Search Results (183)

During the South Asian Summer Monsoon (SASM), intense large-scale uplift and strong deep convective activity over South Asia lead to the formation of a high aerosol concentration zone in the Upper Troposphere and Lower Stratosphere (UTLS), known as the Asian Troposphere Aerosol Layer (ATAL), which appears from June to August. ATAL not only influences the exchange processes of material and energy between the troposphere and stratosphere, but also affects the global climate by altering radiation, cloud formation, and precipitation processes. Therefore, examining the spatiotemporal distribution and climate impacts of ATAL is essential for understanding climate change and evaluating the feasibility of geoengineering. This study systematically reviews research progress on the three-dimensional spatiotemporal distribution, trends, sources, and climatic effects of ATAL. Findings reveal a prominent aerosol layer at the top of the Asian troposphere, and the SASM region potentially serving as a critical conduit for constituents of the boundary layer to reach the stratosphere. However, simulated ATAL components differ significantly across models, particularly in terms of vertical distribution patterns. The precise three-dimensional structure and long-term evolution of ATAL remain unclear, presenting challenges for assessing its climate impact. To advance the understanding of the roles of ATAL in climate change, three future research directions are proposed. Full article

Numerical simulation studies of the dispersion of dimethyl sulfide (DMS) in the air have increased over the last two decades in parallel with the interest in understanding its role as a precursor of non-sea salt aerosols in the lower to middle levels of the troposphere. Here, we review recent numerical modeling studies that have included DMS emissions, their atmospheric oxidation mechanism, and their subsequent impacts on air quality at regional and global scales. In addition, we discuss the available methods for estimating sea–air DMS fluxes, including parameterizations and climatological datasets, as well as their integration into air quality models. At the regional level, modeling studies focus on the Northern Hemisphere, presenting a large gap in Antarctica, Africa, and the Atlantic coast of South America, whereas at the global scale, modeling studies tend to focus more on polar regions, especially the Arctic. Future studies must consider updated climatologies and parameterizations for more realistic results and the reduction in biases in numerical simulations analysis. Full article

Pollutants information can be retrieved from visible (VIS) and ultraviolet (UV) diffuse solar spectra exploiting Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) instruments. In May 2021, the Italian research institute CNR-ISAC acquired and deployed a MAX-DOAS system SkySpec-2D. It is located in the “Giorgio Fea” observatory in San Pietro Capofiume (SPC), in the middle of the Po Valley, where it has constantly acquired zenith and off-axis diffuse solar spectra since the 1st October 2021. This work presents the retrieved tropospheric NO₂ and aerosol extinction profiles (and their columns) derived from the MAX-DOAS measurements using the newly developed DEAP retrieval code. The code has been validated both using synthetic differential Slant Column Densities (dSCDs) from the Fiducial Reference Measurements for Ground-Based DOAS Air-Quality Observations (FRM4DOAS) project and real measured data. For this purpose, DEAP results are compared with the ones obtained with three state-of-the-art retrieval codes. In addition, an inter-comparison with satellite products from Sentinel-5P TROPOMI, for the tropospheric NO₂ Vertical Column Densities (VCDs), and MODIS-MAIAC for the tropospheric Aerosol Optical Depth (AOD), is performed. We find a bias of −0.6 × 10¹⁵ molec/cm² with a standard deviation of 1.8 × 10¹⁵ molec/cm² with respect to Sentinel-5P TROPOMI for NO₂ tropospheric VCDs and of 0.04 ± 0.08 for AOD with respect to MODIS-MAIAC data. The retrieved data show that the SPC measurement site is representative of the background pollution conditions of the Po Valley. For this reason, it is a good candidate for satellite validation and scientific studies over the Po Valley. Full article

Tropospheric aerosols play an important role in the notable warming phenomenon and climate change occurring in the Arctic. The accuracy of Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) aerosol optical depth (AOD) and the distribution of Arctic AOD based on the CALIOP Level 2 aerosol products and the Aerosol Robotic Network (AERONET) AOD data during 2006–2021 were analyzed. The distributions, trends, and three-dimensional (3D) structures of the frequency of occurrences (FoOs) of different aerosol subtypes during 2006–2021 are also discussed. We found that the CALIOP AOD exhibited a high level of agreement with AERONET AOD, with a correlation coefficient of approximately 0.67 and an RMSE of less than 0.1. However, CALIOP usually underestimated AOD over the Arctic, especially in wet conditions during the late spring and early summer. Moreover, the Arctic AOD was typically higher in winter than in autumn, summer, and spring. Specifically, polluted dust (PD), dust, and clean marine (CM) were the dominant aerosol types in spring, autumn, and winter, while in summer, ES (elevated smoke) from frequent wildfires reached the highest FoOs. There were increasing trends in the FoOs of CM and dust, with decreasing trends in the FoOs of PD, PC (polluted continental), and DM (dusty marine) due to Arctic amplification. In general, the vertical distribution patterns of different aerosol types showed little seasonal variation, but their horizontal distribution patterns at various altitudes varied by season. Furthermore, locally sourced aerosols such as dust in Greenland, PD in eastern Siberia, and ES in middle Siberia can spread to surrounding areas and accumulate further north, affecting a broader region in the Arctic. Full article

Isoprene emissions can affect the oxidizing capacity of the atmosphere and are likely to increase with an increase in the world’s biomass. The emission of isoprene is strongest in tropical forested regions, suggesting a major portion of tropospheric chemistry occurs in the tropics. As well as deforestation and reforestation having a direct impact on the world’s climate through land cover, there is also an indirect environmental impact (e.g., global warming, air pollution) through the resulting change in isoprene emissions. Previously, incomplete understanding of isoprene oxidation chemistry caused a model-measurement breakdown for concentrations of HO_x radicals observed over certain low-NO_x regions, such as the pristine Amazon rainforest. Over the last decade, however, understanding of isoprene oxidation chemistry has been vastly improved. Numerous research studies have provided evidence for the involvement of 1,6-H and 1,5-H shift reactions in the isoprene oxidation mechanism, which increases the level of HO_x recycling that occurs. As well as helping to reduce the model-measurement breakdown observed, the updated isoprene oxidation mechanism affects the tropospheric burdens of other species, including carbon monoxide (CO), methane (CH₄), ozone (O₃), organic peroxides (ROOH), secondary organic aerosol (SOA), and organic nitrates (RONO₂). There are still gaps in the understanding of the impacts and oxidation chemistry of isoprene emissions, which this literature review identifies and discusses. In the future, there is still much scope for further research, including modeling future reforestation scenarios with isoprene emissions and their impacts on both global and regional scales. Full article

Thermally driven local-scale precipitation (LSP) is an important type of summer precipitation over China, but the prestorm environmental conditions remain unclear. In order to investigate the major factors controlling the LSP intensity, the meteorological parameters preceding the occurrence of light and heavy afternoon LSP over Eastern China during 2018–2022 are examined using rain gauge, radiosonde sounding, and satellite observations. The temperature differences between heavy and light LSP events are relatively small, but heavy LSP events exhibit larger water vapor mixing ratios (Q_v) below a 5 km altitude than light LSP. With an almost identical vertical temperature distribution, an increment in Q_v increases the relative humidity (RH) in the lower troposphere. Furthermore, large eddy simulations with spectral bin microphysics are performed to investigate the impacts of humidity and aerosols on the LSP intensity. Increased low-level RH leads to larger mass concentrations of rain and graupel at the expense of cloud droplets due to enhanced drop collisions and the riming of ice particles, respectively, thereby reinforcing the LSP. However, an increased aerosol concentration leads to more cloud water but reduced rain water content, resulting mainly from suppressed drop collisions. The graupel mixing ratio exhibits a non-monotonic trend with aerosols, mostly contributed by riming. As a result, the LSP intensity first increases and then decreases with an increment in the aerosol concentration in both dry and humid air. Moreover, more aerosols lead to the humidification of the surrounding air due to the enhanced evaporation of cloud droplets, particularly under lower-RH conditions. These findings provide an enhanced understanding of the effects of covariations in humidity and aerosol concentrations on the afternoon LSP intensity over Eastern China. Full article

Black carbon (BC) aerosols emitted from biomass, fossil fuel, and waste combustion contribute to the radiation budget imbalance and are transported over extensive distances in the Earth’s atmosphere. These aerosols undergo physical and chemical modifications with co-existing aerosols (e.g., nitrate, sulfate, ammonium) through aging processes during long-range transport and are primarily removed from the troposphere by wet deposition. Using precipitation samples collected in North America between 26 October and 1 December 2020 by the National Atmospheric Deposition Program (NADP), we investigated the relationships between BC and both water-soluble ions and water-soluble organic carbon (WSOC) using Spearman’s rank coefficients. We then attempted to identify the sources of BC in the wet deposition using factor analysis (FA) and satellite data of fire smoke. BC showed a very strong correlation with nitrate (ρ = 0.83). Strong correlations were also found with WSOC, ammonium, calcium, and sulfate ions (ρ = 0.78, 0.74, 0.74, and 0.67, respectively). FA showed that BC was in the same factor as nitrate, ammonium, sulfate, and WSOC, indicating that BC could originate from secondary aerosol formation and biomass burning. Supported by satellite data of fire and smoke, BC and other correlated pollutants were believed to be associated with wildfire outbreaks in several states in the United States (US) during November 2020. Full article

We present a multi-year study of Saharan dust intrusions on a mountainous site located in the central Mediterranean Basin regarding their aerosol optical and geometrical properties. The observations were carried out at the Consiglio Nazionale delle Ricerche-Istituto di Metodologie per l’Analisi Ambientale (CNR-IMAA) located in Potenza (40,360N, 15,440E), Italy, from March 2010 to October 2022, using ACTRIS (Aerosol Clouds and Trace Gases Research InfraStructure). A total of 101 night-time lidar measurements of dust intrusions were identified. The following properties were calculated for the periods December, January, February (DJF), March, April, May (MAM), June, July, August (JJA) and September, October, November (SON): aerosol layer center of mass altitude, particle lidar ratio at 355 and 532 nm, particle depolarization ratio at 532 nm and backscattering Ångström exponent at 532–1064 nm. Both geometrical and optical aerosol properties vary considerably with the seasons. During SON and DJF, air masses transporting dust travel at lower altitudes, and become contaminated with local continental particles. In MAM and JJA, dust is also likely to travel at higher altitudes and rarely mix with other aerosol types. As a result, aerosols are larger in size and irregular in shape during the warm months. The ratio of the lidar ratios at 355 and 532 nm is 1.11 ± 0.15 in DJF, 1.12 ± 0.07 in SON, 0.94 ± 0.12 in MAM, and 0.92 ± 0.08 in JJA. The seasonal radiative effect estimated using the Fu–Liou–Gu (FLG) radiative transfer model indicates the most significant impact during the JJA period. A negative dust radiative effect is observed both at the surface (SRF) and at the top of the atmosphere (TOA) in all the seasons, and this could be related to a minimal contribution from black carbon. Specifically, the SRF radiative effect estimation is −14.48 ± 1.32 W/m² in DJF, −18.00 ± 0.89 W/m² in MAM, −22.08 ± 1.36 W/m² in JJA, and −13.47 ± 1.12 W/m² in SON. Instead, radiative effect estimation at the TOA is −22.23 ± 2.06 W/m² in DJF, −38.23 ± 2.16 W/m² in MAM, −51.36 ± 3.53 W/m² in JJA, and −22.57 ± 2.11 W/m² in SON. The results highlight how the radiative effects of the particles depend on the complex relationship between the dust load, their altitude in the troposphere, and their optical properties. Accordingly, the knowledge of aerosols optical property profiles is of primary importance to understand the radiative impact of dust. Full article

Water vapor is an active trace component in the troposphere and has a significant impact on meteorology and the atmospheric environment. In order to meet demands for high-precision water vapor and aerosol observations for numerical weather prediction (NWP), the China Meteorological Administration (CMA) deployed 49 Raman aerosol lidar systems and established the first Raman–Mie scattering lidar network in China (CARLNET) for routine measurements. In this paper, we focus on the water vapor measurement capabilities of the CARLNET. The uncertainty of the water vapor Raman channel calibration coefficient (Cw) is determined using an error propagation formula. The theoretical relationship between the uncertainty of the calibration coefficient and the water vapor mixing ratio (WVMR) is constructed based on least squares fitting. Based on the distribution of lidar in regions with different humidity conditions, the method of real-time calibration and quality control based on radiosonde data is established for the first time. Based on the uncertainty requirements of the World Meteorological Organization for water vapor in data assimilation, the calibration and quality control thresholds of the WVMR in regions with different humidity conditions are determined by fitting real-time lidar and radiosonde data. Lastly, based on the radiosonde results, the calibration algorithm established in this study is used to calibrate CARLNET data from October to December 2023. Compared with traditional calibration results, the results show that the stability and detection accuracy of the CARLNET significantly improved after calibration in regions with different humidity conditions. The deviation of the Cw decreased from 12.84~18.47% to 5.41~11.54%. The inversion error of the WVMR compared to radiosonde decreased from 1.05~0.46 g/kg to 0.82~0.34 g/kg. The reliability of the improved calibration algorithm and the CARLNET’s performance have been verified, enabling them to provide high-precision water vapor products for NWP. Full article

Aerosol vertical stratification significantly influences the Earth’s radiative balance and particulate-matter-related air quality. Continuous vertically resolved observations remain scarce compared to surface-level and column-integrated measurements. This work presents and makes available a novel, long-term (2016–2022) aerosol dataset derived from continuous (24/7) vertical profile observations from three selected stations (Aosta, Rome, Messina) of the Italian Automated Lidar-Ceilometer (ALC) Network (ALICENET). Using original retrieval methodologies, we derive over 600,000 quality-assured profiles of aerosol properties at the 15 min temporal and 15 metre vertical resolutions. These properties include the particulate matter mass concentration (PM), aerosol extinction and optical depth (AOD), i.e., air quality legislated quantities or essential climate variables. Through original ALICENET algorithms, we also derive long-term aerosol vertical layering data, including the mixed aerosol layer (MAL) and elevated aerosol layers (EALs) heights. Based on this new dataset, we obtain an unprecedented, fine spatiotemporal characterisation of the aerosol vertical distributions in Italy across different geographical settings (Alpine, urban, and coastal) and temporal scales (from sub-hourly to seasonal). Our analysis reveals distinct aerosol daily and annual cycles within the mixed layer and above, reflecting the interplay between site-specific environmental conditions and atmospheric circulations in the Mediterranean region. In the lower troposphere, mixing processes efficiently dilute particles in the major urban area of Rome, while mesoscale circulations act either as removal mechanisms (reducing the PM by up to 35% in Rome) or transport pathways (increasing the loads by up to 50% in Aosta). The MAL exhibits pronounced diurnal variability, reaching maximum (summer) heights of >2 km in Rome, while remaining below 1.4 km and 1 km in the Alpine and coastal sites, respectively. The vertical build-up of the AOD shows marked latitudinal and seasonal variability, with 80% (30%) of the total AOD residing in the first 500 m in Aosta-winter (Messina-summer). The seasonal frequency of the EALs reached 40% of the time (Messina-summer), mainly in the 1.5–4.0 km altitude range. An average (wet) PM > 40 μg m⁻³ is associated with the EALs over Rome and Messina. Notably, 10–40% of the EAL-affected days were also associated with increased PM within the MAL, suggesting the entrainment of the EALs in the mixing layer and thus their impact on the surface air quality. We also integrated ALC observations with relevant, state-of-the-art model reanalysis datasets (ERA5 and CAMS) to support our understanding of the aerosol patterns, related sources, and transport dynamics. This further allowed measurement vs. model intercomparisons and relevant examination of discrepancies. A good agreement (within 10–35%) was found between the ALICENET MAL and the ERA5 boundary layer height. The CAMS PM₁₀ values at the surface level well matched relevant in situ observations, while a statistically significant negative bias of 5–15 μg m⁻³ in the first 2–3 km altitude was found with respect to the ALC PM profiles across all the sites and seasons. Full article

To suppress the influence of aerosols scattering on the double-edge detection technique and achieve high-accuracy measurement of the wind field throughout the troposphere to the lower stratosphere, an ultraviolet 355 nm Rayleigh–Brillouin Doppler lidar technology based on a dual-pass dual Fabry–Perot interferometer (FPI) is proposed. The wind speed detection principle of this technology is analyzed, and the formulas for radial wind speed measurement error caused by random noise and wind speed measurement bias caused by Mie scattering signal contamination are derived. Based on the detection principle, the structure of the lidar system is designed. Combining the wind speed measurement error and measurement bias on both sides, the parameters of the dual-pass dual-FPI are optimized. The free spectral range (FSR) of the dual-pass dual-FPI is selected as 12 GHz, the bandwidth as 1.8 GHz, and the peak-to-peak spacing as 6 GHz. Further, the detection performance of this new type of Rayleigh–Brillouin Doppler lidar with the designed system parameters is simulated and analyzed. The simulation results show that at an altitude of 0–20 km, within the radial wind speed dynamic range of ±50 m/s, the radial wind speed measurement bias caused by aerosol scattering signal is less than 0.17 m/s in the cloudless region; within the radial wind speed dynamic range of ±30 m/s, the bias is less than 0.44 m/s and 0.91 m/s in the simulated cumulus cloud at 4 km where aerosol backscatter ratio R_β = 3.8 and cirrus cloud at 9 km where R_β = 2.9, respectively; using a laser with a pulse energy of 350 mJ and a repetition frequency of 50 Hz, a 450 mm aperture telescope, setting the detection zenith angle of 30°, vertical resolution of 26 m@0–10 km, 78 m@10–20 km, and 260 m@20–30 km, and a time resolution of 1 min, with the daytime sky background brightness taking 0.3 WSr⁻¹m⁻²nm⁻¹@355 nm, the radial wind speed measurement errors of the system during the day and night are below 2.9 m/s and 1.6 m/s, respectively, up to 30 km altitude, below 0.28 m/s at 10 km altitude, and below 0.91 m/s at 20 km altitude all day. Full article

Understanding baseline O₃ is important as it defines the fraction of O₃ coming from global sources and not subject to local control. We report the occurrence and sources of high baseline ozone days, defined as a day where the daily maximum 8 h average (MDA8) exceeds 70 ppb, as observed at the Mount Bachelor Observatory (MBO, 2.8 km asl) in Central Oregon from 2004 to 2022. We used various indicators and enhancement ratios to categorize each high-O₃ day: carbon monoxide (CO), aerosol scattering, the water vapor mixing ratio (WV), the aerosol scattering-to-CO ratio, backward trajectories, and the NOAA Hazard Mapping System Fire and Smoke maps. Using these, we identified four causes of high-O₃ days at the MBO: Upper Troposphere/Lower Stratosphere intrusions (UTLS), Asian long-range transport (ALRT), a mixed UTLS/ALRT category, and events enhanced by wildfire emissions. Wildfire sources were further divided into two categories: smoke transported in the boundary layer to the MBO and smoke transported in the free troposphere from more distant fires. Over the 19-year period, 167 high-ozone days were identified, with an increasing fraction due to contributions from wildfire emissions and a decreasing fraction of ALRT events. We further evaluated trends in the O₃ and CO data distributions by season. For O₃, we found an overall increase in the mean and median values of 2.2 and 1.5 ppb, respectively, from the earliest part of the record (2004–2013) compared to the later part (2014–2022), but no significant linear trends in any season. For CO, we found a significant positive trend in the summer 95th percentiles, associated with increasing fires in the Western U.S., and a strong negative trend in the springtime values at all percentiles (1.6% yr⁻¹ for 50th percentile). This decline was likely associated with decreasing emissions from East Asia. Overall, our findings are consistent with the positive trend in wildfires in the Western United States and the efforts in Asia to decrease emissions. This work demonstrates the changing influence of these two source categories on global background O₃ and CO. Full article

This study analyses the wide-band algorithm, Cloud-J v.8.0, from the point of view of the validity of the choice of wide spectral intervals to accelerate the calculations of photolysis rates in the lower and middle atmosphere, considering the features of solar radiation propagation, and to assess the influence of the processes of reflection and scattering on molecules, aerosols, and clouds. The results show that the calculations performed using Cloud-J v.8.0 are in agreement with the data obtained using the high-resolution LibRadtran model. The study also considers the factors influencing the propagation of the solar flux through the atmosphere in Cloud-J v.8.0, which occurs following theoretical concepts. It is shown that the presence of cloud layers can increase photolysis rates by up to 40% in the above-cloud layer and decrease them by up to 20% below the cloud layer. The presence of volcanic aerosol can increase the photolysis rates in the upper part of the layer and above it by up to 75% and decrease them by up to 75% in the underlying atmosphere. Rayleigh scattering can both enhance photolysis rates in the troposphere and reduce them at large zenith angles. Thus, Cloud-J offers a robust method for modelling atmospheric photodissociation processes with high computational efficiency. Full article

Cosmogenic beryllium-10 and beryllium-7, and the ratio of the two (10Be/7Be), are powerful atmospheric tracers of stratosphere–troposphere exchange (STE) processes; however, measurements are sparse for altitudes well above the tropopause. We present a novel high-altitude balloon campaign aimed to measure these isotopes in the mid-stratosphere called Beryllium Isotopes for Resolving Dynamics in the Stratosphere (BIRDIES). BIRDIES targeted gravity waves produced by tropopause-overshooting convection to study their propagation and impact on STE dynamics, including the production of turbulence in the stratosphere. Two custom-designed payloads called FiSH and GASP were flown at altitudes approaching 30 km to measure in situ turbulence and beryllium isotopes (on aerosols), respectively. These were flown on nine high-altitude balloon flights over Kansas, USA, in summer 2022. The atmospheric samples were augmented with a ground-based rainfall collection targeting isotopic signatures of deep convection overshooting. Our GASP samples yielded mostly negligible amounts of both 10Be and 7Be collected in the mid-stratosphere but led to design improvements to increase aerosol capture in low-pressure environments. Observations from FiSH and the precipitation collection were more fruitful. FiSH showed the presence of turbulent velocity, temperature, and acoustic fluctuations in the stratosphere, including length scales in the infra-sonic range and inertial subrange that indicated times of elevated turbulence. The precipitation collection, and subsequent statistical analysis, showed that large spatial datasets of 10Be/7Be can be measured in individual rainfall events with minimum terrestrial contamination. While the spatial patterns in rainfall suggested some evidence for overshooting convection, inter-event temporal variability was clearly observed and predicted with good agreement using the 3D chemical transport model GEOS-CHEM. Full article

This study aims to present the benefits of unmanned aircraft systems (UAS) in atmospheric aerosol research, specifically to obtain information on the vertical variability of aerosol single-scattering properties in the lower troposphere. The results discussed in this paper were obtained during the Polish Radar and Lidar Mobile Observation System (POLIMOS) field campaign in 2018 at a wetland and rural site located in the Rzecin (Poland). UAS was equipped with miniaturised devices (low-cost aerosol optical counter, aethalometer AE-51, RS41 radiosonde) to measure aerosol properties (scattering and absorption coefficient) and air thermodynamic parameters. Typical UAS vertical profiles were conducted up to approximately 1000 m agl. During nighttime, UAS measurements show a very shallow inversion surface layer up to about 100–200 m agl, with significant enhancement of aerosol scattering and absorption coefficient. In this case, the Pearson correlation coefficient between aerosol single-scattering properties measured by ground-based equipment and UAS devices significantly decreases with altitude. In such conditions, aerosol properties at 200 m agl are independent of the ground-based observation. On the contrary, the ground observations are better correlated with UAS measurements at higher altitudes during daytime and under well-mixed conditions. During long-range transport of biomass burning from fire in North America, the aerosol absorption coefficient increases with altitude, probably due to entrainment of such particles into the PBL. Full article