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At least 271 records · Page 15

A14H-04 Analysis of Simulated and Observed Trends in Global Surface PM2.5 and Aerosol Optical Properties from 1958 to 2018 Using the NASA GEOSCCM

Modeling of long-term trends of aerosols and their properties is important for constraining aerosol-climate forcing, and for characterizing changes in particulate matter pollution speciation and exposure. Here we study global and regional long-term trends in surface fine particulate matter (PM ) and aerosol optical properties for 60 years from 1958 to 2018, using simulations performed with the NASA Goddard Earth Observing System Chemistry Climate Model (GEOSCCM), and evaluate the model hindcast with observations for the last three decades. Comparing the modeled aerosols with a diverse set of observations helps interpret observed and simulated trends, and serves as a benchmark for future GEOSCCM developments and input datasets improvements. We first characterize modeled global and regional temporal changes in surface PM and its components, aerosol optical depth (AOD) and single scattering albedo (SSA) and we interpret their link with emissions drivers. We then compare modeled surface PM with ground-based observations from monitoring networks and with global reconstructed PM datasets from observations-model data fusion. Total AOD is compared with long-term satellite measurements from the Moderate Resolution Imaging Spectroradiometer (MODIS) and measurements from the ground-based Aerosol Robotic Network (AERONET). Additional aerosol optical properties, such as absorption and scattering coefficients, are evaluated with ground-based observations from the Global Atmosphere Watch (GAW) records.

aerosols↗

Development of algorithms for using satellite meteorological data sets to study global transport of stratospheric aerosols and ozone

The utilization of stratospheric aerosol and ozone measurements obtained from the NASA developed SAM II and SAGE satellite instruments were investigated for their global scale transports. The stratospheric aerosols showed that during the stratospheric warming of the winter 1978 to 1979, the distribution of the zonal mean aerosol extinction ratio in the northern high latitude exhibited distinct changes. Dynamic processes might have played an important role in maintenance role in maintenance of this zonal mean distribution. As to the stratospheric ozone, large poleward ozone transports are shown to occur in the altitude region from 24 km to 38 km near 55N during this warming. This altitude region is shown to be a transition region of the phase relationship between ozone and temperature waves from an in-phase one above 38 km. It is shown that the ozone solar heating in the upper stratosphere might lead to enhancement of the damping rate of the planetary waves due to infrared radiation alone in agreement with theoretical analyses and an earlier observational study.

Want, P. H.↗

OCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) sea spray organic aerosol emissions – implementation in a global climate model and impacts on clouds

Sea spray aerosol is one of the major sources of atmospheric particulate matter globally. It has increasingly been recognized that organic matter derived from ocean biological precursors contributes significantly to the composition of submicron sea spray and may modify sea spray aerosol impacts on clouds and climate. This paper describes the implementation of the OCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) parameterization for sea spray organic aerosol emissions in a global Earth system model, the Energy Exascale Earth System Model (E3SM). OCEANFILMS is a physically based model that links sea spray chemistry with ocean biogeochemistry using a Langmuir partitioning approach. We describe the implementation details of OCEANFILMS within E3SM, compare simulated aerosol fields with observations, and investigate impacts on simulated clouds and climate. Four sensitivity cases are tested, in which organic emissions either strictly add to or strictly replace sea salt emissions (in mass and number) and are either fully internally or fully externally mixed with sea salt. The simulation with internally mixed, added organics agrees reasonably well with observed seasonal cycles of organic matter in marine aerosol and has been selected as the default configuration of the E3SM. In this configuration, sea spray organic aerosol contributes an additional source of cloud condensation nuclei, adding up to 30 cm -3 to Southern Ocean boundary-layer cloud condensation nuclei concentrations (supersaturation = 0.1 %). The addition of this new aerosol source strengthens shortwave radiative cooling by clouds by -0.36 W m -2 in the global annual mean and contributes more than -3.5 W m -2 to summertime zonal mean cloud forcing in the Southern Ocean, with maximum zonal mean impacts of about -4 W m -2 around 50–60°S. This is consistent with a previous top-down, satellite-based empirical estimate of the radiative forcing by sea spray organic aerosol over the Southern Ocean. Through its mechanistic approach, OCEANFILMS offers a path towards improved understanding of the feedbacks between ocean biology, sea spray organic matter, and climate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Global Assessment of OMI Aerosol Single-scattering Albedo Using Ground-based AERONET and SKYNET Inversions

We compare the aerosol single-scattering albedo (SSA) retrieved by the near-UV two-channel algorithm (OMAERUV) applied to the Aura-Ozone Monitoring Instrument (OMI) measurements with an equivalent inversion made by the ground-based Aerosol Robotic Network (AERONET). This work is the first comprehensive effort to globally compare the OMI-retrieved SSA with that of AERONET using all available sites spanning the regions of biomass burning, dust, and urban pollution. An analysis of the co-located retrievals over 269 sites reveals that about 46 percent (69 percent) of OMI-AERONET matchups agree within the absolute difference of plus or minus 0.03 (plus or minus 0.05) for all aerosol types. The comparison improves to 52 percent (77 percent) when only 'smoke' and 'dust' aerosol types were identified by the OMAERUV algorithm. Regionally, the agreement between the two inversions was robust over the biomass burning sites of South America, Sahel, Indian subcontinent, and oceanic-coastal sites followed by a reasonable agreement over north-east Asia. Over the desert regions, OMI tends to retrieve higher SSA, particularly over the Arabian Peninsula. Globally, the OMI-AERONET matchups agree mostly within plus or minus 0.03 for the aerosol optical depth (440 nanometers) and UV-aerosol index larger than 0.4 and 1.0, respectively. We also compare the OMAERUV SSA against the inversion made by an independent network of ground-based radiometer called SKYNET with its operating sites in Japan, China, South-East Asia, India, and Europe. The advantage of the SKYNET database over AERONET is that it performs retrieval at near-UV wavelengths which facilitate the direct comparison of OMI retrievals with the equivalent ground-based inversion. Comparison of OMI and SKYNET over currently available sites reveals a good agreement between the two where more than 70 percent of matchups agree within the absolute difference of 0.05.

Aerosol Single-scattering Albedo↗

Precipitable water vapor over oceans from the Maritime Aerosol Network: Evaluation of global models and satellite products under clear sky conditions

We present results from an evaluation of precipitable water vapor (W) over remote oceanic areas as derived from global reanalysis models and from satellites against observations from the Maritime Aerosol Network (MAN) for cloudless skies during the period of 2004–2017. They cover polar, mid latitude and tropical oceanic regions and represent a first effort to use MAN observations for such evaluation. The global reanalysis model products evaluated in this study are from the Modern-Era Retrospective analysis for Research and Applications Version 2 (MERRA-2), the European Centre for Medium-Range Weather Forecasts (ECMWF) Interim Reanalysis (ERA I), and the Climate Forecast System Reanalysis (CFSR) model. The satellite products evaluated are from the Moderate Resolution Imaging Spectroradiometer (MODIS), the Polarization and Directionality of the Earth's Reflectances (POLDER), the Global Ozone Monitoring Experiment (GOME-2), the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY), and the Atmospheric Infra-red Sounder (AIRS). Satellite retrievals of W are based on the attenuation of solar reflected light by water vapor absorption bands, except those from AIRS that rely on brightness temperature measurements. A very good agreement is observed between the model estimates and MAN, with mean differences of ~5% and standard deviations of ~15%. These results are within the uncertainties associated with the models and the measurements, indicating the skill of the reanalysis models to estimate W over oceans under clear sky conditions. Mean differences of W between the satellite and MAN products are ~11, 6.7, 12, −7, and 3% for MODIS, POLDER, GOME-2, SCIAMACHY and AIRS respectively, while their standard deviations are 31, 29, 28, 20 and 17%. These differences reveal the need to address inconsistencies among different satellite sensors and ground-based measurements to reduce the uncertainties associated with the retrievals.

Daniel Pérez-Ramírez↗

Assessing effective radiative forcing from aerosol–cloud interactions over the global ocean

How clouds respond to anthropogenic sulfate aerosols is one of the largest sources of uncertainty in the radiative forcing of climate over the industrial era. This uncertainty limits our ability to predict equilibrium climate sensitivity (ECS)—the equilibrium global warming following a doubling of atmospheric CO 2 . Here, we use satellite observations to quantify relationships between sulfate aerosols and low-level clouds while carefully controlling for meteorology. We then combine the relationships with estimates of the change in sulfate concentration since about 1850 to constrain the associated radiative forcing. We estimate that the cloud-mediated radiative forcing from anthropogenic sulfate aerosols is − 1.11 ± 0.43 W m −2 over the global ocean (95% confidence). This constraint implies that ECS is likely between 2.9 and 4.5 K (66% confidence). Our results indicate that aerosol forcing is less uncertain and ECS is probably larger than the ranges proposed by recent climate assessments.

54 ENVIRONMENTAL SCIENCES↗

Development and Evaluation of Chemistry‐Aerosol‐Climate Model CAM5‐Chem‐MAM7‐MOSAIC: Global Atmospheric Distribution and Radiative Effects of Nitrate Aerosol

Abstract An advanced aerosol treatment, with a focus on semivolatile nitrate formation, is introduced into the Community Atmosphere Model version 5 with interactive chemistry (CAM5‐chem) by coupling the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) with the 7‐mode Modal Aerosol Module (MAM7). An important feature of MOSAIC is dynamic partitioning of all condensable gases to the different fine and coarse mode aerosols, as governed by mode‐resolved thermodynamics and heterogeneous chemical reactions. Applied in the free‐running mode from 1995 to 2005 with prescribed historical climatological conditions, the model simulates global distributions of sulfate, nitrate, and ammonium in good agreement with observations and previous studies. Inclusion of nitrate resulted in ∼10% higher global average accumulation mode number concentrations, indicating enhanced growth of Aitken mode aerosols from nitrate formation. While the simulated accumulation mode nitrate burdens are high over the anthropogenic source regions, the sea‐salt and dust modes respectively constitute about 74% and 17% of the annual global average nitrate burden. Regional clear‐sky shortwave radiative cooling of up to −5 W m −2 due to nitrate is seen, with a much smaller global average cooling of −0.05 W m −2 . Significant enhancements in regional cloud condensation nuclei (at 0.1% supersaturation) and cloud droplet number concentrations are also attributed to nitrate, causing an additional global average shortwave cooling of −0.8 W m −2 . Taking into consideration of changes in both longwave and shortwave radiation under all‐sky conditions, the net change in the top of the atmosphere radiative fluxes induced by including nitrate aerosol is −0.7 W m −2 .

54 ENVIRONMENTAL SCIENCES↗

Assessed Using Satellite Data and Ground Based Sun/Sky Radiometers

The short aerosol lifetime and the variety of sources and atmospheric processes that affect the aerosol concentration and properties, generate a very heterogeneous aerosol field. Satellite data are needed to assess the daily global distribution of aerosol loading, properties and radiative forcing of climate. The Moderate Resolution Imaging Spectroradiometer (MODIS) instrument launched in July 1999 measures the aerosol properties and backscattered radiation in 7 spectral channels across the solar channel with spatial resolution of 500 m. Novel inversion techniques are used to derive the aerosol forcing at the top of the atmosphere in these 7 spectral bands with even higher accuracy than the derivation of the aerosol loading or microphysical properties. But satellites cannot sense the aerosol attenuation of radiation reaching the Earth surface. A network of 100 sun/sky radiometers, members of the AErosol RObotic NEtwork (AERONET) is used to assess, simultaneously, the radiative forcing of aerosol at the surface level. The relevance of MODIS and AERONET to assess the global aerosol forcing, and the inversion techniques will be presented and discussed.

Kaufman, Yoram J.↗

A Ten-Year Global Record of Absorbing Aerosols Above Clouds from OMI's Near-UV Observations

Aerosol-cloud interaction continues to be one of the leading uncertain components of climate models, primarily due to the lack of an adequate knowledge of the complex microphysical and radiative processes associated with the aerosol-cloud system. The situations when aerosols and clouds are found in the same atmospheric column, for instance, when light-absorbing aerosols such as biomass burning generated carbonaceous particles or wind-blown dust overlay low-level cloud decks, are commonly found over several regional of the world. Contrary to the cloud-free scenario over dark surface, for which aerosols are known to produce a net cooling effect (negative radiative forcing) on climate, the overlapping situation of absorbing aerosols over cloud can potentially exert a significant level of atmospheric absorption and produces a positive radiative forcing at top-of-atmosphere. The magnitude of direct radiative effects of aerosols above cloud depends directly on the aerosol loading, microphysical-optical properties of the aerosol layer and the underlying cloud deck, and geometric cloud fraction. We help in addressing this problem by introducing a novel product of optical depth of absorbing aerosols above clouds retrieved from near-UV observations made by the Ozone Monitoring Instrument (OMI) on board NASA's Aura platform. The presence of absorbing aerosols above cloud reduces the upwelling radiation reflected by cloud and produces a strong 'color ratio' effect in the near-UV region, which can be unambiguously detected in the OMI measurements. Physically based on this effect, the OMACA algorithm retrieves the optical depths of aerosols and clouds simultaneously under a prescribed state of atmosphere. The algorithm architecture and results from a ten-year global record including global climatology of frequency of occurrence and above-cloud aerosol optical depth, and a discussion on related future field campaigns are presented.

Ozone Monitoring Instrument↗

Atmospheric Teleconnection over Eurasia Induced by Aerosol Radiative Forcing during Boreal Spring

The direct effects of aerosols on global and regional climate during boreal spring are investigated based on numerical simulations with the NASA Global Modeling and Assimilation Office finite-volume general circulation model (fvGCM) with Microphyics of Clouds with the Relaxed Arakawa Schubert Scheme (McRAS), using aerosol forcing functions derived from the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The authors find that anomalous atmospheric heat sources induced by absorbing aerosols (dust and black carbon) excite a planetary-scale teleconnection pattern in sea level pressure, temperature, and geopotential height spanning North Africa through Eurasia to the North Pacific. Surface cooling due to direct effects of aerosols is found in the vicinity and downstream of the aerosol source regions, that is, South Asia, East Asia, and northern and western Africa. Significant atmospheric heating is found in regions with large loading of dust (over northern Africa and the Middle East) and black carbon (over Southeast Asia). Paradoxically, the most pronounced feature in aerosol-induced surface temperature is an east west dipole anomaly with strong cooling over the Caspian Sea and warming over central and northeastern Asia, where aerosol concentrations are low. Analyses of circulation anomalies show that the dipole anomaly is a part of an atmospheric teleconnection pattern driven by atmospheric heating anomalies induced by absorbing aerosols in the source regions, but the influence was conveyed globally through barotropic energy dispersion and sustained by feedback processes associated with the regional circulations. The surface temperature signature associated with the aerosol-induced teleconnection bears striking resemblance to the spatial pattern of observed long-term trend in surface temperature over Eurasia. Additionally, the boreal spring wave train pattern is similar to that reported by Fukutomi et al. associated with the boreal summer precipitation seesaw between eastern and western Siberia. The results of this study raise the possibility that global aerosol forcing during boreal spring may play an important role in spawning atmospheric teleconnections that affect regional and global climates.

Kim, Maeng-Ki↗

Transport and residence times of tropospheric aerosols inferred from a global three-dimensional simulation of Pb-210

A global three-dimensional model is used to investigate the transport and tropospheric residence time of Pb-210, an aerosol tracer produced in the atmosphere by radioactive decay of Rn-222 emitted from soils. The model uses meteorological input with 4 deg x 5 deg horizontal resolution and 4-hour temporal resolution from the Goddard Institute for Space Studies general circulation model (GCM). It computes aerosol scavenging by convective precipitation as part of the wet convective mass transport operator in order to capture the coupling between vertical transport and rainout. Scavenging in convective precipitation accounts for 74% of the global Pb-210 sink in the model; scavenging in large-scale precipitation accounts for 12%, and scavenging in dry deposition accounts for 14%. The model captures 63% of the variance of yearly mean Pb-210 concentrations measured at 85 sites around the world with negligible mean bias, lending support to the computation of aerosol scavenging. There are, however, a number of regional and seasonal discrepancies that reflect in part anomalies in GCM precipitation. Computed residence times with respect to deposition for Pb-210 aerosol in the tropospheric column are about 5 days at southern midlatitudes and 10-15 days in the tropics; values at northern midlatitudes vary from about 5 days in winter to 10 days in summer. The residence time of Pb-210 produced in the lowest 0.5 km of atmosphere is on average four times shorter than that of Pb-210 produced in the upper atmosphere. Both model and observations indicate a weaker decrease of Pb-210 concentrations between the continental mixed layer and the free troposphere than is observed for total aerosol concentrations; an explanation is that Rn-222 is transported to high altitudes in wet convective updrafts, while aerosols and soluble precursors of aerosols are scavenged by precipitation in the updrafts. Thus Pb-210 is not simply a tracer of aerosols produced in the continental boundary layer, but also of aerosols derived from insoluble precursors emitted from the surface of continents. One may draw an analogy between Pb-210 and nitrate, whose precursor NO(sub x) is sparingly soluble, and explain in this manner the strong correlation observed between nitrate and Pb-210 concentrations over the oceans.

Balkanski, Yves J.↗

Global organic and inorganic aerosol hygroscopicity and its effect on radiative forcing

The climate effects of atmospheric aerosol particles serving as cloud condensation nuclei (CCN) depend on chemical composition and hygroscopicity, which are highly variable on spatial and temporal scales. Here we present global CCN measurements, covering diverse environments from pristine to highly polluted conditions. We show that the effective aerosol hygroscopicity, κ, can be derived accurately from the fine aerosol mass fractions of organic particulate matter (ϵ org ) and inorganic ions (ϵ inorg ) through a linear combination, κ = ϵ org · κ org + ϵ inorg · κ inorg . In spite of the chemical complexity of organic matter, its hygroscopicity is well captured and represented by a global average value of κ org = 0.12 ± 0.02 with κinorg = 0.63 ± 0.01 as the corresponding value for inorganic ions. By showing that the sensitivity of global climate forcing to changes in κ org and κ inorg is small, we constrain a critically important aspect of global climate modelling.

54 ENVIRONMENTAL SCIENCES↗

Global Influence of Organic Aerosol Volatility on Aerosol Microphysical Processes: Composition and Number

We present MATRIX-VBS, a new aerosol scheme that simulates organic partitioning in an aerosol microphysics model, as part of the NASA GISS ModelE Earth System Model. MATRIX-VBS builds on its predecessor aerosol microphysics model MATRIX (Bauer et al., 2008, https://doi.org/10.5194/acp-8-6003-2008) and was developed in the box model framework (Gao et al., 2017, https://doi.org/10.5194/gmd-10-751-2017). The scheme features the inclusion of organic partitioning between the gas and particle phases and the photochemical aging process using the volatility-basis set (Donahue et al., 2006, https://doi.org/10.1021/es052297c). To assess the performance of the new model, we compared its mass concentration, number concentration, and activated number concentration to the original scheme MATRIX, and evaluated its mass concentrations in four seasons against data from the NASA Atmospheric Tomography Mission (ATom) aircraft campaign. Results from MATRIX-VBS show that organics are transported further away from their source, and their mass concentration increases aloft and decreases at the surface compared to those in MATRIX. The mass concentration of organics at the surface agrees well with measurements, and there are discrepancies for vertical profiles aloft. In the new scheme, the global mass load of organic aerosols increased by 50%, there is also an increased number of particles at the surface and fewer activated ones in most regions. The new scheme presents advanced and more comprehensive capability in simulating aerosol processes.

aerosol modeling↗

Global sensing of gaseous and aerosol trace species using automated instrumentation on 747 airliners

The Global Atmospheric Sampling Program (GASP) is collecting and analyzing data on gaseous and aerosol trace contaminants in the upper troposphere and lower stratosphere. Measurements are obtained from automated systems installed on four 747 airliners flying global air routes. Improved instruments and analysis techniques are providing an expanding data base for trace species including ozone, carbon monoxide, water vapor, condensation nuclei, and mass concentration of sulfates and nitrates. Simultaneous measurements of several trace species obtained frequently can be used to identify the source of the air mass as being typically tropospheric or stratospheric.

Perkins, P. J.↗

Global sensing of gaseous and aerosol trace species using automated instrumentation on 747 airliners

The Global Atmospheric Sampling Program (GASP) by NASA is collecting and analyzing data on gaseous and aerosol trace species in the upper troposphere and lower stratosphere. Measurements are obtained from automated systems installed on four 747 airliners flying global air routes. Advances were made in airborne sampling instrumentation. Improved instruments and analysis techniques are providing an expanding data base for trace species including ozone, carbon monoxide, water vapor, condensation nuclei and mass concentrations of sulfates and nitrates. Simultaneous measurements of several trace species obtained frequently can be used to uniquely identify the source of the air mass as being typically tropospheric or stratospheric. A quantitative understanding of the tropospheric-stratospheric exchange processes leads to better knowledge of the atmospheric impact of pollution through the development of improved simulation models of the atmosphere.

Perkins, P. J.↗

Climatic effects of atmospheric aerosols

It is shown quantitatively how radiative climatic forcing by aerosols depends on the physical properties of the aerosols. The special case of atmospheric aerosols produced by volcanic explosions is considered, and evidence is presented which indicates that even the simple climate models available today may be able to capture some of the basic effects of aerosols on global climate. Possible effects of anthropogenic aerosols are briefly examined. It is noted that additional evidence for the significant influence of aerosols on climate may be found in data obtained from recent spacecraft missions to Venus and Mars.

Hansen, J. E.↗

Balloon-borne observation of Aitken nuclei in the Antarctic stratosphere and troposphere

Aitken nuclei (0.002 or = r or = 0.1 microns in the atmosphere are produced through gas-to-particle conversion processes, and they grow in size by heterogeneous nucleation processes and others to produce larger aerosol particles. In the study of global background aerosol pollution, full knowledge of such aerosol processes in the clean atmosphere is essentially required. In this sense, it is important to examine the behavior of aerosols in a clean atmosphere which is not contaminated directly by aerosols and gases emitted from the Earth's surface. The Antarctic atmosphere is thought to be such a clean atmosphere. From an extensive surface observation of aerosols carried out at Syowa Station (69 deg 00'S, 39 deg 35'E) Antarctica, it has been revealed that various phenomena relating to long-range transport of trace constituents and/or photochemical processes resulting in production or growth of aerosol particles are clearly observed in Antarctica. This paper gives a preliminary report of observations made by balloon-borne Aitken nuclei sonde in 1983, at Syowa Station.

Ito, T.↗

The application of lidar to stratospheric aerosol studies

The global climatology and understanding of stratospheric aerosols evolving primarily from lidar and satellite measurements is presented. The importance of validation of these remotely sensed data with in situ measurements is also discussed. The advantage of lidar for providing high vertical and horizontal resolution and its independence from a remote source for measurement will become evident with examples of long term lidar data sets at fixed sites and the use of lidar on airborne platforms. Volcanic impacts of the last 20 years are described with emphasis on the last 8 years where satellite data are available. With satellite and high resolution lidar measurements, an understanding of the global circulation of volcanic material is attempted along with the temporal change of aerosol physical parameters and the stratospheric cleansing or decay times associated with these eruptions.

Mccormick, M. P.↗