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At least 73 records · Page 4

Chemistry-Climate Interactions in the GISS GCM: Tropospheric Chemistry Model Description and Evaluation - Part 1

A tropospheric chemistry module has been developed for use within the Goddard Institute for Space Studies (GISS) general circulation model (GCM) to study interactions between chemistry and climate change. The model uses a simplified chemistry scheme based on CO-NOx-CH4 chemistry, and also includes a parameterization for emissions of isoprene, the most important non-methane hydrocarbon. The model reproduces present day annual cycles and mean distributions of key trace gases fairly well, based on extensive comparisons with available observations. Examining the simulated change between present day and pre-industrial conditions, we find that the model has a similar response to that seen in other simulations. It shows a 45% increase in the global tropospheric ozone burden, within the 25% - 57% range seen in other studies. Annual average zonal mean ozone increases by more than 125% at Northern Hemisphere middle latitudes near the surface. Comparison of model runs that allow the calculated ozone to interact with the GCM's radiation and meteorology with those that do not shows only minor differences for ozone. The common usage of ozone fields that are not calculated interactively seems to be adequate to simulate both the present day and the pre-industrial ozone distributions. However, use of coupled chemistry does alter the change in tropospheric oxidation capacity, enlarging the overall decrease in OH concentrations from the pre-industrial to the present by about 10% (-5.3% global annual average in uncoupled mode, -5.9% in coupled mode). This indicates that there may be systematic biases in the simulation of the pre-industrial to present day decrease in the oxidation capacity of the troposphere (though a 10% difference is well within the total uncertainty). Global annual average radiative forcing from pre-industrial to present day ozone change is 0.32 W/sq m. The forcing seems to be increased by about 10% when the chemistry is coupled to the GCM. Forcing values greater than 0.8 W/sq m are seen over large areas of the United States, Southern Europe, North Africa, the Middle East, Central Asia, and the Arctic. Radiative forcing is greater than 1.5 W/sq m over parts of these areas during Northern summer Though there are local differences, the radiative forcing is overall in good agreement with the results of other modeling studies in both its magnitude and spatial distribution, demonstrating that the simplified chemistry is adequate for climate studies.

Shindell, Drew T.↗

Effect of crop development on biogenic emissions from plant populations grown in closed plant growth chambers

The Biomass Production Chamber at John F. Kennedy Space Center is a closed plant growth chamber facility that can be used to monitor the level of biogenic emissions from large populations of plants throughout their entire growth cycle. The head space atmosphere of a 26-day-old lettuce (Lactuca sativa cv. Waldmann's Green) stand was repeatedly sampled and emissions identified and quantified using GC-mass spectrometry. Concentrations of dimethyl sulphide, carbon disulphide, alpha-pinene, furan and 2-methylfuran were not significantly different throughout the day; whereas, isoprene showed significant differences in concentration between samples collected in light and dark periods. Volatile organic compounds from the atmosphere of wheat (Triticum aestivum cv. Yecora Rojo) were analysed and quantified from planting to maturity. Volatile plant-derived compounds included 1-butanol, 2-ethyl-1-hexanol, nonanal, benzaldehyde, tetramethylurea, tetramethylthiourea, 2-methylfuran and 3-methylfuran. Concentrations of volatiles were determined during seedling establishment, vegetative growth, anthesis, grain fill and senescence and found to vary depending on the developmental stage. Atmospheric concentrations of benzaldehyde and nonanal were highest during anthesis, 2-methylfuran and 3-methylfuran concentrations were greatest during grain fill, and the concentration of the tetramethylurea peaked during senescence.

NASA Program CELSS↗

Sensor arrays for detecting analytes in fluids

A sensor array for detecting an analyte in a fluid, comprising at least first and second chemically sensitive resistors electrically connected to an electrical measuring apparatus, wherein each of the chemically sensitive resistors comprises a mixture of nonconductive material and a conductive material. Each resistor provides an electrical path through the mixture of nonconductive material and the conductive material. The resistors also provide a difference in resistance between the conductive elements when contacted with a fluid comprising an analyte at a first concentration, than when contacted with an analyte at a second different concentration. A broad range of analytes can be detected using the sensors of the present invention. Examples of such analytes include, but are not limited to, alkanes, alkenes, alkynes, dienes, alicyclic hydrocarbons, arenes, alcohols, ethers, ketones, aldehydes, carbonyls, carbanions, polynuclear aromatics, organic derivatives, biomolecules, sugars, isoprenes, isoprenoids and fatty acids. Moreover, applications for the sensors of the present invention include, but are not limited to, environmental toxicology, remediation, biomedicine, material quality control, food monitoring and agricultural monitoring.

Lewis, Nathan S.↗

Evaluation of the MOCAGE Chemistry Transport Model during the ICARTT/ITOP Experiment

We evaluate the Meteo-France global chemistry transport 3D model MOCAGE (MOdele de Chimie Atmospherique a Grande Echelle) using the important set of aircraft measurements collected during the ICARRT/ITOP experiment. This experiment took place between US and Europe during summer 2004 (July 15-August 15). Four aircraft were involved in this experiment providing a wealth of chemical data in a large area including the North East of US and western Europe. The model outputs are compared to the following species of which concentration is measured by the aircraft: OH, H2O2, CO, NO, NO2, PAN, HNO3, isoprene, ethane, HCHO and O3. Moreover, to complete this evaluation at larger scale, we used also satellite data such as SCIAMACHY NO2 and MOPITT CO. Interestingly, the comprehensive dataset allowed us to evaluate separately the model representation of emissions, transport and chemical processes. Using a daily emission source of biomass burning, we obtain a very good agreement for CO while the evaluation of NO2 points out incertainties resulting from inaccurate ratio of emission factors of NOx/CO. Moreover, the chemical behavior of O3 is satisfactory as discussed in the paper.

Bousserez, N.↗

Total Observed Organic Carbon (TOOC): A Synthesis of North American Observations

Measurements of organic carbon compounds in both the gas and particle phases made upwind, over and downwind of North America are synthesized to examine the total observed organic carbon (TOOC) in the atmosphere over this region. These include measurements made aboard the NOAA WP-3 and BAe-146 aircraft, the NOAA research vessel Ronald H. Brown, and at the Thompson Farm and Chebogue Point surface sites during the summer 2004 ICARTT campaign. Both winter and summer 2002 measurements during the Pittsburgh Air Quality Study are also included. Lastly, the spring 2002 observations at Trinidad Head, CA, surface measurements made in March 2006 in Mexico City and coincidentally aboard the C-130 aircraft during the MILAGRO campaign and later during the IMPEX campaign off the northwestern United States are incorporated. Concentrations of TOOC in these datasets span more than two orders of magnitude. The daytime mean TOOC ranges from 4.0 to 456 microg C/cubic m from the cleanest site (Trinidad Head) to the most polluted (Mexico City). Organic aerosol makes up 3-17% of this mean TOOC, with highest fractions reported over the northeastern United States, where organic aerosol can comprise up to 50% of TOOC. Carbon monoxide concentrations explain 46 to 86% of the variability in TOOC, with highest TOOC/CO slopes in regions with fresh anthropogenic influence, where we also expect the highest degree of mass closure for TOOC. Correlation with isoprene, formaldehyde, methyl vinyl ketone and methacrolein also indicates that biogenic activity contributes substantially to the variability of TOOC, yet these tracers of biogenic oxidation sources do not explain the variability in organic aerosol observed over North America. We highlight the critical need to develop measurement techniques to routinely detect total gas phase VOCs, and to deploy comprehensive suites of TOOC instruments in diverse environments to quantify the ambient evolution of organic carbon from source to sink.

Heald, C. L.↗

The Sensitivity of U.S. Surface Ozone Formation to NOx, and VOCs as Viewed from Space

We investigated variations in the sensitivity of surface ozone formation in summer to precursor species concentrations of volatile organic compounds (VOCs) and nitrogen oxides (NO(x)) as inferred from the ratio of tropospheric columns of formaldehyde and nitrogen dioxide from the Aura Ozone Monitoring Instrument (OMI). The data indicate that ozone formation became: 1. more sensitive to NO(x) over most of the U.S, from 2005 to 2007 because of substantial decreases in NO(x) emissions primarily from stationary sources, and 2. more sensitive to NO(x) with increasing temperature, in part because emissions of highly reactive, biogenic isoprene increase with temperature, thus increasing the total VOC reactivity. Based on our interpretation of the data, current strategies implemented to reduce unhealthy levels of surface ozone should focus more on reducing NO(x) emissions, except in some downtown areas which have historically benefited from reductions in VOC emissions.

Duncan, Bryan N.↗

Quantifying VOC-Reaction Tracers, Ozone Production, and Continuing Aerosol Production Rates in Urban and Far-Downwind Atmospheres

We have found a surprisingly informative decomposition of the complex question of smoggy ozone production (basically, [HO2] in a more locally determined field of [NO]) in the process of linked investigations of modestly smoggy Eastern North America (by NASA aircraft, July 2004) and rather polluted Flushing, NYC (Queens College, July, 2001). In both rural and very polluted situations, we find that a simple contour graph parameterization of the local principal ozone production rate can be estimated using only the variables [NO] and j(sub rads) [HCHO]: Po(O3) = c (j(sub rads) [HCHO])(sup a) [HCHO](sup b). Here j(sub rads) is the photolysis of HCHO to radicals, presumably capturing many harder-UV photolytic processes and the principle ozone production is that due to HO2; mechanisms suggest that ozone production due to RO2 is closely correlated, often suggesting a limited range of different proportionality factors. The method immediately suggests a local interpretation for concepts of VOC limitation and NOx limitation. We believe that the product j(sub rads) [HCHO] guages the oxidation rate of observed VOC mixtures in a way that also provides [HO2] useful for the principle ozone production rate k [HO2] [NO], and indeed, all ozone chemical production. The success of the method suggests that dominant urban primary-HCHO sources may transition to secondary plume-HCHO sources in a convenient way. Are there other, simple, near-terminal oxidized VOC's which help guage ozone production and aerosol particle formation? Regarding particles, we report on, to the extent NASA Research resources allow, on appealing relationships between far-downwind (Atlantic PBL) HCHO and very fine aerosol (including sulfate. Since j(sub rads) [HCHO] provides a time-scale, we may understand distant-plume particle production in a more quantitative manner. Additionally we report on a statistical search in the nearer field for relationships between glyoxals (important near-terminal aromatic and isoprene reaction products) and aerosol production, looking for VOC's that might be most implicated. All three variables j(sub rads), [HCHO], and [NO] are relatively easily measured in widespread air pollution monitoring networks, and all are deducible form space-borne observations, though estimation of [NO] from [NO2] (the species observable from space) may require care. We report also on airborne and surface observations of HCHO, suggesting that concentrated (urban) and more diffuse (forest) sources may be distinguishable from space. The use of the 3.58 micron microwindow for HCHO remote sensing should allow much sharper resolution of HCHO than the UV. UV sensing requires large and expensive instruments, but even these seem justified since formaldehyde is so informative.

Chatfield, Robert↗

The Utility of the OMI HCHO and NO2 Data Products in Air Quality Decision- Making Activities

We will present three related air quality applications of the OMI HCHO (formaldehyde) and NO2 (nitrogen dioxide) data products, which we us to support mission planning of an OMI-like instrument for the proposed GEO-CAPE satellite that has as one of its objectives to study air quality from space. First, we will discuss a novel and practical application of the data products to the "weight of evidence" in the air quality decision-making process (e.g., State Implementation Plan (SIP)) for a city, region, or state to demonstrate that it is making progress toward attainment of the National Ambient Air Quality Standard (NAAQS) for ozone. Any trend, or lack thereof, in the observed OMI HCHO/NO2, which we use as an air quality indicator, may support that an emission control strategy implemented to reduce ozone is or is not occurring for a metropolitan area. Second, we will discuss how we use variations in the OMI HCHO product as a proxy for variability in the biogenic hydrocarbon, isoprene, which is an important player for the formation of high levels of ozone and the dominant source of HCHO in the eastern U.S. Third, we will discuss the variability of NO2 in the U.S. as indicated by the OMI NO2 product. In addition, we will show the impact of the 2005 hurricanes on pollutant emissions, including those associated with the intensive oil extraction and refining activities, in the Gulf of Mexico region using the OMI NO2 product. The variability of HCHO and NO2 as indicated by OMI helps us to understand changes in the OMI HCHO/NO2 and the implications for ozone formation.

Duncan, Bryan N.↗

Impacts of Climate Change on Surface Ozone and Intercontinental Ozone Pollution: A Multi-Model Study

The impact of climate change between 2000 and 2095 SRES A2 climates on surface ozone (O)3 and on O3 source-receptor (S-R) relationships is quantified using three coupled climate-chemistry models (CCMs). The CCMs exhibit considerable variability in the spatial extent and location of surface O3 increases that occur within parts of high NOx emission source regions (up to 6 ppbv in the annual average and up to 14 ppbv in the season of maximum O3). In these source regions, all three CCMs show a positive relationship between surface O3 change and temperature change. Sensitivity simulations show that a combination of three individual chemical processes-(i) enhanced PAN decomposition, (ii) higher water vapor concentrations, and (iii) enhanced isoprene emission-largely reproduces the global spatial pattern of annual-mean surface O3 response due to climate change (R2 = 0.52). Changes in climate are found to exert a stronger control on the annual-mean surface O3 response through changes in climate-sensitive O3 chemistry than through changes in transport as evaluated from idealized CO-like tracer concentrations. All three CCMs exhibit a similar spatial pattern of annual-mean surface O3 change to 20% regional O3 precursor emission reductions under future climate compared to the same emission reductions applied under present-day climate. The surface O3 response to emission reductions is larger over the source region and smaller downwind in the future than under present-day conditions. All three CCMs show areas within Europe where regional emission reductions larger than 20% are required to compensate climate change impacts on annual-mean surface O3.

Troposphere: constituent transport and chemistry↗

Anthropogenic Emissions of Highly Reactive Volatile Organic Compounds (HRVOCs) Inferred from Oversampling of OMI HCHO Columns

Satellite observations of formaldehyde (HCHO) columns provide top-down constraints on emissions of highly reactive volatile organic compounds (HRVOCs). This approach has been used previously to constrain emissions of isoprene from vegetation, but application to US anthropogenic emissions has been stymied by lack of a discernable HCHO signal. Here we show that oversampling of HCHO data from the Ozone Monitoring Instrument (OMI) for 2005 - 2008 enables quantitative detection of urban and industrial plumes in eastern Texas including Houston, Port Arthur, and Dallas-Fort Worth. By spatially integrating the individual urban-industrial HCHO plumes observed by OMI we can constrain the corresponding HCHO-weighted HRVOC emissions. Application to the Houston plume indicates a HCHO source of 260 plus or minus 110 kmol h-1 and implies a factor of 5.5 plus or minus 2.4 underestimate of anthropogenic HRVOC emissions in the US Environmental Protection Agency inventory. With this approach we are able to monitor the trend in HRVOC emissions over the US, in particular from the oil-gas industry, over the past decade.

AURA↗

Planning, Implementation, and Scientific Goals of the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) Field Missions

The Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field mission based at Ellington Field, Texas, during August and September 2013 employed the most comprehensive airborne payload to date to investigate atmospheric composition over North America. The NASA ER-2, DC-8, and SPEC Inc. Learjet flew 57 science flights from the surface to 20 km. The ER-2 employed seven remote sensing instruments as a satellite surrogate and eight in situ instruments. The DC-8 employed 23 in situ and five remote sensing instruments for radiation, chemistry, and microphysics. The Learjet used 11 instruments to explore cloud microphysics. SEAC4RS launched numerous balloons, augmented Aerosol RObotic NETwork, and collaborated with many existing ground measurement sites. Flights investigating convection included close coordination of all three aircraft. Coordinated DC-8 and ER-2 flights investigated the optical properties of aerosols, the influence of aerosols on clouds, and the performance of new instruments for satellite measurements of clouds and aerosols. ER-2 sorties sampled stratospheric injections of water vapor and other chemicals by local and distant convection. DC-8 flights studied seasonally evolving chemistry in the Southeastern U.S., atmospheric chemistry with lower emissions of NOx and SO2 than in previous decades, isoprene chemistry under high and low NOx conditions at different locations, organic aerosols, air pollution near Houston and in petroleum fields, smoke from wildfires in western forests and from agricultural fires in the Mississippi Valley, and the ways in which the chemistry in the boundary layer and the upper troposphere were influenced by vertical transport in convective clouds.

Toon, Owen B.↗

Quantifying the Causes of Differences in Tropospheric OH Within Global Models

The hydroxyl radical (OH) is the primary daytime oxidant in the troposphere and provides the main loss mechanism for many pollutants and greenhouse gases, including methane (CH4). Global mean tropospheric OH differs by as much as 80% among various global models, for reasons that are not well understood. We use neural networks (NNs), trained using archived output from eight chemical transport models (CTMs) that participated in the Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport Model Intercomparison Project (POLMIP), to quantify the factors responsible for differences in tropospheric OH and resulting CH4 lifetime (Tau CH4) between these models. Annual average Tau CH4, for loss by OH only, ranges from 8.0 to 11.6 years for the eight POLMIP CTMs. The factors driving these differences were quantified by inputting 3-D chemical fields from one CTM into the trained NN of another CTM. Across all CTMs, the largest mean differences in Tau CH4 (Delta Tau CH4) result from variations in chemical mechanisms (Delta Tau CH4 = 0.46 years), the photolysis frequency (J) of O3 yields O(D-1) (0.31 years), local O3 (0.30 years), and CO (0.23 years). The Delta Tau CH4 due to CTM differences in NO(x) (NO + NO2) is relatively low (0.17 years), although large regional variation in OH between the CTMs is attributed to NO(x). Differences in isoprene and J(NO2) have negligible overall effect on globally averaged tropospheric OH, although the extent of OH variations due to each factor depends on the model being examined. This study demonstrates that NNs can serve as a useful tool for quantifying why tropospheric OH varies between global models, provided that essential chemical fields are archived.

Surface Measurements and Models↗

Controlled Nitric Oxide Production via O(1D) + N2O Reactions for Use in Oxidation Flow Reactor Studies

Oxidation flow reactors that use low-pressure mercury lamps to produce hydroxyl (OH) radicals are an emerging technique for studying the oxidative aging of organic aerosols. Here, ozone (O3) is photolyzed at 254 nm to produce O(1D) radicals, which react with water vapor to produce OH. However, the need to use parts-per-million levels of O3 hinders the ability of oxidation flow reactors to simulate NOx-dependent secondary organic aerosol (SOA) formation pathways. Simple addition of nitric oxide (NO) results in fast conversion of NOx (NO+NO2) to nitric acid (HNO3), making it impossible to sustain NOx at levels that are sufficient to compete with hydroperoxy (HO2) radicals as a sink for organic peroxy (RO2) radicals. We developed a new method that is well suited to the characterization of NOx-dependent SOA formation pathways in oxidation flow reactors. NO and NO2 are produced via the reaction O(1D)+N2O->2NO, followed by the reaction NO+O3->NO2+O2. Laboratory measurements coupled with photochemical model simulations suggest that O(1D)+N2O reactions can be used to systematically vary the relative branching ratio of RO2 +NO reactions relative to RO2 +HO2 and/or RO2+RO2 reactions over a range of conditions relevant to atmospheric SOA formation. We demonstrate proof of concept using high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) measurements with nitrate (NO-3 ) reagent ion to detect gas-phase oxidation products of isoprene and -pinene previously observed in NOx-influenced environments and in laboratory chamber experiments.

Lambe, Andrew↗

Surface Ozone in the Colorado Northern Front Range and the Influence of Oil and Gas Development During FRAPPE/DISCOVER-AQ in Summer 2014

High mixing ratios of ozone (O3) in the northern Front Range (NFR) of Colorado are not limited to the urban Denver area but were also observed in rural areas where oil and gas activity is the primary source of O3 precursors. On individual days, oil and gas O3 precursors can contribute in excess of 30 ppb to O3 growth and can lead to exceedances of the EPA O3 National Ambient Air Quality Standard. Data used in this study were gathered from continuous surface O3 monitors for June-August 2013-2015 as well as additional flask measurements and mobile laboratories that were part of the FRAPPE/DISCOVER-AQ field campaign of July-August 2014. Overall observed O3 levels during the summer of 2014 were lower than in 2013, likely due to cooler and damper weather than an average summer. This study determined the median hourly surface O3 mixing ratio in the NFR on summer days with limited photochemical production to be approximately 45-55 ppb. Mobile laboratory and flask data collected on three days provide representative case studies of different O3 formation environments in and around Greeley, Colorado. Observations of several gases (including methane, ethane, CO, nitrous oxide) along with O3 are used to identify sources of O3 precursor emissions. A July 23 survey demonstrated low O3 (45-60 ppb) while August 3 and August 13 surveys recorded O3 levels of 75-80 ppb or more. August 3 exemplifies influence of moderate urban and high oil and gas O3 precursor emissions. August 13 demonstrates high oil and gas emissions, low agricultural emissions, and CO measurements that were well correlated with ethane from oil and gas, suggesting an oil and gas related activity as a NOx and O3 precursor source. Low isoprene levels indicated that they were not a significant contributor to O3 precursors measured during the case studies.

Pollution↗

A Machine Learning Examination of Hydroxyl Radical Differences Among Model Simulations for CCMI-1

Hydroxyl radical (OH) plays critical roles within the troposphere, such as determining the lifetime of methane (CH4), yet is challenging to model due to its fast cycling and dependence on a multitude of sources and sinks. As a result, the reasons for variations in OH and the resulting CH4 lifetime (TCH4), both between models and in time, are difficult to diagnose. We apply a neural network (NN) approach to address this issue within a group of models that participated in the Chemistry-Climate Model Initiative (CCMI). Analysis of the historical specified dynamics simulations performed for CCMI indicates that the primary drivers of TCH4 differences among ten models are the flux of UV light to the troposphere (indicated by the photolysis frequency JO1D) due mostly to clouds, mixing ratio of tropospheric ozone (O3), the abundance of nitrogen oxides (NOx≡NO+NO2), and details of the various chemical mechanisms that drive OH. Water vapor, carbon monoxide (CO), the ratio of NO:NOx, and formaldehyde (HCHO) explain moderate differences in TCH4, while isoprene, CH4, the photolysis frequency of NO2 by visible light (JNO2), overhead O3 column, and temperature account for little-to-no model variation in CH4. We also apply the NNs to analysis of temporal trends in OH from 1980 to 2015. All models that participated in the specified dynamics historical simulation for CCMI demonstrate a decline in CH4 during the analysed timeframe. The significant contributors to this trend, in order of importance, are tropospheric O3, JO1D, NOx, and H2O, with CO also causing substantial interannual variability in OH burden. Finally, the identified trends in TCH4 are compared to calculated trends in the tropospheric mean OH concentration from previous work, based on analysis of observations. The comparison reveals a robust result for the effect of rising water vapor on OH and CH4, imparting an increasing and decreasing trend of about 0.5% decade(exp -1), respectively. The responses due to NOx, O3 column, and temperature are also in reasonably good agreement between the two studies, though a discrepancy in the CH4 response highlights a need for further examination of the CH4 feedback on the abundance of OH.

Julie M Nicely↗

TPSAS-NF1676L-11598-DND

Satellite data show a strong summertime maximum in aerosol optical depth (AOD) over the Southeastern (SE) USA that can not be explained by anthropogenic sulfate or organic aerosols at the surface (Goldstein et al., 2009). The biogenic volatile organic compound (BVOC) emissions peak over the same region and models indicate a large source of secondary organic aerosols (SOA) here (van Donkelaar et al., 2007, Zhang et al., 2007, Liao et al., 2007). Aircraft measurements indicate dominance of organic aerosols over sulfates with altitude and models suggest most SOA production from isoprene oxidation takes place above the surface layers. Goldstein et al. (2009) hypothesized that these SOA drive the AOD maximum in summer with an altitude dependence. We examine the distributions of AOD and other optical properties over SE USA using height resolved aerosol data from CALIPSO. We also use AOD data from MODIS and OMI and UV aerosol index from OMI to characterize the aerosols over SE USA.

J Kar↗

FUTURE LEVELS OF AEROSOLS & RADIATIVE FORCING OVER THE ARCTIC

The Arctic Monitoring and Assessment Programme (AMAP) is currently assessing the impacts of Short-Lived Climate Forcers (SLCF) on Arctic climate and air quality. In support of the assessment, we used the NASA Goddard Institute of Space Sciences (GISS) Earth System Model (modelE2.1), with prescribed sea surface temperature and sea-ice fraction, to simulate SLCF concentrations globally between 1995 and 2015. Two simulations were conducted, using the One-Moment Aerosol (OMA) and the Multiconfiguration Aerosol TRacker of mIXing state (MATRIX) aerosol modules. OMA is a mass-based scheme in which aerosols are assumed to remain externally mixed and have a prescribed and constant size distribution, while MATRIX is an aerosol microphysics scheme based on the quadrature method of moments, which is able to explicitly simulate the mixing state of aerosols. Anthropogenic emissions from the ECLIPSE v6b emissions database were used, along with emissions from aircrafts and open biomass burning from the Coupled Model Intercomparison Project Phase 6 (CMIP6), while the natural emissions of sea salt, DMS, isoprene and dust are calculated interactively. The simulated monthly surface concentrations of sulfate (SO4), black carbon (BC), organic carbon (OA), and ozone (O3) are compared with observations from a set of Arctic stations, extracted from the EBAS and IMPROVE databases, as well as a few additional locations. Simulated aerosol optical depths (AOD) are also compared with Advanced Very-High Resolution Radiometer (AVHRR). The study will present the evaluation of the modelE2.1 in simulating SLCF levels over the Arctic using different aerosol schemes, along with observed and simulated trends of SLCFs over the Arctic between 1995 and 2015.

Aersosols↗

The Ozone–Climate Penalty Over South America and Africa By 2100

Climate change has the potential to increase surface ozone (O3) concentrations, known as the “ozone–climate penalty”, through changes to atmospheric chemistry, transport and dry deposition. In the tropics, the response of surface O3 to changing climate is relatively understudied but has important consequences for air pollution and human and ecosystem health. In this study, we evaluate the change in surface O3 due to climate change over South America and Africa using three state-of-the-art Earth system models that follow the Shared Socioeconomic Pathway 3-7.0 emission scenario from CMIP6. In order to quantify changes due to climate change alone, we evaluate the difference between simulations including climate change and simulations with a fixed present-day climate. We find that by 2100, models predict an ozone–climate penalty in areas where O3 is already predicted to be high due to the impacts of precursor emissions, namely urban and biomass burning areas, although on average, models predict a decrease in surface O3 due to climate change. We identify a small but robust positive trend in annual mean surface O3 over polluted areas. Additionally, during biomass burning seasons, seasonal mean O3 concentrations increase by 15 ppb (model range 12 to 18 ppb) in areas with substantial biomass burning such as the arc of deforestation in the Amazon. The ozone–climate penalty in polluted areas is shown to be driven by an increased rate of O3 chemical production, which is strongly influenced by NOx concentrations and is therefore specific to the emission pathway chosen. Multiple linear regression finds the change in NOx concentration to be a strong predictor of the change in O3 production, whereas increased isoprene emission rate is positively correlated with increased O3 destruction, suggesting NOx-limited conditions over the majority of tropical Africa and South America. However, models disagree on the role of climate change in remote, low-NOx regions, partly because of significant differences in NOx concentrations produced by each model. We also find that the magnitude and location of the ozone–climate penalty in the Congo Basin has greater inter-model variation than that in the Amazon, so further model development and validation are needed to constrain the response in central Africa. We conclude that if the climate were to change according to the emission scenario used here, models predict that forested areas in biomass burning locations and urban populations will be at increasing risk of high O3 exposure, irrespective of any direct impacts on O3 via the prescribed emission scenario.

Surface ozone↗