Aerosol Model Research Articles

Instantaneous aerosol and surface retrieval using satellites in geostationary orbit (iAERUS-GEO) – estimation of 15 min aerosol optical depth from MSG/SEVIRI and evaluation with reference data

Abstract. Geostationary meteorological satellites are unique tools to monitor atmospheric aerosols from space. The observation of the Earth several times per hour allows these types of imaging systems to provide high-temporal-resolution observations of these suspended particles, which are of interest for research and operational topics, including climate, air quality, numerical weather prediction, and volcanic risk management. However, some challenges need to be addressed to achieve the sub-daily retrieval of aerosol properties mainly due to the varying sensitivity of geostationary imagers to aerosols during the day. In this article we propose a new algorithm named iAERUS-GEO (instantaneous Aerosol and surfacE Retrieval Using Satellites in GEOstationary orbit) that estimates the diurnal evolution of aerosol optical depth (AOD) over land and ocean from the Meteosat Second Generation (MSG) satellite. This is achieved by the use of an optimal-estimation method combined with several aerosol models and other features, including the daily retrieval of the surface reflectance directionality using Kalman filtering. AOD estimates provided by iAERUS-GEO every 15 min – the acquisition frequency of the Spinning Enhanced Visible InfraRed Imager (SEVIRI) on MSG – are assessed with collocated reference aerosol observations. First, comparison to AERONET ground-based data proves the overall satisfactory accuracy of iAERUS-GEO over land, with the exception of some higher biases found over bright surfaces and for high scattering angles. The confidence measure provided by iAERUS-GEO is proved useful to filter these less satisfactory retrievals that generally arise due to a low information content on aerosols provided by SEVIRI. Second, comparison to the GRASP/POLDER satellite product shows similar scores for the two aerosol data sets, with a significantly larger number of retrievals for iAERUS-GEO. This added value – which we illustrate here by inspecting the sub-daily variation in AOD over selected regions – allows geostationary satellites to break the temporal barrier set by traditional aerosol remote sensing from the low Earth orbit. Furthermore, the aerosol retrievals presented in this work are expected to be improved in the near future thanks to the enhanced sensing capabilities of the upcoming Meteosat Third Generation Imager mission.

Assessment of severe aerosol events from NASA MODIS and VIIRS aerosol products for data assimilation and climate continuity

Abstract. While the use and data assimilation (DA) of operational Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol data is commonplace, MODIS is scheduled to sunset in the next year. For data continuity, focus has turned to the development of next-generation aerosol products and sensors such as those associated with the Visible Infrared Imaging Radiometer Suite (VIIRS) on Suomi NPOESS Preparation Project (S-NPP) and NOAA-20. Like MODIS algorithms, products from these sensors require their own set of extensive error characterization and correction exercises. This is particularly true in the context of monitoring significant aerosol events that tax an algorithm's ability to separate cloud from aerosol and account for multiple scattering related errors exacerbated by uncertainties in aerosol optical properties. To investigate the performance of polar-orbiting satellite algorithms to monitor and characterize significant events, a level 3 (L3) product has been developed using a consistent aggregation methodology for 4 years of observations (2016–2019) that is referred to as the SSEC/NRL L3 product. Included in this product are the AErosol RObotic NETwork (AERONET), MODIS Dark Target, Deep Blue, and Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithms. These MODIS “baseline algorithms” are compared to NASA's recently released NASA Deep Blue algorithm for use with VIIRS. Using this new dataset, the relative performance of the algorithms for both land and ocean were investigated with a focus on the relative skill of detecting severe events and accuracy of the retrievals using AERONET. Maps of higher-percentile aerosol optical depth (AOD) regions of the world by product identified those with the highest measured AODs and determined what is high by local standards. While patterns in AOD match across products and median to moderate AOD values match well, there are regionally correlated biases between products based on sampling, algorithm differences, and AOD range – in particular for higher AOD events. Most notable are differences in boreal biomass burning and Saharan dust. Significant percentile biases must be accounted for when data are used in trend studies, data assimilation, or inverse modeling. These biases vary by aerosol regime and are likely due to retrieval assumptions in lower boundary conditions and aerosol optical models.

Long-term variability in immersion-mode marine ice-nucleating particles from climate model simulations and observations

Abstract. Ice-nucleating particles (INPs) in the Southern Ocean (SO) atmosphere have significant impacts on cloud radiative and microphysical properties. Yet, INP prediction skill in climate models remains poorly understood, in part because of the lack of long-term measurements. Here we show, for the first time, how model-simulated INP concentrations compare with year-round INP measurements during the Macquarie Island Cloud Radiation Experiment (MICRE) campaign from 2017–2018. We simulate immersion-mode INP concentrations using the Energy Exascale Earth System Model version 1 (E3SMv1) by combining simulated aerosols with recently developed deterministic INP parameterizations and the native classical nucleation theory (CNT) for mineral dust in E3SMv1. Because MICRE did not collect aerosol measurements of super-micron particles, which are more effective ice nucleators, we evaluate the model's aerosol fields at other high-latitude sites using long-term in situ observations of dust and sea spray aerosol. We find that the model underestimates dust and overestimates sea spray aerosol concentrations by 1 to 2 orders of magnitude for most of the high-latitude sites in the Southern Hemisphere. We next compare predicted INP concentrations with concentrations of INPs collected on filter samples (typically for 2 or 3 d) and processed offline using the Colorado State University ice spectrometer (IS) in immersion freezing mode. We find that when deterministic parameterizations for both dust and sea spray INPs are used, simulated INPs are within a factor of 10 of observed INPs more than 60 % of the time during summer. Our results also indicate that the E3SM's current treatment of mineral dust immersion freezing in the SO is impacted by compensating biases – an underprediction of dust amount was compensated by an overprediction of its effectiveness as INPs. We also perform idealized droplet freezing experiments to quantify the implications of the time-dependent behavior assumed by the E3SM's CNT-parameterization and compare with the ice spectrometer observations. We find that the E3SM CNT 10 s diagnostic used in this study is a reasonable approximation of the exact formulation of CNT, when applied to ice spectrometer measurements in low-INP conditions similar to Macquarie Island. However, the linearized 10 s diagnostic underestimates the exact formula by an order of magnitude or more in places with high-INP conditions like the Sahara. Overall, our findings suggest that it is important to correct the biases in E3SM's simulated dust life cycle and update E3SM's INP parameterizations. INP prediction errors of 2 to 3 orders of magnitude can have considerable impacts on the simulated cloud and radiative properties in global climate models. On comparing INP concentrations during MICRE against ship-based campaigns, Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS) and Antarctic Circumnavigation Expedition (ACE), we find that INPs from the latter are significantly higher only in regions closer to Macquarie Island. This alludes to the fact that physical, chemical and biological processes affecting INP concentrations as stimulated by the island could be partly responsible for the high INP concentrations observed at Macquarie Island during the MICRE campaign. Therefore, improvements to both aerosol simulation and INP parameterizations are required to adequately simulate INPs and their cloud impacts in E3SM. It will be helpful to include a parallel measurement of the size-resolved aerosol composition and explore opportunities for long-term measurement platforms in future field campaigns studying INP sources in remote marine regions.

The PACE-MAPP algorithm: Simultaneous aerosol and ocean polarimeter products using coupled atmosphere-ocean vector radiative transfer

We describe the PACE-MAPP algorithm that simultaneously retrieves aerosol and ocean optical parameters using multiangle and multispectral polarimeter measurements from the SPEXone, Hyper-Angular Rainbow Polarimeter 2 (HARP2), and Ocean Color Instrument (OCI) instruments onboard the NASA Plankton, Aerosol, Cloud, ocean Ecosystem (PACE) observing system. PACE-MAPP is adapted from the Research Scanning Polarimeter (RSP) Microphysical Aerosol Properties from Polarimetry (RSP-MAPP) algorithm. The PACE-MAPP algorithm uses a coupled vector radiative transfer model such that the atmosphere and ocean are always considered together as one system. Consequently, this physically consistent treatment of the system across the ultraviolet, (UV: 300–400 nm), visible (VIS: 400–700 nm), near-infrared (NIR: 700–1100 nm), and shortwave infrared (SWIR: 1100–2400 nm) spectral bands ensures that negative water-leaving radiances do not occur. PACE-MAPP uses optimal estimation to simultaneously characterize the optical and microphysical properties of the atmosphere’s aerosol and ocean constituents, find the optimal solution, and evaluate the uncertainties of each parameter. This coupled approach, together with multiangle, multispectral polarimeter measurements, enables retrievals of aerosol and water properties across the Earth’s oceans. The PACE-MAPP algorithm provides aerosol and ocean products for both the open ocean and coastal areas and is designed to be accurate, modular, and efficient by using fast neural networks that replace the time-consuming vector radiative transfer calculations in the forward model. We provide an overview of the PACE-MAPP framework and quantify its expected retrieval performance on simulated PACE-like data using a bimodal aerosol model for observations of fine-mode absorbing aerosols and coarse-mode sea salt particles. We also quantify its performance for observations over the ocean of dust-laden scenes using a trimodal aerosol model that incorporates non-spherical coarse-mode dust particles. Lastly, PACE-MAPP’s modular capabilities are described, and we discuss plans to implement a new ocean bio-optical model that uses a mixture of coated and uncoated particles, as well as a thin cirrus model for detecting and correcting for sub-visual ice clouds.

Using particle-resolved aerosol model simulations to guide the interpretations of cloud condensation nuclei experimental data

Ambient aerosol particles can undergo dynamic mixing processes as they coagulate with particles from other air masses and emission sources. Therefore, aerosols exist in a spectrum, from externally mixed to internally mixed. The mixing state of aerosols can affect their ability to uptake water (hygroscopicity) and their cloud condensation nuclei (CCN) activity, modifying their contribution to the planet’s total radiative budget. However, current water-uptake measurement methods may not be able to capture the complex mixing state. In this research, the dynamic mixing process was simulated by the particle-resolved aerosol model PartMC and also created by experiments in a laminar flow mixing tube. The mixing evolution of ammonium sulfate and sucrose binary mixtures were observed along with the changes in their water uptake properties expressed as the single hygroscopicity parameter, κ. The use of a mixing simulation in conjunction with experiments allow for better identification of the particle mixing state and the particle water uptake and show that no one kappa value can capture the complexity of mixing across the mixed particle size distribution. In other words, the PartMC simulations can be used as a guiding tool to interpret a system’s mixing state based on its experimental droplet activation spectra. This work demonstrates the importance of the integration and use of mixing models to aid in mixing state determination and hygroscopicity measurements of mixed systems.Copyright © 2023 American Association for Aerosol Research

Improvement and validation of aerosol models for natural deposition mechanism in reactor containment

Nuclear safety is the lifeline for the development and application of nuclear energy. In severe accidents of pressurized water reactor (PWR), aerosols, as the main carrier of fission products, are suspended in the containment vessel, posing a potential threat of radioactive contamination caused by leakage into the environment. The gas-phase aerosols suspended in the containment will settle onto the wall or sump water through the natural deposition mechanism, thereby reducing atmospheric radioactivity. Aiming at the low accuracy of the aerosol model in the ISAA code, this paper improves the natural deposition model of aerosol in the containment. The aerosol dynamic shape factor was introduced to correct the natural deposition rate of non-spherical aerosols. Moreover, the gravity, Brownian diffusion, thermophoresis and diffusiophoresis deposition models were improved. In addition, ABCOVE, AHMED and LACE experiments were selected to validate and evaluate the improved ISAA code. According to the calculation results, the improved model can more accurately simulate the peak aerosol mass and respond to the influence of the containment pressure and temperature on the natural deposition rate of aerosols. At the same time, it can significantly improve the calculation accuracy of the residual mass of aerosols in the containment. The performance of improved ISAA can meet the requirements for analyzing the natural deposition behavior of aerosol in containment of advanced PWRs in severe accident. In the future, further optimization will be made to address the problems found in the current aerosol model.

Multi-Box Modelling of Cooking-Generated Aerosols within an Urban Street Canyon

Multi-box models describing the evolution of cooking-generated aerosols emitted inside an urban street canyon are developed. By contrast with previous box models of urban pollutants, multiple boxes are introduced by partitioning the canyon space into dynamically distinct boxes. Aerosol dynamical processes, namely coagulation and deposition, are represented through standard parameterisations; the exchange or ventilation timescale between boxes is specified by the mean residence time, which is obtained from a Lagrangian particle model. Comparison with predictions from a large-eddy simulation model with a coupled sectional aerosol model indicates improved agreement when nine boxes are used in place of a single box; for example, the relative error in the canyon-averaged number concentration for deep-frying emissions decreases from ∼30% to ∼5%. The improvement is smaller for boiling emissions, which contain fewer small particles. The inclusion of extra boxes eliminates the need for explicit segregation corrections and enables the size spectrum and coarse-grained spatial structure of the aerosol number concentration to be captured.

Lunar eclipses illuminate timing and climate impact of medieval volcanism

Explosive volcanism is a key contributor to climate variability on interannual to centennial timescales1. Understanding the far-field societal impacts of eruption-forced climatic changes requires firm event chronologies and reliable estimates of both the burden and altitude (that is, tropospheric versus stratospheric) of volcanic sulfate aerosol2,3. However, despite progress in ice-core dating, uncertainties remain in these key factors4. This particularly hinders investigation of the role of large, temporally clustered eruptions during the High Medieval Period (HMP, 1100–1300 ce), which have been implicated in the transition from the warm Medieval Climate Anomaly to the Little Ice Age5. Here we shed new light on explosive volcanism during the HMP, drawing on analysis of contemporary reports of total lunar eclipses, from which we derive a time series of stratospheric turbidity. By combining this new record with aerosol model simulations and tree-ring-based climate proxies, we refine the estimated dates of five notable eruptions and associate each with stratospheric aerosol veils. Five further eruptions, including one responsible for high sulfur deposition over Greenland circa 1182 ce, affected only the troposphere and had muted climatic consequences. Our findings offer support for further investigation of the decadal-scale to centennial-scale climate response to volcanic eruptions.

Modelling the European wind-blown dust emissions and their impact on particulate matter (PM) concentrations

Abstract. Wind-blown dust (WBD) emitted by the Earth’s surface due to sandblasting can potentially have important effects on both climate and human health via interaction with solar and thermal radiation, reducing air quality. Apart from the main dust “centres” around the world, like deserts, dust can be emitted from partly vegetated mid- and high-latitude areas like Europe if certain conditions are suitable (strong winds, bare soil, reduced soil moisture, etc.). Using a wind-blown dust model (WBDUST) along with a chemical transport model (Comprehensive Air-quality model with Extensions, CAMx) coupled to a regional climate model (Weather Research and Forecasting, WRF), this study is one of the first to provide a model-based estimate of such emissions over Europe as well as the long-term impact of WBD emissions on the total particulate matter (PM) concentrations for the 2007–2016 period. We estimated average WBD emissions of about 0.5 and 1.5 Mgyr-1km-2 in fine and coarse modes. Maximum emissions occur over Germany, where the average seasonal fine- and coarse-mode emission flux can reach 0.5 and 1 gs-1km-2, respectively. Large variability is seen in the averaged daily emissions with values of up to 2 gs-1km-2 for the coarse-mode aerosol on selected days. The WBD emissions increased the modelled winter PM2.5 and PM10 concentrations by up to 10 and 20 µg m−3, respectively, especially over Germany, where the highest emissions occur. The impact on other seasons is lower. Much higher impacts are modelled, however, on selected days when occasionally the urban PM2.5 and PM10 concentrations are increased by more than 50 and 100 µg m−3. The comparison with measurements revealed that if WBD is considered, the summer biases are reduced; however, the winter PM is overestimated even more greatly (so the bias increases). We identified a strong overestimation of the modelled wind speed (the maximum daily wind is almost 2 times higher in WRF than the measured ones) suggesting that WBD emissions are also overestimated – hence the enhanced winter PM biases. Moreover, we investigated the secondary impacts of the crustal composition of fine WBD particles on secondary inorganic aerosol (SIA): sulfates (PSO4), nitrates (PNO3) and ammonium (PNH4). Because the water pH value, and thus the uptake of the gaseous precursors of SIA, is perturbed and because the increased aerosol surface serves as an oxidation site, we modelled seasonal PSO4 and PNO3 concentrations increased by up to 0.1 µg m−3 and PNH4 ones decreased by up to −0.05 µg m−3, especially during winter. In terms of average daily impact, these numbers can, however, reach much larger values of up to 1–2 µg m−3 for sulfates and nitrates, while the decrease in ammonium due to WBD can reach −1 µg m−3 on selected days. The sensitivity test on the choice of the inorganic equilibrium model (ISORROPIA vs. EQuilibrium Simplified Aerosol Model V4, EQSAM) showed that if EQSAM is used, the impact on SIA is slightly stronger (by a few 10 %) due to larger number of cations considered for water pH in EQSAM. Our results have to be regarded as a first estimate of the long-term WBD emissions and the related effects on PM over Europe. Due to the strong positive wind bias and hence strong WBD emissions, we should consider these results as an upper bound. More sensitivity studies involving the impact of the driving meteorological fields, WBD model choice and the input data used to describe the land surface need to be carried out in future to better constrain these emissions.

Marine aerosols in coastal areas and their impact on cave drip water – A monitoring study from Northern Spain

Marine aerosols affect coastal environments and human infrastructure, hence assessing the marine aerosol deposition in coastal areas is important. Field observations of marine aerosol deposition in coastal regions is commonly limited to a single station at high temporal resolution, which does not provide strong constraints on the spatial changes in the rate of aerosol delivery over the first 10 km distance from the coast, a gradient with the potential to constrain scavenging terms in aerosol models. Here, we provide data of monthly marine aerosol deposition (wet and dry) within the first 10 km from the coast during a 15-month monitoring study. Along a transect, a strong decrease of marine aerosols (Na, Mg, S and K) in the first 3 km from the coast but little decrease between 3 and 10 km is found. Based on fluxes of Na, the most conservative component measured and most completely attributed to marine aerosol sources, overall dry aerosol deposition decreases by nearly 20 to 30-fold from the coast to the station 10 km inland. Wet and dry marine aerosol deposition is significantly increased during the windy season (October until March), which is also the season of higher precipitation. The wind effect on aerosol deposition was greatest at the coast and diminished inland: between October and November 2019, the 3-fold increase in cumulative wind speed above the whitecap threshold caused a nearly 10-fold increase in the most proximal site, a 4-fold increase in 3.2 km sites, but only a 2-fold increase in dry aerosol deposition in the most distal sites. Independent of the season, the aerosol deposition rate >3 km from the coast drops to less than 20% of the most coast proximal station. Comparison of elemental ratios with seawater composition confirms the marine origin of Na and Mg in aerosols, but indicates additional sources and sinks for other elements (S and K) which do not correspond with expected marine sources. Furthermore, we test the time-integrated aerosol deposition in shallow groundwaters intercepted as cave drip waters from 13 caves, which confirm the decreasing contribution with distance from the coast but also reveal additional effects on the natural capture of wet and dry aerosols such as wind shielding effects and vegetation cover. The Na/Mg ratio of drip waters can be used to assess the significance of marine aerosols vs. bedrock to cave waters in the present day.

Evaluation of MODIS combined DT and DB AOD retrievals and their association with meteorological variables over Qena, Egypt

The purpose of this study is to validate the daily Terra-MODIS level 2 combined dark target (DT) and deep blue (DB) aerosol optical depth (AOD) retrievals with a spatial resolution of 10 km against the ground-based AERONET AOD data to be used in evaluating the air pollution and impact of meteorological variables over Qena, Egypt, in 2019. The regression analysis demonstrated an accepted agreement between the MODIS and AERONET AOD data with a correlation coefficient (R) of 0.7118 and 74.22% of the collocated points fall within the expected error (EE) limits. Quality flag filtering and spatial and temporal collocation were found to have a significant impact on the regression results. Quality flag filtering increased R by 0.2091 and % within EE by 17.97, spatial collocation increased R by 0.0143 and % within EE by 1.13, and temporal collocation increased R by 0.0089 and % within EE by 4.43. By validating the MODIS AOD data seasonally and analyzing the temporal distribution of the seasonal AOD data to show the retrieval accuracy variations between seasons, it was found that the MODIS AOD observations overestimated the AERONET AOD values in all seasons, and this may be because of underestimating the surface reflectance. Perhaps the main reason for the highest overestimation in summer and autumn is the transportation of aerosols from other regions, which changes the aerosol model in Qena, making accurate aerosol-type assumptions more difficult. Therefore, this study recommends necessary improvements regarding the aerosol model selection and the surface reflectance calculations. Temperature and relative humidity were found to have a strong negative relationship with a correlation of − 0.735, and both have a moderate association with AOD with a correlation of 0.451 and − 0.356, respectively. Because Qena is not a rainy city, precipitation was found to have no correlation with the other variables.

SCIATRAN software package (V4.6): update and further development of aerosol, clouds, surface reflectance databases and models

Abstract. Since the initiation of development at the Institute of Environmental Physics (IUP), University of Bremen, in 1994, the radiative transfer model SCIATRAN (formerly GOMETRAN) has been continuously improved and new versions have been released (Rozanov et al., 1997, 2002, 2005, 2014, 2017). In the course of development, the SCIATRAN software package became capable of simulating radiative transfer processes through the Earth's atmosphere or coupled atmosphere–ocean system with a variety of approaches to treat the sphericity of the atmosphere (plane-parallel, pseudo-spherical, approximately spherical and full-spherical solutions) in both scalar and vector modes. Supported by a variety of built-in databases and parameterizations, these capabilities made SCIATRAN widely used for various remote-sensing applications related to the retrieval of atmospheric trace gases and characteristics of aerosols, clouds and surfaces. This paper presents an overview of the cloud, aerosol and surface (CAS) databases and models implemented in the SCIATRAN software package (V4.6) and provides some recommendations on their usage. The new implementations offer potential users a flexible interface to perform radiative transfer simulations: (1) accounting for multilayer liquid water, ice and mixed-phase clouds; (2) employing typical aerosol-type parameterizations (including vertical variability) used in the satellite and model communities as well as updated databases; (3) including various surface bidirectional reflectance distribution function (BRDF) and albedo models for land, vegetation, ocean, snow and melt ponds on sea ice. The most recent version of the radiative transfer model SCIATRAN is freely available at the website of the IUP, University of Bremen: http://www.iup.physik.uni-bremen.de/sciatran (last access: November 2022).

An improved method for retrieving aerosol optical depth over Ebinur Lake Basin from Gaofen-1

Lake Ebinur is the largest saltwater lake in Xinjiang. In recent years, the exposed dry lake bottom surface has become a remarkable source of salt and dust owing to the desiccation of the lake. Given the importance of the lake basin to human livelihoods, comprehensive monitoring of basin behavior is required. Remote sensing offers numerous novel approaches to monitoring the spatial and temporal distribution of aerosols. During this study, high spatial resolution aerosol optical depth (AOD) inversion at Lake Ebinur was still in the gap stage. The wide-field-of-view (WFV) data from four cameras on the GaoFen-1 (GF-1) satellite, launched by China in April 2013, offers high spatial and temporal resolution and excellent potential for AOD estimation. Owing to the shortwave infrared band (SWIR) deficiency and the complexity of surface reflectance, the coefficient of variation (CV) was proposed as a measure of surface reflectance to develop a surface reflectance database for land cover characteristics in the Ebinur Lake Basin. The significant improvements of the algorithm include (1) the design of an accurate and universal cloud detection algorithm through the blue and red bands. (2) The CV was used to assess the robustness of surface reflectance under long time series. After dividing the surface reflectance image pixels with low robustness, a reasonable value was assigned according to the surface reflectance variation characteristics of the image pixels. (3) Aerosol models were determined from the long-term measurements of the CIMEL solar photometer (CE318), and the validation of ground-based observations showed good correlation that WFV/GF-1 AOD was comparable to CE318 AOD (R = 0.705; root mean square error (RMSE) = 0.098; mean absolute error (MAE) = 0.078), and the smaller MAE and RMSE confirmed the feasibility of inversion of AOD by this method.

Indoor air aerosol modeling and evaluation based on simulation chamber experiments

High levels of particulate matter (PM) are observed in indoor environments and are of great concern to human health. INCA-Indoor is an indoor air quality (IAQ) model that is able to simulate more than 1200 gaseous species in several rooms of a building. The present study details the aerosol module of this model, which is implemented to simulate aerosol formation by the nucleation of gaseous species, the growth of particles by coagulation and condensation, their deposition on surfaces, and their exchanges with the outdoors and between rooms. To assess the performance of the new modeling system, the simulations are compared with measurements from atmosphere simulation chambers obtained from the EUROCHAMP-2020 database. Two different types of processes are studied: the growth of diesel soot in the AIDA chamber and secondary organic aerosol (SOA) formation and evolution following the ozonolysis of α-pinene in the EUPHORE chamber. INCA-Indoor nicely reproduces the evolution of the number of diesel soot particles, their size distribution during growth by coagulation, and their deposition surfaces. The model also nicely reproduces the formation of aerosols from the ozonolysis of α-pinene, the competitive growth processes, condensation and coagulation, and aerosol deposition. The simulations confirm previous experimental findings and associated assumptions regarding aerosol formation by ozonolysis.

The Low‐Altitude Ionosphere of the Ice Giant Planets

AbstractThe study of atmospheric electricity of the lower stratosphere and upper troposphere of the ice giant planets can help to understand several physical phenomena such as cloud formation, lightning generation, aerosols growth, or chemical composition. At these depths, galactic radiation is the main energy source able to ionize the atmospheric constituents and to produce a low altitude ionospheric layer that can be similar in magnitude to the upper ionosphere produced by solar radiation and auroral electrons. The presence of aerosols affects the ion‐neutral chemistry by capturing electrons and ions depending on the aerosol size and number density. Here, we present a new one dimensional ionospheric model of Uranus and Neptune able to calculate the number densities of electrons and ions as well as the charging of aerosols between 100 Pa and 4 × 105 Pa. Since the results depends upon the amount and size of the atmospheric aerosols, as well as on the flux of the incoming cosmic radiation, several aerosol models, solar‐cycle conditions, and the effect of the intrinsic magnetic field are considered.

Difference between global and regional aerosol model classifications and associated implications for spaceborne aerosol optical depth retrieval

AbstractAerosol model are generally adopted to describe the physical and optical characteristics of aerosols in different regions, and this is important for climate and environmental studies as well as satellite aerosol retrieval. However, current mainstream aerosol retrieval algorithms still lack differentiated and dynamic descriptions of aerosol models, and the aerosol optical depth (AOD) retrieval accuracy is hence largely compromised. Therefore, in this study, we aimed to investigate the difference between global and regional aerosol model classifications and the impact of these differences on satellite AOD retrieval. We developed global and regional (for China) aerosol models through the K-means cluster analysis method, and used the 6SV radiative transfer model based on these global and regional aerosol models to simulate air pollution events. The cluster analysis revealed that both global and regional aerosols can be clustered into five main aerosol types with different optical and physical parameters. The aerosol types include strongly absorbing, moderately absorbing, weakly absorbing, dust and coarse-fine mixed aerosols. These two aerosol models exhibited distinct seasonal variations. Comparing the clustering results obtained with the two models at five Aerosol Robotic Network (AERONET) sites, we found that the proportion of strongly absorbing aerosols in the global results is low. According to the China clustering results, a higher proportion of strongly absorbing aerosols occurred in autumn, winter, and early spring, and dust aerosols attained an increasing proportion in spring. Comparing the aerosol parameters with observational data, the regional aerosol model performed better than the global aerosol model. Simulations of AOD during a pollution episode and in different seasons at the Beijing-CAMS site with the 6SV radiative transfer model further confirmed that the regional aerosol model achieved a better simulation accuracy than the global model. The findings suggest that regional aerosol models can provide a useful reference for satellite remote sensing algorithm, climate change and air pollution assessment, and that the dynamic description of the aerosol model is a key parameter in satellite AOD retrieval algorithms.

Single-scattering properties of ellipsoidal dust aerosols constrained by measured dust shape distributions

Abstract. Most global aerosol models approximate dust as spherical particles, whereas most remote sensing retrieval algorithms approximate dust as spheroidal particles with a shape distribution that conflicts with measurements. These inconsistent and inaccurate shape assumptions generate biases in dust single-scattering properties. Here, we obtain dust single-scattering properties by approximating dust as triaxial ellipsoidal particles with observationally constrained shape distributions. We find that, relative to the ellipsoidal dust optics obtained here, the spherical dust optics used in most aerosol models underestimate dust single-scattering albedo, mass extinction efficiency, and asymmetry parameter for almost all dust sizes in both the shortwave and longwave spectra. We further find that the ellipsoidal dust optics are in substantially better agreement with observations of the scattering matrix and linear depolarization ratio than the spheroidal dust optics used in most retrieval algorithms. However, relative to observations, the ellipsoidal dust optics overestimate the lidar ratio by underestimating the backscattering intensity by a factor of ∼2. This occurs largely because the computational method used to simulate ellipsoidal dust optics (i.e., the improved geometric optics method) underestimates the backscattering intensity by a factor of ∼2 relative to other computational methods (e.g., the physical geometric optics method). We conclude that the ellipsoidal dust optics with observationally constrained shape distributions can help improve global aerosol models and possibly remote sensing retrieval algorithms that do not use the backscattering signal.

A high-precision aerosol retrieval algorithm for FY-3D MERSI-II images

The Medium Resolution Spectral Imager-II (MERSI-II) onboard the recently launched Chinese Fengyun-3D (FY-3D) satellite has great capability in detecting global aerosols as it includes aerosol bands similar to Moderate Resolution Imaging Spectroradiometer (MODIS). However, to date, aerosol retrieval based on MERSI-II is still limited to dark target regions and there is no official aerosol products for the MERSI-II. This study focuses on developing a high-precision algorithm to retrieve aerosol optical depth (AOD) suitable for entire land areas (except snow/ice and inland waters) based on MERSI-II measurements. Considering both the accuracy and retrieval efficiency, a new cost function is constructed based on (1) the fact that the AOD (550 nm) retrieved independently from different bands should be the same with the correct aerosol model, and (2) the assumption that the aerosol types are the same in the 5 × 5 km spatial range. The retrieval method based on the new cost function is nearly 50 times faster than most current methods using iterative calculations. To extend the application adaption of the FY-3D MERSI-II AOD retrieval and avoid the errors caused by the surface Lambertian hypothesis, a bidirectional reflectance distribution function (BRDF) database is built using MODIS products. Eight candidate aerosol models in different natural zones of China are constructed based on AERONET aerosol products from 2010 − 2021. The new method is applied to MERSI-II images over China and validated against ground-based measurements at 14 stations from 2020 to 2021. MODIS aerosol products from three operational algorithms are also used for comparison purposes. The results show that MERSI-II AOD retrievals agree well with the ground-based measurements with correlation coefficient (R), root mean square error (RMSE), and relative mean bias (RMB) of 0.913, 0.123, and 0.955, respectively. In addition, 72.19 % of AOD matchups fall within the expected error (EE) envelopes. The MERSI-II retrievals show higher accuracy than that of MODIS dark target (DT) and deep blue (DB) products and comparable accuracy of the MODIS Multi-Angle Implementation of Atmospheric Correction (MAIAC) product. MERSI-II AOD also shows higher stability in terms of spatial and temporal and better performance under heavy aerosol loading conditions than MODIS products. A good AOD agreement with R from 0.777 to 0.863 between MERSI-II and MODIS products is found over the land of China. The new method showing high retrieval efficiency and accuracy has great potential to be operationally applied on AOD retrieval for MERSI-II.

Parametric MELCOR 2.2 sensitivity and uncertainty study with a focus on aerosols based on Phébus test FPT1

The Phébus test FPT-1 was carried out to investigate the fission product release, transportation, and distribution in the reactor coolant system and the simulated containment during a severe accident. The test was divided into three phases: the core degradation, aerosol transport, and containment phenomena. In this work, a parametric sensitivity and uncertainty analysis of the two first phases, i.e., core degradation and aerosol transport, is conducted with the focus on aerosol parameters.The study was done in a frame of WP4 of the European MUSA project whose main objective is to develop a methodology for severe accident uncertainty analysis.Due to the wide scope of the MUSA project, this study focuses not only on the UQ analysis but also on the parametric dependency and data interpretation. The main subject was investigating the uncertainty of the MELCOR 2.2 aerosol models and the relation between the chosen parameters as well as evaluating the usability of essential analytical tools available for such analyses.The calculations were carried out using the integral severe accident code MELCOR2.2 and the generic input deck of the FPT-1 experiment. The uncertainty quantification tool DAKOTA was used as a statistical tool. It was coupled with MELCOR within the SNAP environment.Fifteen uncertain parameters related with the aerosol release and transport were investigated. Two figures of merit were chosen to be the amount of deposition of Cs in the reactor coolant circuit, and the mass of air-borne aerosol in the containment. Preliminary analysis showed a significant correlation between the aerosol dynamic and agglomeration shape factors, density and minimum aerosol diameter with both FOMs. In addition to the standard uncertainty analysis, five MELCOR/DAKOTA UQ sensitivity calculations with modified parameters were performed and analyzed. Additionally, the impact of the parameters was investigated by excluding the most correlated ones from the analysis. The results confirm the strong correlation of shape factors and the importance of their ranges for overall UQ results.The authors show that by coupling the chosen analytical tools together, it is possible to carry out uncertainty quantification of severe accident analysis.Based on the study performed, the authors underline the need for further investigation of parameter distributions, the effect of the chosen number of samples on the results, and a global time-dependent UQ analysis.

Rapid membrane surface functionalization with Ag nanoparticles via coupling electrospray and polymeric solvent bonding for enhanced antifouling and catalytic performance: Deposition and interfacial reaction mechanisms

Electrospray is an effective, fast, and potentially scalable approach for membrane surface functionalization using various engineered nanomaterials (ENMs). However, the lack of fundamental understandings of the deposition process hinders the controlled deposition, efficient utilization, and long-term stabilization of the ENMs, and thus the practical applications of the nanocomposite membranes. To bridge this critical knowledge gap, advanced online characterization techniques (laser diffraction size measurement and laser doppler velocimetry) coupled with mathematical aerosol modeling are utilized to understand the three key process parameters: droplet size, deposition velocity, and evaporation rate. After deposition, polymeric solvent bonding (i.e., interdiffusion and subsequent entanglement of polymers) was found to substantially stabilize the deposited Ag NPs. We further provide a comprehensive description of such interfacial reaction mechanisms. Our results show a consistency between theoretical predication and measurement of the droplet size or deposition velocity, whereas realistic droplet evaporation rate is lower than the theoretical value due to the addition of the polymer. Successful stabilization of Ag NPs via interfacial polymeric bonding occurs under the conditions of large material contact area, high material compatibility, proper temperature (e.g., 22 °C), and polymer-to-solvent ratio (e.g., 3–5%). Our coupled approach achieves superior Ag NP coverage with high stability within minutes. Despite some reduction in water permeance, the resultant membrane shows markedly improved catalytic and antimicrobial (antibiofouling) performance (>90% enhancement) and maintained rejection. Taken together, our findings provide fundamental insights into the coupled process of electrospray deposition and polymeric solvent bonding to enable additive manufacturing of novel nanocomposite membranes with diverse structures and multiple functions.