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DOE OSTI2020

Mercury linked to Deccan Traps volcanism, climate change and the end-Cretaceous mass extinction

Mercury (Hg) anomalies linked to Large Igneous Provinces (LIP) volcanism have been identified in sediments across all five major mass extinctions in Earth's history. This study tests whether Hg in marine sediments is a reliable proxy linking Deccan Traps volcanic eruptions to late Maastrichtian global climate warming and the mass extinction at the Cretaceous-Paleogene boundary (KPB). Our primary test site is the Elles section in Tunisia, the auxiliary Global Stratotype Section and Point (GSSP) to El Kef. Elles has the most complete marine sedimentary record and a high average sedimentation rate of ~4.7 cm/ky. Here, we chose the Hor Hahar section in Israel to corroborate the geographic distribution of Hg fallout from Deccan volcanism. Reliability of the Hg proxy over the last 550 ky of the Maastrichtian to early Danian was evaluated based on high-resolution age control (orbital cyclostratigraphy), stable isotope climate record, Hg concentrations, biotic turnover and mass extinction. These results were correlated with the pulsed Deccan eruptive history constrained previously by U-Pb zircon geochronology. Our results support Hg as robust proxy for Deccan volcanism with large Hg spikes marking “extreme event” (EE) pulsed eruptions correlative with climate warming peaks separated by steady, less intense eruptions. Long-term global climate warming began near ~350 ky pre-KPB, reached maximum warming (3–4 °C) between 285 and 200 ky pre-KPB, followed by gradual cooling and rapid temperature drop between 45 and 25 ky pre-KPB. During the last 25 ky before the KPB, multiple Hg EE eruptions correlate with hyperthermal warming that culminated in the rapid mass extinction at Elles during ≤1000 years of the Cretaceous. These latest Cretaceous Hg peaks may correlate with massive, distal, Deccan-sourced lava flows (>1000 km long) that traversed the Indian subcontinent and flowed into the Bay of Bengal, bracketing the mass extinction. These results support Deccan volcanism as a primary driver of the end-Cretaceous mass extinction.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

Investigations of effect of phase change mass transfer rate on cavitation process with homogeneous relaxation model

The super high fuel injection pressure and micro size of nozzle orifice has been an important development trend for the fuel injection system. Accordingly, cavitation transient process, fuel compressibility, amount of noncondensable gas in the fuel and cavitation erosion have attracted more attention. Based on the fact of cavitation in itself is a kind of thermodynamic phase change process, this paper takes the perspective of the cavitation phase change mass transfer process to analyze above mentioned phenomenon. The two-phase cavitating turbulent flow simulations with VOF approach coupled with HRM cavitation model and U-RANS of standard k-ε turbulence model were performed for investigations of cavitation phase change mass transfer process. It is concluded the mass transfer time scale coefficient in the Homogenous Relaxation Model (HRM) representing mass transfer rate should tend to be as small as possible in a condition that ensured the solver stable. At very fast mass transfer rate, the phase change occurs at very thin interface between liquid and vapor phase and condensation occurs more focused and then will contribute predictably to a more serious cavitation erosion. Both the initial non-condensable gas in fuel and the fuel compressibility can accelerate the cavitation mass transfer process.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Atomic masses with machine learning for the astrophysical r process

The astrophysical r process plays a vital role in the production of heavy elements. Modeling of the r process is sensitive to masses and further requires knowledge of masses beyond current experimental reach. Therefore, simulations of the r process offer a unique test bed for predicting mass extrapolations. We take a Machine-Learning (ML) approach to model the masses across the entire chart of nuclides. For the first time, we simulate r-process nucleosynthesis with a physics-based ML mass model. We compare simulated abundances to solar data in order to evaluate the model's performance far from stability. The resulting r-process abundances up to thorium and uranium qualitatively match those of the observed solar system abundance pattern, with the characteristic peaks well positioned. We propagate the mass uncertainties obtained from the ML model to r-process abundance yields to estimate an uncertainty band associated with our approach. The size of the uncertainty band is approximately one order of magnitude which aligns with the uncertainty reported using alternative techniques.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2018

Added-mass effects on a horizontal-axis tidal turbine using FAST v8

Added mass on tidal turbine blades has the potential to alter the blade dynamic response, such as natural frequencies and vibration amplitudes, as a response to blade acceleration. Currently, most aeroelastic design tools do not consider such effects as they are complex and expensive to model, and they are not an intrinsic part of most blade-element momentum theory codes, which are commonly used in the tidal energy industry. This article outlines the addition of added-mass effects to the National Renewable Energy Laboratory's design tool FAST v8. A verification is presented for a spring-mass system with an initial displacement, and a case study is performed for the Reference Model 1 20-m-diameter tidal turbine. For the 20-m-diameter turbine, it was shown that the natural frequency of vibration is reduced by 65% when added mass is considered. Further, the thrust loads are increased by 2.5% when the blades are excited by a 5% step increase in inflow velocity when added mass is considered. This decrease can have a significant impact on the overall turbine design, as it is important to design the blades with a natural frequency so that they are not excited by the rotor speed and its harmonics, wherein aerodynamic excitation can lead to fatigue damage. However, it was shown that when turbulent inflow with an intensity of 20% was modeled, there was almost no impact on the loads and blade displacement with added-mass effects except for a small difference in the fatigue response of the blade to turbulent load fluctuations.

13 HYDRO ENERGY↗

DOE OSTI2013

Synchrotron based mass spectrometry to investigate the molecular properties of mineral-organic associations

Soil organic matter (OM) is important because its decay drives life processes in the biosphere. Analysis of organic compounds in geological systems is difficult because of their intimate association with mineral surfaces. To date there is no procedure capable of quantitatively separating organic from mineral phases without creating artifacts or mass loss. Therefore, analytical techniques that can (a) generate information about both organic and mineral phases simultaneously and (b) allow the examination of predetermined high-interest regions of the sample as opposed to conventional bulk analytical techniques are valuable. Laser Desorption Synchrotron Postionization (synchrotron-LDPI) mass spectrometry is introduced as a novel analytical tool to characterize the molecular properties of organic compounds in mineral-organic samples from terrestrial systems, and it is demonstrated that when combined with Secondary Ion Mass Spectrometry (SIMS), can provide complementary information on mineral composition. Mass spectrometry along a decomposition gradient in density fractions, verifies the consistency of our results with bulk analytical techniques. We further demonstrate that by changing laser and photoionization energies, variations in molecular stability of organic compounds associated with mineral surfaces can be determined. The combination of synchrotron-LDPI and SIMS shows that the energetic conditions involved in desorption and ionization of organic matter may be a greater determinant of mass spectral signatures than the inherent molecular structure of the organic compounds investigated. The latter has implications for molecular models of natural organic matter that are based on mass spectrometric information.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Single-Particle Isotopic Analysis Using the Liquid Sampling-Atmospheric Pressure Glow Discharge Microplasma Coupled to an Orbitrap Mass Spectrometer

Isotope ratio (IR) determinations on individual particles can provide valuable information relative to the sample, including processing and dating, which could be valuable to geological and nuclear material analysis communities. In comparison to “bulk” measurements, in which all particle information is lost and homogenized within a sample, “particle” measurements allow for fingerprinting and can provide unique insights related to the sample’s nano- and micro- compositions. Furthermore, the complex nature of particles, with potential isobaric interferences from either the matrix or other elements within the same particle, poses a significant analytical challenge for conventional mass spectrometry platforms employed for elemental analysis due to their limited mass resolution. Presented here is the first demonstration of an ultrahigh resolution method for single particle (SP) isotopic analysis using the liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma ionization source coupled to an Orbitrap mass spectrometer and FTMS Booster X2T acquisition/processing system. For proof of concept, well-characterized CeO 2 microparticles with a nominal diameter of 1.0 μm were analyzed at a mass resolution of ∼330,000. Important instrumental parameters were optimized to enable the detection of single particles. The 142 Ce/ 140 Ce ratio of individual particles and the population average were determined and compared to an SP inductively coupled plasma time-of-flight mass spectrometry (ICP-TOF-MS) analysis. The isotopic accuracy and precision were determined by two methods and found to be in good agreement with the SP-ICP-TOF-MS method, with the linear regression slope method providing a more accurate ratio, showing a ∼1.4% relative difference from the ratio determined from a particle digest. The encouraging performance of the method was further supported by a determined detection limit of 2.9 fg ( 142 Ce). The developed method is anticipated to overcome many of the challenges posed by isobaric interferences encountered in conventional mass spectrometry techniques when analyzing real-world samples for particle isotopic composition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2013

Deconstruction of Activity-Dependent Covalent Modification of Heme in Human Neutrophil Myeloperoxidase by Multistage Mass Spectrometry (MS[superscript 4])

Myeloperoxidase (MPO) is known to be inactivated and covalently modified by treatment with hydrogen peroxide and agents similar to 3-(2-ethoxypropyl)-2-thioxo-2,3-dihydro-1H-purin-6(9H)-one (1), a 254.08 Da derivative of 2-thioxanthine. Peptide mapping by liquid chromatography and mass spectrometry detected modification by 1 in a labile peptide-heme-peptide fragment of the enzyme, accompanied by a mass increase of 252.08 Da. The loss of two hydrogen atoms was consistent with mechanism-based oxidative coupling. Multistage mass spectrometry (MS{sup 4}) of the modified fragment in an ion trap/Orbitrap spectrometer demonstrated that 1 was coupled directly to heme. Use of a 10 amu window delivered the full isotopic envelope of each precursor ion to collision-induced dissociation, preserving definitive isotopic profiles for iron-containing fragments through successive steps of multistage mass spectrometry. Iron isotope signatures and accurate mass measurements supported the structural assignments. Crystallographic analysis confirmed linkage between the methyl substituent of the heme pyrrole D ring and the sulfur atom of 1. The final orientation of 1 perpendicular to the plane of the heme ring suggested a mechanism consisting of two consecutive one-electron oxidations of 1 by MPO. Multistage mass spectrometry using stage-specific collision energies permits stepwise deconstruction of modifications of heme enzymes containing covalent links between the heme group and the polypeptide chain.

08 HYDROGEN↗

DOE OSTI2021

MolDiscovery: learning mass spectrometry fragmentation of small molecules

Identification of small molecules is a critical task in various areas of life science. Recent advances in mass spectrometry have enabled the collection of tandem mass spectra of small molecules from hundreds of thousands of environments. To identify which molecules are present in a sample, one can search mass spectra collected from the sample against millions of molecular structures in small molecule databases. The existing approaches are based on chemistry domain knowledge, and they fail to explain many of the peaks in mass spectra of small molecules. Here, we present molDiscovery, a mass spectral database search method that improves both efficiency and accuracy of small molecule identification by learning a probabilistic model to match small molecules with their mass spectra. A search of over 8 million spectra from the Global Natural Product Social molecular networking infrastructure shows that molDiscovery correctly identify six times more unique small molecules than previous methods.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2012

Comparison of nuclear mass models at nuclearmasses.org

Nuclear masses are crucial in many astrophysics studies, as well as other areas of basic and applied nuclear science. There are now many different global theoretical models of nuclear masses - but choosing the best model for a given application can be challenging. The suite of codes online at nuclearmasses.org greatly facilitates the comparison of nuclear models with evaluated masses as well as the intercomparison of theoretical models. We demonstrate the utility of this suite by comparing the RMS deviations of 13 different theoretical mass models from the AME2003 evaluated masses over mass ranges appropriate for astrophysics.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2014

Optically detected, single nanoparticle mass spectrometer with pre-filtered electrospray nanoparticle source

An instrument designed for non-destructive mass analysis of single trapped nanoparticles is described. The heart of the instrument is a 3D quadrupole (Paul) trap constructed to give optical access to the trap center along ten directions, allowing passage of lasers for particle heating and detection, particle injection, collection of scattered or fluorescent photons for particle detection and mass analysis, and collection of particles on TEM grids for analysis, as needed. Nanoparticles are injected using an electrospray ionization (ESI) source, and conditions are described for spraying and trapping polymer particles, bare metal particles, and ligand stabilized particles with masses ranging from 200 kDa to >3 GDa. Conditions appropriate to ESI and injection of different types of particles are described. The instrument is equipped with two ion guides separating the ESI source and nanoparticle trap. The first ion guide is mostly to allow desolvation and differential pumping before the particles enter the trap section of the instrument. The second is a linear quadrupole guide, which can be operated in mass selective or mass band-pass modes to limit transmission to species with mass-to-charge ratios in the range of interest. With a little experience, the design allows injection of single particles into the trap upon demand.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Impact of surface and residual stresses and electro-/magnetostatic axial loading on the suspended nanomechanical based mass sensors: A theoretical study

Suspended nanomechanical mass sensors are capable to detect the attached molecules or particles through the shifts in the resonant frequencies. However, surface and residual stresses can as well cause a shift of the sensor resonances. As result, understanding the impact of stresses in an accuracy and sensitivity of the mass sensors is a fundamental requirement for a rigorous analysis of experimental data. Here, we present a detailed theoretical study of the suspended nanomechanical resonators and mass sensors under axial load created by surface (residual) stresses or electrostatic (magnetostatic) forces. Easily accessible formulas allowing one either to accurately predict the resonant frequencies of the beam under tension/compression or to disentangle the effects of stresses (axial forces) and the molecule mass on the frequency shift of the suspended mass sensors have been derived. A dimensionless parameter enabling us a simple characterization of the device vibrational regime (i.e., beam, string, or beam-to-string transition) has been identified. Based on the results, the applicability limits of the classical beam theory with and without axial loading have been found. We also show that tuning the beam resonant frequencies enhances the mass sensitivity.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2014

PINGU sensitivity to neutrino mass hierarchy

Determination of the neutrino mass hierarchy (NMH) is among the most fundamental questions in particle physics. Recent measurements of 1) a large mixing angle between the first and the third neutrino mass eigenstates and 2) the first observation of atmospheric neutrino oscillations at tens of GeV with neutrino telescopes, open the intriguing new possibility to exploit matter effects in neutrino oscillation to determine the neutrino mass hierarchy. A further extension of IceCube/DeepCore called PINGU (Precision IceCube Next Generation Upgrade) has been recently envisioned with the ultimate goal to measure neutrino mass hierarchy. PINGU would consist of additional IceCube-like strings of detectors deployed in the deepest and cleanest ice in the center of IceCube. More densely deployed instrumentation would provide a threshold substantially below 10 GeV and enhance the sensitivity to the mass hierarchy signal in atmospheric neutrinos. Here we discuss an estimate of the PINGU sensitivity to the mass hierarchy determined using an approximation with an Asimov dataset and an oscillation parameter fit.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2015

Removal of ordering ambiguity for a class of position dependent mass quantum systems with an application to the quadratic Liénard type nonlinear oscillators

We consider the problem of removal of ordering ambiguity in position dependent mass quantum systems characterized by a generalized position dependent mass Hamiltonian which generalizes a number of Hermitian as well as non-Hermitian ordered forms of the Hamiltonian. We implement point canonical transformation method to map one-dimensional time-independent position dependent mass Schrödinger equation endowed with potentials onto constant mass counterparts which are considered to be exactly solvable. We observe that a class of mass functions and the corresponding potentials give rise to solutions that do not depend on any particular ordering, leading to the removal of ambiguity in it. In this case, it is imperative that the ordering is Hermitian. For non-Hermitian ordering, we show that the class of systems can also be exactly solvable and is also shown to be iso-spectral using suitable similarity transformations. We also discuss the normalization of the eigenfunctions obtained from both Hermitian and non-Hermitian orderings. We illustrate the technique with the quadratic Liénard type nonlinear oscillators, which admit position dependent mass Hamiltonians.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

Effect of {sup 12}C+{sup 12}C reaction and convective mixing on the progenitor mass of ONe white dwarfs

Stars in the mass range ∼8 - 12 M{sub ⊙} are the most numerous massive stars. This mass range is critical because it may lead to supernova (SN) explosion, so it is important for the production of heavy elements and the chemical evolution of the galaxy. We investigate the critical transition mass (M{sub up}), which is the minimum initial stellar mass that attains the conditions for hydrostatic carbon burning. Stars of masses < M{sub up} evolve to the Asymptotic Giant Branch and then develop CO White Dwarfs, while stars of masses ≥ M{sub up} ignite carbon in a partially degenerate CO core and form electron degenerate ONe cores. These stars evolve to the Super AGB (SAGB) phase and either become progenitors of ONe White Dwarfs or eventually explode as electron-capture SN (EC-SN). We study the sensitivity of M{sub up} to the C-burning reaction rate and to the treatment of convective mixing. In particular, we show the effect of a recent determination of the {sup 12}C+{sup 12}C fusion rate, as well as the extension of the convective core during hydrogen and helium burning on M{sub up} in solar metallicity stars. We choose the 9 M{sub ⊙} model to show the detailed characteristics of the evolution with the new C-burning rate.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2016

Hole effective masses and subband splitting in type-II superlattice infrared detectors

We explore band structure effects to help determine the suitability of n-type type-II superlattice (T2SL) absorbers for infrared detectors. It is often assumed that the exceedingly large growth-direction band-edge curvature hole effective mass in n-type long wavelength infrared (LWIR) T2SL would lead to low hole mobility and therefore low detector collection quantum efficiency. We computed the thermally averaged conductivity effective mass and show that the LWIR T2SL hole conductivity effective mass along the growth direction can be orders of magnitude smaller than the corresponding band-edge effective mass. LWIR InAs/GaSb T2SL can have significantly smaller growth-direction hole conductivity effective mass than its InAs/InAsSb counterpart. For the InAs/InAsSb T2SL, higher Sb fraction is more favorable for hole transport. Achieving long hole diffusion length becomes progressively more difficult for the InAs/InAsSb T2SL as the cutoff wavelength increases, since its growth-direction hole conductivity effective mass increases significantly with decreasing band gap. However, this is mitigated by the fact that the splitting between the top valence subbands also increases with the cutoff wavelength, leading to reduced inter-subband scattering and increased relaxation time.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

Imaging Dirac-mass disorder from magnetic dopant atoms in the ferromagnetic topological insulator Cr x (Bi 0.1 Sb 0.9 ) 2-x Te 3

To achieve and use the most exotic electronic phenomena predicted for the surface states of 3D topological insulators (TIs), it is necessary to open a “Dirac-mass gap” in their spectrum by breaking time-reversal symmetry. Use of magnetic dopant atoms to generate a ferromagnetic state is the most widely applied approach. However, it is unknown how the spatial arrangements of the magnetic dopant atoms influence the Dirac-mass gap at the atomic scale or, conversely, whether the ferromagnetic interactions between dopant atoms are influenced by the topological surface states. Here we image the locations of the magnetic (Cr) dopant atoms in the ferromagnetic TI Cr₀.₀₈(Bi₀.₁Sb₀.₉)₁.₉₂Te₃. Simultaneous visualization of the Dirac-mass gap Δ(r) reveals its intense disorder, which we demonstrate is directly related to fluctuations in n(r), the Cr atom areal density in the termination layer. We find the relationship of surface-state Fermi wavevectors to the anisotropic structure of Δ(r) not inconsistent with predictions for surface ferromagnetism mediated by those states. Moreover, despite the intense Dirac-mass disorder, the anticipated relationship Δ(r)∝n(r) is confirmed throughout and exhibits an electron–dopant interaction energy J* = 145 meV·nm². In addition, these observations reveal how magnetic dopant atoms actually generate the TI mass gap locally and that, to achieve the novel physics expected of time-reversal symmetry breaking TI materials, control of the resulting Dirac-mass gap disorder will be essential.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2013

EVOLUTION IN THE H I GAS CONTENT OF GALAXY GROUPS: PRE-PROCESSING AND MASS ASSEMBLY IN THE CURRENT EPOCH

We present an analysis of the neutral hydrogen (H I) content and distribution of galaxies in groups as a function of their parent dark matter halo mass. The Arecibo Legacy Fast ALFA survey α.40 data release allows us, for the first time, to study the H I properties of over 740 galaxy groups in the volume of sky common to the Sloan Digital Sky Survey (SDSS) and ALFALFA surveys. We assigned ALFALFA H I detections a group membership based on an existing magnitude/volume-limited SDSS Data Release 7 group/cluster catalog. Additionally, we assigned group ''proximity' membership to H I detected objects whose optical counterpart falls below the limiting optical magnitude—thereby not contributing substantially to the estimate of the group stellar mass, but significantly to the total group H I mass. We find that only 25% of the H I detected galaxies reside in groups or clusters, in contrast to approximately half of all optically detected galaxies. Further, we plot the relative positions of optical and H I detections in groups as a function of parent dark matter halo mass to reveal strong evidence that H I is being processed in galaxies as a result of the group environment: as optical membership increases, groups become increasingly deficient of H I rich galaxies at their center and the H I distribution of galaxies in the most massive groups starts to resemble the distribution observed in comparatively more extreme cluster environments. We find that the lowest H I mass objects lose their gas first as they are processed in the group environment, and it is evident that the infall of gas rich objects is important to the continuing growth of large scale structure at the present epoch, replenishing the neutral gas supply of groups. Finally, we compare our results to those of cosmological simulations and find that current models cannot simultaneously predict the H I selected halo occupation distribution for both low and high mass halos.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2015

The relationship between stellar mass, gas metallicity, and star formation rate for Hα-selected galaxies at z ≈ 0.8 from the NewHα survey

Using a sample of 299 Hα-selected galaxies at z≈0.8, we study the relationship between galaxy stellar mass, gas-phase metallicity, and star formation rate (SFR), and compare to previous results. We use deep optical spectra obtained with the IMACS spectrograph at the Magellan telescope to measure strong oxygen lines. We combine these spectra and metallicities with (1) rest-frame UV-to-optical imaging, which allows us to determine stellar masses and dust attenuation corrections, and (2) Hα narrowband imaging, which provides a robust measurement of the instantaneous SFR. Our sample spans stellar masses of ∼10{sup 9}–6 × 10{sup 11} M{sub ⊙}, SFRs of 0.4–270 M{sub ⊙} yr{sup −1}, and metal abundances of 12+log(O/H)≈8.3–9.1 (≈0.4–2.6 Z{sub ⊙}). The correlations that we find between the Hα-based SFR and stellar mass (i.e., the star-forming “main sequence”) and between the stellar mass and metallicity are both consistent with previous z∼1 studies of star-forming galaxies. We then study the relationship between the three properties using various plane-fitting techniques and a curve-fitting projection. In all cases, we exclude strong dependence of the M{sub ⋆}–Z relation on SFR, but are unable to distinguish between moderate and no dependence. Our results are consistent with previous mass–metallicity–SFR studies. We check whether data set limitations may obscure a strong dependence on the SFR by using mock samples drawn from the Sloan Digital Sky Survey. These experiments reveal that the adopted signal-to-noise ratio cuts may have a significant effect on the measured dependence. Further work is needed to investigate these results, and to test whether a “fundamental metallicity relation” or a “fundamental plane” describes star-forming galaxies across cosmic time.

79 ASTRONOMY AND ASTROPHYSICS↗