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At least 73 records · Page 4

Direct measurement of small particle growth and aging at SGP

Atmospheric aerosols influence climate directly by scattering and absorbing solar radiation and indirectly through their influence on the reflectivity and lifetime of clouds. But that influence is limited to only those particles large enough to efficiently interact with solar radiation (diameter, D p ≳ 100 nm) and/or to form cloud droplets at typical atmospheric supersaturations (D p ≳ 50 nm). Many cloud condensation nuclei (CCN) originate as ~1 nm nucleated particles that must grow to those threshold sizes before being lost to coagulation with larger particles. Though there is consensus that new particle formation and growth contributes significantly to total CCN concentrations, different groups using different models and assumptions have arrived at diverse estimates.

54 ENVIRONMENTAL SCIENCES↗

Backscatter laser depolarization studies of simulated stratospheric aerosols: Crystallized sulfuric acid droplets

The optical depolarizing properties of simulated stratospheric aerosols were studied in laboratory laser (0.633 micrometer) backscattering experiments for application to polarization lidar observations. Clouds composed of sulfuric acid solution droplets, some treated with ammonia gas, were observed during evaporation. The results indicate that the formation of minute ammonium sulfate particles from the evaporation of acid droplets produces linear depolarization ratios of beta equivalent to 0.02, but beta equivalent to 0.10 to 0.15 are generated from aged acid cloud aerosols and acid droplet crystallization effects following the introduction of ammonia gas into the chamber. It is concluded that partially crystallized sulfuric acid droplets are a likely candidate for explaining the lidar beta equivalent to 0.10 values that have been observed in the lower stratosphere in the absence of the relatively strong backscattering from homogeneous sulfuric acid droplet (beta equivalent to 0) or ice crystal (beta equivalent to 0.5) clouds.

Sassen, Kenneth↗

Backscatter laser depolarization studies of simulated stratospheric aerosols - Crystallized sulfuric acid droplets

The optical depolarizing properties of simulated stratospheric aerosols were studied in laboratory laser (0.633 micrometer) backscattering experiments for application to polarization lidar observations. Clouds composed of sulfuric acid solution droplets, some treated with ammonia gas, were observed during evaporation. The results indicate that the formation of minute ammonium sulfate particles from the evaporation of acid droplets produces linear depolarization ratios of beta equivalent to 0.02, but beta equivalent to 0.10 to 0.15 are generated from aged acid cloud aerosols and acid droplet crystalization effects following the introduction of ammonia gas into the chamber. It is concluded that partially crystallized sulfuric acid droplets are a likely candidate for explaining the lidar beta equivalent to 0.10 values that have been observed in the lower stratosphere in the absence of the relatively strong backscattering from homogeneous sulfuric acid droplet (beta equivalent to 0) or ice crystal (beta equivalent to 0.5) clouds.

Sassen, Kenneth↗

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↗

The Extreme Forest Fires in California/Oregon in 2020: Aerosol Optical and Physical Properties and Comparisons of Aged Versus Fresh Smoke

Wildfire activity in the western United States during August to October 2020 was exceptional in terms of the fire severity and area burned. Extremely dry biomass fuels from near historic multi-year drought conditions were further exacerbated with very hot and dry conditions in 2020. These conditions when coupled with strong offshore flow allowed many ignitions to grow into extremely large and severe wildfires. Long-term monitoring at a few AERONET sites in California showed that the number of days with high Aerosol Optical Depth at 440 nm (AOD 440 >1) in 2020 was greater than any other year going back to the beginning of the data records in 2002. A wide range of fine mode particle volume median radii were retrieved from AERONET data over the course of these fires suggesting significant variability in combustion conditions and aging processes. Additionally, the fine mode radii in some of these smoke plumes in 2020 were very large especially at high AOD (∼0.22–0.32 μm volume median radius), likely due to both coagulation and condensation occurring during aging at very high particulate concentrations. The largest fine mode particle radii combined with narrow distributions resulted in some very rare AOD spectra showing peak AOD at 500 nm and decreasing to lower AOD at both shorter and longer wavelengths. The most extreme retrieved size distributions and associated measured AOD spectra were principally observed in long-distance transported smoke plumes from these western United States fires at sites in Colorado, Maryland and Virginia, possibly due to further aging during transport. Additionally, strong absorption was sometimes observed at short wavelengths with much lower single scattering albedo at 440 nm compared to 675 nm in some plumes consistent with significant brown carbon (BrC) and/or coated black carbon (BC) absorption in biomass burning particles. This strong spectral absorption signature observed at some California sites and dates remained similarly strong in some smoke plumes observed at some east coast sites in Maryland and Virginia, thereby suggesting that the lifetime of these particular BrC and/or coated BC absorbing species was greater than 5 days.

Aerosol↗

Wildfire smoke triggers cirrus formation: lidar observations over the eastern Mediterranean

The number of intense wildfires may increase further in upcoming years as a consequence of climate change. It is therefore necessary to improve our knowledge about the role of smoke in the climate system, with emphasis on the impact of smoke particles on the evolution of clouds, precipitation, and cloud radiative properties. Presently, one key aspect of research is whether or not wildfire smoke particles can initiate cirrus formation. In this study, we present lidar observations over Limassol, Cyprus, from 27 October to 3 November 2020, when extended wildfire smoke fields crossed the Mediterranean Basin from Portugal to Cyprus. We found strong evidence that aged smoke (organic aerosol particles) originating from wildfires in North America triggered significant ice nucleation at temperatures from -47 to -53 °C and caused the formation of extended cirrus layers. The observations suggest that the ice crystals were nucleated just below the tropopause in the presence of smoke particles serving as ice-nucleating particles (INPs). The main part of the 2–3 km thick smoke layer was, however, in the lower stratosphere just above the tropopause. With actual radiosonde observations of temperature and relative humidity and lidar-derived smoke particle surface area concentrations used as starting values, gravity wave simulations show that the lofting of air by 100–200 m is sufficient to initiate significant ice nucleation on the smoke particles, leading to ice crystal number concentrations of 1–100 L -1 .

54 ENVIRONMENTAL SCIENCES↗

Alternative Aviation Fuel Experiment (AAFEX)

The rising cost of oil coupled with the need to reduce pollution and dependence on foreign suppliers has spurred great interest and activity in developing alternative aviation fuels. Although a variety of fuels have been produced that have similar properties to standard Jet A, detailed studies are required to ascertain the exact impacts of the fuels on engine operation and exhaust composition. In response to this need, NASA acquired and burned a variety of alternative aviation fuel mixtures in the Dryden Flight Research Center DC-8 to assess changes in the aircraft s CFM-56 engine performance and emission parameters relative to operation with standard JP-8. This Alternative Aviation Fuel Experiment, or AAFEX, was conducted at NASA Dryden s Aircraft Operations Facility (DAOF) in Palmdale, California, from January 19 to February 3, 2009 and specifically sought to establish fuel matrix effects on: 1) engine and exhaust gas temperatures and compressor speeds; 2) engine and auxiliary power unit (APU) gas phase and particle emissions and characteristics; and 3) volatile aerosol formation in aging exhaust plumes

Anderson, B. E.↗

Controlled Nitric Oxide Production via O(1D) + N2O Reactions for Use in Oxidation Flow Reactor Studies

Oxidation flow reactors that use low-pressure mercury lamps to produce hydroxyl (OH) radicals are an emerging technique for studying the oxidative aging of organic aerosols. Here, ozone (O3) is photolyzed at 254 nm to produce O(1D) radicals, which react with water vapor to produce OH. However, the need to use parts-per-million levels of O3 hinders the ability of oxidation flow reactors to simulate NOx-dependent secondary organic aerosol (SOA) formation pathways. Simple addition of nitric oxide (NO) results in fast conversion of NOx (NO+NO2) to nitric acid (HNO3), making it impossible to sustain NOx at levels that are sufficient to compete with hydroperoxy (HO2) radicals as a sink for organic peroxy (RO2) radicals. We developed a new method that is well suited to the characterization of NOx-dependent SOA formation pathways in oxidation flow reactors. NO and NO2 are produced via the reaction O(1D)+N2O->2NO, followed by the reaction NO+O3->NO2+O2. Laboratory measurements coupled with photochemical model simulations suggest that O(1D)+N2O reactions can be used to systematically vary the relative branching ratio of RO2 +NO reactions relative to RO2 +HO2 and/or RO2+RO2 reactions over a range of conditions relevant to atmospheric SOA formation. We demonstrate proof of concept using high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) measurements with nitrate (NO-3 ) reagent ion to detect gas-phase oxidation products of isoprene and -pinene previously observed in NOx-influenced environments and in laboratory chamber experiments.

Lambe, Andrew↗

MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

volatility-basis set↗

The Present and Future of Secondary Organic Aerosol Direct Forcing on Climate

Secondary organic aerosols (SOA), a subset of organic aerosols that are chemically produced in the atmosphere, are included in climate modeling calculations using very simple parameterizations. Estimates on their shortwave forcing on climate span almost two orders of magnitude, being potentially comparable to sulfate direct forcing. In the longwave, a neglected part of the spectrum when it comes to SOA, the direct SOA forcing could exceed that of sulfate and black carbon, although in absolute values it is much weaker than the shortwave forcing. Critical for these estimates is the vertical distribution of the climate active agents, pointing to SOA temperature-dependent volatility. Over the last few years, research also revealed the highly oxidized character of organic aerosol and its chemical aging in the atmosphere that partially leads to the formation of brown carbon, an absorbing form of organic aerosol. This review summarizes critical advances in the understanding of SOA behavior and properties relevant to direct climate forcing and puts them in perspective with regard to primary organic aerosol and brown carbon. These findings also demonstrate an emerging dynamic picture of organic aerosol that has not yet been integrated in climate modeling. The challenges for the coming years in order to reduce uncertainties in the direct organic aerosol climate impact are discussed. High priority for future model development should be given to the dynamic link between “white” and “brown” organic aerosol and between primary and secondary organic aerosol. The SOA temperature-dependent volatility parameterizations and wavelength-dependent refractive index should be also included.

Kostas Tsigaridis↗

Source apportionment of soot particles and aqueous-phase processing of black carbon coatings in an urban environment

Abstract. The impacts of soot particles on climate and human health depend on the concentration of black carbon (BC) as well as the thickness and composition of the coating material, i.e., organic and inorganic compounds internally mixed with BC. In this study, the size-resolved chemical composition of BC-containing aerosol was measured using a high-resolution soot particle aerosol mass spectrometer (SP-AMS) during wintertime in Fresno, California, a location influenced by abundant combustion emissions and frequent fog events. Concurrently, particle optical properties were measured to investigate the BC absorption enhancement. Positive matrix factorization (PMF) analysis was performed on the SP-AMS mass spectral measurements to explore the sources of soot particles and the atmospheric processes affecting the properties of BC coatings. The analysis revealed that residential woodburning and traffic are the dominant sources of soot particles. Alongside primary soot particles originating from biomass burning (BBOABC) and vehicles (HOABC) two distinct types of processed BC-containing aerosol were identified: fog-related oxidized organic aerosol (FOOABC) and winter-background OOABC (WOOABC). Both types of OOABC showed evidence of having undergone aqueous processing, albeit with differences. The concentration of FOOABC was substantially elevated during fog events, indicating the formation of aqueous secondary organic aerosol (aqSOA) within fog droplets. On the other hand, WOOABC was present at a relatively consistent concentration throughout the winter and was likely related to the formation of secondary organic aerosol (SOA) in both the gas phase and aerosol liquid water. By comparing the chemical properties and temporal variations in FOOABC and WOOABC, we gain insights into the key aging processes of BC aerosol. It was found that aqueous-phase reactions facilitated by fog droplets had a significant impact on the thickness and chemical composition of BC coatings, thereby affecting the light absorption and hygroscopic properties of soot particles. These findings underscore the important role of chemical reactions occurring within clouds and fogs and influencing the climate forcing of BC aerosol in the atmosphere.

54 ENVIRONMENTAL SCIENCES↗

Differences in the Evolution of Pyrocumulonimbus and Volcanic Stratospheric Plumes as Observed by CATS and CALIOP Space-Based Lidars

Recent fire seasons have featured volcanic-sized injections of smoke aerosols into the stratosphere where they persist for many months. Unfortunately, the aging and transport of these aerosols are not well understood. Using space-based lidar, the vertical and spatial propagation of these aerosols can be tracked and inferences can be made as to their size and shape. In this study, space-based CATS and CALIOP lidar were used to track the evolution of the stratospheric aerosol plumes resulting from the 2019–2020 Australian bushfire and 2017 Pacific Northwest pyrocumulonimbus events and were compared to two volcanic events: Calbuco (2015) and Puyehue (2011). The pyrocumulonimbus and volcanic aerosol plumes evolved distinctly, with pyrocumulonimbus plumes rising upwards of 10 km after injection to altitudes of 30 km or more, compared to small to modest altitude increases in the volcanic plumes. We also show that layer-integrated depolarization ratios in these large pyrocumulonimbus plumes have a strong altitude dependence with more irregularly shaped particles in the higher altitude plumes, unlike the volcanic events studied.

Kenneth Christian↗

Similarities in the Lidar-Observed Optical Properties in the 2020 Australian Bushfire PyroCb and the 2017 Pacific Northwest PyroCb Stratospheric Plumes

Recent fire seasons have featured volcanic-sized injections of smoke aerosols into the stratosphere where they persist for many months. Unfortunately, the aging and transport of these aerosols are not well understood. Using space-based lidar, the vertical and spatial propagation of these aerosol layers can be tracked and inferences can be made as to the size and shape of the constituent aerosol particles. In this study, space-based CALIOP and CATS lidar were used to track the evolution of the stratospheric aerosol plumes resulting from the 2019 - 2020 Australian bushfire and 2017 Pacific Northwest pyrocumulonimbus events and were compared to two volcanic events: Calbuco (2015) and Puyehue (2011) and two smaller pyrocumulonimbus events: California’s Rim Fire (2013) and Australia’s Black Saturday (2009). The aerosol plumes from the large pyrocumulonimbus events rose many kilometers in the stratosphere in the weeks after injection to upwards of 30km in altitude. The layer-integrated depolarization ratios and color ratios of the 2020 Australian bushfire and 2017 Pacific Northwest pyrocumulonimbus plumes both vary by altitude with the lidar-measured depolarization and color ratios indicating the higher altitude aerosol layers contain smaller and more irregularly shaped aerosol particles. This relationship between altitude and optical properties was not observed in the smaller pyrocumulonimbus or the volcanic event stratospheric plumes.

Kenneth Christian↗

An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June-October), aerosol particles reaching 3-5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

54 ENVIRONMENTAL SCIENCES↗

An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Southern Africa produces almost a third of the Earth’s biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~ 350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~ 100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

Jens Redemann↗