orthogonalized enriched FE basis with the linearized augmented plane-wave + local orbitals basis, both in terms of accuracy and efficiency. Notably, we demonstrate that the orthogonalized enriched FE basis can handle large system sizes of ~10 000 electrons. Finally, we observe good parallel scalability of our implementation with 92% efficiency at 22× speedup for a system with 620 electrons

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Oxidative Grafting for Catalyst Synthesis in Surface Organometallic Chemistry

The development of new methods of catalyst synthesis with the potential to generate active site structures orthogonal to those accessible by traditional protocols is of great importance for discovering new materials for addressing challenges in the evolving energy and chemical economy. Here, in this work, the generality of oxidative grafting of organometallic and well-defined molecular metal precursors onto redox-active surfaces such as manganese dioxide (MnO 2 ) and lithium manganese oxide (LiMn 2 O 4 ) is investigated. Nine molecular metal precursors are explored, spanning groups 4–11 and each of the three periods of the transition metal series. The byproducts of the oxidative grafting reaction, a mixture of protodemetalation and ligand homocoupling for several organometallic precursors, was found to provide insights into the mechanism of the grafting reaction, suggesting oxidation of both the metal d-orbitals, as well as the metal–carbon σ-bonds, resulting in ejection of the ligand radical fragment. Analysis of the supported structures and oxidation state by X-ray absorption spectroscopy (XAS) and X-ray photoelectron spectroscopy (XPS) suggests that several of the chemisorbed metal ions are intercalated into interstitial vacancies of the surface structure while other complexes form intact molecular fragments on the surface. Proof of concept for the use of this metalation protocol to generate diverse, metal-dependent catalytic performance is demonstrated by the application of these materials in the conversion of cyclohexane to K/A oil (cyclohexanol and cyclohexanone) with tert-butyl hydroperoxide, as well as in the low-temperature (T ≤ 50 °C) oxidation of carbon monoxide to carbon dioxide.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Best practices in catalysis: A perspective

Catalysis, from its roots in petrochemical refining and conversion, has emerged as a transdisciplinary field that now encompasses synthesis of materials and molecules that enable applications in energy conversion and storage, environmental remediation, medicine, plastics, and fertilizer production, among numerous others. A handful of disciplines can claim relevance and success over such an extended period of time and continue to claim a preeminent role in defining the state-of-the-art in science and technology. Syncretic and rapid advancements in formulation and spectroscopic characterization of materials and molecules useful as catalysts, high-level density functional and molecular orbital theory calculations, and a strong foundation in concepts of physical chemistry, thermodynamics, and chemical kinetics offer new and abundant opportunities at the present day for addressing the grand challenge of controlling chemical transformations using catalysis. Here, we examine what we have learned of concepts that underpin heterogeneous catalysis but more importantly, how we learned to archive our knowledge in context of a set of best practices and standards that have emerged in the course of our learnings—ones we seek to highlight herein. Our perspective emphasizes concepts in synthesis, characterization, kinetics, and theory, because these four elements combined enable description of molecular acts that happen on surfaces and how fast they occur. In revisiting best practices in heterogeneous catalysis in these sub-fields and in authorship and peer review we aspire to augment clarity, reproducibility, and rigor in the science and practice of catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

An over-approximation of entropy for elemental multiconfigurational ground state electronic structures

The ability to predict the chemical and physical properties of a material is directly related to the structure and interactions of its electrons. For materials comprised of f-block elements (the lanthanides and actinides found in the last two rows of the periodic table), the complexity of electronic structure has presented great difficulty in understanding, modeling, and predicting material properties. The complexity of multiconfigurational ground state electronic structures is illustrated herein by the combinatorics of electron permutations within individual and cumulative occupancy configurations. A non-integer orbital occupancy representation of multiconfigurational ground states is described for superposition mixing between multiple near-energy degenerate occupancy configurations and generalized in such a way that established ground states are returned by approximation for elements with less-complex electronic structures. By considering the occupancy configurations as statistical mechanics macrostates, and the permutations of electrons as statistical mechanics microstates within those macrostates, an over-approximation of entropy for multiconfigurational elemental ground state electronic structures has been calculated.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Chaotic and integrable magnetic fields in one-dimensional hybrid Vlasov–Maxwell equilibria

The construction of kinetic equilibrium states is important for studying stability and wave propagation in collisionless plasmas. Thus, many studies over the past decades have been focused on calculating Vlasov–Maxwell equilibria using analytical and numerical methods. However, the problem of kinetic equilibrium of hybrid models is less studied, and self-consistent treatments often adopt restrictive assumptions ruling out cases with irregular and chaotic behaviour, although such behaviour is observed in spacecraft observations of space plasmas. In this paper, we develop a one-dimensional (1-D), quasineutral, hybrid Vlasov–Maxwell equilibrium model with kinetic ions and massless fluid electrons and derive associated solutions. The model allows for an electrostatic potential that is expressed in terms of the vector potential components through the quasineutrality condition. The equilibrium states are calculated upon solving an inhomogeneous Beltrami equation that determines the magnetic field, where the inhomogeneous term is the current density of the kinetic ions and the homogeneous term represents the electron current density. We show that the corresponding 1-D system is Hamiltonian, with position playing the role of time, and its trajectories have a regular, periodic behaviour for ion distribution functions that are symmetric in the two conserved particle canonical momenta. For asymmetric distribution functions, the system is nonintegrable, resulting in irregular and chaotic behaviour of the fields. The electron current density can modify the magnetic field phase space structure, inducing orbit trapping and the organization of orbits into large islands of stability. Thus, the electron contribution can be responsible for the emergence of localized electric field structures that induce ion trapping. We also provide a paradigm for the analytical construction of hybrid equilibria using a rotating two-dimensional harmonic oscillator Hamiltonian, enabling the calculation of analytic magnetic fields and the construction of the corresponding distribution functions in terms of Hermite polynomials.

Kaltsas, Dimitrios A. (ORCID:0000000300769015)↗

DOE OSTI2024

Real-Space Pseudopotential Method for the Calculation of Third-Row Elements X-ray Photoelectron Spectroscopic Signatures

X-ray photoelectron spectroscopy (XPS) is a powerful characterization technique that unveils subtle chemical environment differences via core– electron binding energy (CEBE) analysis. We extend the development of realspace pseudopotential methods to calculating 1s, 2s, and 2p 3/2 CEBEs of third-row elements (S, P, and Si) within the framework of Kohn–Sham density-functional theory (KS-DFT). The new approach systematically prevents variational collapse and simplifies core-excited orbital selection within dense energy level distributions. However, careful error cancellation analysis is required to achieve accuracy comparable to all-electron methods and experiments. Combined with real-space KS-DFT implementation, this development enables large-scale simulations with both Dirichlet boundary conditions and periodic boundary conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Correlation matrix renormalization theory in multi-band lattice systems

An appropriate treatment of electronic correlation effects plays an important role in accurate descriptions of physical and chemical properties of real materials. The recently proposed correlation matrix renormalization theory with sum rule correction (CMR) for studying correlated-electron materials has shown good performance in molecular systems and a periodic hydrogen chain in comparison with various quantum chemistry and quantum Monte Carlo calculations. Additionally, this work gives a detailed formulation and computational code implementation of CMR in multi-band periodic lattice systems. This lattice CMR ab initio theory is highly efficient, has no material specific adjustable parameters, and has no double counting issues faced by the hybrid approaches like LDA + U, DFT + DMFT and DFT + GA type theories. Benchmark studies on materials with s and p orbitals in this study show that CMR in its current implementation consistently performs well for these systems as the electron correlation increases from the bonding region to the bond breaking region.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

CEBAF 22 GeV FFA energy upgrade

Extending the energy reach of CEBAF by increasing the number of recirculations, while using the existing linacs is explored. This energy upgrade is based on the multi-pass acceleration of electrons in a single non-scaling Fixed Field Alternating Gradient (FFA) beam line, using Halbach-style permanent magnets. Encouraged by the recent successful demonstration of CBETA, a proposal was formulated to nearly double the energy of CEBAF from 12 to 22~GeV by replacing the highest energy arcs with FFA transport. The new FFA arcs would support simultaneous transport of an additional 6 passes spanning roughly a factor of two in energy. One of the challenges of the multi-pass (11) linac optics is to assure uniform focusing over a wide range of energies. Here, we propose a triplet lattice that provides a stable periodic solution covering an energy ratio of 1:33. The current CEBAF injection at 123 MeV, makes optical matching in the first linac impossible due to the extremely high energy ratio (1:175). Replacement of the current injector with a 650 MeV recirculating injector will alleviate this issue. Orbital and optical matching from the FFA arcs to the linacs is implemented as a compact non-adiabatic insert. The design presented here is anticipated to deliver a 22 GeV beam with normalized emittance of 76 mm·mrad and a relative energy spread of 1×10\textsuperscript{-3}. Further recirculation beyond 22 GeV is limited by the large (974 MeV per electron) energy loss due to synchrotron radiation.

Benesch, J.↗

DOE OSTI2023

CEBAF 22 GeV FFA energy upgrade

Benesch, J.↗

DOE OSTI2023

Status of CEBAF Upgrades

Extending CEBAF energy reach by increasing the number of recirculations, while using the existing SRF system is being explored. Proposed energy upgrade is based on a new approach to multi-pass acceleration of electrons in a single Fixed Field Alternating Gradient (FFA) beam line, configured with Halbach-style permanent magnets. Encouraged by recent success of CBETA, a proposal was formulated to nearly ?double? CEBAF energy by replacing the highest energy arcs with a pair of FFA arcs. The new non-scaling FFA arcs would support simultaneous transport of additional 6 passes with energies spanning a factor of two. One of the challenges of the multi-pass (11) linac optics is to assure uniform focusing in a vast range of energies, in a fixed field lattice. Here, we propose a triplet lattice that would provide a stable periodic solution covering energy ratio of 1:33. The current CEBAF injection at 123 MeV, makes optical matching in the first linac virtually impossible due to extremely high energy span ratio (1:175). Replacement of the current injector with a 650 MeV recirculating injector will alleviate that problem. Orbital and optical matching from the FFA arcs to the linacs is implemented as a compact non-adiabatic insert. Presented scheme would promise to deliver a 22 GeV beam with normalized emittance of 76 mm·mrad and with a relative energy spread of 1×10-3. Further recirculation beyond 22 GeV is limited by large, 974 MeV per electron, energy loss due to synchrotron radiation

Bogacz, Alex↗

DOE OSTI2026

Ab Initio Many Body Quantum Embedding and Local Correlation in Crystalline Materials using Interpolative Separable Density Fitting

We present an efficient implementation of ab initio many-body quantum embedding and local correlation methods for infinite periodic systems through translational symmetry adapted interpolative separable density fitting, an approach which reduces the scaling of the calculations to only linear with the number of k-points. Employing this methodology, we compute correlated ground-state coupled cluster energies within density matrix embedding and local natural orbital correlation frameworks for both weakly and strongly correlated solids, using up to 1000 k-points. By extrapolating the local correlation domains and k-point sampling we further obtain estimates of the full coupled cluster with singles, doubles, and perturbative triples ground-state energies in the thermodynamic limit.

Chemical Physics (physics.chem-ph)↗

DOE OSTI2024

Search for Periodic Time Variations of the Solar 8 B Neutrino Flux between 1996 and 2018 in Super-Kamiokande

We report a search for time variations of the solar 8 B neutrino flux using 5804 live days of Super-Kamiokande data collected between May 31, 1996, and May 30, 2018. Super-Kamiokande measured the precise time of each solar neutrino interaction over 22 calendar years to search for solar neutrino flux modulations with unprecedented precision. Periodic modulations are searched for in a dataset comprising five-day interval solar neutrino flux measurements with a maximum likelihood method. We also applied the Lomb-Scargle method to this dataset to compare it with previous reports. The only significant modulation found is due to the elliptic orbit of the Earth around the Sun. The observed modulation is consistent with astronomical data: we measured an eccentricity of (1.53 ± 0.35)%, and a perihelion shift of (−1.5 ± 13.5) days.

astroparticle detectors↗

DOE OSTI2023

An implicit, conservative and asymptotic-preserving electrostatic particle-in-cell algorithm for arbitrarily magnetized plasmas in uniform magnetic fields

Here, we introduce a new electrostatic particle-in-cell algorithm capable of using large timesteps compared to particle gyro-period under a uniform external magnetic field. The algorithm extends earlier electrostatic fully implicit PIC implementations with a new asymptotic-preserving particle-push scheme that allows timesteps much larger than particle gyroperiods. In the large-timestep limit, the integrator preserves all particle drifts, while recovering the full orbit for small timesteps. The scheme allows for a seamless, efficient treatment of particles with coexisting magnetized and unmagnetized species, and conserves energy and charge exactly without spoiling implicit solver performance. We demonstrate by numerical experiment with several problems of variable species magnetization (diocotron instability, modified two-stream instability, and drift instability) that orders of magnitude wall-clock-time speedups vs. the standard fully implicit electrostatic PIC algorithm are possible without sacrificing solution accuracy.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Million-scale data integrated deep neural network for phonon properties of heuslers spanning the periodic table

Existing machine learning potentials for predicting phonon properties of crystals are typically limited on a material-to-material basis, primarily due to the exponential scaling of model complexity with the number of atomic species. We address this bottleneck with the developed Elemental Spatial Density Neural Network Force Field, namely Elemental-SDNNFF. The effectiveness and precision of our Elemental-SDNNFF approach are demonstrated on 11,866 full, half, and quaternary Heusler structures spanning 55 elements in the periodic table by prediction of complete phonon properties. Self-improvement schemes including active learning and data augmentation techniques provide an abundant 9.4 million atomic data for training. Deep insight into predicted ultralow lattice thermal conductivity (<1 Wm –1 K –1 ) of 774 Heusler structures is gained by p–d orbital hybridization analysis. Additionally, a class of two-band charge-2 Weyl points, referred to as “double Weyl points”, are found in 68% and 87% of 1662 half and 1550 quaternary Heuslers, respectively.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Real-space representation of the quasiparticle self-consistent GW self-energy and its application to defect calculations

The quasiparticle self-consistent (QS) GW (G for Green's function, W for screened Coulomb interaction) approach incorporates the corrections of the quasiparticle energies from their Kohn-Sham density functional theory (DFT) eigenvalues by means of an energy-independent and Hermitian self-energy matrix usually given in the basis set of the DFT eigenstates. By expanding these into an atom-centered basis set (specifically here the linearized muffin-tin orbitals) a real space representation of the self-energy corrections becomes possible. In this work, We show that this representation is relatively short-ranged. This offers opportunities to construct the self-energy of a complex system from parts of the system by a cut-and-paste method. Specifically for a point defect, represented in a large supercell, the self-energy can be constructed from those of the host and a smaller defect-containing cell. The self-energy of the periodic host can be constructed simply from a GW calculation for the primitive cell. We show for the case of the As Ga in GaAs that the defect part can already be well represented by a minimal eight-atom cell and allows us to construct the self-energy for a 64-atom cell in good agreement with direct QSGW calculations for the large cell. Using this approach to an even larger 216-atom cell shows the defect band approaches an isolated defect level. The calculations also allow us to identify a second defect band which appears as a resonance near the conduction band minimum. The results on the extracted defect levels agree well with Green's function calculations for an isolated defect and with experimental data.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Unveiling the Role of Surface Ir-Oxo Species in O 2 Evolution at IrO 2 Electrocatalysts via Embedded Cluster Multireference Calculations

Understanding the mechanisms driving the oxygen evolution reaction (OER) on iridium oxide (IrO 2 )-based catalysts is essential to improving their performance and enabling an actual scale-up of water-splitting photoelectrochemical cells. The mechanistic pathways at IrO 2 interfaces have been extensively investigated computationally using density functional theory (DFT), which predicts a high-energy barrier for the last step of the OER of molecular oxygen detachment and release from the catalyst surface. Nevertheless, surface O 2 over- and under-binding results by standard generalized gradient approximation and hybrid density functionals, respectively, call for further analysis of this crucial step via multireference methods. Aiming at unveiling the nature of such a barrier, we hereby address the formation of O 2 from the most-stable IrO 2 (110) surface with both periodic DFT and an electrostatic embedded cluster approach at the n-electron valence-state perturbation theory. With this multireference approach, we find a value for the aforementioned energy barrier that is much closer to experimental indications than DFT ones. Here, an in-depth analysis of the involved molecular orbitals suggests that the origin of this barrier is related to the breaking of a π interaction between O 2 and Ir surface atom and to a significant additional O 2 interaction with adjacent electrophilic Ir-oxo species, which is present under experimental operating conditions. Besides shedding light on the mechanism of the OER on IrO 2 , these findings point out the importance of multireference methods for dissecting complex reactions at electrocatalytic interfaces and pave the route for further investigations with effective embedding approaches.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗