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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Impacts of sea ice leads on sea salt aerosols and atmospheric chemistry in the Arctic

Abstract. The processes contributing to Arctic cold-season (November–April) sea salt aerosols (SSAs) remain uncertain. Observations from coastal Alaska suggest that emissions from open leads in sea ice, which are not included in climate models, may play a dominant role. Their Arctic-wide significance has not yet been quantified. Here, we create an emission parameterization of SSAs from leads by combining satellite data of lead area (the Advanced Microwave Scanning Radiometer–Earth Observation System (AMSR-E) product) and a chemical transport model (GEOS-Chem) to quantify pan-Arctic SSA emissions from leads during the cold season from 2002 to 2008 and to predict their impacts on atmospheric chemistry, evaluating the results of our simulated SSAs against in situ observations. The AMSR-E product detects large leads with certainty (> 3 km in size), and, hence, our study is limited to quantifying emissions from large leads. Lead emissions vary seasonally and interannually. Simulated total monthly SSA emissions increase by 1.1 %–1.8 % (≥60° N latitude) and 5.6 %–7.5 % (≥75° N) for the 2002–2008 cold seasons. SSA concentrations primarily increase at the location of leads, where standard model concentrations are low. GEOS-Chem overestimates SSA concentrations at Arctic sites compared to ground observations, even when lead emissions are not included, suggesting underestimation of SSA sinks and/or uncertainties in SSA emissions from blowing snow and the open ocean. Multi-year monthly mean surface bromine atom (Br) concentrations increase by 2.8 %–8.8 % due to SSAs from leads for the 2002–2008 cold seasons. Changes in ozone concentrations are negligible. While leads contribute < 10 % to Arctic-wide SSA emissions in the years 2002–2008, these emissions occur in regions of low background aerosol concentrations. Leads may increase in frequency under future climate change, which could increase SSA emissions from leads.

Emme, Erin J. (ORCID:0000000268406352)↗
NASA NTRS1999

Remote Sensing of Aerosol and their Radiative Forcing of Climate

Remote sensing of aerosol and aerosol radiative forcing of climate is going through a major transformation. The launch in next few years of new satellites designed specifically for remote sensing of aerosol is expected to further revolutionized aerosol measurements: until five years ago satellites were not designed for remote sensing of aerosol. Aerosol optical thickness was derived as a by product, only over the oceans using one AVHRR channel with errors of approx. 50%. However it already revealed a very important first global picture of the distribution and sources of aerosol. In the last 5 years we saw the introduction of polarization and multi-view observations (POLDER and ATSR) for satellite remote sensing of aerosol over land and ocean. Better products are derived from AVHRR using its two channels. The new TOMS aerosol index shows the location and transport of aerosol over land and ocean. Now we anticipate the launch of EOS-Terra with MODIS, MISR and CERES on board for multi-view, multi-spectral remote sensing of aerosol and its radiative forcing. This will allow application of new techniques, e.g. using a wide spectral range (0.55-2.2 microns) to derive precise optical thickness, particle size and mass loading. Aerosol is transparent in the 2.2 microns channel, therefore this channel can be used to detect surface features that in turn are used to derive the aerosol optical thickness in the visible part of the spectrum. New techniques are developed to derive the aerosol single scattering albedo, a measure of absorption of sunlight, and techniques to derive directly the aerosol forcing at the top of the atmosphere. In the last 5 years a global network of sun/sky radiometers was formed, designed to communicate in real time the spectral optical thickness from 50-80 locations every day, every 15 minutes. The sky angular and spectral information is also measured and used to retrieve the aerosol size distribution, refractive index, single scattering albedo and the spectral flux reaching the surface. Effort to introduce remote sensing from lidars will literally additional dimension to aerosol remote sensing. The vertical dimension is a critical link between the global satellite observations and modeling of aerosol transport. Lidars are also critical to study aerosol impact on cloud microphysics and reflectance. Both lidar ground networks and satellite systems are in development. This new capability is expected to put remote sensing in the forefront of aerosol and climate studies. Together with field experiments, chemical analysis and chemical transport models we anticipate, in the next decade, to be able to resolve some of the outstanding questions regarding the role of aerosol in climate, in atmospheric chemistry and its influence on human health and life on this planet.

Kaufman, Yoram J.↗
NASA NTRS2007

Effects of Deep Convection on Atmospheric Chemistry

This presentation will trace the important research developments of the last 20+ years in defining the roles of deep convection in tropospheric chemistry. The role of deep convection in vertically redistributing trace gases was first verified through field experiments conducted in 1985. The consequences of deep convection have been noted in many other field programs conducted in subsequent years. Modeling efforts predicted that deep convection occurring over polluted continental regions would cause downstream enhancements in photochemical ozone production in the middle and upper troposphere due to the vertical redistribution of ozone precursors. Particularly large post-convective enhancements of ozone production were estimated for convection occurring over regions of pollution from biomass burning and urban areas. These estimates were verified by measurements taken downstream of biomass burning regions of South America. Models also indicate that convective transport of pristine marine boundary layer air causes decreases in ozone production rates in the upper troposphere and that convective downdrafts bring ozone into the boundary layer where it can be destroyed more rapidly. Additional consequences of deep convection are perturbation of photolysis rates, effective wet scavenging of soluble species, nucleation of new particles in convective outflow, and the potential fix stratosphere-troposphere exchange in thunderstorm anvils. The remainder of the talk will focus on production of NO by lightning, its subsequent transport within convective clouds . and its effects on downwind ozone production. Recent applications of cloud/chemistry model simulations combined with anvil NO and lightning flash observations in estimating NO Introduction per flash will be described. These cloud-resolving case-study simulations of convective transport and lightning NO production in different environments have yielded results which are directly applicable to the design of lightning parameterizations for global chemical transport models. The range of mean values (factor of 3) of NO production per flash (or per meter of lightning channel length) that have been deduced from the model will be shown and compared with values of production in the literature that have been deduced using other methods, Results show that on a per flash basis, IC flashes are nearly as productive of NO as CG flashes. When combined with the global flash rate of 44 flashes per second from NASA's Optical Transient Detector (OTD) measurements, these estimates and the results from other techniques yield global NO production rates of 2-9 TgN/year. Vertical profiles of lightning NOx mass at the end of the 3-D storm simulations have been summarized to yield suggested profiles for use in global models. Simulations of the photochemistry over the 24 hours following a storm have been performed to determine the additional ozone production which can be attributed to lightning NO.

Pickering, Kenneth E.↗
NASA NTRS2005

Trends from the Long-term Data Record and Models: What Do They Tell Us About our Ability to Predict Ozone Recovery?

Our industrial society has performed an experiment on the stratospheric ozone layer over the last several decades. The initial part of this experiment was the rapidly increasing release of halogen-containing compounds that carry chlorine and bromine to the stratosphere where they can cause a loss of ozone. The present part of this experiment is the implementation of the Montreal Protocol, which has led to a leveling off of these halogen compounds and the beginning of their slow removal from the atmosphere. The observation and attribution of ozone response to the halogens has been a particularly important and difficult task because of the impact of solar cycle uv variation, two major volcanic eruptions (El Chichon and Pinatubo), and interannual dynamic variability of the stratosphere. We have run 3 different simulations of the chemistry and transport of ozone and the minor constituents that affect ozone to help evaluate our understanding of the causes of ozone change and to assess our ability to predict ozone recovery with the removal of halogens from the stratosphere. One simulation, using the Goddard chemical transport model (CTM), had interannual variability in the dynamics for the entire 50 years of simulation, which included the past 3 decades (1974-2004) and the next 2 decades to 2022. The other two simulations used the Global Modeling Initiative (GMI) CTM with no dynamical variability: one used a the winds and temperatures from a repeating warm Arctic winter and the other used a repeating cold Arctic winter. All simulations included the effects of aerosol surfaces from volcanic eruptions on chemical reactions as well as the variation in UV over the 11-year solar cycle.

Strahan, Susan↗
NASA NTRS2011

The Various Influences due to Aerosol Depositions

Recently the issue on glacier retreats comes up and many factors should be relevant to the issue. The absorbing aerosols such as dust and black carbon (BC) are considered to be one of the factors. After they deposited onto the snow surface, it will reduce snow albedo (called snow darkening effect) and probably contribute to further melting of glacier. The Goddard Earth Observing System version 5 (GEOS-5) has developed at NASA/GSFC. However, the original snowpack model used in the land surface model in the GEOS-5 did not consider the snow darkening effect. Here we developed the new snow albedo scheme which can consider the snow darkening effect. In addition, another scheme on calculating mass concentrations on the absorbing aerosols in snowpack was also developed, in which the direct aerosol depositions from the chemical transport model in the GEOS-5 were used. The scheme has been validated with the observed data obtained at backyard of the Institute of Low Temperature Science, Hokkaido University, by Dr. Teruo Aoki (Meteorological Research Institute) et al. including me. The observed data was obtained when I was Ph.D.caftdidate. The original GEOS-5 during 2007-2009 over the Himalayas and Tibetan Plateau region showed more reductions of snow than that of the new GEOS-5 because the original one used lower albedo settings. On snow cover fraction, the new GEOS-5 simulated more realistic snow-covered area comparing to the MODIS snow cover fraction. The reductions on snow albedo, snow cover fraction, and snow water equivalent were seen with statistically significance if we consider the snow darkening effect comparing to the results without the snow darkening effect. In the real world, debris cover, inside refreezing process, surface flow of glacier, etc. affect glacier mass balance and the simulated results immediately do not affect whole glacier retreating. However, our results indicate that some surface melting over non debris covered parts of the glacier would be explained by the snow darkening effect. Further discussion and observations are necessary to assess the glacier issue.

Yasunari, Teppei↗
NASA NTRS2012

Incorporation of the Mass Concentration and the New Snow Albedo Schemes into the Global Forecasting Model, GEOS-5 and the Impact of the New Schemes over Himalayan Glaciers

Recently the issue on glacier retreats comes up and many factors should be relevant to the issue. The absorbing aerosols such as dust and black carbon (BC) are considered to be one of the factors. After they deposited onto the snow surface, it will reduce snow albedo (called snow darkening effect) and probably contribute to further melting of glacier. The Goddard Earth Observing System version 5 (GEOS-5) has developed at NASA/GSFC. However, the original snowpack model used in the land surface model in the GEOS-5 did not consider the snow darkening effect. Here we developed the new snow albedo scheme which can consider the snow darkening effect. In addition, another scheme on calculating mass concentrations on the absorbing aerosols in snowpack was also developed, in which the direct aerosol depositions from the chemical transport model in the GEOS-5 were used. The scheme has been validated with the observed data obtained at backyard of the Institute of Low Temperature Science, Hokkaido University, by Dr. Teruo Aoki (Meteorological Research Institute) et aL including me. The observed data was obtained when I was Ph.D. candidate. The original GEOS-5during 2007-2009 over the Himalayas and Tibetan Plateau region showed more reductions of snow than that of the new GEOS-5 because the original one used lower albedo settings. On snow cover fraction, the new GEOS-5 simulated more realistic snow-covered area comparing to the MODIS snow cover fraction. The reductions on snow albedo, snow cover fraction, and snow water equivalent were seen with statistically significance if we consider the snow darkening effect comparing to the results without the snow darkening effect. In the real world, debris cover, inside refreezing process, surface flow of glacier, etc. affect glacier mass balance and the simulated results immediately do not affect whole glacier retreating. However, our results indicate that some surface melting over non debris covered parts of the glacier would be explained by the snow darkening effect. Further discussion and observations are necessary to assess the glacier issue.

Yasunari, Teppei↗
NASA NTRS2016

Why Do Models Overestimate Surface Ozone in the Southeast United States?

Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NO(x) triple bond NO + NO2) and biogenic isoprene. Model estimates of surface ozone concentrations tend to be biased high in the region and this is of concern for designing effective emission control strategies to meet air quality standards. We use detailed chemical observations from the SEAC(exp 4)RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model at 0.25 deg x 0.3125 deg horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NO(x) from the US Environmental Protection Agency (EPA) is too high. This finding is based on SEAC(exp 4)RS observations of NO(x) and its oxidation products, surface network observations of nitrate wet deposition fluxes, and OMI satellite observations of tropospheric NO2 columns. Our results indicate that NEI NO(x) emissions from mobile and industrial sources must be reduced by 30-60%, dependent on the assumption of the contribution by soil NO(x) emissions. Upper-tropospheric NO2 from lightning makes a large contribution to satellite observations of tropospheric NO2 that must be accounted for when using these data to estimate surface NO(x) emissions. We find that only half of isoprene oxidation proceeds by the high-NO(x) pathway to produce ozone; this fraction is only moderately sensitive to changes in NO(x) emissions because isoprene and NO(x) emissions are spatially segregated. GEOS-Chem with reduced NO(x) emissions provides an unbiased simulation of ozone observations from the aircraft and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NO(x) oxidation products. However, the model is still biased high by 6 plus or minus 14 ppb relative to observed surface ozone in the Southeast US. Ozonesondes launched during midday hours show a 7 ppb ozone decrease from 1.5 km to the surface that GEOS-Chem does not capture. This bias may reflect a combination of excessive vertical mixing and net ozone production in the model boundary layer.

Oxidation↗
NASA NTRS2022

Clumped-Isotope Constraint on Upper-Tropospheric Cooling During the Last Glacial Maximum

Ice cores and other paleotemperature proxies, together with general circulation models, have provided information on past surface temperatures and the atmosphere's composition in different climates. Little is known, however, about past temperatures at high altitudes, which play a crucial role in Earth's radiative energy budget. Paleoclimate records at high-altitude sites are sparse, and the few that are available show poor agreement with climate model predictions. These disagreements could be due to insufficient spatial coverage, spatiotemporal biases, or model physics; new records that can mitigate or avoid these uncertainties are needed. Here, we constrain the change in upper-tropospheric temperature at the global scale during the Last Glacial Maximum (LGM) using the clumped-isotope composition of molecular oxygen trapped in polar ice cores. Aided by global three-dimensional chemical transport modeling, we exploit the intrinsic temperature sensitivity of the clumped-isotope composition of atmospheric oxygen to infer that the upper troposphere (effective mean altitude 10–11 km) was 6–9°C cooler during the LGM than during the late preindustrial Holocene. A complementary energy balance approach supports a minor or negligible steepening of atmospheric lapse rates during the LGM, which is consistent with a range of climate model simulations. Proxy-model disagreements with other high-altitude records may stem from inaccuracies in regional hydroclimate simulation, possibly related to land-atmosphere feedbacks.

clumped isotope↗
NASA NTRS2004

Sensitivity of the FVGCM to Changes in Ozone

We have carried out an experiment with the finite volume general circulation model (FVGCM). This experiment consisted of two different imposed changes in the climatological ozone fields assumed in the radiation code. for conditions with no significant ozone hole. This distribution was obtained from a 50-year simulation of the full stratospheric ozone chemistry, with a time-dependent chlorine loading, done with our off-line chemical transport model (CTM). Three years (1978-1980) of this simulation were averaged to form a monthly, zonal-mean ozone distribution that was used in the 20-year integration of the FVGCM for "unperturbed" conditions. The second 20-year GCM integration included a fully-developed ozone hole. This ozone distribution was from three years, 1998-2000, from the same CTM simulation. The goal of this work is to determine the coupled response of the chemistry and dynamics of the stratosphere. These experiments are the first step in understanding the coupled response. An important initial question concerns the significance of the signals: if 20-year integrations turn out to be too short, the runs will be extended.

Stolarski↗
NASA NTRS2016

High Upward Fluxes of Formic Acid from a Boreal Forest Canopy

Eddy covariance fluxes of formic acid, HCOOH, were measured over a boreal forest canopy in spring/summer 2014. The HCOOH fluxes were bidirectional but mostly upward during daytime, in contrast to studies elsewhere that reported mostly downward fluxes. Downward flux episodes were explained well by modeled dry deposition rates. The sum of net observed flux and modeled dry deposition yields an upward gross flux of HCOOH, which could not be quantitatively explained by literature estimates of direct vegetative soil emissions nor by efficient chemical production from other volatile organic compounds, suggesting missing or greatly underestimated HCOOH sources in the boreal ecosystem. We implemented a vegetative HCOOH source into the GEOS-Chem chemical transport model to match our derived gross flux and evaluated the updated model against airborne and spaceborne observations. Model biases in the boundary layer were substantially reduced based on this revised treatment, but biases in the free troposphere remain unexplained.

forest↗
NASA NTRS2016

Model Sensitivity Studies of the Decrease in Atmospheric Carbon Tetrachloride

Carbon tetrachloride (CCl4) is an ozone-depleting substance, which is controlled by the Montreal Protocol and for which the atmospheric abundance is decreasing. However, the current observed rate of this decrease is known to be slower than expected based on reported CCl4 emissions and its estimated overall atmospheric lifetime. Here we use a three-dimensional (3-D) chemical transport model to investigate the impact on its predicted decay of uncertainties in the rates at which CCl4 is removed from the atmosphere by photolysis, by ocean uptake and by degradation in soils. The largest sink is atmospheric photolysis (74% of total), but a reported 10% uncertainty in its combined photolysis cross section and quantum yield has only a modest impact on the modelled rate of CCl4 decay. This is partly due to the limiting effect of the rate of transport of CCl4 from the main tropospheric reservoir to the stratosphere, where photolytic loss occurs. The model suggests large interannual variability in the magnitude of this stratospheric photolysis sink caused by variations in transport. The impact of uncertainty in the minor soil sink (9%of total) is also relatively small. In contrast, the model shows that uncertainty in ocean loss (17%of total) has the largest impact on modelled CCl4 decay due to its sizeable contribution to CCl4 loss and large lifetime uncertainty range (147 to 241 years). With an assumed CCl4 emission rate of 39 Gg year(exp -1), the reference simulation with the best estimate of loss processes still underestimates the observed CCl4 (overestimates the decay) over the past 2 decades but to a smaller extent than previous studies. Changes to the rate of CCl4 loss processes, in line with known uncertainties, could bring the model into agreement with in situ surface and remote-sensing measurements, as could an increase in emissions to around 47 Gg year(exp -1). Further progress in constraining the CCl4 budget is partly limited by systematic biases between observational datasets. For example, surface observations from the National Oceanic and Atmospheric Administration (NOAA) network are larger than from the Advanced Global Atmospheric Gases Experiment (AGAGE) network but have shown a steeper decreasing trend over the past 2 decades. These differences imply a difference in emissions which is significant relative to uncertainties in the magnitudes of the CCl4 sinks.

Carbon Trechloride↗
NASA NTRS2017

Ozone Production by Corona Discharges During a Convective Event in DISCOVER-AQ Houston

An ozonesonde launched near electrically active convection in Houston, TX on 5 September 2013 during the NASA DISCOVER-AQ project measured a large enhancement of ozone throughout the troposphere. A separate ozonesonde was launched from Smith Point, TX (approx. 58 km southeast of the Houston site) at approximately the same time as the launch from Houston and did not measure that enhancement. Furthermore, ozone profiles for the descent of both sondes agreed well with the ascending Smith Point profile, suggesting a highly localized event in both space and time in which an anomalously large enhancement of 70 - 100 ppbv appeared in the ascending Houston ozonesonde data. Compared to literature values, such an enhancement appears to be the largest observed to date. Potential sources of the localized ozone enhancement such as entrainment of urban or biomass burning emissions, downward transport from the stratosphere, photochemical production from lightning NO(sub x), and direct ozone production from corona discharges were investigated using model simulations. We conclude that the most likely explanation for the large ozone enhancement is direct ozone production by corona discharges. Integrating the enhancement seen in the Houston ozone profile and using the number of electrical discharges detected by the NLDN (or HLMA), we estimate a production of 2.48 x 10(exp. 28) molecules of ozone per flash which falls within the range of previously recorded values (9.89 x 10(exp. 26) - 9.82 x 10)exp. 28) molecules of ozone per flash). Since there is currently no parameterization for the direct production of ozone from corona discharges we propose the implementation of an equation into a chemical transport model. Ultimately, additional work is needed to further understand the occurrence and impact of corona discharges on tropospheric chemistry on short and long timescales.

ozone↗
NASA NTRS2009

Sensitivity of Photolysis Frequencies and Key Tropospheric Oxidants in a Global Model to Cloud Vertical Distributions and Optical Properties

Clouds affect tropospheric photochemistry through modification of solar radiation that determines photolysis frequencies. As a follow-up study to our recent assessment of the radiative effects of clouds on tropospheric chemistry, this paper presents an analysis of the sensitivity of such effects to cloud vertical distributions and optical properties (cloud optical depths (CODs) and cloud single scattering albedo), in a global 3-D chemical transport model (GEOS-Chem). GEOS-Chem was driven with a series of meteorological archives (GEOS1- STRAT, GEOS-3 and GEOS-4) generated by the NASA Goddard Earth Observing System data assimilation system. Clouds in GEOS1-STRAT and GEOS-3 have more similar vertical distributions (with substantially smaller CODs in GEOS1-STRAT) while those in GEOS-4 are optically much thinner in the tropical upper troposphere. We find that the radiative impact of clouds on global photolysis frequencies and hydroxyl radical (OH) is more sensitive to the vertical distribution of clouds than to the magnitude of column CODs. With random vertical overlap for clouds, the model calculated changes in global mean OH (J(O1D), J(NO2)) due to the radiative effects of clouds in June are about 0.0% (0.4%, 0.9%), 0.8% (1.7%, 3.1%), and 7.3% (4.1%, 6.0%), for GEOS1-STRAT, GEOS-3 and GEOS-4, respectively; the geographic distributions of these quantities show much larger changes, with maximum decrease in OH concentrations of approx.15-35% near the midlatitude surface. The much larger global impact of clouds in GEOS-4 reflects the fact that more solar radiation is able to penetrate through the optically thin upper-tropospheric clouds, increasing backscattering from low-level clouds. Model simulations with each of the three cloud distributions all show that the change in the global burden of ozone due to clouds is less than 5%. Model perturbation experiments with GEOS-3, where the magnitude of 3-D CODs are progressively varied from -100% to 100%, predict only modest changes (<5%) in global mean OH concentrations. J(O1D), J(NO2) and OH3 concentrations show the strongest sensitivity for small CODs and become insensitive at large CODs due to saturation effects. Caution should be exercised not to use in photochemical models a value for cloud single scattering albedo lower than about 0.999 in order to be consistent with the current knowledge of cloud absorption at the ultraviolet wavelengths.

Liu, Hongyu↗
DOE OSTI2022

Role of climate goals and clean-air policies on reducing future air pollution deaths in China: a modelling study

Over 3 million people still die every year from diseases caused by exposure to outdoor PM 2.5 air pollution, and more than a quarter of these premature deaths occur in China. In addition to clean air policies that target pollution emissions, climate policies aimed at reducing fossil-fuel CO 2 emissions (e.g., to avoid 1.5°C of warming) may also dramatically improve air quality and public health. Yet there has been no comprehensive accounting of public health outcomes under different energy pathways and local clean air management decisions in China. In particular, further research is needed to understand the relationships among climate and clean air polices and future health burdens in China, where an aging population will further exacerbate the impacts of air pollution. Using a China-focused integrated assessment model (GCAM-China) and a dynamic emission projection model (DPEC), we project future Chinese air quality in scenarios spanning a range of global climate targets (i.e. 1.5°0C, 2°C, NDC, unambitious, baseline, and 4.5°C) as well as national clean air actions (i.e. 2015-pollution, current-pollution, and ambitious-pollution). We then evaluate the health impacts of PM2·5 air pollution of scenario matrix using the chemical transport model WRF-CMAQ and the latest epidemiological concentration–response (C-R) functions (i.e. GBD2019). We find that, without ambitious climate mitigation (e.g., under current NDC pledges), Chinese deaths related the PM2.5 air pollution do not substantially decrease—and often grow—by mid-century, regardless of clean air policies and air quality improvements. For example, in scenarios that track China’s current NDC pledge and deploy best-available pollution control technologies, PM 2.5 -related deaths in China decrease slightly by 2030 (to 1.2 million per year) but no further by mid-century (Ambitious-pollution-NDC-goals; 1.2 million deaths in 2050) despite substantial and continuous improvements in population-weighted air quality (27.2 to 16.0 µg/m 3 from 2030 to 2050). The contrary trends of improving air quality and increasing PM 2·5 -related deaths in many of our scenarios reveals the extent to which extra efforts are needed to compensate for the established fact of increasing age of China’s population in future. Substantial decreases in China’s PM 2.5 -related deaths and age-standardized death rates (e.g., decreasing by 0.3–0.5 million deaths and 10.2–14.2 per 100,000 population age-standardized death rates per year) thus require the sort of large-scale transition in energy sources entailed by scenarios that meet international climate goals to avoid 1.5°C and 2°C of warming (Ambitious-pollution-2°C- and 1.5°C-goals).

58 GEOSCIENCES↗
NASA NTRS2014

Simultaneous Retrieval of Aerosol Properties and Clear-Sky Direct Radiative Effect Over the Global Ocean from MODIS

A unified satellite algorithm is presented to simultaneously retrieve aerosol properties (aerosol optical depth; AOD and aerosol type) and clear-sky shortwave direct radiative effect (hereafter, DREA) over ocean. The algorithm is applied to Moderate Resolution Imaging spectroradiometer (MODIS) observations for a period from 2003 to 2010 to assess the DREA over the global ocean. The simultaneous retrieval utilizes lookup table (LUT) containing both spectral reflectances and solar irradiances calculated using a single radiative transfer model with the same aerosol input data. This study finds that aerosols cool the top-of-atmosphere (TOA) and bottom-of-atmosphere (BOA) by 5.2 +/- 0.5 W/sq m and 8.3 W/sq m, respectively, and correspondingly warm the atmosphere (hereafter, ATM) by 3.1 W/sq m. These quantities, solely based on the MODIS observations, are consistent with those of previous studies incorporating chemical transport model simulations and satellite observations. However, the DREAs at BOA and ATM are expected to be less accurate compared to that of TOA due to low sensitivity in retrieving aerosol type information, which is related with the atmospheric heating by aerosols, particularly in low AOD conditions; consequently, the uncertainties could not be quantified. Despite the issue in the aerosol type information, the present method allows us to confine the DREA attributed only to fine-mode dominant aerosols, which are expected to be mostly anthropogenic origin, in the range from 1.1 W/sq m to 1.3 W/sq m at TOA. Improvements in size-resolved AOD and SSA retrievals from current and upcoming satellite instruments are suggested to better assess the DREA, particularly at BOA and ATM, where aerosol absorptivity induces substantial uncertainty.

MODIS↗
DOE OSTI2023

Contrasting changes in ozone during 2019–2021 between eastern and the other regions of China attributed to anthropogenic emissions and meteorological conditions

Ozone pollution is one of the most severe air quality issues in China that poses a serious threat to human health and ecosystems. During 2019–2021, the maximum daily 8-h average ozone concentrations in eastern China (110–122.5°E, 26–42°N) and the rest of China (ROC) show different decreasing patterns, with ozone concentrations in eastern China decreasing by 14.9 μg/m 3 , which is much larger than 4.8 μg/m 3 in ROC. Here, based on two independent methods, the atmospheric chemical transport model (GEOS-Chem) simulations and the machine learning (ML) model (LightGBM) predictions, the reasons for the differences in ozone changes between eastern China and ROC during the warm season (April to September) are investigated. According to the GEOS-Chem (LightGBM) results, changes in the meteorological conditions contributed to an ozone decrease by 7.3 (6.8) μg/m 3 in eastern China due to decreased chemical production and an ozone decrease by 6.8 (7.0) μg/m 3 in ROC attributed to the weakened horizontal and vertical advection. With the influence of meteorological factors excluded, the observations show that changes in anthropogenic emissions resulted in an ozone decrease by 7.6 (8.1) μg/m 3 in eastern China and an ozone increase by 2.0 (2.2) μg/m 3 in ROC, which is primarily induced by the changes in NO x emissions. The surface measurements and satellite retrievals also indicate that the reduction in NO x emissions in ROC is less efficient than that in the more developed eastern China, leading to contrasting changes in ozone concentrations between eastern China and ROC during 2019–2021. In conclusion, our results highlight the critical need to reduce ozone precursor emissions in the rest regions of China apart from eastern China.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2003

The 2002 Antarctic Ozone Hole

Since 1979, the ozone hole has grown from near zero size to over 24 Million km2. This area is most strongly controlled by levels of inorganic chlorine and bromine oncentrations. In addition, dynamical variations modulate the size of the ozone hole by either cooling or warming the polar vortex collar region. We will review the size observations, the size trends, and the interannual variability of the size. Using a simple trajectory model, we will demonstrate the sensitivity of the ozone hole to dynamical forcing, and we will use these observations to discuss the size of the ozone hole during the 2002 Austral spring. We will further show how the Cly decreases in the stratosphere will cause the ozone hole to decrease by 1-1.5% per year. We will also show results from a 3-D chemical transport model (CTM) that has been continuously run since 1999. These CTM results directly show how strong dynamics acts to reduce the size of the ozone hole.

Newman, P. A.↗
NASA NTRS2006

Formaldehyde Distribution over North America: Implications for Satellite Retrievals of Formaldehyde Columns and Isoprene Emission

Formaldehyde (HCHO) columns measured from space provide constraints on emissions of volatile organic compounds (VOCs). Quantitative interpretation requires characterization of errors in HCHO column retrievals and relating these columns to VOC emissions. Retrieval error is mainly in the air mass factor (AMF) which relates fitted backscattered radiances to vertical columns and requires external information on HCHO, aerosols, and clouds. Here we use aircraft data collected over North America and the Atlantic to determine the local relationships between HCHO columns and VOC emissions, calculate AMFs for HCHO retrievals, assess the errors in deriving AMFs with a chemical transport model (GEOS-Chem), and draw conclusions regarding space-based mapping of VOC emissions. We show that isoprene drives observed HCHO column variability over North America; HCHO column data from space can thus be used effectively as a proxy for isoprene emission. From observed HCHO and isoprene profiles we find an HCHO molar yield from isoprene oxidation of 1.6 +/- 0.5, consistent with current chemical mechanisms. Clouds are the primary error source in the AMF calculation; errors in the HCHO vertical profile and aerosols have comparatively little effect. The mean bias and 1Q uncertainty in the GEOS-Chem AMF calculation increase from <1% and 15% for clear skies to 17% and 24% for half-cloudy scenes. With fitting errors, this gives an overall 1 Q error in HCHO satellite measurements of 25-31%. Retrieval errors, combined with uncertainties in the HCHO yield from isoprene oxidation, result in a 40% (1sigma) error in inferring isoprene emissions from HCHO satellite measurements.

Millet, Dylan B.↗