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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 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Demonstration of a MOT in a sub-millimeter membrane hole

Abstract We demonstrate the generation of a cold-atom ensemble within a sub-millimeter diameter hole in a transparent membrane, a so-called “membrane MOT”. With a sub-Doppler cooling process, the atoms trapped by the membrane MOT are cooled down to 10 $$\upmu$$ μ K. The atom number inside the unbridged/bridged membrane hole is about $$10^4$$ 10 4 to $$10^5$$ 10 5 , and the $$1/e^2$$ 1 / e 2 -diameter of the MOT cloud is about 180 $$\upmu$$ μ m for a 400 $$\upmu$$ μ m-diameter membrane hole. Such a membrane device can, in principle, efficiently load cold atoms into the evanescent-field optical trap generated by the suspended membrane waveguide for strong atom-light interaction and provide the capability of sufficient heat dissipation at the waveguide. This represents a key step toward the photonic atom trap integrated platform (ATIP).

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Machine learning molecular dynamics simulations toward exploration of high-temperature properties of nuclear fuel materials: case study of thorium dioxide

Predicting materials properties of nuclear fuel compounds is a challenging task in materials science. Their thermodynamical behaviors around and above the operational temperature are essential for the design of nuclear reactors. However, they are not easy to measure, because the target temperature range is too high to perform various standard experiments safely and accurately. Moreover, theoretical methods such as first-principles calculations also suffer from the computational limitations in calculating thermodynamical properties due to their high calculation-costs and complicated electronic structures stemming from f-orbital occupations of valence electrons in actinide elements. Here, we demonstrate, for the first time, machine-learning molecular-dynamics to theoretically explore high-temperature thermodynamical properties of a nuclear fuel material, thorium dioxide. The target compound satisfies first-principles calculation accuracy because f-electron occupation coincidentally diminishes and the scheme meets sampling sufficiency because it works at the computational cost of classical molecular-dynamics levels. We prepare a set of training data using first-principles molecular dynamics with small number of atoms, which cannot directly evaluate thermodynamical properties but captures essential atomistic dynamics at the high temperature range. Then, we construct a machine-learning molecular-dynamics potential and carry out large-scale molecular-dynamics calculations. Consequently, we successfully access two kinds of thermodynamic phase transitions, namely the melting and the anomalous λ transition induced by large diffusions of oxygen atoms. Furthermore, we quantitatively reproduce various experimental data in the best agreement manner by selecting a density functional scheme known as SCAN. Our results suggest that the present scale-up simulation-scheme using machine-learning techniques opens up a new pathway on theoretical studies of not only nuclear fuel compounds, but also a variety of similar materials that contain both heavy and light elements, like thorium dioxide.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

One-colour (~220 nm) resonance-enhanced (S 1 –S 0 ) multi-photon dissociation of acetylene: probe of the C 2 A 1 Π u – X 1 Σ + g band by frequency-modulation spectroscopy

In a recent paper, we demonstrated that one-colour (~220 nm), resonance-enhanced (S 1 –S 0 ), photodissociation of acetylene generates strong $C_2$ Swan band ($d^3Π_g–a^3Π_u$) and $C_2$ Deslandres-d'Azambuja band ($C^1Π_g–A^1Π_u$) fluorescence, and long-lived (>3 µs) fluorescence from an electronically-excited $C_2$H * species. It was not known whether the $C_2A^1Π_u$ and $X^1Σ^+_g$ states are also directly populated in this process. In this paper, multiple vibration-rotation transitions between the $C_2A$-state v = 2 and the X-state v = 0 level are examined by time-resolved frequency-modulation (FM) spectroscopy. The photolysis laser wavelength is tuned into resonance at the one-photon level with S 1 –S 0 transitions that populate individual rotational levels of the S 1 $_{trans}$-conformer $3^2,3^3,$ and $3^4$ vibrational states. By comparing the phase of the FM signals from the $C_2A–X$ transitions with that from the Rb D 1 -line absorption transition, we determine that, for all of the probed A–X transitions, the X-state level is more populated than the A-state level. We propose that the acetylene S 1 level is excited by the second photon to an acetylene dissociation precursor state, which undergoes sequential C-H bond-breaking to produce the $C_2X$ state. The dissociation precursor is assigned as the $1^1B_g(trans-bent)/1^1B_1(cis-bent)$ valence state, which correlates to a doubly-excited configuration, $(1π_u)^2(1π_g)^2$, at linear geometry. Based on the rotational distributions of the $C_2X$-state fragments, we believe that at least one of the transition states involved in the photolysis via S 1 $3^4$ has a larger CC-H bend-angle for the departing H-atom than that involved in the S 1 $3^2$ and $3^3$ photolysis.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Towards C P -violation studies on superheavy molecules: Theoretical and experimental perspectives

Molecules containing superheavy atoms can be artificially created to serve as sensitive probes to study symmetry-violating phenomena. Here, we provide detailed theoretical studies of quantities relevant to the electron electric dipole moment (eEDM) and nucleus-electron scalar-pseudoscalar interactions in diatomic molecules containing superheavy lawrencium nuclei. The sensitivity to parity and time (or, equivalently, CP) reversal violating properties is studied for different neutral and ionic molecules. The effective electric fields in these systems are found to be about 3–4 times larger than other known molecules on which eEDM experiments are being performed. Similarly, these superheavy molecules exhibit an enhancement of more than 3 times for CP-violating scalar-pseudoscalar nucleus-electron interactions. Our preliminary analysis using the Woods-Saxon nuclear model also demonstrates that these results are sensitive to the diffuse surface interactions inside the Lr nucleus. We also briefly comment on some experimental aspects by discussing the production of these systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Superfluid transition temperature and fluctuation theory of spin-orbit- and Rabi-coupled fermions with tunable interactions

Here, we obtain the superfluid transition temperature of equal Rashba-Dresselhaus spin-orbit- and Rabi-coupled Fermi superfluids, from the Bardeen-Cooper-Schrieffer (BCS) to Bose-Einstein condensate (BEC) regimes in three dimensions for tunable s-wave interactions. In the presence of Rabi coupling, we find that spin-orbit coupling enhances (reduces) the critical temperature in the BEC (BCS) limit. For fixed interactions, we show that spin-orbit coupling can convert a first-order (discontinuous) phase transition into a second-order (continuous) phase transition, as a function of Rabi coupling. We derive the Ginzburg-Landau free energy to sixth power in the superfluid order parameter to describe both continuous and discontinuous phase transitions as a function of spin-orbit and Rabi couplings. Lastly, we develop a time-dependent Ginzburg-Landau fluctuation theory for an arbitrary mixture of Rashba and Dresselhaus spin-orbit couplings at any interaction strength.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Tunneling magnetoresistance in MgO tunnel junctions with Fe-based leads in empirically corrected density functional theory

The minority-spin Fe/MgO interface states are at the Fermi level in density functional theory (DFT), but experimental evidence and GW calculations place them slightly higher in energy. This small shift can strongly influence tunneling magnetoresistance (TMR) in junctions with a thin MgO barrier and its dependence on the concentration of Co in the electrodes. Here, in this study, an empirical potential correction to DFT is introduced to shift the interface states up to match the tunnel spectroscopy data. With this shift, TMR in Fe/MgO/Fe junctions exceeds 800% and 3000% at 3 and 4 monolayers (ML) of MgO, respectively. We further consider the effect of alloying of the Fe electrodes with up to 30% Co or 10% V, treating them in the coherent potential approximation (CPA). Alloying with Co broadens the interface states and brings a large incoherent minority-spin spectral weight to the Fermi level. Alloying with V brings the minority-spin resonant states close to the Fermi level. However, in both cases the minority-spin spectral weight at the Fermi level resides primarily at the periphery of the Brillouin zone, which is favorable for spin filtering. Using convolutions of k II -resolved barrier densities of states calculated in CPA, it is found that TMR is strongly reduced by alloying with Co or V but still remains above 500% at 4 ML of MgO up to 30% of Co or 5% V. At 5 ML, the TMR increases above 1000% in all systems considered. However, while TMR declines sharply with increasing bias up to 0.2 eV in the tunnel junctions with pure Fe leads, it remains almost constant up to 0.5 eV if leads are alloyed with Co.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Transition energy measurements of the X-ray lines of neon-like europium

Here, we report the measurements of the n = 3 → n = 2 L-shell X-ray transitions of neon-like Eu 53+ . These include all seven allowed electric dipole (E1) transitions, five electric quadrupole (E2) transitions, and one magnetic quadrupole (M2) transition. The measurements were carried out at the EBIT-I electron beam ion trap facility at Livermore using an X-ray calorimeter. The measured values agree with many-body perturbation theory calculations within the experimental uncertainties. This includes the transitions that involve a 2s electron and that are, therefore, strongly affected by quantum electrodynamical effects.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Measurements of the L-shell X-ray emission of fluorine-like europium

Measurements of the L-shell X-ray emission of fluorine-like europium ions (Eu 54+ ) were made under controlled laboratory conditions on the EBIT-I electron beam ion trap at Livermore using an X-ray calorimeter, extending such measurements to the middle of the rare earth elements. Comparing the calorimeter spectra with atomic data from the flexible atomic code, we have identified and analyzed several prominent n = 3 → n = 2 transitions, including one two-electron, one-photon core changing transition and one electric quadrupole transition. We find that the measured energies are typically up to several eV higher than predicted.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

The Nuclei Of Atoms In The Third Period Of The Periodic Table Of Elements (Monograph No.3)

Nuclei are shown for the elements sodium, magnesium, aluminum, silicon, phosphorus, sulphur, chlorine, and argon. Individual nucleons are not identified as protons or neutrons. Nucleons are illustrated using a sphere schematic of the wave functions of singular, linear, and tetrahedral nucleon arrangements. Nucleon arrangements in protium, deuteron, triton, helion, and alpha are shown as building blocks in the nuclei of elements in the third period of the periodic table of elements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Boson Fermion Nuclei Energy Levels In The Third Period Of The Periodic Table Of Elements (Monograph No.5)

The boson fermion nucleus (BFN) energy level is shown for sodium, magnesium, aluminum, silicon, phosphorus, sulphur, chlorine, and argon. The BFN energy levels are compared to the energy levels in the shell nuclear model. Individual nucleon fermions in the BFN make minor contributions to the nucleus energy level. Nucleons rearrange into boson structures during stellar nucleosynthesis and condense into the lowest-level energy state. Deconstruction of the BFN structure and conversion to a shell or liquid-drop model brings about a higher energy state. This is not favored in nature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

The Generality of the GUGA MRCI Approach in COLUMBUS for Treating Complex Quantum Chemistry

The core part of the program system COLUMBUS allows highly efficient calculations using variational multireference (MR) methods in the framework of configuration interaction with single and double excitations (MR-CISD) and averaged quadratic coupled-cluster calculations (MR-AQCC), based on uncontracted sets of configurations and the graphical unitary group approach (GUGA). The availability of analytic MR-CISD and MR-AQCC energy gradients and analytic nonadiabatic couplings for MR-CISD enables exciting applications including, e.g., investigations of π-conjugated biradicaloid compounds, calculations of multitudes of excited states, development of diabatization procedures, and furnishing the electronic structure information for on-the-fly surface nonadiabatic dynamics. With fully variational uncontracted spin-orbit MRCI, COLUMBUS provides a unique possibility of performing high-level calculations on compounds containing heavy atoms up to lanthanides and actinides. Crucial for carrying out all of these calculations effectively is the availability of an efficient parallel code for the CI step. Configuration spaces of several billion in size now can be treated quite routinely on standard parallel computer clusters. Emerging developments in COLUMBUS, including the all configuration mean energy multiconfiguration self-consistent field method and the graphically contracted function method, promise to allow practically unlimited configuration space dimensions. Spin density based on the GUGA approach, analytic spin-orbit energy gradients, possibilities for local electron correlation MR calculations, development of general interfaces for nonadiabatic dynamics, and MRCI linear vibronic coupling models conclude this overview.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Temperature-dependent rotationally inelastic collisions of OH – and He

We have studied the fundamental rotational relaxation and excitation collision of OH – J = 0 ↔ 1 with helium at different collision energies. Using state-selected photodetachment in a cryogenic ion trap, the collisional excitation of the first excited rotational state of OH – has been investigated and absolute inelastic collision rate coefficients have been extracted for collision temperatures between 20 and 35 K. Furthermore, the rates are compared with accurate quantum scattering calculations for three different potential-energy surfaces. Good agreement is found within the experimental accuracy, but the experimental trend of increasing collision rates with temperature is only in part reflected in the calculations.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Absolute dissociative electron attachment cross-section measurement of difluoromethane

Dissociative electron attachment (DEA) to difluoromethane (CH 2 F 2 ) has been studied in the electron energy range of 0 to 16 eV. Two resonant states around 2 and 11.4 eV leading to three different fragment anions (F - , CHF - , and F 2 - ) are observed. Ion-yield curves of the negative ions help us to locate the position of the resonant states. In the ion-yield curve of F - ions, one small hump near 9.8 eV followed by a peak around 15.2 eV is also observed. Absolute DEA cross sections of the F - ion is measured by using the well-known relative flow technique. Dissociation channels associated with each resonant states are identified by density-functional theory (DFT) calculations of the threshold energies. The theory matches quite well within the experimental uncertainty.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Strong-field ionization of plasmonic nanoparticles

We modeled strong-field ionization of metal nanoparticles by intense infrared laser pulses, accounting for and distinguishing in photoelectron (PE) momentum distributions the effects of PE correlation, PE–residual-charge interactions, PE rescattering and recombination, and transient laser-induced plasmonic fields. Our numerical results for 5-, 30-, and 70-nm-diameter gold nanospheres and peak laser-pulse intensities of 8.0×10 12 and 1.2×10 13 W/cm 2 show how PE velocity-map images are distinctly shaped by PE Coulomb repulsion, residual-charge accumulations, and plasmonic near fields. In contrast to gaseous atomic targets and dielectric nanoparticles, we find very large PE cutoff energies, for both directly emitted and rescattered PEs, that exceed the incident laser-pulse ponderomotive energy by two orders of magnitude.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Imaging ring-current wave packets in the helium atom

We study the reconstruction of a wave packet and the corresponding electron dynamics in an atom via photoelectron angular distributions (PADs) in a pump-probe scheme as a function of time delay. The method is applied to the superposition of ground and one or two excited states in helium atom representing field-free charge migrations on the attosecond timescale in form of ring currents around the core. It is based on the interference between one- and two-photon transitions from ground and excited states into the continuum. In the reconstruction predictions of first- and second-order perturbation theory are used to determine the unknown phases and amplitudes from the PADs, which we simulate via solutions of the time-dependent Schrödinger equation in single-active-electron approximation. Results of calculations show that the reconstruction technique works well for peak laser intensities less than 10 13 W/cm 2 . Knowledge of the electric field of the probe pulse is required with shot-to-shot variations of carrier-to-envelope phase and peak intensity of up to 10% and 20%, respectively. The relevance of different one- and two-photon pathways for the reconstruction as a function of peak intensity and pulse duration is analyzed—specifically their role for ultrashort probe pulses with broad bandwidths.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Uncovering extreme nonlinear dynamics in solids through time-domain field analysis

Time-domain analysis of harmonic fields with sub-cycle resolution is now experimentally viable due to the emergence of sensitive, on-chip techniques for petahertz-scale optical-field sampling. We demonstrate how such a time-domain, field-resolved analysis uncovers the extreme nonlinear electron dynamics responsible for high-harmonic generation within solids. Time-dependent density functional theory was used to simulate harmonic generation from a solid-state band-gap system driven by near- to mid-infrared waveforms. Particular attention was paid to regimes where both intraband and interband emission mechanisms play a critical role in shaping the nonlinear response. We show that a time-domain analysis of the harmonic radiation fields identifies the interplay between intra- and interband dynamical processes underlying the nonlinear light generation. With further analysis, we show that changes to the dominant emission regime can occur after only slight changes to the peak driving intensity and central driving wavelength. Furthermore, time-domain analysis of harmonic fields also reveals, for the first time, the possibility of rapid changes in the dominant emission mechanism within the temporal window of the driving pulse envelope. Finally, we examine the experimental viability of performing time-domain analysis of harmonic fields with sub-cycle resolution using realistic parameters.

74 ATOMIC AND MOLECULAR PHYSICS↗