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DOE OSTI2025

Extreme shape coexistence observed in 70 Co

The shape of the atomic nucleus is a property that underpins our understanding of nuclear systems, impacts the limits of nuclear existence, and enables probes of physics beyond the Standard Model. Nuclei can adopt a variety of shapes, including spheres, axially deformed spheroids, and pear shapes. In some regions of the nuclear chart where a spherical nucleus would naively be expected, deformed nuclear states can result from the collective action of constituent protons and neutrons. In a small subset of nuclei both spherical and deformed nuclear states have been experimentally observed, a phenomenon termed shape coexistence. We present spectroscopic evidence for the coexistence of J π = 1 + spherical and deformed states in 70 Co, separated by less than 275 keV. This close degeneracy of levels with the same J π and different shapes demonstrates an extreme example of shape coexistence resulting from the interplay of independent particle motion and collective behavior in highly unstable nuclear systems and identifies the Co isotopes as a transition point between deformed ground states observed in the Cr isotopes and spherical configurations observed in the closed-shell Ni isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Toward alcohol synthesis from CO hydrogenation on Cu(111)-supported MoS 2 – predictions from DFT+KMC

In the quest for cheap and efficient catalysts for alcohol synthesis from syngas, a material of interest is single-layer MoS2 owing to its low cost, abundancy, and flexible structure. Because of the inertness of its basal plane, however, it is essential to find ways that make it catalytically active. Herein, by means of density functional theory based calculations of reaction pathways and activation energy barriers and accompanying kinetic Monte Carlo simulations, we show that while S vacancy row structures activate the MoS 2 basal plane, further enhancement of chemical activity and selectivity can be achieved by interfacing the MoS 2 layer with a metallic support. When defect-laden MoS2 is grown on Cu(111), there is not only an increase in the active region (surface area of active sites) but also charge transfer from Cu to MoS 2 , resulting in a shift of the Fermi level such that the frontier states (d orbitals of the exposed Mo atoms) appear close to it, making the MoS 2 /Cu(111) system ready for catalytic activity. Finally, our calculated thermodynamics of reaction pathways lead to the conclusion that the Cu(111) substrate promotes both methanol and ethanol as the products, while kinetic Monte Carlo simulations suggest a high selectivity toward the formation of ethanol.

2D materials↗
DOE OSTI2023

Manipulating Growth and Propagation of Correlations in Dipolar Multilayers: From Pair Production to Bosonic Kitaev Models

Here, we study the nonequilibrium dynamics of dipoles confined in multiple stacked two-dimensional layers realizing a long-range interacting quantum spin 1/2 XXX model. We demonstrate that strong in-plane interactions can protect a manifold of collective layer dynamics. This then allows us to map the many-body spin dynamics to bosonic models. In a bilayer configuration we show how to engineer the paradigmatic two-mode squeezing Hamiltonian known from quantum optics, resulting in exponential production of entangled pairs and generation of metrologically useful entanglement from initially prepared product states. In multilayer configurations we engineer a bosonic variant of the Kitaev model displaying chiral propagation along the layer direction. Our study illustrates how the control over interactions, lattice geometry, and state preparation in interacting dipolar systems uniquely afforded by AMO platforms such as Rydberg and magnetic atoms, polar molecules, or trapped ions allows for the control over the temporal and spatial propagation of correlations for applications in quantum sensing and quantum simulation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

X-ray and molecular dynamics study of the temperature-dependent structure of molten NaF-Zr⁢F 4

The local atomic structure of NaF-Zr⁢F 4 (53–47 mol%) molten system and its evolution with temperature are examined with x-ray scattering measurements which are then used to validate the quality of ab initio and neural network-based molecular dynamics (NNMD) calculations in the temperature range 515–700°⁢C. The machine-learning enhanced NNMD calculations offer improved efficiency while maintaining accuracy at higher distances compared to ab initio calculations. Looking at the evolution of the pair distribution function with increasing temperature, a fundamental change in the liquid structure within the selected temperature range, accompanied by a slight decrease in overall correlation is revealed. NNMD calculations indicate the coexistence of three different fluorozirconate complexes: [Zr⁢F 6 ] 2– , [Zr⁢F 7 ] 3– , and [Zr⁢F 8 ] 4– , with a shift in the dominant coordination state from the 7-coordinated Zr cation toward a 6-coordinated cation with increasing temperature. The study also highlights the metastability of different local coordination structures, with frequent interconversions between the 6- and 7-coordinate states. Analysis of the Zr-F-Zr angular distribution function reveals the presence of both “edge-sharing” and “corner-sharing” fluorozirconate complexes with specific bond angles and distances in accord with previous studies, while the next-nearest-neighbor cation-cation correlations demonstrate a clear preference for unlike cations as nearest-neighbor pairs, emphasizing nonrandom arrangement. Finally, these findings contribute to a comprehensive understanding of the complex local structure of the molten salt, providing insights into temperature-dependent preferences and correlations within the molten system.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Targeted synthesis of predicted metastable compounds using modulated elemental reactants

Three metastable compounds predicted to be kinetically stable using an “island” approach were successfully synthesized from designed modulated elemental reactants. Fe0.8V0.2Se2 was synthesized by depositing ultrathin elemental layers in a V|Fe|Se sequence to control the local composition. An alloyed rock salt structured Pb3Mn2Se5 constituent layer, which does not exist as a bulk compound, was synthesized in the heterostructure (Pb3Mn2Se5)0.6VSe2 by depositing a precursor with a V|Se|Pb|Se|Mn|Se|Pb|Se|Mn|Se|Pb|Se sequence of elemental layers that mimicked the compositional profile of the targeted heterostructure. The heterostructure (PbSe)1+δ(FeSe2)2 was prepared by depositing a precursor with a repeating layering sequence of Fe|Pb|Fe|Se, where each sequence contains the number of atoms required to form a single unit cell. In all three systems, the local compositions in the layer sequence kinetically favored the nucleation and growth of the targeted products during the deposition. The diffusion lengths to form the targeted compounds were short, and the diffusion was limited by postdeposition low temperature annealing to favor the growth of the targeted compounds and avoid the decomposition into a mixture of thermodynamically stable compounds.

Lemon, Mellie (ORCID:0000000328705881)↗
DOE OSTI2026

Evidence for an isomeric {pi}½{sup +}[411] state in {sup 183}Ta

We report on the identification of a new isomeric state in Ta populated via the ground-state -decay of Hf. The experiment was performed at the KISS setup at RIKEN, where neutron-rich hafnium isotopes were produced via multi-nucleon transfer (MNT) reactions, followed by laser ionization of hafnium atoms, mass separation, and detection using an electron-gamma coincidence system. Isomeric spectroscopy was carried out by gating on different electron-gamma time correlations. A 459.1 keV -ray transition was identified in delayed spectra, and a half-life of μ was extracted through time-distribution fitting. The 459.1 keV state in Ta is known from previous work and has been assigned a Nilsson orbital configuration of , while a proposed new isomeric state above it is interpreted as a configuration that decays to via a low-energy, unobserved E2 transition. This is consistent with the systematic trends in neighbouring odd-A nuclei and transition rate calculations. Similar content being viewed by others

Doshi, S.↗
DOE OSTI2020

rlmolecule: A library for general-purpose material and molecular optimization using AlphaZero-style reinforcement learning

This library includes in-progress code for the optimization of materials and molecules using reinforcement learning. This project seeks to develop a generalized machine learning approach for optimizing targeted, and often complex, functional properties over the space of possible material structures, allowing faster identification of promising candidates. Electronic and transport properties of materials are determined by their molecular structure (for molecules) or their crystal structure (for in-organic crystalline materials). The atomic composition, bonding, and 3-D-spatial arrangement in these systems therefore represent a vast, discontinuous search space for optimal candidates. This library implements AlphaZero style reinforcement learning applied to two worked examples: the optimization of stable organic radicals for redox flow batteries, and the determination of stable electrolyte species for solid state batteries. The current code contains proof-of-concept results run on the Eagle HPC system, while the completed package will be a flexible tool for material optimization across of number of energy-relevant fields, which leverages cloud compute resources for the majority of the computational heavy lifting.

Biagioni, David↗
DOE OSTI2024

Summary Report on Ion Irradiation Study of Ceramic Coating on Suppressing FCCI

Advanced cladding is critical for advanced nuclear reactors with an enhanced performance in radiation tolerance and neutron transparency. Using advanced cladding will ensure the adequate thermal conductivity and mechanical stability of the cladding base material, corrosion resistance, high-temperature coolant compatibility of the cladding surface, and chemical stability in the cladding inner wall against fuel cladding chemical interaction (FCCI). An innovative cladding with a three-layer structure (i.e., a modified surface, a clad base material, and a modified inner wall) promises to meet all these requirements. Initial research and development (R&D) regarding this innovative cladding seek to demonstrate the effectiveness of a thin ceramic coating in suppressing FCCI under ion irradiation to high dose. This United States (U.S.) Department of Energy (DOE)–Office of Nuclear Energy (NE) project report summarizes the results of recent ion irradiation studies of diffusion-couple samples with details of an ion irradiation experiment, the characterization of the interface microstructure of cerium (Ce)/titanium nitride (TiN)/oxide-dispersion strengthened (ODS), Ce/TiN/iron (Fe), Ce/ODS, and Ce/Fe samples irradiated with 80 million electron-volts (MeV) of xenon (Xe) ions to 100 displacements per atom (dpa) at 500?C using the Argonne Tandem Linac Accelerator System (ATLAS) facility at Argonne National Laboratory (ANL). The results of the ODS-substrate sample are encouraging and demonstrate the effectiveness of a thin ceramic coating on FCCI mitigation under irradiation. The results from an Fe-substrate sample revealed a complex microstructure, and the root cause is discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Ab Initio Molecular Dynamics Insights into Stress Corrosion Cracking and Dissolution of Metal Oxides

Oxide phases such as α-Fe2O3 (hematite) and α-Al2O3 (corundum) are highly insoluble in water; however, subcritical crack growth has been observed in humidity nonetheless. Chemically induced bond breaking at the crack tip appears unlikely due to sterically hindered molecular transport. The molecular mechanics of a crack in corundum with a reactive force field reveal minimal lattice trapping, leading to bond breaking before sufficient space opens for water transport. To address this, we model a pre-built blunt crack with space for H2O molecule adsorption at the tip and show that it reduces fracture toughness by lowering the critical J-integral. Then, we explore stress-enhanced dissolution to understand the mechanism of crack tip blunting in the oxide/water system. Density functional theory combined with metadynamics was employed to describe atomic dissolution from flat hematite and corundum surfaces in pure water. Strain accelerates dissolution, stabilizing intermediate states with broken bonds before full atom detachment, while the free energy profile of unstrained surfaces is almost monotonic. The atomistic calculations provided input for a kinetic model, predicting the shape evolution of a blunt crack tip, which displays three distinct regimes: (i) dissolution primarily away from the tip, (ii) enhanced blunting near but not at the apex, and (iii) sharpening near the apex. The transition between regimes occurs at a low strain, highlighting the critical role of water in the subcritical crack growth of oxide scales, with dissolution as the fundamental microscopic mechanism behind this process.

Chemistry↗
DOE OSTI2020

Ground state wave functions for single-band Hubbard models from the Gutzwiller conjugate gradient minimisation theory

The Gutzwiller conjugate gradient minimisation (GCGM) theory is an ab initio quantum many-body theory for computing the ground-state properties of infinite systems. Previous applications of GCGM provides satisfying accuracy of ground-state energy of Hubbard models. In the current work, we address the problem of whether the obtained wave function is a good approximation for the true ground state by comparing the correlation functions with the benchmark data. Additionally, our results confirms the accuracy of the reproduced ground state of the regular Hubbard model, but with some exception for the frustrated Hubbard model.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

ORNL_AISD_NiPt_108atoms

This dataset describes the nickel-platinum (NiPt) solid solution binary alloy, where the two constituent elements nickel (Ni) and platinum (Pt) are randomly placed on the face centered cubic (FCC) crystal structure, with the lattice constant of 3.840 angstroms. The dataset comprises data for crystal structures with 108 atoms with 1,900 configurations. The data set was generated for concentrations ranging from 0at% of Pt to 100at% of Pt in the NiPt binary system, with increasing the concentration of Pt in the system every 5at%. For each one of the chemical compositions, 100 random configurations were generated, each with a different random seed. Each of the output files contains the mass, type, atomic coordinates, energy per atom, and forces in x, y, and z directions respectively. For each atomic configuration, the output was collected every 150 steps during the minimization stage and every 1000 steps during the replica exchange stage. Large-scale Atomic/Molecular Massively Parallel Simulator (LAMMPS) [1], which is a molecular dynamics code, was used to generate data for NiPt alloy. The simulation used the interatomic potential for NiPt binary system 'MEAM_LAMMPS_KimSeolJi_2017_PtNi__MO_020840179467_001' [3] from the OpenKIM library (Open Knowledgebase of Interatomic Models) [2]. This potential was developed based on the second nearest-neighbor modified embedded-atom method (2NN MEAM). The simulation process begins with the generation of the random NiPt structure and follows with the short minimization and replica exchange simulation. The minimization procedure adjusts atomic coordinates and performs energy minimization, which typically leads to a local potential energy minimum. The method used for the minimization was the conjugate gradient algorithm. A short replica exchange (parallel tempering) simulation involves four replicas (ensembles) of a system and follows the minimization stage. Multiple snapshots of the configuration were collected during the minimization and replica exchange stages. NiPt alloy is interesting due to its magnetic and charge transfer properties [4]. The data is provided in a compressed zipped folders atoms108.zip. The zipped folder contains the data structured in the following way: - Ni_ground_state.cfg --> atomic configuration for the pure nickel - Pt_ground_state.cfg --> atomic configuration for the pure platinum - Pt#_filtered --> folders containing atomic configurations for #at% concentration of platinum. The folder contains 100 atomic configurations, each saved in a subfolder - Each subfolder named config* is associated with a specific atomic configuration. Each of these subfolders contains files with .cfg format, corresponding to outputs for each atomic configuration The total number of atomic configurations contained in atoms108.zip is 66,132. This dataset is an extension to the dataset ORNL_AISD_NiPt [5] that has been previously released with crystal structures of 256 atoms, 864 atoms, and 2,048 atoms, with the same methodology for data collection. References [1] https://www.lammps.org/ [2] https://openkim.org/ [3] https://openkim.org/id/MEAM_LAMMPS_KimSeolJi_2017_PtNi__MO_020840179467_001 [4] El-Gendy, Ahmed A. and Hampel, Silke and Büchner, Bernd and Klingeler, Rüdiger, Tuneable magnetic properties of carbon-shielded NiPt-nanoalloys, RSC Adv., volume 6, issue 57, pages 52427-52433, 2016, The Royal Society of Chemistry, doi:10.1039/C6RA05910D [5] M. Karabin, M. Lupo Pasini, and M. Eisenbach. ORNL_AISD_NiPt. United States: N. p., 2023. Web. doi:10.13139/OLCF/1958172.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Large-scale integration of artificial atoms in hybrid photonic circuits

A central challenge in developing quantum computers and long-range quantum networks is the distribution of entanglement across many individually controllable qubits. Colour centres in diamond have emerged as leading solid-state ‘artificial atom’ qubits because they enable on-demand remote entanglement, coherent control of over ten ancillae qubits with minute-long coherence times and memory-enhanced quantum communication. A critical next step is to integrate large numbers of artificial atoms with photonic architectures to enable large-scale quantum information processing systems. So far, these efforts have been stymied by qubit inhomogeneities, low device yield and complex device requirements. Here we introduce a process for the high-yield heterogeneous integration of ‘quantum microchiplets’—diamond waveguide arrays containing highly coherent colour centres—on a photonic integrated circuit (PIC). We use this process to realize a 128-channel, defect-free array of germanium-vacancy and silicon-vacancy colour centres in an aluminium nitride PIC. Photoluminescence spectroscopy reveals long-term, stable and narrow average optical linewidths of 54 megahertz (146 megahertz) for germanium-vacancy (silicon-vacancy) emitters, close to the lifetime-limited linewidth of 32 megahertz (93 megahertz). We show that inhomogeneities of individual colour centre optical transitions can be compensated in situ by integrated tuning over 50 gigahertz without linewidth degradation. The ability to assemble large numbers of nearly indistinguishable and tunable artificial atoms into phase-stable PICs marks a key step towards multiplexed quantum repeaters and general-purpose quantum processors

36 MATERIALS SCIENCE↗
DOE OSTI2022

High Accuracy Transition Metal Effective Cores for the Many-Body Diffusion Monte Carlo Method

Practical applications of the real-space diffusion Monte Carlo (DMC) method require the removal of core electrons, where currently localization approximations of semilocal potentials are generally used in the projector. Accurate calculations of complex solids and large molecules demand minimizing the impact of approximated atomic cores. Prior works have shown that the errors from such approximations can be sizable in both finite and periodic systems. In this work, we show that a class of differential pseudopotentials, known as pseudo-Hamiltonians, can be constructed for the 3d transition metal atoms, entirely removing the need for any localization scheme in the DMC projector. As a proof of principle, we demonstrate the approach for the case of Co. In order to minimize errors in the pseudo-Hamiltonian at the many-body level, we generalize the recently proposed correlation-consistent pseudopotential generation scheme to successively close semilocal representations of the differential potentials. Our generation scheme successfully produces potentials tailored specifically for real space projector quantum Monte Carlo methods with low error at the many-body level, i.e., with many-body scattering properties very close to relativistic all-electron results. In particular, we show that the agreement with respect to atomic and molecular quantities reach chemical accuracy in many cases-on par with the most accurate semilocal pseudopotentials available. Further, our pseudo-Hamiltonian generation scheme utilizes standard quantum chemistry codes designed only to work with semilocal pseudopotentials, enabling straightforward generation of pseudo-Hamiltonians for additional elements in future works.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Designing Ceria/Alumina for Efficient Trapping of Platinum Single Atoms

Cerium oxide (ceria) has been shown to be very effective at trapping platinum atoms, due to formation of stable surface complexes at step edges, where coordinatively unsaturated cerium cations are present. But ceria loses its effectiveness when heated to high temperatures, due to loss of surface area and growth in particle size associated with sintering of the oxide. Being a rare-earth, and with limited supplies worldwide, it is important to develop methods to improve the effectiveness of ceria as a catalyst support. Here we explore the performance for trapping Pt atoms when the ceria is supported on a high surface area alumina carrier. This helps create a more sustainable catalyst formulation, especially if we can retain the high dispersion of Pt seen on ceria supports. For this work, we studied the atom trapping efficacy of ceria/alumina samples with increasing ceria content (8 wt% - 50%) and contrasted the behavior with pure ceria. Electron microscopy reveals that when dispersed on alumina, ceria is present in the form of crystalline nanoparticles as well as isolated cerium ions. These two forms of ceria differ markedly in their ability to trap Pt atoms. Atomically dispersed cerium is present in the form of Ce 3+ cations on alumina, however this form of ceria is not effective for trapping Pt atoms. Our results show that the atom trapped Pt resides primarily on crystalline ceria nanoparticles. CO oxidation was used as a probe reaction to evaluate the performance of these Pt AT /ceria-alumina catalysts. As a result, we conclude that over the range of ceria loadings we investigated, 50% ceria/alumina represents the optimal catalyst support for achieving high surface area and atom trapping efficiency while helping reduce the total ceria content in this catalyst system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

A nonlinear journey from structural phase transitions to quantum annealing

Motivated by an exact mapping between equilibrium properties of a one-dimensional chain of quantum Ising spins in a transverse field (the transverse field Ising (TFI) model) and a two-dimensional classical array of particles in double-well potentials (the “$\phi$ 4 model”) with weak inter-chain coupling, we explore connections between the driven variants of the two systems. Here, we argue that coupling between the fundamental topological solitary waves in the form of kinks between neighboring chains in the classical $\phi$ 4 system is the analog of the competing effect of the transverse field on spin flips in the quantum TFI model. As an example application, we mimic simplified measurement protocols in a closed quantum model system by studying the classical $\phi$ 4 model subjected to periodic perturbations. This reveals memory/loss of memory and coherence/decoherence regimes, whose quantum analogs are essential in annealing phenomena. In particular, we examine regimes where the topological excitations control the thermal equilibration following perturbations. This paves the way for further explorations of the analogy between lower-dimensional linear quantum and higher-dimensional classical nonlinear systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Systems and methods for photothermal material

Chinese ink is applied on various materials and stabilized by atomic layer deposition to fabricate solar steam generation devices. The encapsulated ink has excellent photothermal properties and evaporation efficiency under simulated sunlight, holding great promise in solar evaporation device applications.

Yang, Hao-Cheng↗
DOE OSTI2021

Predicting orientation-dependent plastic susceptibility from static structure in amorphous solids via deep learning

It has been a long-standing materials science challenge to establish structure-property relations in amorphous solids. Here we introduce a rotationally non-invariant local structure representation that enables different predictions for different loading orientations, which is found essential for high-fidelity prediction of the propensity for stress-driven shear transformations. This novel structure representation, when combined with convolutional neural network (CNN), a powerful deep learning algorithm, leads to unprecedented accuracy for identifying atoms with high propensity for shear transformations (i.e., plastic susceptibility), solely from the static structure in both two- and three-dimensional model glasses. The data-driven models trained on samples at one composition and a given processing history are found transferrable to glass samples with different processing histories or at different compositions in the same alloy system. Our analysis of the new structure representation also provides valuable insight into key atomic packing features that influence the local mechanical response and its anisotropy in glasses.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Quantum simulations of SO(5) many-fermion systems using qudits

The structure and dynamics of many-body systems are the result of a delicate interplay between underlying interactions. Fermionic pairing, for example, plays a central role in various physical systems, ranging from condensed matter to nuclear systems, where it can lead to collective phenomena such as superconductivity and superfluidity. In atomic nuclei, the interplay between pairing and particle-hole interactions leads to a high degree of complexity and intricate entanglement structures. Despite this apparent complexity, symmetries emerge and manifest themselves in observable regular patterns. These symmetries and their breakings have long been used to determine relevant degrees of freedom and simplify classical descriptions of many-body systems. Here, this work explores the potential utility of quantum computers with arrays of qudits in simulating interacting fermionic systems, when the qudits can naturally map the relevant degrees of freedom determined by an underlying symmetry group. The Agassi model of fermions interacting via particle-hole and pairing interactions is based on an underlying so(5) algebra. Such systems can intuitively be partitioned into pairs of modes with five basis states, which thus naturally map to arrays of d = 5 qudits (qu5its). Classical noiseless simulations of the time evolution of systems with up to twelve qu5its are performed, by implementing quantum circuits that are developed herein, using PYTHON codes invoking Google's CIRQ software. The resource requirements of the qu5it circuits are analyzed and compared with two different mappings to qubit systems: a physics-aware Jordan-Wigner mapping requiring four qubits per mode pair and a state-to-state mapping requiring three qubits per mode pair. While the dimensionality of Hilbert spaces in mappings to qu5it systems are less than those for the corresponding qubit systems, the number of entangling operations, depending on the available hardware, can either be greater or smaller than for the physics-aware Jordan-Wigner mapping. The state-to-state mapping, while having a smaller Hilbert space than Jordan-Wigner mappings, appears to be the least efficient in gate counts. Further, a previously unknown sign problem has been identified from Trotterization errors in time evolving high-energy excitations. There appear to be advantages in employing quantum computers with arrays of qudits to perform simulations of many-body dynamics that exploit the role of underlying symmetries, specifically in lowering the required quantum resources and in reducing anticipated errors that take the simulation out of the physical space. If the necessary entangling gates are not directly supported by the hardware, physics-aware mappings to qubits may, however, be advantageous for other aspects.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗