The spectral color of natural and anthropogenic time series and its impact on the statistical significance of cross correlation
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We present here a first global modeling study on the influence of gas-phase chemistry/aerosol interactions on estimates of anthropogenic forcing by tropospheric O3 and aerosols. Concentrations of gas-phase species and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols in the preindustrial, present-day, and year 2100 (IPCC SRES A2) atmospheres are simulated online in the Goddard Institute for Space Studies general circulation model II' (GISS GCM II'). With fully coupled chemistry and aerosols, the preindustrial, presentday, and year 2100 global burdens of tropospheric ozone are predicted to be 190, 319, and 519 Tg, respectively. The burdens of sulfate, nitrate, black carbon, and organic carbon are predicted respectively to be 0.32. 0.18, 0.01, 0.33 Tg in preindustrial time, 1.40, 0.48, 0.23, 1.60 Tg in presentday, and 1.37, 1.97, 0.54, 3.31 Tg in year 2100. Anthropogenic O3 is predicted to have a globally and annually averaged present-day forcing of +0.22 W m(sup -2) and year 2100 forcing of +0.57 W m(sup -2) at the top of the atmosphere (TOA). Net anthropogenic TOA forcing by internally mixed sulfate, nitrate, organic carbon, and black carbon aerosols is estimated to be virtually zero in the present-day and +0.34 W m(sup -2) in year 2100, whereas it is predicted to be -0.39 W m(sup -2) in present-day and -0.61 W m(sup -2) in year 2100 if the aerosols are externally mixed. Heterogeneous reactions are shown to be important in affecting anthropogenic forcing. When reactions of N2O5, NO3, NO2, and HO2 on aerosols are accounted for, TOA anthropogenic O3 forcing is less by 20-45% in present-day and by 20-32% in year 2100 at mid to high latitudes in the Northern Hemisphere, as compared with values predicted in the absence of heterogeneous gas aerosol reactions. Mineral dust uptake of HNO3 and O3 is shown to have practically no influence on anthropogenic O3 forcing. Heterogeneous reactions of N2Os, NO3, NO2, and HO2 are predicted to have noticeable impacts on anthropogenic aerosol forcing over industrialized areas, leading to 0-2 W m(sup -2) more anthropogenic aerosol cooling in present-day and 2-8 W m(sup -2) more cooling in year 2100 in these areas as compared with forcings calculated in the absence of heterogeneous reactions. Sea salt uptake of SO2 reduces the magnitude of TOA aerosol cooling by 0.5-1 W m(sup -2) over the oceans around 60 N in the present-day and year 2100 scenarios. Near dust sources, mineral dust uptake of SO2 and HNO3 leads to less anthropogenic aerosol cooling by 0.5-1 W m(sup -2) in the present day and 1-2 W m(sup -2) in year 2100.
Daytime heat is often associated with reduced soil moisture and cloud cover, while nighttime heat is connected to high humidity and increased cloud cover. Due to these differing mechanisms, compound daytime and nighttime heat events may respond differently to major anthropogenic forcings (greenhouse gases, anthropogenic aerosols, land-use and land-cover change). Here, we use GISS ModelE2.1-G historical single-forcing runs from 1955 to 2014 to examine how individual anthropogenic forcings affect compound heat events—specifically warm daytime and nighttime temperatures compounded with dry precipitation or high humidity conditions. We show that greenhouse gases alone amplify the natural frequency of warm-dry events by 1.5–5 times and warm-humid events by 2–9 times in tropical and extratropical latitudes. Conversely, aerosols and land-use/land-cover change reduce the frequency of these events, resulting in more modest increases and in some regions, declines, in the historical 'all-forcings' scenario. Individually, aerosol effects are stronger and more widespread compared to land-use, oftentimes reducing the natural frequency of these events by 60%–100%. The responses of these compound events are primarily driven by changes in daytime and nighttime temperatures through large-scale warming via greenhouse gases and cooling from aerosols and land-use/land-cover change. However, changes in warm-dry events are amplified in regions with concurrent precipitation declines (e.g. Central America, Mediterranean regions) and warm-humid events are amplified by global concurrent humidity increases. Additionally, we find differences between daytime and nighttime compound responses in the historical experiment that can be traced back to the individual forcings. In particular, aerosols produce a greater cooling effect on daytime relative to nighttime temperatures, which notably results in a historical reduction of Northern Hemisphere daytime warm-dry events relative to natural conditions. Our analysis provides a more comprehensive understanding of the significant impacts of different anthropogenic climate forcings on daytime and nighttime warm-dry and warm-humid events, informing future risk and impact assessments.
The unintended consequences of reductions in regional anthropogenic sulfur dioxide (SO2) emissions implemented to protect human health are poorly understood. SO2 decreases began in the 1970s in the US and Europe and are expected to continue into the future, while recent emissions decreases in China are also projected to continue. In addition to the well-documented climate effects (warming) from reducing aerosols, tropospheric oxidation is impacted via aerosol modification of photolysis rates and radical sinks. Impacts on the hydroxyl radical and other trace constituents directly affect climate and air quality metrics such as surface ozone levels. We use the Geophysical Fluid Dynamics Laboratory Atmospheric Model version 3 nudged towards National Centers for Environmental Prediction (NCEP) reanalysis wind velocities to estimate the impact of SO2 emissions from the US, Europe, and China by differencing a control simulation with an otherwise identical simulation in which 2015 anthropogenic SO2 emissions are set to zero over one of the regions. Springtime sulfate aerosol changes occur both locally to the emission region and also throughout the Northern Hemispheric troposphere, including remote oceanic regions and the Arctic. Hydroperoxy (HO2) radicals are directly removed via heterogeneous chemistry on aerosol surfaces, including sulfate, in the model, and we find that sulfate aerosol produced by SO2 emissions from the three individual northern mid-latitude regions strongly reduces both HO2 and hydroxyl (OH) by up to 10 % year-round throughout most of the troposphere north of 30∘ N latitude. Regional SO2 emissions significantly increase nitrogen oxides (NOx) by about 5 %–8 % throughout most of the free troposphere in the Northern Hemisphere by increasing the NOx lifetime as the heterogeneous sink of HO2 on sulfate aerosol declines. Despite the NOx increases, tropospheric ozone decreases at northern mid-latitudes by 1 %–4 % zonally averaged and by up to 5 ppbv in summertime surface air over China, where the decreases in HO2 and OH suppress O3 production. Since 2015 anthropogenic SO2 emissions in China exceed those in the US or Europe, the oxidative response is greatest for the China perturbation simulation. Chemical effects of aerosols on oxidation (reactive uptake) dominate over radiative effects (photolysis rates), the latter of which are only statistically significant locally for the large perturbation over China. We find that the SO2 emissions decrease in China, which has yet to be fully realized, will have the largest impact on oxidants and related species in the Northern Hemisphere free troposphere compared to future decreases in Europe or the US. Our results bolster previous calls for a multipollutant strategy for air pollution mitigation to avoid the unintended consequence of aerosol removal leading to surface ozone increases that offset or mask surface ozone gains achieved by regulation of other pollutants, especially in countries where current usage of high-sulfur emitting fuels may be phased out in the future.
The UNH investigation during TRACE-P provided measurements of selected acidic gases and aerosol species aboard the NASA DC-8 research aircraft. Our investigation focused on measuring HNO3, SO2, and fine (less than 2 microns) aerosol SO4(sup 2-) with two minute time resolution in near-real-time. We also quantified mixing ratios of aerosol ionic species, and aerosol (210)Pb and (7)Be collected onto bulk filters at better than 10 minute resolution. This suite of measurements contributed extensively to achieving the principal objectives of TRACE-P. In the context of the full data set collected by experimental teams on the DC-8, our observations provide a solid basis for assessing decadal changes in the chemical composition and source strength of Asian continental outflow. This region of the Pacific should be impacted profoundly by Asian emissions at this time with significant degradation of air quality over the next few decades. Atmospheric measurements in the western Pacific region will provide a valuable time series to help quantify the impact of Asian anthropogenic activities. Our data also provide important insight into the chemical and physical processes transforming Asian outflow during transport over the Pacific, particularly uptake and reactions of soluble gases on aerosol particles. In addition, the TRACE-P data set provide strong constraints for assessing and improving the chemical fields simulated by chemical transport models.
Ozone fields simulated for the first phase of the Chemistry-Climate Model Initiative (CCMI-1) will be used as forcing data in the 6th Coupled Model Intercomparison Project. Here we assess, using reference and sensitivity simulations produced for CCMI-1, the suitability of CCMI-1 model results for this process, investigating the degree of consistency amongst models regarding their responses to variations in individual forcings. We consider the influences of methane, nitrous oxide, a combination of chlorinated or brominated ozone-depleting substances, and a combination of carbon dioxide and other greenhouse gases. We find varying degrees of consistency in the models' responses in ozone to these individual forcings, including some considerable disagreement. In particular, the response of total-column ozone to these forcings is less consistent across the multi-model ensemble than profile comparisons. We analyse how stratospheric age of air, a commonly used diagnostic of stratospheric transport, responds to the forcings. For this diagnostic we find some salient differences in model behaviour, which may explain some of the findings for ozone. The findings imply that the ozone fields derived from CCMI-1 are subject to considerable uncertainties regarding the impacts of these anthropogenic forcings. We offer some thoughts on how to best approach the problem of generating a consensus ozone database from a multi-model ensemble such as CCMI-1.
Future climate change may bring local benefits or penalties to surface ozone pollution, resulting from changing temperature, precipitation, and transport patterns, as well as climate-sensitive natural precursor emissions. Here, we estimate climate penalty and benefits at the end of this century using version 2.0 of the Global Change and Air Pollution (GCAP 2.0) model framework, a one-way offline coupling between version E2.1 of the NASA Goddard Institute for Space Studies (GISS) general circulation model (GCM) and the GEOS-Chem global 3-D chemical-transport model (CTM). We archive meteorology for driving GEOS-Chem from the E2.1 contributions to Phase 6 of the Coupled Model Intercomparison Project (CMIP6) for the present day (2005-2014 C.E.) and end-of-the 21st century (2090-2099 C.E.). Emissions and boundary conditions used for input to GEOS-Chem are consistent with the CMIP6 experimental design. We apply the model to isolate the impact of forecasted anthropogenic precursor emission changes versus climate-only driven changes on surface ozone for warming limited to 1.9 W m-2 versus 8.5 W m-2 above preindustrial levels. We find a global climate penalty of 47 (16-77) thousand additional deaths due to surface ozone at the end of the century in the extreme warming scenario, but only 13 (4-21) thousand additional deaths in the extreme mitigation scenario. Similarly, the extreme warming scenario is associated with a 40 % increase in economic losses due to crop damage from climate-only changes in surface ozone, but only an 8 % increase in the extreme mitigation scenario. The simulated climate penalties to surface ozone are most severe in South and East Asia.
Accurate representation of vegetation states is required for the modeling of terrestrial water-energy-carbon exchanges and the characterization of the impacts of natural and anthropogenic vegetation changes on the land surface. This study presents a comprehensive evaluation of the impact of assimilating remote sensing-based Leaf Area Index (LAI) retrievals over the Continental U.S. in the Noah-MP land surface model, during a time period of 2000 to 2017. The results demonstrate that the assimilation has a beneficial impact on the simulation of key water budget terms such as soil moisture, evapotranspiration, snow depth, terrestrial water storage and streamflow, when compared with a large suite of reference datasets. In addition, the assimilation of LAI is also found to improve the carbon fluxes of Gross Primary Production (GPP) and Net Ecosystem Exchange (NEE). Most prominent improvements in the water and carbon variables are observed over the agricultural areas of the U.S., where assimilation improves the representation of vegetation seasonality impacted by cropping schedules. The systematic, added improvements from assimilation in a configuration that employs high quality boundary conditions highlight the significant utility of LAI data assimilation in capturing the impacts of vegetation changes.
In this study, we examine seasonal and geographical variability of marine aerosol fine-mode fraction (f(sub m)) and its impacts on deriving the anthropogenic component of aerosol optical depth (tau(sub a)) and direct radiative forcing from multispectral satellite measurements. A proxy of f(sub m), empirically derived from the Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 5 data, shows large seasonal and geographical variations that are consistent with the Goddard Chemistry Aerosol Radiation Transport (GOCART) and Global Modeling Initiative (GMI) model simulations. The so-derived seasonally and spatially varying f(sub m) is then implemented into a method of estimating tau(sub a) and direct radiative forcing from the MODIS measurements. It is found that the use of a constant value for fm as in previous studies would have overestimated Ta by about 20% over global ocean, with the overestimation up to 45% in some regions and seasons. The 7-year (2001-2007) global ocean average tau(sub a) is 0.035, with yearly average ranging from 0.031 to 0.039. Future improvement in measurements is needed to better separate anthropogenic aerosol from natural ones and to narrow down the wide range of aerosol direct radiative forcing.
The impact of natural and anthropogenic sources of aerosols has gained increasing attention from scientific communities in recent years. Indeed, tropospheric aerosols not only perturb radiative energy balance by interacting with solar and terrestrial radiation, but also by changing cloud properties and lifetime. Furthermore, these anthropogenic and natural air particles, once generated over the source regions, can be transported out of the boundary layer into the free troposphere and can travel thousands of kilometers across oceans and continents resulting in important biogeochemical impacts on the ecosystem. With the launch of SeaWiFS in 1997, Terra/MODIS in 1999, and Aqua/MODIS in 2002, high quality comprehensive aerosol climatology is becoming feasible for the first time. As a result of these unprecedented data records, studies of the radiative and biogeochemical effects due to tropospheric aerosols are now possible. In this talk, we will demonstrate how this newly available SeaWiFS/MODIS aerosol climatology can provide an important piece of puzzles in reducing the uncertainty of estimated climatic forcing due to aerosols. We will start with the global distribution of aerosol loading and their variabilities over both land and ocean on short- and long-term temporal scales observed over the last decade. The recent progress made in Deep Blue aerosol algorithm on improving accuracy of these Sea WiFS / MODIS aerosol products in particular over land will be discussed. The impacts on quantifying physical and optical processes of aerosols over source regions of adding the Deep Blue products of aerosol properties over bright-reflecting surfaces into Sea WiFS / MODIS as well as VIIRS data suite will also be addressed. We will also show the intercomparison results of SeaWiFS/MODIS retrieved aerosol optical thickness with data from ground based AERONET sunphotometers over land and ocean as well as with other satellite measurements. The trends observed in global aerosol loadings of both natural and anthropogenic sources based upon more than a decade of combined MODIS/SeaWiFS data (1997-2011) will be discussed. We will also address the importance of various key issues such as differences in spatial-temporal sampling rates and observation time between different satellite measurements could potentially impact these intercomparisons results, especially for using the monthly mean data, and thus on estimates of long-term aerosol trends.
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This study evaluates source attribution of ozone (O3) in the southeast US within O3 lamina observed by the University of Alabama in Huntsville (UAH) Tropospheric Ozone Lidar Network (TOLNet) system during June 2013. This research applies surface-level and airborne in situ data and chemical transport model, GEOS-Chem, simulations in order to quantify the impact of North American anthropogenic emissions, wildfires, lightning NOx, and background stratospheric transport on the observed O3 lamina. During the summer of 2013, two anomalous O3 layers were observed and evaluated: 1) a nocturnal near-surface enhancement and 2) a late evening elevated (3-6 km above ground level) O3 plume. A "brute force" zeroing method was applied in GEOS-Chem to quantify the impact of individual emission sources and transport pathways on the vertical distribution of O3 during the two observed lamina. These model simulations suggest that the nocturnal O3 enhancement on June 12, 2013 below 3 km was primarily due to wildfire emissions and the fact that daily maximum anthropogenic emission contributions occurred during these night-time hours. During the second case study it was predicted that above average contributions from background stratospheric transport was largely contributing to the O3 lamina observed on June 29, 2013 between 3-6 km. Further evaluation suggested that a stratospheric intrusion was likely the main source contributing to this O3 enhancement between 3-6 km. Supporting information from other models, remote-sensing observations, and ground-based airborne in situ data agree with the source attribution predicted by GEOS-Chem simulations for both case studies. Overall, this study demonstrates the dynamic atmospheric chemistry occurring in the southeast US and displays the various emission sources and transport processes impacting O3 enhancements at different vertical levels of the troposphere.
The impact of natural and anthropogenic sources of mineral dust has gained increasing attention from scientific communities in recent years. Indeed, these airborne dust particles, once lifted over the source regions, can be transported out of the boundary layer into the free troposphere and can travel thousands of kilometers across the oceans resulting in important biogeochemical impacts on the ecosystem. Due to the relatively short lifetime (a few hours to about a week), the distributions of these mineral dust particles vary extensively in both space and time. Consequently, satellite observations are needed over both source and sink regions for continuous temporal and spatial sampling of aerosol properties. With the launch of SeaWiFS in 1997, Terra/MODIS in 1999, and Aqua/MODIS in 2002, high quality comprehensive aerosol climatology is becoming feasible for the first time. As a result of these unprecedented satellite data records, studies of the radiative and biogeochemical effects due to dust aerosols are now possible. In this study, we will show the comparisons of satellite retrieved aerosol optical thickness using Deep Blue algorithm with data from AERONET sunphotometers over desert and semi-desert regions as well as vegetated areas. Our results indicate reasonable agreements between these two. These new satellite products will allow scientists to determine quantitatively the aerosol properties near sources using high spatial resolution measurements from Sea WiFS and MODIS-like instruments. The multiyear satellite measurements since 1997 from Sea WiFS will be compared with those retrieved from MODIS and MISR, and will be utilized to investigate the interannual variability of source, pathway, and dust loading associated with the dust outbreaks over the entire globe. Finally, the trends observed over the last decade based upon the SeaWiFS time series in the amounts of tropospheric aerosols due to natural and anthropogenic sources (such as changes in the frequency of dust storms) will be discussed.
This project involved the design and construction of a new instrument for airborne measurement of DMS and SO2. The instrument is intended for use on field missions to study the global atmospheric sulfur cycle. The ultimate scientific goal is to provide insight into the mechanisms of atmospheric transport and transformations impacting both natural and anthropogenic sulfur emissions. This report summarizes the progress made to date and the goals for future work on the project. The PI's for this project have recently relocated from the University of Miami to the University of California, Irvine, and a request has been made to transfer remaining funds to UCI. All equipment associated with this project has been transferred to UCI. The instrument design goal was to develop an instrument roughly one quarter the size and weight of currently available airborne instrumentation used for DMS and S02 measurements. Another goal was full automation, to allow unattended operation for the duration of a P-3 or DC-8 flight. The original performance design specifications for the instrument are given.
Evidence-based responses to climate change by society require operational and sustained information including biophysical indicator systems that provide up-to-date measures of trends and patterns against historical baselines. Two key components linking anthropogenic climate change to impacts on socio-ecological systems are the periodic inter- and intra-annual variations in physical climate systems (seasonality) and in plant and animal life cycles (phenology). We describe a set of national indicators that reflect sub-seasonal to seasonal drivers and responses of terrestrial physical and biological systems to climate change and variability at the national scale. Proposed indicators and metrics include seasonality of surface climate conditions (e.g., frost and freeze dates and durations), seasonality of freeze/thaw in freshwater systems (e.g., timing of stream runoff and durations of lake/river ice), seasonality in ecosystem disturbances (e.g., wildfire season timing and duration), seasonality in vegetated land surfaces (e.g., green-up and brown-down of landscapes), and seasonality of organismal life-history stages (e.g., timings of bird migration). Recommended indicators have strong linkages to variable and changing climates, include abiotic and biotic responses and feedback mechanisms, and are sufficiently simple to facilitate communication to broad audiences and stakeholders interested in understanding and adapting to climate change.
Precipitation has increased across the arid Central Asia region over recent decades. However, the underlying mechanisms of this trend are poorly understood. Here, we analyze multi-model simulations from the Precipitation Driver and Response Model Intercomparison Project (PDRMIP) to investigate potential drivers of the observed precipitation trend. We find that anthropogenic sulfate aerosols over remote polluted regions in South and East Asia lead to increased summer precipitation, especially convective and extreme precipitation, in arid Central Asia. Elevated concentrations of sulfate aerosols over remote polluted Asia cause an equatorward shift of the Asian Westerly Jet Stream through a fast response to cooling of the local atmosphere at mid-latitudes. This shift favours moisture supply from low-latitudes and moisture flux convergence over arid Central Asia, which is confirmed by a moisture budget analysis. High levels of absorbing black carbon lead to opposing changes in the Asian Westerly Jet Stream and reduced local precipitation, which can mask the impact of sulfate aerosols. This teleconnection between arid Central Asia precipitation and anthropogenic aerosols in remote Asian polluted regions highlights long-range impacts of anthropogenic aerosols on atmospheric circulations and the hydrological cycle.
The societal impacts of climate change during the late Holocene leads to regional anthropogenic changes over the Nile region floodplain and could have acted in tandem with natural factors like major volcanic eruptions on the regional climate system to magnify the local climatic impacts. This study aims to explore and investigate the sensitivity of climatic changes to the regional anthropogenic changes due to various factors over the Nile river floodplains during the late-Holocene (2.5K years before present). The GISS ModelE Earth system model will be used to simulate the various scenarios of regional increasing/decreasing river fraction, changes in vegetation type and cover, along with changes in land surface type against the no-changes scenario in absence of volcanic eruptions. The spatial coverage of the Nile river basin is estimated using the GIS shapefile based on elevation data from Shuttle Radar Topography Mission (SRTM) at 3 Arc-seconds (approx. 90-meter) horizontal resolution. The extent of flooding in the model grid (2.0°x2.5° in latitude and longitude) is estimated using the existing high-resolution (0.125°x0.125°) gridded topographic elevation information and mapped over the Nile river floodplains. This study also focuses on evaluating the NASA GISS ModelE for resolving the climate feedbacks and response on climate system due to anthropogenic changes and volcanic eruptions. It is also aimed to analyze and quantify the impact of various anthropogenic factors over the African monsoon system and rainfall over the region, which feeds the Nile River.
This study develops a new approach to improve simulations of the particulate matter of aerodynamic diameter smaller than 2.5μm (PM2.5) in the Community Multiscale Air Quality (CMAQ) model via assimilation of Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth(AOD) retrievals using the Grid point Statistical Interpolation (GSI) system. In contrast to previous studies that only consider errors due to transport, our computation of the background error covariance matrix incorporates uncertainties in anthropogenic emissions. To understand the impact of this approach, three experiments (one background and two assimilations) are performed over the contiguous United States(CONUS) from 15 July to 14 August 2014. The background CMAQ experiment significantly underestimates both the MODIS AOD and surface PM2.5levels. MODIS AOD assimilation pushes both the CMAQ AOD and surface PM2.5distributions toward the observed distributions, but CMAQ still underestimates the observations. Averaged over CONUS, the two assimilation experiments with and without including the anthropogenic emission uncertainties improve the correlation coefficient between the model and independent observations of PM2.5 by ~67% and ~48%, respectively, and reduces the mean bias by ~38% and~10%, respectively. The assimilation improves the model performance everywhere over CONUS, except the New York and Wisconsin, where CMAQ overestimates the observed PM2.5during nighttime after assimilation likely because of overcorrection of aerosol mass concentrations by the AOD assimilation. Future work should incorporate uncertainties in other processes (biomass burning and biogenic emissions, deposition, chemistry, transport, and boundary conditions) to further enhance the value of assimilating spaceborne AOD retrievals.