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NASA NTRS2015

Aircraft Measurements of BrO, IO, Glyoxal, NO2, H2O, O2-O2 and Aerosol Extinction Profiles in the Tropics: Comparison with Aircraft-/Ship-Based in Situ and Lidar Measurements

Tropospheric chemistry of halogens and organic carbon over tropical oceans modifies ozone and atmospheric aerosols, yet atmospheric models remain largely untested for lack of vertically resolved measurements of bromine monoxide (BrO), iodine monoxide (IO) and small oxygenated hydrocarbons like glyoxal (CHOCHO) in the tropical troposphere. BrO, IO, glyoxal, nitrogen dioxide (NO2), water vapor (H2O) and O2-O2 collision complexes (O4/ were measured by the University of Colorado Airborne Multi-AXis Differential Optical Absorption Spectroscopy (CU AMAXDOAS) instrument, aerosol extinction by high spectral resolution lidar (HSRL), in situ aerosol size distributions by an ultra high sensitivity aerosol spectrometer (UHSAS) and in situ H2O by vertical-cavity surface-emitting laser (VCSEL) hygrometer. Data are presented from two research flights (RF12, RF17) aboard the National Science Foundation/ National Center for Atmospheric Research Gulfstream V aircraft over the tropical Eastern Pacific Ocean (tEPO) as part of the "Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated hydrocarbons" (TORERO) project (January/February 2012). We assess the accuracy of O4 slant column density (SCD) measurements in the presence and absence of aerosols. Our O4-inferred aerosol extinction profiles at 477 nm agree within 6% with HSRL in the boundary layer and closely resemble the renormalized profile shape of Mie calculations constrained by UHSAS at low (sub-Rayleigh) aerosol extinction in the free troposphere. CU AMAX-DOAS provides a flexible choice of geometry, which we exploit to minimize the SCD in the reference spectrum (SCDREF, maximize signal-to-noise ratio) and to test the robustness of BrO, IO and glyoxal differential SCDs. The RF12 case study was conducted in pristine marine and free tropospheric air. The RF17 case study was conducted above the NOAA RV Ka'imimoana (TORERO cruise, KA-12-01) and provides independent validation data from ship-based in situ cavity-enhanced DOAS and MAX-DOAS. Inside the marine boundary layer (MBL) no BrO was detected (smaller than 0.5 pptv), and 0.2-0.55 pptv IO and 32-36 pptv glyoxal were observed. The near-surface concentrations agree within 30% (IO) and 10% (glyoxal) between ship and air-craft. The BrO concentration strongly increased with altitude to 3.0 pptv at 14.5 km (RF12, 9.1 to 8.6 deg N; 101.2 to 97.4 deg W). At 14.5 km, 5-10 pptv NO2 agree with model predictions and demonstrate good control over separating tropospheric from stratospheric absorbers (NO2 and BrO). Our profile retrievals have 12-20 degrees of freedom (DoF) and up to 500m vertical resolution. The tropospheric BrO vertical column density (VCD) was 1.5 x 10(exp 13) molec cm(exp -2) (RF12) and at least 0.5 x 10(exp 13) molec cm(exp -2) (RF17, 0- 10 km, lower limit). Tropospheric IO VCDs correspond to 2.1 x 10(exp 12) molec cm(exp -2) (RF12) and 2.5 x 10(exp 12) molec cm(exp -2) (RF17) and glyoxal VCDs of 2.6 x 10(exp 14) molec cm(exp -2) (RF12) and 2.7 x 10(exp 14) molec cm(exp -2) (RF17). Surprisingly, essentially all BrO as well as the dominant IO and glyoxal VCD fraction was located above 2 km (IO: 58 plus or minus 5 %, 0.1-0.2 pptv; glyoxal: 52 plus or minus 5 %, 3-20 pptv). To our knowledge there are no previous vertically resolved measurements of BrO and glyoxal from aircraft in the tropical free troposphere. The atmospheric implications are briefly discussed. Future studies are necessary to better understand the sources and impacts of free tropospheric halogens and oxygenated hydrocarbons on tropospheric ozone, aerosols, mercury oxidation and the oxidation capacity of the atmosphere.

Volkamer, R.↗
NASA NTRS2016

CATS Aerosol Typing and Future Directions

The Cloud Aerosol Transport System (CATS), launched in January of 2015, is a lidar remote sensing instrument that will provide range-resolved profile measurements of atmospheric aerosols and clouds from the International Space Station (ISS). CATS is intended to operate on-orbit for at least six months, and up to three years. Status of CATS Level 2 and Plans for the Future:Version. 1. Aerosol Typing (ongoing): Mode 1: L1B data released later this summer; L2 data released shortly after; Identify algorithm biases (ex. striping, FOV (field of view) biases). Mode 2: Processed Released Currently working on correcting algorithm issues. Version 2 Aerosol Typing (Fall, 2016): Implementation of version 1 modifications Integrate GEOS-5 aerosols for typing guidance for non spherical aerosols. Version 3 Aerosol Typing (2017): Implementation of 1-D Var Assimilation into GEOS-5 Dynamic lidar ratio that will evolve in conjunction with simulated aerosol mixtures.

McGill, Matt↗
NASA NTRS2017

Answering the Call for Model-Relevant Observations of Aerosols and Clouds

We describe a technique for combining multiple A-Train aerosol data sets, namely MODIS spectral AOD (aerosol optical depth), OMI AAOD (absorption aerosol optical depth) and CALIOP aerosol backscatter retrievals (hereafter referred to as MOC retrievals) to estimate full spectral sets of aerosol radiative properties, and ultimately to calculate the 3-D distribution of direct aerosol radiative effects (DARE). We present MOC results using almost two years of data collected in 2007 and 2008, and show comparisons of the aerosol radiative property estimates to collocated AERONET retrievals. We compare the spatio-temporal distribution of the MOC retrievals and MOC-based calculations of seasonal clear-sky DARE to values derived from four models that participated in the Phase II AeroCom model intercomparison initiative. Comparisons of seasonal aerosol property to AeroCom Phase II results show generally good agreement best agreement with forcing results at TOA is found with GMI-MerraV3.We discuss the challenges in making observations that really address deficiencies in models, with some of the more relevant aspects being representativeness of the observations for climatological states, and whether a given model-measurement difference addresses a sampling or a model error.

Redemann, J.↗
NASA NTRS2018

Aerosol-Radiation-Cloud Interactions in the South-East Atlantic: Results from the ORACLES-2016 Deployment and a First Look at ORACLES-2017 and Beyond

Seasonal biomass burning (BB) in Southern Africa during the Southern hemisphere spring produces almost a third of the Earth's BB aerosol particles. These particles are lofted into the mid-troposphere and transported westward over the South-East (SE) Atlantic, where they interact with one of the three semi-permanent subtropical stratocumulus (Sc) cloud decks in the world. These interactions include adjustments to aerosol-induced solar heating and microphysical effects. The representation of these interactions in climate models remains highly uncertain, because of the scarcity of observational constraints on both, the aerosol and cloud properties, and the governing physical processes. The first deployment of the NASA P-3 and ER-2 aircraft in the ORACLES (ObseRvations of Aerosols Above Clouds and Their IntEractionS) project in August/September of 2016 has started to fill this observational gap by providing an unprecedented look at the SE Atlantic cloud-aerosol system. We provide an overview of the first deployment, highlighting aerosol absorptive and cloud-nucleating properties, their vertical distribution relative to clouds, the locations and degree of aerosol mixing into clouds, cloud changes in response to such mixing, and cloud top stability relationships to the aerosol. We also expect to describe preliminary results of the second ORACLES deployment from Sao Tome and Pri­ncipe in August 2017. We will make an initial assessment of the differences and similarities of the BB plume and cloud properties as observed from a deployment site near the plume's northern edge. We will conclude with an outlook for the third ORACLES deployment in October 2018.

Redemann, Jens↗
NASA NTRS2018

Characterizing Differences in the Aerosol Plume and Cloud Structure over Ascension Island During the 2016 and 2017 Biomass Burning Seasons

Marine boundary layer clouds, including the transition from stratocumulus to cumulus, are poorly represented in numerical weather prediction and general circulation models. In many cases, the complex physical relationships between marine boundary cloud morphology and the environmental conditions in which the clouds exist are not well understood. Such uncertainties arise in the presence of biomass burning carbonaceous aerosol, as is the case over the southeast Atlantic Ocean. It is likely that the absorbing and heating properties of these aerosols influence the microphysical composition and macrophysical arrangement of marine stratocumulus and trade cumulus in this region; however, this has yet to be quantified. The deployment of the Atmospheric Radiation Measurement Mobile Facility #1 (AMF1) in support of LASIC (Layered Atlantic Smoke Interactions with Clouds) provided a unique opportunity to collect observations of cloud and aerosol properties during two consecutive biomass burning seasons during July through October of 2016 and 2017 over Ascension Island (7.96 S, 14.35 W). Through the use of AMF1 observations, the Modern Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2), and back trajectories from the Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT), it will be demonstrated that differences in the atmospheric circulation during the two years result in varying aerosol conditions over Ascension Island. When the aerosol plume is overhead, the aerosol loading is higher during the 2016 season as a result of a weaker subtropical high-pressure system. Furthermore, the aerosol plume originates from central Africa in 2016, but further south in 2017. Contrasts in the season-to-season and day-to-day aerosol loading are used to categorize boundary layer cloud and sub-cloud turbulence measurements above Ascension Island using the AMF1 Doppler lidar and cloud radar.

Collow, Allison B. Marquardt↗
NASA NTRS2018

The Ozone Mapping and Profiler Suite (OMPS) Limb Profiler (LP) Version 1 Aerosol Extinction Retrieval Algorithm: Theoretical Basis

The theoretical basis of the Ozone Mapping and Profiler Suite (OMPS) Limb Profiler (LP) Version 1 aerosol extinction retrieval algorithm is presented. The algorithm uses an assumed bimodal lognormal aerosol size distribution to retrieve aerosol extinction profiles at 675 nm from OMPS LP radiance measurements. A first-guess aerosol extinction profile is updated by iteration using the Chahine nonlinear relaxation method, based on comparisons between the measured radiance profile at 675 nm and the radiance profile calculated by the Gauss Seidel limb-scattering (GSLS) radiative transfer model for a spherical-shell atmosphere. This algorithm is discussed in the context of previous limb-scattering aerosol extinction retrieval algorithms, and the most significant error sources are enumerated. The retrieval algorithm is limited primarily by uncertainty about the aerosol phase function. Horizontal variations in aerosol extinction, which violate the spherical-shell atmosphere assumed in the version 1 algorithm, may also limit the quality of the retrieved aerosol extinction profiles significantly.

Loughman, Robert↗
NASA NTRS2018

A Satellite-Based Estimate of Combustion Aerosol Cloud Microphysical Effects over the Arctic Ocean

Climate predictions for the rapidly changing Arctic are highly uncertain, largely due to a poor understanding of the processes driving cloud properties. In particular, cloud fraction (CF) and cloud phase (CP) have major impacts on energy budgets, but are poorly represented in most models, often because of uncertainties in aerosol–cloud interactions. Here, we use over 10 million satellite observations coupled with aerosol transport model simulations to quantify large scale microphysical effects of aerosols on CF and CP over the Arctic Ocean during polar night, when direct and semi-direct aerosol effects are minimal. Combustion aerosols over sea ice are associated with very large (~10W/sq.m) differences in longwave cloud radiative effects at the sea ice surface. However, co-varying meteorological changes on factors such as CF likely explain the majority of this signal. For example, combustion aerosols explain at most 40% of the CF differences between the full dataset and the clean-condition subset, compared to between 57% and 91% of the differences that can be predicted by co-varying meteorology. After normalizing for meteorological regime, aerosol microphysical effects have small but significant impacts on CF, CP, and precipitation frequency on an Arctic-wide scale. These effects indicate that dominant aerosol–cloud microphysical mechanisms are related to the relative fraction of liquid-containing clouds, with implications for a warming Arctic.

Zamora, Lauren M.↗
NASA NTRS2019

Assimilation of Aerosol Observations in the NASA GEOS Model

In the GEOS near real-time system, as well as in MERRA-2 which is the latest reanalysis produced at NASA's Global Modeling Assimilation Office (GMAO), the assimilation of aerosol observations is performed by means of a so-called analysis splitting method. The prognostic model is based on the GEOS model radiatively coupled to GOCART aerosol module and includes assimilation of bias-corrected Aerosol Optical Depth (AOD) at 550 nm from various space-based remote sensing platforms. In line with the transition of the GEOS meteorological data assimilation system to a hybrid Ensemble-Variational formulation, we are updating the aerosol component of our assimilation system to a variational ensemble type of scheme. In this talk we will examine the impact of replacing the current analysis splitting scheme with this new approach. Starting with the assimilation of satellite based single-channel retrievals; we will discuss the impact of this aerosol data assimilation technique on the 3D aerosol distributions by means of innovation statistics and verification against independent datasets such as the Aerosol Robotic Network (AERONET) and surface PM2.5. We will also present preliminary results related to the introduction of new aerosol data types in GEOS, including multi-spectral AOD retrievals.

AERONET↗
NASA NTRS2020

Aerosol Retrievals from Different Polarimeters During the ACEPOL Campaign Using a Common Retrieval Algorithm

In this paper, we present aerosol retrieval results from the ACEPOL (Aerosol Characterization from Polarimeter and Lidar) campaign, which was a joint initiative between NASA and SRON – the Netherlands Institute for Space Research. The campaign took place in October–November 2017 over the western part of the United States. During ACEPOL six different instruments were deployed on the NASA ER-2 high-altitude aircraft, including four multi-angle polarimeters (MAPs): SPEX airborne, the Airborne Hyper Angular Rainbow Polarimeter (AirHARP), the Airborne Multi-angle SpectroPolarimetric Imager (AirMSPI), and the Research Scanning Polarimeter (RSP). Also, two lidars participated: the High Spectral Resolution Lidar-2 (HSRL-2) and the Cloud Physics Lidar (CPL). Flights were conducted mainly for scenes with low aerosol load over land, but some cases with higher AOD were also observed. We perform aerosol retrievals from SPEX airborne, RSP (410–865 nm range only), and AirMSPI using the SRON aerosol retrieval algorithm and compare the results against AERONET (AErosol RObotic NETwork) and HSRL-2 measurements (for SPEX airborne and RSP). All three MAPs compare well against AERONET for the aerosol optical depth (AOD), with a mean absolute error (MAE) between 0.014 and 0.024 at 440 nm. For the fine-mode effective radius the MAE ranges between 0.021 and 0.028 µm. For the comparison with HSRL-2 we focus on a day with low AOD (0.02–0.14 at 532 nm) over the California Central Valley, Arizona, and Nevada (26 October) as well as a flight with high AOD (including measurements with AOD>1.0 at 532 nm) over a prescribed forest fire in Arizona (9 November). For the day with low AOD the MAEs in AOD (at 532 nm) with HSRL-2 are 0.014 and 0.022 for SPEX and RSP, respectively, showing the capability of MAPs to provide accurate AOD retrievals for the challenging case of low AOD over land. For the retrievals over the smoke plume a reasonable agreement in AOD between the MAPs and HSRL-2 was also found (MAE 0.088 and 0.079 for SPEX and RSP, respectively), despite the fact that the comparison is hampered by large spatial variability in AOD throughout the smoke plume. A good comparison is also found between the MAPs and HSRL-2 for the aerosol depolarization ratio (a measure of particle sphericity), with an MAE of 0.023 and 0.016 for SPEX and RSP, respectively. Finally, SPEX and RSP agree very well for the retrieved microphysical and optical properties of the smoke plume.

Fu, Guangliang↗
NASA NTRS2018

Advantages of Measuring the Q Stokes Parameter in Addition to the Total Radiance I in the Detection of Absorbing Aerosols: a Proof of Concept Using Vector Radiative Transfer, Neural Networks, and Optimal Estimation

A simple but novel study was conducted to investigate whether an imager-type spectroradiometer instrument like MODIS, currently flying on board the Aqua and Terra satellites, or MERIS, which flew on board Envisat, could detect absorbing aerosols if they could measure the Q Stokes parameter in addition to the total radiance I, that is if they could also measure the linear polarization of the light. Accurate radiative transfer calculations were used to train a fast neural network forward model, which together with a simple statistical optimal estimation scheme was used to retrieve three aerosol parameters: aerosol optical depth, fraction of absorbing aerosols, and aerosol location. The aerosols were assumed to be located either between 0 and 2 km or between 2 and 4 km in the Earth’s atmosphere. From simulated data it was found that by itself the total radiance I was generally insufficient to retrieve all three aerosol parameters, but that together with the Q Stokes component it was possible to reliably retrieve values of aerosol optical depth, fraction, and location.

Stamnes, Snorre↗
NASA NTRS2020

Untangling causality in midlatitude aerosol–cloud adjustments

Aerosol–cloud interactions represent the leading uncertainty in our ability to infer climate sensitivity from the observational record. The forcing from changes in cloud albedo driven by increases in cloud droplet number (Nd) (the first indirect effect) is confidently negative and has narrowed its probable range in the last decade, but the sign and strength of forcing associated with changes in cloud macrophysics in response to aerosol (aerosol–cloud adjustments) remain uncertain. This uncertainty reflects our inability to accurately quantify variability not associated with a causal link flowing from the cloud microphysical state to the cloud macrophysical state. Once variability associated with meteorology has been removed, covariance between the liquid water path (LWP) averaged across cloudy and clear regions (here characterizing the macrophysical state) and Nd (characterizing the microphysical) is the sum of two causal pathways linking Nd to LWP: Nd altering LWP (adjustments) and precipitation scavenging aerosol and thus depleting Nd. Only the former term is relevant to constraining adjustments, but disentangling these terms in observations is challenging. We hypothesize that the diversity of constraints on aerosol–cloud adjustments in the literature may be partly due to not explicitly characterizing covariance flowing from cloud to aerosol and aerosol to cloud. Here, we restrict our analysis to the regime of extratropical clouds outside of low-pressure centers associated with cyclonic activity. Observations from MAC-LWP (Multisensor Advanced Climatology of Liquid Water Path) and MODIS are compared to simulations in the Met Office Unified Model (UM) GA7.1 (the atmosphere model of HadGEM3-GC3.1 and UKESM1). The meteorological predictors of LWP are found to be similar between the model and observations. There is also agreement with previous literature on cloud-controlling factors finding that increasing stability, moisture, and sensible heat flux enhance LWP, while increasing subsidence and sea surface temperature decrease it. A simulation where cloud microphysics are insensitive to changes in Nd is used to characterize covariance between Nd and LWP that is induced by factors other than aerosol–cloud adjustments. By removing variability associated with meteorology and scavenging, we infer the sensitivity of LWP to changes in Nd. Application of this technique to UM GA7.1 simulations reproduces the true model adjustment strength. Observational constraints developed using simulated covariability not induced by adjustments and observed covariability between Nd and LWP predict a 25 %–30 % overestimate by the UM GA7.1 in LWP change and a 30 %–35 % overestimate in associated radiative forcing.

Daniel T. McCoy↗
NASA NTRS2021

Evidence for Systematic Changes in the Stratospheric Aerosol Size Following Volcanic Eruptions of Diverse Magnitudes Using Space-Based Instruments

An analysis of multiwavelength stratospheric aerosol extinction coefficient data from the Stratospheric Aerosol and Gas Experiment II and III/ISS instruments is used to demonstrate a coherent relationship between the perturbation in extinction coefficient in an eruption’s main aerosol layer and an apparent change in aerosol size distribution that spans multiple orders of magnitude in the stratospheric impact of an volcanic event. The relationship is measurement-based and does not rely on assumptions about the aerosol size distribution. In this respect, it may be a unique tool to verify the performance of interactive aerosol models used in GCMs and ESMs and may suggest an avenue for improving aerosol extinction coefficient measurements from single channel observations such the Optical Spectrograph and Infrared Imager System. We note limitations on this analysis including that the presence of significant amounts of ash in the main aerosol layer may significantly modulate these results.

Larry Thomason↗
NASA NTRSDate not supplied

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↗
NASA NTRSDate not supplied

Going With the Flow: Using a Particle Dispersion Model to Reveal Links Between Ocean Ecosystems and Marine Aerosols

Marine biogenic particle contributions to atmospheric aerosol concentrations are not well understood though they are important for determining cloud optical and cloud nucleating properties. Here we examine the relationship between marine aerosol measurements with satellite and model fields of ocean biology and meteorological variables during the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES). NAAMES consisted of four field campaigns between November 2015 and April 2018 that aligned with the four major phases of the annual phytoplankton bloom cycle. The FLEXPART Lagrangian particle dispersion model is used to connect these variables spatiotemporally to ship-based aerosol. We find that correlations between some aerosol measurements with satellite measured and modelled variables increase with increasing trajectory length. This indicates biological and meteorological processes over the air mass history are influential to measured particle properties. For example, results show organic aerosol mass is driven by biogenic volatile organic compound (VOC) emissions from photosynthesis by phytoplankton stocks during advection into the region. In contrast, primary marine aerosol (PMA) concentrations showed better correlations to variables weighted with shorter air mass residence times, which reflects their localized origin as primary emissions. Evidence also suggest variability in PMA concentrations likely play an important role in VOC emission removal. The removal of VOCs lessen their impact on particle number and mass concentrations. The sensitivity of marine aerosols to the main ecosystem-atmosphere drivers and its dependence on air mass history are to be further discussed.

Kevin J Sanchez↗
NASA NTRS2020

Influence of Synoptic-Dynamic Meteorology on the Long-Range Transport of Indochina Biomass Burning Aerosols

Impacts of long-range transported biomass burning aerosols from northern Indochina on regional air quality, atmospheric visibility, and climate effects have been discussed extensively in the literature over the past decade. However, the mechanism between aerosol transport and the low-level jet (LLJ) in synoptic meteorology dynamics (e.g., the frontal system) is still not fully understood. In this study, we present results of aerosol-LLJ interaction based on the National Aeronautics and Space Administration/Modern Era Retrospective-analysis for Research and Application version 2 (NASA/MERRA-2) dataset simultaneous to field campaigns in spring 2013–2015 over Southeast Asia. For linking the atmospheric circulation to aerosol transport, a general meteorological condition favorable for aerosol transport is demonstrated. Biomass burning aerosol accumulation over the source region (i.e., northern Indochina) coincided with weak westerly system over the northern South China Sea, and as the synoptic weather system evolved, the aerosols were transported to downwind regions (i.e., Taiwan and West Pacific) by a cold front and LLJ dynamics. The MERRA-2 reanalysis data show the postcold front accompanied a LLJ stream at approximately 700 hPa (3 km) and accelerated the haze plume transport eastward with a life cycle of approximately 3–5 days, an event that reoccurred multiple times from March to April. Our results indicate that coexistence of LLJ and a South China Sea anticyclone at 700 hPa, which primarily could drive the mechanism behind these transport events. Furthermore, more observational data from Southeast Asia would greatly benefit studies of aerosol-meteorology interactions in the region.

Hsiang-Yu Huang↗
NASA NTRS2021

Variabilities in Pm2.5 and Black Carbon Surface Concentrations Reproduced by Aerosol Optical Properties Estimated by In-Situ Data, Ground Based Remote Sensing and Modeling

Because of the increased temporal and spatial resolutions of the sensors onboard recently launched satellites, satellite-based surface aerosol concentration, which is usually estimated from the aerosol optical depth (AOD), is expected to become a strategic tool for air quality studies in the future. By further exploring the relationships of aerosol concentrations and their optical properties using ground observations, the accuracies of these products can be improved. Here, we analyzed collocated observations of surface mass concentrations of fine particulate matter (PM2.5) and black carbon (BC), as well as columnar aerosol optical properties from a sky radiometer and aerosol extinction profiles obtained by multi-axis differential optical absorption spectroscopy (MAX-DOAS), during the 2019–2020 period. We focused the analyses on a daily scale, emphasizing the role of the ultraviolet (UV) spectral region. Generally, the correlation between the AOD of the fine fraction (i.e., fAOD) and the PM2.5 surface concentration was moderately strong, regardless of considerations of boundary layer humidity and altitude. In contrast, the fAOD of the partial column below 1 km, which was obtained by combining sky radiometer and MAX-DOAS retrievals, better reproduced the variability of the PM2.5 and resulted in a linear relationship. In the same manner, we demonstrated that the absorption AOD of the fine fraction (fAAOD) of the partial column was related to the variability of the BC concentration. Analogous analyses based on aerosol products from the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) confirmed these findings and highlighted the importance of the shape of the aerosol profile. Overall, our results indicated a remarkable consistency among the retrieved datasets, and between the datasets and MERRA-2 products. These results confirmed the well-known sensitivity to aerosol absorption in the UV spectral region; they also highlighted the efficacy of combined MAX-DOAS and sky radiometer observations.

Alessandro Damiani↗
NASA NTRS2022

Opportunistic Experiments to Constrain Aerosol Effective Radiative Forcing

Aerosol-cloud interactions (ACI) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The non-linearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well defined sources provide ‘opportunistic experiments’ (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatio-temporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors.We review the different experimental conditions and conduct a synthesis of the available satellite data sets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change.

Matthew W Christensen↗
NASA NTRS2022

Measurement report: Closure Analysis of Aerosol–cloud Composition in Tropical Maritime Warm Convection

Cloud droplet chemical composition is a key observable property that can aid understanding of how aerosols and clouds interact. As part of the Clouds, Aerosols and Monsoon Processes – Philippines Experiment (CAMP2Ex), three case studies were analyzed involving collocated airborne sampling of relevant clear and cloudy air masses associated with maritime warm convection. Two of the cases represented a polluted marine background, with signatures of transported East Asian regional pollution, aged over water for several days, while the third case comprised a major smoke transport event from Kalimantan fires. Sea salt was a dominant component of cloud droplet composition, in spite of fine particulate enhancement from regional anthropogenic sources. Furthermore, the proportion of sea salt was enhanced relative to sulfate in rainwater and may indicate both a propensity for sea salt to aid warm rain production and an increased collection efficiency of large sea salt particles by rain in subsaturated environments. Amongst cases, as precipitation became more significant, so too did the variability in the sea salt to (non-sea salt) sulfate ratio. Across cases, nitrate and ammonium were fractionally greater in cloud water than fine-mode aerosol particles; however, a strong covariability in cloud water nitrate and sea salt was suggestive of prior uptake of nitrate on large salt particles. A mass-based closure analysis of non-sea salt sulfate compared the cloud water air-equivalent mass concentration to the concentration of aerosol particles serving as cloud condensation nuclei for droplet activation. While sulfate found in cloud was generally constrained by the sub-cloud aerosol concentration, there was significant intra-cloud variability that was attributed to entrainment – causing evaporation of sulfate-containing droplets –and losses due to precipitation. In addition, precipitation tended to promote mesoscale variability in the sub-cloud aerosol through a combination of removal, convective downdrafts, and dynamically driven convergence. Physical mechanisms exerted such strong control over the cloud water compositional budget that it was not possible to isolate any signature of chemical production/loss using in-cloud observations. The cloud-free environment surrounding the non-precipitating smoke case indicated sulfate enhancement compared to convective mixing quantified by a stable gas tracer; however, this was not observed in the cloud water (either through use of ratios or the mass closure), perhaps implying that the warm convective cloud timescale was too short for chemical production to be a leading-order budgetary term and because precursors had already been predominantly exhausted. Closure of other species was truncated by incomplete characterization of coarse aerosol (e.g., it was found that only 10 %–50% of sea salt mass found in cloud was captured during clear-air sampling) and unmeasured gasphase abundances affecting closure of semi-volatile aerosol species (e.g., ammonium, nitrate and organic) and soluble volatile organic compound contributions to total organic carbon in cloud water.

Ewan Crosbie↗