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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 163 records · Page 9
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DOE OSTI2025

Pomeranchuk instability from electronic correlations in CsTi 3 Bi 5 kagome metal

Electronic nematicity, the spontaneous breaking of rotational symmetry, has emerged as a key instability in correlated quantum systems. CsTi 3 Bi 5 , a kagome metal of the AV 3 Sb 5 (A = K, Rb, Cs) family, hosts rich unconventional electronic phases, yet the origin of its nematicity remains unsettled. Here, we combine polarization-dependent angle-resolved photoemission spectroscopy with functional renormalization group calculations on a fully interacting ab initio model. We reveal an orbital-selective nematic deformation in the low-energy band structure and identify a finite angular momentum (d-wave) Pomeranchuk instability driven by electronic correlations in specific orbital channels and detuning from Van Hove singularities. Our results establish a direct link between orbital selectivity and symmetry-breaking instabilities in CsTi 3 Bi 5 , providing a microscopic framework for nematic order in kagome systems.

Bigi, Chiara [Synchrotron SOLEIL, Saint-Aubin (Fra↗
DOE OSTI2025

Integrated modeling of alpha particle losses in JET DT plasmas

Alpha particle confinement is crucial for sustaining burning plasmas and designing future reactor concepts. Along with classical/prompt losses, various magnetohydrodynamic instabilities can lead to wave-particle interactions which can transport alpha particles outward from the plasma. This can result in a reduction in plasma heating/performance, and, at worst, damage in-vessel components. Joint European Torus’s recent deuterium–tritium campaigns in 2021–2023 have produced numerous alpha particle loss measurements with its scintillator probe and Faraday cup array fast ion loss detectors as discussed in Bonofiglo et al (2024 Nucl. Fusion 64 096038). This paper will report on integrated energetic particle transport modeling in support of those measurements. The modeling is accomplished with the TRANSP and ORBIT-kick codes with the use of recently developed reduced models which calculate mode structure, amplitude, and the evolving dynamics. When possible, constraints and comparisons to experiment are conducted. Case studies are performed on a variety of magnetohydrodynamic activity, including: fishbones, tearing modes (TMs), and sawtooth crashes. Additionally, a special case of an alpha-driven toroidal Alfvén eigenmode is briefly discussed, where modeling showed marginally weak alpha losses and was unable to support experimental observations. Coupled effects between a TM and toroidal field ripple are presented and were unable to replicate the observations in lost particle pitch but did duplicate the localized flattening of the measured neutron profile. Additional modeling results compare the magnitude of losses and energy/velocity-space sensitivities against experimental observations/measurements for each scenario. This work corroborates numeric alpha transport modeling while also identifying model deficiencies. While this report details alpha transport, it also presents open issues for discussion in assessing the validity of our numerical models towards burning plasmas.

Bonofiglo, Phillip J. [Princeton Plasma Physics La↗
DOE OSTI2024

Nodal fermions in the strongly spin-orbit coupled pyrochlore-lattice compound RbBi2

We explore the topological electronic band structure of the pyrochlore lattice in the strong spin-orbit coupling regime. Using angle-resolved photoemission spectroscopy, first-principles calculations, and symmetry analysis, we have investigated the bulk electronic structure of RbBi2, which has a Bi pyrochlore network. We observe the presence of 3D massless Dirac fermions enforced by nonsymmorphic symmetry, as well as a 3D quadratic band crossing protected by cubic crystalline symmetry. Furthermore, we identify an additional 3D linear Dirac dispersion associated with band inversion protected by threefold rotation symmetry. These observations reveal the rich band topology of itinerant pyrochlore lattice systems in the strong SOC limit and serve as a starting point to explore correlated topological phases in geometrically frustrated lattices.

Oh, Dongjin↗
DOE OSTI2024

Materials for Ultra‐Coherent, Mobile, Electron‐Spin Qubits

This research project has had the goal of gaining a better understanding of the physics of electrons bound to the surface of superfluid helium from both experimental and theoretical perspectives. It has particularly been aimed at two areas which had not been well studied: the relaxation and decoherence of the spin of the electrons on the helium surface and how the properties of underlying metallic layers affect the behavior of the electrons when the helium covering the metal is thin. This work is motivated in part by interest in using the spin of these electrons as a quantum bit, or qubit. Low levels of decoherence are advantageous for qubits, and moving the electrons, as one might do in a quantum processor, will be easiest if thin helium films can be employed. It had been suggested that spin decoherence should be very weak for electrons bound to superfluid He, but before this work there have been no quantitative studies of spin relaxation and decoherence. It is especially important to know how moving the electrons across the helium surface would affect their spin coherence. Calculations performed as part of this project show that the Rashba effective magnetic field, the mechanism which limits the spin coherence of mobile electrons in silicon-based devices (an actively pursued qubit technology), is exceptionally weak for electrons bound to helium. This project has identified other decoherence mechanisms which are stronger, but still weak compared to analogous silicon-based structures. Calculated spin coherence times for mobile electrons approach one day, as compared to microseconds in silicon. With coherence times of this magnitude, the spin qubit errors on helium will be completely dominated by errors in the quantum gates. In related work, the possibility of using an artificial spin-orbit interaction (a gradient magnetic field) for quantum operations on the electrons spins was considered. The calculations show that a moderate gradient field, small enough to be generated by a narrow superconducting wire, will enable high-fidelity quantum operations on electrons held in lithographically-defined quantum dots by driving them with a microwave electric field. The spin and motional coherence of the electrons is sufficient to allow high-fidelity 2-qubit quantum operations between electrons in neighboring quantum dots. As an outgrowth of experiments aiming to measure electron spin coherence it was discovered that very high densities of electrons can be stably supported on thin helium films coating ultra-smooth amorphous metallic layers. The measured densities are high enough that the electron system has almost certainly transitioned from an ordered array of electrons, known as a Wigner crystal (ordered by the electrons’ mutual repulsion), to a quantum fluid known as a Fermi liquid. This transition has been a subject of intense interest for over 40 years, since the electron Wigner crystal was first observed with electrons bound to superfluid helium, but it has never been unambiguously observed. Experiments are still underway in these new structures to definitively determine whether true quantum melting of the Wigner crystal has been demonstrated. This work has also catalyzed the development of a new approach for measuring the transport of electrons across very thin helium films, as will be needed for some of the quantum computing applications. The high electron density experiments as well as experiments with electrons bound in quantum dots have led to new techniques which may enable spin coherence measurements.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Effects of the Inverse Trans-Influence in a Berkelium(III) Phosphine Oxide Complex

An example of a 249 Bk 3+ phosphine oxide complex has been prepared to examine and quantify the effects of the inverse trans-influence (ITI) on a late actinide complex. This has been accomplished through a comparison of cis and trans Bk-ligand bonds in the meridional berkelium(III) complex, BkBr 3 (OPCy 3 ) 3 (OPCy 3 = tricyclohexylphosphine oxide). A detailed bond metric analysis was completed that includes the shortest published distance for a Bk 3+ −O bond, attributed to the smaller coordination number of Bk 3+ of six in mer-BkBr 3 (OPCy 3 ) 3 . ITI calculations of the trans Bk 3+ −O bond provide an ITI value (98.5(2)%) comparable to that of mer-AmBr 3 (OPCy 3 ) 3 (98.2(2)%) and indicate a small 5f orbital contribution to bonding. This effect is discussed in the context of the isomorphous lanthanide(III) series where the ITI is calculated to be higher for mer-BkBr 3 (OPCy 3 ) 3 than in most Ln 3+ analogues.

Actinides↗
DOE OSTI2026

Synthesis of Cp* Terphenylamido U(III) Iodide Complexes with a Substitutable Iodide Position to Generate Terminal U(III)–(κ 3 -BH 4 ) Complexes

Reaction of Cp*UI 2 (THF) 3 (Cp* = pentamethylcyclopentadienide; THF = tetrahydrofuran) with Na R3 TerNH ( R3 Ter = 2,6(2,4,6-R 3 C 6 H 2 ) 2 C 6 H 3 ; R = Me, Et, iPr) gave the U(III) monoiodide complexes Cp*( R3 TerNH)UI (R = Me, 1-Me; R = Et, 2-Et; R = iPr, 3-iPr). These complexes contain a functionalizable iodide position which reacts favorably with NaBH4 to give the κ 3 -borohydride complexes Cp*( R3 TerNH)U(H 3 BH) (R = Me, 4-Me; R = Et, 5-Et; R = iPr, 6-iPr). All compounds were experimentally characterized by SC-XRD, 1 H and 11 B NMR spectroscopy as well as UV–vis–NIR and FTIR analyses. DFT calculations corroborate the experimental findings, confirming the 5f 3 U(III) configuration across the entire series and revealing an increased U 5f orbital contribution in the borohydride derivatives. All compounds exhibit small but non-negligible U(III)–(η 6 -arene) δ-back-bonding interactions arising from the unpaired 5f electrons. Calculated steric parameters show progressively greater shielding of the U(III) center with increasing bulk of the terphenyl substituents from Me to iPr.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Excited electronic states of Na 2 and K 2 : The potential for long-lived “reservoir” states leading to collision induced population inversions

Potential energy curves (PECs) for the spin-free (ΛS) and spin–orbit (Ω) states associated with the four lowest-lying dissociation channels of Na 2 and K 2 were calculated at the SA-CASSCF/SO-CASPT2/aug-cc-pwCVQZ-DK level. The PECs of Na 2 were consistent with the experimental data and with the FS-CCSD (2,0) calculations, reproducing the double-well and the “shelf” character for some of the potentials of the excited states. For K 2 , the PECs behaved in a similar way and the spectroscopic parameters for the ground and the excited states are in good agreement with the available experimental values. The dissociation energy of K 2 was predicted to be D e = 4454 cm −1 , within an agreement of 5 cm −1 with the experiments. For Na 2 , D e = 5789 cm −1 compared to the experimental value of 6022 cm −1 . The inclusion of spin–orbit coupling effects resulted in avoided crossings, which affect the PECs. Spin–orbit changes the predicted curves for some excited Ω states arising from ΛS states that overlap each other, affecting their associated vibrational frequencies and bond distances. Here, the current studies of the low-lying states in K 2 reveal a similar structure to those of Na 2 , which suggests the accessibility of long-lived energy storing reservoir states and possible population inversions in K 2 following prior experimental work on the reaction of halogen atoms with Na 3 to produce excited states of Na 2 .

Ab-initio methods↗
DOE OSTI2024

Ground state property calculations of LiH n complexes using IBM Qiskit’s quantum simulator

In this study, the variational quantum eigensolver (VQE) on a quantum simulator is used in calculating ground state electronic structure properties of the LiH n , n = 1–3, complexes including their singly charged ions. Results calculated using classical electronic structure algorithms are also included. We investigate the use of the unitary coupled cluster with singles and doubles (UCCSD) Ansatz using VQE within Qiskit and compare results to full configuration interaction (FCI) calculations. Computed ground state energies, electron affinities, ionization potentials, and dipole moments are considered. We report the first-of-its-kind simulated quantum computing results of selected LiH n species and use the parity orbital to qubit mapping scheme. We find that VQE/UCCSD results are comparable to classical coupled clusters with singles and doubles for all considered systems with respect to FCI. A VQE calculation cost evaluation is included in which we evaluate performance using both Jordan–Wigner and parity orbital to qubit mapping schemes. We also discuss some of the current limitations of utilizing VQE for the study of chemical systems.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2024

Interpretable, extensible linear and symbolic regression models for charge density prediction using a hierarchy of many-body correlation descriptors

Here, density functional theory (DFT) is routinely used to make electronic structure predictions for high-throughput screening of materials and molecules for technologically relevant areas, like the identification of better catalysts, electronic materials, and drug discovery. However, the DFT formalism is limited by (a) its poor (quadratic-to-quartic) scaling, and (b) the need to perform repeated eigenvalue computations of the electronic Hamiltonian as part of its self-consistent field (SCF) iteration procedure to obtain the converged ground state electron density, ρ (r). Approaches that directly predict ρ (r) of a structure with high accuracy can accelerate conventional SCF calculations and can also be used in linearly scaling methods such as orbital-free DFT. To this end, we present a procedure to predict the ground state electron density of molecular and periodic three-dimensional systems directly from the atomic structure with a particular emphasis on physical interpretability. In our framework, ρ (r) is modeled using many-body correlation descriptors that accurately capture the effects of local atomic arrangements in the neighborhood of a grid point. Our use of a linear regression scheme to fit to charge density data enables transparent analysis of the relative contributions of various types of local atomic correlations. By systematically including increasingly complex correlations, our model is shown to accurately predict ρ (r) for a variety of chemically and electronically diverse systems — amorphous Ge, Al(001) slab, crystalline Ga 2 O 3 , molecular benzene, and polyethylene. We then demonstrate a symbolic regression-based protocol to construct easily computable, interpretable features from lower-order correlations that significantly improves our electron density predictions with effectively no increase in the computational cost.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

An Orbital Basis Set for Double Photoionization of Atoms and Molecules

The ab initio theoretical treatment of one-photon double photoionization processes has been limited to atoms and diatomic molecules by the challenges posed by large grid-based representations of the double ionized continuum wave function. To provide a path for extensions to polyatomics, an energy-adapted orbital basis approach is demonstrated that reduces the dimensions of such representations and simultaneously allows larger time steps in time-dependent computational descriptions of double ionization. Additionally, an algorithm that exploits the diagonal nature of the two-electron integrals in the grid basis and dramatically accelerates the transformation between grid and orbital representations is presented. Excellent agreement between the present results and benchmark theoretical calculations is found for H – and Be atoms, as well as the hydrogen molecule, including for the triply differential cross sections that relate the angular distribution and energy sharing of all of the particles in the molecular frame.

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

Anion Photoelectron Spectroscopy and Ab Initio Studies of the UF – Anion

A synergistic anion photoelectron spectroscopic and ab initio computational study of photodetachment of UF – is reported. The measurement determined a vertical detachment energy of 0.63(03) eV, which is consistent with a spinor-based relativistic coupled-cluster CCSD(T) value of 0.61 eV. The complex spectral features due to excited electronic states and vibrational progressions of UF are analyzed and assigned with the help of spin–orbit-coupled multireference perturbation theory and spinor-based relativistic coupled-cluster calculations. UF and UF – are confirmed to be dominated by ionic bonding. Furthermore, the usefulness of the spinor CCSD(T) approach is demonstrated.

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

Hyperfine interactions for small systems including transition-metal elements using self-interaction corrected density-functional theory

The interactions between the electronic magnetic moment and the nuclear spin moment, i.e., magnetic hyperfine (HF) interactions, play an important role in understanding electronic properties of magnetic systems and in realizing platforms for quantum information science applications. We investigate the HF interactions for atomic systems and small molecules, including Ti or Mn, by using Fermi–Löwdin orbital (FLO) based self-interaction corrected (SIC) density-functional theory. We calculate the Fermi contact (FC) and spin-dipole terms for the systems within the local density approximation (LDA) in the FLO-SIC method and compare them with the corresponding values without SIC within the LDA and generalized-gradient approximation (GGA), as well as experimental data. For the moderately heavy atomic systems (atomic number Z ≤ 25), we find that the mean absolute error of the FLO-SIC FC term is about 27 MHz (percentage error is 6.4%), while that of the LDA and GGA results is almost double that. Therefore, in this case, the FLO-SIC results are in better agreement with the experimental data. For the non-transition-metal molecules, the FLO-SIC FC term has the mean absolute error of 68 MHz, which is comparable to both the LDA and GGA results without SIC. For the seven transition-metal-based molecules, the FLO-SIC mean absolute error is 59 MHz, whereas the corresponding LDA and GGA errors are 101 and 82 MHz, respectively. Therefore, for the transition-metal-based molecules, the FLO-SIC FC term agrees better with experiment than the LDA and GGA results. We observe that the FC term from the FLO-SIC calculation is not necessarily larger than that from the LDA or GGA for all the considered systems due to the core spin polarization, in contrast to the expectation that SIC would increase the spin density near atomic nuclei, leading to larger FC terms.

Chemistry↗
DOE OSTI2024

Unconventional fieldlike spin torques in CrPt 3

The topological semimetal CrPt 3 has potential for generating unconventional spin torques due to its ferrimagnetic ordering, topological band structure, and high anomalous Hall effect. CrPt 3 exhibits ferrimagnetic behavior only in its chemically ordered phase and is paramagnetic in its chemically disordered phase. By controlling the growth and annealing temperatures, we prepare epitaxial films of both chemically ordered and chemically disordered phases of CrPt 3 , allowing us to investigate the effect of magnetic ordering on unconventional-torque generation. We use angle-dependent spin-torque-ferromagnetic-resonance and second-harmonic Hall measurements to probe the spin torques generated from epitaxial CrPt 3 in CrPt 3 /Cu/Ni 81 ⁢Fe 19 heterostructures. With current applied along specific directions with respect to the crystal order, we reveal unconventional spin torques in both ordered and disordered films. When current flows parallel to the [$1\bar{1}1$] and [ $\bar{1}11$] directions, we observe an unconventional fieldlike torque that is opposite in sign for the two directions. Finally, our calculations reveal that this unconventional torque originates from an indirect nonlocal spin-orbit torque due to spin scattering at the CrPt 3 /Cu interface, in addition to symmetry breaking at this interface.

ferromagnetic resonance↗
DOE OSTI2025

Quantum graph models for transport in filamentary switching

The formation of metallic nanofilaments bridging two electrodes across an insulator is a mechanism for resistive switching. Examples of such phenomena include atomic synapses, which constitute a distinct class of memristive devices the behavior of which is closely tied to the properties of the filament. Until recently, experimental investigation of the low-temperature regime and quantum transport effects has been limited. However, with growing interest in understanding the true impacts of the filament on device conductance, comprehending quantum effects has become crucial for quantum neuromorphic hardware. Here, we discuss quantum transport resulting from filamentary switching in a narrow region where the continuous approximation of the contact is not valid, and only a few atoms are involved. In this scenario, the filament can be represented by a graph depicting the adjacency of atoms and the overlap between atomic orbitals. Using the theory of quantum graphs with locally diffusive node scattering, we calculate the scattering amplitude of charge carriers on this graph and explore the interplay between filamentary formation and quantum transport effects.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Uncovering an Interfacial Band Resulting from Orbital Hybridization in Nickelate Heterostructures

The interaction of atomic orbitals at the interface of perovskite oxide heterostructures has been investigated for its profound impact on the band structures and electronic properties, giving rise to unique electronic states and a variety of tunable functionalities. In this study, we conducted an extensive investigation of the optical and electronic properties of epitaxial NdNiO 3 thin films grown on a series of single crystal substrates. Unlike films synthesized on other substrates, NdNiO 3 on SrTiO 3 (NNO/STO) gives rise to a unique band structure which features an additional unoccupied band situated above the Fermi level. Our comprehensive investigation, which incorporated a wide array of experimental techniques and density functional theory calculations, revealed that the emergence of the interfacial band structure is primarily driven by the orbital hybridization between Ti 3d orbitals of the STO substrate and O 2p orbitals of the NNO thin film. Furthermore, exciton peaks have been detected in the optical spectra of the NNO/STO film, attributable to the pronounced electron-electron (e-e) and electron-hole (e-h) interactions propagating from the STO substrate into the NNO film. Further, these findings underscore the substantial influence of interfacial orbital hybridization on the electronic structure of oxide thin-films, thereby offering key insights into tuning their interfacial properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Tracing Long-Lived Atomic Coherences Generated via Molecular Conical Intersections

Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections, which generate coherences between electronic states in molecules. We show with accurate calculations performed on gas-phase methyl iodide that electronic coherences of spin-orbit-split states persist in atomic iodine after dissociation. Our simulation predicts a maximum magnitude of vibronic coherence in the molecular regime of 0.75% of the initially photoexcited state population. Upon dissociation, one-third of this coherence magnitude is transferred to a long-lived atomic coherence where vibrational decoherence can no longer occur. To trace these dynamics, we propose a tabletop experimental approach—heterodyned attosecond four-wave-mixing spectroscopy. This technique can temporally resolve small electronic coherence magnitudes and reconstruct the full complex coherence function via phase cycling. Hence, heterodyned attosecond four-wave-mixing spectroscopy leads the way to a complete understanding and optimal control of spin-orbit-coupled electronic states in photochemistry.

Chemical Physics↗
DOE OSTI2025

Energetic and Electronic Properties of AcX and LaX (X = O and F)

The bonding and spectroscopic properties of LaX and AcX (X = O and F) diatomic molecules were studied by highlevel ab initio CCSD(T) and SO-CASPT2 electronic structure calculations. Bond dissociation energies (BDEs) were calculated at the Feller−Peterson−Dixon (FPD) level. Potential energy curves and spectroscopic constants for the lowest-lying spin−orbit Ω states were obtained at the SO-CASPT2/aQ-DK level. A dense manifold of excited states was described for the monofluorides with the ground states well separated from the excited states. The spectroscopic parameters were in good agreement with those reported experimentally for LaO and LaF. For the diatomic molecules containing actinides, no experimental data of these parameters was found, but the results were consistent with other high-level calculations. The BDEs calculated at the FPD level were 791.3 (LaO), 705.2 (AcO), 650.0 (LaF), and 678.6 (AcF) kJ/ mol. The NBO analysis showed that the monofluorides are essentially ionic, which explains why the BDE(AcF) is higher than BDE(LaF); for the monoxides, covalent contributions involving the d orbitals of the metal and the p orbitals of the oxygen are stronger for LaO than AcO, which explains the higher BDE for LaO. Finally, the bond orders are predicted to be 2 for LaF and AcF, 3 for AcO, and higher than 3 for LaO.

Basis sets↗
DOE OSTI2025

A Thorough Characterization of the Tellurocyanate Anion

Tellurocyanate, [TeCN] − , is the heaviest group 16 congener of the cyanate anion, [OCN] − . Due to the relative instability of the C─Te bond, tellurocyanate chemistry has seen only scarce attention. Here, we present the facile synthesis and thorough characterization of [K@crypt-222][TeCN]. The anion is essentially linear with interatomic distances C─N = 1.150(6)Å and C─Te = 2.051(4)Å, thus approximating a C≡N triple bond and for C─Te a bond order between 1 and 2. Fully 13 C and 15 N labeled [Te 13 C 15 N] − allowed for the extraction of chemical shifts and all possible coupling constants ( 13 C = 77.8 ppm, 15 N = 285.7 ppm, 125 Te = −566 ppm, 1 J 13C-15N = 8 Hz, 1 J 13C-125Te = 748 Hz, 2 J1 5N-125Te = 55 Hz), which were also determined independently by quantum chemical calculations. In the series [ChCN] − (Ch = O─Te), [TeCN] − shows the strongest spin-orbit coupling (SOC) induced heavy-atom effect on the light-atom shielding (SO-HALA-effect). In contrast, 15 N shifts are also well described without considering relativistic effects and/or SOC. Negative-ion photoelectron spectroscopy was used to extract the electron affinity (EA = 3.034 eV) and spin-orbit splitting (3807 cm −1 ) of [TeCN] • . These values continue the trends of falling EA and rising SOC in the series [ChCN] • .

Bonding analysis↗