Atmosphere-Ocean Ozone Exchange – A Global Modeling Study of Biogeochemical, Atmospheric and Water-Side Turbulence Dependencies

The significance of the removal of tropospheric ozone by the oceans, covering ~2/3 of the Earth's surface, has only been addressed in a few studies involving water tank, aircraft, and tower flux measurements. On the basis of results from these few observations of the ozone dry deposition velocity (VdO3), atmospheric chemistry models generally apply an empirical, constant ocean uptake rate of 0.05 cm s-1. This value is substantially smaller than the atmospheric turbulent transport velocity for ozone. On the other hand, the uptake is higher than expected from the solubility of ozone in clean water alone, suggesting that there is an enhancement in oceanic ozone uptake, e.g., through a chemical destruction mechanism. We present an evaluation of a global-scale analysis with a new mechanistic representation of atmosphere-ocean ozone exchange. The applied atmosphere chemistry-climate model includes not only atmospheric but also waterside turbulence and the role of waterside chemical loss processes as a function of oceanic biogeochemistry. The simulations suggest a larger role of biogeochemistry in tropical and subtropical ozone oceanic uptake with a relative small temporal variability, whereas in midlatitude and high-latitude regions, highly variable ozone uptake rates are expected because of the stronger influence of waterside turbulence. Despite a relatively large range in the explicitly calculated ocean uptake rate, there is a surprisingly small sensitivity of simulated Marine Boundary Layer ozone concentrations compared to the sensitivity for the commonly applied constant ocean uptake approach. This small sensitivity points at compensating effects through inclusion of the process-based ocean uptake mechanisms to consider variability in oceanic O3 deposition consistent with that in atmospheric and oceanic physical, chemical, and biological processe

Modeled global effects of airborne desert dust on air quality and premature mortality

Fine particulate matter is one of the most important factors contributing to air pollution. Epidemiological studies have related increased levels of atmospheric particulate matter to premature human mortality caused by cardiopulmonary disease and lung cancer. However, a limited number of investigations have focused on the contribution of airborne desert dust particles. Here we assess the effects of dust particles with an aerodynamic diameter smaller than 2.5 μm (DU_2.5) on human mortality for the year 2005. We used the EMAC atmospheric–chemistry general circulation model at high resolution to simulate global atmospheric dust concentrations. We applied a health impact function to estimate premature mortality for the global population of 30 yr and older, using parameters from epidemiological studies. We estimate a global cardiopulmonary mortality of about 402 000 in 2005. The associated years of life lost are about 3.47 million per year. We estimate the global fraction of the cardiopulmonary deaths caused by atmospheric desert dust to be about 1.8%, though in the 20 countries most affected by dust this is much higher, about 15–50%. These countries are primarily found in the so-called "dust belt" from North Africa across the Middle East and South Asia to East Asi

Prácticas profesionalizantes de secundaria técnica en contexto de pandemia: tensiones entre formatos y sentidos formativos del campo

El presente artículo tiene como objetivo describir y poner en discusión el desarrollo de las Prácticas Profesionalizantes (PP) para el sostenimiento de la continuidad pedagógica durante la pandemia del COVID-19, considerando las propuestas de la especialidad “Informática profesional y personal” de tres escuelas secundarias técnicas de Corrientes. Se parte desde una perspectiva conceptual que considera la construcción del campo de PP desde dos dimensiones: la política-normativa y la pedagógica-didáctica del sentido de la práctica en la formación. Así, desde una mirada multinivel se busca poner en diálogo lo normativo con las voces de los actores involucrados. Se identifican y analizan normas referidas a las PP en pandemia y los proyectos institucionales de PP de cada escuela, como así también, se realizan entrevistas a referentes jurisdiccionales, directivos y docentes de estos espacios. Este recorrido permite describir las experiencias de PP desarrolladas en un contexto de excepcionalidad, a partir de lo cual se ponen en discusión las adaptaciones realizadas, problematizando los alcances y los sentidos desde los cuales se construyen las PP en la formación de técnicos y las complejidades de la articulación escuela y medio socio productivo

Temperature-(208-318 K) and pressure-(18-696Torr) dependent rate coefficients for the reaction between OH and HNO3

Abstract. Rate coefficients (k5) for the title reaction were ob- tained using pulsed laser photolytic generation of OH cou- pled to its detection by laser-induced fluorescence (PLP– LIF). More than 80 determinations of k5 were carried out in nitrogen or air bath gas at various temperatures and pres- sures. The accuracy of the rate coefficients obtained was en- hanced by in situ measurement of the concentrations of both HNO3 reactant and NO2 impurity. The rate coefficients show both temperature and pressure dependence with a rapid in- crease in k5 at low temperatures. The pressure dependence was weak at room temperature but increased significantly at low temperatures. The entire data set was combined with se- lected literature values of k5 and parameterised using a com- bination of pressure-dependent and -independent terms to give an expression that covers the relevant pressure and tem- perature range for the atmosphere. A global model, using the new parameterisation for k 5 rather than those presently ac- cepted, indicated small but significant latitude- and altitude- dependent changes in the HNO 3 / NO x ratio of between − 6 and + 6 %. Effective HNO 3 absorption cross sections (184.95 and 213.86 nm, units of cm 2 molecule − 1 ) were ob- tained as part of this work: σ 213 . 86 = 4.52 + 0 . 23 − 0 . 12 × 10 − 19 and σ 184 . 95 = 1.61 + 0 . 08 − 0 . 04 × 10 − 17

A hierarchical time-splitting approach for solving finite-time optimal control problems

The self-cleaning or oxidation capacity of the atmosphere is principally controlled by hydroxyl (OH) radicals in the troposphere. Hydroxyl has primary (P) and secondary (S) sources, the former mainly through the photodissociation of ozone, the latter through OH recycling in radical reaction chains. We used the recent Mainz Organics Mechanism (MOM) to advance volatile organic carbon (VOC) chemistry in the general circulation model EMAC (ECHAM/MESSy Atmospheric Chemistry) and show that S is larger than previously assumed. By including emissions of a large number of primary VOC, and accounting for their complete breakdown and intermediate products, MOM is mass-conserving and calculates substantially higher OH reactivity from VOC oxidation compared to predecessor models. Whereas previously P and S were found to be of similar magnitude, the present work indicates that S may be twice as large, mostly due to OH recycling in the free troposphere. Further, we find that nighttime OH formation may be significant in the polluted subtropical boundary layer in summer. With a mean OH recycling probability of about 67 %, global OH is buffered and not sensitive to perturbations by natural or anthropogenic emission changes. Complementary primary and secondary OH formation mechanisms in pristine and polluted environments in the continental and marine troposphere, connected through long-range transport of O3, can maintain stable global OH levels

Measurement report: Hydrogen peroxide in the upper tropical troposphere over the Atlantic Ocean and western Africa during the CAFE-Africa aircraft campaign

This study focuses on the distribution of hydrogen peroxide (H2O2) in the upper tropical troposphere at altitudes between 8 and 15 km based on in situ observations during the Chemistry of the Atmosphere: Field Experiment in Africa (CAFE-Africa) campaign conducted in August–September 2018 over the tropical Atlantic Ocean and western Africa. The measured hydrogen peroxide mixing ratios in the upper troposphere show no clear trend in the latitudinal distribution with locally increased levels (up to 1 ppbv​​​​​​​) within the Intertropical Convergence Zone (ITCZ), over the African coastal area, as well as during measurements performed in proximity to the tropical storm Florence (later developing into a hurricane). The observed H2O2 distribution suggests that mixing ratios in the upper troposphere seem to be far less dependent on latitude than assumed previously and the corresponding factors influencing the photochemical production and loss of H2O2. The observed levels of H2O2 in the upper troposphere indicate the influence of convective transport processes on the distribution of the species not only in the tropical but also in the subtropical regions. The measurements are compared to observation-based photostationary steady-state (PSS) calculations and numerical simulations by the global ECHAM/MESSy Atmospheric Chemistry (EMAC) model. North of the ITCZ, PSS calculations produce mostly lower H2O2 mixing ratios relative to the observations. The observed mixing ratios tend to exceed the PSS calculations by up to a factor of 2. With the exception of local events, the comparison between the calculated PSS values and the observations indicates enhanced H2O2 mixing ratios relative to the expectations based on PSS calculations in the north of the ITCZ. On the other hand, PSS calculations tend to overestimate the H2O2 mixing ratios in most of the sampled area in the south of the ITCZ by a factor of up to 3. The significant influence of convection in the ITCZ and the enhanced presence of clouds towards the Southern Hemisphere indicate contributions of atmospheric transport and cloud scavenging in the sampled region. Simulations performed by the EMAC model also overestimate hydrogen peroxide levels particularly in the Southern Hemisphere, most likely due to underestimated cloud scavenging. EMAC simulations and PSS calculations both indicate a latitudinal gradient from the Equator towards the subtropics. In contrast, the measurements show no clear gradient with latitude in the mixing ratios of H2O2 in the upper troposphere with a slight decrease from the ITCZ towards the subtropics, indicating a relatively low dependency on the solar radiation intensity and the corresponding photolytic activity. The largest model deviations relative to the observations correspond with the underestimated hydrogen peroxide loss due to enhanced cloud presence, scavenging, and rainout in the ITCZ and towards the south.</p

Impact of the South Asian monsoon outflow on atmospheric hydroperoxides in the upper troposphere

During the OMO (Oxidation Mechanism Observation) mission, trace gas measurements were performed on board the HALO (High Altitude Long Range) research aircraft in summer 2015 in order to investigate the outflow of the South Asian summer monsoon and its influence on the composition of the Asian monsoon anticyclone (AMA) in the upper troposphere over the eastern Mediterranean and the Arabian Peninsula. This study focuses on in situ observations of hydrogen peroxide (H$_{2}$O$_{2}$$^{obs}$) and organic hydroperoxides (ROOH$^{obs}$) as well as their precursors and loss processes. Observations are compared to photostationary-state (PSS) calculations of H$_{2}$O$_{2}$$^{PSS}$ and extended by a separation of ROOH$^{obs}$ into methyl hydroperoxide (MHP$^{PSS}$) and inferred unidentified hydroperoxide (UHP$^{PSS}$) mixing ratios using PSS calculations. Measurements are also contrasted to simulations with the general circulation ECHAM–MESSy for Atmospheric Chemistry (EMAC) model. We observed enhanced mixing ratios of H$_{2}$O$_{2}$$^{obs}$ (45 %), MHP$^{PSS}$ (9 %), and UHPPSS (136 %) in the AMA relative to the northern hemispheric background. Highest concentrations for H$_{2}$O$_{2}$$^{obs}$ and MHP$^{PSS}$ of 211 and 152 ppb$_{V}$, respectively, were found in the tropics outside the AMA, while for UHP$^{PSS}$, with 208 ppt$_{V}$, highest concentrations were found within the AMA. In general, the observed concentrations are higher than steady-state calculations and EMAC simulations by a factor of 3 and 2, respectively. Especially in the AMA, EMAC underestimates the H$_{2}$O$_{2}$$^{EMAC}$ (medians: 71 ppt$_{V}$ vs. 164 ppt$_{V}$) and ROOHEMAC (medians: 25 ppt$_{V}$ vs. 278 ppt$_{V}$) mixing ratios. Longitudinal gradients indicate a pool of hydroperoxides towards the center of the AMA, most likely associated with upwind convection over India. This indicates main contributions of atmospheric transport to the local budgets of hydroperoxides along the flight track, explaining strong deviations from steady-state calculations which only account for local photochemistry. Underestimation of H$_{2}$O$_{2}$$^{EMAC}$ by approximately a factor of 2 in the Northern Hemisphere (NH) and the AMA and overestimation in the Southern Hemisphere (SH; factor 1.3) are most likely due to uncertainties in the scavenging efficiencies for individual hydroperoxides in deep convective transport to the upper troposphere, corroborated by a sensitivity study. It seems that the observed excess UHPPSS is excess MHP transported to the west from an upper tropospheric source related to convection in the summer monsoon over Southeast Asia

The atmospheric chemistry general circulation model ECHAM5/MESSy1: consistent simulation of ozone from the surface to the mesosphere

International audienceThe new Modular Earth Submodel System (MESSy) describes atmospheric chemistry and meteorological processes in a modular framework, following strict coding standards. It has been coupled to the ECHAM5 general circulation model, which has been slightly modified for this purpose. A 90-layer model version up to 0.01 hPa was used at T42 resolution (~2.8 latitude and longitude) to simulate the lower and middle atmosphere. The model meteorology has been tested to check the influence of the changes to ECHAM5 and the radiation interactions with the new representation of atmospheric composition. A Newtonian relaxation technique was applied in the tropospheric part of the domain to weakly nudge the model towards the analysed meteorology during the period 1998?2005. It is shown that the tropospheric wave forcing of the stratosphere in the model suffices to reproduce the Quasi-Biennial Oscillation and major stratospheric warming events leading e.g. to the vortex split over Antarctica in 2002. Characteristic features such as dehydration and denitrification caused by the sedimentation of polar stratospheric cloud particles and ozone depletion during winter and spring are simulated accurately, although ozone loss in the lower polar stratosphere is slightly underestimated. The model realistically simulates stratosphere-troposphere exchange processes as indicated by comparisons with satellite and in situ measurements. The evaluation of tropospheric chemistry presented here focuses on the distributions of ozone, hydroxyl radicals, carbon monoxide and reactive nitrogen compounds. In spite of minor shortcomings, mostly related to the relatively coarse T42 resolution and the neglect of interannual changes in biomass burning emissions, the main characteristics of the trace gas distributions are generally reproduced well. The MESSy submodels and the ECHAM5/MESSy1 model output are available through the internet on request

Global tropospheric effects of aromatic chemistry with the SAPRC-11 mechanism implemented in GEOS-Chem version 9-02

The Goddard Earth Observing System with chemistry (GEOS-Chem) model has been updated with the State-wide Air Pollution Research Center version 11 (SAPRC-11) aromatics chemical mechanism, with the purpose of evaluating global and regional effects of the most abundant aromatics (benzene, toluene, xylenes) on the chemical species important for tropospheric oxidation capacity. The model evaluation based on surface and aircraft observations indicates good agreement for aromatics and ozone. A comparison between scenarios in GEOS-Chem with simplified aromatic chemistry (as in the standard setup, with no ozone formation from related peroxy radicals or recycling of NOx) and with the SAPRC-11 scheme reveals relatively slight changes in ozone, the hydroxyl radical, and nitrogen oxides on a global mean basis (1&thinsp;%–4&thinsp;%), although remarkable regional differences (5&thinsp;%–20&thinsp;%) exist near the source regions. NOx decreases over the source regions and increases in the remote troposphere, due mainly to more efficient transport of peroxyacetyl nitrate (PAN), which is increased with the SAPRC aromatic chemistry. Model ozone mixing ratios with the updated aromatic chemistry increase by up to 5&thinsp;ppb (more than 10&thinsp;%), especially in industrially polluted regions. The ozone change is partly due to the direct influence of aromatic oxidation products on ozone production rates, and in part to the altered spatial distribution of NOx that enhances the tropospheric ozone production efficiency. Improved representation of aromatics is important to simulate the tropospheric oxidation.</p