Tropospheric Aerosols Research Articles

On the рossibility of multichannel optical backscattering sondes for joint balloon and lidar studies of the aerosol composition of the middle atmosphere

Aerosol backscattering sondes in the practice of aerological sounding, along with lidar observations, are used at night to study and monitor polar stratospheric clouds, tropospheric and stratospheric aerosol, cirrus clouds, pyroconvection, volcanic aerosol, as well as to verify remote methods and means of ground-based and satellite-based aerosol observations. For aerosol sondes, a simple two-wave measurement technique is used, which makes it possible to diagnose changes in aerosol composition by color index. The possibilities of the two-wave technique have limitations, which are discussed in this article. Aerological sounding combined with lidar observations expands the wavelength range for multi-wavelength studies, and direct measurements of atmospheric temperature increase the accuracy of aerosol sensing. The paper considers the application of 3 or more wavelenght techniques. Data from probe measurements using wavelengths of 470, 528, 850 and 940 nm and lidar sensing at wavelengths of 355 and 532 nm are presented.

Influence of columnar versus vertical distribution of aerosol properties on the modulation of shortwave radiative effects

Quantifying the interaction of atmospheric aerosols with incoming solar radiation remains a challenge owing to the limitations associated with measuring aerosol optical properties. This study investigates how the distribution of aerosol properties, whether columnar or vertical, affects the aerosol radiative forcing (ARF) and heating rates (HRs) across different atmospheric layers under cloud-free conditions in the shortwave region. We also assess the atmospheric parameters, namely, pressure, temperature, water vapour density, and ozone density, from in-situ measurements, reanalysis data, and a standard tropical atmosphere to understand their impact on ARF and HR estimates across seasons. Our findings show that aerosol absorption is highest during monsoon, while it is lowest in the winter. Significant atmospheric warming due to aerosols resulted from the substantial cooling at the surface. Columnar properties of aerosols measured at limited or multiple wavelengths yield similar ARF and HR estimates, provided spectral dependency is considered using the Angstrom exponent across seasons. However, the vertical profiles of aerosol extinction, together with a constant single scattering albedo (SSA) along the atmospheric column versus an actual SSA profile, led to notable differences in ARF and HRs, specifically in pre-monsoon and monsoon periods. Free tropospheric aerosol absorption is underestimated when using columnar properties compared to vertical distribution, while boundary layer absorption is overestimated (> 10 Wm-2). The heterogeneity in aerosol types across atmospheric layers significantly influenced aerosol absorption, highlighting the importance of accurate vertical distribution information. HR profiles obtained with vertical distribution reflect the structure of aerosol extinction, whereas those estimated with columnar properties result in smoother profiles that fail to capture altitude gradients. Aerosol-induced HRs are higher within the boundary layer and free troposphere in the monsoon season for all scenarios of defined aerosol properties. These findings underscore the need for actual vertical profile measurements of aerosol properties to quantify aerosol radiation interaction.

Lidar–radar synergistic method to retrieve ice, supercooled water and mixed-phase cloud properties

Abstract. Mixed-phase clouds are not well represented in climate and weather forecasting models, due to a lack of the key processes controlling their life cycle. Developing methods to study these clouds is therefore essential, despite the complexity of mixed-phase cloud processes and the difficulty of observing two cloud phases simultaneously. We propose in this paper a new method to retrieve the microphysical properties of mixed-phase clouds, ice clouds and supercooled water clouds using airborne or satellite radar and lidar measurements, called VarPy-mix. This new approach extends an existing variational method developed for ice cloud retrieval using lidar, radar and passive radiometers. We assume that the lidar attenuated backscatter β at 532 nm is more sensitive to particle concentration and is consequently mainly sensitive to the presence of supercooled water. In addition, radar reflectivity Z at 95 GHz is sensitive to the size of hydrometeors and hence more sensitive to the presence of ice particles. Consequently, in the mixed phase the supercooled droplets are retrieved with the lidar signal and the ice particles with the radar signal, meaning that the retrievals rely strongly on a priori and error values. This method retrieves simultaneously the visible extinction for ice αice and liquid αliq particles, the ice and liquid water contents IWC and LWC, the effective radius of ice re,ice and liquid re,liq particles, and the ice and liquid number concentrations Nice and Nliq. Moreover, total extinction αtot, total water content (TWC) and total number concentration Ntot can also be estimated. As the retrieval of ice and liquid is different, it is necessary to correctly identify each phase of the cloud. To this end, a cloud-phase classification is used as input to the algorithm and has been adapted for mixed-phase retrieval. The data used in this study are from DARDAR-MASK v2.23 products, based on the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and Cloud Profiling Radar (CPR) observations from the CALIPSO and CloudSat satellites, respectively, belonging to the A-Train constellation launched in 2006. Airborne in situ measurements performed on 7 April 2007 during the Arctic Study of Tropospheric Aerosol, Clouds and Radiation (ASTAR) campaign and collected under the track of CloudSat–CALIPSO are compared with the retrievals of the new algorithm to validate its performance. Visible extinctions, water contents, effective radii and number concentrations derived from in situ measurements and the retrievals showed similar trends and are globally in good agreement. The mean percent error between the retrievals and in situ measurements is 39 % for αliq, 398 % for αice, 49 % for LWC and 75 % for IWC. It is also important to note that temporal and spatial collocations are not perfect, with a maximum spatial shift of 1.68 km and a maximum temporal shift of about 10 min between the two platforms. In addition, the sensitivity of remote sensing and that of in situ measurements is not the same, and in situ measurement uncertainties are between 25 % and 60 %.

High-accuracy measurement of 36SF5 + signal using an ultrahigh-resolution isotope ratio mass spectrometer.

The Δ36S standard deviation measured in a conventional isotope ratio mass spectrometer such as MAT 253 is ca 0.1‰ to 0.3‰. At this precision, it is difficult to resolve the origin of non-mass-dependent sulfur isotope fractionation in tropospheric sulfate aerosol and in Martian meteorites or small deviations from the canonical mass-dependent fractionation laws. Interfering ions with m/z at 131 of 36SF5 + are suggested by the community as the cause of the poor precision, but the exact ion species has not been identified or confirmed. Here we examined the potential interfering ions by using a Thermo Scientific ultrahigh-resolution isotope ratio mass spectrometer to measure SF6 working gas and SF6 gases converted from IAEA-S1/2/3 Ag2S reference materials. We found that there are two resolvable peaks to the right of the 36SF5 + peak when a new filament was installed, which are 186WF4 2+ followed by 12C3F5 +. However, only the 12C3F5 + interference peak was observed after more than three days of filament use. 12C3F5 + is generated inside the instrument during the ionization process. Avoiding the interfering signals, we were able to achieve a Δ36S standard deviation of 0.046‰ (n = 8) for SF6 zero-enrichment and 0.069‰ (n = 8) for overall measurement start from silver sulfide IAEA-S1. Aging the filament with SF6 gas can avoid the interference of 186WF4 2+. Minimizing the presence of carbon-bearing compounds and avoiding the interfering signals of 12C3F5 + from 36SF5 +, we can improve Δ36S measurement accuracy and precision, which helps to open new territories for research using quadruple sulfur isotope composition.

Hydrogen peroxide serves as pivotal fountainhead for aerosol aqueous sulfate formation from a global perspective

Traditional atmospheric chemistry posits that sulfur dioxide (SO2) can be oxidized to sulfate (SO42–) through aqueous-phase reactions in clouds and gas-phase oxidation. Despite adequate knowledge of traditional mechanisms, several studies have highlighted the potential for SO2 oxidation within aerosol water. Given the widespread presence of tropospheric aerosols, SO42− production through aqueous-phase oxidation in aerosol water could have a pervasive global impact. Here, we quantify the potential contributions of aerosol aqueous pathways to global sulfate formation based on the GEOS-Chem simulations and subsequent theoretical calculations. Hydrogen peroxide (H2O2) oxidation significantly influences continental regions both horizontally and vertically. Over the past two decades, shifts in the formation pathways within typical cities reveal an intriguing trend: despite reductions in SO2 emissions, the increased atmospheric oxidation capacities, like rising H2O2 levels, prevent a steady decline in SO42− concentrations. Abating oxidants would facilitate the benefit of SO2 reduction and the positive feedback in sulfate mitigation.

The Recovery and Re-Calibration of a 13-Month Aerosol Extinction Profiles Dataset from Searchlight Observations from New Mexico, after the 1963 Agung Eruption

The recovery and re-calibration of a dataset of vertical aerosol extinction profiles of the 1963/64 stratospheric aerosol layer measured by a searchlight at 32° N in New Mexico, US, is reported. The recovered dataset consists of 105 aerosol extinction profiles at 550 nm that cover the period from December 1963 to December 1964. It is a unique record of the portion of the aerosol cloud from the March 1963 Agung volcanic eruption that was transported into the Northern Hemisphere subtropics. The data-recovery methodology involved re-digitizing the 105 original aerosol extinction profiles from individual Figures within a research report, followed by the re-calibration. It involves inverting the original equation used to compute the aerosol extinction profile to retrieve the corresponding normalized detector response profile. The re-calibration of the original aerosol extinction profiles used Rayleigh extinction profiles calculated from local soundings. Rayleigh and aerosol slant transmission corrections are applied using the MODTRAN code in transmission mode. Also, a best-estimate aerosol phase function was calculated from observations and applied to the entire column. The tropospheric aerosol phase function from an AERONET station in the vicinity of the searchlight location was applied between 2.76 to 11.7 km. The stratospheric phase function, applied for a 12.2 to 35.2 km altitude range, is calculated from particle-size distributions measured by a high-altitude aircraft in the vicinity of the searchlight in early 1964. The original error estimate was updated considering unaccounted errors. Both the re-calibrated aerosol extinction profiles and the re-calibrated stratospheric aerosol optical depth magnitudes showed higher magnitudes than the original aerosol extinction profiles and the original stratospheric aerosol optical depth, respectively. However, the magnitudes of the re-calibrated variables show a reasonable agreement with other contemporary observations. The re-calibrated stratospheric aerosol optical depth demonstrated its consistency with the tropics-to-pole decreasing trend, associated with the major volcanic eruption stratospheric aerosol pattern when compared to the time-coincident stratospheric aerosol optical depth lidar observations at Lexington at 42° N.

Assessing Lidar Ratio Impact on CALIPSO Retrievals Utilized for the Estimation of Aerosol SW Radiative Effects across North Africa, the Middle East, and Europe

North Africa, the Middle East, and Europe (NAMEE domain) host a variety of suspended particles characterized by different optical and microphysical properties. In the current study, we investigate the importance of the lidar ratio (LR) on Cloud-Aerosol Lidar with Orthogonal Polarization–Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIOP-CALIPSO) aerosol retrievals towards assessing aerosols’ impact on the Earth-atmosphere radiation budget. A holistic approach has been adopted involving collocated Aerosol Robotic Network (AERONET) observations, Radiative Transfer Model (RTM) simulations, as well as reference radiation measurements acquired using spaceborne (Clouds and the Earth’s Radiant Energy System-CERES) and ground-based (Baseline Surface Radiation Network-BSRN) instruments. We are assessing the clear-sky shortwave (SW) direct radiative effects (DREs) on 550 atmospheric scenes, identified within the 2007–2020 period, in which the primary tropospheric aerosol species (dust, marine, polluted continental/smoke, elevated smoke, and clean continental) are probed using CALIPSO. RTM runs have been performed relying on CALIOP retrievals in which the default and the DeLiAn (Depolarization ratio, Lidar ratio, and Ångström exponent)-based aerosol-speciated LRs are considered. The simulated fields from both configurations are compared against those produced when AERONET AODs are applied. Overall, the DeLiAn LRs leads to better results mainly when mineral particles are either solely recorded or coexist with other aerosol species (e.g., sea-salt). In quantitative terms, the errors in DREs are reduced by ~26–27% at the surface (from 5.3 to 3.9 W/m2) and within the atmosphere (from −3.3 to −2.4 W/m2). The improvements become more significant (reaching up to ~35%) for moderate-to-high aerosol loads (AOD ≥ 0.2).

The investigation of retrieval method for aerosol and water vapor profiles based on MAX-DOAS technology

Simultaneously obtaining the vertical distribution and profile of aerosol and water vapor is crucial for in-depth understanding of the Earth's radiation balance, regional water cycle, and the causes of frequent haze weather in China. This study developed a system and inversion method based on multi-axis differential optical absorption spectroscopy (MAX-DOAS) to simultaneously retrieve tropospheric aerosol and water vapor profiles. The absorption of dioxy (O4) was obtained by multi-elevation measurement using the developed ground-based MAX-DOAS system. By minimizing a cost function combining an atmospheric radiative transfer model, aerosol extinction profiles were first inverted, followed by water vapor profiles. Optimized parameter selection in the look-up table method reduced reliance on prior profile information, enhancing pollutant distribution retrieval accuracy. In the monitoring period in Huaibei region, aerosols were mainly below 1.5 km, while water vapor concentrations decreased with altitude. Comparisons of water vapor vertical column densities (VCDs) retrieved through the look-up table method with the European Centre for Medium-Range Weather Forecasts(ECMWF) ERA5 model and geometric approximation showed good agreement, with correlation coefficients of 0.93 and 0.98, respectively. To comprehend water vapor sources at various vertical layers, a 24-h backward trajectory clustering analysis was conducted using the HYSPLIT model based on observed wind fields. Findings revealed that at 500 m altitude, water vapor primarily emanated from the southeast, whereas at 1 km and 2 km altitudes, it predominantly originated from the southwest. The study advances simultaneous tropospheric aerosol and water vapor profile retrieval, providing reliable technical support for the investigation of regional pollution.

Above-cloud concentrations of cloud condensation nuclei help to sustain some Arctic low-level clouds

Abstract. Previous studies have found that low-level Arctic clouds often persist for long periods even in the face of very low surface cloud condensation nuclei (CCN) concentrations. Here, we investigate whether these conditions could occur due to continuous entrainment of aerosol particles from the free troposphere (FT). We use an idealized large eddy simulation (LES) modeling framework, where aerosol concentrations are low in the boundary layer (BL) but increased up to 50× in the free troposphere. We find that the tests with higher tropospheric aerosol concentrations simulated clouds, which persisted for longer and maintained higher liquid water paths (LWPs). This is due to direct entrainment of the tropospheric aerosol into the cloud layer, which results in a precipitation suppression from the increase in cloud droplet number and in stronger cloud-top radiative cooling, which causes stronger circulations maintaining the cloud in the absence of surface forcing. Together, these two responses result in a more well-mixed boundary layer with a top that remains in contact with the tropospheric aerosol reservoir and can maintain entrainment of those aerosol particles. The surface aerosol concentrations, however, remained low in all simulations. The free-tropospheric aerosol concentration necessary to maintain the clouds is consistent with concentrations that are frequently seen in observations.

The Tibetan Plateau space-based tropospheric aerosol climatology: 2007–2020

Abstract. A comprehensive and robust dataset of tropospheric aerosol properties is important for understanding the effects of aerosol–radiation feedback on the climate system and reducing the uncertainties of climate models. The “Third Pole” of Earth (Tibetan Plateau, TP) is highly challenging for obtaining long-term in situ aerosol data due to its harsh environmental conditions. Here, we provide the more reliable new vertical aerosol index (AI) parameter from the spaceborne-based lidar CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) on board CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) for daytime and nighttime to investigate the aerosol's climatology over the TP region during 2007–2020. The calculated vertical AI was derived from the aerosol extinction coefficient (EC), which was rigorously quality-checked and validated for passive satellite sensors (MODIS) and ground-based lidar measurements. Generally, our results demonstrated that there was agreement of the AI dataset with the CALIOP and ground-based lidar. In addition, the results showed that, after removing the low-reliability aerosol target signal, the optimized data can obtain the aerosol characteristics with higher reliability. The data also reveal the patterns and concentrations of high-altitude vertical structure characteristics of the tropospheric aerosol over the TP. They will also help to update and make up the observational aerosol data in the TP. We encourage climate modelling groups to consider new analyses of the AI vertical patterns, comparing the more accurate datasets, with the potential to increase our understanding of the aerosol–cloud interaction (ACI) and aerosol–radiation interaction (ARI) and their climate effects. Data described in this work are available at https://doi.org/10.11888/Atmos.tpdc.300614 (Huang, 2023).

Tropical tropospheric aerosol sources and chemical composition observed at high altitude in the Bolivian Andes

Abstract. The chemical composition of PM10 and non-overlapping PM2.5 was studied at the summit of Mt. Chacaltaya (5380 m a.s.l., lat. −16.346950°, long. −68.128250°) providing a unique long-term record spanning from December 2011 to March 2020. The chemical composition of aerosol at the Chacaltaya Global Atmosphere Watch (GAW) site is representative of the regional background, seasonally affected by biomass burning practices and by nearby anthropogenic emissions from the metropolitan area of La Paz–El Alto. Concentration levels are clearly influenced by seasons with minima occurring during the wet season (December to March) and maxima occurring during the dry and transition seasons (April to November). Ions, total carbon (EC + OC), and saccharide interquartile ranges for concentrations are 558–1785, 384–1120, and 4.3–25.5 ng m−3 for bulk PM10 and 917–2308, 519–1175, and 3.9–24.1 ng m−3 for PM2.5, respectively, with most of the aerosol seemingly present in the PM2.5 fraction. Such concentrations are overall lower compared to other high-altitude stations around the globe but higher than Amazonian remote sites (except for OC). For PM10, there is dominance of insoluble mineral matter (33 %–56 % of the mass), organic matter (7 %–34 %), and secondary inorganic aerosol (15 %–26 %). Chemical composition profiles were identified for different origins: EC, NO3-, NH4+, glucose, and C2O42- for the nearby urban and rural areas; OC, EC, NO3-, K+, acetate, formate, levoglucosan, and some F− and Br− for biomass burning; MeSO3-, Na+, Mg2+, K+, and Ca2+ for aged marine emissions from the Pacific Ocean; arabitol, mannitol, and glucose for biogenic emissions; Na+, Ca2+, Mg2+, and K+ for soil dust; and SO42-, F−, and some Cl− for volcanism. Regional biomass burning practices influence the soluble fraction of the aerosol between June and November. The organic fraction is present all year round and has both anthropogenic (biomass burning and other combustion sources) and natural (primary and secondary biogenic emissions) origins, with the OC/EC mass ratio being practically constant all year round (10.5 ± 5.7, IQR 8.1–13.3). Peruvian volcanism has dominated the SO42- concentration since 2014, though it presents strong temporal variability due to the intermittence of the sources and seasonal changes in the transport patterns. These measurements represent some of the first long-term observations of aerosol chemical composition at a continental high-altitude site in the tropical Southern Hemisphere.

A Regional Aerosol Model for the Middle Urals Based on CALIPSO Measurements

The present work aims to develop a regional Middle Urals Aerosol model (MUrA model) based on the joint analysis of long-term ground-based photometric measurements of the Aerosol Robotic NETwork (AERONET) and the results of lidar measurements of the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) satellite relying on information on the air trajectories at different altitudes calculated using the HYSPLIT (Hybrid Single Particle Lagrangian Integrated Trajectory model) software package. The MUrA model contains parameters of normalized volume size distributions (NVSDs) characterizing the tropospheric aerosol subtypes detected by the CALIPSO satellite. When comparing the MUrA model with the global CALIPSO Aerosol Model (CAMel), we found significant differences in NVSDs for elevated smoke and clean continental aerosol types. NVSDs for dust and polluted continental/smoke aerosol types in the global and regional models differ much less. The total volumes of aerosol particles along the atmospheric column reconstructed from satellite measurements of the attenuation coefficient at a wavelength of 532 nm based on the regional MUrA model and global CAMel are compared with the AERONET inversion data. The mean bias error for the regional model is 0.016 μm3/μm2, and 0.043 μm3/μm2 for the global model.

Jupiter's Multi‐Year Cycles of Temperature and Aerosol Variability From Ground‐Based Mid‐Infrared Imaging

AbstractWe use a long‐term record of ground‐based mid‐infrared (7.9–24.5 μm) observations, captured between 1984 and late 2019 from 3‐m and 8‐m class observatories (mainly NASA's Infrared Telescope Facility, ESO's Very Large Telescope, and the Subaru Telescope), to characterize the long‐term, multi‐decade variability of the thermal and aerosol structure in Jupiter's atmosphere. In this study, spectral cubes assembled from images in multiple filters are inverted to provide estimations of stratospheric and tropospheric temperatures and tropospheric aerosol opacity. We find evidence of non‐seasonal and quasi‐seasonal variations of the stratospheric temperatures at 10 mbar, with a permanent hemispherical asymmetry at mid‐latitudes, where the northern mid‐latitudes are overall warmer than southern mid‐latitudes. A correlation analysis between stratospheric and tropospheric temperature variations reveals a moderate anticorrelation between the 10‐mbar and 330‐mbar temperatures at the equator, revealing that upper‐tropospheric equatorial temperatures are coupled to Jupiter’s Equatorial Stratospheric Oscillation. The North and South Equatorial Belts show temporal variability in their aerosol opacity and tropospheric temperatures that are in approximate antiphase with one another, with moderate negative correlations in the North Equatorial Belt and South Equatorial Belt changes between conjugate latitudes at 10°–16°. This long‐term anticorrelation between belts separated by ∼15° is still not understood. Finally we characterize the lag between thermal and aerosol opacity changes at a number of latitudes, finding that aerosol variations tend to lag after thermal variations by around 6 months at multiple latitudes.

Description and performance of a sectional aerosol microphysical model in the Community Earth System Model (CESM2)

Abstract. We implemented the Community Aerosol and Radiation Model for Atmospheres (CARMA) in both the high- and low-top model versions of the Community Earth System Model Version 2 (CESM2). CARMA is a sectional microphysical model, which we use for aerosol in both the troposphere and stratosphere. CARMA is fully coupled to chemistry, clouds, radiation, and transport routines in CESM2. This development enables the comparison of simulations with a sectional (CARMA) and a modal (MAM4) aerosol microphysical model in the same modeling framework. The new implementation of CARMA has been adopted from previous work, with some additions that align with the current CESM2 Modal Aerosol Model (MAM4) implementation. The main updates include an interactive secondary organic aerosol description in CARMA, using the volatility basis set (VBS) approach, updated wet removal, and the use of transient emissions of aerosols and trace gases. In addition, we implemented an alternative aerosol nucleation scheme in CARMA, which is also used in MAM4. Detailed comparisons of stratospheric aerosol properties after the Mount Pinatubo eruption reveal the importance of prescribing sulfur injections in a larger region rather than in a single column to better represent the observed evolution of aerosols. Both CARMA and MAM4 in CESM2 are able to represent stratospheric and tropospheric aerosol properties reasonably well when compared to observations. Several differences in the performance of the two aerosol models show, in general, an improved representation of aerosols when using the sectional aerosol model in CESM2. These include a better representation of the aerosol size distribution after the Mount Pinatubo volcanic eruption in CARMA compared to MAM4. MAM4 produces on average smaller aerosols and less removal than CARMA, which results in a larger total mass. Both CARMA and MAM4 reproduce the stratospheric aerosol optical depth (AOD) within the error bar of the observations between 2001 and 2020, except for recent larger volcanic eruptions that are overestimated by both model configurations. The CARMA background surface area density and aerosol size distribution in the stratosphere and troposphere compare well to observations, with some underestimation of the Aitken-mode size range. MAM4 shows shortcomings in reproducing coarse-mode aerosol distributions in the stratosphere and troposphere. This work outlines additional development needs for CESM2 CARMA to improve the model compared to observations in both the troposphere and stratosphere.

“Investigating and mapping day-night urban heat island and its driving factors using Sentinel/MODIS data and Google Earth Engine. Case study: Greater Cairo, Egypt”

Urban heat islands (UHI) represent one of the substantial human-induced challenges endangering urban livelihoods. UHI and climate change have significant interactions. Progressively rising warming tendencies are exacerbating higher temperatures in UHI regions. Using time-series data, we examined annual and seasonal day-night UHI intensity and its driving factors in Greater Cairo (GC), which is considered Egypt's megacity, between April 2021 and March 2022. Since Sentinel-1 synthetic aperture radar (SAR) proposes unique horizons for mapping urban areas, we used SAR data and the Random Forest (RF) algorithm for urban footprint extraction in the search region. Sentinel-3 SLSTR thermal images were utilized to derive annual and seasonal day-night land surface temperatures (LST) during the research period. A spatio-temporal assessment of tropospheric NO2, SO2, CO, and aerosol concentrations was performed via the Sentinel-5 Precursor TROPOspheric Monitoring Instrument (TROPOMI), MODIS, and Google Earth Engine (GEE) applications. The annual average UHI intensity was higher in Egypt's megacity during the nighttime (3.27 K) than during the daytime (0.50 K). This finding indicates that driving forces are boosting temperatures in urban regions at night. The seasonal average day-night UHI intensities have the highest values during the winter, followed by the summer. Significant influencing factors concerning UHI intensity varied between the daytime and nighttime. Moreover, NDBI, PV, NDVI, altitude, and wind speed were the driving factors that were influential during the day and at night. These results can be used to establish effective adaptation measures for combating the impacts of climatic change and UHI.

Temporal assessment of air quality in major cities in Nigeria using satellite data

This study evaluated the concentrations of tropospheric nitrogen dioxide (NO2), carbon monoxide (CO), ozone (O3), and Aerosol Index (AI) as well as different meteorological parameters, including atmospheric temperature (AT), relative humidity (RH), and wind speed (WS) in nine Nigerian cities: Aba, Benin, Ibadan, Kaduna, Kano, Lagos, Onitsha, Port Harcourt, and Umuahia. The role of socioeconomic activities on air pollution was also investigated using nighttime light radiance as a surrogate measure. Welch's one-way ANOVA test was performed for the variance study to evaluate the concentration dynamics of the selected tropospheric air pollutants and their association with nighttime light radiance. The mean concentration of CO and AI was highest in Kano, while that of O3 was the lowest. A similar pattern was also observed in the spatiotemporal transition of the selected pollutants and the nighttime light during the study period. Further, the correlation analysis revealed that AT is positively correlated with NO2 except in Aba and Benin cities, while it is positively correlated with CO and AI for all cities. The principal component analysis (PCA) revealed that O3 and RH have strong negative factor loadings, whereas CO, AI, and AT have strong positive factor loadings. This study will guide future researchers by associating the level of pollution with socioeconomic activities, especially during the absence of permanent air quality stations.

Annual cycle of aerosol properties over the central Arctic during MOSAiC 2019–2020 – light-extinction, CCN, and INP levels from the boundary layer to the tropopause

Abstract. The MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition was the largest Arctic field campaign ever conducted. MOSAiC offered the unique opportunity to monitor and characterize aerosols and clouds with high vertical resolution up to 30 km height at latitudes from 80 to 90∘ N over an entire year (October 2019 to September 2020). Without a clear knowledge of the complex aerosol layering, vertical structures, and dominant aerosol types and their impact on cloud formation, a full understanding of the meteorological processes in the Arctic, and thus advanced climate change research, is impossible. Widespread ground-based in situ observations in the Arctic are insufficient to provide these required aerosol and cloud data. In this article, a summary of our MOSAiC observations of tropospheric aerosol profiles with a state-of-the-art multiwavelength polarization Raman lidar aboard the icebreaker Polarstern is presented. Particle optical properties, i.e., light-extinction profiles and aerosol optical thickness (AOT), and estimates of cloud-relevant aerosol properties such as the number concentration of cloud condensation nuclei (CCN) and ice-nucleating particles (INPs) are discussed, separately for the lowest part of the troposphere (atmospheric boundary layer, ABL), within the lower free troposphere (around 2000 m height), and at the cirrus level close to the tropopause. In situ observations of the particle number concentration and INPs aboard Polarstern are included in the study. A strong decrease in the aerosol amount with height in winter and moderate vertical variations in summer were observed in terms of the particle extinction coefficient. The 532 nm light-extinction values dropped from >50 Mm−1 close to the surface to <5 Mm−1 at 4–6 km height in the winter months. Lofted, aged wildfire smoke layers caused a re-increase in the aerosol concentration towards the tropopause. In summer (June to August 2020), much lower particle extinction coefficients, frequently as low as 1–5 Mm−1, were observed in the ABL. Aerosol removal, controlled by in-cloud and below-cloud scavenging processes (widely suppressed in winter and very efficient in summer) in the lowermost 1–2 km of the atmosphere, seems to be the main reason for the strong differences between winter and summer aerosol conditions. A complete annual cycle of the AOT in the central Arctic could be measured. This is a valuable addition to the summertime observations with the sun photometers of the Arctic Aerosol Robotic Network (AERONET). In line with the pronounced annual cycle in the aerosol optical properties, typical CCN number concentrations (0.2 % supersaturation level) ranged from 50–500 cm−3 in winter to 10–100 cm−3 in summer in the ABL. In the lower free troposphere (at 2000 m), however, the CCN level was roughly constant throughout the year, with values mostly from 30 to 100 cm−3. A strong contrast between winter and summer was also given in terms of ABL INPs which control ice production in low-level clouds. While soil dust (from surrounding continents) is probably the main INP type during the autumn, winter, and spring months, local sea spray aerosol (with a biogenic aerosol component) seems to dominate the ice nucleation in the ABL during the summer months (June–August). The strong winter vs. summer contrast in the INP number concentration by roughly 2–3 orders of magnitude in the lower troposphere is, however, mainly caused by the strong cloud temperature contrast. A unique event of the MOSAiC expedition was the occurrence of a long-lasting wildfire smoke layer in the upper troposphere and lower stratosphere. Our observations suggest that the smoke particles frequently triggered cirrus formation close to the tropopause from October 2019 to May 2020.

Global Scale Inversions from MOPITT CO and MODIS AOD

Top-down observational constraints on emissions flux estimates from satellite observations of chemical composition are subject to biases and errors stemming from transport, chemistry and prior emissions estimates. In this context, we developed an ensemble data assimilation system to optimize the initial conditions for carbon monoxide (CO) and aerosols, while also quantifying the respective emission fluxes with a distinct attribution of anthropogenic and wildfire sources. We present the separate assimilation of CO profile v9 retrievals from the Measurements of Pollution in the Troposphere (MOPITT) instrument and Aerosol Optical Depth (AOD), collection 6.1, from the Moderate Resolution Imaging Spectroradiometer (MODIS) instruments. This assimilation system is built on the Data Assimilation Research Testbed (DART) and includes a meteorological ensemble to assimilate weather observations within the online Community Atmosphere Model with Chemistry (CAM-chem). Inversions indicate an underestimation of CO emissions in CAMS-GLOB-ANT_v5.1 in China for 2015 and an overestimation of CO emissions in the Fire INventory from NCAR (FINN) version 2.2, especially in the tropics. These emissions increments are consistent between the MODIS AOD and the MOPITT CO-based inversions. Additional simulations and comparison with in situ observations from the NASA Atmospheric Tomography Mission (ATom) show that biases in hydroxyl radical (OH) chemistry dominate the CO errors.

Surface tension of single suspended aerosol microdroplets

The surface tension of troposphere aerosols can significantly influence their atmospheric processes and key properties, particularly on the morphology, the phase transition, the activation as cloud condensation nuclei, and the gas-particle partitioning. However, directly measuring the surface tension of single ambient aerosol is quite challenging, due to the limitations of their picolitre volumes and thermal motion. Here, we developed a dual laser tweezers Raman spectroscopy (DLT-RS) system to directly sense the surface tension of single airborne microdroplets (PM10 particles). A pair of aerosol droplets were trapped and driven to coalesce by the laser tweezers. Meanwhile, the backscattering light intensity and bright-field images during the coalescence process were recorded to characterize the aerosol surface tension. A remarkable advantage of directly sensing aerosol surface tension is that the solutes in aerosols are often supersaturated, which is common in atmospheric aerosols but almost unavailable in bulk solutions. We experimentally measured the surface tension of aerosols composed of nitrates or oxalic acid/nitrate mixture. Besides, the variation of surface tension during aerosol aging process was also explored, which brings possible implications on the surface evolution of actual ambient aerosol during their atmospheric lifetime.

Comparison of the Performance of the GRASP and MERRA2 Models in Reproducing Tropospheric Aerosol Layers

Two approaches, based on Generalized Retrieval of Aerosol and Surface Properties (GRASP) and Modern-Era Retrospective Analysis for Research and Applications version 2 (MERRA-2) models, are investigated for reproducing aerosol layers in the troposphere. The GRASP algorithm is supplied with synergistic LIDAR and sunphotometer measurements to obtain aerosol extinction profiles. MERRA-2 is an atmospheric reanalysis coupling model that includes an external mixture of sea salt, dust, organic carbon, black carbon, and sulfate aerosols. A data set from Racibórz observatory, obtained with LIDAR and a sunphotometer in the 2017–2020 period, is analysed with GRASP along with the closest grid point data given by MERRA-2. The models demonstrate satisfactory agreement, yet some discrepancies were observed, indicating the presence of biases. For vertically integrated profiles, the correlation coefficient (R) between aerosol optical thickness was calculated to be 0.84, indicating a strong linear relationship. The Pearson correlation coefficient calculated between profiles for the selected altitude sectors varies between 0.428 and 0.824, indicating moderate to good agreement at all altitudes. GRASP shows denser aerosol layers in the mid-troposphere, while MERRA-2 gives higher aerosol extinctions throughout the high troposphere to low stratosphere region. Moreover, GRASP does not provide vertical variability in the extinction profile near the ground, due to a lack of data in the LIDAR’s incomplete overlap range. Lastly, the aerosol layer identification and type recognition are validated with statistical analysis of air mass backward trajectories with endpoints spatially and temporally collocated with individual identified layers. These reveal potential source regions that are located within areas known to be significant sources for the different identified aerosol types.