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BrO and Inferred Bry Profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer

We report measurements of bromine monoxide (BrO) and use an observationally constrained chemical box model to infer total gas-phase inorganic bromine (Br(sub y)) over the tropical western Pacific Ocean (tWPO) during the CONTRAST field campaign (January-February 2014). The observed BrO and inferred Bry profiles peak in the marine boundary layer (MBL), suggesting the need for a bromine source from sea-salt aerosol (SSA), in addition to organic bromine (CBry ). Both profiles are found to be C-shaped with local maxima in the upper free troposphere (FT). The median tropospheric BrO vertical column density (VCD) was measured as 1.6 x 10(exp 13) molec cm(exp -2), compared to model predictions of 0.9 x 10(exp 13) molec cm(exp -2) in GEOS-Chem (CBr(sub y) but no SSA source), 0.4 x 10(exp 13) molec cm(exp -2) in CAM-Chem (CBr(sub y) and SSA), and 2.1 x 10(exp 13) molec cm(exp -2) in GEOS-Chem (CBry and SSA). Neither global model fully captures the Cshape of the Br(sun y) profile. A local Br(sub y) maximum of 3.6 ppt (2.9-4.4 ppt; 95% confidence interval, CI) is inferred between 9.5 and 13.5 km in air masses influenced by recent convective outflow. Unlike BrO, which increases from the convective tropical tropopause layer (TTL) to the aged TTL, gas-phase Br(sub y) decreases from the convective TTL to the aged TTL. Analysis of gas-phase Br(sub y) against multiple tracers (CFC-11, H2O/O3 ratio, and potential temperature) reveals a Br(sub y) minimum of 2.7 ppt (2.3-3.1 ppt; 95% CI) in the aged TTL, which agrees closely with a stratospheric injection of 2.6 +/- 0.6 ppt of inorganic Br(sub y) (estimated from CFC-11 correlations), and is remarkably insensitive to assumptions about heterogeneous chemistry. Bry increases to 6.3 ppt (5.6-7.0 ppt; 95% CI) in the stratospheric "middleworld" and 6.9 ppt (6.5-7.3 ppt; 95% CI) in the stratospheric "overworld". The local Br(sub y) minimum in the aged TTL is qualitatively (but not quantitatively) captured by CAM-Chem, and suggests a more complex partitioning of gas-phase and aerosol Br(sub y) species than previously recognized. Our data provide corroborating evidence that inorganic bromine sources (e.g., SSA-derived gas-phase Br(sub y) ) are needed to explain the gas-phase Br(sub y) budget in the upper free troposphere and TTL. They are also consistent with observations of significant bromide in Upper Troposphere-Lower Stratosphere aerosols. The total Br(sub y) budget in the TTL is currently not closed, because of the lack of concurrent quantitative measurements of gas-phase Br(sub y) species (i.e., BrO, HOBr, HBr, etc.) and aerosol bromide. Such simultaneous measurements are needed to (1) quantify SSA-derived Br(sub y) in the upper FT, (2) test Br(sub y) partitioning, and possibly explain the gas-phase Br(sub y) minimum in the aged TTL, (3) constrain heterogeneous reaction rates of bromine, and (4) account for all of the sources of Br(sub y) to the lower stratosphere.

Atmospheric Chemistry; bromine; troposphere; CONTR↗

The Evolution of Lidar Networks: A US Perspective

Atmospheric aerosols and clouds play an important role in climate by directly scattering and absorbing sunlight. Aerosol-cloud interactions modify the particle properties causing indirect effects, alter aerosol deposition and rainfall, and contribute substantially to the uncertainties in predicting climate effects. Aerosols also affect air quality and both constituents modulate boundary layer dynamics to a certain extent, in turn impacting aerosol transport and aerosol-cloud interactions. The spatiotemporal distribution of aerosol and cloud layers is thus important, and lidar remains the primary instrument for determining the vertical distribution of aerosols and thin clouds. Lidar still provides important information for opaque cloud layers by determining base heights. Combined lidar and radar data provide a comprehensive coverage of aerosol and cloud vertical distributions, and thus locations where and when they interact. Lidar data provide a means of constraining column aerosol loading observations (e.g. AOD) to vertical extents. In addition, lidar has proven effective at determining a proxy for boundary layer height by examining aerosol gradients and/or cloud base heights in lidar profiles. Polarized lidars provide additional information on particle shape, allowing estimates of cloud phase and separation of dust or smoke from sulfate and sea salt aerosols. Given the importance of lidar observations and a critical maturation in technology and retrieval techniques, several organizations began to build operational lidar networks around 2000. The European Aerosol Research Lidar Network (EARLINET) was started as a research focused network of advanced lidars across Europe. The Asian Dust Lidar Network (ADNET) was also developed as a regional network providing lidar profiles of dust and pollution across Eastern Asia. In the US, the NASA Micro Pulse Lidar Network (MPLNET) was created to provide global lidar profiling at key sites in the NASA Aerosol Robotic Network (AERONET). The Network for the Detection of Atmospheric Composition Change (NDACC) pre-dates these networks and many sites have lidar, but it is not strictly a lidar network and at the time focused less on the lower troposphere. Finally, there were already existing ceilometer networks operated by various meteorological agencies, but in particular here in the US the profile data has not been available. The ceilometer networks were used to provide only clouds base heights and estimates of PBL height. Thus, the distinguishing feature between lidar and ceilometer networks was historically the ability to actually provide profile information (in addition to differences in wavelength, and advanced retrievals such as the raman technique). As time progressed, each lidar network matured and developed more operational capabilities and data sets, coupled with viable data centers providing DAAC services and access to near-real-time (NRT) data. In 2008 under WMO guidance, the Global Atmospheric Watch (GAW) Aerosol Lidar Observation Network (GALION) was formed as a global network made up of the existing lidar networks. The goal was to share information, best practices, and develop frameworks and techniques for quality data. GALION grew to include several other regional lidar networks and this has led to a vast increase in quality lidar sites worldwide.

Welton, Ellsworth J.↗

FUTURE LEVELS OF AEROSOLS & RADIATIVE FORCING OVER THE ARCTIC

The Arctic Monitoring and Assessment Programme (AMAP) is currently assessing the impacts of Short-Lived Climate Forcers (SLCF) on Arctic climate and air quality. In support of the assessment, we used the NASA Goddard Institute of Space Sciences (GISS) Earth System Model (modelE2.1), with prescribed sea surface temperature and sea-ice fraction, to simulate SLCF concentrations globally between 1995 and 2015. Two simulations were conducted, using the One-Moment Aerosol (OMA) and the Multiconfiguration Aerosol TRacker of mIXing state (MATRIX) aerosol modules. OMA is a mass-based scheme in which aerosols are assumed to remain externally mixed and have a prescribed and constant size distribution, while MATRIX is an aerosol microphysics scheme based on the quadrature method of moments, which is able to explicitly simulate the mixing state of aerosols. Anthropogenic emissions from the ECLIPSE v6b emissions database were used, along with emissions from aircrafts and open biomass burning from the Coupled Model Intercomparison Project Phase 6 (CMIP6), while the natural emissions of sea salt, DMS, isoprene and dust are calculated interactively. The simulated monthly surface concentrations of sulfate (SO4), black carbon (BC), organic carbon (OA), and ozone (O3) are compared with observations from a set of Arctic stations, extracted from the EBAS and IMPROVE databases, as well as a few additional locations. Simulated aerosol optical depths (AOD) are also compared with Advanced Very-High Resolution Radiometer (AVHRR). The study will present the evaluation of the modelE2.1 in simulating SLCF levels over the Arctic using different aerosol schemes, along with observed and simulated trends of SLCFs over the Arctic between 1995 and 2015.

Aersosols↗

Apparent dust size discrepancy in aerosol reanalysis in north African dust after long-range transport

North African dust reaches the southeastern United States every summer. Size-resolved dust mass measurements taken in Miami, Florida, indicate that more than one-half of the surface dust mass concentrations reside in particles with geometric diameters less than 2.1 µm, while vertical profiles of micropulse lidar depolarization ratios show dust reaching above 4 km during pronounced events. These observations are compared to the representation of dust in the Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) aerosol reanalysis and closely related Goddard Earth Observing System model version 5 (GEOS-5) Forward Processing (FP) aerosol product, both of which assimilate satellite-derived aerosol optical depths using a similar protocol and inputs. These capture the day-to-day variability in aerosol optical depth well, in a comparison to an independent sun-photometer-derived aerosol optical depth dataset. Most of the modeled dust mass resides in diameters between 2 and 6 µm, in contrast to the measurements. Model-specified mass extinction efficiencies equate light extinction with approximately 3 times as much aerosol mass, in this size range, compared to the measured dust sizes. GEOS-5 FP surface-layer sea salt mass concentrations greatly exceed observed values, despite realistic winds and relative humidities. In combination, these observations help explain why, despite realistic total aerosol optical depths, (1) free-tropospheric model volume extinction coefficients are lower than those retrieved from the micro-pulse lidar, suggesting too-low model dust loadings in the free troposphere, and (2) model dust mass concentrations near the surface can be higher than those measured. The modeled vertical distribution of dust, when captured, is reasonable. Large, aspherical particles exceeding the modeled dust sizes are also occasionally present, but dust particles with diameters exceeding 10 µm contribute little to the measured total dust mass concentrations after such long-range transport. Remaining uncertainties warrant a further integrated assessment to confirm this study's interpretations.

MEERA-2 aerosols reanalysis↗

AeroCom Phase III Multi-Model Evaluation of the Aerosol Life Cycle and Optical Properties Using Ground and Space-Based Remote Sensing as Well as Surface In Situ Observations

Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes. Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50 % decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2∕3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1. Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AODf, AODc), Ångström exponent (AE), dry surface scattering (SCdry), and absorption (ACdry) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21 % ± 20 % (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from −37 % (MODIS-Terra) to −16 % (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R>0.75), suggesting that the models are capable of capturing spatio-temporal variations in AOD. We find a much larger underestimate in coarse AODc (∼ −45 % ± 25 %) than in fine AODf (∼ −15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AODc bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AODc. Column AEs are underestimated by about 10 % ± 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. +140 % if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment. Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of −35 % ± 25 % and −20 % ± 18 % for SCdry and ACdry, respectively. The larger underestimate of SCdry than ACdry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SCdry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models. Considerable inter-model diversity in the simulated optical properties is often found in regions that are, unfortunately, not or only sparsely covered by ground-based observations. This includes, for instance, the Sahara, Amazonia, central Australia, and the South Pacific. This highlights the need for a better site coverage in the observations, which would enable us to better assess the models, but also the performance of satellite products in these regions. Using fine-mode AOD as a proxy for present-day aerosol forcing estimates, our results suggest that models underestimate aerosol forcing by ca. −15 %, however, with a considerably large interquartile range, suggesting a spread between −35 % and +10 %.

space-based remote sensing↗

Determination of Lidar Ratio for Major Aerosol Types over Western North Pacific Based on Long-Term MPLNET Data

East Asia is the most complex region in the world for aerosol studies, as it encounters a lot of varieties of aerosols, and aerosol classification can be a challenge in this region. In the present study, we focused on the relationship between aerosol types and aerosol optical properties. We analyzed the long-term (2005–2012) data of vertical profiles of aerosol extinction coefficients, lidar ratio (Sp), and other aerosol optical properties obtained from a NASA Micro-Pulse Lidar Network and Aerosol Robotic Network site in northern Taiwan, which frequently receives Asian continental outflows. Based on aerosol extinction vertical profiles, the profiles were classified into two types: type 1 (single-layer structure) and type 2 (two-layer structure). Fall season (October–November) was the prevailing season for the Type 1, whereas type 2 mainly happened in spring (March–April). In type 1, air masses normally originated from three regional sectors, i.e., Asia continental (AC), Pacific Ocean (PO), and Southeast Asia (SA). The mean Sp values were 39 ± 17 sr, 30 ± 12 sr, and 38 ± 18 sr for the AC, PO, and SA sectors, respectively. The Sp results suggested that aerosols from the AC sector contained dust and anthropogenic particles, and aerosols from the PO sector were most likely sea salts. We further combined the EPA dust event database and backward trajectory analysis for type 2. Results showed that Sp was 41 ± 14 sr and 53 ± 21 sr for dust storm and biomass-burning events, respectively. The Sp for biomass-burning events in type 2 showed two peaks patterns. The first peak occurred within range of 30–50 sr corresponding to urban pollutant, and the second peak occurred within range of 60–80 sr in relation to biomass burning. Finally, our study summarized the Sp values for four major aerosol types over northern Taiwan, viz., urban (42 ± 18 sr), dust (34 ± 6 sr), biomass-burning (69 ± 12 sr), and oceanic (30 ± 12 sr). Our findings provide useful references for aerosol classification and air pollution identification over the western North Pacific.

Sheng-Hsiang Wang↗

Assessment of Natural and Anthropogenic Aerosol Air Pollution In the Middle East Using MERRA-2, CAMS Data Assimilation Products, and High-Resolution WRF-Chem Model Simulations

Modern-Era Retrospective analysis for Research and Applications v.2 (MERRA-2), Copernicus Atmosphere Monitoring Service Operational Analysis (CAMS-OA), and a high-resolution regional Weather Research and Forecasting model coupled with chemistry (WRF-Chem) were used to evaluate natural and anthropogenic particulate matter (PM) air pollution in the Middle East (ME) during 2015–2016. Two Moderate Resolution Imaging Spectrometer (MODIS) retrievals – combined product Deep Blue and Deep Target (MODIS-DB&DT) and Multi-Angle Implementation of Atmospheric Correction (MAIAC) – and Aerosol Robotic Network (AERONET) aerosol optical depth (AOD) observations as well as in situ PM measurements for 2016 were used for validation of the WRF-Chem output and both assimilation products. MERRA-2 and CAMS-OA assimilate AOD observations. WRF-Chem is a free-running model, but dust emission in WRF-Chem is tuned to fit AOD and aerosol volume size distributions obtained from AERONET. MERRA-2 was used to construct WRF-Chem initial and boundary conditions both for meteorology and chemical and aerosol species. SO2 emissions in WRF-Chem are based on the novel OMI-HTAP SO2 emission dataset. The correlation with the AERONET AOD is highest for MERRA-2 (0.72–0.91), MAIAC (0.63–0.96), and CAMSOA (0.65–0.87), followed by MODIS-DB&DT (0.56–0.84) and WRF-Chem (0.43–0.85). However, CAMS-OA has a relatively high positive mean bias with respect to AERONET AOD. The spatial distributions of seasonally averaged AODs from WRF-Chem, assimilation products, and MAIAC are well correlated with MODIS-DB&DT AOD product. MAIAC has the highest correlation (R = 0.8), followed by MERRA-2 (R = 0.66), CAMS-OA (R = 0.65), and WRF-Chem (R = 0.61). WRF-Chem, MERRA-2, and MAIAC underestimate and CAMS-OA overestimates MODIS-DB&DT AOD. The simulated and observed PM concentrations might differ by a factor of 2 because it is more challenging for the model and the assimilation products to reproduce PM concentration measured within the city. Although aerosol fields in WRF-Chem and assimilation products are entirely consistent, WRF-Chem is preferable for analysis of regional air quality over the ME due to its higher spatial resolution and better SO2 emissions. The WRF-Chem’s PM background concentrations exceed the World Health Organization (WHO) guidelines over the entire ME. Mineral dust is the major contributor to PM (≈ 75%–95%) compared to other aerosol types. Near and downwind from the SO2 emission sources, non-dust aerosols (primarily sulfate) contribute up to 30% to PM(sub 2.5). The contribution of sea salt to PM in coastal regions can reach 5%. The contributions of organic matter, black carbon and organic carbon to PM over the Middle East are insignificant. In the major cities over the Arabian Peninsula, the 90th percentile of PM(sub 10) and PM(sub 2.5) (particles with diameters less than 10 and 2.5 μm, respectively) daily mean surface concentrations exceed the corresponding Kingdom of Saudi Arabia air quality limits. The contribution of the non-dust component to PM(sub 2.5) is < 25%, which limits the emission control effect on air quality. The mitigation of the dust effect on air quality requires the development of environment-based approaches like growing tree belts around the cities and enhancing in-city vegetation cover. The WRF-Chem configuration presented in this study could be a prototype of a future air quality forecast system that warns the population against air pollution hazards.

Alexander Ukhov↗

Overview of ACTIVATE’s First Year of Flights Targeting Aerosol-Cloud-Meteorology Interactions

The Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) included 40 research flights in the winter and summer months of 2020 using a two-aircraft approach to simultaneously obtain in situ and remote sensing data of regions below, inside, and above boundary layer clouds. This presentation will summarize early findings from the first year of ACTIVATE flights with focus on aerosol and cloud droplet number concentration behavior, formation and evolution of clouds, and analysis of remote sensing retrievals of aerosol and cloud properties. There is a clear annual cycle in cloud droplet number concentration suggesting a marked annual cycle in aerosol-cloud interactions. Although aerosol particles are more abundant in spring and summer, the conditions needed to activate those particles into cloud droplets are weaker than in other colder months. Several flights targeted post-frontal clouds associated with cold air outbreaks pointing to enhanced levels of nucleated particles immediately above such clouds, and that ice formation hastens the transition from closed to open cloud structures in the sampled CAO events. Also observed in the marine boundary layer during CAOs is the frequent occurrence of non-spherical sea salt particles, which has significant implications for remote sensing retrievals.

Taylor Shingler↗

Analysis of Near-Cloud Changes in Atmospheric Aerosols Using Satellite Observations and Global Model Simulations

This paper examines cloud-related variations of atmospheric aerosols that occur in partly cloudy regions containing low-altitude clouds. The goal is to better understand aerosol behaviors and to help better represent the radiative effects of aerosols on climate. For this, the paper presents a statistical analysis of a multi-month global dataset that combines data from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instruments with data from the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) global reanalysis. Among other findings, the results reveal that near-cloud enhancements in lidar backscatter (closely related to aerosol optical depth) are larger (1) over land than ocean by 35%, (2) near optically thicker clouds by substantial amounts, (3) for sea salt than for other aerosol types, with the difference from dust reaching 50%. Finally, the study found that mean lidar backscatter is higher near clouds not because of large-scale variations in meteorological conditions, but because of local processes associated with individual clouds. The results help improve our understanding of aerosol-cloud-radiation interactions and our ability to represent them in climate models and other atmospheric models

aerosol↗

Identifying Chemical Aerosol Signatures Using Optical Suborbital Observations: How Much Can Optical Properties Tell us about Aerosol Composition?

Improvements in air quality and Earth’s climate predictions require improvements of the aerosol speciation in chemical transport models, using observational constraints. Aerosol speciation (e.g., organic aerosols, black carbon, sulfate, nitrate, ammonium, dust or sea salt) is typically determined using in situ instrumentation. Continuous, routine surface network aerosol composition measurements are not uniformly widespread over the globe. Satellites, on the other hand, can provide a maximum coverage of the horizontal and vertical atmosphere but observe aerosol optical properties (and not aerosol speciation) based on remote sensing instrumentation. Combinations of satellite-derived aerosol optical properties can inform on air mass aerosol types (AMTs e.g., clean marine, dust, polluted continental). However, these AMTs are subjectively defined, might often be misclassified and are hard to relate to the critical parameters that need to be refined in models. In this paper, we derive AMTs that are more directly related to sources and hence to speciation. They are defined, characterized, and derived using simultaneous in situ gas-phase, chemical and optical instruments on the same aircraft during the Study of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS, US, summer of 2013). First, we prescribe well-informed AMTs that display distinct aerosol chemical and optical signatures to act as a training AMT dataset. These in situ observations reduce the errors and ambiguities in the selection of the AMT training dataset. We also investigate the relative skill of various combinations of aerosol optical properties to define AMTs and how much these optical properties can capture dominant aerosol speciation. We find distinct optical signatures for biomass burning (from agricultural or wildfires), biogenic and dust-influence AMTs. Useful aerosol optical properties to characterize these signatures are the extinction angstrom exponent (EAE), the single scattering albedo, the difference of single scattering albedo in two wavelengths, the absorption coefficient, the absorption angstrom exponent (AAE), and the real part of the refractive index (RRI). We find that all four AMTs studied when prescribed using mostly airborne in situ gas measurements, can be successfully extracted from at least three combinations of airborne in situ aerosol optical properties (e.g., EAE, AAE and RRI) over the US during SEAC4RS. However, we find that the optically based classifications for BB from agricultural fires and polluted dust include a large percentage of misclassifications that limit the usefulness of results relating to those classes. The technique and results presented in this study are suitable to develop a representative, robust and diverse source-based AMT database. This database could then be used for widespread retrievals of AMTs using existing and future remote sensing suborbital instruments/networks. Ultimately, it has the potential to provide a much broader observational aerosol data set to evaluate chemical transport and air quality models than is currently available by direct in situ measurements. This study illustrates how essential it is to explore existing airborne datasets to bridge chemical and optical signatures of different AMTs, before the implementation of future spaceborne missions (e.g., the next generation of Earth Observing System (EOS) satellites addressing Aerosol, Cloud, Convection and Precipitation (ACCP) designated observables).

Meloe S F Kacenelenbogen↗

Using PACE Aerosol Optical and Microphysical Properties to Capture Aerosol Composition

Improvements in air quality and Earth’s climate predictions can only be achieved through improvements of the aerosol speciation in chemical transport models, using observational constraints. Aerosol speciation (e.g., organic aerosols, black carbon, sulfate, nitrate, ammonium, dust or sea salt) is typically determined using in situ instrumentation. Continuous, routine surface network aerosol composition measurements are not uniformly widespread over the globe. Satellites, on the other hand, can provide a maximum coverage of the horizontal and vertical atmosphere but observe aerosol optical properties (and not aerosol speciation) based on remote sensing instrumentation. Combinations of satellite-derived aerosol optical properties can inform on air mass aerosol types (e.g., clean marine, dust, polluted continental). We investigate the relative skill of various combinations of aerosol optical properties used as tools to define air mass aerosol types and how much these optical properties can capture dominant aerosol speciation.

Meloe Shenandoah Kacenelenbogen↗

A Coupled Evaluation of Operational MODIS and Model Aerosol Products for Maritime Environments Using Sun Photometry: Evaluation of the Fine and Coarse Mode

Although satellite retrievals and data assimilation have progressed to where there is a good skill for monitoring maritime Aerosol Optical Depth (AOD), there remains uncertainty in achieving further degrees of freedom, such as distinguishing fine and coarse mode dominated species in maritime environments (e.g., coarse mode sea salt and dust versus fine mode terrestrial anthropogenic emissions, biomass burning, and maritime secondary production). For the years 2016 through 2019, we performed an analysis of 550 nm total AOD550, fine mode AOD (FAOD550; also known as FM AOD in the literature), coarse mode AOD (CAOD550), and fine mode fraction (η550) between Moderate Resolution Spectral Imaging Radiometer (MODIS) V6.1 MOD/MYD04 dark target aerosol retrievals and the International Cooperative for Aerosol Prediction (ICAP) core four multi-model consensus (C4C) of analyses/short term forecasts that assimilate total MODIS AOD550. Differences were adjudicated by the global shipboard Maritime Aerosol Network (MAN) and selected island AERONET sun photometer observations with the application of the spectral deconvolution algorithm (SDA). Through a series of conditional and regional analyses, we found divergence included regions of terrestrial influence and latitudinal dependencies in the remote oceans. Notably, MODIS and the C4C and its members, while having good correlations overall, have a persistent +0.04 to +0.02 biases relative to MAN and AERONET for typical AOD550 values (84th% < 0.28), with the C4C underestimating significant events thereafter. Second, high biases in AOD550 are largely associated with the attribution of the fine mode in satellites and models alike. Thus, both MODIS and C4C members are systematically overestimating AOD550 and FAOD550 but perform better in characterizing the CAOD550. Third, for MODIS, findings are consistent with previous reports of a high bias in the retrieved Ångström Exponent, and we diagnosed both the optical model and cloud masking as likely causal factors for the AOD550 and FAOD550 high bias, whereas for the C4C, it is likely from secondary overproduction and perhaps numerical diffusion. Fourth, while there is no wind-speed-dependent bias for surface winds <12 m s−1, the C4C and MODIS AOD550s also overestimate CAOD550 and FAOD550, respectively, for wind speeds above 12 m/s. Finally, sampling bias inherent in MAN, as well as other circumstantial evidence, suggests biases in MODIS are likely MODIS and the C4C products have their own strengths and challenges for a given climate application and discuss needed research. even larger than what was diagnosed here. We conclude with a discussion on how

Aerosols↗

The PolCube CubeSat Polarimeter for Earth Science

PolCube is a 12U CubeSat + polarimeter instrument designed by NASA Langley and the Korea Astronomy and Space Science Institute (KASI) for Earth Science. PolCube is based on the PolCam polarimeter onboard the Korean Pathfinder Lunar Observatory (KPLO) that launched in August 2022. The objective of the PolCube instrument is to retrieve detailed fine-mode (pollution and smoke) and coarse-mode (sea-salt and dust) aerosol properties over the ocean for a range of light to heavy aerosol loadings using its polarimetric-imaging capability at multiple angles and wavelengths from 410 − 865 nm. An additional objective is to discriminate aerosols from thin clouds. We quantify the performance of aerosol and ocean remote sensing products from the PolCube polarimeter instrument using the Microphysical Aerosol Properties from Polarimetry (MAPP) remote sensing retrieval algorithm. PolCube’s accurate and high-resolution aerosol-retrieval products will provide unique spatial and temporal coverage of the Earth that can be used synergistically with other instruments, such as the PACE (Plankton, Aerosols, Clouds and Ecosystems) and GEMS (Geostationary Environmental Monitoring Spectrometer) mission to improve air-quality forecasting. We present the PolCube-MAPP retrieval algorithm, which used optimal estimation and artificial intelligence, as well as multiple powerful inherent optical property look-up-tables for the Earth’s aerosol, cloud, and hydrosol particles. We estimate that PolCube can retrieve total aerosol optical depth at 555 nm (AOD555) within ±0.068, fine-mode AOD555 within ±0.078, and fine-mode single-scattering albedo within ±0.036, where all uncertainties are expressed as one standard deviation (1σ).

Snorre Stamnes↗

Global Burden of Tropospheric Ozone: Effects of Particulate Nitrate Photolysis and Assimilation of NO2 Measurements

Tropospheric ozone is a major pollutant, a greenhouse gas, and the primary source of the hydroxyl radical. It is largely produced in situ from the oxidation of CO and volatile organic compounds in the presence of nitrogen oxides (NOx=NO+NO2). Global atmospheric chemistry models generally underestimate NOx and CO concentrations in the northern hemisphere away from source regions, which would lead to an underestimate in the tropospheric ozone burden. Here we evaluate the tropospheric ozone simulation in the GEOS-Chem model (version 14) using observations from satellite, aircraft, and ozonesondes. We include GEOS-Chem simulations conducted in the standard offline mode, as well as in the online mode within the NASA GEOS earth system model which forms the basis for the GEOS Composition Forecasts (GEOS-CF). In both configurations, GEOS-Chem underestimates ozone concentrations in the northern midlatitude free troposphere in spring and summer. We find that we can improve the ozone simulation by including an additional NOx source over the oceans from particulate nitrate photolysis on sea salt aerosols at rates inferred from field studies over the Atlantic Ocean. We investigate whether further improvements in the ozone simulation can be achieved by assimilating satellite measurements of NO2 from the Ozone Monitoring Instrument (OMI) and CO from the Measurement of Pollution in the Troposphere (MOPITT) instruments.

tropospheric ozone↗

The Tables of Aerosol Optics (TAO) Project

The Table of Aerosol Optics (TAO) project is a community repository of optics computations (extinction, absorption, single-scatter albedo, lidar ratio, etc) that are useful for global models and remote sensing applications. TAO expands upon historical efforts (e.g., Hess et al., 1998) by building an open database that uses recent measurements and new computational techniques for non-spherical particles. The ‘open’ aspect of TAO is important, since the size distributions, hygroscopicities, refractive indices, and morphological recommendations of today will undoubtedly yield to different values in the future; the open framework of TAO allows scientists to keep adding new computations to the database as the science evolves. TAO is meant to be a community repository where specialists can put their computations for other scientists to use. So for instance, some groups are advancing new techniques that can accommodate complex fractal aggregates of black carbon, other groups are working on realistic irregular shapes for mineral dust, and different groups are updating the hygroscopicity of various aerosol types using new techniques. The TAO database gives these scientists a place to distribute their products. As TAO grows, modelers and remote sensing specialists will look to TAO as a place to find a wide variety of choices for testing. Meanwhile, global modelers can also use TAO to lobby for new tables that accommodate their needs. Eventually, TAO will provide mass extinction coefficients, mass absorption coefficients, lidar ratios, etc., at popular remote sensing and global modeling wavelengths (0.25-40 µm) for all pertinent species (sulfate, sea salt, BC, OC, BrC, dust, etc.). TAO will also accept computations for aerosol ‘type’ (e.g., biomass burning, urban, background, etc.) that may include regional and seasonal variability. Multiple tables may be created for each species or type to account for the multiple valid size distributions, hygroscopicities, complex refractive indices, and shapes that can be found in the literature.

Greg Schuster↗

Mapping Aerosol Lidar Ratios Over Ocean for CALIPSO Using Modis AOD-Constrained Retrievals and A Global Aerosol Model

The CALIPSO aerosol algorithms currently assign one lidar ratio value for each of the seven tropospheric aerosol types. In a future data products release, the CALIPSO project aims to improve these algorithms by developing regional and seasonal lidar ratio climatologies. In this study, aerosol lidar ratios are inferred through Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) backscatter profiles constrained by collocated aerosol optical depth from Aqua Moderate Resolution Imaging Spectroradiometer (MODIS) datasets. The analysis is subsampled for only those profiles that are cloud-free and contain one aerosol type (based on CALIOP feature classification). In addition, the CALIOP profiles are collocated with aerosol volume fractions simulated by the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model. In this talk, the twelve-year (2006-2017) mean spatial distributions of inferred aerosol lidar ratios for CALIOP-classified marine aerosols and the corresponding modeled sea salt volume fractions (SSVF) will be shown. Model-assisted climatological lidar ratio maps on a seasonal scale will also be presented, developed from the empirical relationship found between the modeled SSVF and lidar ratios. A comparison with past studies will be provided as well as results of a sensitivity study regarding the variability of retrieved lidar ratios as a function of horizontal averaging resolution. While the majority of this talk will focus on lidar ratios for CALIOP-classified marine aerosols, preliminary results will be shown for other aerosol types over ocean, such as dust and elevated smoke.

Travis Toth↗

The Tables of Aerosol Optics (TAO) Project

The Table of Aerosol Optics (TAO) project is a community repository of optics computations (extinction, absorption, single-scatter albedo, lidar ratio, etc) that are useful for global models and remote sensing applications. TAO expands upon historical efforts (e.g., Hess et al., 1998) by building an open database that uses recent measurements and new computational techniques for non-spherical particles. The ‘open’ aspect of TAO is important, since the size distributions, hygroscopicities, refractive indices, and morphological recommendations of today will undoubtedly yield to different values in the future; the open framework of TAO allows scientists to keep adding new computations to the database as the science evolves. TAO is meant to be a community repository where specialists can put their computations for other scientists to use. So for instance, some groups are advancing new techniques that can accommodate complex fractal aggregates of black carbon, other groups are working on realistic irregular shapes for mineral dust, and different groups are updating the hygroscopicity of various aerosol types using new techniques. The TAO database gives these scientists a place to distribute their products. As TAO grows, modelers and remote sensing specialists will look to TAO as a place to find a wide variety of choices for testing. Meanwhile, global modelers can also use TAO to lobby for new tables that accommodate their needs. Eventually, TAO will provide mass extinction coefficients, mass absorption coefficients, lidar ratios, etc., at popular remote sensing and global modeling wavelengths (0.25-40 µm) for all pertinent species (sulfate, sea salt, BC, OC, BrC, dust, etc.). TAO will also accept computations for aerosol ‘type’ (e.g., biomass burning, urban, background, etc.) that may include regional and seasonal variability. Multiple tables may be created for each species or type to account for the multiple valid size distributions, hygroscopicities, complex refractive indices, and shapes that can be found in the literature.

Elisabeth Andrews↗

Creating Seasonal Climatologies of Aerosol Lidar Ratios Over Ocean Using MODIS AOD Constrained Retrievals and GOCART Model Simulations

The current CALIPSO algorithms assign one lidar ratio (i.e., extinction-to-backscatter ratio; LR) value globally for each of the seven tropospheric aerosol types. In a future data products release, the CALIPSO project aims to improve these algorithms through the development of regional and seasonal LR climatologies. In this work, aerosol LRs are inferred through CALIOP backscatter profiles constrained by collocated aerosol optical depth (AOD) from Aqua Moderate Resolution Imaging Spectroradiometer (MODIS) data. This analysis is subsampled for those profiles that are cloud-free and contain only one CALIOP-classified aerosol type (e.g., marine). The CALIOP profiles are then collocated with aerosol volume fractions obtained through Goddard Chemistry Aerosol Radiation and Transport (GOCART) model simulations. In this poster, we show twelve-year (June 2006-August 2018) mean spatial distributions of inferred aerosol LRs for CALIOP-classified marine aerosols and how they correspond inversely with patterns of GOCART sea salt volume fraction (SSVF). Near land masses, smaller SSVFs and larger LRs are found (due to the influence of over-land aerosols). In the remote ocean regions (likely less impacted by over-land aerosols), larger SSVFs and smaller LRs are found. The developed relationship between the GOCART model SSVFs and MODIS AOD constrained LRs is used to create model-assisted seasonal LR maps. Additionally, we show maps of inferred LRs from constrained retrievals using the CALIPSO Ocean Derived Column Optical Depth (ODCOD) product and comparisons with those from the MODIS analyses. The technique demonstrated here benefits CALIPSO in the near-term, but similar methods can also be applied to the next generation space-based elastic backscatter lidars with collocated passive sensors, such as those of the upcoming NASA Atmosphere Observing System (AOS).

Travis Toth↗