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At least 577 records · Page 32
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

A Valentine’s tribute to Lab love: Watch clips from 1943 wedding of two staff

She was a secretary for Director J. Robert Oppenheimer. He was a physicist who helped create the world’s first atomic bombs. And for 65 years they were Mr. and Mrs. Bradner. Hugh Bradner was the first person that Marjorie Hall met upon arrival to join the Lab’s clandestine war-time efforts. He happened to be in Dorothy McKibbin’s Santa Fe office when Marjorie walked in. It was love at first sight, Marjorie recalled years later in an interview. The Bradners were married in September 1943 at McKibbin’s home. It was one of many weddings there during the Manhattan Project era. Los Alamos was fenced and guarded during this time, as staff raced to secretly develop nuclear weapons to help end World War II. Most were young – the average age was late 20s – and many, like the Bradners, met their lifelong partners then. The Bradners left Los Alamos after the war ended in 1945. Hugh is credited with inventing the neoprene wetsuit in 1951. The couple had one daughter. Marjorie, 89, and Hugh, 92, died just a few weeks apart in 2008 in California. Many of their home movies from their time in Los Alamos are preserved at the Lab. They are part of the collections in the National Security Research Center, which is the Lab’s classified library and also houses unclassified artifacts.

99 GENERAL AND MISCELLANEOUS↗
DOE OSTI2024

Assessment of the Impact of Realistic Sensor Physics and the Integration of Ex-Core Sensors on Reactor Power Synthesis

In the work documented in this report, a weighting function–based core power synthesis method was applied to multiple Monte Carlo N-Particle (MCNP) reactor models, which are informed based on simulated self-powered neutron detector (SPND) responses. The weighting function method used has been coined the point-based iterative (PBI) method. The goal of this application is to assess the impact of considering realistic sensor physics in the generation of the simulated SPND outputs as well as to consider how the synthesis is impacted based on the inclusion of ex-core detectors in the model. The NuScale small modular reactor (SMR) and Westinghouse AP1000 pressurized water reactor (PWR) are the models that served as the testbeds for the assessment of realistic sensor physics; this was achieved by using Geant4 SPND models in comparison with analytical models, such that the effect of electron transport in realistic SPND geometries in the Geant4 model can be understood in terms of synthesis error and convergence time. The comparison was considered for fuel burnup–induced perturbations, for a range of sensor string densities and synthesized power distribution axial fidelities. The Texas A&M Testing, Research, Isotopes, General Atomics Reactor (TAMU TRIGA) reactor MCNP model was used to assess the impact of ex-core sensors; this was done by performing synthesis with and without the ex-core detectors and by quantifying the synthesis error and number of iterations associated with Gaussian-type perturbations in many locations in the core. The TAMU TRIGA model was particularly pertinent for this study because of the interest in future experimental tests with SPNDs in this reactor, as well as the ease of modifying the MCNP model to include ex-core detectors with heterogeneously described response functions. Results from the comparison between the Geant4 and analytical SPND models indicate that similar average and maximum synthesis errors were obtained for burnup-induced perturbations in both the NuScale SMR and the AP1000. This was true for a range of sensor string densities and axial fidelities. However, there were marked differences between both the Geant4 and analytically informed models in terms of the iterations required to converge on the synthesized power distribution. Namely, the Geant4-informed models tended to lead to fewer iterations, except for a few sensor–core configurations that had particularly numerous iterations. Results from the ex-core sensor assessment with the TAMU TRIGA model indicate that the inclusion of ex-core sensors drastically reduces the synthesis error of Gaussian-type perturbations close to the edge of the core, and it slightly reduces synthesis errors for perturbations closer to the center of the core. This was achieved with a minimal increase in computational cost—that is, the number of iterations required for convergence. The errors were identified to be in the same location as the perturbation in the core, indicating that the methodology remains robust for unperturbed regions of the core. A secondary result from this study with the TAMU TRIGA was yielded by analysis of the neutron flux levels in the in-core and ex-core sensor locations of the core; these flux levels indicate that SPNDs could be used as both in-core and ex-core sensors, so long as the emitter material is sensitive to thermal neutrons. The results from these studies provide a quantitative understanding of the importance of considering realistic sensor physics and including ex-core sensors to perform accurate and timely power distribution synthesis of a reactor core.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2022

Thermodynamics of the Metal Carbonates and Bicarbonates of Mn, Co, Ni, Cu, and Zn Relevant to Mineral Energetics

The gas phase heats of formation of ground-state MCO 3 , M(HCO 3 ) 2 , and M(HCO 3 )(OH), where M = Mn, Co, Ni, Cu, and Zn, have been predicted using the correlated molecular orbital theory at the CCSD(T) level extrapolated to the complete basis set limit using the Feller–Peterson–Dixon (FPD) approach. Cohesive energies of the carbonates were predicted based on the calculated gas phase and experimental solid heats of formation. Coulombic dissociation energies (CDEs) between metal cations and anions show a near-linear correlation with Shannon metal cation atomic radii, yet no correlation is found with the hardness of these cations. The total reaction dissociation energies (TRDEs) of transition metals are higher than their CDEs for the di-bicarbonates, in contrast to those for Mg and Ca based on our prior work. In addition to differences in the energies needed to prepare the transition metal dications, electron donation from the ligands to the 3d orbitals of open-shell transition metal dications from lone pairs of adjacent O atoms also plays a role. No electron donation from the ligands to the fully occupied 3d orbitals of Zn and Cd was found. Decomposition energies for generating MO, CO 2 , and/or H 2 O were calculated. Gas phase metal exchange energies only partially correlate with the electrochemical series for M(s) → M 2+( aq). The FPD heats of formation were used to benchmark a range of density functional theory exchange–correlation functionals, including those commonly used in solid-state mineral calculations. None of the functionals provided chemical accuracy agreement (±1 kcal/mol) with the FPD results. So, the best agreement with the FPD results is predicted for the $\tau$-HCTH functional with an average unsigned error of 8.3 kcal/mol.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Propagation of priors for more accurate and efficient spectroscopic functional fits and their application to ferroelectric hysteresis

Multi-dimensional spectral-imaging is a mainstay of the scanning probe and electron microscopies, micro-Raman, and various forms of chemical imaging. In many cases, individual spectra can be fit to a specific functional form, with the model parameter maps, providing direct insight into material properties. Since spectra are often acquired across a spatial grid of points, spatially adjacent spectra are likely to be similar to one another; yet, this fact is almost never used when considering parameter estimation for functional fits. On datasets tried here, we show that by utilizing proximal information, whether it be in the spatial or spectral domains, it is possible to improve the reliability and increase the speed of such functional fits by ~2-3x, as compared to random priors. We explore and compare three distinct new methods: (1) spatially averaging neighborhood spectra, and propagating priors based on functional fits to the averaged case, (2) hierarchical clustering-based methods where spectra are grouped hierarchically based on response, with the priors propagated progressively down the hierarchy, and (3) regular clustering without hierarchical methods with priors propagated from fits to cluster means. Our results highlight that utilizing spatial and spectral neighborhood information is often critical for accurate parameter estimation in noisy environments, which we show for ferroelectric hysteresis loops acquired on a prototypical PbTiO3 thin film with piezoresponse spectroscopy. This method is general and applicable to any spatially measured spectra where functional forms are available. Examples include exploring the superconducting gap with tunneling spectroscopy, using the Dynes formula, or current-voltage curve fits in conductive atomic force microscopy mapping. Here we explore the problem for ferroelectric hysteresis, which, given its large parameter space, constitutes a more difficult task than, for example, fitting current-voltage curves with a Schottky emission formula.

42 ENGINEERING↗
DOE OSTI2023

Towards Realistic and High Fidelity Models for Nuclear Reactor Power Synthesis Simulation with Self-Powered Neutron Detectors

As presented in this report, a weighting function–based inferencing method is being applied to synthesize the power distribution in next-generation and university research reactors based on simulated self power neutron detector (SPND) responses. The overall goal is to assess the impacts of sensor uncertainty and true power distribution perturbations on the error in the synthesized power distribution. Regarding sensor uncertainty, the NuScale Small Modular Reactor (SMR) and the Westinghouse AP1000 serve as testbeds for analyzing the impact of varying the sensor uncertainty, as well as varying the number of sensors per sensor string in the reactor core. The reactor models are informed by Monte Carlo N-Particle (MCNP) neutron flux tallies. For the NuScale SMR and Westinghouse AP1000, the SPND response functions (i.e., the response of the SPNDs to individual segments of fuel) were determined homogeneously. Regarding an analysis of power distribution perturbation detection, the Texas A&M Testing, Research, Isotopes, General Atomics Reactor (TAMU TRIGA) reactor was used as a demonstration case with one particular arrangement of SPNDs; the response functions for this reactor model were determined heterogeneously, making this a uniquely high-fidelity demonstration of perturbation detection. Finally, SPND models generated in the Geometry and Tracking 4 (Geant4) code have been generated and tested for comparison with traditionally implemented analytical SPND models, with the intent for Geant4 integration with the full methodological framework. SPND current outputs as a function of distance from some fuel assembly segment in the NuScale SMR are compared with the analytically determined currents. Results from the sensor uncertainty simulations for the NuScale SMR and AP1000 indicate that the average error in the inferred power distribution on the fuel assembly segment level is reasonably low, being slightly less than the random uncertainty applied to all respective SPNDs in both cores. For example, if all SPNDs in the core have a random uncertainty of 5%, then the corresponding fuel assembly segment level error (i.e. difference between the true and inferred local power) is ~2–3%. However, the maximum error in the inferred power distribution on the fuel assembly segment level can be considerably high (>15%) when SPND random uncertainties start to exceed ~3%. In general, the average and maximum errors in the inferred power distribution were slightly higher in the AP1000 as opposed to the NuScale SMR for the sensor string configurations considered herein. Another result determined from analysis of the sensor uncertainty simulations was that increasing the number of SPNDs per string does not clearly reduce inferred power distribution error and can in fact make the error large in some cases; however, this assessment may skewed due to imposed iteration limits. Results from the perturbation detection demonstration using the high-fidelity TAMU TRIGA model indicate that, given the arrangement of 17 SPND strings and 4 SPNDs per string considered herein, there is a clear, provable ability to infer a localized Gaussian-type peak perturbation in the 3D power distribution. Such a perturbation was detected with an average fuel assembly segment level error of 0.19%, and the general visualization of the detected perturbation clearly indicates that the magnitude and shape were appropriately resolved. Finally, the electrical current output generated by the Geant4 modeled SPND indicates significant magnitude differences than the analytically modeled SPND, demonstrating the need for accurate SPND models which account for finite sensor geometry effects to inform the power synthesis work described herein.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2021

Flow reduction of hydrocarbon liquid in silica nanochannel: Insight from many-body dissipative particle dynamics simulations

A modified many-body dissipative particle dynamics (mDPD) model recently developed for realistic mesoscale multiphase flow simulations is rigorously parameterized, calibrated, and applied for elucidating the flow mechanisms of hydrocarbon liquids (i.e., heptane in this work) in amorphous silica cylindrical nanochannels with inner diameters ranging from 4.5 to 22.5 nm. The simulation results suggest the presence of a strong threshold of pressure gradient under which heptane cannot be driven to flow. The threshold for the 4.5 nm diameter pore is 10 to 100 times as high as for the 9–22.5 nm diameter pore, highlighting a remarkable nanoconfinement effect. Fluid viscosity is found to exhibit a shear-thinning phenomenon with intensity to weaken with increasing channel diameter — a phenomenon not observed in nanochannel flow of liquid water and gas in literature. Most remarkably, the radial profiles of average longitudinal flow velocity fitted by the modified Hagen-Poiseuille equation showed a negative slip length (–2.5% to –0.5% relative to the diameter) and a reduction of apparent permeability by 16% to 23%. Furthermore, this finding suggests silica nanochannels tend to deter hydrocarbon flow, a phenomenon that is opposed to the flow enhancement reported in most of the prior nanochannel flow studies in literature.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Towards Elucidating Structure–Spectra Relationships in Rhamnogalacturonan II: Computational Protocols for Accurate 13C and 1H Shifts for Apiose and Its Borate Esters

Apiose is a naturally occurring, uncommon branched-chain pentose found in plant cell walls as part of the complex polysaccharide Rhamnogalacturonan II (RG-II). The structural elucidation of the three-dimensional structure of RG-II by nuclear magnetic resonance (NMR) spectroscopy is significantly complicated by the ability of apiose to cross-link via borate ester linkages to form RG-II dimers. Here, we developed a computational approach to gain insight into the structure–spectra relationships of apio–borate complexes in an effort to complement experimental assignments of NMR signals in RG-II. Our protocol involved structure optimizations using density functional theory (DFT) followed by isotropic magnetic shielding constant calculations using the gauge-invariant atomic orbital (GIAO) approach to predict chemical shifts. We evaluated the accuracy of 23 different functional–basis set (FBS) combinations with and without implicit solvation for predicting the experimental 1 H and 13 C shifts of a methyl apioside and its three borate derivatives. The computed NMR predictions were evaluated on the basis of the overall shift accuracy, relative shift ordering, and the ability to distinguish between dimers and monomers. We demonstrate that the consideration of implicit solvation during geometry optimizations in addition to the magnetic shielding constant calculations greatly increases the accuracy of NMR chemical shift predictions and can correctly reproduce the ordering of the 13 C shifts and yield predictions that are, on average, within 1.50 ppm for 13 C and 0.12 ppm for 1 H shifts for apio–borate compounds.

BASIC BIOLOGICAL SCIENCES,BIOMASS FUELS↗
DOE OSTI2023

Chemical identification of new particle formation and growth precursors through positive matrix factorization of ambient ion measurements

Abstract. In the lower troposphere, rapid collisions between ions and trace gases result in the transfer of positive charge to the highest proton affinity species and negative charge to the lowest proton affinity species. Measurements of the chemical composition of ambient ions thus provide direct insight into the most acidic and basic trace gases and their ion–molecule clusters – compounds thought to be important for new particle formation and growth. We deployed an atmospheric pressure interface time-of-flight mass spectrometer (APi-ToF) to measure ambient ion chemical composition during the 2016 Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) campaign at the United States Department of Energy Atmospheric Radiation Measurement facility in the Southern Great Plains (SGP), an agricultural region. Cations and anions were measured for alternating periods of ∼ 24 h over 1 month. We use binned positive matrix factorization (binPMF) and generalized Kendrick analysis (GKA) to obtain information about the chemical formulas and temporal variation in ionic composition without the need for averaging over a long timescale or a priori high-resolution peak fitting. Negative ions consist of strong acids including sulfuric and nitric acid, organosulfates, and clusters of NO3- with highly oxygenated organic molecules (HOMs) derived from monoterpene (MT) and sesquiterpene (SQT) oxidation. Organonitrates derived from SQTs account for most of the HOM signal. Combined with the diel profiles and back trajectory analysis, these results suggest that NO3 radical chemistry is active at this site. SQT oxidation products likely contribute to particle growth at the SGP site. The positive ions consist of bases including alkyl pyridines and amines and a series of high-mass species. Nearly all the positive ions contained only one nitrogen atom and in general support ammonia and amines as being the dominant bases that could participate in new particle formation. Overall, this work demonstrates how APi-ToF measurements combined with binPMF analysis can provide insight into the temporal evolution of compounds important for new particle formation and growth.

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

Angularly resolved photoionization dynamics in atoms and molecules combining temporally and spectrally resolved experiments at ATTOLab and Synchrotron SOLEIL

We report results for XUV-IR two-photon ionization of Ar, Ne, NO, and O2, where an XUV attosecond pulse train is superimposed with a synchronized IR pulse, obtained at the ATTOLab laser facility using electron–ion coincidence 3D momentum spectroscopy. Temporally resolved photoelectron angular distributions providing angle-resolved time-delays for np ionization of Ar and Ne, achieved by reconstruction of attosecond beating by interference of two-photon transitions through a unified formalism (Joseph et al. in J Phys B At Mol Opt Phys 53:184007, 2020), are summarized. For inner valence XUV-IR dissociative photoionization of NO and O2 molecules, we report electron–ion kinetic energy correlation diagrams and disentangle the dissociative photoionization processes relying on parallel XUV experiments at Synchrotron SOLEIL. For ionization into the NO+(c3Π) ionic state, extending the formalism developed for single-photon ionization, we focus on photoelectron angular distributions averaged on the delay between the XUV and the IR field in the field frame, molecular frame, and electron frame of reference.

Joseph, J↗
DOE OSTI2020

Backpropagated frame transformation theory: A reformulation

In this work, the energy-dependent frame transformation theory of Gao and Greene [H. Gao and C. H. Greene, Phys. Rev. A 42, 6946 (1990)] is extended to yield a quantitatively accurate description of the dissociative recombination process. Evidence is presented to show that direct application of the original theory leads to inaccurate cross sections. A major revision, based on an interaction-free backpropagation of the Born-Oppenheimer solutions, markedly improves the frame transformation theory, reducing its average error by orders of magnitude. The original theory and its extension are tested on the previously explored two-dimensional (2D) model that is tailored to describe the singlet ungerade states of molecular hydrogen. The 2D model can be solved exactly (within the numerical accuracy) without implementing the Born-Oppenheimer approximation. These exact results then serve as a benchmark for the frame transformation theory developed in this paper.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Correlation-aware binning for small-angle neutron scattering via Gaussian-process inference

Binning in small-angle neutron scattering (SANS) is typically performed empirically, with fixed parameters chosen for convenience rather than statistical optimality. Such practices often fail to balance statistical precision and spatial resolution, leading to inconsistencies across instruments and datasets. Here we establish a correlation-aware framework that determines the optimal bin width from first principles by extending the classical Freedman–Diaconis (FD) rule to account for inter-bin correlations with a Gaussian process. In this formulation, the scattering intensity is treated as a smooth stochastic field whose statistical coherence is described by a covariance matrix. Analytical expressions of errors derived from this model yield closed-form criteria that separate the total deviation into contributions from counting noise, aliasing distortion and curvature-dependent correlation effects. Expressed in reduced variables, the resulting dimensionless error surface reveals a continuous transition from the uncorrelated FD regime to the correlation-dominated limit, providing a unified description of noise suppression and resolution control. Because the formulation depends only on the profile characteristics of scattering intensity I(Q), specifically its average intensity and first- and second-order derivatives, it applies generally to any SANS measurement regardless of sample, instrument or geometry. Experimental validation using small- and ultra-small-angle neutron scattering data confirms the predicted scaling behavior, demonstrating that correlation-aware inference systematically reduces mean-squared error and enables information-efficient reproducible data reduction across materials and instruments.

Tung, Chi-Huan [ORNL] (ORCID:0000000221972074)↗
DOE OSTI2022

The influence of nitrogen and nitrides on the structure and properties of proton irradiated ferritic/martensitic steel

The 12Cr1MoWV (wt%) ferritic/martensitic steel HT9 is a candidate material for fuel cladding in advanced nuclear reactors, such as the Versatile Test Reactor currently under development. As such, understanding the relationship between microstructure and mechanical properties in the context of irradiation environments for these steels is critical. N content, and more specifically interstitial N, has been hypothesized to be detrimental to irradiated properties at lower temperatures (less than 0.3T m ) to a total of 6 dpa; however, in this work at a dose of 1 dpa the irradiated microstructure was improved with added N, leading to less irradiation hardening. Three variants of HT9 were irradiated with 1.5 MeV protons to a dose of 1 dpa at 300°C. The HT9 variants included Low (10 ppm), Mid (190 ppm), and High (440 ppm) N alloys that were otherwise nearly identical. Changing the N content had a variety of effects on the irradiated defect structures. As N content increased, the average dislocation loop diameter decreased, while the number density of loops increased. Additionally, extensive Ni clustering was observed on dislocations and interfaces. The Mid and High N specimens exhibited significantly less hardening (ΔHV≃100) relative to the Low N specimen (ΔHV≃160). The decrease in hardening is attributed to vanadium carbonitride acting as a sink for Ni clusters that would otherwise form on dislocations. Under the irradiation conditions used, these results suggest increasing the N content in HT9 may have a desirable effect on the irradiated structure and properties at the dose studied, as well as the swelling resistance at higher doses. In other words, N content appears to be a powerful tool for tailoring the self-interstitial atom cluster mobility in F/M steels for different temperature and dose applications.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Electronic Configurational Transformation of Network Modifiers in Aluminate Glass above Megabar Pressures

Electronic responses of glasses under extreme pressures differ from those of crystalline analogs. Their distinct electronic environments are found in network formers with well-defined, covalent-bonded coordination environments (e.g., [4] Si and [4] Al) and in network modifiers with more disordered, ionic-bonded configurations (e.g., [5,6,7] Ca). Deciphering the evolution of the bonding environment of network modifier cations upon compression provides atomic insights into the pressure-driven hardening and transport properties of glasses. Despite the importance, in contrast to extensive efforts to uncover how network formers behave under pressure, considerable structural disorder around network modifiers makes it challenging to probe their electronic bonding environments under compression. Our understanding of the evolution of network modifiers above megabars is currently absent. Here, we report a discovery of highly densified electronic configurations of network modifier Ca in aluminate glass under extreme compression via the first inelastic X-ray scattering at the Ca L-edge up to 140 GPa. As evidenced by the prominent pressure-driven increases in electronic dispersion and delocalization, densified calcium environments are characterized by a decreased average Ca–O distance, the formation of highly coordinated calcium, a broader distribution of topological variables, and a greater distortion of Ca polyhedra above megabars. The spectral features for the Ca environments reveal significant electronic and bonding modifications, including pressure-driven increases in the ligand field interaction, the covalence characteristic of the Ca–O bond, and the electron–hole Coulomb interaction. These densification paths identify the electronic adaptation of network modifiers above megabars, shedding light on the origins of enhanced electron transport and the electron-storing capacity of glasses under pressure.

amorphous materials↗
DOE OSTI2022

Precision Tomography of a Three-Qubit Donor Quantum Processor in Silicon

Nuclear spins were among the first physical platforms to be considered for quantum information processing, because of their exceptional quantum coherence and atomic-scale footprint. However, their full potential for quantum computing has not yet been realized, owing to the lack of methods with which to link nuclear qubits within a scalable device combined with multi-qubit operations with sufficient fidelity to sustain fault-tolerant quantum computation. Here we demonstrate universal quantum logic operations using a pair of ion-implanted 31 P donor nuclei in a silicon nanoelectronic device. A nuclear two-qubit controlled-Z gate is obtained by imparting a geometric phase to a shared electron spin, and used to prepare entangled Bell states with fidelities up to 94.2(2.7)%. The quantum operations are precisely characterized using gate set tomography (GST), yielding one-qubit average gate fidelities up to 99.95(2)%, two-qubit average gate fidelity of 99.37(11)% and two-qubit preparation/measurement fidelities of 98.95(4)%. These three metrics indicate that nuclear spins in silicon are approaching the performance demanded in fault-tolerant quantum processors. We then demonstrate entanglement between the two nuclei and the shared electron by producing a Greenberger-Horne-Zeilinger three-qubit state with 92.5(1.0)% fidelity. Because electron spin qubits in semiconductors can be further coupled to other electrons or physically shuttled across different locations, these results establish a viable route for scalable quantum information processing using donor nuclear and electron spins.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Underlying mechanism of structural transformation between GaSb and GaAs response to intense electronic excitation

Ion irradiation of semiconductors has emerged as a promising approach for fabricating self-organized nanosystems with high atomic precision, despite often being accompanied by undesirable phenomena. Exploring the mechanisms underlying structural transformations is crucial for assessing nanostructure array types under complex irradiation environments. By quantitatively calculating the thermodynamically driven processes and analyzing the impact of intrinsic structural parameters, distinct structural transformations in response to intense electronic excitation are systematically investigated in gallium antimonide (GaSb) and gallium arsenide (GaAs) systems. In high-energy regimes, the nanofibers layer of GaSb exhibits intriguing structural discrepancy, characterized by partial nanofibers with coherent boundaries, interspersed nanopores accompanied by antisite defects and Ga precipitates, distinguishing to a series of discontinuous latent tracks that emerged within cylindrical trajectories in GaAs. Furthermore, significant diffusion behaviors of the nanohillocks are discovered in GaAs, with higher average roughness than GaSb, driven by the gradient stress distribution influenced by the free-surface effects. The deposition energy for melting phase formation, Gibbs free energy, and Ga diffusion coefficients contribute to the distinctive structural features, evidencing relatively stable morphological configurations and higher irradiation resistance in GaAs. Consequently, special optoelectronic properties associated with structural discrepancies facilitate the design and optimization of material functionalities by irradiation technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Alternate InP synthesis with aminophosphines: solution–liquid–solid nanowire growth

Indium phosphide nanowires are important components in high-speed electronics and optoelectronics, including photodetectors and photovoltaics. However, most syntheses either use high-temperature and costly vapor-phase methodology or highly toxic and pyrophoric tris(trimethylsilyl)phosphine. To expand on the success of the aminophosphine-based InP colloidal quantum dot synthesis, we developed a synthesis for thin (~11 nm) zinc blende InP nanowires at 180 °C using indium tris(trifluoroacetate) and tris(diethylamino)phosphine. A flat nanoribbon morphology was identified by transmission electron and atomic force microscopy analysis, with the stoichiometric (110) lattice plane exposed. Nanowire growth proceeded through a solution–liquid–solid mechanism from in situ-formed indium metal nanoparticles. Molecular byproducts of tris(oleylamino)phosphine oxide and N-oleyltrifluoroacetamide observed by 31 P and 19 F NMR spectroscopy inform a proposed mechanism of indium reduction by the aminophosphine. Morphological control over the nanowire product was achieved by varying the phosphorus injection to control the aspect ratio, the In : P ratio to toggle between nanowires and multipods, and the pre-hot injection evacuation step to favor a quantum dot product. Furthermore, replacing the indium precursor with indium tris(trifluoromethanesulfonate) was found to make bulk zinc blende InP nanowires with an average diameter of >250 nm and tens of microns in length.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Multifrequency stimulated Raman scattering of light in a calcite single crystal

Using pulses of multifrequency stimulated Raman scattering (SRS) in calcite, nonlinear photoluminescence in a stilbene molecular crystal is excited. When multifrequency SRS is excited by the radiation of a Nd{sup 3+} : YAG laser with a wavelength of 1064 nm, eleven anti-Stokes components are observed in the visible spectrum with an average frequency shift of 1086 cm{sup −1} between them. Using the second harmonic of the Nd {sup 3+} : YAG laser radiation allowed three anti-Stokes and four Stokes components to be recorded. The large spectral range of the frequency comb facilitated effective reduction in the duration and increase in the intensity of the radiation pulse of multifrequency SRS. (nonlinear optical phenomena)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Influence of Cation Size on the Local Atomic Structure and Electronic Properties of Ta Perovskite Oxynitrides

Partial anion substitution in transition metal oxides provides rich opportunities to control and tune physical and chemical properties, for example, combining the merits of oxides and nitrides. In addition, the possibility of resulting anion sublattice order provides a means to target polar and chiral structures based on a wide array of accessible structural archetypes by design. Here, in this work, we investigate the local structures of a family of perovskite tantalum oxynitrides—ATaO 2 N (A = Ba, Sr, and Ca)—using a combination of experimental and theoretical approaches including neutron total scattering, density functional theory (DFT), and ab initio molecular dynamics (AIMD) simulations. We present the first experimental study of chemical short-range order (CSRO) in CaTaO 2 N, confirming local cis N ordering of the anion sub-lattice. Our systematic exploration of a local structure across the A cation size series (from the larger Ba to the smaller Ca) reveals a perovskite motif increasingly distorted with respect to long-range average structures. DFT and AIMD simulations support the observed trends. Overall, structures with cis ordering of the nitrogen anions in each TaO 4 N 2 octahedron are favored over those with trans ordering. With diminishing A cation size, local cis ordering and Ta off-centering play decreasing roles in overall lattice stability, overshadowed by the stabilizing effects of octahedral tilting. The influence of these factors on local dipole formation and frustrated dipole ordering are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗