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196 records · Page 11

Impacts of Stratospheric Ozone Recovery on Southern Ocean Temperature and Heat Budget

The impacts of stratospheric ozone recovery on Southern Ocean surface and interior temperature, heat content, heat uptake, and heat transport are investigated by contrasting two ensemble chemistry-climate model simulations in 2005–2099: one with fixed ozone depleting substances (ODSs) and another with decreasing ODSs. In our simulations ozone recovery significantly affects Southern Ocean temperature, with large latitudinal and vertical variations. Ozone recovery causes a dipole change of the full-depth ocean heat content (OHC) with an increase south of 60°S and a decrease between 45°S and 60°S. Integrated over latitudes south of 40°S, OHC decreases in response to ozone recovery. This ocean heat loss is shown to be driven by weakened poleward ocean heat transport (OHT) across 40°S, which is partly canceled by enhanced heat uptake. The weakening of poleward OHT into the Southern Ocean is caused by the ozone-induced equatorward shift of the meridional overturning circulation.

stratospheric ozone↗

Projected Changes in Temperature and Precipitation Over the United States, Central America, and the Caribbean in CMIP6 GCMs

The Coupled Model Intercomparison Project Phase 6 (CMIP6) dataset is used to examine projected changes in temperature and precipitation over the United States (U.S.), Central America and the Caribbean. The changes are computed using an ensemble of 31 models for three future time slices (2021–2040, 2041–2060, and 2080–2099) relative to the reference period (1995–2014) under three Shared Socioeconomic Pathways (SSPs; SSP1-2.6, SSP2-4.5, and SSP5-8.5). The CMIP6 ensemble reproduces the observed annual cycle and distribution of mean annual temperature and precipitation with biases between – 0.93 and 1.27 °C and – 37.90 to 58.45%, respectively, for most of the region. However, modeled precipitation is too large over the western and Midwestern U.S. during winter and spring and over the North American monsoon region in summer, while too small over southern Central America. Temperature is projected to increase over the entire domain under all three SSPs, by as much as 6 °C under SSP5-8.5, and with more pronounced increases in the northern latitudes over the regions that receive snow in the present climate. Annual precipitation projections for the end of the twenty-first century have more uncertainty, as expected, and exhibit a meridional dipole-like pattern, with precipitation increasing by 10–30% over much of the U.S. and decreasing by 10–40% over Central America and the Caribbean, especially over the monsoon region. Seasonally, precipitation over the eastern and central subregions is projected to increase during winter and spring and decrease during summer and autumn. Over the monsoon region and Central America, precipitation is projected to decrease in all seasons except autumn. The analysis was repeated on a subset of 9 models with the best performance in the reference period; however, no significant difference was found, suggesting that model bias is not strongly influencing the projections.

54 ENVIRONMENTAL SCIENCES↗

Modeling of the Magnetosphere-Ionosphere-Atmosphere System

This grant covered the transition period between the ISTP/GGS main mission MAMI work (NAGW5-1097) to the extended mission of GGS/SolaxMax. During this period we concentrated on the following subjects: (1) Ionospheric modeling and in particular the coupling of the ionosphere and the magnetosphere require knowledge of the ionospheric conductances. We have an algorithm to derive these conductances from POLAR UVI or POLAR VIS images. The image analysis requires carefully calibrated measurements, separation of auroral brightness from scattered solar EUV and emissions caused by photoelectrons, and modeling of the auroral conditions, Under this grant we evaluated the various sources of uncertainty that contribute to the conductance calculation by comparing different model approaches and we conducted sensitivity studies. A joint modeling effort between our ionospheric models and a global MHD magnetospheric model with S. Slinker and J. Fedder lead to improved parameterizations for the MHD model. The predictions of that new model were validated using data from ground based instruments, POLAR UVI images, and DMSP satellites. These findings were presented at the GEM meeting in Snowmass, and at the Huntsville modeling workshop in Guntersville. A manuscript for publication is in preparation. A study to evaluate the thermospheric effects of large substorms and storms was con- ducted with the TIE-GCM model. Of particular interest are compositional changes of the thermosphere in the southern hemisphere. Southern hemisphere effects are stronger than those on the northern hemisphere because of the larger offset of the magnetic dipole from the rotational axis. These results were presented at the Huntsville modeling workshop in Guntersville.

Source record↗

ELECTRONIC STRUCTURE METHODS AND PROTOCOLS WITH APPLICATION TO DYNAMICS, KINETICS AND THERMOCHEMISTRY

Hydrocarbon combustion involves the reaction dynamics of a tremendous number of species beginning with many-component fuel mixtures and proceeding via a complex system of intermediates to form primary and secondary products. Combustion conditions corresponding to new advanced engines and/or alternative fuels rely increasingly on autoignition and low-temperature-combustion chemistry. In these regimes various transient radical species such as HO2, ROO·, ·QOOH, HCO, NO2, HOCO, and Criegee intermediates play important roles in determining the detailed as well as more general dynamics. A clear understanding and accurate representation of these processes is needed for effective modeling. Given the difficulties associated with making reliable experimental measurements of these systems, computation can play an important role in developing these energy technologies. Accurate calculations have their own challenges since even within the simplest dynamical approximations such as transition state theory, the rates depend exponentially on critical barrier heights and these may be sensitive to the level of quantum chemistry. Moreover, it is well-known that in many cases it is necessary to go beyond statistical theories and consider the dynamics. Quantum tunneling, resonances, radiative transitions, and non-adiabatic effects governed by spin-orbit or derivative coupling can be determining factors in those dynamics. Building upon progress made during a period of prior support through the DOE Early Career Program, this project combines developments in the areas of potential energy surface (PES) fitting and multistate multireference quantum chemistry to allow spectroscopically and dynamically/kinetically accurate investigations of key molecular systems (such as those mentioned above), many of which are radicals with strong multireference character and have the possibility of multiple electronic states contributing to the observed dynamics. An ongoing area of investigation is to develop general strategies for robustly convergent electronic structure theory for global multichannel reactive surfaces including diabatization of energy and other relevant surfaces such as dipole transition. Combining advances in ab initio methods with automated interpolative PES fitting allows the construction of high-quality PESs (incorporating thousands of high-level data) to be done rapidly through parallel processing on high-performance computing (HPC) clusters. In addition, new methods and approaches to electronic structure theory will be developed and tested through applications. This project will explore limitations in traditional multireference calculations (e.g., MRCI) such as those imposed by internal contraction, lack of high-order correlation treatment and poor scaling. Methods such as DMRG-based extended active-space CASSCF and various Quantum Monte Carlo (QMC) methods will be applied (including VMC/DMC and FCIQMC). Insight into the relative significance of different orbital spaces and the robustness of application of these approaches on leadership class computing architectures will be gained. Synergy with other components of this research program such as automated PES fitting and multireference quantum chemistry will be used to address challenges encountered by the standard approaches to computational thermochemistry (those being single-reference quantum chemistry and perturbative treatments of the anharmonic vibrational energy, which break down for some cases of electronic structure or floppy strongly coupled vibrational modes).

74 ATOMIC AND MOLECULAR PHYSICS↗

Fine structure of the isovector giant dipole resonance in Nd 142 – 150 and Sm 152

Inelastic proton scattering at energies of a few hundred MeV and very-forward scattering angles including 0° has been established as a tool for the study of electric-dipole strength distributions in nuclei. The present work reports a systematic investigation of the chain of stable even-mass Nd isotopes representing a transition from spherical to quadrupole-deformed nuclei. Extraction of the equivalent photo-absorption cross sections and analysis of their fine structure in the energy region of the isovector giant dipole resonance (IVGDR). Method: Proton inelastic scattering reactions of 200 MeV protons were measured at the iThemba Laboratory for Accelerator Based Sciences in Cape Town, South Africa. The scattering products were momentum-analyzed by the K600 magnetic spectrometer positioned at θ Lab = 0°. Using dispersion-matching techniques, energy resolutions of ΔE ≈ 40–50 keV (full width at half maximum) were obtained. After subtraction of background and contributions from other multipoles, the spectra were converted to photoabsorption cross sections using the equivalent virtual-photon method. Wavelet-analysis techniques are used to extract characteristic energy scales of the fine structure of the IVGDR from the experimental data. Fine structure of the IVGDR is observed even for the most deformed nuclei studied. Comparisons between the extracted experimental energy scales and those energy scales obtained from the quasiparticle-phonon model (QPM) and Skyrme separable random phase approximation (SSRPA) predictions provide insight into the role of different giant-resonance damping mechanisms. It can be seen that the scales in the spherical and most likely also in the deformed nuclei mainly result from the fragmentation of the one-particle-one-hole (1p1h) strength into several dominant transitions serving as doorway states. In cases where calculations beyond the 1p1h level are available, some impact of the spreading due to coupling of the two-particle-two-hole (2p2h) states to the 1p1h doorway states is observed. New virtual-photon absorption data for the chain of stable Nd isotopes and 152 Sm are presented, with a focus on the phenomenon of nonstatistical cross-section fluctuations, referred to as fine structure, in the energy region of the IVGDR. The wavelet-analysis techniques used allowed for the features of the fine structure to be quantified in the form of characteristic scales. Finally, comparisons between experimental results and model predictions indicate that Landau damping seems to be the main source of the fine structure in both the spherical and deformed nuclei, but calculations including 2p2h degrees of freedom would be beneficial to confirm this for the deformed cases.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Synthetic Tuning of Exciton–Phonon Coupling in Janus WS 2(1-x) Se 2x Monolayers Revealed by Resonant Raman Excitation Spectroscopy for Optoelectronic Applications

Janus monolayers, such as WSSe, have broken out-of-plane symmetry and an intrinsic dipole moment, impacting exciton transport, lifetime, and phonon interactions while imbuing piezoelectric, photocatalytic, and Rashba spin-splitting properties to transition metal dichalcogenides (TMDs). The new properties of this atomically thin material can be used for optoelectronic device applications. As TMDs are converted into Janus monolayers, e.g., top selenization of WS2 to WSSe, the bandgap and structure smoothly evolve, impacting not only the formation of excitons but also their complex interactions with different phonon modes. Resonant Raman excitation profiles (REPs) are uniquely well-suited to reveal both excitonic transitions and exciton–phonon coupling. Here, the resonant REPs of $A^{'}_{1}$ WS 2 and A 1 WSSe modes are measured to understand the strength of their coupling with the A, B, and C excitonic bands of a WS2 monolayer throughout its stepwise transformation into Janus WSSe by pulsed laser deposition (PLD) of energetic selenium species. In situ Raman spectroscopy during deposition is used to controllably prepare stable intermediate Janus structures, WS 2(1-x) Se 2x (0 ≤ x ≤ 0.5), for ex situ measurement of their resonant REPs. As x increases, REPs reveal not only pronounced excitonic bands that gradually shift toward lower photon energies but also strong, mode-selective exciton–phonon coupling. First-principles resonant Raman simulations independently predict this spectral behavior and are shown capable of matching the spectrally broadened, experimentally observed REP profiles in this model system, indicating their strong predictive capability for future experiments. The combination of controlled synthesis, REP characterization, and predictive theory employed here demonstrates a powerful pathway to understand and ultimately tune exciton–phonon interactions for future quantum optical devices.

Janus monolayers↗

Editorial: Understanding the Causes of Asymmetries in Earth’S Magnetosphere-Ionosphere System

Geomagnetic activity observed in geospace, the upper atmosphere, and on the ground results from solar-terrestrial interactions. Such interactions correspond to the coupling between the solar wind, magnetosphere, and the thermosphere-ionosphere (MIT) system (Khazanov, 2016). However, given the complexity of the whole system and its large spatial scale and long-term solar variability, effects resulting from this coupling can be asymmetric. For example, inter-hemispherical asymmetric responses can arise when a hemisphere receives more energy than the other (e.g., Knipp et al., 2021; Pakhotin et al., 2021), local time effects can take place due to the occurrence of intense dawn-dusk interplanetary electric fields (e.g.,Haaland et al., 2017), and asymmetric geomagnetic field and mapping are caused by the Earth’s dipole offset and tilt (e.g., Laundal et al., 2017). The drivers that generate asymmetric MIT coupling response are generally recognized as long term: solar activity (Zhang et al., 2022) and dipole offset and tilt (Laundal et al., 2017); middle term: seasons (Lu et al., 2010); and short term: the y and z components of the interplanetary magnetic field (IMF) (Cowley, 1981; Li et al., 2011; Knipp et al., 2021). Thermospheric neutral mass density can present local time asymmetries associated with IMF By (Forster et al., 2017), and inter-hemispheric asymmetries can be generated by cross-hemispheric propagation of large-scale gravity waves (Bruinsma and Forbes, 2007). In addition, forcing from the mesosphere and lower thermosphere can generate inter-hemispheric neutral wind asymmetric patterns that can in turn asymmetrically impact neutral density in different hemispheres (Stober et al., 2021).

magnetosphere-ionophere coupling↗

Towards grounding nuclear physics in QCD

Exascale computing could soon enable a predictive theory of nuclear structure and reactions rooted in the Standard Model, with quantifiable and systematically improvable uncertainties. Such a predictive theory will help exploit experiments that use nucleons and nuclei as laboratories for testing the Standard Model and its limitations. Examples include direct dark matter detection, neutrinoless double beta decay, and searches for permanent electric dipole moments of the neutron and atoms. It will also help connect QCD to the properties of cold neutron stars and hot supernova cores. We discuss how a quantitative bridge between QCD and the properties of nuclei and nuclear matter will require a synthesis of lattice QCD (especially as applied to two- and three- nucleon interactions), effective field theory, and ab initio methods for solving the nuclear many-body problem. While there are significant challenges that must be addressed in developing this triad of theoretical tools, the rapid advance of computing is accelerating progress. In particular, we focus this review on the anticipated advances from lattice QCD and how these advances will impact few-body effective theories of nuclear physics by providing critical input, such as constraints on unknown low-energy constants of the effective (field) theories. We also review particular challenges that must be overcome for the successful application of lattice QCD for low-energy nuclear physics. We describe progress in developing few-body effective (field) theories of nuclear physics, with an emphasis on HOBET, a non-relativistic effective theory of nuclear physics, which is less common in the literature. We use the examples of neutrinoless double beta decay and the nuclear-matter equation of state to illustrate how the coupling of lattice QCD to effective theory might impact our understanding of symmetries and exotic astrophysical environments.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Fast Responses on Pre-Industrial Climate from Present-Day Aerosols in A CMIP6 Multi-Model Study

In this work, we use Coupled Model Intercomparison Project Phase 6 (CMIP6) simulations from 10 Earth system models (ESMs) and general circulation models (GCMs) to study the fast climate responses on pre-industrial climate, due to present-day aerosols. All models carried out two sets of simulations: a control experiment with all forcings set to the year 1850 and a perturbation experiment with all forcings identical to the control, except for aerosols with precursor emissions set to the year 2014. In response to the pattern of all aerosols effective radiative forcing (ERF), the fast temperature responses are characterized by cooling over the continental areas, especially in the Northern Hemisphere, with the largest cooling over East Asia and India, sulfate being the dominant aerosol surface temperature driver for present-day emissions. In the Arctic there is a warming signal for winter in the ensemble mean of fast temperature responses, but the model-to-model variability is large, and it is presumably linked to aerosol-induced circulation changes. The largest fast precipitation responses are seen in the tropical belt regions, generally characterized by a reduction over continental regions and presumably a southward shift of the tropical rain belt. This is a characteristic and robust feature among most models in this study, associated with weakening of the monsoon systems around the globe (Asia, Africa and America) in response to hemispherically asymmetric cooling from a Northern Hemisphere aerosol perturbation, forcing possibly the Intertropical Convergence Zone (ITCZ) and tropical precipitation to shift away from the cooled hemisphere despite that aerosols' effects on temperature and precipitation are only partly realized in these simulations as the sea surface temperatures are kept fixed. An interesting feature in aerosol-induced circulation changes is a characteristic dipole pattern with intensification of the Icelandic Low and an anticyclonic anomaly over southeastern Europe, inducing warm air advection towards the northern polar latitudes in winter.

Pre-industrial climate↗

Near-Threshold Dipole Strength in 10 Be with Isoscalar Character

Isoscalar dipole transitions are a distinctive fingerprint of cluster structures. A 1 − resonance at 7.27(10) MeV, located just below the 𝛼-emission threshold, has been observed in the deuteron inelastic scattering reactions off 10 Be. The deformation lengths of the excited states in 10 Be below 9 MeV have been inferred from the differential cross sections using coupled channel calculations. This observed 1 − resonance has isoscalar characteristics and exhausts approximately 5%–15% of the isoscalar dipole energy-weighted sum rule, providing evidence for pronounced 𝛼 cluster structure in 10 Be. The Gamow coupled channel approach supports this interpretation and suggests the near-threshold effect might be playing an important role in this excitation energy domain. Here, the 𝛼 +𝛼 +𝑛 +𝑛 four-body calculation reproduces the observed enhanced dipole strength, implying that the four-body cluster structure is essential to describe the 1 − states in 10 Be.

Cluster models↗

Research on Spectroscopy, Opacity, and Atmospheres

I propose to continue providing observers with basic data for interpreting spectra from stars, novas, supernovas, clusters, and galaxies. These data will include allowed and forbidden line lists, both laboratory and computed, for the first five to ten ions of all atoms and for all relevant diatomic molecules. I will eventually expand to all ions of the first thirty elements to treat far UV and X-ray spectra, and for envelope opacities. I also include triatomic molecules provided by other researchers. I have also made CDs with Partridge and Schwenke's water data for work on UV stars. The line data also serve as input to my model atmosphere and synthesis programs that generate energy distributions, photometry, limb darkening, and spectra that can be used for planning observations and for fitting observed spectra. The spectrum synthesis programs produce detailed plots with the lines identified. Grids of stellar spectra can be used for radial velocity-, rotation-, or abundance templates and for population synthesis. I am fitting spectra of bright stars to test the data and to produce atlases to guide observers. For each star the whole spectrum is computed from the UV to the far IR. The line data, opacities, models, spectra, and programs are freely distributed on CDs and on my Web site and represent a unique resource for many NASA programs. I am now in full production of new line lists for atoms. I am computing all ions of all elements from H to Zn and the first 5 ions of all the heavier elements, about 800 ions. For each ion I treat as many as 61 even and 61 odd configurations, computing all energy levels and eigenvectors. The Hamiltonian is determined from a scaled-Hartree-Fock starting guess by least squares fitting the observed energy levels. The average energy of each configuration is used in computing scaled-Thomas-Fermi-Dirac wavefunctions for each configuration which in turn are used to compute allowed and forbidden transition integrals. These are multiplied into the LS allowed and forbidden transition arrays. The transition arrays are transformed to the observed coupling to yield the allowed and forbidden line lists. Results are put on the web as they are finished. Provided I get funding,there will be more than 500 million lines. I will then compare ion by ion, to all the laboratory and computed data in the literature and make up a working line list for spectrum synthesis and opacity calculations with the best available data. As the laboratory spectrum analyses are improved, I will redo the calculations with the new energy levels. My original plan when I started the new calculations was to run through all the atoms using my old Cray programs from the 1980's that were limited to 1100 x 1100 arrays in the Hamiltonian for each J. Then I would go back and rerun the more complicated cases with 3000 x 3000 arrays so that I could include many more configurations and more configuration interactions. At present I am limited to 61 even and 61 odd configurations and I try to include everything up through n = 9. The current program runs on Alpha workstations. I decided to test the big program on Fe I and Fe II to see whether there was any great difference in the low configurations compared to those from the Cray program. Besides increasing the number of E1 lines by a factor of 6 to 7.7 million, there was an unexpected result: the electric quadrupole transitions were 10 times stronger than before because the transition integrals are weighted by r(exp 2) ---they become very large for high n, and because there are numerous configuration interactions that mix the low and high configurations. As a check I was able to reproduce Carstang's (1962) lower results by running his three configurations with my program. Since my model atom is still only a subset of a real Fe II ion, the true quadrupole A values are probably larger than mine. The magnetic dipole lines are affected by the mixing but the overall scale does not change. Because of this scovery I decided that there was no point in computing the small array cases. I have been running with as many configurations as I can and with thousands of parameters in the Hamiltonian. The computer runs take much longer to set up and produce than I had expected. I have concentrated on redoing the low iron group spectra, especially to get data for supernova modelers. I have done only Ca I -- Zn I, Ca II -- Zn II, CU I -- Cu XXIX, Zn I - Zn XXX, for practice at high stages of ionization, C I, C II, S I, and CL I and Ag I for people who were working on the laboratory spectra. Check my web site kurucz.harvard.edu for current additions. My latest calculations have been for carbon I and sulphur I, and silicon I is under way using the same elaborate approach as for C I, which took many months to do. These line lists greatly increase the number of lines in the ultraviolet, in the visible, and especially in the infrared. They will increase the opacity in A, F, and G stars. They will account for many unidentified lines in the sun.

Kurucz, Robert L.↗

Revealing the Predominant Surface Facets of Rough Cu Electrodes under Electrochemical Conditions

Metal electrodes with rough surfaces are frequently found to convert CO or CO 2 to hydrocarbons and oxygenates with high selectivity and at high reaction rates in comparison with their smooth counterparts. The atomic-level morphology of a rough electrode is likely one key factor responsible for its comparatively high catalytic selectivity and activity. However, few methods are capable of probing the atomic-level structure of rough metal electrodes under electrocatalytic conditions. As a result, the nuances in the atomic-level surface morphology that control the catalytic characteristics of these electrodes have remained largely unexplored. Because the C≡O stretching frequency of atop-bound CO (CO atop ) depends on the coordination of the underlying metal atom, the IR spectrum of this reaction intermediate on the copper electrode could, in principle, provide structural information about the catalytic surface during electrolysis. However, other effects, such as dynamic dipole coupling, easily obscure the dependence of the frequency on the surface morphology. Further, in the limit of low CO atop coverage, where coupling effects are small, the C≡O stretching frequencies of CO atop on Cu(111) and Cu(100) facets are virtually identical. Therefore, on the basis of the C≡O stretching frequency, it is not straightforward to distinguish between these two ubiquitous surface facets, which exhibit vastly different CO reduction activities. Herein, we show that key features of the atomic-level surface morphology of rough copper electrodes can be inferred from the potential dependence of the line shape of the C≡O stretching band of CO atop . Specifically, we compared two types of rough copper thin-film electrodes that are routinely employed in the context of surface-enhanced infrared absorption spectroscopy (SEIRAS). We found that copper films that are electrochemically deposited on Si-supported Au films (CuAu–Si) are poor catalysts for the reduction of CO to ethylene in comparison to copper films (Cu–Si) that are electrolessly deposited onto Si crystals. As quantified by differential electrochemical mass spectrometry (DEMS), the onset potential for ethylene is ~200 ± 65 mV more cathodic for CuAu–Si than that for Cu–Si. To reveal the origin of the disparate catalytic properties of Cu–Si and CuAu–Si, we probed the surfaces of the electrodes with cyclic voltammetry (CV) and SEIRAS. The CV characterization suggests that the (111) surface facet predominates on CuAu–Si, whereas the (100) facet is more common on Cu–Si. SEIRAS reveals that the line shape of the C≡O stretching of CO atop is composed of two bands that are attributable to CO atop on terrace and defect sites. The different surface structures manifest themselves in the form of starkly different potential dependences of the line shape of the C≡O stretching mode of CO atop on the two types of electrodes. With a simple Boltzmann model that considers the different adsorption energies of CO atop on terrace and defect sites, and the resulting CO atop populations on terrace and defect sites, we deduced that the observed electrode-specific potential dependence of the line shape is consistent with the presence of different predominant terrace sites on the two types of films. This strategy for assessing the atomic-level morphology is not restricted to SEIRAS but could also be applied to the C≡O stretching bands recorded with surface-enhanced Raman spectroscopy (SERS), which is suitable for probing a wide range of rough copper electrodes. Therefore, with this work, we establish the potential dependence of the C≡O stretching band of CO atop as a probe of the atomic-level surface structure of rough metal electrodes under electrochemical conditions. When it is coupled with complementary techniques, this methodology provides essential structural information for further improvement in the reaction selectivity of rough metal electrodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Relaxation Matrix for Symmetric Tops with Inversion Symmetry. I. Effects of Line Coupling on Self-Broadened v (sub 1) and Pure Rotational Bands of NH3

The Robert-Bonamy formalism has been commonly used to calculate half-widths and shifts of spectral lines for decades. This formalism is based on several approximations. Among them, two have not been fully addressed: the isolated line approximation and the neglect of coupling between the translational and internal motions. Recently, we have shown that the isolated line approximation is not necessary in developing semi-classical line shape theories. Based on this progress, we have been able to develop a new formalism that enables not only to reduce uncertainties on calculated half-widths and shifts, but also to model line mixing effects on spectra starting from the knowledge of the intermolecular potential. In our previous studies, the new formalism had been applied to linear and asymmetric-top molecules. In the present study, the method has been extended to symmetric-top molecules with inversion symmetry. As expected, the inversion splitting induces a complete failure of the isolated line approximation. We have calculated the complex relaxation matrices of selfbroadened NH3. The half-widths and shifts in the ν1 and the pure rotational bands are reported in the present paper. When compared with measurements, the calculated half-widths match the experimental data very well, since the inapplicable isolated line approximation has been removed. With respect to the shifts, only qualitative results are obtained and discussed. Calculated off-diagonal elements of the relaxation matrix and a comparison with the observed line mixing effects are reported in the companion paper (Paper II).

Trajectory models↗

Multiyear Dry Periods in Southern Africa

Characteristics and physical features related to low precipitation across many years in Southern Africa that lead to societal disruptions are diagnosed using observed analyses and an ensemble of historical coupled climate model simulations during 1921 to 2014. Four regions are evaluated, as identified through a hierarchical clustering algorithm applied to the Standardized Precipitation Index (SPI) during the October–April precipitation season. Although dryness spanning many October–April occurs periodically in each region, they seldom occur simultaneously, consistent with largely insignificant SPI cross-correlations between them. However, characteristics relevant to low precipitation across many years are generalizable between the four regions, including the serial persistence of October–April precipitation, the likelihood of consecutive dry October–April, and the likelihood of dry October–April in temporal extents of up to 10 consecutive such 7-month seasons. Systematic precipitation persistence is not a feature in any of the four Southern Africa regions, as serial correlations of October–April SPI are not statistically significant at any time lags. It follows that there is an exponential-folding decay in the likelihood of consecutive October–April for various SPI thresholds and that there is a large spread in the likelihood of low October–April SPI across many years. In terms of physical features, low October–April SPI in each Southern Africa region is closely related to local atmospheric circulations; however, they are not as closely related to sea surface temperatures (SSTs). These results suggest that dryness spanning many years is determined primarily by persistent local circulations related to atmospheric variability and to a lesser extent variability related to SST anomalies, including the El Niño–Southern Oscillation.

subtropical Indian Ocean dipole↗

On the 2018 Outburst of the Accreting Millisecond X-Ray Pulsar Swift J1756.9-2508 As Seen with NICER

We report on the coherent timing analysis of the 182 Hz accreting millisecond X-ray pulsar SwiftJ1756.92508during its 2018 outburst as observed with the Neutron Star Interior Composition Explorer (NICER). Combiningour NICER observations with Rossi X-ray Timing Explorer observations of the 2007 and 2009 outbursts, we alsostudied the long-term spin and orbital evolution of this source. We find that the binary system is well describedby a constant orbital period model, with an upper limit on the orbital period derivative of Pb < 7.4 ´ 10-13 ss1.Additionally, we improve upon the source coordinates through astrometric analysis of the pulse arrival times,finding R.A.=17h56m57 18±0 08 and decl.=25°0627 8±3 5, while simultaneously measuring thelong-term spin frequency derivative as n = -7.3 ´ 10-16 Hzs1. We briefly discuss the implications of thesemeasurements in the context of the wider population of accreting millisecond pulsars. We reported on the coherent timing analysis of the 2018 outburst of Swift J1756 as observed with NICER. Consistent with analyses of the previous outbursts (Krimm et al. 2007b; Patruno et al. 2010), we find that the X-ray pulsations have energy dependent amplitudes; the fractional amplitude of the fundamental increases with energy, whereas the fractional amplitude of the harmonic shows a slight decline with energy. This energy dependent behavior is not unusual in AMXPs (Patruno & Watts 2012) and can be interpreted in terms of the thermal emission from the stellar hotspot and reprocessing in the accretion column (e.g., Gierliński et al. 2002; Ibragimov & Poutanen 2009). The pulse arrival times of the 2018 outburst are well described by a timing model consisting of a circular orbit with a constant spin frequency. The pulse phases with respect to this model do not show spurious residuals with time or orbital phase, and no evidence is found that the pulse arrival times exhibit an additional delay associated with passing through the gravitational well of the companion star (Shapiro delay). We note, however, that the expected Shapiro delay is given as (Shapiro et al. 1971) Equation (5) where Φ is the orbital phase, G is the gravitational constant, c is the speed of light, and i is the inclination. Even for the maximum allowed companion mass, ${M}_{C}=0.030\,{M}_{\odot }$ (Krimm et al. 2007b, but see Section 4.2 for more details) and an inclination of 90°, the largest delay we can expect is only 4 μs. As this time-delay is smaller than the uncertainty on our phase residuals by nearly two orders of magnitude (see Figure 1), we are not sensitive to Shapiro delays in Swift J1756. Comparing our measurements for the 2018 outburst with those of the 2007 and 2009 outbursts as observed with RXTE, we analyzed the long-term evolution of this source. We found that the binary system is consistent with having a constant orbital period and that the pulsar shows a spin frequency derivative of $\dot{\nu }=-7.3\times {10}^{-16}\,\mathrm{Hz}\,{{\rm{s}}}^{-1}$. 4.1. Spin-down Evolution The long-term spin frequency derivative measured in Swift J1756 is of the same order as the spin frequency derivatives measured in other AMXPs (Hartman et al. 2008; Patruno 2010; Riggio et al. 2011). This frequency change is most likely driven by the neutron star's loss of rotational energy. If so, then the spin-down luminosity is given as Equation (6) where I represents the neutron star moment of inertia. The long-term spin-down of a neutron star is usually assumed to be dominated by the braking torque associated with a spinning magnetic field. Assuming this mechanism is responsible for the observed spin-down in Swift J1756, we can compute the magnetic dipole moment as (Spitkovsky 2006) Equation (7) where α is the misalignment angle between the rotational and magnetic poles. Considering α = 0°–90°, we then find a magnetic field strength of $B\simeq (4\mbox{--}6)\times {10}^{8}$ G at the stellar magnetic poles. This magnetic field strength estimate is in line with those obtained for other accreting millisecond pulsars (see Mukherjee et al. 2015 and references therein). 4.2. Orbit Evolution The observed long-term binary evolution of Swift J1756 is consistent with this source having a constant orbital period and a lower limit on the evolutionary timescale of Equation (8) Binary evolution theory predicts that systems of this type evolve due to angular momentum loss through gravitational radiation (Kraft et al. 1962; Rappaport et al. 1982; Verbunt 1993). For conservative mass transfer, the binary period derivative is given by di Salvo et al. (2008), Equation (9) where MNS is the neutron star mass, $q={M}_{C}/{M}_{\mathrm{NS}}$ is the binary mass ratio, and −1/3 < n < 1 is the mass–radius index of the companion star. Depending on the source inclination, Krimm et al. (2007b) derived a companion mass of ${M}_{C}\,=0.007\mbox{--}0.022\,{M}_{\odot }$ for a neutron star mass of 1.4 ${M}_{\odot }$. For a neutron star mass of 2.2 ${M}_{\odot }$, the allowed range increased to ${M}_{C}=0.009\mbox{--}0.030\,{M}_{\odot }$. In both cases, they assumed an upper limit on the inclination of i < 85°, motivated by the fact that Swift J1756 does not show eclipses in its light curve. Accounting for the extreme cases of stellar masses and n, the binary may either be contracting or expanding. In either case, however, the rate of change is limited to $| {\dot{P}}_{b}| \lesssim 7\times {10}^{-14}$ s s−1, which is well below the upper limit obtained in this work. Although the binary evolution timescale we obtain for Swift J1756 is consistent with theory, it is worth noting that this is not generally true for low-mass X-ray binaries (see Patruno et al. 2017, for a comprehensive discussion). The AMXP SAX J1808.4–3658, in particular, has been found to evolve on a much shorter timescale, with a first derivative on the orbital period of $3.5\times {10}^{-12}$ s s−1 (Hartman et al. 2008; Patruno et al. 2012; Sanna et al. 2017a). Two models have been proposed to explain this discrepancy: highly nonconservative mass transfer due to irradiation of the companion star by the pulsar (di Salvo et al. 2008; Burderi et al. 2009), and spin–orbit coupling in the companion star (Hartman et al. 2008, 2009). While the latter depends on the companion star, and may vary from source to source, the former should operate in all AMXPs (see also Patruno 2017; Sanna et al. 2017c), including Swift J1756. The spin-down luminosity impinging on the companion star can be estimated as Equation (10) where ${\dot{E}}_{\mathrm{abl}}$ is the ablation luminosity, RL2 is the Roche lobe radius of the companion (Eggleton 1983), and a the binary separation. The irradiation fraction is $f={\dot{E}}_{\mathrm{abl}}/{\dot{E}}_{\mathrm{sd}}$, which, accounting for the range of allowed neutron star and companion masses, evaluates to f = 0.15%–0.35%. The associated mass loss for the companion is given by Equation (11) such that, assuming an efficiency of η = 100%, ${\dot{M}}_{C}\,\sim -3\times {10}^{-10}\,{M}_{\odot }$ yr−1. The effect of this mass loss on the orbital period follows through the relation (Frank et al. 2002) Equation (12) giving a period derivative due to mass loss of ${\dot{P}}_{b,\mathrm{ML}}\,=5\times {10}^{-12}$ s s−1. This value is well above our limit on the period derivative. Hence, in order for this mechanism to be consistent with our observations of Swift J1756, the efficiency at which the companion star converts the incident luminosity into mass loss must be η < 15%. This value is very different from the 40% required in SAX J1808.4–3658 (Patruno et al. 2016) and is instead in line with the <5% efficiency determined for IGR J00291+5934 (Patruno 2017). This work was supported by NASA through the NICER mission and the Astrophysics Explorers Program, and made use of data and software provided by the High Energy Astrophysics Science Archive Research Center (HEASARC). P.B. was supported by an NPP fellowship at NASA Goddard Space Flight Center. D.A. acknowledges support from the Royal Society.

Bult, Peter↗

Aeolian Sand Transport in the Planetary Context: Respective Roles of Aerodynamic and Bed-Dilatancy Thresholds

The traditional view of aeolian sand transport generally estimates flux from the perspective of aerodynamic forces creating the airborne grain population, although it has been recognized that "reptation" causes a significant part of the total airborne flux; reptation involves both ballistic injection of grains into the air stream by the impact of saltating grains as well as the "nudging" of surface grains into a creeping motion. Whilst aerodynamic forces may initiate sand motion, it is proposed here that within a fully-matured grain cloud, flux is actually governed by two thresholds: an aerodynamic threshold, and a bed-dilatancy threshold. It is the latter which controls the reptation population, and its significance increases proportionally with transport energy. Because we only have experience with terrestrial sand transport, extrapolations of aeolian theory to Mars and Venus have adjusted only the aerodynamic factor, taking gravitational forces and atmospheric density as the prime variables in the aerodynamic equations, but neglecting reptation. The basis for our perspective on the importance of reptation and bed dilatancy is a set of experiments that were designed to simulate sand transport across the surface of a martian dune. Using a modified sporting crossbow in which a sand-impelling sabot replaced the bolt-firing mechanism, individual grains of sand were fired at loose sand targets with glancing angles typical of saltation impact; grains were projected at about 80 m/s to simulate velocities commensurate with those predicted for extreme martian aeolian conditions. The sabot impelling method permitted study of individual impacts without the masking effect of bed mobilization encountered in wind-tunnel studies. At these martian impact velocities, grains produced small craters formed by the ejection of several hundred grains from the bed. Unexpectedly, the craters were not elongated, despite glancing impact; the craters were very close to circular in planform. High-speed photography showed them to grow in both diameter and depth after the impactor had ricochetted from the crater site. The delayed response of the bed was "explosive" in nature, and created a miniature ejecta curtain spreading upward and outward for many centimeters for impact of 100-300 micron-diameter grains into similar material. Elastic energy deposited in the bed by the impacting grain creates a subsurface stress regime or "quasi-Boussinesq" compression field. Elastic recovery of the bed occurs by dilatancy; shear stresses suddenly convert the grains from closed to open packing, and grains are consequently able to eject themselves forcefully from the impact site. Random jostling of the grains causes radial homogenization of stress vectors and a resulting circular crater. There is a great temptation to draw parallels with cratering produced by meteorite impacts, but a rigorous search for common modelling ground between the two phenomena has not been conducted at this time. For every impact of an aerodynamically energized grain, there are several hundred grains ejected into the wind for the high-energy transport that might occur on Mars. Many of these grains will themselves become subject to the boundary layer's aerodynamic lift forces (their motion will not immediately die and add to the creep population), and these grains will become indistinguishable from those lifted entirely by aerodynamic forces. As each grain impacts the bed, it will eject even more grains into the flow. A cascading effect will take place, but because it must be finite in its growth, damping will occur as the number of grains set in motion causes mid-air collisions that prevent much of the impact energy from reaching the surface of the bed -thus creating a dynamic equilibrium in a high-density saltation cloud. It is apparent that for a given impact energy, the stress field permits a smaller volume of grains to convert to open packing as the size of the bed grains increases, or as the energy of the "percussive" grain decreases (by decrease in velocity or mass). Thus, the mass of the "repercussive" grain population that is ejected from the impact site becomes a function of the scale of the stress field in relation to the scale of the bed material (self-similarity being applicable if both bed size and energy are simultaneously adjusted). In other words, in a very high energy aeolian system where an aerodynamically raised grain can ballistically raise many more grains, the amount of material lifted into the wind becomes largely a function of a dilatancy threshold. If this threshold is exceeded, grains are repercussively injected into the saltation cloud. The "dilatancy threshold" may be defined in terms of the saltation percussive force required to convert the bed, through elastic response, from a closed to an open packing system. If open packing cannot be created, the grains cannot escape from the impact site, even though the elastic deformation and percussive force may be able to reorganize the grains with respect to one another. As the crossbow experiments showed, for an ever-increasing bed grain size, a point is reached when no material can be moved because the energy of the percussive grain is insufficient to dilate the relatively coarse bed. Although this seems to be stating the obvious -- that too little energy will not cause the bed to splash -- the consequences of exceeding the "splash threshold" by dilatancy are not so obvious for high-energy aeolian transport. It is noted that the force required to elastically dilate the bed has to overcome Coulombic grain attractions such as dipole-dipole coupling, dielectric, monopole, contact-induced dipole attractions, van der Waals forces, molecular monolayer capillary forces, as well as the mechanical interlocking frictional resistance of the grains. On Mars, it is predicted that the dilatancy threshold may be the prime control of grain flux. Additional information is contained in the original.

Marshall, J. R.↗