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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Isobar analog states (IAS), double isobar analog states (DIAS), configuration states (CS), and double configuration states (DCS) in halo nuclei. Halo isomers

It has been shown that IAS, DIAS, CS, and DCS can simultaneously have n-n, n-p, and p-p halo components in their wave functions. Differences in halo structure of the excited and ground states can result in the formation of isomers (halo-isomers). Both the Borromean and tango halo types can be observed for n-p configurations of atomic nuclei. The structure of the ground and excited states with different isospin quantum number in halo like nuclei is discussed. B(Mλ) and B(Eλ) for γ-transitions in {sup 6,7,8}Li, {sup 8,9,10}Be, {sup 8,10,11}B, {sup 10,11,12,13,14}C, {sup 13,14,15,16,17}N, {sup 15,16,17,19}O, and {sup 17}F are analyzed. Special attention is given to nuclei whose ground state does not exhibit halo structure but the excited state may have one.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2015

Representing the thermal state in time-dependent density functional theory

Classical molecular dynamics (MD) provides a powerful and widely used approach to determining thermodynamic properties by integrating the classical equations of motion of a system of atoms. Time-Dependent Density Functional Theory (TDDFT) provides a powerful and increasingly useful approach to integrating the quantum equations of motion for a system of electrons. TDDFT efficiently captures the unitary evolution of a many-electron state by mapping the system into a fictitious non-interacting system. In analogy to MD, one could imagine obtaining the thermodynamic properties of an electronic system from a TDDFT simulation in which the electrons are excited from their ground state by a time-dependent potential and then allowed to evolve freely in time while statistical data are captured from periodic snapshots of the system. For a variety of systems (e.g., many metals), the electrons reach an effective state of internal equilibrium due to electron-electron interactions on a time scale that is short compared to electron-phonon equilibration. During the initial time-evolution of such systems following electronic excitation, electron-phonon interactions should be negligible, and therefore, TDDFT should successfully capture the internal thermalization of the electrons. However, it is unclear how TDDFT represents the resulting thermal state. In particular, the thermal state is usually represented in quantum statistical mechanics as a mixed state, while the occupations of the TDDFT wavefunctions are fixed by the initial state in TDDFT. We work to address this puzzle by (A) reformulating quantum statistical mechanics so that thermodynamic expectations can be obtained as an unweighted average over a set of many-body pure states and (B) constructing a family of non-interacting (single determinant) TDDFT states that approximate the required many-body states for the canonical ensemble.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

State-to-state reaction dynamics of {sup 18}O+{sup 32}O{sub 2} studied by a time-dependent quantum wavepacket method

The title isotope exchange reaction was studied by converged time-dependent wave packet calculations, where an efficient 4th order split operator was applied to propagate the initial wave packet. State-to-state differential and integral cross sections up to the collision energy of 0.35 eV were obtained with {sup 32}O{sub 2} in the hypothetical j{sub 0} = 0 state. It is discovered that the differential cross sections are largely forward biased in the studied collision energy range, due to the fact that there is a considerable part of the reaction occurring with large impact parameter and short lifetime relative to the rotational period of the intermediate complex. The oscillations of the forward scattering amplitude as a function of collision energy, which result from coherent contribution of adjacent resonances, may be a sensitive probe for examining the quality of the underlying potential energy surface. A good agreement between the theoretical and recent experimental integral and differential cross sections at collision energy of 7.3 kcal/mol is obtained. However, the theoretical results predict slightly too much forward scattering and colder rotational distributions than the experimental observations at collision energy of 5.7 kcal/mol.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2019

Excited states via coupled cluster theory without equation-of-motion methods: Seeking higher roots with application to doubly excited states and double core hole states

Here, in this work, we revisited the idea of using the coupled-cluster (CC) ground state formalism to target excited states. Our main focus was targeting doubly excited states and double core hole states. Typical equation-of-motion (EOM) approaches for obtaining these states struggle without higher-order excitations than doubles. We showed that by using a non-Aufbau determinant optimized via the maximum overlap method, the CC ground state solver can target higher energy states. Furthermore, just with singles and doubles (i.e., CCSD), we demonstrated that the accuracy of ΔCCSD and ΔCCSD(T) (triples) far surpasses that of EOM-CCSD for doubly excited states. The accuracy of ΔCCSD(T) is nearly exact for doubly excited states considered in this work. For double core hole states, we used an improved ansatz for greater numerical stability by freezing core hole orbitals. The improved methods, core valence separation (CVS)-ΔCCSD and CVS-ΔCCSD(T), were applied to the calculation of the double ionization potential of small molecules. Even without relativistic corrections, we observed qualitatively accurate results with CVS-ΔCCSD and CVS-ΔCCSD(T). Remaining challenges in ΔCC include the description of open-shell singlet excited states with the single-reference CC ground state formalism as well as excited states with genuine multireference character. The tools and intuition developed in this work may serve as a stepping stone toward directly targeting arbitrary excited states using ground state CC methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Creating large Fock states and massively squeezed states in optics using systems with nonlinear bound states in the continuum

The quantization of the electromagnetic field leads directly to the existence of quantum mechanical states, called Fock states, with an exact integer number of photons. Despite these fundamental states being long-understood, and despite their many potential applications, generating them is largely an open problem. For example, at optical frequencies, it is challenging to deterministically generate Fock states of order two and beyond. Here, we predict the existence of an effect in nonlinear optics, which enables the deterministic generation of large Fock states at arbitrary frequencies. The effect, which we call an n-photon bound state in the continuum, is one in which a photonic resonance (such as a cavity mode) becomes lossless when a precise number of photons n is inside the resonance. Based on analytical theory and numerical simulations, we show that these bound states enable a remarkable phenomenon in which a coherent state of light, when injected into a system supporting this bound state, can spontaneously evolve into a Fock state of a controllable photon number. This effect is also directly applicable for creating (highly) squeezed states of light, whose photon number fluctuations are (far) below the value expected from classical physics (i.e., shot noise). In conclusion, we suggest several examples of systems to experimentally realize the effects predicted here in nonlinear nanophotonic systems, showing examples of generating both optical Fock states with large n (n > 10), as well as more macroscopic photonic states with very large squeezing, with over 90% less noise (10 dB) than the classical value associated with shot noise.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Involvement of a low-lying Rydberg state in the ultrafast relaxation dynamics of ethylene

We present a measurement of the time-resolved photoelectron kinetic energy spectrum of ethylene using 156 nm and 260 nm laser pulses. The 156 nm pulse first excites ethylene to the {sup 1}B{sub 1u} (ππ{sup ∗}) electronic state where 260 nm light photoionizes the system to probe the relaxation dynamics with sub-30 fs resolution. Recent ab initio calculations by Mori et al. [J. Phys. Chem. A 116, 2808-2818 (2012)] have predicted an ultrafast population transfer from the initially excited state to a low-lying Rydberg state during the relaxation of photoexcited ethylene. The measured photoelectron kinetic energy spectrum reveals wave packet motion on the valence state and shows indications that the low-lying π3s Rydberg state is indeed transiently populated via internal conversion following excitation to the ππ{sup ∗} state, supporting the theoretical predictions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Quantification of Steady-State Ion Transport through Single Conical Nanopores and a Nonuniform Distribution of Surface Charges

Electrostatic interactions of mobile charges in solution with the fixed surface charges are known to strongly affect stochastic sensing and electrochemical energy conversion processes at nanodevices or devices with nanostructured interfaces. The key parameter to describe this interaction, surface charge density (SCD), is not directly accessible at nanometer scale and often extrapolated from ensemble values. In this report, the steady-state current–voltage (i–V) curves measured using single conical glass nanopores in different electrolyte solutions are fitted by solving Poisson and Nernst–Planck equations through finite element approach. Both high and low conductivity state currents of the rectified i–V curve are quantitatively fitted in simulation at less than 5% error. The overestimation of low conductivity state current using existing models is overcome by the introduction of an exponential SCD distribution inside the conical nanopore. A maximum SCD value at the pore orifice is determined from the fitting of the high conductivity state current, while the distribution length of the exponential SCD gradient is determined by fitting the low conductivity state current. Quantitative fitting of the rectified i–V responses and the efficacy of the proposed model are further validated by the comparison of electrolytes with different types of cations (K + and Li + ). In conclusion, the gradient distribution of surface charges is proposed to be dependent on the local electric field distribution inside the conical nanopore.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2018

Behavior of the maximum likelihood in quantum state tomography

Quantum state tomography on a d-dimensional system demands resources that grow rapidly with d. They may be reduced by using model selection to tailor the number of parameters in the model (i.e., the size of the density matrix). Most model selection methods typically rely on a test statistic and a null theory that describes its behavior when two models are equally good. Here, we consider the loglikelihood ratio. Because of the positivity constraint ρ ≥ 0, quantum state space does not generally satisfy local asymptotic normality (LAN), meaning the classical null theory for the loglikelihood ratio (the Wilks theorem) should not be used. Thus, understanding and quantifying how positivity affects the null behavior of this test statistic is necessary for its use in model selection for state tomography. We define a new generalization of LAN, metric-projected LAN, show that quantum state space satisfies it, and derive a replacement for the Wilks theorem. In addition to enabling reliable model selection, our results shed more light on the qualitative effects of the positivity constraint on state tomography.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

F-state quenching with CH{sub 4} for buffer-gas cooled {sup 171}Y b{sup +} frequency standard

We report that methane, CH{sub 4}, can be used as an efficient F-state quenching gas for trapped ytterbium ions. The quenching rate coefficient is measured to be (2.8 ± 0.3) × 10{sup 6} s{sup −1} Torr{sup −1}. For applications that use microwave hyperfine transitions of the ground-state {sup 171}Y b ions, the CH{sub 4} induced frequency shift coefficient and the decoherence rate coefficient are measured as δν/ν = (−3.6 ± 0.1) × 10{sup −6} Torr{sup −1} and 1/T{sub 2} = (1.5 ± 0.2) × 10{sup 5} s{sup −1} Torr{sup −1}. In our buffer-gas cooled {sup 171}Y b{sup +} microwave clock system, we find that only ≤10{sup −8} Torr of CH{sub 4} is required under normal operating conditions to efficiently clear the F-state and maintain ≥85% of trapped ions in the ground state with insignificant pressure shift and collisional decoherence of the clock resonance.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2011

Quantification of terrestrial ecosystem carbon dynamics in the conterminous United States combining a process-based biogeochemical model and MODIS and AmeriFlux data

Satellite remote sensing provides continuous temporal and spatial information of terrestrial ecosystems. Using these remote sensing data and eddy flux measurements and biogeochemical models, such as the Terrestrial Ecosystem Model (TEM), should provide a more adequate quantification of carbon dynamics of terrestrial ecosystems. Here we use Moderate Resolution Imaging Spectroradiometer (MODIS) Enhanced Vegetation Index (EVI), Land Surface Water Index (LSWI) and carbon flux data of AmeriFlux to conduct such a study. First we modify the gross primary production (GPP) modeling in TEM by incorporating EVI and LSWI to account for the effects of the changes of canopy photosynthetic capacity, phenology and water stress. Second, we parameterize and verify the new version of TEM with eddy flux data. We then apply the model to the conterminous United States over the period 2000–2005 at a 0.05° × 0.05° spatial resolution. We find that the new version of TEM made improvement over the previous version and generally captured the expected temporal and spatial patterns of regional carbon dynamics. We estimate that regional GPP is between 7.02 and 7.78 PgC yr -1 and net primary production (NPP) ranges from 3.81 to 4.38 Pg Cyr -1 and net ecosystem production (NEP) varies within 0.08– 0.73 PgC yr -1 over the period 2000–2005 for the conterminous United States. The uncertainty due to parameterization is 0.34, 0.65 and 0.18 PgC yr -1 for the regional estimates of GPP, NPP and NEP, respectively. The effects of extreme climate and disturbances such as severe drought in 2002 and destructive Hurricane Katrina in 2005 were captured by the model. Lastly, our study provides a new independent and more adequate measure of carbon fluxes for the conterminous United States, which will benefit studies of carbon-climate feedback and facilitate policy-making of carbon management and climate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Non-equilibrium oxidation states of zirconium during early stages of metal oxidation

The chemical state of Zr during the initial, self-limiting stage of oxidation on single crystal zirconium (0001), with oxide thickness on the order of 1 nm, was probed by synchrotron x-ray photoelectron spectroscopy. Quantitative analysis of the Zr 3d spectrum by the spectrum reconstruction method demonstrated the formation of Zr 1+ , Zr 2+ , and Zr 3+ as non-equilibrium oxidation states, in addition to Zr 4+ in the stoichiometric ZrO 2 . This finding resolves the long-debated question of whether it is possible to form any valence states between Zr 0 and Zr 4+ at the metal-oxide interface. As a result, the presence of local strong electric fields and the minimization of interfacial energy are assessed and demonstrated as mechanisms that can drive the formation of these non-equilibrium valence states of Zr.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗