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DOE OSTI2020

Microwave measurements of the high magnetic field vortex motion pinning parameters in Nb$_3$Sn

The high frequency vortex motion in Nb3Sn was analyzed in this work up to 12 T. We used a dielectric loaded resonator tuned at 15 GHz to evaluate the surface impedance Z of a Nb3Sn bulk sample (24.8 at.%Sn). From the field induced variation of Z, the high frequency vortex parameters (the pinning constant k p , the depinning frequency ν p and the flux flow resistivity ρ ff ) were obtained over a large temperature and field range; their field and temperature dependencies were analyzed. Comparison with other superconducting materials shows that high frequency applications in strong magnetic fields are also feasible with Nb3Sn. In the present work, we report the first measurements about the microwave response in Nb3Sn in strong magnetic fields.

Alimenti, Andrea↗

DOE OSTI2020

Structural modeling and dynamic analysis of condensate storage tanks in nuclear power plants

Condensate storage tanks (CSTs) in nuclear power plants (NPPs) are classified as critical equipment capable of surviving strong shaking in a design basis earthquake to assure the ability to subsequently provide cooling water. Structural modeling and dynamic analysis of CSTs are complicated due to fluid-structure interaction (FSI) and coupling issues, which could have significant effects on seismic response. The capability of a number of approximate models to capture seismic response is investigated using dynamic analysis results from detailed finite element models. Modal analyses and time history analyses are carried out using both 2D and 3D models to predict the dynamic behavior of CSTs as a function of ground motion intensity. Although 2D simplified models can be used to quickly evaluate the dynamic response of CSTs when there is substantial margin to failure, a detailed 3D model is required when it is necessary to examine a limit state associated with the failure mode of the tank. The findings show good agreement between the natural frequencies of convective modes determined from the 2D and 3D CST models. The difference between the frequencies of impulsive modes were found to be equal to or less than 25%.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Beyond the Condon limit: Condensed phase optical spectra from atomistic simulations

While dark transitions made bright by molecular motions determine the optoelectronic properties of many materials, simulating such non-Condon effects in condensed phase spectroscopy remains a fundamental challenge. We derive a Gaussian theory to predict and analyze condensed phase optical spectra beyond the Condon limit. Our theory introduces novel quantities that encode how nuclear motions modulate the energy gap and transition dipole of electronic transitions in the form of spectral densities. By formulating the theory through a statistical framework of thermal averages and fluctuations, we circumvent the limitations of widely used microscopically harmonic theories, allowing us to tackle systems with generally anharmonic atomistic interactions and non-Condon fluctuations of arbitrary strength. We show how to calculate these spectral densities using first-principles simulations, capturing realistic molecular interactions and incorporating finite-temperature, disorder, and dynamical effects. Our theory accurately predicts the spectra of systems known to exhibit strong non-Condon effects (phenolate in various solvents) and reveals distinct mechanisms for electronic peak splitting: timescale separation of modes that tune non-Condon effects and spectral interference from correlated energy gap and transition dipole fluctuations. We further introduce analysis tools to identify how intramolecular vibrations, solute–solvent interactions, and environmental polarization effects impact dark transitions. Moreover, we prove an upper bound on the strength of cross correlated energy gap and transition dipole fluctuations, thereby elucidating a simple condition that a system must follow for our theory to accurately predict its spectrum.

Chemistry↗

DOE OSTI2020

Femtosecond stimulated Raman spectro-microscopy for probing chemical reaction dynamics in solid-state materials

Femtosecond stimulated Raman spectroscopy (FSRS) is a chemically specific vibrational technique that has the ability to follow structural dynamics during photoinduced processes such as charge transfer on the ultrafast timescale. FSRS has a strong background in following structural dynamics and elucidating chemical mechanisms; however, its use with solid-state materials has been limited. As photovoltaic and electronic devices rely on solid-state materials, having the ability to track the evolving dynamics during their charge transfer and transport processes is crucial. Following the structural dynamics in these solid-state materials will lead to the identification of specific chemical structures responsible for various photoinduced charge transfer reactions, leading to a greater understanding of the structure–function relationships needed to improve upon current technologies. Furthermore, isolating the specific nuclear motions and molecular structures that drive a desired physical process will provide a chemical blueprint, leading to the rational design and fabrication of efficient electronic and photovoltaic devices. In this perspective, we discuss technical challenges and experimental developments that have facilitated the use of FSRS with solid-state samples, explore previous studies that have identified structure–function relationships in charge transfer reactions, and analyze the future developments that will broaden and advance the field.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

From weak antilocalization to Kondo scattering in a magnetic complex oxide interface

Quantum corrections to electrical resistance can serve as sensitive probes of the magnetic landscape of a material. For example, interference between time-reversed electron paths gives rise to weak localization effects, which can provide information about the coupling between spins and orbital motion, while the Kondo effect is sensitive to the presence of spin impurities. In this work, we use low-temperature magnetotransport measurements to reveal a gradual transition from weak antilocalization (WAL) to Kondo scattering in the quasi-two-dimensional electron gas formed at the interface between SrTiO 3 and the Mott insulator NdTiO 3 . This transition occurs as the thickness of the NdTiO 3 layer is increased. Analysis of the Kondo scattering and WAL points to the presence of atomic-scale magnetic impurities coexisting with nanoscale magnetic regions that affect transport via a strong magnetic exchange interaction. This leads to distinct magnetoresistance behaviors that can serve as a sensitive probe of magnetic properties in two dimensions.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Synchronization effects on rest frame energy and momentum densities in the proton

We obtain two-dimensional relativistic densities and currents of energy and momentum in a proton at rest. These densities are obtained at surfaces of fixed light front time, which physically corresponds to using an alternative synchronization convention. Mathematically, this is done using tilted light front coordinates, which consist of light front time and ordinary spatial coordinates. In this coordinate system, all 16 components of the energy-momentum tensor (EMT) obtain clear physical interpretations, and the nine Galilean components reproduce results from standard light front coordinates. We find angular modulations in several densities that are absent in the corresponding instant form results, which are explained as optical effects arising from using fixed light front time when motion is present within the target. Additionally, transversely polarized spin-half targets exhibit an energy dipole moment—which evaluates to −1/4 for all targets if the Belinfante EMT is used, but which is target dependent and vanishes for pointlike fermions if the asymmetric EMT is instead used.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

The derivation of CRSS in pure Ti and Ti-Al alloys

The work focuses on the determination of the critical resolved shear stress (CRSS) in titanium (Ti) and titanium-aluminum (Ti-Al) alloys, influenced by an array of factors such as non-symmetric fault energies and minimum energy paths, dislocation core-widths, short-range order (SRO) effects which alter the local atomic environment, and tension-compression (T-C) asymmetry affected by intermittent slip motion. To address these multifaceted complexities, an advanced theory has been developed, offering an in-depth understanding of the mechanisms underlying slip behavior. The active slip systems in these materials are basal, prismatic, and pyramidal planes, with the latter involving both $\langle$a$\rangle$ and $\langle$c + a$\rangle$ dislocations. Each slip system is characterized by distinct Wigner-Seitz cell configurations for misfit energy calculations, varying partial dislocation separation distances, and unique dislocation trajectories—all critical to precise CRSS calculations. The theoretical CRSS results were validated against a comprehensive range of experimental data, demonstrating a strong agreement and underscoring the model's efficacy.

Critical stress↗

DOE OSTI2025

Deformation and Collectivity in Doubly Magic 208 Pb

Lead-208 is the heaviest known doubly magic nucleus and its structure is therefore of special interest. Despite this magicity, which acts to provide a strong restorative force toward sphericity, it is known to exhibit both strong octupole correlations and some of the strongest quadrupole collectivity observed in doubly magic systems. In this Letter, we employ state-of-the-art experimental equipment to conclusively demonstrate, through four Coulomb-excitation measurements, the presence of a large, negative, spectroscopic quadrupole moment for both the vibrational octupole 3$^{−}_{1}$ and quadrupole 2$^{+}_{1}$ state, indicative of a preference for prolate deformation of the states. The observed quadrupole moment is discussed in the context of the expected splitting of the 3 − ⊗3 − two-phonon states, due to the coupling of the quadrupole and octupole motion. These results are compared with theoretical values from three different methods, which are unable to reproduce both the sign and magnitude of this deformation. Thus, in spite of its well-studied nature, 208 Pb remains a puzzle for our understanding of nuclear structure.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Coupled cluster and dislocation dynamics modeling of microstructure evolution in irradiated materials

We develop here a coupled cluster and dislocation dynamics framework to study the microstructure evolution of irradiated materials. The framework not only accounts for the three dimensional diffusion of radiation-generated clusters, but also their interaction with dislocation networks and the resultant climb motion of discrete dislocations within finite crystals. The framework is solved with a superposition solution scheme, and is applied to investigate the evolution of the irradiation-induced dislocation loops in zirconium (Zr), considering the effects of various bias factors including the diffusion anisotropy difference (DAD) of interstitials and interstitial clusters, the dislocation bias of defects to discrete dislocation segments, and the production bias of defects from the radiation cascade. We find that the DAD is the most critical factor influencing the kinetics of the loop evolution in Zr, while the recombination/interaction of mobile defects can induce a strong spatial dependence of the loop evolution together with the DAD. Here, the method is also adopted to study the evolution of interstitial $\langle$a$\rangle$ and vacancy $\langle$c$\rangle$ dislocation loop ensembles consistent with the microstructure observed during irradiation-induced growth of Zr. Our findings not only reveal the spatial dependence of the size and ellipticity of the dislocation loops, but also suggest a limit on the anisotropy factor of interstitials to reproduce the co-growth of $\langle$a$\rangle$ and $\langle$c$\rangle$ loops in zirconium, in good agreement with experimental observations and other simulation results.

Bias factors↗

DOE OSTI2020

Detailed space–time variations of the seismic response of the shallow crust to small earthquakes from analysis of dense array data

SUMMARY We compute high-resolution space–time variations of subsurface seismic properties from autocorrelation functions (ACF’s) of noise and local earthquakes, recorded by the Sage Brush Flat dense array deployed around the Clark branch of the San Jacinto fault. The resolved temporal changes are referred to as apparent velocity changes because they reflect both nonlinear response and variations of material properties such as cracking and damage. Apparent velocity changes are estimated at four frequency bands (10–15, 10–20, 15–30 and 20–40 Hz) for two local earthquake data sets. In one analysis, ACF’s from P- and S-wave windows of 31 small events with magnitudes below 3.1 are used to compute the apparent velocity variations with respect to the mean ACF of each phase, and we also use the mean ACF of noise data as reference to estimate the changes. In a further analysis, the temporal evolution of properties is computed using moving time windows in continuous waveform over one-hour long data with noise and earthquake signals. The apparent velocity changes and recovery times are frequency dependent and present a strong spatial variability across the array. The resolved changes are larger and recovery time shorter with data associated with higher frequencies. At frequencies larger than 15 Hz, and using the mean ACF of noise data as a reference, the apparent average velocity changes across the array during the passage of the P and S waves from the small local events are 2.5 per cent and 6 per cent, respectively. The apparent velocity changes decrease by one order of magnitude when the earthquake data are used as a reference. The relatively large changes in response to very low ground motion have important implications on nonlinear processes involving degradation and healing of the subsurface material during common earthquake shaking.

Geochemistry & Geophysics↗

DOE OSTI2021

The Stars Kepler Missed: Investigating the Kepler Target Selection Function Using Gaia DR2

The Kepler Mission revolutionized exoplanet science and stellar astrophysics by obtaining highly precise photometry of over 200,000 stars over 4 yr. A critical piece of information to exploit Kepler data is its selection function, since all targets had to be selected from a sample of half a million stars on the Kepler CCDs using limited information. Here we use Gaia DR2 to reconstruct the Kepler selection function and explore possible biases with respect to evolutionary state, stellar multiplicity, and kinematics. We find that the Kepler target selection is nearly complete for stars brighter than Kp < 14 mag and was effective at selecting main-sequence stars, with the fraction of observed stars decreasing from 95% to 60% between 14 < Kp < 16 mag. We find that the observed fraction for subgiant stars is only 10% lower, confirming that a significant number of subgiants selected for observation were believed to be main-sequence stars. Conversely we find a strong selection bias against low-luminosity red giant stars (R ≈ 3–5R {sub ⊙}, T {sub eff} ≈ 5500 K), dropping from 90% at Kp = 14 mag to below 30% at Kp = 16 mag, confirming that the target selection was efficient at distinguishing dwarfs from giants. We compare the Gaia Re-normalized Unit Weight Error (RUWE) values of the observed and nonobserved main-sequence stars and find a difference in elevated (>1.2) RUWE values at ∼σ significance, suggesting that the Kepler target selection shows some bias against either close or wide binaries. We furthermore use the Gaia proper motions to show that the Kepler selection function was unbiased with respect to kinematics.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Theoretical framework for new magnetic materials for quantum computing and information storage. Final report for the Award No. DE-SC0018910

The focus of this grant was on molecular magnetic materials for information storage and quantum computing. We have been developing robust, first-principle methods for computing relevant electronic and magnetic properties of molecular building blocks (SMMs) of novel magnetic materials and quantum computers. These tools enable theoretical modeling of SMMs’ behavior, facilitating the interpretation of experimental studies and aiding the design of novel magnetic materials. Our strategy is based on the spin-flip (SF) approach, which extends the hierarchy of black-box single-reference methods to strongly correlated systems. Specifically, we developed general scalable algorithms and computer codes for calculating molecular properties, with an emphasis on spin-related properties, such as zero-field splittings, hyperfine couplings, and g-tensors. While our primary focus was on SF wave functions and SF-TDDFT, the underlying theory and computer codes were formulated using reduced density matrices, such that these tools are applicable to a broader class of methods. To extend the scope of applicability of wave-function-based SF methods to larger systems, we developed reduced-scaling approaches for the equation-of-motion coupled-cluster (EOM-CC) methods and continue developing libtensor (our open-source general tensor contraction library for many-body methods). We carried out extensive benchmarks and also carried out several applications.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Lightwave terahertz quantum manipulation of nonequilibrium superconductor phases and their collective modes

In this work, we present a gauge-invariant density matrix description of nonequilibrium superconductor (SC) states with spatial and temporal correlations driven by intense terahertz (THz) lightwaves. We derive superconductor Bloch-Maxwell equations of motion that extend Anderson pseudospin models to include the Cooper pair center-of-mass motion and electromagnetic propagation effects. We thus describe quantum control of dynamical phases, collective modes, quasiparticle coherence, and high nonlinearities during cycles of carrier wave oscillations, which relates to our recent experiments. Coherent photogeneration of a nonlinear supercurrent with a dc component, achieved via condensate acceleration by an effective lightwave field, dynamically breaks the equilibrium inversion symmetry. Experimental signatures include high harmonic light emission at equilibrium-symmetry-forbidden frequencies, Rabi-Higgs collective modes and quasiparticle coherence, and nonequilibrium moving condensate states tuned by few-cycle THz fields. We use such lightwaves as an oscillating accelerating force that drives strong nonlinearities and anisotropic quasiparticle populations to control and amplify different classes of collective modes, e.g., damped oscillations, persistent oscillations, and overdamped dynamics via Rabi flopping. Recent phase-coherent nonlinear spectroscopy experiments can be modeled by solving the full nonlinear quantum dynamics including self-consistent light-matter coupling.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Collective dynamics and defect generation for Wigner crystal ratchets

Here we consider a two-dimensional Wigner crystal coupled to a quasi-one-dimensional asymmetric potential under ac or dc driving. As a function of electron density, substrate strength, and ac amplitude, we find that the system exhibits ordered and disordered pinned and dynamical states. Ratchet effects can appear under an applied ac drive and can be associated with pronounced structural changes from a disordered state to a one-dimensional smecticlike state. We observe a pinned phase, a diodelike ratchet where motion only occurs along the easy direction of the substrate asymmetry, a plastic ratchet where motion occurs in both directions but there is only a net drift in the easy direction, and an elastic ratchet where the system forms a crystal without plastic deformation that can still undergo ratcheting. At high filling, we find that there can be a ratchet reversal in which the net drift is along the hard direction of the substrate asymmetry. For weak disorder, there is an Aubry transition to a floating phase where the ratchet effects are lost. We map out the different dynamical phases as a function of substrate strength, filling, ac amplitude, and ac frequency. The ratchet effect on strong substrates is enhanced by thermal fluctuations, but is destroyed when the fluctuations become too large. Based on our results, we suggest other ways to detect Wigner crystals as well as methods for creating different types of devices to control disordered charge flow.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Monitoring Seasonal Shear Wave Velocity Changes in the Top 6 m at Garner Valley in Southern California With Borehole Data

Abstract Subsurface structures play important roles in seismic ground motion, crustal hydrology, stability of the built environment, and more. Constraining temporal changes of subsurface shear wave velocity ( V S ) can provide useful information to all these topics and the growing field of hydrological monitoring with seismic velocity. Using borehole records at Garner Valley, CA, we estimate seasonal subsurface V S variations from impulse response functions (IRFs) of earthquake data (2005–2018) along with IRFs and cross‐correlation of cross‐hole experiment data (2015–2018). The inferred V S variations are up to ∼25% in the top 6 m and ∼10% at 2–5 m in depth. The V S variations correlate strongly with the water table depth changes, suggesting that the changes are mostly due to fluctuations of pore pressure in the shallow material. The shallow velocity changes alter the near‐surface conditions, can affect seismic hazard estimation, and may be improperly attributed to deeper processes without careful analysis.

58 GEOSCIENCES↗

DOE OSTI2022

Blanco DECam Bulge Survey (BDBS)

The Blanco DECam Bulge Survey (BDBS) has imaged more than 200 square degrees of the southern Galactic bulge, providing photometry in the ugrizy filters for ~250 million unique stars. The presence of a strong foreground disk population, along with complex reddening and extreme image crowding, has made it difficult to constrain the presence of young and intermediate age stars in the bulge population. We employed an accurate cross-match of BDBS with the latest data release (EDR3) from the Gaia mission, matching more than 140 million sources with BDBS photometry and Gaia EDR3 photometry and astrometry. We relied on Gaia EDR3 astrometry, without any photometric selection, to produce clean BDBS bulge colour-magnitude diagrams (CMDs). Gaia parallaxes were used to filter out bright foreground sources, and a Gaussian mixture model fit to Galactic proper motions could identify stars kinematically consistent with bulge membership. We applied this method to 127 different bulge fields of 1 deg 2 each, with |$\ell$| ≤ 9.5 ° and –9.5 ° ≤ b ≤ –2.5 °. The astrometric cleaning procedure removes the majority of blue stars in each field, especially near the Galactic plane, where the ratio of blue to red stars is .10%, increasing to values ~20% at higher Galactic latitudes. We rule out the presence of a widespread population of stars younger than 2 Gyr. The vast majority of blue stars brighter than the turnoff belong to the foreground population, according to their measured astrometry. We introduce the distance between the observed red giant branch bump and the red clump as a simple age proxy for the dominant population in the field, and we confirm the picture of a predominantly old bulge. Further work is needed to apply the method to estimate ages to fields at higher latitudes, and to model the complex morphology of the Galactic bulge. We also produce transverse kinematic maps, recovering expected patterns related to the presence of the bar and of the X-shaped nature of the bulge.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Full radiator-perturber interaction in computer simulations of hydrogenic spectral line broadening by plasmas

Spectral line broadening by plasmas can be computed by solving the equation of motion for the dipole of the radiating system perturbed by a fluctuating potential obtained from computer simulations. Such calculations have relied on the multipole expansion of the radiator-plasma interaction often keeping only the dipole term. With increasing density, however, higher multipoles as well as plasma perturbers overlapping the bound electron wave functions are expected to become important. For hydrogenic systems, the atomic matrix elements of the full Coulomb and screened Coulomb interactions are given by analytical formulas. Using these results, a computer simulation approach that accounts for the full radiator-plasma interaction is developed. One benefit is the removal of inherent strong collision divergences in the multipole expansion approximation. Furthermore, it yields the plasma polarization shift produced by perturbers penetrating the wave function of the radiator bound electrons. Here, the model was applied to hydrogenic argon Ly-α , Ly- β , and Ly-$\gamma$ spectral lines in a dense argon plasma at free electron densities of 10 24 or 10 25 cm ⁻3 and temperature of $800$ $eV$ relevant to plasma diagnostic techniques for inertial confinement fusion implosions.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2025

Signatures of chiral superconductivity in rhombohedral graphene

Chiral superconductors are unconventional superconducting states that break time-reversal symmetry spontaneously and typically feature Cooper pairing at non-zero angular momentum. Such states may host Majorana fermions and provide an important platform for topological physics research and fault-tolerant quantum computing. Despite intensive search and prolonged studies of several candidate systems, chiral superconductivity has remained elusive so far. Here we report the discovery of robust unconventional superconductivity in rhombohedral tetralayer and pentalayer graphene without moiré superlattice effects. We observed two superconducting states in the gate-induced flat conduction bands with T c up to 300 mK and charge density n e down to 2.4 ×10 11 cm −2 in five devices. Spontaneous time-reversal-symmetry breaking (TRSB) owing to orbital motion of the electron is found and several observations indicate the chiral nature of these superconducting states, including: (1) in the superconducting state, R xx shows magnetic hysteresis in varying out-of-plane magnetic field B ⊥ —absent from all other superconductors; (2) the superconducting states are robust against in-plane magnetic field and are developed within a spin-polarized and valley-polarized quarter-metal (QM) phase; (3) the normal states show anomalous Hall signals at zero magnetic field and magnetic hysteresis. Here, we also observed a critical B ⊥ of 1.4 T, higher than any graphene superconductivity, which indicates a strong-coupling superconductivity close to the Bardeen–Cooper–Schrieffer (BCS)–Bose–Einstein condensate (BEC) crossover. Our observations establish a pure carbon material for the study of topological superconductivity, with the promise to explore Majorana modes and topological quantum computing.

36 MATERIALS SCIENCE↗