Aerosol Observations Research Articles

Design and Verification of a Double-Grating Spectrometer System (DGSS) for Simultaneous Observation of Aerosols, Water Vapor and Clouds

Simultaneous observation of aerosols, water vapor, and clouds is conducive to the analysis of their interactions, and the consistency of observation equipment, instrument performance, and observation time is crucial. Molecular oxygen A-band (758–778 nm) and water vapor absorption band (758–880 nm) are two bands with similar wavelengths, and the hyperspectral remote sensing information of these two bands can be exploited to invert the vertical profile of aerosol and water vapor. In this paper, a double-grating spectrometer system (DGSS) was developed. DGSS uses a telescope system and fiber to introduce multi-angle, double-band sunlight, and it splits light synchronously (non-sequentially) to different positions of the detector through a slit plate and two gratings. The DGSS was calibrated in the laboratory and observed in the external field. The results indicated that the spectral resolution reached 0.06 nm (molecular oxygen A-band, 758–778 nm) and 0.24 nm (water vapor absorption band, 758–880 nm). Meanwhile, the spectra of the two bands (three angles in each band) are not aliased on the detector. Besides, the multi-angle simultaneous observation of the high-resolution spectra of the two bands is realized, which proves the effectiveness of this method. This study will provide a scientific basis for the observation of aerosol, water vapor, and cloud ground-based networks.

Assessing the Impact of Atmospheric CO2 and NO2 Measurements From Space on Estimating City-Scale Fossil Fuel CO2 Emissions in a Data Assimilation System

The European Copernicus programme plans to install a constellation of multiple polar orbiting satellites (Copernicus Anthropogenic CO2 Monitoring Mission, CO2M mission) for observing atmospheric CO2 content with the aim to estimate fossil fuel CO2 emissions. We explore the impact of potential CO2M observations of column-averaged CO2 (XCO2), nitrogen dioxide (NO2), and aerosols in a 200 × 200 km2 domain around Berlin. For the quantification of anticipated XCO2 random and systematic errors we developed and applied new error parameterisation formulae based on artificial neural networks. For the interpretation of these data, we further established a CCFFDAS modelling chain from parameters of emission models to XCO2 and NO2 observations to simulate the 24 h periods preceeding simulated CO2M overpasses over the study area. For one overpass in winter and one in summer, we present a number of assessments of observation impact in terms of the posterior uncertainty in fossil fuel emissions on scales ranging from 2 to 200 km. This means the assessments include temporal and spatial scales typically not covered by inventories. The assessments differentiate the fossil fuel CO2 emissions into two sectors, an energy generation sector (power plants) and the complement, which we call “other sector.” We find that combined measurements of XCO2 and aerosols provide a powerful constraint on emissions from larger power plants; the uncertainty in fossil fuel emissions from the largest three power plants in the domain was reduced by 60%–90% after assimilating the observations. Likewise, these measurements achieve an uncertainty reduction for the other sector that increases when aggregated to larger spatial scales. When aggregated over Berlin the uncertainty reduction for the other sector varies between 28% and 48%. Our assessments show a considerable contribution of aerosol observations onboard CO2M to the constraint of the XCO2 measurements on emissions from all power plants and for the other sector on all spatial scales. NO2 measurements onboard CO2M provide a powerful additional constraint on the emissions from power plants and from the other sector. We further apply a Jacobian representation of the CCFFDAS modelling chain to decompose a simulated CO2 column in terms of spatial emission impact. This analysis reveals the complex structure of the footprint of an observed CO2 column, which indicates the limits of simple mass balances approaches for interpretation of such observations.

The COMBLE Campaign: A Study of Marine Boundary Layer Clouds in Arctic Cold-Air Outbreaks

Abstract One of the most intense air mass transformations on Earth happens when cold air flows from frozen surfaces to much warmer open water in cold-air outbreaks (CAOs), a process captured beautifully in satellite imagery. Despite the ubiquity of the CAO cloud regime over high-latitude oceans, we have a rather poor understanding of its properties, its role in energy and water cycles, and its treatment in weather and climate models. The Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) was conducted to better understand this regime and its representation in models. COMBLE aimed to examine the relations between surface fluxes, boundary layer structure, aerosol, cloud, and precipitation properties, and mesoscale circulations in marine CAOs. Processes affecting these properties largely fall in a range of scales where boundary layer processes, convection, and precipitation are tightly coupled, which makes accurate representation of the CAO cloud regime in numerical weather prediction and global climate models most challenging. COMBLE deployed an Atmospheric Radiation Measurement Mobile Facility at a coastal site in northern Scandinavia (69°N), with additional instruments on Bear Island (75°N), from December 2019 to May 2020. CAO conditions were experienced 19% (21%) of the time at the main site (on Bear Island). A comprehensive suite of continuous in situ and remote sensing observations of atmospheric conditions, clouds, precipitation, and aerosol were collected. Because of the clouds’ well-defined origin, their shallow depth, and the broad range of observed temperature and aerosol concentrations, the COMBLE dataset provides a powerful modeling testbed for improving the representation of mixed-phase cloud processes in large-eddy simulations and large-scale models.

Probing into the wintertime meteorology and particulate matter (PM2.5 and PM10) forecast over Delhi

The Indian Institute of Tropical Meteorology (IITM), in partnership with the National Center for Atmospheric Research (NCAR), has developed a high resolution (400 m) air-quality Early Warning System (EWS) for Delhi using an advanced approach of assimilating aerosol optical depth, fire emissions from a space-borne platform, and real-time aerosol observations from in-situ network in WRF-Chem model to produce a 72-h forecast. The present study summarizes the performance of EWS forecast and prevailing meteorological conditions for winter months of 2020–2021. We examined the performance of model-simulated meteorology by comparing against the in-situ observations. The model shows a positive bias in downwelling shortwave radiation (≈ 34 Wm−2) and warm bias in near-surface temperature (≈ 3 K). The simulated winds while having realistic magnitudes depict more southwesterly behavior compared to the observations. The model struggles to accurately predict Planetary Boundary Layer Height. The model realistically simulates the relationship between wind and air quality parameters. The air quality forecast from the model is found to be skillful in three different AQI categories, with accuracy > 88% for critical category events. The model also exhibits good statistical performance in predicting AQI, with low mean bias (¡ 8%), high correlation (¿ 0.68), and low variance (NMSE ¡ 0.09).

Aircraft measurements of water vapor heavy isotope ratios in the marine boundary layer and lower troposphere during ORACLES

Abstract. This paper presents aircraft in situ measurements of water concentration and heavy water isotope ratios D/H and 18O/16O during the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) project. The aircraft measurement system is also presented. The dataset is unique in that (1) it contains both total water and cloud condensed water isotope ratios; (2) it spans sufficient space and time to enable construction of spatially resolved climatology of isotope ratios in the lower troposphere; and (3) it is paired with a wealth of complementary measurements on atmospheric thermodynamic, chemical, aerosol, and radiative properties. Aircraft sampling took place in the southeast Atlantic marine boundary layer and lower troposphere (Equator to 22∘ S) over the months of September 2016, August 2017, and October 2018. Isotope measurements were made using cavity ring-down spectroscopic analyzers integrated into the Water Isotope System for Precipitation and Entrainment Research (WISPER). From an isotope perspective, the 300+ h of 1 Hz in situ data at levels in the atmosphere ranging from 70 m to 7 km represents a remarkably large and vertically resolved dataset. This paper provides a brief overview of the ORACLES mission and describes how water vapor heavy isotope ratios fit within the experimental design. Overviews of the sampling region and sampling strategy are presented, followed by the WISPER system setup and calibration details. The three data formats available to the users are each covered (latitude–altitude curtains, individual vertical profiles, and time series), with illustrative examples to highlight some features of the dataset and provide a plausibility check. The curtains and profiles demonstrate the dataset's potential to provide a comprehensive perspective on moisture transport and isotopic content in this region. Finally, measurement uncertainties are provided. Curtain and vertical profile data for all sampling periods can be accessed at https://doi.org/10.5281/zenodo.5748368 (see Henze et al., 2022). Time series data for the September 2016, August 2017, and October 2018 sampling periods can be accessed at https://doi.org/10.5067/Suborbital/ORACLES/P3/2016_V3, https://doi.org/10.5067/Suborbital/ORACLES/P3/2017_V3, and https://doi.org/10.5067/Suborbital/ORACLES/ P3/2018_V3, respectively (see references for ORACLES Science Team, 2020a–c, 2016 P3 data, 2017 P3 data, and 2018 P3 data).

Simultaneous Characterization of Wildfire Smoke and Surface Properties With Imaging Spectroscopy During the FIREX-AQ Field Campaign.

We introduce and evaluate an approach for the simultaneous retrieval of aerosol and surface properties from Airborne Visible/Infrared Imaging Spectrometer Classic (AVIRIS‐C) data collected during wildfires. The joint National Aeronautics and Space Administration (NASA) National Oceanic and Atmospheric Administration Fire Influence on Regional to Global Environments and Air Quality field campaign took place in August 2019, and involved two aircraft and coordinated ground‐based observations. The AVIRIS‐C instrument acquired data from onboard NASA's high altitude ER‐2 research aircraft, coincident in space and time with aerosol observations obtained from the Aerosol Robotic Network (AERONET) DRAGON mobile platform in the smoke plume downwind of the Williams Flats Fire in northern Washington in August 2019. Observations in this smoke plume were used to assess the capacity of optimal‐estimation based retrievals to simultaneously estimate aerosol optical depth (AOD) and surface reflectance from Visible Shortwave Infrared (VSWIR) imaging spectroscopy. Radiative transfer modeling of the sensitivities in spectral information collected over smoke reveal the potential capacity of high spectral resolution retrievals to distinguish between sulfate and smoke aerosol models, as well as sensitivity to the aerosol size distribution. Comparison with ground‐based AERONET observations demonstrates that AVIRIS‐C retrievals of AOD compare favorably with direct sun AOD measurements. Our analyses suggest that spectral information collected from the full VSWIR spectral interval, not just the shortest wavelengths, enables accurate retrievals. We use this approach to continuously map both aerosols and surface reflectance at high spatial resolution across heterogeneous terrain, even under relatively high AOD conditions associated with wildfire smoke.

Optical properties and spectral dependence of aerosol light absorption over the Brazilian Pantanal

Characterizing optical properties of aerosols, particularly the absorption processes, is fundamental for understanding the role of these particles in ecosystems as well as the climate, in general. Currently, changes in precipitation regimes in the southern Amazon basin have resulted in a considerable increase in biomass burning, whereby large amounts of aerosols and gases are emitted into the atmosphere. These increased emissions can impact the ecosystem, modifying mass and energy flows at the surface. This study, motivated by the need for more aerosol observations was the result of a long-term campaign carried out in the Brazilian Pantanal, which provided continuous in-situ measurements of aerosol optical properties between January 2017 and December 2019. From these data, optical properties of aerosols were quantified and analyzed seasonally. Corrected estimates for absorption coefficient (σabs) and Angstrom absorption exponent (αabs) were utilized to characterize the spectral dependence of absorption by aerosols. With additional measurements of the scattering coefficient (σscat), it was possible to evaluate the single scattering albedo (ω0). The mean values for σabs, σscat, ω0 at 525 nm and αabs 370–880 nm during the wet season were 0.66 ± 0.58 Mm−1, 6.16 ± 5.75 Mm−1, 0.90 ± 0.06 and 1.43 ± 0.49, respectively. These values, within measurement uncertainties, were similar to results found in the central Amazon. During the dry season, absorption and scattering increased approximately 88% and 86%, respectively, providing strong evidence for the contribution of local and regional emissions from biomass burning. The values of ω0 did not reveal significant seasonal differences, however, a sharp reduction was observed, medians below 0.8, at the beginning of the burning period, which was associated with more recent local burnings and, therefore, greater absorption. The mean values evaluated for different spectral intervals reveal a strong contribution of brown carbon (BrC) during the dry season, with medians of 1.78 and 0.87 for the intervals of 370–590 nm and 590–880 nm, respectively. This work also quantified BC concentrations for the dry and wet seasons, obtaining mean values of 0.75 ± 0.83 and 0.12 ± 0.09 μgm−3, respectively. In general, a striking similarity was encountered for aerosol optical properties between the Pantanal and the Central Amazon during the wet season. The results presented here characterize the background values for aerosol optical properties in the Pantanal, and the additional effects resulting from biomass burning emissions, therefore providing essential information to assess the effects these particles have on the ecosystem.

Observations of the Development and Vertical Structure of the Lake-Breeze Circulation during the 2017 Lake Michigan Ozone Study

Abstract Ground-based thermodynamic and kinematic profilers were placed adjacent to the western shore of Lake Michigan at two sites as part of the 2017 Lake Michigan Ozone Study. The southern site near Zion, Illinois, hosted a microwave radiometer (MWR) and a sodar wind profiler, while the northern site in Sheboygan, Wisconsin, featured an Atmospheric Emitted Radiance Interferometer (AERI), a Doppler lidar, and a High Spectral Resolution Lidar (HSRL). Each site experienced several lake-breeze events during the experiment. Composite time series and time–height cross sections were constructed relative to the lake-breeze arrival time so that commonalities across events could be explored. The composited surface observations indicate that the wind direction of the lake breeze was consistently southeasterly at both sites regardless of its direction before the arrival of the lake-breeze front. Surface relative humidity increased with the arriving lake breeze, though this was due to cooler air temperatures as absolute moisture content stayed the same or decreased. The profiler observations show that the lake breeze penetrated deeper when the local environment was unstable and preexisting flow was weak. The cold air associated with the lake breeze remained confined to the lowest 200 m of the troposphere even if the wind shift was observed at higher altitudes. The evolution of the lake breeze corresponded well to observed changes in baroclinicity and calculated changes in circulation. Collocated observations of aerosols showed increases in number and mass concentrations after the passage of the lake-breeze front.

Plumes and blooms – Locally-sourced Fe-rich aeolian mineral dust drives phytoplankton growth off southwest Africa

Ocean-based photosynthesis accounts for half of global primary production. Productivity rates, driven by phytoplanktonic responses to nutrient availability, are however highly variable both spatially and temporally throughout the oceans. Intense primary production in the ocean's most productive areas, the Eastern Boundary Upwelling Systems (EBUS), cannot be fully explained by nutrient upwelling alone, with the role of local dust sources and complimentary aeolian nutrient delivery largely overlooked. Here we explore relationships between iron-rich dust plumes emanating from a significant regional dust source, Namibia's ephemeral river valleys, and blooms of phytoplankton growth off southwest Africa in the Benguela Upwelling System (BUS). We constrain dust source dynamics through field measurement of in-valley airborne dust concentrations made at daily resolution, and couple these with satellite observations of atmospheric aerosols, ocean phytoplankton concentrations, and sea surface temperature over a six-month period encompassing the known ‘dust season’ of the valley sources. Phytoplanktonic responses in BUS waters to individual dust emission events were identified and were importantly shown to be unassociated with upwelling events. We demonstrate a fast (1–2 day) chlorophyllic response to observed iron-rich dust emissions, a relationship that is concealed by monthly averaged data. We show that terrestrial in-valley airborne dust concentrations correlate with offshore increases in phytoplankton concentrations, providing the first study of oceanic response that is directly linked with a specific monitored terrestrial dust source.

A three-dimensional variational data assimilation system for aerosol optical properties based on WRF-Chem v4.0: design, development, and application of assimilating Himawari-8 aerosol observations

Abstract. This paper presents a three-dimensional variational (3DVAR) data assimilation (DA) system for aerosol optical properties, including aerosol optical thickness (AOT) retrievals and lidar-based aerosol profiles, developed for the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) within the Weather Research and Forecasting model coupled to Chemistry (WRF-Chem) model. For computational efficiency, 32 model variables in the MOSAIC_4bin scheme are lumped into 20 aerosol state variables that are representative of mass concentrations in the DA system. To directly assimilate aerosol optical properties, an observation operator based on the Mie scattering theory was employed, which was obtained by simplifying the optical module in WRF-Chem. The tangent linear (TL) and adjoint (AD) operators were then established and passed the TL/AD sensitivity test. The Himawari-8 derived AOT data were assimilated to validate the system and investigate the effects of assimilation on both AOT and PM2.5 simulations. Two comparative experiments were performed with a cycle of 24 h from 23 to 29 November 2018, during which a heavy air pollution event occurred in northern China. The DA performances of the model simulation were evaluated against independent aerosol observations, including the Aerosol Robotic Network (AERONET) AOT and surface PM2.5 measurements. The results show that Himawari-8 AOT assimilation can significantly improve model AOT analyses and forecasts. Generally, the control experiments without assimilation seriously underestimated AOTs compared with observed values and were therefore unable to describe real aerosol pollution. The analysis fields closer to observations improved AOT simulations, indicating that the system successfully assimilated AOT observations into the model. In terms of statistical metrics, assimilating Himawari-8 AOTs only limitedly improved PM2.5 analyses in the inner simulation domain (D02); however, the positive effect can last for over 24 h. Assimilation effectively enlarged the underestimated PM2.5 concentrations to be closer to the real distribution in northern China, which is of great value for studying heavy air pollution events.

Factors affecting precipitation formation and precipitation susceptibility of marine stratocumulus with variable above- and below-cloud aerosol concentrations over the Southeast Atlantic

Abstract. Aerosol–cloud–precipitation interactions (ACIs) provide the greatest source of uncertainties in predicting changes in Earth's energy budget due to poor representation of marine stratocumulus and the associated ACIs in climate models. Using in situ data from 329 cloud profiles across 24 research flights from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign in September 2016, August 2017, and October 2018, it is shown that contact between above-cloud biomass burning aerosols and marine stratocumulus over the Southeast Atlantic Ocean was associated with precipitation suppression and a decrease in the precipitation susceptibility (So) to aerosols. The 173 “contact” profiles with aerosol concentration (Na) greater than 500 cm−3 within 100 m above cloud tops had a 50 % lower precipitation rate (Rp) and a 20 % lower So, on average, compared to 156 “separated” profiles with Na less than 500 cm−3 up to at least 100 m above cloud tops. Contact and separated profiles had statistically significant differences in droplet concentration (Nc) and effective radius (Re) (95 % confidence intervals from a two-sample t test are reported). Contact profiles had 84 to 90 cm−3 higher Nc and 1.4 to 1.6 µm lower Re compared to separated profiles. In clean boundary layers (below-cloud Na less than 350 cm−3), contact profiles had 25 to 31 cm−3 higher Nc and 0.2 to 0.5 µm lower Re. In polluted boundary layers (below-cloud Na exceeding 350 cm−3), contact profiles had 98 to 108 cm−3 higher Nc and 1.6 to 1.8 µm lower Re. On the other hand, contact and separated profiles had statistically insignificant differences between the average liquid water path, cloud thickness, and meteorological parameters like surface temperature, lower tropospheric stability, and estimated inversion strength. These results suggest the changes in cloud microphysical properties were driven by ACIs rather than meteorological effects, and adjustments to existing relationships between Rp and Nc in model parameterizations should be considered to account for the role of ACIs.

Indications of a Decrease in the Depth of Deep Convective Cores with Increasing Aerosol Concentration during the CACTI Campaign

AbstractAn aerosol indirect effect on deep convective cores (DCCs), by which increasing aerosol concentration increases cloud-top height via enhanced latent heating and updraft velocity, has been proposed in many studies. However, the magnitude of this effect remains uncertain due to aerosol measurement limitations, modulation of the effect by meteorological conditions, and difficulties untangling meteorological and aerosol effects on DCCs. The Cloud, Aerosol, and Complex Terrain Interactions (CACTI) campaign in 2018–19 produced concentrated aerosol and cloud observations in a location with frequent DCCs, providing an opportunity to examine the proposed aerosol indirect effect on DCC depth in a rigorous and robust manner. For periods throughout the campaign with well-mixed boundary layers, we analyze relationships that exist between aerosol variables (condensation nuclei concentration > 10 nm, 0.4% cloud condensation nuclei concentration, 55–1000-nm aerosol concentration, and aerosol optical depth) and meteorological variables [level of neutral buoyancy (LNB), convective available potential energy, midlevel relative humidity, and deep-layer vertical wind shear] with the maximum radar-echo-top height and cloud-top temperature (CTT) of DCCs. Meteorological variables such as LNB and deep-layer shear are strongly correlated with DCC depth. LNB is also highly correlated with three of the aerosol variables. After accounting for meteorological correlations, increasing values of the aerosol variables [with the exception of one formulation of aerosol optical depth (AOD)] are generally correlated at a statistically significant level with a warmer CTT of DCCs. Therefore, for the study region and period considered, increasing aerosol concentration is mostly associated with a decrease in DCC depth.

On the stratospheric chemistry of midlatitude wildfire smoke

SignificanceLarge wildfires have been observed to inject smoke into the stratosphere, raising questions about their potential to affect the stratospheric ozone layer that protects life on Earth from biologically damaging ultraviolet radiation. Multiple observations of aerosol and NO2 concentrations from three independent satellite instruments are used here together with model calculations to identify decreases in stratospheric NO2 concentrations following major Australian 2019 through 2020 wildfires. The data confirm that important chemistry did occur on the smoke particle surfaces. The observed behavior in NO2 with increasing particle concentrations is a marker for surface chemistry that contributes to midlatitude ozone depletion. The results indicate that increasing wildfire activity in a warming world may slow the recovery of the ozone layer.

Year-round observation of atmospheric inorganic aerosols in urban Beijing: Size distribution, source analysis, and reduction mechanism

To investigate particle characteristics and find an effective measure to control severe particle pollution, year-round observation of size-segregated inorganic aerosols was conducted in Beijing from January to December, 2016. The sampled atmospheric particles all presented bimodal size distribution at four pollution levels (clear, slight pollution, moderate pollution and severe pollution), and peak values appeared at the size range of 0.7-2.1 μm and >9.0 μm, respectively. As dominant particle compositions, NO3−, SO42−, and NH4+ in four pollution levels all showed significant peaks in fine mode, especially at the size range of 1.1-2.1 μm. Secondary inorganic aerosols accounted for about 67.6% (36.3% (secondary sulfates) + 31.3% (secondary nitrates)) of the total sources of fine particles in urban Beijing. Severe pollution of fine particles was mainly caused by the air masses transported from nearby western and southern areas, which are industrial and densely populated region, respectively. Sensitivity tests further revealed that the control measures focusing on ammonium emission reduction was the most effective for particle pollution mitigation, and fine particles all showed nonlinear responses after reducing ammonium, nitrate, and sulfate concentrations, with the fitting curves of y = -120.8x - 306.1x2 + 290.2x3, y = -43.5x - 67.8x2, and y = -25.8x - 110.4x2 + 7.6x3, respectively (y and x present fine particle mass variation (μg/m3) and concentration reduction ratio (CRR)/100 (dimensionless)). Overall, our study presents useful information for understanding the characteristics of atmospheric inorganic aerosols in urban Beijing, as well as offers policy makers with effective measure for mitigating particle pollution.

A Novel Network‐Based Approach to Determining Measurement Representation Error for Model Evaluation of Aerosol Microphysical Properties

AbstractAtmospheric aerosol size and abundance influence radiative effects and climate change. To date, efforts to constrain global climate models' radiative forcing with in situ aerosol observations have been hamstrung by uncertainty. One source of error, the regional “representation error,” arises when accurate but sparse single‐point measurements of atmospheric aerosol distributions are compared with a model value, assuming that the single‐point measurement is representative of the model domain. The Portable Optical Particle Spectrometer network in the Southern Great Plains (POPSnet‐SGP) campaign has demonstrated that a network of nearly autonomous aerosol instruments operating at ambient temperature and relative humidity (with low measurement error) may be used to quantify measurement representation error and investigate the factors introducing heterogeneity in aerosol distributions across a rural, continental background region. Measurements were made using Portable Optical Particle Spectrometer (POPS) instruments at several sites for five months across the Department of Energy's Aerosol Radiation Measurement Southern Great Plains (ARM‐SGP) User Facility in the central USA. Measurement representation error decreased with longer averaging periods (20%–40% between 1 s and 1 day), varied between sites by 10%–20% for aerosol concentration 140–2,500 nm in diameter (N_140), and was higher for aerosols >400 nm in diameter (N_400). Our measurements also show the influence of local meteorology on aerosol surface area (A_140) and size distributions: A_140 is positively correlated with wind speed and relative humidity, negatively correlated with precipitation, and lower given westerly winds. We conclude that the POPSnet approach provides considerably more insight into the spatial variability in the aerosol population that can be used to constrain climate models than would be available from similar networks of PM 2.5 monitors.

Biomass burning aerosol heating rates from the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) 2016 and 2017 experiments

Abstract. Aerosol heating due to shortwave absorption has implications for local atmospheric stability and regional dynamics. The derivation of heating rate profiles from space-based observations is challenging because it requires the vertical profile of relevant properties such as the aerosol extinction coefficient and single-scattering albedo (SSA). In the southeastern Atlantic, this challenge is amplified by the presence of stratocumulus clouds below the biomass burning plume advected from Africa, since the cloud properties affect the magnitude of the aerosol heating aloft, which may in turn lead to changes in the cloud properties and life cycle. The combination of spaceborne lidar data with passive imagers shows promise for future derivations of heating rate profiles and curtains, but new algorithms require careful testing with data from aircraft experiments where measurements of radiation, aerosol, and cloud parameters are better colocated and readily available. In this study, we derive heating rate profiles and vertical cross sections (curtains) from aircraft measurements during the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) project in the southeastern Atlantic. Spectrally resolved irradiance measurements and the derived column absorption allow for the separation of total heating rates into aerosol and gas (primarily water vapor) absorption. The nine cases we analyzed capture some of the co-variability of heating rate profiles and their primary drivers, leading to the development of a new concept: the heating rate efficiency (HRE; the heating rate per unit aerosol extinction). HRE, which accounts for the overall aerosol loading as well as vertical distribution of the aerosol layer, varies little with altitude as opposed to the standard heating rate. The large case-to-case variability for ORACLES is significantly reduced after converting from heating rate to HRE, allowing us to quantify its dependence on SSA, cloud albedo, and solar zenith angle.

Modeled and observed properties related to the direct aerosol radiative effect of biomass burning aerosol over the southeastern Atlantic

Abstract. Biomass burning smoke is advected over the southeastern Atlantic Ocean between July and October of each year. This smoke plume overlies and mixes into a region of persistent low marine clouds. Model calculations of climate forcing by this plume vary significantly in both magnitude and sign. NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) had deployments for field campaigns off the west coast of Africa in 3 consecutive years (September 2016, August 2017, and October 2018) with the goal of better characterizing this plume as a function of the monthly evolution by measuring the parameters necessary to calculate the direct aerosol radiative effect. Here, this dataset and satellite retrievals of cloud properties are used to test the representation of the smoke plume and the underlying cloud layer in two regional models (WRF-CAM5 and CNRM-ALADIN) and two global models (GEOS and UM-UKCA). The focus is on the comparisons of those aerosol and cloud properties that are the primary determinants of the direct aerosol radiative effect and on the vertical distribution of the plume and its properties. The representativeness of the observations to monthly averages are tested for each field campaign, with the sampled mean aerosol light extinction generally found to be within 20 % of the monthly mean at plume altitudes. When compared to the observations, in all models, the simulated plume is too vertically diffuse and has smaller vertical gradients, and in two of the models (GEOS and UM-UKCA), the plume core is displaced lower than in the observations. Plume carbon monoxide, black carbon, and organic aerosol masses indicate underestimates in modeled plume concentrations, leading, in general, to underestimates in mid-visible aerosol extinction and optical depth. Biases in mid-visible single scatter albedo are both positive and negative across the models. Observed vertical gradients in single scatter albedo are not captured by the models, but the models do capture the coarse temporal evolution, correctly simulating higher values in October (2018) than in August (2017) and September (2016). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (<4 %) uncertainty in integrated solar absorption by the aerosol and, therefore, in the aerosol direct radiative effect. Model biases in cloud fraction, and, therefore, the scene albedo below the plume, vary significantly across the four models. The optical thickness of clouds is, on average, well simulated in the WRF-CAM5 and ALADIN models in the stratocumulus region and is underestimated in the GEOS model; UM-UKCA simulates cloud optical thickness that is significantly too high. Overall, the study demonstrates the utility of repeated, semi-random sampling across multiple years that can give insights into model biases and how these biases affect modeled climate forcing. The combined impact of these aerosol and cloud biases on the direct aerosol radiative effect (DARE) is estimated using a first-order approximation for a subset of five comparison grid boxes. A significant finding is that the observed grid box average aerosol and cloud properties yield a positive (warming) aerosol direct radiative effect for all five grid boxes, whereas DARE using the grid-box-averaged modeled properties ranges from much larger positive values to small, negative values. It is shown quantitatively how model biases can offset each other, so that model improvements that reduce biases in only one property (e.g., single scatter albedo but not cloud fraction) would lead to even greater biases in DARE. Across the models, biases in aerosol extinction and in cloud fraction and optical depth contribute the largest biases in DARE, with aerosol single scatter albedo also making a significant contribution.

Seasonal observation and source apportionment of carbonaceous aerosol from forested rural site (Lithuania)

In this work, we conducted a study of the stable carbon isotope ratios of total carbon (δ13CTC) for submicron aerosol particles (<1 μm) that were collected year round (2014) at a hemiboreal forest site in Lithuania. Higher δ13CTC values characterised the seasonal variation in δ13CTC during the cold season (average −26.9 ± 0.7‰) with lower values observed during the warm season (−27.6 ± 0.6‰). The total carbon (TC) concentration was below 8 μg/m3 during the one-year measurement period. There was one pollution event in autumn when concentrations reached up to 14.8 μg/m3. In addition to the offline analysis of the filter samples, the online measurements of aerosol physical and chemical properties were conducted from 15 May to September 27, 2014 by operating the Aethalometer AE-31 and a quadrupole-type Aerosol Chemical Speciation Monitor (ACSM). Source apportionment was conducted by analysing the ACSM mass spectra using Positive Matrix Factorisation (PMF). Three main factors were derived, pointing to primary emissions from biomass burning along with the secondary formation of less and more oxygenated organic aerosol of biogenic origin. A comparative analysis of δ13CTC with organic carbon (OC), elemental carbon (EC), and organic markers justified two dominant sources (biomass burning and fossil fuel combustion) of aerosol particles at the hemiboreal forest site during the cold season.

The SOLA Award in 2021

The Editorial Committee of Scientific Online Letters on the Atmosphere (SOLA) gives The SOLA Award to outstanding paper(s) published each year. We are pleased to announce that The SOLA Award in 2021 will be presented to the paper by Drs. Koichi Shiraishi and Takashi Shibata, entitled “Seasonal variation in high arctic stratospheric aerosols observed by lidar at Ny Ålesund, Svalbard between March 2014 and February 2018” (Shiraishi and Shibata 2021). Stratospheric aerosols play essential roles in radiative and chemical processes in the atmosphere and impact the climate of the Earth. The lidar observations of the temporal and spatial variations of the aerosols will provide essential information to understand the atmospheric processes related to the aerosols. Thus, there have been many studies on lidar observations of aerosols in the low and middle latitude regions. However, the observations in the Arctic are limited. In particular, there are no long-term observations of stratospheric aerosols throughout the year in the high Arctic. This study investigates the seasonal variations of stratospheric aerosols in the high Arctic by using long-term observations for about four years at Ny Ålesund, Svalbard. By carefully removing data affected by polar stratospheric clouds and volcanic eruption, the analysis shows the robust characteristics of the seasonal variations of background aerosols in the stratosphere. It is found that the backscattering ratio takes maximum values at altitudes between 13 and 16 km from December to March and at altitudes between 17 and 20 km from April to November. This observational evidence is highly evaluated in presenting the seasonal variations of stratospheric aerosols in the high Arctic, which will be helpful to understand the dynamical and chemical processes in the stratosphere. The Editorial Committee of SOLA highly evaluates the significance of this study and therefore presents “The SOLA Award.”

Simultaneous Measurements of Carbonaceous Aerosol in Three Major Cities in the Beijing-Tianjin-Hebei Region, China

Simultaneous observations of carbonaceous aerosols in multiple cities are of great significance for a comprehensive understanding of the level of carbonaceous aerosol pollution in the Beijing-Tianjin-Hebei (BTH) region. In this study, PM2.5 samples were collected simultaneously in Beijing (BJ), Tianjin (TJ), and Shijiazhuang (SJZ) during the 2017–2018 heating season, and the contents of organic carbon (OC) and elemental carbon (EC) in the samples were measured. The mean mass concentrations were 10.15‒46.23 µg m–3 for OC, and 2.13‒10.42 µg m–3 for EC in three cities. SJZ had more serious carbonaceous aerosols pollution compared with BJ and TJ. The OC and EC levels in three cities, especially in Beijing, were significantly lower than those reported in previous studies, implying the effectivity of strict air pollution control measures in 2017. Based on the OC/EC minimum ratio method, the mass concentration of secondary organic carbon (SOC) was estimated, and SOC pollution in BJ was relatively light. Analysis of eight carbonaceous components showed that the gasoline vehicle exhaust sources made high contributions to the levels of carbonaceous aerosols in all three cities. Compared with SJZ, the carbonaceous aerosols in BJ and TJ were more affected by road dust pollution. Analysis of backward trajectory indicated that the carbonaceous aerosols in the three cities were affected by pollution transport from the BTH region and surrounding areas, in addition to local sources. In contrast to the other two cities, OC and EC in SJZ were greatly affected by short-distance air mass transport from Hebei Province.