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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 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Implementing contact angle boundary conditions for second-order Phase-Field models of wall-bounded multiphase flows

In the present work, a general formulation is proposed to implement the contact angle boundary conditions for the second-order Phase-Field models, which is applicable to N-phase (N ≥ 2) moving contact line problems. To remedy the issue of mass change due to the contact angle boundary condition, a source term or Lagrange multiplier is added to the original second-order Phase-Field models, which is determined by the consistent and conservative volume distribution algorithm so that the summation of the order parameters and the consistency of reduction are not influenced. To physically couple the proposed formulation to the hydrodynamics, especially for large-density-ratio problems, the consistent formulation is employed. The reduction-consistent conservative Allen-Cahn models are chosen as examples to illustrate the application of the proposed formulation. The numerical scheme that preserves the consistency and conservation of the proposed formulation is employed to demonstrate its effectiveness. Results produced by the proposed formulation are in good agreement with the exact and/or asymptotic solutions. The proposed method captures complex dynamics of moving contact line problems having large density ratios.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Possible impacts of Mo chemical banding and second phase impurities on the irradiation behavior of monolithic U-10Mo fuels

This study investigated the microstructural behavior of both full-size and mini-size monolithic U-10Mo fuel plates irradiated to high burnup with a focus on the evolution of the second phase impurities in monolithic U-Mo using scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), and wavelength dispersive spectroscopy (WDS). Key indicators of possible mechanical and thermal compromise include cracks, large fission gas porosity, and interconnection of fission gas pores. For the fission densities evaluated in this work (3.5 × 10 21 fissions/cm 3 -5.1 × 10 21 fissions/cm 3 ), fine porosity can develop along the UC phase boundary; however, the size of the fission gas pores is no more than those observed in the U-Mo fuel phase. Further, other inclusions such as Si-rich second-phase impurities found in the as-fabricated microstructure were difficult to resolve post-irradiation because they can become overshadowed by porosity development in the fuel phase. Additionally, the presence of a Fe-rich sublayer formed in the Zr diffusion layer during fabrication remained enriched in the Zr layer in the irradiated U-10Mo microstructures near the U-Mo/Zr interface; however, based on the burnup assessed in this study the identified impurities did not appear to contribute to notable microstructural degradation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Irradiation-induced amorphization of Fe-Y-based second phase particles in accident-tolerant FeCrAl alloys

Here, second phase intermetallic particles in an advanced accident-tolerant FeCrAl (Fe-13Cr-5Al-2Mo) alloy are formed in the α-Fe matrix during processing. These particles are prominently related to the added Y. Neutron irradiation to ~7 displacements per atom (dpa) with a dose rate of ~8.16 × 10 -7 dpa/s at 282 °C resulted in the amorphization of these precipitates which could degrade the mechanical properties of the FeCrAl alloys. Analytical electron microscopy and diffraction analysis combined with structural freedom analysis have been used to investigate the radiation resistance of the second phase particles. Radiation tolerance is closely linked to the particle Fe-Y content and can be tailored using the structure freedom value.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Which “second-best” climate policies are best? Simulating cost-effective policy mixes for passenger vehicles

In the real-world of political opposition and complex market failures, carbon pricing alone will not achieve deep GHG mitigation targets. Hence, in this study, we search for the most cost-effective “second-best” policies. Focusing on the light-duty vehicle sector in the case of Canada, we compare several policies in terms of effectiveness (regarding 2030 GHG goals) and mitigation costs, namely: (i) a carbon tax; (ii) a vehicle emission standard (or VES); (iii) a zero emissions vehicle (ZEV) mandate, and (iv) combinations of all three at various stringencies. In this effort, we apply the AUtomaker-consumer Model (AUM), which endogenously simulates consumer and automaker decisions and technological change. Comparing individual policies, the regulations are about three times more expensive than the carbon tax. Among “second-best” policies, the VES is cheaper than a ZEV mandate at lower stringencies, but at higher stringencies the two are similarly efficient (both incentivize widespread ZEV deployment). In policy mixes, cost-effectiveness is improved by a carbon tax. Specifically, inclusion of a CDN$100–150/tonne tax can achieve targets while being 30–40% less costly than a regulation alone. We suggest that policymakers implement carbon pricing as stringently as politically feasible (for efficiency), complemented by regulations as needed (for efficacy) to meet GHG targets.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2021

Second Linear Response Theory and the Analytic Calculation of Excited-State Properties

We present a method based on second linear response time-dependent density func- tional theory (TDDFT) to calculate permanent and transition multipoles of excited states, which are required to compute excited-state absorption/emission spectra, multi- photon optical processes, among others. In previous work, we examined computations based on second linear response theory in which linear response TDDFT was employed twice. In contrast, the present methodology only requires information from a single linear response calculation to compute the excited-state properties. These are eval- uated analytically through various algebraic operations involving electron repulsion integrals and excitation vectors. The present derivation focuses on full many-body wave functions instead of single orbitals, as in our previous approach. Here, we test the proposed method by applying it to several diatomic and triatomic molecules. This shows that the computed excited-state dipoles are consistent with respect to reference equation-of-motion coupled cluster calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Second Harmonic Generation Electric Field Triplet Interferometry for Absolute Phasing

We report second harmonic generation (SHG) electric field triplet interferometry performed using three mutually coherent ultrafast pulses in a common path with controllable relative phases, namely, the light fields of a sample signal (SI), a reference oscillator (RO), and a local oscillator (LO). The ROLO phase determined from the interference of the light fields produced by two quartz wafers is subtracted from the phase determined from the SIROLO interferogram to yield the signal phase, ϕ SI . The new method also calibrates the measured SHG intensity from a given sample internally by sending the fundamental light field reflected from the sample into one of the quartz wafers in the ROLO element. The approach avoids having to exchange the sample against a reference material with a known χ(2) value or known phase and accounts on-the-fly for situations where the reflected fundamental light field intensity changes with experimental conditions. The new method is successfully benchmarked against z-cut α-quartz, fused silica held at its point of zero charge, and hematite nanolayers in air, across three different interferometers. Furthermore, the approach should be applicable for other second-order nonlinear spectroscopies, such as vibrational or electronic sum-frequency generation.

Interfaces↗
DOE OSTI2022

Templating Bicarbonate in the Second Coordination Sphere Enhances Electrochemical CO 2 Reduction Catalyzed by Iron Porphyrins

Bicarbonate-based electrolytes are ubiquitous in aqueous electrochemical CO 2 reduction, particularly in heterogenous catalysis, where they demonstrate improved catalytic performance relative to other buffers. In contrast, the presence of bicarbonate in organic electrolytes and its roles in homogeneous electrocatalysis remain underexplored. Here, we investigate the influence of bicarbonate on iron porphyrin-catalyzed electrochemical CO 2 reduction. In this work, we show that bicarbonate is a viable proton donor in organic electrolyte (p K a = 20.8 in dimethyl sulfoxide) and that urea pendants in the second coordination sphere can be used to template bicarbonate in the vicinity of a molecular iron porphyrin catalyst. The templated binding of bicarbonate increases its acidity, resulting in a 1500-fold enhancement in catalytic rates relative to unmodified parent iron porphyrin. This work emphasizes the importance of bicarbonate speciation in wet organic electrolytes and establishes second-sphere bicarbonate templating as a design strategy to harness this adventitious acid and enhance CO 2 reduction catalysis.

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

Prediction of organic homolytic bond dissociation enthalpies at near chemical accuracy with sub-second computational cost

Bond dissociation enthalpies (BDEs) of organic molecules play a fundamental role in determining chemical reactivity and selectivity. However, BDE computations at sufficiently high levels of quantum mechanical theory require substantial computing resources. In this paper, we develop a machine learning model capable of accurately predicting BDEs for organic molecules in a fraction of a second. We perform automated density functional theory (DFT) calculations at the M06-2X/def2-TZVP level of theory for 42,577 small organic molecules, resulting in 290,664 BDEs. A graph neural network trained on a subset of these results achieves a mean absolute error of 0.58 kcal mol-1 (vs DFT) for BDEs of unseen molecules. We further demonstrate the model on two applications: first, we rapidly and accurately predict major sites of hydrogen abstraction in the metabolism of drug-like molecules, and second, we determine the dominant molecular fragmentation pathways during soot formation.

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

Visualizing group II intron dynamics between the first and second steps of splicing

Group II introns are ubiquitous self-splicing ribozymes and retrotransposable elements evolutionarily and chemically related to the eukaryotic spliceosome, with potential applications as gene-editing tools. Recent biochemical and structural data have captured the intron in multiple conformations at different stages of catalysis. Here, we employ enzymatic assays, X-ray crystallography, and molecular simulations to resolve the spatiotemporal location and function of conformational changes occurring between the first and the second step of splicing. We show that the first residue of the highly-conserved catalytic triad is protonated upon 5’-splice-site scission, promoting a reversible structural rearrangement of the active site (toggling). Protonation and active site dynamics induced by the first step of splicing facilitate the progression to the second step. Our insights into the mechanism of group II intron splicing parallels functional data on the spliceosome, thus reinforcing the notion that these evolutionarily-related molecular machines share the same enzymatic strategy.

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

Diffuse auroral precipitation driven by lower-band chorus second harmonics

Diffuse aurora at the Earth’s high latitude regions is mainly caused by the low-energy (0.1–30 keV) electron precipitation which carries the major energy flux into the nightside upper atmosphere. Previous studies have demonstrated that combined scattering by the upper- and lower- band chorus waves acts as the dominant cause of diffuse auroral precipitation, but that is not necessarily the case as these two types of waves do not always occur simultaneously, with the lower-band more often. Here we report that the lower-band chorus satisfying the preferred condition can generate their second harmonics so as to trigger the diffuse auroral electron precipitation. We find that the lower-band chorus alone can only cause the precipitation of electrons greater than 4 keV, while the self-consistently generated second harmonic is weak but still able to result in the electron precipitation below 4 keV. The combined effect of those modes results in the observed pancake electron distributions and the diffuse aurora. Our results clearly demonstrate an alternative but universal mechanism of chorus-driven diffuse aurora in the Earth, which may also apply to the auroral formation in other planetary magnetospheres.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

Two-colour dissipative solitons and breathers in microresonator second-harmonic generation

Frequency conversion of dissipative solitons associated with the generation of broadband optical frequency combs having a tooth spacing of hundreds of giga-hertz is a topical challenge holding the key to practical applications in precision spectroscopy and data processing. The work in this direction is underpinned by fundamental problems in nonlinear and quantum optics. Here, we present the dissipative two-colour bright-bright and dark-dark solitons in a quasi-phase-matched microresonator pumped for the second-harmonic generation in the near-infrared spectral range. We also found the breather states associated with the pulse front motion and collisions. The soliton regime is found to be typical in slightly phase-mismatched resonators, while the phase-matched ones reveal broader but incoherent spectra and higher-order harmonic generation. Soliton and breather effects reported here exist for the negative tilt of the resonance line, which is possible only via the dominant contribution of second-order nonlinearity.

42 ENGINEERING↗
DOE OSTI2024

Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml package

Abstract Optical second harmonic generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. Closed-form analytical solution of the nonlinear optical responses is essential for evaluating materials whose optical properties are unknown a priori. A recent open-source code, ♯SHAARP. si , can provide such closed form solutions for crystals with arbitrary symmetries, orientations, and anisotropic properties at a single interface. However, optical components are often in the form of slabs, thin films on substrates, and multilayer heterostructures with multiple reflections of both the fundamental and up to ten different SHG waves at each interface, adding significant complexity. Many approximations have therefore been employed in the existing analytical approaches, such as slowly varying approximation, weak reflection of the nonlinear polarization, transparent medium, high crystallographic symmetry, Kleinman symmetry, easy crystal orientation along a high-symmetry direction, phase matching conditions and negligible interference among nonlinear waves, which may lead to large errors in the reported material properties. To avoid these approximations, we have developed an open-source package named Second Harmonic Analysis of Anisotropic Rotational Polarimetry in Multilayers (♯SHAARP. ml ). The reliability and accuracy are established by experimentally benchmarking with both the SHG polarimetry and Maker fringes using standard and commonly used nonlinear optical materials as well as twisted 2-dimensional heterostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Structural and mechanistic insights into the bifunctional HISN2 enzyme catalyzing the second and third steps of histidine biosynthesis in plants

The second and third steps of the histidine biosynthetic pathway (HBP) in plants are catalyzed by a bifunctional enzyme–HISN2. The enzyme consists of two distinct domains, active respectively as a phosphoribosyl-AMP cyclohydrolase (PRA-CH) and phosphoribosyl-ATP pyrophosphatase (PRA-PH). The domains are analogous to single-domain enzymes encoded by bacterial hisI and hisE genes, respectively. The calculated sequence similarity networks between HISN2 analogs from prokaryotes and eukaryotes suggest that the plant enzymes are closest relatives of those in the class of Deltaproteobacteria. In this work, we obtained crystal structures of HISN2 enzyme from Medicago truncatula (MtHISN2) and described its architecture and interactions with AMP. The AMP molecule bound to the PRA-PH domain shows positioning of the N1-phosphoribosyl relevant to catalysis. AMP bound to the PRA-CH domain mimics a part of the substrate, giving insights into the reaction mechanism. The latter interaction also arises as a possible second-tier regulatory mechanism of the HBP flux, as indicated by inhibition assays and isothermal titration calorimetry.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Large second harmonic generation in a penta-CdO 2 sheet exfoliated from its bulk phase

Two-dimensional (2D) materials composed solely of pentagonal motifs are of particular interest due to their unique geometries and novel properties. Especially, the broken centrosymmetry and in-plane mirror symmetry in penta-graphene-like materials result in both in-plane and out-of-plane second harmonic generation (SHG). Transition metal cations with a filled d 10 shell (d 10 -TM) can significantly enhance the SHG response as found in many previously studied bulk materials. Here, in this study, based on first-principles calculations combined with independent particle approximation, we show that large SHG can also exist in some 2D d 10 -TM oxides, such as penta-CdO 2 , which can be chemically exfoliated from its bulk phase with its dynamical, thermal, and mechanical stability intact. We further find that penta-CdO 2 possesses extraordinary in-plane and out-of-plane SHG responses with large static SHG susceptibilities of χ sheet 14 (0) = χ sheet 25 (0) = χ sheet 36 (0) = 8.86 pm 2 V -1 due to the phase-matching between fundamental and second-harmonic light. In addition, the low thermal expansion and a large optical band gap of 3.24 eV endow the penta-CdO 2 sheet with a high laser-induced damage threshold. Discussions are also made on the penta-ZnO 2 sheet. This study expands the family of 2D materials with outstanding SHG performance.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Stochastic evaluation of four-component relativistic second-order many-body perturbation energies: A potentially quadratic-scaling correlation method

A second-order many-body perturbation correction to the relativistic Dirac-Hartree-Fock energy is evaluated stochastically by integrating 13-dimensional products of four-component spinors and Coulomb potentials. The integration in the real space of electron coordinates is carried out by the Monte Carlo (MC) method with the Metropolis sampling, whereas the MC integration in the imaginary-time domain is performed by the inverse-CDF (cumulative distribution function) method. The computational cost to reach a given relative statistical error for spatially compact but heavy molecules is observed to be no worse than cubic and possibly quadratic with the number of electrons or basis functions. This is a vast improvement over the quintic scaling of the conventional, deterministic second-order many-body perturbation method. The algorithm is also easily and efficiently parallelized with demonstrated 92% strong scalability going from 64 to 4096 processors for a fixed job size.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Porting fragmentation methods to GPUs using an OpenMP API: Offloading the resolution-of-the-identity second-order Møller–Plesset perturbation method

Here, using an OpenMP Application Programming Interface, the resolution-of-the-identity second-order Møller–Plesset perturbation (RI-MP2) method has been off-loaded onto graphical processing units (GPUs), both as a standalone method in the GAMESS electronic structure program and as an electron correlation energy component in the effective fragment molecular orbital (EFMO) framework. First, a new scheme has been proposed to maximize data digestion on GPUs that subsequently linearizes data transfer from central processing units (CPUs) to GPUs. Second, the GAMESS Fortran code has been interfaced with GPU numerical libraries (e.g., NVIDIA cuBLAS and cuSOLVER) for efficient matrix operations (e.g., matrix multiplication, matrix decomposition, and matrix inversion). The standalone GPU RI-MP2 code shows an increasing speedup of up to 7.5× using one NVIDIA V100 GPU with one IBM 42-core P9 CPU for calculations on fullerenes of increasing size from 40 to 260 carbon atoms using the 6-31G(d)/cc-pVDZ-RI basis sets. A single Summit node with six V100s can compute the RI-MP2 correlation energy of a cluster of 175 water molecules using the correlation consistent basis sets cc-pVDZ/cc-pVDZ-RI containing 4375 atomic orbitals and 14 700 auxiliary basis functions in ~0.85 h. In the EFMO framework, the GPU RI-MP2 component shows near linear scaling for a large number of V100s when computing the energy of an 1800-atom mesoporous silica nanoparticle in a bath of 4000 water molecules. The parallel efficiencies of the GPU RI-MP2 component with 2304 and 4608 V100s are 98.0% and 96.1%, respectively.

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

Second-harmonic generation in zinc blende crystals under combined action of femtosecond optical and strong terahertz fields

The influence of a short intense (with an electric field strength up to 250 kV cm{sup −1}) terahertz (THz) pulse on the generation of second harmonic (SH) of Ti : sapphire laser radiation in crystals of zinc blende type (InAs and GaAs), characterised by nonzero bulk quadratic susceptibility, is investigated. It is experimentally shown for InAs(100) that, in the case of s-polarised first and second harmonics, an application of s-polarised THz field changes significantly the SH signal. The THz field-induced azimuthal dependence of the SH signal is in good agreement with the results of theoretical calculation within a phenomenological approach. The dependence of the SH signal on the delay time between the optical and THz pulses is investigated. This dependence for the GaAs crystal repeats the envelope of the THz pulse intensity, whereas in the case of InAs crystal there is a significant discrepancy, caused by the nonlinear dynamics of strong THz field in InAs. (nonlinear optical phenomena)

36 MATERIALS SCIENCE↗
DOE OSTI2020

Accuracy of the duration estimates of ultrashort laser pulses using a single-shot second-order intensity autocorrelator

The accuracy of estimating the duration of single-cycle laser pulses with centre wavelengths of 910 and 780 nm is analysed using a single-shot second-order intensity autocorrelator. It is shown that estimates of the single-cycle pulse duration with an error of less than 5 % require the use of KDP crystals with a thickness of no more than 10 μm for the second harmonic generation. At the same time, to estimate the duration of a transform-limited pulse containing ten optical cycles, the crystal thickness can be up to 1 mm. In this case, at an optimum angle of convergence of the first-harmonic beams, the duration estimation error is less than 2 %. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗