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We compare observations of Hifrom the Very Large Array (VLA) and the Arecibo Observatory and observations of HCO⁺from the Atacama Large Millimeter/submillimeter Array (ALMA) and the Northern Extended Millimeter Array (NOEMA) in the diffuse (A_V≲ 1) interstellar medium (ISM) to predictions from a photodissociation region (PDR) chemical model and multiphase ISM simulations. Using a coarse grid of PDR models, we estimate the density, FUV radiation field, and cosmic-ray ionization rate (CRIR) for each structure identified in HCO⁺and Hiabsorption. These structures fall into two categories. Structures withT_s< 40 K, mostly withN(HCO⁺) ≲ 10¹²cm⁻², are consistent with modest density, FUV radiation field, and CRIR models, typical of the diffuse molecular ISM. Structures with spin temperatureT_s> 40 K, mostly withN(HCO⁺) ≳ 10¹²cm⁻², are consistent with high density, FUV radiation field, and CRIR models, characteristic of environments close to massive star formation. The latter are also found in directions with a significant fraction of thermally unstable Hi. In at least one case, we rule out the PDR model parameters, suggesting that alternative mechanisms (e.g., nonequilibrium processes like turbulent dissipation and/or shocks) are required to explain the observed HCO⁺in this direction. Similarly, while our observations and simulations of the turbulent, multiphase ISM agree that HCO⁺formation occurs along sight lines withN(H I) ≳ 10²¹cm⁻², the simulated data fail to explain HCO⁺column densities ≳ few × 10¹²cm⁻². Because a majority of our sight lines with HCO⁺had such high column densities, this likely indicates that nonequilibrium chemistry is important for these lines of sight.

 

We have complemented existing observations of Hiabsorption with new observations of HCO⁺, C₂H, HCN, and HNC absorption from the Atacama Large Millimeter/submillimeter Array and the Northern Extended Millimeter Array in the directions of 20 background radio continuum sources with 4° ≤ ∣b∣ ≤ 81° to constrain the atomic gas conditions that are suitable for the formation of diffuse molecular gas. We find that these molecular species form along sightlines whereA_V≳ 0.25, consistent with the threshold for the Hi-to-H₂transition at solar metallicity. Moreover, we find that molecular gas is associated only with structures that have an Hioptical depth >0.1, a spin temperature <80 K, and a turbulent Mach number ≳ 2. We also identify a broad, faint component to the HCO⁺absorption in a majority of sightlines. Compared to the velocities where strong, narrow HCO⁺absorption is observed, the Hiat these velocities has a lower cold neutral medium fraction and negligible CO emission. The relative column densities and linewidths of the different molecular species observed here are similar to those observed in previous experiments over a range of Galactic latitudes, suggesting that gas in the solar neighborhood and gas in the Galactic plane are chemically similar. For a select sample of previously observed sightlines, we show that the absorption line profiles of HCO⁺, HCN, HNC, and C₂H are stable over periods of ∼3 yr and ∼25 yr, likely indicating that molecular gas structures in these directions are at least ≳100 au in size.

 

Abstract Ambient fine particulate matter (PM 2.5 ) is the world’s leading environmental health risk factor. Reducing the PM 2.5 disease burden requires specific strategies that target dominant sources across multiple spatial scales. We provide a contemporary and comprehensive evaluation of sector- and fuel-specific contributions to this disease burden across 21 regions, 204 countries, and 200 sub-national areas by integrating 24 global atmospheric chemistry-transport model sensitivity simulations, high-resolution satellite-derived PM 2.5 exposure estimates, and disease-specific concentration response relationships. Globally, 1.05 (95% Confidence Interval: 0.74–1.36) million deaths were avoidable in 2017 by eliminating fossil-fuel combustion (27.3% of the total PM 2.5 burden), with coal contributing to over half. Other dominant global sources included residential (0.74 [0.52–0.95] million deaths; 19.2%), industrial (0.45 [0.32–0.58] million deaths; 11.7%), and energy (0.39 [0.28–0.51] million deaths; 10.2%) sectors. Our results show that regions with large anthropogenic contributions generally had the highest attributable deaths, suggesting substantial health benefits from replacing traditional energy sources. 

We investigate and assess how well a global chemical transport model (GEOS‐Chem) simulates submicron aerosol mass concentrations in the remote troposphere. The simulated speciated aerosol (organic aerosol (OA), black carbon, sulfate, nitrate, and ammonium) mass concentrations are evaluated against airborne observations made during all four seasons of the NASA Atmospheric Tomography Mission (ATom) deployments over the remote Pacific and Atlantic Oceans. Such measurements over pristine environments offer fresh insights into the spatial (Northern [NH] and Southern Hemispheres [SH], Atlantic, and Pacific Oceans) and temporal (all seasons) variability in aerosol composition and lifetime, away from continental sources. The model captures the dominance of fine OA and sulfate aerosol mass concentrations in all seasons. There is a high bias across all species in the ATom‐2 (NH winter) simulations; implementing recent updates to the wet scavenging parameterization improves our simulations, eliminating the large ATom‐2 (NH winter) bias, improving the ATom‐1 (NH summer) and ATom‐3 (NH fall) simulations, but producing a model underestimate in aerosol mass concentrations for the ATom‐4 (NH spring) simulations. Following the wet scavenging updates, simulated global annual mean aerosol lifetimes vary from 1.9 to 4.0 days, depending on species. Aerosol lifetimes in each hemisphere vary by season, and are longest for carbonaceous aerosol during the southern hemispheric fire season. The updated wet scavenging parameterization brings simulated concentrations closer to observations and reduces global aerosol lifetime for all species, indicating the sensitivity of global aerosol lifetime and burden to wet removal processes.

 

Investigating the physical and chemical structure of massive star-forming regions is critical for understanding the formation and early evolution of massive stars. We performed a detailed line survey toward six dense cores, named MM1, MM4, MM6, MM7, MM8, and MM11, in the G9.62+0.19 star-forming region resolved in Atacama Large Millimeter/submillimeter Array (ALMA) band 3 observations. Toward these cores, about 172 transitions have been identified and attributed to 16 species, including organic oxygen-, nitrogen-, and sulphur-bearing molecules and their isotopologues. Four dense cores, MM7, MM8, MM4, and MM11, are line-rich sources. Modelling of these spectral lines reveals that the rotational temperature lies in the range 72–115, 100–163, 102–204, and 84–123 K for MM7, MM8, MM4, and MM11, respectively. The molecular column densities are 1.6 × 1015–9.2 × 1017 cm−2 toward the four cores. The cores MM8 and MM4 show a chemical difference between oxygen- and nitrogen-bearing species, i.e. MM4 is rich in oxygen-bearing molecules, while nitrogen-bearing molecules, especially vibrationally excited HC3N lines, are mainly observed in MM8. The distinct initial temperatures at the accretion phase may lead to this N/O differentiation. Through analysing column densities and spatial distributions of O-bearing complex organic molecules (COMs), we found that C2H5OH and CH3OCH3 might have a common precursor, CH3OH. CH3OCHO and CH3OCH3 are likely chemically linked. In addition, the observed variation in HC3N and HC5N emission may indicate their different formation mechanisms in hot and cold regions.

 

Atmospheric ammonia plays an important role in a number of environmental issues, including new particle formation and aerosol indirect radiative forcing. Over the United States, atmospheric ammonia has seen an increasing trend due in most part to the declining SO₂and NO_xemissions. We conduct the first comprehensive assessment of multiyear Goddard Earth Observing System (GEOS)‐Chem simulated ammonia concentration ([NH₃]) over conterminous United States along with surface observations from all 90 National Atmospheric Deposition Program Ammonia Monitoring Network (AMoN) sites that have at least 2 years of continuous measurements. Model‐simulated [NH₃] is along empirically expected lines with regard to temporal trends, seasonal variations, and spatial distribution. GEOS‐Chem‐simulated [NH₃], compared to AMoN observed values, has weighted average correlation (τ) of 0.50 ± 0.15 and mean fractional bias (MFB) of −8.8 ± 56%. Most sites (63 out of 90) have −60% <MFB< +60%. The deviations from observed values vary spatially and seasonally, and there is significant wintertime underestimation (−44 ± 58%) across most of conterminous United States (except the Pacific states). The largest positive deviations occur in the Pacific states (101 ± 46%) and the largest negative deviations in the Southern Plain states (−73 ± 39%) and the Mountain states (−73 ± 84%), both in the winter months. Over the Great Plains region, GEOS‐Chem simulated [NH₃] shows a much stronger dependence to emissions than AMoN observed [NH₃], indicating scope for improved representation of emissions for the region. Over Southeast United States, there appears to be the strong effect of the changing emissions of SO₂and NO_xin both modeled and observed [NH₃].

 

Ice crystal habit significantly impacts ice crystal processes such as growth by vapor deposition. Despite this, most bulk microphysical models disregard this natural shape effect and assume ice to grow spherically. This paper focuses on how the evolution of ice crystal shape and choice of ice nucleation parameterization in the adaptive habit microphysics model (AHM) influence the lake-effect storm that occurred during intensive observing period 4 (IOP4) of the Ontario Winter Lake-effect Systems (OWLeS) field campaign. This localized snowstorm produced total accumulated liquid-equivalent precipitation amounts up to 17.92 mm during a 16-h time period, providing a natural laboratory to investigate the ice–liquid partitioning within the cloud, various microphysical process rates, the accumulated precipitation magnitude, and its associated spatial distribution. Two nucleation parameterizations were implemented, and aerosol data from a size-resolved advanced particle microphysics (APM) model were ingested into the AHM for use in parameterizing ice and cloud condensation nuclei. Simulations allowing ice crystals to grow nonspherically produced 1.6%–2.3% greater precipitation while altering the nucleation parameterization changed the type of accumulating hydrometeors. In addition, all simulations were highly sensitive to the domain resolution and the source of initial and boundary conditions. These findings form the foundational understanding of relationships among ice crystal habit, nucleation parameterizations, and resultant cold-season mesoscale precipitation within detailed bulk microphysical models allowing adaptive habit.