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NASA NTRS2016

Spaceborne Remote Sensing of Aerosol Type: Global Distribution, Model Evaluation and Translation into Chemical Speciation

It is essential to evaluate and refine aerosol classification methods applied to passive satellite remote sensing. We have developed an aerosol classification algorithm (called Specified Clustering and Mahalanobis Classification, SCMC) that assigns an aerosol type to multi-parameter retrievals by spaceborne, airborne or ground-based passive remote sensing instruments [1]. The aerosol types identified by our scheme are pure dust, polluted dust, urban-industrialdeveloped economy, urban-industrialdeveloping economy, dark biomass smoke, light biomass smoke and pure marine. We apply the SCMC method to inversions from the ground-based AErosol RObotic NETwork (AERONET [2]) and retrievals from the space-borne Polarization and Directionality of Earths Reflectances instrument (POLDER, [3]). The POLDER retrievals that we use differ from the standard POLDER retrievals [4] as they make full use of multi-angle, multispectral polarimetric data [5]. We analyze agreement in the aerosol types inferred from both AERONET and POLDER and evaluate GEOS-Chem [6] simulations over the globe. Finally, we use in-situ observations from the SEAC4RS airborne field experiment to bridge the gap between remote sensing-inferred qualitative SCMC aerosol types and their corresponding quantitative chemical speciation. We apply the SCMC method to airborne in-situ observations from the NASA Langley Aerosol Research Group Experiment (LARGE, [7]) and the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP, [8]) instruments; we then relate each coarsely defined SCMC type to a sum of percentage of individual aerosol species, using in-situ observations from the Particle Analysis by Laser Mass Spectrometry (PALMS, [9]), the Soluble Acidic Gases and Aerosol (SAGA, [10]), and the High - Resolution Time - of - Flight Aerosol Mass Spectrometer (HR ToF AMS, [11]).

airborne↗

NASA NTRS1998

The 1985 Biomass Burning Season in South America: Satellite Remote Sensing of Fires, Smoke, and Regional Radiative Energy Budgets

Using satellite imagery, more than five million square kilometers of the forest and cerrado regions over South America are extensively studied to monitor fires and smoke during the 1985 biomass burning season. The results are characterized for four major ecosystems, namely: (1) tropical rain forest, (2) tropical broadleaf seasonal, (3) savannah/grass and seasonal woods (SGW), and (4) mild/warm/hot grass/shrub (MGS). The spatial and temporal distribution of fires are examined from two different methods using the multispectral Advanced Very High Resolution Radiometer Local Area Coverage data. Using collocated measurements from the instantaneous scanner Earth Radiation Budget Experiment data, the direct regional radiative forcing of biomass burning aerosols is computed. The results show that more than 70% of the fires occur in the MGS and SGW ecosystems due to agricultural practices. The smoke generated from biomass burning has negative instantaneous net radiative forcing values for all four major ecosystems within South America. The smoke found directly over the fires has mean net radiative forcing values ranging from -25.6 to -33.9 W m(exp -2). These results confirm that the regional net radiative impact of biomass burning is one of cooling. The spectral and broadband properties for clear-sky and smoke regions are also presented that could be used as input and/or validation for other studies attempting to model the impact of aerosols on the earth-atmosphere system. These results have important applications for future instruments from the Earth Observing System (EOS) program. Specifically, the combination of the Visible Infrared Scanner and Clouds and the Earth's Radiant Energy System (CERES) instruments from the Tropical Rainfall Measuring Mission and the combination of Moderate Resolution Imaging Spectrometer and CERES instruments from the EOS morning crossing mission could provide reliable estimates of the direct radiative forcing of aerosols on a global scale, thereby reducing the uncertainties in current global aerosol radiative forcing values.

Christopher, Sundar A.↗

NASA NTRS2011

Workshop Summary: International Cooperative for Aerosol Prediction Workshop On Aerosol Forecast Verification

The purpose of this workshop was to reinforce the working partnership between centers who are actively involved in global aerosol forecasting, and to discuss issues related to forecast verification. Participants included representatives from operational centers with global aerosol forecasting requirements, a panel of experts on Numerical Weather Prediction and Air Quality forecast verification, data providers, and several observers from the research community. The presentations centered on a review of current NWP and AQ practices with subsequent discussion focused on the challenges in defining appropriate verification measures for the next generation of aerosol forecast systems.

Benedetti, Angela↗

NASA NTRS2011

International Cooperative for Aerosol Prediction Workshop on Aerosol Forecast Verification

Benedetti, Angela↗

DOE OSTI2023

Properties and Controlling Processes of Aerosol and Cloud Condensation Nuclei in Marine Boundary Layer Over Eastern North Atlantic (Final Report)

Remote marine low cloud systems have large spatial and temporal coverages. Because of their relatively low optical thickness and background aerosol concentrations, marine low clouds are particularly susceptible to perturbations in aerosols associated with anthropogenic emissions. Recent studies show that a large fraction of the global aerosol indirect forcing can be attributed to changes in marine low clouds, despite their relatively long distance from most anthropogenic sources. Currently, there remain large uncertainties in the magnitude of the global aerosol indirect radiative forcing. One major contribution to this large uncertainty derives from poor understanding of the aerosols under natural conditions, the perturbation by anthropogenic emissions, and the processes that drive them. In this project, we took advantage of the comprehensive, multi-dimensional characterization of meteorological parameters, trace gases, aerosol, cloud, and drizzle fields during the Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) and the long-term measurements at the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) site on Graciosa Island. By synergistically combining in situ measurements, remote sensing retrievals, and model simulations, we quantified aerosol properties in the ENA, their vertical profiles, and variations with season, synoptic state, and airmass. We investigated key aerosol processes, including entrainment of free troposphere aerosol into marine boundary layer, new particle formation, growth of Aitken mode particles, and the influences of these processes on the cloud condensation nuclei (CCN) population in marine boundary layer. The representation of key aerosol processes in the Energy Exascale Earth System Model (E3SM) was evaluated using the observations. This project has led to 26 publications, which are listed at the end of this report.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2000

How Well Will MODIS Measure Top of Atmosphere Aerosol Direct Radiative Forcing?

The new generation of satellite sensors such as the Moderate Resolution Imaging Spectroradiometer (MODIS) will be able to detect and characterize global aerosols with an unprecedented accuracy. The question remains whether this accuracy will be sufficient to narrow the uncertainties in our estimates of aerosol radiative forcing at the top of the atmosphere. Satellite remote sensing detects aerosol optical thickness with the least amount of relative error when aerosol loading is high. Satellites are less effective when aerosol loading is low. We use the monthly mean results of two global aerosol transport models to simulate the spatial distribution of smoke aerosol in the Southern Hemisphere during the tropical biomass burning season. This spatial distribution allows us to determine that 87-94% of the smoke aerosol forcing at the top of the atmosphere occurs in grid squares with sufficient signal to noise ratio to be detectable from space. The uncertainty of quantifying the smoke aerosol forcing in the Southern Hemisphere depends on the uncertainty introduced by errors in estimating the background aerosol, errors resulting from uncertainties in surface properties and errors resulting from uncertainties in assumptions of aerosol properties. These three errors combine to give overall uncertainties of 1.5 to 2.2 Wm-2 (21-56%) in determining the Southern Hemisphere smoke aerosol forcing at the top of the atmosphere. The range of values depend on which estimate of MODIS retrieval uncertainty is used, either the theoretical calculation (upper bound) or the empirical estimate (lower bound). Strategies that use the satellite data to derive flux directly or use the data in conjunction with ground-based remote sensing and aerosol transport models can reduce these uncertainties.

Remer, Lorraine A.↗

NASA NTRS2005

Overview of Aerosol Distribution

Our knowledge of atmospheric aerosols (smoke, pollution, dust or sea salt particles, small enough to be suspended in the air), their evolution, composition, variability in space and time and interaction with clouds and precipitation is still lacking despite decades of research. Understanding the global aerosol system is fundamental for progress in climate change and hydrological cycle research. While a single instrument was used to demonstrate 50 years ago that the global CO2 levels are rising, posing threat of global warming, we need an array of satellites and field measurements coupled with chemical transport models to understand the global aerosol system. This complexity of the aerosol problem results from their short lifetime (1 week) and variable chemical composition. A new generation of satellites provides exciting opportunities to measure the global distribution of aerosols, distinguishing natural from anthropogenic aerosol and measuring their interaction with clouds and climate. I shall discuss these topics and application of the data to air quality monitoring.

Kaufman, Yoram↗

NASA NTRS2006

Satellite Observations of the Effect of Natural and Anthropogenic Aerosols on Clouds

Our knowledge of atmospheric aerosols (smoke, pollution, dust or sea salt particles, small enough to be suspended in the air), their evolution, composition, variability in space and time and interaction with clouds and precipitation is still lacking despite decades of research. Understanding the global aerosol system is critical to quantifying anthropogenic climate change, to determine climate sensitivity from observations and to understand the hydrological cycle. While a single instrument was used to demonstrate 50 years ago that the global CO2 levels are rising, posing threat of global warming, we need an array of satellites and field measurements coupled with chemical transport models to understand the global aerosol system. This complexity of the aerosol problem results from their short lifetime (1 week) and variable chemical composition. A new generation of satellites provides exciting opportunities to measure the global distribution of aerosols, distinguishing natural from anthropogenic aerosol and measuring their interaction with clouds and climate.

Kaufman, Yoram J.↗

NASA NTRS2006

Consistency of Global Modis Aerosol Optical Depths over Ocean on Terra and Aqua Ceres SSF Datasets

Aerosol retrievals over ocean from the Moderate Resolution Imaging Spectroradiometer (MODIS) onboard Terra and Aqua platforms are available from the Clouds and the Earth's Radiant Energy System (CERES) Single Scanner Footprint (SSF) datasets generated at NASA Langley Research Center (LaRC). Two aerosol products are reported side-by-side. The primary M product is generated by sub-setting and remapping the multi-spectral (0.47-2.1 micrometer) MODIS produced oceanic aerosol (MOD04/MYD04 for Terra/Aqua) onto CERES footprints. M*D04 processing uses cloud screening and aerosol algorithms developed by the MODIS science team. The secondary AVHRR-like A product is generated in only two MODIS bands 1 and 6 (on Aqua, bands 1 and 7). The A processing uses the CERES cloud screening algorithm, and NOAA/NESDIS glint identification, and single-channel aerosol retrieval algorithms. The M and A products have been documented elsewhere and preliminarily compared using 2 weeks of global Terra CERES SSF Edition 1A data in which the M product was based on MOD04 collection 3. In this study, the comparisons between the M and A aerosol optical depths (AOD) in MODIS band 1 (0.64 micrometers), tau(sub 1M) and tau(sub 1A) are re-examined using 9 days of global CERES SSF Terra Edition 2A and Aqua Edition 1B data from 13 - 21 October 2002, and extended to include cross-platform comparisons. The M and A products on the new CERES SSF release are generated using the same aerosol algorithms as before, but with different preprocessing and sampling procedures, lending themselves to a simple sensitivity check to non-aerosol factors. Both tau(sub 1M) and tau(sub 1A) generally compare well across platforms. However, the M product shows some differences, which increase with ambient cloud amount and towards the solar side of the orbit. Three types of comparisons conducted in this study - cross-platform, cross-product, and cross-release confirm the previously made observation that the major area for improvement in the current aerosol processing lies in a more formalized and standardized sampling (and most importantly, cloud screening) whereas optimization of the aerosol algorithm is deemed to be an important yet less critical element.

Ignatov, Alexander↗

NASA NTRS1995

A Unified Picture of Pinatubo Aerosol Global-to Micro-Scale Evolution, From Space, Air, and Ground Measurements

We combine a variety of measurements to develop a composite picture of the post-Pinatubo aerosol and assess the consistency and uncertainties of the measurement and retrieval techniques. Satellite infrared spectroscopy, particle morphology, and evaporation temperature measurements are in accord with theoretical calculations in showing a dominant particle composition of H2SO4-H2O mixture, with H2SO4 weight fraction of 65-80% for most stratospheric temperatures and humidities. Important exceptions are: (1) the presence of volcanic ash at all altitudes initially and in a layer just above the tropopause until at least March 1992, and (2) much smaller H2SO4 weight fractions at the low temperatures attained in high latitude winters and at the tropical tropopause, Laboratory spectroscopy and theoretical calculations yield wavelength- and temperature-dependent refractive indices for the dominant H2SO4-H2O droplets. These in turn permit derivation of particle size spectra from measured optical depth spectra, for comparison to direct measurements by impactors and optical counters. All three techniques paint a generally consistent picture of the evolution of R(sub eff), the effective, or area-weighted, particle radius. In the first month after the eruption, although particle numbers increased by orders of magnitude, R(sub eff) was similar to the preemption value of 0.1 to 0.2 microns, because both small (r less than 0.2 microns) and large (r greater than 0.6 micron particles increased in number. Over the next 3-6 months, R(sub eff) increased to about 0.5 microns reflecting particle growth through condensation and coagulation. In general, R(sub eff) continued to increase for about a year after the eruption. Extinction spectra computed from in situ size distribution measurements are consistent with optical depth measurements, which show spectra with maxima initially at wavelengths of 0.42 microns or less, and thereafter progressively increasing to between 0.78 and 1 micron. Not until 1993 do optical depth spectra begin to show a clear return to the preemption signature of maximizing at the shortest visible wavelengths or in the near UV. This coupled evolution in particle size distribution and optical depth spectra helps explain the relationship between the global maps of 0.5- 1.0- micron optical depth derived from the AVHRR and SAGE satellite measurements.

Russell, Philip B.↗

NASA NTRS1984

SAGE and SAM II measurements of global stratospheric aerosol optical depth and mass loading

Several volcanic eruptions between November 1979 and April 1981 have injected material into the stratosphere. The SAGE and SAM II satellite systems have measured, with global coverage, the 1-micron extinction produced by this material, and examples of the data product are shown in the form of global maps of stratospheric optical depth and altitude-latitude plots of zonal mean extinction. These data, and that for the volcanically quiet period in early 1979, have been used to determine the changes in the total stratospheric mass loading. Estimates have also been made of the contribution to the total aerosol mass from each eruption. It has been found that between 1979 and mid-1981, the total stratospheric aerosol mass increased from a background level of approximately 570,000 metric tons to a peak of approximately 1,300,000 metric tons.

Kent, G. S.↗

NASA NTRS1995

Pinatubo Aerosol Global-to-Micro-Scale Evolution: A Unified Picture From Space, Air, and Ground Measurements

We combine a variety of measurements to develop a composite picture of the post-Pinatubo aerosol and assess the consistency and uncertainties of the measurement and retrieval techniques Satellite infrared spectroscopy, particle morphology, and evaporation temperature measurements are in accord with theoretical calculations In showing a dominant particle composition of H2SO4-H2O mature with H2SO4 weight traction of 65-80% for most stratospheric temperatures and humidities. Important exceptions are: (1) the presence of volcanic ash at all attitudes initially and in a layer just above the tropopause until at least March 1992, and (2) much smaller H2SO4 weight fractions at the low temperatures attained In high latitude winters and at the tropical tropopause. Laboratory spectroscopy and theoretical calculations yield wavelength- and temperature-dependent refractive indices for the dominant H2SO4-H2O droplets. These in turn permit derivation of particle size spectra from measured optical depth spectra for comparison to direct measurements by impactors and optical counters, All three techniques paint a generally consistent picture of the evolution of R(sub eff) the effective, or area-weighted, particle radius. In the first month after the eruption, although particle numbers increased by orders of magnitude, R(sub eff) was similar to the pre-eruption value of 0.1 to 0.2 microns because both small (r less than 0.2 microns) and large (r greater than 0.6 microns) particles increased in number. Over the next 3-6 months, R(sub eff) increased to about 0.5 microns, reflecting particle growth through condensation and coagulation. In general, R(sub eff) continued to increase for about a year after the eruption. Extinction spectra computed from in situ size distribution measurements are consistent with optical depth measurements, which show spectra with maxima initially at wavelengths of 0.42 microns or less, and thereafter progressively increasing to between 0.78 and 1 micron. Not until 1993 does optical depth spectra begin to show a clear return to the preeruption signature of maximizing at the shortest visible wavelengths or in the near UV. This coupled evolution in particle size distribution and optical depth spectra helps explain the relationship between the global maps of 0.5- and 1.0-kilometer optical depth derived from the AVHRR and SAGE satellite measurements. It also sets a context for evaluating remaining uncertainties in each of these satellite data products. We also show how the effects of wavelength-dependent refractive index on backscatter spectra can influence particle sizes retrieved from multiwavelength lidar measurements.

Russell, Philip B.↗

NASA NTRSDate not supplied

Models, In situ, and Remote Sensing of Aerosols (MIRA)

There is a natural partitioning of scientific interest amongst three specialties of aerosol re-search: modeling, in situ measurements, and remote sensing. The broader aerosol community benefits when these groups interact, and this strengthens overall scientific impact on climate and air quality research and predictions. The new MIRA working group establishes a forum for identifying collaborations and improving discussions amongst specialties and across regional boundaries. One area of keen interest is uniting satellite and ground-based lidar groups with other aerosol disciplines. Elastic backscatter lidars depend upon a priori knowledge of aerosol properties to convert measured lidar profiles into aerosol extinction profiles. Acquiring additional insight on aerosol properties and transport is highly valuable to these lidar groups to improve the data quality and aid in their scientific interpretation. Another area of interest is to facilitate the incorporation of measurements into global aerosol models. Modelers need aerosol optical look-up tables that enable quick conversions of hydrated (and dry) polydisperse size distributions into aerosol optical properties (extinction, scattering, etc.), but many of the existing tables are based upon outdated measurements. Thus, MIRA is building the Tables of Aerosol Optics (TAO), which is a community collection of aerosol optical calculations. This expands on the historical efforts of Shettle and Fenn, d’Almeida, GADS, OPAC, etc., except that TAO seeks continual input from the community. Thus, as aerosol measurement and computational techniques advance, so does the TAO collective. Since TAO is a community collective, it is expected that users will optionally upload computations for aerosol type as well as computations for all of the traditional aerosol species(like amm sulfate, amm nitrate, organics, etc.). The near-term purpose of the MIRA working group is to: *Characterize regional aerosol lidar ratios to support improvements of aerosol extinction profiles and understanding of aerosol typing. *Create TAO --a community cooperative of aerosol optical tables. *Facilitate international communications between aerosol measurement and modeling groups. *Encourage the use of regional knowledge to develop and improve remote sensing techniques for current and future backscatter lidars located in space. *Enable and foster communication between the scientists who run global aerosol models and scientists who analyze space-based lidar data. We will discuss how a collaborative aerosol working group will be organized on this topic. Those who are interested in MIRA can sign up for the MIRA email listserver at https://forms.gle/qdbCnngzNJc5YJi57.

Greg Schuster↗

NASA NTRSDate not supplied

Models, In situ, and Remote sensing of Aerosols (MIRA): Formation of an International Working Group

There is a natural partitioning of scientific interest amongst three specialties of aerosol re- search: modeling, in situ measurements, and remote sensing. The broader aerosol community benefits when these groups interact, and this strengthens overall scientific impact on climate and air quality research and predictions. The new MIRA working group establishes a forum for identifying collaborations and improving discussions amongst specialties and across regional boundaries. One area of keen interest is uniting satellite and ground-based lidar groups with other aerosol disciplines. Elastic backscatter lidars depend upon a priori knowledge of aerosol properties to convert measured lidar profiles into aerosol extinction profiles. Acquiring additional insight on aerosol properties and transport is highly valuable to these lidar groups to improve the data quality and aid in their scientific interpretation. Another area of interest is to facilitate the incorporation of measurements into global aerosol models. Modelers need aerosol optical look-up tables that enable quick conversions of hydrated (and dry) polydisperse size distributions into aerosol optical properties (extinction, scattering, etc.), but many of the existing tables are based upon outdated measurements. Thus, MIRA is building the Tables of Aerosol Optics (TAO), which is a community collection of aerosol optical calculations. This expands on the historical efforts of Shettle and Fenn, d’Almeida, GADS, OPAC, etc., except that TAO seeks continual input from the community. Thus, as aerosol measurement and computational techniques advance, so does the TAO collective. Since TAO is a community collective, it is expected that users will optionally upload computations for aerosol type as well as computations for all of the traditional aerosol species (like amm sulfate, amm nitrate, organics, etc.). The near-term purpose of the MIRA working group is to: * Characterize regional aerosol lidar ratios to support improvements of aerosol extinction profiles and understanding of aerosol typing. * Create TAO -- a community cooperative of aerosol optical tables. * Facilitate international communications between aerosol measurement and modeling groups. * Encourage the use of regional knowledge to develop and improve remote sensing techniques for current and future backscatter lidars located in space. * Enable and foster communication between the scientists who run global aerosol models and scientists who analyze space-based lidar data. We will discuss how a collaborative aerosol working group will be organized on this topic. Send email to calipso_v5alr-join@lists.nasa.gov with the word `subscribe' in the subject line to join MIRA.

Gregory Schuster↗

NASA NTRS2012

Spatially Refined Aerosol Direct Radiative Forcing Efficiencies

Global aerosol direct radiative forcing (DRF) is an important metric for assessing potential climate impacts of future emissions changes. However, the radiative consequences of emissions perturbations are not readily quantified nor well understood at the level of detail necessary to assess realistic policy options. To address this challenge, here we show how adjoint model sensitivities can be used to provide highly spatially resolved estimates of the DRF from emissions of black carbon (BC), primary organic carbon (OC), sulfur dioxide (SO2), and ammonia (NH3), using the example of emissions from each sector and country following multiple Representative Concentration Pathway (RCPs). The radiative forcing efficiencies of many individual emissions are found to differ considerably from regional or sectoral averages for NH3, SO2 from the power sector, and BC from domestic, industrial, transportation and biomass burning sources. Consequently, the amount of emissions controls required to attain a specific DRF varies at intracontinental scales by up to a factor of 4. These results thus demonstrate both a need and means for incorporating spatially refined aerosol DRF into analysis of future emissions scenario and design of air quality and climate change mitigation policies.

Climate↗

NASA NTRS2005

It's a Sooty Problem: Black Carbon and Aerosols from Space

Our knowledge of atmospheric aerosols (smoke, pollution, dust or sea salt particles, small enough to be suspended in the air), their evolution, composition, variability in space and time and interaction with solar radiation, clouds and precipitation is lacking despite decades of research. Just recently we recognized that understanding the global aerosol system is fundamental for progress in climate change and hydrological cycle research. While a single instrument was used to demonstrate 50 yrs ago that the global CO2 levels are rising, posing thread to our climate, we need an may of satellites, surface networks of radiometers, elaborated laboratory and field experiments coupled with chemical transport models to understand the global aerosol system. This complexity of the aerosol problem results from their short lifetime (1 week), variability of the chemical composition and complex chemical and physical processes in the atmosphere. The result is a heterogeneous distribution of aerosol and their properties. The new generation of satellites and surface networks of radiometers provides exciting opportunities to measure the aerosol properties and their interaction with clouds and climate. However farther development in the satellite capability, aerosol chemical models and climate models is needed to fully decipher the aerosol secrets with accuracy required to predict future climates.

Kaufman, Yoram J.↗

DOE OSTI2020

An evaluation of global organic aerosol schemes using airborne observations

Chemical transport models have historically struggled to accurately simulate the magnitude and variability of observed organic aerosol (OA), with previous studies demonstrating that models significantly underestimate observed concentrations in the troposphere. In this study, we explore two different model OA schemes within the standard GEOS-Chem chemical transport model and evaluate the simulations against a suite of 15 globally distributed airborne campaigns from 2008 to 2017, primarily in the spring and summer seasons. These include the ATom, KORUS-AQ, GoAmazon,FRAPPE, SEAC4RS, SENEX, DC3, CalNex, OP3, EUCAARI, ARCTAS and ARCPAC campaigns and provide broad coverage over a diverse set of atmospheric composition regimes – anthropogenic, biogenic, pyrogenic and remote. The schemes include significant differences in their treatment of the primary and secondary components of OA – a “simple scheme” that models primary OA (POA) as non-volatile and takes a fixed-yield approach to secondary OA (SOA) formation and a “complex scheme” that simulates POA as semi-volatile and uses a more sophisticated volatility basis set approach for non-isoprene SOA, with an explicit aqueous uptake mechanism to model isoprene SOA. Despite these substantial differences, both the simple and complex schemes perform comparably across the aggregate dataset in their ability to capture the observed variability (with an R2 of 0.41 and 0.44, respectively). The simple scheme displays greater skill in minimizing the overall model bias (with a normalized mean bias of 0.04 compared to 0.30 for the complex scheme). Across both schemes, the model skill in reproducing observed OA is superior to previous model evaluations and approaches the fidelity of the sulfate simulation within the GEOS-Chem model. However,there are significant differences in model performance across different chemical source regimes, classified here into seven categories.Higher-resolution nested regional simulations indicate that model resolution is an important factor in capturing variability in highly localized campaigns, while also demonstrating the importance of well-constrained emissions inventories and local meteorology, particularly over Asia. Our analysis suggests that a semi-volatile treatment of POA is superior to anon-volatile treatment. It is also likely that the complex scheme parameterization overestimates biogenic SOA at the global scale. While this study identifies factors within the SOA schemes that likely contribute to OA model bias (such as a strong dependency of the bias in the complex scheme on relative humidity and sulfate concentrations), comparisons with the skill of the sulfate aerosol scheme in GEOS-Chem indicate the importance of other drivers of bias, such as emissions, transport and deposition, that are exogenous to the OA chemical scheme.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2021

Aerosol Absorption in Global Models From AeroCom Phase III

Aerosol-induced absorption of shortwave radiation can modify the climate through local atmospheric heating, which affects lapse rates, precipitation, and cloud formation. Presently, the total amount of aerosol absorption is poorly constrained, and the main absorbing aerosol species (black carbon (BC), organic aerosols (OA), and mineral dust) are diversely quantified in global climate models. As part of the third phase of the Aerosol Comparisons between Observations and Models (AeroCom) intercomparison initiative (AeroCom phase III), we here document the distribution and magnitude of aerosol absorption in current global aerosol models and quantify the sources of intermodel spread, highlighting the difficulties of attributing absorption to different species. In total, 15 models have provided total present-day absorption at 550 nm (using year 2010 emissions), 11 of which have provided absorption per absorbing species. The multi-model global annual mean total absorption aerosol optical depth (AAOD) is 0.0054 (0.0020 to 0.0098; 550 nm), with the range given as the minimum and maximum model values. This is 28 % higher compared to the 0.0042 (0.0021 to 0.0076) multi-model mean in AeroCom phase II (using year 2000 emissions), but the difference is within 1 standard deviation, which, in this study, is 0.0023 (0.0019 in Phase II). Of the summed component AAOD, 60 % (range 36 %–84 %) is estimated to be due to BC, 31 % (12 %–49 %) is due to dust, and 11 % (0 %–24 %) is due to OA; however, the components are not independent in terms of their absorbing efficiency. In models with internal mixtures of absorbing aerosols, a major challenge is the lack of a common and simple method to attribute absorption to the different absorbing species. Therefore, when possible, the models with internally mixed aerosols in the present study have performed simulations using the same method for estimating absorption due to BC, OA, and dust, namely by removing it and comparing runs with and without the absorbing species. We discuss the challenges of attributing absorption to different species; we compare burden, refractive indices, and density; and we contrast models with internal mixing to models with external mixing. The model mean BC mass absorption coefficient (MAC) value is 10.1 (3.1 to 17.7) m 2 g −1 (550 nm), and the model mean BC AAOD is 0.0030 (0.0007 to 0.0077). The difference in lifetime (and burden) in the models explains as much of the BC AAOD spread as the difference in BC MAC values. The difference in the spectral dependency between the models is striking. Several models have an absorption Ångstrøm exponent (AAE) close to 1, which likely is too low given current knowledge of spectral aerosol optical properties. Most models do not account for brown carbon and underestimate the spectral dependency for OA.

Aerosol absorption↗