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At least 721 records · Page 40

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NASA NTRSDate not supplied

Efficient Implementation for Unitary Coupled Cluster State Preparation for Near-Term Quantum Computers

Unitary coupled cluster theory (UCC) is a common wave function ansatz for quantum simulation of molecular electronic structure using the variational quantum eigenvalue solver (VQE). Even for small molecules using a double-ζ basis, the number of variational parameters required to minimize the electronic energy (i.e., optimize the circuit) is large and beyond the reach of current quantum computers. For example, a circuit simulating C2 using the UCCSD ansatz and the cc-pVDZ basis set with frozen-core will require over 10,000 variational parameters and a Hilbert space of over 10^(8) determinants. To make progress on simulating such molecular systems on near-term quantum computers, we explore how much of the optimization can be approximately prepared with classical simulation while reducing the number of optimization steps performed on a quantum device. Recently, Chen, Cheng, and Freericks [J. Chem. Theory Comput. 2021, 17, 841-847] presented an algorithm for the factorized form of the UCC ansatz that allows for efficient UCC optimizations on classical hardware. We flip the algorithm around and use it to prepare approximate quantum circuits for systems that require a large number of qubits to represent. We will present results from our implementation and discuss strategies for incorporating this implementation for algorithms involving near-term quantum computers.

Quantum Computing↗

NASA NTRSDate not supplied

Efficient Implementation for Unitary Coupled Cluster State Preparation for Near-Term Quantum Computers

Quantum Computing↗

NASA NTRSDate not supplied

Metal Hydroxide and Oxyhydroxide Gas Database

In a high temperature combustion situation such as a gas turbine or rocket engine, combustion products include water vapor. This water vapor reacts with oxides in the hot-gas-path to form volatile hydroxides and oxyhydroxides. The oxides may be structural oxide components or protective oxides on alloys or non-oxide ceramics. In either case, this enhanced volatilization leads to degradation of components. Reliable thermochemical data for many metal hydroxides and oxyhydroxides has not been available. We review a database put together at NASA over many years based on experimental and ab initio computations for thermochemical data of Al, Si, Ti, Cr, Mn, Y, Zr, La, Ta, Gd, and Yb hydroxides and oxyhydroxides. Experimental methods for measuring thermodynamic quantities of metal hydroxides and oxyhydroxides are limited since the required high temperatures and high pressures preclude many conventional methods. Nonetheless, transpiration has proven a valuable tool in our laboratories for the Si-O-H, Cr-O-H, and Ti-O-H systems. Data are analyzed with second and third law methods. These data can be leveraged with quantum chemistry to provide reliable free energy functions for the third law calculation and comparison to the derived enthalpies of formation. Both wave function and DFT methods can be utilized for deriving the thermodynamic functions for the various metal hydroxides and oxyhydroxides. We have found that, in general, reasonable molecular geometries and spectroscopic data can be derived with a relatively low level of theory, i.e. DFT with the B3LYP functional. Accurate calculations of the enthalpy of formation require higher levels of theory, such as the Coupled Cluster, Singles, Doubles, and perturbative Triples CCSD(T) approach with complete basis sets (CBS). Also, corrections for hindered rotations and anharmonicity are necessary. For some symmetries, the anharmonic correction has proven to be a challenge and we have found that this is only treated properly by certain codes. The database lists the fHo(298), So(298), and Cp in the form Cp = A + BT + CT2 + D/T + E/T2, where A, B, C, D, and E are the fitting constants. Thus, it can be easily used in any of the common computational thermochemistry codes. To date, the database contains 51 gaseous species of the formula MOx(OH)y.

Metal Hydroxides↗

NASA NTRSDate not supplied

Incorporating ADAPT-VQE with a Sparse Wavefunction Circuit Simulator to Find Compact Quantum Circuits for Chemical Applications

We implemented the ADAPT-VQE algorithm into our recent classical sparse wavefunction circuit simulator to demonstrate that classical resources can (1) efficiently find a physically motivated compact wavefunction ansatz for further refinement on near-term quantum hardware and (2) benchmark expected results of VQE-based algorithms once the quantum hardware is available to study large-scale applications. In particular, we study the role of the ADAPT-VQE operator pool, molecular basis set selection, and variations such as TETRIS-ADAPT-VQE on the performance of our classical circuit simulator. This work demonstrates the promise of using classical resources to generate highly accurate wavefunctions that can be prepared on quantum hardware to initiate other quantum algorithms such as phase estimation. Our approach harnesses the power of high-performance computing resources with the more limited available quantum computers to map a path toward quantum advantage for electronic structure calculations in chemistry and materials science.

Quantum Computing↗

NASA NTRSDate not supplied

Exploring Quantum State Preparation Using Tensor Networks and Sparse Wavefunction Simulations

The variational quantum eigenvalue solver is a powerful hybrid quantum-classical approach that has been suggested as a candidate method to run on near-term quantum hardware for computing ground state electronic energies of molecular systems. However, even for small molecules, the number of variational parameters and qubits required to minimize the electronic energy is beyond the reach of current quantum computers except for small basis sets. We explore a new paradigm for state preparation where we test how much of the optimization can be approximately prepared with classical computers to reduce the number of optimization steps performed using a quantum device. By adapting a recent algorithm for the factorized form of the UCC ansatz, we can study molecular electronic structure problems with up to 64 qubits. In addition, we also test a related approach of using tensor networks to optimize quantum circuits in order to benchmark various lattice models. We present results using these approaches and discuss strategies for incorporating these ideas into variational algorithms involving near-term quantum computers. Our results help demonstrate the strength of the UCC ansatz and address pressing questions about optimal initial parameterizations and circuit construction.

quantum computing↗

NASA NTRS2024

Global Influence of Organic Aerosol Volatility on Aerosol Microphysical Processes: Composition and Number

We present MATRIX-VBS, a new aerosol scheme that simulates organic partitioning in an aerosol microphysics model, as part of the NASA GISS ModelE Earth System Model. MATRIX-VBS builds on its predecessor aerosol microphysics model MATRIX (Bauer et al., 2008, https://doi.org/10.5194/acp-8-6003-2008) and was developed in the box model framework (Gao et al., 2017, https://doi.org/10.5194/gmd-10-751-2017). The scheme features the inclusion of organic partitioning between the gas and particle phases and the photochemical aging process using the volatility-basis set (Donahue et al., 2006, https://doi.org/10.1021/es052297c). To assess the performance of the new model, we compared its mass concentration, number concentration, and activated number concentration to the original scheme MATRIX, and evaluated its mass concentrations in four seasons against data from the NASA Atmospheric Tomography Mission (ATom) aircraft campaign. Results from MATRIX-VBS show that organics are transported further away from their source, and their mass concentration increases aloft and decreases at the surface compared to those in MATRIX. The mass concentration of organics at the surface agrees well with measurements, and there are discrepancies for vertical profiles aloft. In the new scheme, the global mass load of organic aerosols increased by 50%, there is also an increased number of particles at the surface and fewer activated ones in most regions. The new scheme presents advanced and more comprehensive capability in simulating aerosol processes.

aerosol modeling↗

NASA NTRSDate not supplied

Reliable IR Line Lists for N2O and OCS Isotopologues for High Temperature Applications up to 2000 K

To address the needs of planetary and exoplanetary atmosphere studies towards JWST, HWO and future IR astronomy missions, theoretical IR line lists of Carbonyl Sulfide (OCS) and Nitrous Oxide (N2O) are generated to provide complete, reliable, and consistent IR reference data in the range of 0 - 15,000 cm-1, or wavelength longer than 0.67 Å, for temperature up to 2000 K. The line lists are quantum mechanically computed using spectroscopically accurate potential energy surfaces empirically refined with reliable high-resolution experimental data, and high-quality dipole moment surfaces constructed at CCSD(T) level with aug-cc-pVT/Q/5(+d)Z basis and extrapolations to complete basis set limit. The Ames N2O line list includes the primary isotopologue 14N2 16O (denoted "446") with J=0-210 and E' up to 25,000 cm-1, and 11 minor isotopologues of 15N and 17/18O with J=0-150 and lower E' cutoffs. For OCS, Ames "natural" 296 K line list includes 12 most abundant isotopologues. The intensity contribution of OCS minor isotopologues at higher temperature is non-negligible, e.g., 8.6 ± 4.9% at 1000 K. The 16O12C32S (93.7%) and 16O12C34S (4.2%) transitions are computed with J=0-240 and E'< 22,000 cm-1, plus J=0-150 and E' < 16,000 cm-1 for five more minor isotopologues. Reliable Effective Hamiltonian models (e.g., NOSL-296 for 14N2 16O), experimental data collections, and reliable HITRAN or MARVEL levels are combined with quantum rovibrational calculations to deliver accurate and consistent empirical corrections for line positions. The reliability and accuracy of our IR intensity predictions are demonstrated by comparison with available databases, line lists, and experiments, at both room temperature and at high temperature. The line lists will be freely available to public online at ZENODO and NAS data portal. We acknowledge the financial support from NASA XRP and APRA programs.

Planetary↗

DOE OSTI2020

STRUCTURE AND PROPERTIES STUDY ON ENERGY MATERIALS: THERMOELECTRIC MATERIAL TETRAHEDRITE AND LITHIUM ION CONDUCTOR

Development of efficient energy materials is critical in order to ease the energy demand and reduce our dependence of fossil fuel. Thermoelectric materials are promising due to their capability of generating electrical power by recovering waste heat. The performance of thermoelectric materials is quantified by a dimensionless figure of merit zT, which depends on their properties such as electrical conductivity, Seebeck coefficient and thermal conductivity. Tetrahedrites, a copper antimony sulfosalt mineral, typified by Cu 12-x MxSb 4 S 13 , where M is a transition metal element such as Ni, Zn, Fe or Mn, have great potential for thermoelectric application due to their relatively high zT (close to 1 at 700 K), earth-abundance, environmental friendliness, favorable electrical properties, and most importantly intrinsic low lattice thermal conductivity (less than 1 W m -1 K -1 ) in wide temperature. In addition to energy recovery, reliable energy storage devices are also emerging to relieve the energy demand and improve the efficiency of consuming energy resources. Lithium-ion batteries are known to be reliable and successful electrochemical energy storage devices and appliable in various aspects, including laptops, smartphones and electrical vehicles. Lithium phosphorous oxynitride (LiPON) are widely used as thin-film solid-state electrolytes in Li-ion battery, which is the only demonstrated solid-state electrolyte that is quite stable in direct contact with Li metal at potentials from 0-5 V. However, the structure of LiPON, the effects of N doping, and the origin of its good electrochemical stability remains inconclusive. In this thesis, reliable modeling techniques accompanied with experimental tools, are applied to study the thermoelectric material tetrahedrite and the ionic conductor LiPON, in order to study their structural and dynamical properties. Accurate and efficient density-functional theory (DFT) and density-functional tight-binding (DFTB) methods, combined with molecular dynamics (MD) simulations are utilized in order to investigate the structures and properties of these energy materials. The incoherent and coherent atomic dynamics study of tetrahedrite Cu 10.5 NiZn 0.5 Sb 4 S 13 provides the origin of softening upon cooling by investigate the motion of Cu12e at different temperatures. The dynamic structure factors in the longitudinal and transverse direction will also be discussed. The Cu movement of Cu-rich tetrahedrite Cu 14 Sb 4 S 13 is revealed by Cu self-diffusivity, nuclear density map and “nudged elastic band” (NEB). Moreover, we investigate the effect of simulation cell size and basis sets on the DFT-based MD simulation results using tetrahedrite Cu1 0 Zn 2 Sb 4 S 13 thermoelectric as a model material, showing the advantage of larger cell by accessing smaller Q range. In addition, the low-temperature structural properties of Cu 12 Sb 4 S 13 is measured by neutron diffraction, which indicates that no cubic to tetragonal transition occurs at metal-semiconductor transition (MST) temperature. Thermoelectric properties such as Seebeck coefficient, electrical resistivity and electrical thermal conductivity will also be investigated. DFTB method is implemented to study the structure and transport properties of Li 3 PO 4 and LiPON, while the exploration of N doping effect is included. Lastly, the LiPON/Li interphase will be revealed in order to study the origin of electrochemical stability.

Li, Junchao↗

DOE OSTI2021

Tailored computational approaches to interrogate heavy element chemistry and structure in condensed phase

In this chapter we are presenting a brief review of the challenges encountered in the study of 4f and 5f block elements in the condensed phase. Their recovery, use in molten salt reactors and other interesting applications necessitate the use of molecular dynamics and large-scale models that take into account both the electronic structure and relativistic corrections. Sampling the multitude of electronic and atomic configurational states is at the heart of reliable predictions of structure, reactivity, dynamics and transport of heavy metals in complex environments. We present three examples that combine lanthanide elements with large scale models: i) our recent developments of a versatile adaptive learning method that enables global optimization in high dimensional spaces, ii) results of computed pKa values of lanthanide aqua complexes, and iii) structure and computed EXAFS of heavy elements in molten salts. The latter two employ our recently-optimized lanthanide pseudo-potentials and companion basis sets for condensed phase ab initio molecular dynamics.

Nguyen, Manh Thuong↗

DOE OSTI2025

2025 ASMS Investigation of the Collision-Induced Dissociation Mechanism of Protonated TODGA with IRIS

Title (20 words): Investigation of the Collision-Induced Dissociation Mechanism of Protonated TODGA with IRIS Introduction (120 words): One of the challenges facing wide-spread adoption of nuclear power is the development of efficient separation processes for used nuclear fuel. The molecules in separation processes are subjected to an extreme environment due to the high radiation fields from the used fuel and highly acidic media used for fuel dissolution, which results in significant molecular degradation, leading to reduced process efficiency. These degradation products must be identified and studied so mitigation strategies can be developed to maintain process efficiency. However, complex systems can have many degradation products, complicating identification. Untargeted analysis tools could be used to understand radiation chemistry in complex systems. However, this would necessitate improved understanding of the gas-phase fragmentation mechanisms of fuel cycle molecules like tetraoctyldiglycolamide (TODGA). Methods (120 words): The gas-phase fragmentation of protonated TODGA was investigated using collision-induced dissociation (CID), resonance ejection, and infrared ion spectroscopy (IRIS). CID and resonance ejection experiments were conducted using a Bruker Daltonics (Bremen, Gemany) SolariX XR fourier transform ion cyclotron resonance (FT-ICR) mass spectrometer. IRIS spectra of protonated TODGA and its two CID fragmentation products were measured using a modified Bruker amaZon Speed ETD 3D quadrupole ion trap mass spectrometer coupled to the Free Electron Lasers for Infrared eXperiments (FELIX) free electron laser. Measured spectra were compared with density functional theory (DFT) calculations using the Gaussian 16, Revision C.02 software package with the ?B97X-D functional and def2-TZVPP basis sets. Candidate structures were generated using the CREST 3.0 conformational sampling software tool. Preliminary Data (300 words): Collision-induced dissociation of protonated TODGA ([C36H73N2O3]+, m/z=581.562) results two fragment ions, one at m/z=340.285 assigned as [C20H38NO3]+ and the other at m/z=312.290, assigned as [C19H38NO2]+. Based on the assigned formula and the structure of protonated TODGA, the fragment at m/z=340.285 is likely formed from elimination of neutral dioctylamine. Comparison of the IRIS spectrum of m/z=340.285 with DFT predictions suggests it contains a ring structure, and is assigned as N-octyl-N-(6-oxo-1,4-dioxan-2-ylidene)octan-1-aminium. Based on this structure and the structure of protonated TODGA, we hypothesize this fragment formed from elimination of neutral dioctylamine followed by a ring closure mechanism. Comparison of the IRIS spectrum of the fragment at m/z=312.290 with DFT predictions also indicated the presence of a ring structure, assigned as N-(1,3-dioxolan-4-ylidene)-N-octyloctan-1-aminium. This product could be formed from elimination of carbon monoxide from the ring of m/z=340.285 as a sequential fragmentation or formed directly from protonated TODGA via elimination of neutral N,N-dioctylformamide followed by a ring closure. Resonance ejection experiments where m/z=340 was continuously ejected from the IRC cell showed no decrease in intensity of m/z=312.290 across several collision energies, suggesting that the later, direct formation mechanism, dominates. The location of the ionizing proton in protonated TODGA is important for modeling the fragmentation mechanisms. DFT calculations suggested that the position of bands involving the coupled vibrations of the amide C—N and C=O bonds in TODGA are the most sensitive to proton location. Evaluation of the IRIS spectrum of protonated TODGA suggests that the ionizing proton is located between the two amid oxygens. This protonation location was calculated to lie approximately 30 kJ/mol lower in energy than the next lowest energy location, with the proton located solely on one of the amide oxygens. Novel aspect (20 words): Infrared ion spectroscopy combined with resonance ejection experiments and density functional theory to probe the collision-induced dissociation mechanism of tetraoctyldiglycolamide.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗

NASA NTRS1996

Design of Multi-Parameter Steerable Functions Using Cascade Basis Reduction

A new cascade basis reduction method of computing the optimal least-squares set of basis functions steering a given function is presented. The method combines the Lie group-theoretic and the singular value decomposition approaches in such a way that their respective strengths complement each other. Since the Lie group-theoretic approach is used, the set of basis and steering functions computed can be expressed analytically. Because the singular value decomposition method is used, this set of basis and steering functions is optimal in the least-squares sense. Furthermore, the computational complexity in designing basis functions for transformation groups with large numbers of parameters is significantly reduced. The efficiency of the cascade basis reduction method is demonstrated by designing a set of basis functions that steers a Gabor function under the four-parameter linear transformation group.

Teo, P.↗

DOE OSTI2020

Methods for delineating cellular regions and classifying regions of histopathology and microanatomy

Embodiments disclosed herein provide methods and systems for delineating cell nuclei and classifying regions of histopathology or microanatomy while remaining invariant to batch effects. These systems and methods can include providing a plurality of reference images of histology sections. A first set of basis functions can then be determined from the reference images. Then, the histopathology or microanatomy of the histology sections can be classified by reference to the first set of basis functions, or reference to human engineered features. A second set of basis functions can then be calculated for delineating cell nuclei from the reference images and delineating the nuclear regions of the histology sections based on the second set of basis functions.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS2006

Parameter and Structure Inference for Nonlinear Dynamical Systems

A great many systems can be modeled in the non-linear dynamical systems framework, as x = f(x) + xi(t), where f() is the potential function for the system, and xi is the excitation noise. Modeling the potential using a set of basis functions, we derive the posterior for the basis coefficients. A more challenging problem is to determine the set of basis functions that are required to model a particular system. We show that using the Bayesian Information Criteria (BIC) to rank models, and the beam search technique, that we can accurately determine the structure of simple non-linear dynamical system models, and the structure of the coupling between non-linear dynamical systems where the individual systems are known. This last case has important ecological applications.

Morris, Robin D.↗

NASA NTRS2008

New Basis Functions for the Electromagnetic Solution of Arbitrarily-shaped, Three Dimensional Conducting Bodies using Method of Moments

In this work, we present a new set of basis functions, defined over a pair of planar triangular patches, for the solution of electromagnetic scattering and radiation problems associated with arbitrarily-shaped surfaces using the method of moments solution procedure. The basis functions are constant over the function subdomain and resemble pulse functions for one and two dimensional problems. Further, another set of basis functions, point-wise orthogonal to the first set, is also defined over the same function space. The primary objective of developing these basis functions is to utilize them for the electromagnetic solution involving conducting, dielectric, and composite bodies. However, in the present work, only the conducting body solution is presented and compared with other data.

Mackenzie, Anne I.↗

NASA NTRS2007

New Basis Functions for the Electromagnetic Solution of Arbitrarily-shaped, Three Dimensional Conducting Bodies Using Method of Moments

In this work, we present a new set of basis functions, de ned over a pair of planar triangular patches, for the solution of electromagnetic scattering and radiation problems associated with arbitrarily-shaped surfaces using the method of moments solution procedure. The basis functions are constant over the function subdomain and resemble pulse functions for one and two dimensional problems. Further, another set of basis functions, point-wise orthogonal to the first set, is also de ned over the same function space. The primary objective of developing these basis functions is to utilize them for the electromagnetic solution involving conducting, dielectric, and composite bodies. However, in the present work, only the conducting body solution is presented and compared with other data.

Mackenzie, Anne I.↗

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↗

NASA NTRS1999

Proper Orthogonal Decomposition in Optimal Control of Fluids

In this article, we present a reduced order modeling approach suitable for active control of fluid dynamical systems based on proper orthogonal decomposition (POD). The rationale behind the reduced order modeling is that numerical simulation of Navier-Stokes equations is still too costly for the purpose of optimization and control of unsteady flows. We examine the possibility of obtaining reduced order models that reduce computational complexity associated with the Navier-Stokes equations while capturing the essential dynamics by using the POD. The POD allows extraction of certain optimal set of basis functions, perhaps few, from a computational or experimental data-base through an eigenvalue analysis. The solution is then obtained as a linear combination of these optimal set of basis functions by means of Galerkin projection. This makes it attractive for optimal control and estimation of systems governed by partial differential equations. We here use it in active control of fluid flows governed by the Navier-Stokes equations. We show that the resulting reduced order model can be very efficient for the computations of optimization and control problems in unsteady flows. Finally, implementational issues and numerical experiments are presented for simulations and optimal control of fluid flow through channels.

Ravindran, S. S.↗

DOE OSTI2021

Global patterns of forest autotrophic carbon fluxes

Carbon (C) fixation, allocation, and metabolism by trees set the basis for energy and material flows in forest ecosystems and define their interactions with Earth’s changing climate. However, we lack a cohesive synthesis on how forest carbon fluxes vary globally with respect to climate and one another. Here, we draw upon 1,319 records from the Global Forest Carbon Database (ForC), representing all major forest types and the nine most significant autotrophic carbon fluxes, to comprehensively explore how C cycling in mature, undisturbed forests varies with latitude and climate on a global scale. We show that, across all flux variables analyzed, C cycling decreases continuously with absolute latitude – a finding that confirms multiple previous studies but contradicts the idea that net primary productivity of temperate forests rivals that of tropical forests. C flux variables generally displayed similar trends across latitude and multiple climate variables, with no differences in allocation detected at this global scale. Temperature variables in general, and mean annual temperature and temperature seasonality in particular, were the best univariate predictors of C flux, explaining 19 - 71% of variation in the C fluxes analyzed. The effects of temperature were modified by moisture availability, with C flux reduced under hot and dry conditions and sometimes under very high precipitation. C fluxes increased with growing season length, but this was never the best univariate predictor. Within the growing season, the influence of climate on C cycling was small but significant for a number of flux variables. These findings clarify how forest C flux varies with latitude and climate on a global scale. In a period of accelerating climatic change, this improved understanding of the fundamental climatic controls on forest C cycling sets a foundation for understanding patterns of change.

Banbury Morgan, Rebecca↗