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At least 577 records · Page 32

Estimation of Sea Spray Aerosol Surface Area Over the Southern Ocean Using Scattering Measurements

This study focuses on methods to estimate dry marine aerosol surface area (SA) from bulk optical measurements. Aerosol SA is used in many models' ice nucleating particle (INP) parameterizations, as well as influencing particle light scattering, hygroscopic growth, and reactivity, but direct observations are scarce in the Southern Ocean (SO). Two campaigns jointly conducted in austral summer 2018 provided co-located measurements of aerosol SA from particle size distributions and lidar to evaluate SA estimation methods in this region. Mie theory calculations based on measured size distributions were used to test a proposed approximation for dry aerosol SA, which relies on estimating effective scattering efficiency (Q) as a function of Ångström exponent (å). For distributions with dry å < 1, Q = 2 was found to be a good approximation within ±50%, but for distributions with dry å > 1, an assumption of Q = 3 as in some prior studies underestimates dry aerosol SA by a factor of 2 or more. We propose a new relationship between dry å and Q, which can be used for –0.2 < å < 2, and suggest å = 0.8 as the cutoff between primary and secondary marine aerosol-dominated distributions. Application of a published methodology to retrieve dry marine aerosol SA from lidar extinction profiles overestimated aerosol SA by a factor of 3–5 during these campaigns. Using Microtops aerosol optical thickness measurements, we derive alternative lidar conversion parameters from our observations, applicable to marine aerosol over the SO.

54 ENVIRONMENTAL SCIENCES↗

The Role of In-Cloud Wet Removal in Simulating Aerosol Vertical Profiles and Cloud Radiative Forcing

Among the physical processes controlling aerosol vertical profiles, in-cloud wet removal is of utmost importance while its representation in global climate models (GCMs) is crude. In this study, we implement into the Community Atmosphere Model version 6 (CAM6) a physically based aerosol wet removal parameterization scheme that explicitly treats aerosol activation, removal and resuspension. Evaluation against in-situ observations shows that the default scheme substantially overestimates the upper tropospheric black carbon (BC) and sea salt mass. Our physically based scheme reduces BC and sea salt mass by a factor of 10 and 1,000, respectively, in better agreement with observations. Also, the new scheme slightly increases number of aerosol particles between 12 nm and 4.8 μm in diameter, thereby mitigating the aerosol number underestimation in the default scheme. Our new scheme reduces the overestimation of coarse-mode aerosol (0.5–4.8 μm) number. Overall, the aerosol property changes (mass decrease and number increase) reduce the cloud condensation nuclei (CCN) concentration at low supersaturation (i.e., 0.02% and 0.1%), and increase CCN at high supersaturations (i.e., 0.5% and 1%). Consequently, the global annual mean cloud liquid water path increases by 1.89 g m -2 and the ice water path increases by 0.51 g m -2 . The global annual mean shortwave, longwave, and net cloud radiative forcing change by -1.06, 0.57, and -0.48 W m -2 , respectively. Further improvement is needed to reflect the real physics that the removal efficiencies for aerosol mass and number are disproportionate and to advect cloud-borne (activated) aerosols for a complete aerosol lifecycle.

54 ENVIRONMENTAL SCIENCES↗

Polar primary aerosols across the ocean-sea ice-snow-atmosphere interface: From sources to impacts

Primary aerosols play a critical role in polar climate systems, influencing cloud formation, precipitation, radiative balance, and surface energy budgets. This paper provides a comprehensive synthesis of primary aerosol sources, transformation and removal processes, and broader atmospheric impacts in polar regions, emphasizing their links to ocean and sea ice biogeochemistry. These aerosols (including sea salt, primary organic aerosol, and primary biological aerosol particles) originate from marine and cryospheric environments and are emitted through physical processes, such as wave breaking, bubble bursting, and blowing snow. Emission sources include seawater, sea ice, snow, and freshwater from river discharge and glacial runoff. Once airborne, these particles can serve as a chemical reservoir, influencing atmospheric composition and reactivity, and as seeds for cloud droplet and ice crystal formation, influencing cloud microphysics and polar climate. Despite their importance, many of the processes governing primary aerosol emissions and transformations remain poorly constrained. The most pressing knowledge gaps pertain to emission processes, limited spatiotemporal observational coverage, instrumentation constraints, parameterization development, and the integration of interdisciplinary expertise. To improve our understanding of primary aerosol drivers and their response to climate, future research efforts should prioritize strategically coordinated and cross-disciplinary process studies, advancements in measurement technologies and coverage, and close collaboration between modelers and observational scientists to inform and refine model parameterizations. As polar regions continue to undergo profound changes marked by increased precipitation, reduced sea and land ice, freshening oceans, and shifting ecosystem dynamics, characterizing present-day primary aerosol populations is vital. Improved understanding will be essential for anticipating future changes in aerosol-radiation and aerosol-cloud interactions and their implications for polar and global climate systems.

Aerosol-cloud↗

Elevated Aerosol Layers and Their Radiative Impact over Kanpur During Monsoon Onset Period

Accurate information about aerosol vertical distribution is needed to reduce uncertainties in aerosol radiative forcing and its effect on atmospheric dynamics. The present study deals with synergistic analyses of aerosol vertical distribution and aerosol optical depth (AOD) with meteorological variables using multisatellite and ground-based remote sensors over Kanpur in central Indo-Gangetic Plain (IGP). Micro-Pulse Lidar Network-derived aerosol vertical extinction (sigma) profiles are analyzed to quantify the interannual and daytime variations during monsoon onset period (May-June) for 2009-2011. The mean aerosol profile is broadly categorized into two layers viz., a surface layer (SL) extending up to 1.5 km (where sigma decreased exponentially with height) and an elevated aerosol layer (EAL) extending between 1.5 and 5.5 km. The increase in total columnar aerosol loading is associated with relatively higher increase in contribution from EAL loading than that from SL. The mean contributions of EALs are about 60%, 51%, and 50% to total columnar AOD during 2009, 2010, and 2011, respectively. We observe distinct parabolic EALs during early morning and late evening but uniformly mixed EALs during midday. The interannual and daytime variations of EALs are mainly influenced by long-range transport and convective capacity of the local emissions, respectively. Radiative flux analysis shows that clear-sky incoming solar radiation at surface is reduced with increase in AOD, which indicates significant cooling at surface. Collocated analysis of atmospheric temperature and aerosol loading reveals that increase in AOD not only resulted in surface dimming but also reduced the temperature (approximately 2-3 C) of lower troposphere (below 3 km altitude). Radiative transfer simulations indicate that the reduction of incoming solar radiation at surface is mainly due to increased absorption by EALs (with increase in total AOD). The observed cooling in lower troposphere in high aerosol loading scenario could be understood as a dynamical feedback of EAL-induced stratification of lower troposphere. Further, the observed radiative effect of EALs increases the stability of the lower troposphere, which could modulate the large-scale atmospheric dynamics during monsoon onset period. These findings encourage follow-up studies on the implication of EALs to the Indian summer monsoon dynamics using numerical models.

aerosol vertical distribution↗

Influence of Cloud, Fog, and High Relative Humidity during Pollution Transport Events in South Korea: Aerosol Properties and PM2.5 Variability

This investigation examines aerosol dynamics during major fine mode aerosol transboundary pollution events in South Korea primarily during the KORUS-AQ campaign from May 1 – June 10, 2016, particularly when cloud fraction was high and/or fog was present to quantify the change in aerosol characteristics due to near-cloud or fog interaction. We analyze the new AERONET Version 3 data that have significant changes to cloud screening algorithms, allowing many more fine-mode observations in the near vicinity of clouds or fog. Case studies for detailed investigation include May 25–26, 2016 when cloud fraction was high over much of the peninsula, associated with a weak frontal passage and advection of pollution from China. These cloud-influenced Chinese transport dates also had the highest aerosol optical depth (AOD), surface PM2.5 concentrations and fine mode particle sizes of the entire campaign. Another likewise cloud/high relative humidity (RH) case is June 9 and 10, 2016 when fog was present over the Yellow Sea that appears to have affected aerosol properties well downwind over the Korean peninsula. In comparison we also investigated aerosol properties on air stagnation days with very low cloud cover and relatively low RH (May 17 & 18, 2016), when local Korean emissions dominated. Aerosol volume size distributions show marked differences between the transport days (with high RH and cloud influences) and the local pollution stagnation days, with total column-integrated particle fine mode volume being an order of magnitude greater on the pollution transport dates. The PM2.5 over central Seoul were significantly greater than for coastal sites on the transboundary transport days yet not on stagnation days, suggesting addi-tional particle formation from gaseous urban emissions in cloud/fog droplets and/or in the high RH humidified aerosol environment. Many days had KORUS-AQ research aircraft flights that provided observations of aerosol absorption, particle chemistry and vertical profiles of extinction. AERONET retrievals and aircraft in situ mea-surements both showed high single scattering albedo (weak absorption) on the cloudy or cloud influenced days, plus aircraft profile in situ measurements showed large AOD enhancements (versus dried aerosol) at ambient relative humidity (RH) on the pollution transport days, consistent with the significantly larger fine mode particle radii and weak absorption.

Aerosol↗

Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE) Science Plan

Coastal cities provide the opportunity to characterize marine clouds and the substantial effects of manmade particles on cloud properties and processes. La Jolla lies to the north of San Diego, California, but it is often about a day directly downwind of the major pollution sources located in the ports of Los Angeles and Long Beach. The large dynamic range of aerosol particle concentrations combined with the multi-hour to multi-day persistence of stratocumulus cloud layers makes the site ideal for investigating the seasonal changes in cloud and aerosol properties as well as the quantitative relationships between cloud and aerosol properties. The focus of the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE) is to characterize the extent, radiative properties, aerosol interactions, and precipitation characteristics of stratocumulus clouds in the Eastern Pacific across all four seasons at a coastal location, the Scripps Pier and the Scripps Mt. Soledad sites in La Jolla. An important enhancement to this study will be the collection of simultaneous in-cloud aerosol and droplet measurements to investigate the differences in these cloud properties during regional polluted and clean marine conditions. The combined observations will provide an unprecedented set of constraints for the following questions: 1. Cloud and Aerosol Climatology: What are the seasonal and diurnal cycles of marine stratocumulus cloud and aerosol properties on the northeastern Pacific coast? 2. Cloud Radiative Fluxes: How do cloud properties, including the ratio of direct-to-diffuse radiation, change as coastal clouds are advected inland? 3. Aerosol-Cloud Interactions: Will retrieved cloud properties reflect the regional signatures of aerosol?

Eastern Pacific Cloud Aerosol Precipitation Experi↗

Modeling Novel Aqueous Particle and Cloud Chemistry Processes of Biomass Burning Phenols and Their Potential to Form Secondary Organic Aerosols

Phenols emitted from biomass burning contribute significantly to secondary organic aerosol (SOA) formation through the partitioning of semivolatile products formed from gas-phase chemistry and multiphase chemistry in aerosol liquid water and clouds. The aqueous-phase SOA (aqSOA) formed via hydroxyl radical (˙OH), singlet molecular oxygen ( 1 O 2 *), and triplet excited states of organic compounds ( 3 C*), which oxidize dissolved phenols in the aqueous phase, might play a significant role in the evolution of organic aerosol (OA). However, a quantitative and predictive understanding of aqSOA has been challenging. Here, we develop a stand-alone box model to investigate the formation of SOA from gas-phase ˙OH chemistry and aqSOA formed by the dissolution of phenols followed by their aqueous-phase reactions with ˙OH, 1 O 2 *, and 3 C* in cloud droplets and aerosol liquid water. Here, we investigate four phenolic compounds, i.e., phenol, guaiacol, syringol, and guaiacyl acetone (GA), which represent some of the key potential sources of aqSOA from biomass burning in clouds. For the same initial precursor organic gas that dissolves in aerosol/cloud liquid water and subsequently reacts with aqueous phase oxidants, we predict that the aqSOA formation potential (defined as aqSOA formed per unit dissolved organic gas concentration) of these phenols is higher than that of isoprene-epoxydiol (IEPOX), a well-known aqSOA precursor. Cloud droplets can dissolve a broader range of soluble phenols compared to aqueous aerosols, since the liquid water contents of aerosols are orders of magnitude smaller than cloud droplets. Further, our simulations suggest that highly soluble and reactive multifunctional phenols like GA would predominantly undergo cloud chemistry within cloud layers, while gas-phase chemistry is likely to be more important for less soluble phenols. But in the absence of clouds, the condensation of low-volatility products from gas-phase oxidation followed by their reversible partitioning to organic aerosols dominates SOA formation, while the SOA formed through aqueous aerosol chemistry increases with relative humidity (RH), approaching 40% of the sum of gas and aqueous aerosol chemistry at 95% RH for GA. Our model developments of biomass-burning phenols and their aqueous chemistry can be readily implemented in regional and global atmospheric chemistry models to investigate the aqueous aerosol and cloud chemistry of biomass-burning organic gases in the atmosphere.

09 BIOMASS FUELS↗

Correcting for filter-based aerosol light absorption biases at the Atmospheric Radiation Measurement program's Southern Great Plains site using photoacoustic measurements and machine learning

Abstract. Measurement of light absorption of solar radiation by aerosols is vital for assessing direct aerosol radiative forcing, which affects local and global climate. Low-cost and easy-to-operate filter-based instruments, such as the Particle Soot Absorption Photometer (PSAP), that collect aerosols on a filter and measure light attenuation through the filter are widely used to infer aerosol light absorption. However, filter-based absorption measurements are subject to artifacts that are difficult to quantify. These artifacts are associated with the presence of the filter medium and the complex interactions between the filter fibers and accumulated aerosols. Various correction algorithms have been introduced to correct for the filter-based absorption coefficient measurements toward predicting the particle-phase absorption coefficient (Babs). However, the inability of these algorithms to incorporate into their formulations the complex matrix of influencing parameters such as particle asymmetry parameter, particle size, and particle penetration depth results in prediction of particle-phase absorption coefficients with relatively low accuracy. The analytical forms of corrections also suffer from a lack of universal applicability: different corrections are required for rural and urban sites across the world. In this study, we analyzed and compared 3 months of high-time-resolution ambient aerosol absorption data collected synchronously using a three-wavelength photoacoustic absorption spectrometer (PASS) and PSAP. Both instruments were operated on the same sampling inlet at the Department of Energy's Atmospheric Radiation Measurement program's Southern Great Plains (SGP) user facility in Oklahoma. We implemented the two most commonly used analytical correction algorithms, namely, Virkkula (2010) and the average of Virkkula (2010) and Ogren (2010)–Bond et al. (1999) as well as a random forest regression (RFR) machine learning algorithm to predict Babs values from the PSAP's filter-based measurements. The predicted Babs was compared against the reference Babs measured by the PASS. The RFR algorithm performed the best by yielding the lowest root mean square error of prediction. The algorithm was trained using input datasets from the PSAP (transmission and uncorrected absorption coefficient), a co-located nephelometer (scattering coefficients), and the Aerosol Chemical Speciation Monitor (mass concentration of non-refractory aerosol particles). A revised form of the Virkkula (2010) algorithm suitable for the SGP site has been proposed; however, its performance yields approximately 2-fold errors when compared to the RFR algorithm. To generalize the accuracy and applicability of our proposed RFR algorithm, we trained and tested it on a dataset of laboratory measurements of combustion aerosols. Input variables to the algorithm included the aerosol number size distribution from the Scanning Mobility Particle Sizer, absorption coefficients from the filter-based Tricolor Absorption Photometer, and scattering coefficients from a multiwavelength nephelometer. The RFR algorithm predicted Babs values within 5 % of the reference Babs measured by the multiwavelength PASS during the laboratory experiments. Thus, we show that machine learning approaches offer a promising path to correct for biases in long-term filter-based absorption datasets and accurately quantify their variability and trends needed for robust radiative forcing determination.

54 ENVIRONMENTAL SCIENCES↗

Radiative Forcing of the Direct Aerosol Effect from AeroCom Phase II Simulations

We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 16 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from −0.58 to −0.02 W m(sup−2), with a mean of −0.27 W m(sup−2 for the 16 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of −0.35 W m(sup−2). Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study.We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results

Computer simulation↗

The Messy Aerosol Submodel MADE3 (v2.0b): Description and a Box Model Test

We introduce MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, 3rd generation), an aerosol dynamics submodel for application within the MESSy framework (Modular Earth Submodel System). MADE3 builds on the predecessor aerosol submodels MADE and MADE-in. Its main new features are the explicit representation of coarse particle interactions both with other particles and with condensable gases, and the inclusion of hydrochloric acid (HCl)chloride (Cl) partitioning between the gas and condensed phases. The aerosol size distribution is represented in the new submodel as a superposition of nine lognormal modes: one for fully soluble particles, one for insoluble particles, and one for mixed particles in each of three size ranges (Aitken, accumulation, and coarse mode size ranges). In order to assess the performance of MADE3 we compare it to its predecessor MADE and to the much more detailed particle-resolved aerosol model PartMC-MOSAIC in a box model simulation of an idealized marine boundary layer test case. MADE3 and MADE results are very similar, except in the coarse mode, where the aerosol is dominated by sea spray particles. Cl is reduced in MADE3 with respect to MADE due to the HClCl partitioning that leads to Cl removal from the sea spray aerosol in our test case. Additionally, aerosol nitrate concentration is higher in MADE3 due to the condensation of nitric acid on coarse particles. MADE3 and PartMC- MOSAIC show substantial differences in the fine particle size distributions (sizes about 2 micrometers) that could be relevant when simulating climate effects on a global scale. Nevertheless, the agreement between MADE3 and PartMC-MOSAIC is very good when it comes to coarse particle size distribution, and also in terms of aerosol composition. Considering these results and the well-established ability of MADE in reproducing observed aerosol loadings and composition, MADE3 seems suitable for application within a global model.

Mixing state↗

Simultaneous Retrieval of Aerosol Properties and Clear-Sky Direct Radiative Effect Over the Global Ocean from MODIS

A unified satellite algorithm is presented to simultaneously retrieve aerosol properties (aerosol optical depth; AOD and aerosol type) and clear-sky shortwave direct radiative effect (hereafter, DREA) over ocean. The algorithm is applied to Moderate Resolution Imaging spectroradiometer (MODIS) observations for a period from 2003 to 2010 to assess the DREA over the global ocean. The simultaneous retrieval utilizes lookup table (LUT) containing both spectral reflectances and solar irradiances calculated using a single radiative transfer model with the same aerosol input data. This study finds that aerosols cool the top-of-atmosphere (TOA) and bottom-of-atmosphere (BOA) by 5.2 +/- 0.5 W/sq m and 8.3 W/sq m, respectively, and correspondingly warm the atmosphere (hereafter, ATM) by 3.1 W/sq m. These quantities, solely based on the MODIS observations, are consistent with those of previous studies incorporating chemical transport model simulations and satellite observations. However, the DREAs at BOA and ATM are expected to be less accurate compared to that of TOA due to low sensitivity in retrieving aerosol type information, which is related with the atmospheric heating by aerosols, particularly in low AOD conditions; consequently, the uncertainties could not be quantified. Despite the issue in the aerosol type information, the present method allows us to confine the DREA attributed only to fine-mode dominant aerosols, which are expected to be mostly anthropogenic origin, in the range from 1.1 W/sq m to 1.3 W/sq m at TOA. Improvements in size-resolved AOD and SSA retrievals from current and upcoming satellite instruments are suggested to better assess the DREA, particularly at BOA and ATM, where aerosol absorptivity induces substantial uncertainty.

MODIS↗

Aerosol Seasonal Variations over Urban-Industrial Regions in Ukraine According to AERONET and POLDER Measurements

The paper presents an investigation of aerosol seasonal variations in several urban-industrial regions in Ukraine. Our analysis of seasonal variations of optical and physical aerosol parameters is based on the sun-photometer 2008-2013 data from two urban ground-based AERONET (AErosol RObotic NETwork) sites in Ukraine (Kyiv, Lugansk) as well as on satellite POLDER instrument data for urban-industrial areas in Ukraine. We also analyzed the data from one AERONET site in Belarus (Minsk) in order to compare with the Ukrainian sites. Aerosol amount and optical depth (AOD) values in the atmosphere columns over the large urbanized areas like Kyiv and Minsk have maximum values in the spring (April-May) and late summer (August), whereas minimum values are observed in late autumn. The results show that fine-mode particles are most frequently detected during the spring and late summer seasons. The analysis of the seasonal AOD variations over the urban-industrial areas in the eastern and central parts of Ukraine according to both ground-based and POLDER data exhibits the similar traits. The seasonal variation similarity in the regions denotes the resemblance in basic aerosol sources that are closely related to properties of aerosol particles. The behavior of basic aerosol parameters in the western part of Ukraine is different from eastern and central regions and shows an earlier appearance of the spring and summer AOD maxima. Spectral single-scattering albedo, complex refractive index and size distribution of aerosol particles in the atmosphere column over Kyiv have different behavior for warm (April-October) and cold seasons. The seasonal features of fine and coarse aerosol particle behavior over the Kyiv site were analyzed. A prevailing influence of the fine-mode particles on the optical properties of the aerosol layer over the region has been established. The back-trajectory and cluster analysis techniques were applied to study the seasonal back trajectories and prevailing directions of the arrived air mass for the Kyiv and Minsk sites.

Ukraine↗

Using High-Resolution Airborne Remote Sensing to Study Aerosol Near Clouds

The horizontal space in between clear and cloudy air is very complex. This so-called twilight zone includes activated aerosols that are not quite clouds, thin cloud fragments that are not easily observable, and dying clouds that have not quite disappeared. This is a huge challenge for satellite remote sensing, specifically for retrieval of aerosol properties. Identifying what is cloud versus what is not cloud is critically important for attributing radiative effects and forcings to aerosols. At the same time, the radiative interactions between clouds and the surrounding media (molecules, surface and aerosols themselves) will contaminate retrieval of aerosol properties, even in clear skies. Most studies on aerosol cloud interactions are relevant to moderate resolution imagery (e.g. 500 m) from sensors such as MODIS. Since standard aerosol retrieval algorithms tend to keep a distance (e.g. 1 km) from the nearest detected cloud, it is impossible to evaluate what happens closer to the cloud. During Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS), the NASA ER-2 flew with the enhanced MODIS Airborne Simulator (eMAS), providing MODIS-like spectral observations at high (50 m) spatial resolution. We have applied MODIS-like aerosol retrieval for the eMAS data, providing new detail to characterization of aerosol near clouds. Interpretation and evaluation of these eMAS aerosol retrievals is aided by independent MODIS-like cloud retrievals, as well as profiles from the co-flying Cloud Physics Lidar (CPL). Understanding aerosolcloud retrieval at high resolution will lead to better characterization and interpretation of long-term, global products from lower resolution (e.g.MODIS) satellite retrievals.

aerosols near clouds↗

The Sensitivity of SeaWiFS Ocean Color Retrievals to Aerosol Amount and Type

As atmospheric reflectance dominates top-of-the-atmosphere radiance over ocean, atmospheric correction is a critical component of ocean color retrievals. This paper explores the operational Sea-viewing Wide Field-of-View Sensor (SeaWiFS) algorithm atmospheric correction with approximately 13 000 coincident surface-based aerosol measurements. Aerosol optical depth at 440 nm (AOD(sub 440)) is overestimated for AOD below approximately 0.1-0.15 and is increasingly underestimated at higher AOD; also, single-scattering albedo (SSA) appears overestimated when the actual value less than approximately 0.96.AOD(sub 440) and its spectral slope tend to be overestimated preferentially for coarse-mode particles. Sensitivity analysis shows that changes in these factors lead to systematic differences in derived ocean water-leaving reflectance (Rrs) at 440 nm. The standard SeaWiFS algorithm compensates for AOD anomalies in the presence of nonabsorbing, medium-size-dominated aerosols. However, at low AOD and with absorbing aerosols, in situ observations and previous case studies demonstrate that retrieved Rrs is sensitive to spectral AOD and possibly also SSA anomalies. Stratifying the dataset by aerosol-type proxies shows the dependence of the AOD anomaly and resulting Rrs patterns on aerosol type, though the correlation with the SSA anomaly is too subtle to be quantified with these data. Retrieved chlorophyll-a concentrations (Chl) are affected in a complex way by Rrs differences, and these effects occur preferentially at high and low Chl values. Absorbing aerosol effects are likely to be most important over biologically productive waters near coasts and along major aerosol transport pathways. These results suggest that future ocean color spacecraft missions aiming to cover the range of naturally occurring and anthropogenic aerosols, especially at wavelengths shorter than 440 nm, will require better aerosol amount and type constraints.

single scattering albedo↗

Radiative Effect of Springtime Biomass-Burning Aerosols over Northern Indochina During 7-SEAS Baseline 2013 Campaign

The direct aerosol radiative effects of biomass-burning (BB) aerosols over northern Indochina were estimated by using aerosol properties (physical, chemical, and optical) along with the vertical profile measurements from ground-based measurements with integration of an optical and a radiative transfer model during the Seven South East Asian Studies Biomass-Burning Aerosols Stratocumulus Environment: Lifecycles Interactions Experiment (7-SEASBASELInE) conducted in spring 2013. Cluster analysis of backward trajectories showed the air masses arriving at mountainous background site (Doi Ang Khang; 19.93degN, 99.05degE, 1536 m above mean sea level) in northern Indochina, mainly from near-source inland BB activities and being confined in the planetary boundary layer. The PM(sub10) and black carbon (BC)mass were 87 +/- 28 and 7 +/- 2 micrograms m(exp -3), respectively. The aerosol optical depth (AOD (sub 500) was found to be 0.26--1.13 (0.71 +/- 0.24). Finer (fine mode fraction is approximately or equal to 0.95, angstrom-exponent at 440-870 nm is approximately or equal to 1.77) and significantly absorbing aerosols(single scattering albedo is approximately or equal to 0.89, asymmetry-parameter is approximately or equal to 0.67, and absorption AOD 0.1 at 440 nm) dominated over this region. BB aerosols (water soluble and BC) were the main contributor to the aerosol radiative forcing (ARF), while others (water insoluble, sea salt and mineral dust) were negligible mainly due to their low extinction efficiency. BC contributed only 6 to the surface aerosol mass but its contribution to AOD was 12 (2 times higher). The overall mean ARF was 8.0 and -31.4 W m(exp -2) at top-of-atmosphere (TOA) and at the surface (SFC), respectively. Likely, ARF due to BC was +10.7 and -18.1 W m(exp -2) at TOA and SFC, respectively. BC imposed the heating rate of +1.4 K d(exp -1) within the atmosphere and highlighting its pivotal role in modifying the radiation budget. We propose that to upgrade our knowledge on BB aerosol radiative effects in BB source region, the long-term and extensive field measurements are needed.

aerosol optical properties↗

Satellite-Surface Perspectives of Air Quality and Aerosol-Cloud Effects on the Environment: An Overview of 7-SEAS BASELInE

The objectives of 7-SEASBASELInE (Seven SouthEast Asian Studies Biomass-burning Aerosols and Stratocumulus Environment: Lifecycles and Interactions Experiment) campaigns in spring 2013-2015 were to synergize measurements from uniquely distributed ground-based networks (e.g., AERONET (AErosol RObotic NETwork)), MPLNET ( NASA Micro-Pulse Lidar Network)) and sophisticated platforms (e.g.,SMARTLabs (Surface-based Mobile Atmospheric Research and Testbed Laboratories), regional contributing instruments), along with satellite observations retrievals and regional atmospheric transport chemical models to establish a critically needed database, and to advance our understanding of biomass-burning aerosols and trace gases in Southeast Asia (SEA). We present a satellite-surface perspective of 7-SEASBASELInE and highlight scientific findings concerning: (1) regional meteorology of moisture fields conducive to the production and maintenance of low-level stratiform clouds over land; (2) atmospheric composition in a biomass-burning environment, particularly tracers-markers to serve as important indicators for assessing the state and evolution of atmospheric constituents; (3) applications of remote sensing to air quality and impact on radiative energetics, examining the effect of diurnal variability of boundary-layer height on aerosol loading; (4) aerosol hygroscopicity and ground-based cloud radar measurements in aerosol-cloud processes by advanced cloud ensemble models; and (5) implications of air quality, in terms of toxicity of nanoparticles and trace gases, to human health. This volume is the third 7-SEAS special issue (after Atmospheric Research, vol. 122, 2013; and Atmospheric Environment, vol. 78, 2013) and includes 27 papers published, with emphasis on air quality and aerosol-cloud effects on the environment. BASELInE observations of stratiform clouds over SEA are unique, such clouds are embedded in a heavy aerosol-laden environment and feature characteristically greater stability over land than over ocean, with minimal radar surface clutter at a high vertical spatial resolution. To facilitate an improved understanding of regional aerosol-cloud effects, we envision that future BASELInE-like measurement modeling needs fall into two categories: (1) efficient yet critical in-situ profiling of the boundary layer for validating remote-sensing retrievals and for initializing regional transport chemical and cloud ensemble models; and (2) fully utilizing the high observing frequencies of geostationary satellites for resolving the diurnal cycle of the boundary layerheight as it affects the loading of biomass-burning aerosols, air quality and radiative energetics.

AERONET↗

Evaluation of Global Simulations of Aerosol Particle and Cloud Condensation Nuclei Number, with Implications for Cloud Droplet Formation

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011-2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of -24% and -35% for particles with dry diameters > 50 and > 120nm, as well as -36% and -34% for CCN at supersaturations of 0.2% and 1.0%, respectively. However, they seem to behave differently for particles activating at very low supersaturations (< 0.1%) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN(0.2)) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40% during winter and 20% in summer.

cloud droplets↗

Above-Cloud Aerosol Radiative Effects based on ORACLES 2016 and ORACLES 2017 Aircraft Experiments

Determining the direct aerosol radiative effect (DARE) of absorbing aerosols above clouds from satellite observations alone is a challenging task, in part because the radiative signal of the aerosol layer is not easily untangled from that of the clouds below. In this study, we use aircraft measurements from the NASA ObseRvations of CLouds above Aerosols and their intEractionS (ORACLES) project in the southeastern Atlantic to derive it with as few assumptions as possible. This is accomplished by using spectral irradiance measurements (Solar Spectral Flux Radiometer, SSFR) and aerosol optical depth (AOD) retrievals (Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research, 4STAR) during vertical profiles (spirals) that minimize the albedo variability of the underlying cloud field – thus isolating aerosol radiative effects from those of the cloud field below. For two representative cases, we retrieve spectral aerosol single scattering albedo (SSA) and the asymmetry parameter (g) from these profile measurements and calculate DARE given the albedo range measured by SSFR on horizontal legs above clouds. For mid-visible wavelengths, we find SSA values from 0.80 to 0.85 and a significant spectral dependence of g. As the cloud albedo increases, the aerosol increasingly warms the column. The transition from a cooling to a warming top-of-aerosol radiative effect occurs at an albedo value (critical albedo) just above 0.2 in the mid-visible wavelength range. In a companion paper, we use the techniques introduced here to generalize our findings to all 2016 and 2017 measurements and parameterize aerosol radiative effects.

Cloud aerosol↗