Search NASA⌕ Search

SEARCH · Search NASA

Results for “state specific”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Tracking Excited States in Wave Function Optimization Using Density Matrices and Variational Principles

We introduce an approach for finding individual excited states' energy stationary points in complete active space self-consistent field theory that is compatible with standard optimization methods and highly effective at overcoming difficulties due to root flipping and near-degeneracies. Inspired by both the maximum overlap method and recent progress in excited-state variational principles, our approach combines these ideas in order to track individual excited states throughout the orbital optimization process. In a series of tests involving root flipping, near-degeneracies, charge transfers, and double excitations, we show that this approach is more effective for state-specific optimization than either the naive selection of roots on the basis of energy ordering or a more direct generalization of the maximum overlap method. We offer evidence that this state-specific approach improves the performance of complete active space perturbation theory for vertical excitation energies. Furthermore, we find that the state-specific optimization can help avoid state-averaging-induced discontinuities on potential energy surfaces. With a simple implementation, a low cost, and compatibility with large active space methods, the approach is designed to be useful in a wide range of excited-state investigations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Monte Carlo simulation of nitrogen dissociation based on state-resolved cross sections

State-resolved analyses of N + N{sub 2} are performed using the direct simulation Monte Carlo (DSMC) method. In describing the elastic collisions by a state-resolved method, a state-specific total cross section is proposed. The state-resolved method is constructed from the state-specific total cross section and the rovibrational state-to-state transition cross sections for bound-bound and bound-free transitions taken from a NASA database. This approach makes it possible to analyze the rotational-to-translational, vibrational-to-translational, and rotational-to-vibrational energy transfers and the chemical reactions without relying on macroscopic properties and phenomenological models. In nonequilibrium heat bath calculations, the results of present state-resolved DSMC calculations are validated with those of the master equation calculations and the existing shock-tube experimental data for bound-bound and bound-free transitions. In various equilibrium and nonequilibrium heat bath conditions and 2D cylindrical flows, the DSMC calculations by the state-resolved method are compared with those obtained with previous phenomenological DSMC models. In these previous DSMC models, the variable soft sphere, phenomenological Larsen-Borgnakke, quantum kinetic, and total collision energy models are considered. From these studies, it is concluded that the state-resolved method can accurately describe the rotational-to-translational, vibrational-to-translational, and rotational-to-vibrational transfers and quasi-steady state of rotational and vibrational energies in nonequilibrium chemical reactions by state-to-state kinetics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1980

Improving Building Construction Specifications in State and Local Governments

State and local governments can benefit from master specifications systems that centralize data on all types of building materials, products, and processes. Most of these systems are organized according to the MASTERFORMAT system, which, along with guide specifications that require the insertion or deletion of standardized information, resulted from the specific needs of users and providers. For jurisdictions preparing their own specifications, staff time and cost are reduced. For those subcontracting the preparation, master specifications provide a means of evaluating the specifications submitted. Current management specification systems described include SPECINTACT, OMSPEC, MASTERPEC, and the NAVFAC, Corps of Engineers, and GSA guide specifications.

Source record↗
DOE OSTI2019

Dynamically weighted multireference perturbation theory: Combining the advantages of multi-state and state-averaged methods

In this paper, we introduce two new approaches to compute near-degenerate electronic states based on the driven similarity renormalization group (DSRG) framework. The first approach is a unitary multi-state formalism based on the DSRG (MS-DSRG), whereby an effective Hamiltonian is built from a set of state-specific solutions. The second approach employs a dynamic weighting parameter to smoothly interpolate between the multi-state and the state-averaged DSRG schemes. The resulting dynamically weighted DSRG (DW-DSRG) theory incorporates the most desirable features of both multi-state approaches (ability to accurately treat many states) and state-averaged methods (correct description of avoided crossings and conical intersections). We formulate second-order perturbation theories (PT2) based on the MS- and DW-DSRG and study the potential energy curves of LiF, the conical intersection of the two lowest singlet states of NH 3 , and several low-lying excited states of benzene, naphthalene, and anthracene. The DW-DSRG-PT2 predicts the correct avoided crossing of LiF and avoids artifacts produced by the corresponding state-specific and multi-state theories. Excitation energies of the acenes computed with the DW-DSRG-PT2 are found to be more accurate than the corresponding state-averaged values, showing a small dependence on the number of states computed.

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

Stabilization of Charge-Transfer Excited States in Biological Systems: A Computational Focus on the Special Pair in Photosystem II Reaction Centers

Charge-transfer (CT) excited states play an important role in many biological processes. However, many computational approaches often inadequately address the equilibration effects of nuclear and environmental degrees of freedom on these states. One prominent example of systems in which CT states are of utmost importance is reaction centers (RC) in photosystems. Here we use a multiscale approach combined with time-dependent density functional theory to explore the lowest CT excited state of the special pair P D1 –P D2 in the Photosystem II-RC of a cyanobacterium. We find that the nonequilibrium CT excited state resides near the Soret band, making an exciton the lowest-energy excited state. However, accounting for nuclear and state-specific dielectric equilibration along the CT potential energy surface (PES), the CT state P D1 – –P D2 + stabilizes energetically below the excitonic state. Importantly, this underscores the crucial role of state-specific solvation in mapping the PES of CT states, as demonstrated in a simplified dimer model.

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

Upscaling ab-initio chemistry models to non-equilibrium flow simulations

Thermochemical nonequilibrium is generated by hypersonic cruise vehicles, high speed combustion and detonations. Nonequilibrium interactions affect reaction rates and energy transfer that are critical for many engineering applications. Ab-initio potential energy surfaces can be used in quasi-classical trajectory (QCT) calculations to calculate state-specific dissociation rates and cross sections, as well as state-to-state energy exchange rates and cross sections. These rates and cross sections are needed for simulating such nonequilibrium flows. However, there are two main challenges in extending QCT calculations to modeling all chemical processes found in typical engineering flowfields. First, ab-initio surfaces for many collision partners are not available and when available their fidelity is not quantified. Second, state-to-state cross section datasets are typically on the order of 1000 4, , and are too large to be efficiently implemented in engineering simulations. This work focuses on O 2 +O interactions because of prevalence of oxygen in many engineering application; however, all of the models developed here may be applied to other diatom-atom interactions and can be extended to other diatom-diatom combinations. It is shown in this work that at temperatures between 2,500 and 20,000K, state-specific cross sections are not highly sensitive to potentials and a Morse additive pairwise (MAP) potential is proposed for modeling collisions for which ab-initio potentials are not available. Next, this work suggests an approach to model state-to-state cross sections based on maximum entropy considerations. The calculated cross sections are fit to a new model with just 8 parameters, which can be easily scaled up to flow simulations.

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

Solvent effects in time-dependent self-consistent field methods. II. Variational formulations and analytical gradients

This study describes variational energy expressions and analytical excited state energy gradients for time-dependent self-consistent field methods with polarizable solvent effects. Linear response, vertical excitation, and state-specific solventmodels are examined. Enforcing a variational ground stateenergy expression in the state-specific model is found to reduce it to the vertical excitation model. Variational excited state energy expressions are then provided for the linear response and vertical excitation models and analytical gradients are formulated. Using semiempiricalmodel chemistry, the variational expressions are verified by numerical and analytical differentiation with respect to a static external electric field. Lastly, analytical gradients are further tested by performing microcanonical excited state molecular dynamics with p-nitroaniline.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Higher-Form Anomalies on Lattices

We show that generic gapped quantum many-body states which respect an anomalous finite higher-form symmetry have an exponentially small overlap with any short-range entangled (SRE) state. Hence, anomalies of higher-form symmetries enforce $intrinsic$ long-range entanglement, which is in contrast with anomalies of ordinary (0-form) symmetries which are compatible with symmetric SRE states (specifically, symmetric cat states). As an application, we show that the anomalies of strong higher-form symmetries provide a diagnostic for mixed-state topological order in $d \geq 2$ spatial dimensions. We also identify a new (3+1)D intrinsic mixed-state topological order that does not obey remote-detectability by local decoherence of the (3+1)D Toric Code with fermionic loop excitations. This breakdown of remote detectability, as encoded in anomalies of strong higher-form symmetries, provides a partial characterization of intrinsically mixed-state topological order.

Feng, Yitao [Peking University, Beijing (China)] (↗
DOE OSTI2013

Clean Energy Application Center

The Mid Atlantic Clean Energy Application Center (MACEAC), managed by The Penn State College of Engineering, serves the six states in the Mid-Atlantic region (Pennsylvania, New Jersey, Delaware, Maryland, Virginia and West Virginia) plus the District of Columbia. The goals of the Mid-Atlantic CEAC are to promote the adoption of Combined Heat and Power (CHP), Waste Heat Recovery (WHR) and District Energy Systems (DES) in the Mid Atlantic area through education and technical support to more than 1,200 regional industry and government representatives in the region. The successful promotion of these technologies by the MACEAC was accomplished through the following efforts; (1)The MACEAC developed a series of technology transfer networks with State energy and environmental offices, Association of Energy Engineers local chapters, local community development organizations, utilities and, Penn State Department of Architectural Engineering alumni and their firms to effectively educate local practitioners about the energy utilization, environmental and economic advantages of CHP, WHR and DES; (2) Completed assessments of the regional technical and market potential for CHP, WHR and DE technologies application in the context of state specific energy prices, state energy and efficiency portfolio development. The studies were completed for Pennsylvania, New Jersey and Maryland and included a set of incentive adoption probability models used as a to guide during implementation discussions with State energy policy makers; (3) Using the technical and market assessments and adoption incentive models, the Mid Atlantic CEAC developed regional strategic action plans for the promotion of CHP Application technology for Pennsylvania, New Jersey and Maryland; (4) The CHP market assessment and incentive adoption model information was discussed, on a continuing basis, with relevant state agencies, policy makers and Public Utility Commission organizations resulting in CHP favorable incentive programs in New Jersey, Pennsylvania, Maryland and Delaware; (5) Developed and maintained a MACEAC website to provide technical information and regional CHP, WHR and DE case studies and site profiles for use by interested stakeholders in information transfer and policy discussions; (6) Provided Technical Assistance through feasibility studies and on site evaluations. The MACEAC completed 28 technical evaluations and 9 Level 1 CHP analyses ; and (7) the MACEAC provided Technical Education to the region through a series of 29 workshops and webinars, 37 technical presentations, 14 seminars and participation in 13 CHP conferences.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2022

Considerations for Safeguards Implementation in the Post-Operational Facility Life Cycle

Hundreds of facilities around the world under International Atomic Energy Agency (IAEA) safeguards are currently permanently shutdown or undergoing decommissioning. For facilities in States with a comprehensive safeguards agreement (CSA) in force, safeguards obligations under the CSA extend until the IAEA has determined for safeguards purposes that a facility has been decommissioned (i.e., the IAEA has verified that the nuclear material has been removed and residual structures and equipment essential for its use have been removed or rendered inoperable). The IAEA Department of Safeguards recently issued a report providing high-level guidance to States on IAEA safeguards implementation throughout the post-operational life cycle phases of facilities and locations outside facilities. These phases include permanent shutdown, closed-down, and decommissioned for safeguards purposes. Additional consideration is needed for how post-operational facilities might be consistently evaluated when developing State-level safeguards approaches. This work presents ideas about how the IAEA might implement the State-level concept and associated elements (e.g., State-specific factors) throughout the post-operational life cycle, focusing on maintaining effectiveness and gaining efficiencies where appropriate. Considerations include whether State-specific factors should influence facility status, how a change in a facility’s post-operational status might impact a State’s acquisition path analysis, and how rendering inoperable/removal of essential equipment could affect resources expended on safeguards implementation.

Hogue, Karen↗
DOE OSTI2016

Quantifying local exciton, charge resonance, and multiexciton character in correlated wave functions of multichromophoric systems

A new method for quantifying the contributions of local excitation, charge resonance, and multiexciton configurations in correlated wave functions of multichromophoric systems is presented. The approach relies on fragment-localized orbitals and employs spin correlators. Its utility is illustrated by calculations on model clusters of hydrogen, ethylene, and tetracene molecules using adiabatic restricted-active-space configuration interaction wave functions. In addition to the wave function analysis, this approach provides a basis for a simple state-specific energy correction accounting for insufficient description of electron correlation. The decomposition scheme also allows one to compute energies of the diabatic states of the local excitonic, charge-resonance, and multi-excitonic character. The new method provides insight into electronic structure of multichromophoric systems and delivers valuable reference data for validating excitonic models.

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

LOW-TEMPERATURE ION TRAP STUDIES OF N{sup +}({sup 3} P{sub ja} ) + H{sub 2}(j) {yields} NH{sup +} + H

Using a low-temperature 22-pole ion trap apparatus, detailed measurements for the title reaction have been performed between 10 K and 100 K in order to get some state specific information about this fundamental hydrogen abstraction process. The relative population of the two lowest H{sub 2} rotational states, j = 0 and 1, has been varied systematically. NH{sup +} formation is nearly thermo-neutral; however, to date, the energetics are not known with the accuracy required for low-temperature astrochemistry. Additional complications arise from the fact that, so far, there is no reliable theoretical or experimental information on how the reactivity of the N{sup +} ion depends on its fine-structure (FS) state {sup 3} P{sub ja} . Since in the present trapping experiment, thermalization of the initially hot FS population competes with hydrogen abstraction, the evaluation of the decay of N{sup +} ions over long storage times and at various He and H{sub 2} gas densities provides information on these processes. First assuming strict adiabatic behavior, a set of state specific rate coefficients is derived from the measured thermal rate coefficients. In addition, by recording the disappearance of the N{sup +} ions over several orders of magnitude, information on nonadiabatic transitions is extracted including FS-changing collisions.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2016

Transition state region in the A-Band photodissociation of allyl iodide—A femtosecond extreme ultraviolet transient absorption study

Femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy based on a high-harmonic generation source is used to study the 266 nm induced A-band photodissociation dynamics of allyl iodide (CH{sub 2} =CHCH{sub 2}I). The photolysis of the C—I bond at this wavelength produces iodine atoms both in the ground ({sup 2}P{sub 3/2}, I) and spin-orbit excited ({sup 2}P{sub 1/2}, I*) states, with the latter as the predominant channel. Using XUV absorption at the iodine N{sub 4/5} edge (45–60 eV), the experiments constitute a direct probe of not only the long-lived atomic iodine reaction products but also the fleeting transition state region of the repulsive n{sub I}σ{sup ∗}{sub C—I} excited states. Specifically, three distinct features are identified in the XUV transient absorption spectrum at 45.3 eV, 47.4 eV, and 48.4 eV (denoted transients A, B, and C, respectively), which arise from the repulsive valence-excited nσ{sup ∗} states and project onto the high-lying core-excited states of the dissociating molecule via excitation of 4d(I) core electrons. Transients A and B originate from 4d(I) → n(I) core-to-valence transitions, whereas transient C is best assigned to a 4d(I) →σ{sup ∗}(C—I) transition. The measured differential absorbance of these new features along with the I/I* branching ratios known from the literature is used to suggest a more definitive assignment, albeit provisional, of the transients to specific dissociative states within the A-band manifold. The transients are found to peak around 55 fs–65 fs and decay completely by 145 fs–185 fs, demonstrating the ability of XUV spectroscopy to map the evolution of reactants into products in real time. The similarity in the energies of transients A and B with analogous features observed in methyl iodide [Attar et al. J. Phys. Chem. Lett. 6, 5072, (2015)] together with the new observation of transient C in the present work provides a more complete picture of the valence electronic structure in the transition state region. The results provide a benchmark for theoretical calculations on the nature of core-excited states in halogenated hydrocarbons, especially in the transition state region along the C—I reaction coordinate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1983

Potential impact of remote sensing data on sea-state analysis and prediction

The severe North Atlantic storm which damaged the ocean liner Queen Elizabeth 2 (QE2) was studied to assess the impact of remotely sensed marine surface wind data obtained by SEASAT-A, on sea state specifications and forecasts. Alternate representations of the surface wind field in the QE2 storm were produced from the SEASAT enhanced data base, and from operational analyses based upon conventional data. The wind fields were used to drive a high resolution spectral ocean surface wave prediction model. Results show that sea state analyses would have been vastly improved during the period of storm formation and explosive development had remote sensing wind data been available in real time. A modest improvement in operational 12 to 24 hour wave forecasts would have followed automatically from the improved initial state specification made possible by the remote sensing data in both numerical and sea state prediction models. Significantly improved 24 to 48 hour wave forecasts require in addition to remote sensing data, refinement in the numerical and physical aspects of weather prediction models.

Cardone, V. J.↗
NASA NTRS1991

A new generation of high performance engines for spacecraft propulsion

Experimental data validating advanced engine designs at three thrust levels (5, 15, and 100 lbF) is presented. All of the three engine designs considered employ a Moog bipropellant torque motor valve, platelet injector design, and iridium-lined rhenium combustion chamber. Attention is focused on the performance, robustness, duration, and flexibility characteristics of the engines. It is noted that the 5- and 15-lbF thrust engines can deliver a steady state specific impulse in excess of 310 lbF-sec/lbm at an area ratio of 150:1, while the 150-lbF thrust engines deliver a steady state specific impulse of 320 lbF-sec/lbm at an area ratio of 250:1. The hot-fire test results reveal specific impulse improvements of 15 to 25 sec over conventional fuel film cooled columbium chamber designs while operating at maximum chamber temperatures.

Rosenberg, Sanders D.↗
DOE OSTI2022

Computing x-ray absorption spectra from linear-response particles atop optimized holes

State specific orbital optimized density functional theory (OO-DFT) methods, such as restricted open-shell Kohn–Sham (ROKS), can attain semiquantitative accuracy for predicting x-ray absorption spectra of closed-shell molecules. OO-DFT methods, however, require that each state be individually optimized. In this Communication, we present an approach to generate an approximate core-excited state density for use with the ROKS energy ansatz, which is capable of giving reasonable accuracy without requiring state-specific optimization. Herein, this is achieved by fully optimizing the core-hole through the core-ionized state, followed by the use of electron-addition configuration interaction singles to obtain the particle level. This hybrid approach can be viewed as a DFT generalization of the static-exchange (STEX) method and can attain ~0.6 eV rms error for the K-edges of C–F through the use of local functionals, such as PBE and OLYP. This ROKS(STEX) approach can also be used to identify important transitions for full OO ROKS treatment and can thus help reduce the computational cost of obtaining OO-DFT quality spectra. ROKS(STEX), therefore, appears to be a useful technique for the efficient prediction of x-ray absorption spectra.

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

Quantum minimal surfaces from quantum error correction

We show that complementary state-specific reconstruction of logical (bulk) operators is equivalent to the existence of a quantum minimal surface prescription for physical (boundary) entropies. This significantly generalizes both sides of an equivalence previously shown by Harlow[1]; in particular, we do not require the entanglement wedge to be the same for all states in the code space. In developing this theorem, we construct an emergent bulk geometry for general quantum codes, defining ``areas'' associated to arbitrary logical subsystems, and argue that this definition is ``functionally unique.'' We also formalize a definition of bulk reconstruction that we call ``state-specific product unitary’’ reconstruction. This definition captures the quantum error correction (QEC) properties present in holographic codes and has potential independent interest as a very broad generalization of QEC; it includes most traditional versions of QEC as special cases. Our results extend to approximate codes, and even to the ``non-isometric codes'' that seem to describe the interior of a black hole at late times.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗