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DOE OSTI2024

Aerosol hygroscopicity over the southeast Atlantic Ocean during the biomass burning season – Part 1: From the perspective of scattering enhancement​​​​​​​

Aerosol hygroscopicity plays a vital role in aerosol radiative forcing. One key parameter describing hygroscopicity is the scattering enhancement factor, f(RH), defined as the ratio of the scattering coefficient at humidified relative humidity (RH) to its dry value. Here, we utilize the f(80 %) from ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) 2016 and 2018 airborne measurements to investigate the hygroscopicity of aerosols, its vertical distribution, its relationship with chemical composition, and its sensitivity to organic aerosol (OA) hygroscopicity over the southeast Atlantic (SEA) Ocean during the biomass burning (BB) season. We found that aerosol hygroscopicity remains steady above 2 km, with a mean f(80 %) of 1.40 ± 0.17. Below 2 km, aerosol hygroscopicity increases with decreasing altitude, with a mean f(80 %) of 1.51 ± 0.22, consistent with higher values of BB aerosol hygroscopicity found in the literature. The hygroscopicity parameter of OA (κ OA ) is retrieved from the Mie model with a mean value of 0.11 ± 0.08, which is in the middle to upper range compared to the literature. Higher OA hygroscopicity is related to aerosols that are more aged, oxidized, and present at lower altitudes. The enhanced biomass burning aerosol (BBA) hygroscopicity at lower altitudes is mainly due to a lower OA fraction, increased sulfate fraction, and greater κ OA at lower altitudes. We propose a parameterization that quantifies f(RH) with chemical composition and κOA based on Mie simulation of internally mixed OA–(NH 4 ) 2 SO 4 –BC mixtures. The good agreement between the predictions and the ORACLES measurements implies that the aerosols in the SEA during the BB season can be largely represented by the OA–(NH 4 ) 2 SO 4 –BC internal mixture with respect to the f(RH) prediction. The sensitivity of f(RH) to κ OA indicates that applying a constant κ OA is only suitable when the OA fraction is low and κ OA shows limited variation. However, in situations deviating these two criteria, κ OA can notably impact scattering coefficients and aerosol radiative effect; therefore, accounting for κ OA variability is recommended.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Assessing the sensitivity of aerosol mass budget and effective radiative forcing to horizontal grid spacing in E3SMv1 using a regional refinement approach

Abstract. Atmospheric aerosols have important impacts on air quality and the Earth–atmospheric energy balance. However, as computing power is limited, Earth system models generally use coarse spatial grids and parameterize finer-scale atmospheric processes. These parameterizations and the simulation of atmospheric aerosols are often sensitive to model horizontal resolutions. Understanding the sensitivities is necessary for the development of Earth system models at higher resolutions with the deployment of more powerful supercomputers. Using the Energy Exascale Earth System Model (E3SM) version 1, this study investigates the impact of horizontal grid spacing on the simulated aerosol mass budget, aerosol–cloud interactions, and the effective radiative forcing of anthropogenic aerosols (ERFaer) over the contiguous United States. We examine the resolution sensitivity by comparing the nudged simulation results for 2016 from the low-resolution model (LR) and the regional refinement model (RRM). As expected, the simulated emissions of natural dust, sea salt, and marine organic matter are substantially higher in the RRM than in the LR. In addition, RRM simulates stronger aqueous-phase production of sulfate through the enhanced oxidation of sulfur dioxide by hydrogen peroxide due to increased cloud liquid water content. In contrast, the gas-phase chemical production of sulfate is slightly suppressed. The RRM resolves more large-scale precipitation and produces less convective precipitation than the LR, leading to increased (decreased) aerosol wet scavenging by large-scale (convective) precipitation. Regarding aerosol effects on clouds, RRM produces larger temporal variabilities in the large-scale liquid cloud fractions than LR, resulting in increased microphysical cloud processing of aerosols (more interstitial aerosols are converted to cloud-borne aerosols via aerosol activation) in RRM. Water vapor condensation is also enhanced in RRM compared to LR. Consequently, the RRM simulation produces more cloud droplets, a larger cloud droplet radius, a higher liquid water path, and a larger cloud optical depth than the LR simulation. A comparison of the present-day and pre-industrial simulations indicates that, for this contiguous United States domain, the higher-resolution increases ERFaer at the top of the model by about 12 %, which is mainly attributed to the strengthened indirect effect associated with aerosol–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Stratospheric aerosol forcing for CMIP7 – Part 1: optical properties for pre-industrial, historical, and scenario simulations

Stratospheric aerosols, most of which originate from explosive volcanic sulfur emissions into the stratosphere, are a key natural driver of climate variability. They are thus a forcing provided by the Coupled Model Intercomparison Project (CMIP) Climate Forcings Task Team to climate modelling groups participating in phase 7 of CMIP. For the historical period, we provide two datasets covering 1750–2023: (i) a volcanic upper tropospheric-stratospheric sulfur emission dataset, documented in a companion paper; and (ii) a stratospheric sulfate aerosol optical property dataset, documented in this paper. For the satellite era (from 1979 onwards), stratospheric aerosol optical properties are derived from the Global Space-based Stratospheric Aerosol Climatology (GloSSAC) dataset. For the pre-satellite era (1750–1978), optical properties are derived from our volcanic SO 2 emission dataset using a new version of the reduced-complexity volcanic aerosol model Easy Volcanic Aerosol (Height) (EVA_H v2). A background, non-volcanic stratospheric aerosol climatology is derived from the 1998–2001 period with a trend over 1850–1978 accounting for increasing anthropogenic aerosols. A monthly stratospheric aerosol climatology is derived from the 1850–2021 average for both pre-industrial and scenario (future) simulations, with a 9-year ramp over 2022–2030 for scenario simulations to ensure a smooth transition from the historical period. CMIP7 simulations should use version 2.2.1 of our pre-industrial and historical datasets, and version 2.2.2 of our scenario dataset. Our methodology to produce historical aerosol optical properties significantly differs from CMIP6 for the pre-satellite era, and the resulting forcings in turn largely differ. In particular, the CMIP6 dataset was mostly based on the sparse and uncertain pyrheliometer record, which resulted in strongly underrepresented emissions from small-to-moderate magnitude eruptions. The resulting bias is addressed in CMIP7, which is entirely emission-derived in the pre-satellite era and uses more recent ice-core-based volcanic sulfur emission inventories than CMIP6. Our approach results in an overall larger volcanic aerosol forcing for CMIP7, with the 1850–2014 mean mid-visible global mean stratospheric aerosol optical depth (SAOD) in CMIP7 (0.0138) being 29 % higher than in CMIP6 (0.0107). The pre-industrial mean of the same variable is 26 % higher in CMIP7 (0.0135, derived from the historical 1850–2021) than CMIP6 (0.0107, derived from the historical 1850–2014 mean). Using a reduced-complexity climate model, we simulate a global mean surface temperature that is 0.07 °C colder for 1850–1900 when using the CMIP7 dataset instead of CMIP6, whereas 2000–2014 is 0.03 °C warmer in CMIP7. Our dataset also exhibits lower forcing for 1960–1980, resulting in temperatures 0.06 °C warmer when averaged over 1960–1990, a period for which CMIP6 climate models exhibit a cold bias. Given the large uncertainties characterizing the dataset, in particular for the pre-satellite era, we advise against treating the CMIP7 or CMIP6 dataset as uniquely superior for any specific year and highlight the need for further evaluation. We conclude the study by discussing sources of uncertainty for the dataset, future research avenues to improve it, as well as requirements to operationalize the production of the dataset, i.e. extend it and update it on an annual basis instead of every 5–7 years following CMIP cycles.

Aubry, Thomas J. [Univ. of Exeter, Devon (United K↗
NASA NTRS1998

Combining data from lidar and in situ instruments to characterize the vertical structure of aerosol optical properties

Over the last decade, the quantification of tropospheric aerosol abundance, composition and radiative impacts has become an important research endeavor. For the most part, the interest in tropospheric aerosols is derived from questions related to the global and local (instantaneous) radiative forcing of climate due to these aerosols. One approach is to study local forcing under well-defined conditions, and to extrapolate such results to global scales. To estimate local aerosol forcing, appropriate radiative transfer models can be employed (e.g., the Fu-Liou radiative transfer code, [Fu and Liou, 1993]). In general, such models require information on derived aerosol properties [Toon, 1994]; namely the aerosol optical depth, single-scattering albedo, and asymmetry factor (phase function), all of which appear in the equations of radiative transfer. In this paper, we report on a method that utilizes lidar data and in situ aerosol size distribution measurements to deduce the vertical structure of the aerosol complex index of refraction in the near IR, thus identifying the aerosol type. Together with aerosol size distributions obtained in situ, the aerosol refractive index can be used to calculate the necessary derived aerosol properties. The data analyzed here were collected during NASA's PEM West-B (Pacific Exploratory Mission) experiment, which took place in February/March 1994. The platform for the measurements was the NASA DC-8 aircraft. The primary goal of the PEM West missions [Browell et al., 1996] was the assessment of potential anthropogenic perturbations of the chemistry in the Pacific Basin troposphere. For this purpose the timing of PEM West-B corresponded to the seasonal peak in transport from the Asian continent into the Pacific basin [Merrill et al., in press]. This period normally occurs during Northern Hemisphere spring, when the Japan jet is well developed.

Redemann, J.↗
NASA NTRS1999

Global and Seasonal Aerosol Optical Depths Derived From Ultraviolet Observations by Satellites (TOMS)

It has been shown that absorbing aerosols (dust, smoke, volcanic ash) can be detected in the ultraviolet wavelengths (331 nm to 380 nm) from satellite observations (TOMS, Total Ozone Mapping Spectrometer) over both land and water. The theoretical basis for these observations and their conversions to optical depths is discussed in terms of an aerosol index AI or N-value residue (assigned positive for absorbing aerosols). The theoretical considerations show that negative values of the AI frequently represent the presence of non-absorbing aerosols (NA) in the troposphere (mostly pollution in the form of sulfates, hydrocarbons, etc., and some natural sulfate aerosols) with particle sizes near 0.1 to 0.2 microns or less. The detection of small-particle non-absorbing aerosols from the measured backscattered radiances is based on the observed wavelength dependence from Mie scattering after the background Rayleigh scattering is subtracted. The Mie scattering from larger particles, 1 micron or more (e.g., cloud water droplets) has too small a wavelength dependence to be detected by this method. In regions that are mostly cloud free, aerosols of all sizes can be seen in the single channel 380 nm or 360 nm radiance data. The most prominent Al feature observed is the strong asymmetry in aerosol amount between the Northern and Southern Hemispheres, with the large majority of NA occurring above 20degN latitude. The maximum values of non-absorbing aerosols are observed over the eastern U.S. and most of western Europe corresponding to the areas of highest industrial pollution. Annual cycles in the amount of NA are observed over Europe and North America with maxima occurring in the summer corresponding to times of minimum wind transport. Similarly, the maxima in the winter over the Atlantic Ocean occurs because of wind borne transport from the land. Most regions of the world have the maximum amount of non-absorbing aerosol in the December to January period except for the eastern North America and Europe. Comparisons of the estimated TOMS aerosol optical depths show good agreement in magnitude and seasonal dependence with sun-photometer optical depths obtained at Goddard Space Flight Center (39degN 76.88degW) in the U.S. and in Lille (50.63degN 3.07degE) in France. The study of these aerosols is important for detecting the sources of industrial pollution and its redistribution by winds on a global basis, as well as its effect on reducing the UV irradiance at the Earth's surface.

Herman, J. R.↗
NASA NTRS1998

Raman Lidar Measurements of Aerosol Extinction and Backscattering: Methods and Comparisons - Report 1

This paper examines the aerosol backscattering and extinction profiles measured at night by the NASA Goddard Space Flight Center Scanning Raman Lidar (SRL) during the remote cloud sensing (RCS) intensive operations period (IOP) at the Department of Energy Atmospheric Radiation Measurement (ARM) southern Great Plains (SGP) site in April 1994. These lidar data are used to derive aerosol profiles for altitudes between 0.0 1 5 and 5 km. Since this lidar detects Raman scattering from nitrogen and oxygen molecules as well as the elastic scattering from molecules and aerosols, it measures both aerosol backscattering and extinction simultaneously. The aerosol extinction/backscattering ratio varied between approximately 30 sr and 75 sr at 351 nm. Aerosol optical thicknesses derived by integrating the lidar profiles of aerosol extinction measured at night between 0. I and 5 km are found to be about 10-40% lower than those measured by a Sun photometer during the day. This difference is attributed to the contribution by stratospheric aerosols not included in the lidar estimates as well as to diurnal differences in aerosol properties and concentrations. Aerosol profiles close to the surface were acquired by pointing the lidar nearly horizontally. Measurements of aerosol scattering from a tower-mounted nephelometer are found to be 40% lower than lidar measurements of aerosol extinction over a wide range of relative humidities even after accounting for the difference in wavelengths. The reasons for this difference are not clear but may be due to the inability of the nephelometer to accurately measure scattering by large particles.

Ferrare, R. A.↗
NASA NTRS2000

North Atlantic Aerosol Properties and Direct Radiative Effects: Key Results from TARFOX and ACE-2

Aerosol effects on atmospheric radiative fluxes provide a forcing function that can change the climate In potentially significant ways. This aerosol radiative forcing is a major source of uncertainty in understanding the observed climate change of the past century and in predicting future climate. To help reduce this uncertainty, the International Global Atmospheric Chemistry Project (IGAC) has endorsed a series of multiplatform aerosol field campaigns. The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the second Aerosol Characterization Experiment (ACE-2) were the first IGAC campaigns to address the impact of anthropogenic aerosols, Both TARFOX and ACE-2 gathered extensive data sets on aerosol properties and radiative effects, TARFOX focused on the urban-industrial haze plume flowing from the eastern United States over the western Atlantic Ocean, whereas ACE-2 studied aerosols carried over the eastern Atlantic from both European urban/industrial and African mineral sources. These aerosols often have a marked influence on the top-of-atmosphere radiances measured by satellites. Shown there are contours of aerosol optical depth derived from radiances measured by the AVHRR sensor on the NOAA-11 satellite. The contours readily show that aerosols originating in North America, Europe, and Africa impact the radiative properties of air over the North Atlantic. However, the accurate derivation of flux changes, or radiative forcing, from the satellite measured radiances or retrieved optical depths remains a difficult challenge. In this paper we summarize key initial results from TARFOX and, to a lesser extent, ACE-2, with a focus on those results that allow an improved assessment of the flux changes caused by North Atlantic aerosols at middle latitudes.

Russell, P. B.↗
NASA NTRS2000

Aerosol Radiative Forcing in Asian Continental Outflow

Aerosols in elevated layers were sampled with FSSP-probes and wire impactors over the Pacific ocean aboard the NASA DC-8 aircraft. Analyses of particle size and morphology identifies two distinctly different aerosol types for cases when the mid-visible extinctions exceed 0.2/km. Smaller sizes (effective radii of 0.2 um) and moderate absorption (mid-visible single scattering albedo of.935) are typical for urban-industrial pollution. Larger sizes (effective radii of 0.7 um) and weak absorption (mid-visible single scattering albedo of 0.985) identify dust. This aerosol classification is in agreement with its origin as determined by airmass back trajectory analysis. Based on lidar vertical profiling, aerosol dominated by dust and urban-industrial pollution above 3km were assigned mid-visible optical depths of 0.50 and 0.27, respectively. Radiative transfer simulations, considering a 50% cloud-cover below the aerosol layers, suggest (on a daily tP C)C> basis) small reductions (-4W/m2) to the energy budget at the top of the atmosphere for both aerosol types. For c' 0 dust, more backscattering of sunlight (weaker solar absorption) is compensated by a stronger greenhouse effect due to larger sizes. Forced reductions to the energy budget at the surface are 12W/m2 for both aerosol types. In contrast, impacts on heating rates within the aerosol layers are quite different: While urban-industrial aerosol warms the layer (at +0.6K/day as solar heating dominates), dust cools (at -0.5K/day as infrared cooling dominates). Sensitivity tests show the dependence of the aerosol climatic impact on the optical depth, particle size, absorptivity, and altitude of the layers, as well as clouds and surface properties. Climatic cooling can be eliminated (1) for the urban-industrial aerosol if absorption is increased to yield a mid-visible single scattering albedo of 0.89, or if the ocean is replaced by a land surface; (2) for the dust aerosol if the effective radius is increased from 0.7 to 1.2 um. The removal of low-level clouds doubles the cooling at the top of the atmosphere to about -8W/m2.

Pueschel, R.↗
NASA NTRS2000

Airborne Aerosol Closure Studies During PRIDE

The Puerto Rico Dust Experiment (PRIDE) was conducted during June/July of 2000 to study the properties of Saharan dust aerosols transported across the Atlantic Ocean to the Caribbean Islands. During PRIDE, the NASA Ames Research Center six-channel (380 - 1020 nm) airborne autotracking sunphotometer (AATS-6) was operated aboard a Piper Navajo airplane alongside a suite of in situ aerosol instruments. The in situ aerosol instrumentation relevant to this paper included a Forward Scattering Spectrometer Probe (FSSP-100) and a Passive Cavity Aerosol Spectrometer Probe (PCASP), covering the radius range of approx. 0.05 to 10 microns. The simultaneous and collocated measurement of multi-spectral aerosol optical depth and in situ particle size distribution data permits a variety of closure studies. For example, vertical profiles of aerosol optical depth obtained during local aircraft ascents and descents can be differentiated with respect to altitude and compared to extinction profiles calculated using the in situ particle size distribution data (and reasonable estimates of the aerosol index of refraction). Additionally, aerosol extinction (optical depth) spectra can be inverted to retrieve estimates of the particle size distributions, which can be compared directly to the in situ size distributions. In this paper we will report on such closure studies using data from a select number of vertical profiles at Cabras Island, Puerto Rico, including measurements in distinct Saharan Dust Layers. Preliminary results show good agreement to within 30% between mid-visible aerosol extinction derived from the AATS-6 optical depth profiles and extinction profiles forward calculated using 60s-average in situ particle size distributions and standard Saharan dust aerosol refractive indices published in the literature. In agreement with tendencies observed in previous studies, our initial results show an underestimate of aerosol extinction calculated based on the in situ size distributions relative to the extinction obtained from the sunphotometer measurements. However, a more extensive analysis of all available AATS-6 and in situ size distribution data is necessary to ascertain whether the preliminary results regarding the degree of extinction closure is representative of the entire range of dust conditions encountered in PRIDE. Finally, we will compare the spectral extinction measurements obtained in PRIDE to similar data obtained in Saharan dust layers encountered above the Canary Islands during ACE-2 (Aerosol Characterization Experiment) in July 1997. Thus, the evolution of Saharan dust spectral properties during its transport across the Atlantic can be investigated, provided the dust origin and microphysical properties are found to be comparable.

Redemann, Jens↗
NASA NTRS2001

Aerosol Optical Properties over the Oceans: Summary and Interpretation of Shadow-Band Radiometer Data from Six Cruises

The aerosol scattering component of the total radiance measured at the detectors of ocean color satellites is determined with atmospheric correction algorithms. These algorithms are based on aerosol optical thickness measurements made in two channels that lie in the near-infrared portion of the electromagnetic spectrum. The aerosol properties in the near-infrared region are used because there is no significant contribution to the satellite-measured radiance from the underlying ocean surface in that spectral region. In the visible wavelength bands, the spectrum of radiation scattered from the turbid atmosphere is convolved with the spectrum of radiation scattered from the surface layers of the ocean. The radiance contribution made by aerosols in the visible bands is determined from the near-infrared measurements through the use of aerosol models and radiation transfer codes. Selection of appropriate aerosol models from the near-infrared measurements is a fundamental challenge. There are several challenges with respect to the development, improvement, and evaluation of satellite ocean-color atmospheric correction algorithms. A common thread among these challenges is the lack of over-ocean aerosol data. Until recently, one of the most important limitations has been the lack of techniques and instruments to make aerosol measurements at sea. There has been steady progress in this area over the past five years, and there are several new and promising devices and techniques for data collection. The development of new instruments and the collection of more aerosol data from over the world's oceans have brought the realization that aerosol measurements that can be directly compared with aerosol measurements from ocean color satellite measurements are difficult to obtain. There are two problems that limit these types of comparisons: the cloudiness of the atmosphere over the world's oceans and the limitations of the techniques and instruments used to collect aerosol data from ships. To address the latter, we have developed a new type of shipboard sun photometer.

Miller, Mark A.↗
NASA NTRS2001

Transport of Aerosols from Asia and Their Radiative Effects Over the Western Pacific: A 3-D Model Study for ACE-Asia Experiment During Spring 2001

The Aerosol Characterization Experiment-Asia (ACE-Asia) took place in Spring 2001 in the East Asia-West Pacific Ocean. During the ACE-Asia intensive field operation period, high concentrations of dust and anthropogenic aerosols were observed over the Yellow Sea and the Sea of Japan, which were transported out from the Asian continent, with the plume often extending to 6-8 km altitude. The multi-component aerosols originated from Asia are expected to exert a significant radiative forcing over the Pacific region. We present here results from the Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model of aerosol transport and radiative forcing in the context of ACE-Asia. The model calculated aerosol concentrations, extinctions, optical thickness, size distributions, and vertical profiles are compared with the aircraft and ship measurements, and the distributions of aerosols are compared with satellite data. The model will be used to understand the origins of the aerosols observed in ACE-Asia, estimate the contributions from anthropogenic and natural aerosols to the total aerosol optical thickness, investigate the effects of humidification and clouds on aerosol properties, and assess the radiative forcing of Asian aerosols over the Pacific region and in the northern hemisphere.

Chin, Mian↗
NASA NTRS1998

Radiative Flux Changes by Aerosols from North America, Europe, and Africa over the Atlantic Ocean: Measurements and Calculations from TARFOX and ACE-2

Aerosol effects on atmospheric radiative fluxes provide a forcing function that is a major source of uncertainty in understanding the past climate and predicting climate change. To help reduce this uncertainty, the 1996 Tropospheric Aerosol Radiative Forcing Experiment (TARFOX) and the 1997 second Aerosol Characterization Experiment (ACE-2) measured the properties and radiative effects of American, European, and African aerosols over the Atlantic. In TARFOX, radiative fluxes and microphysics of the American aerosol were measured from the UK C-130 while optical depth spectra, aerosol composition, and other properties were measured by the University of Washington C-131A and the CIRPAS Pelican. Closure studies show that the measured flux changes agree with those derived from the aerosol measurements using several modelling approaches. The best-fit midvisible single-scatter albedos (approx. 0.89 to 0.93) obtained from the TARFOX flux comparisons are in accord with values derived by independent techniques. In ACE-2 we measured optical depth and extinction spectra for both European urban-marine aerosols and free-tropospheric African dust aerosols, using sunphotometers on the R/V Vodyanitskiy and the Pelican. Preliminary values for the radiative flux sensitivities (Delta Flux / Delta Optical depth) computed for ACE-2 aerosols (boundary layer and African dust) over ocean are similar to those found in TARFOX. Combining a satellite-derived optical depth climatology with the aerosol optical model validated for flux sensitivities in TARFOX provides first-cut estimates of aerosol-induced flux changes over the Atlantic Ocean.

Russell, P. B.↗
NASA NTRS1998

North Atlantic Aerosol Properties and Direct Radiative Effects: Key Results from TARFOX and ACE-2

Aerosol effects on atmospheric radiative fluxes provide a forcing function that can change the climate in potentially significant ways. This aerosol radiative Forcing is a major source of uncertainty in understanding the observed climate change of the past century and in predicting, future climate. To help reduce this uncertainty, the International Global Atmospheric Chemistry Project (IGAC) has endorsed a series of multiplatform aerosol field campaigns. The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the second Aerosol Characterization Experiment (ACE-2) were the first IGAC campaigns to address the impact of anthropogenic aerosols. Both TARFOX and ACE-2 gathered extensive data sets on aerosol properties and radiative effects. TARFOX focused on the urban-industrial haze plume flowing from the eastern United States over the western Atlantic Ocean, whereas ACE-2 studied aerosols carried over the eastern Atlantic from both European urban/industrial and African mineral sources. These aerosols often have a marked influence on the top-of-atmosphere radiances measured by satellites, as illustrated in Figure 1. Shown there are contours of aerosol optical depth derived from radiances measured by the AVHRR sensor on the NOAA-11 satellite. The contours readily show that aerosols originating in North America, Europe, and Africa impact the radiative properties of air over the North Atlantic. However, the accurate derivation of flux chances, or radiative forcing, from the satellite-measured radiances or 'etrieved optical depths remains a difficult challenge. In this paper we summarize key Initial results from TARFOX and, to a lesser extent ACE-2, with a focus on those results that allow an improved assessment of the flux changes caused by North Atlantic aerosols at middle and high latitudes.

Russell, P. B.↗
NASA NTRS2003

Infrared Aerosol Radiative Forcing at the Surface and the Top of the Atmosphere

We study the clear-sky aerosol radiative forcing at infrared wavelengths using data from the Aerosol Characterization Experiment (ACE-Asia) cruise of the NOAA R/V Ronald H. Brown. Limited number of data points is analyzed mostly from ship and collocated satellite values. An optical model is derived from chemical measurements, lidar profiles, and visible extinction measurements which is used to and estimate the infrared aerosol optical thickness and the single scattering albedo. The IR model results are compared to detailed Fourier Transform Interferometer based infrared aerosol forcing estimates, pyrgeometer based infrared downward fluxes, and against the direct solar forcing observations. This combined approach attests for the self-consistency of the optical model and allows to derive quantities such as the infrared forcing at the top of the atmosphere or the infrared optical thickness. The mean infrared aerosol optical thickness at 10 microns is 0.08 and the single scattering albedo is 0.55. The modeled infrared aerosol forcing reaches 10 W/sq m during the cruise, which is a significant contribution to the total direct aerosol forcing. The surface infrared aerosol radiative forcing is between 10 to 25% of the shortwave aerosol forcing. The infrared aerosol forcing at the top of the atmosphere can go up to 19% of the solar aerosol forcing. We show good agreement between satellite (CERES instrument) retrievals and model results at the top of the atmosphere. Over the Sea of Japan, the average infrared radiative forcing is 4.6 W/sq m in the window region at the surface and it is 1.5 W/sq m at top of the atmosphere. The top of the atmosphere IR forcing efficiency is a strong function of aerosol temperature while the surface IR forcing efficiency varies between 37 and 55 W/sq m (per infrared optical depth unit). and changes between 10 to 18 W/sq m (per infrared optical depth unit).

Markowicz, Krzysztof M.↗
NASA NTRS2003

Synergism of MODIS Aerosol Remote Sensing from Terra and Aqua

The MODerate-resolution Imaging Spectro-radiometer (MODIS) sensors, aboard the Earth Observing System (EOS) Terra and Aqua satellites, are showing excellent competence at measuring the global distribution and properties of aerosols. Terra and Aqua were launched on December 18, 1999 and May 4, 2002 respectively, with daytime equator crossing times of approximately 10:30 am and 1:30 pm respectively. Several aerosol parameters are retrieved at 10-km spatial resolution from MODIS daytime data over land and ocean surfaces. The parameters retrieved include: aerosol optical thickness (AOT) at 0.47, 0.55 and 0.66 micron wavelengths over land, and at 0.47, 0.55, 0.66, 0.87, 1.2, 1.6, and 2.1 microns over ocean; Angstrom exponent over land and ocean; and effective radii, and the proportion of AOT contributed by the small mode aerosols over ocean. Since the beginning of its operation, the quality of Terra-MODIS aerosol products (especially AOT) have been evaluated periodically by cross-correlation with equivalent data sets acquired by ground-based (and occasionally also airborne) sunphotometers, particularly those coordinated within the framework of the AErosol Robotic NETwork (AERONET). Terra-MODIS AOT data have been found to meet or exceed pre-launch accuracy expectations, and have been applied to various studies dealing with local, regional, and global aerosol monitoring. The results of these Terra-MODIS aerosol data validation efforts and studies have been reported in several scientific papers and conferences. Although Aqua-MODIS is still young, it is already yielding formidable aerosol data products, which are also subjected to careful periodic evaluation similar to that implemented for the Terra-MODIS products. This paper presents results of validation of Aqua-MODIS aerosol products with AERONET, as well as comparative evaluation against corresponding Terra-MODIS data. In addition, we show interesting independent and synergistic applications of MODIS aerosol data from both Terra and Aqua. In certain situations, this combined analysis of Terra- and Aqua-MODIS data offers an insight into the diurnal cycle of aerosol loading.

Ichoku, Charles↗
NASA NTRS2004

In-Situ Measurements of Aerosol Optical Properties using New Cavity Ring-Down and Photoacoustics Instruments and Comparison with more Traditional Techniques

Carbonaceous species (BC and OC) are responsible for most of the absorption associated with aerosol particles. The amount of radiant energy an aerosol absorbs has profound effects on climate and air quality. It is ironic that aerosol absorption coefficient is one of the most difficult aerosol properties to measure. A new cavity ring-down (CRD) instrument, called Cadenza (NASA-ARC), measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. Absorption coefficient is obtained from the difference of measured extinction and scattering within the instrument. Aerosol absorption coefficient is also measured by a photoacoustic (PA) instrument (DRI) that was operated on an aircraft for the first time during the DOE Aerosol Intensive Operating Period (IOP). This paper will report on measurements made with this new instrument and other in-situ instruments during two field recent field studies. The first field study was an airborne cam;oaign, the DOE Aerosol Intensive Operating Period flown in May, 2003 over northern Oklahoma. One of the main purposes of the IOP was to assess our ability to measure extinction and absorption coefficient in situ. This paper compares measurements of these aerosol optical properties made by the CRD, PA, nephelometer, and Particle Soot Absorption Photometer (PSAP) aboard the CIRPAS Twin-Otter. During the IOP, several significant aerosol layers were sampled aloft. These layers are identified in the remote (AATS-14) as well as in situ measurements. Extinction profiles measured by Cadenza are compared to those derived from the Ames Airborne Tracking Sunphotometer (AATS-14, NASA-ARC). The regional radiative impact of these layers is assessed by using the measured aerosol optical properties in a radiative transfer model. The second study was conducted in the Caldecott Tunnel, a heavily-used tunnel located north of San Francisco, Ca. The aerosol sampled in this study was characterized by fresh automobile and diesel exhaust. Measurements from Cadenza and from an aethalometer are presented. The aethalometer is a filter-based photometer and the infrared channel is calibrated to produce a measure of BC mass loading.

Strawa, A. W.↗
NASA NTRS2004

A New, More Physically Based Algorithm, for Retrieving Aerosol Properties over Land from MODIS

The MOD Imaging Spectrometer (MODIS) has been successfully retrieving aerosol properties, beginning in early 2000 from Terra and from mid 2002 from Aqua. Over land, the retrieval algorithm makes use of three MODIS channels, in the blue, red and infrared wavelengths. As part of the validation exercises, retrieved spectral aerosol optical thickness (AOT) has been compared via scatterplots against spectral AOT measured by the global Aerosol Robotic NETwork (AERONET). On one hand, global and long term validation looks promising, with two-thirds (average plus and minus one standard deviation) of all points falling between published expected error bars. On the other hand, regression of these points shows a positive y-offset and a slope less than 1.0. For individual regions, such as along the U.S. East Coast, the offset and slope are even worse. Here, we introduce an overhaul of the algorithm for retrieving aerosol properties over land. Some well-known weaknesses in the current aerosol retrieval from MODIS include: a) rigid assumptions about the underlying surface reflectance, b) limited aerosol models to choose from, c) simplified (scalar) radiative transfer (RT) calculations used to simulate satellite observations, and d) assumption that aerosol is transparent in the infrared channel. The new algorithm attempts to address all four problems: a) The new algorithm will include surface type information, instead of fixed ratios of the reflectance in the visible channels to the mid-IR reflectance. b) It will include updated aerosol optical properties to reflect the growing aerosol retrieved from eight-plus years of AERONE". operation. c) The effects of polarization will be including using vector RT calculations. d) Most importantly, the new algorithm does not assume that aerosol is transparent in the infrared channel. It will be an inversion of reflectance observed in the three channels (blue, red, and infrared), rather than iterative single channel retrievals. Thus, this new formulation of the MODIS aerosol retrieval over land includes more physically based surface, aerosol and radiative transfer with fewer potentially erroneous assumptions.

Levy, Robert C.↗
NASA NTRS2005

Effects of Aerosol on Atmospheric Dynamics and Hydrologic Processes during Boreal Spring and Summer

Global and regional climate impacts of present-day aerosol loading during boreal spring are investigated using the NASA finite volume General Circulation Model (fvGCM). Three-dimensional distributions of loadings of five species of tropospheric aerosols, i.e., sulfate, black carbon, organic carbon, soil dust, and sea salt are prescribed from outputs of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol loadings are used to calculate the extinction coefficient, single scattering albedo, and asymmetric factor at eleven spectral wavelengths in the radiative transfer code. We find that aerosol-radiative forcing during boreal spring excites a wavetrain-like pattern in tropospheric temperature and geopotential height that emanates from Northern Africa, through Eurasia, to northeastern Pacific. Associated with the teleconnection is strong surface cooling over regions with large aerosol loading, i.e., China, India, and Africa. Low-to-mid tropospheric heating due to shortwave absorption is found in regions with large loading of dust (Northern Africa, and central East Asia), and black carbon (South and East Asia). In addition pronounced surface cooling is found over the Caspian Sea and warming over Eurasian and northeastern Asia, where aerosol loadings are relatively low. These warming and cooling are components of teleconnection pattern produced primarily by atmospheric heating from absorbing aerosols, i.e., dust from North Africa and.black carbon from South and East Asia. Effects of aerosols on atmospheric hydrologic cycle in the Asian monsoon region are also investigated. Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in an early onset of the Indian summer monsoon. Absorbing aerosols also enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol-induced large-scale surface temperature cooling leads to a reduction of monsoon rainfall over the East Asia continent, and adjacent oceanic regions.

Lau, William K. M.↗