Changes In Aerosol Properties Research Articles

Changes in aerosol properties at the El Arenosillo site in Southern Europe as a result of the 2023 Canadian forest fires

From the beginning of May 2023 to the end of August 2023, the Northern Hemisphere experienced significant wildfire activity with the most widespread fires occurring in Canada. Forest fires in Canada destroyed more than 15.6 million hectares of forests. These wildfires worsened air quality across the region and other parts of the world. The smoke reached southern Europe by the end of June 2023. To better understand the consequences of such forest fires far from the site of origin, aerosol optical, microphysical and radiative properties were analyzed during this event for southern Europe using data from the Visible Infrared Imaging Radiometer Suite (VIIRS), TROPOspheric Monitoring Instrument (TROPOMI), and Aerosol Robotic Network (AERONET). TROPOMI aerosol index (AI) and the carbon monoxide (CO) product confirm that the smoke originated directly from these forest fires. AERONET data from the El Arenosillo site in southern Spain showed maximum aerosol optical depth (AOD) values on June 27 reached 2.36. Data on Angstrom Exponent (AE), aerosol volume size distribution (VSD), single scattering albedo (SSA), fine mode fraction (FMF), volume particle concentration, effective radius (REff), absorption AOD (AAOD), extinction AE (EAE) and absorption AE (AAE) showed that fine-mode particles with carbonaceous aerosols contribution predominated in the atmosphere above the El Arenosillo site. Direct aerosol radiative forcing (DARF) at the top (DARFTOA) and bottom of atmosphere (DARFBOA) were −103.1 and −198.93 Wm−2, respectively. The atmospheric aerosol radiative forcing (DARFATM) was found to be 95.83 Wm−2 and with a heating rate 2.69 K day−1, which indicates the resulting warming of the atmosphere.

Time series retrieval of Multi-wavelength Aerosol optical depth by adapting Transformer (TMAT) using Himawari-8 AHI data

Accurate aerosol optical depth (AOD) with high temporal resolution is required for dynamic monitoring changes of aerosol properties. The Himawari-8 Advanced Himawari imager (AHI) data with 10-min temporal resolution has been widely used for AOD retrieval but usually involves radiative transfer models and assumptions on surface reflection and aerosol properties that are hard to satisfy. This paper introduces a data-driven algorithm without any priori assumptions on surface or aerosol properties called Time series retrieval of Multi-wavelength AOD by adapting Transformer (TMAT). TMAT directly retrieves AOD at eight-wavelengths every 10-min throughout the day, using AHI top of atmosphere (TOA) reflectances in 6 wavebands and ancillary data. TMAT explores diurnal temporal change patterns of AOD and surface reflection using time series data. TMAT was trained and evaluated using samples derived by matching a year (2019) of AHI full-disk data and AERONET/SONET observations with 12,768 diurnal time series, each of which includes up to 81 10-min 6-band AHI TOA observations and 81 (time) × 8 (wavelength) AOD values per day. There are up to 273,413 (<12,768 × 81) TOA observations in 6 wavebands and up to 1,420,716 (<12,768 × 81 × 8) AOD values in all the time series samples, with filled values (−9999) to represent no data due to cloud contamination and incomplete wavelength configurations of AOD stations. The masking mechanism in Transformer is leveraged to exclude the contribution of the AHI filled values in time series AOD retrieval and exclude the contribution of AOD filled values in training. TMAT was trained with a physical constraint that the retrieved AOD decreases toward longer wavelengths. TMAT AOD was evaluated by separating training and validation samples using site-specific leave-one-station-out validation. TMAT AOD shows extremely high accuracy at all wavelengths, with RMSE = 0.101, R = 0.949 and 81.69% of retrievals within ±0.05+15%∗AODsites for the AOD at 550 nm. We also validated the accuracy of the NASA multiangle implementation of atmospheric correction (MAIAC) AHI AOD over these sites with RMSE = 0.186, R = 0.832 and 52.10% of retrievals within ±0.05+15%∗AODsites. The Ångström exponent (AE) derived from the multi-wavelength TMAT AOD also shows good agreement with AERONET/SONET AE, with a correlation coefficient of 0.620 and an RMSE of 0.291. The TMAT effectiveness to capture diurnal temporal change patterns of surface reflection and AOD was evidenced by the significant reduction of AOD accuracy when using a non-time series deep learning method. The effectiveness of multi-wavelength joint retrieval was evidenced by the significant reduction of AE accuracy when using single wavelength retrieval models. Evidence shows the training and evaluation split methods have a large impact on evaluation accuracy and this study further used ground network independent training and evaluation split to confirm the leave-one-station-out validation accuracy. Despite this, future study will focus on more spatially independent validation and more comprehensive comparison between the MAIAC and TMAT results.

Long-term analysis of AOD separated by aerosol type in East Asia

This study aimed to identify the temporal variations in aerosol loadings and sizes in East Asia based on a method that uses the linear particle depolarization ratio (δP) and coarse-mode fraction of volume concentration (CMFvc) from AERONET Sun/Sky radiometer data. East Asia is the polluted region. Pollution levels continue to increase as a result of population growth and increasing industrialization. The main pollution sources are derived from anthropogenic activities and Asian dust. The data were used to separate the total aerosol optical depths (τ) of mixed aerosol plumes into optical depths contributed by dust (τD), coarse- (τPC), and fine-mode pollution (τPF). We used data taken from 1999 to 2021 in East Asia (Beijing, Xianghe on the west, Seoul, Yonsei, Anmyon, and Gwangju in the middle, Osaka and Shirahama in the east, and Taipei in the south). We identified the regional differences; the contribution of τD and τPC to the total τ of Chinese sites was almost twice that of other East Asian sites. We analyzed the monthly, seasonal and annual values each of the three aerosol types contributed to total optical depth. The annual variations in τD and τPC from 1999 to 2021 showed a decreasing trend. In contrast, τPF either increased or became stagnant during that time. We conclude that aerosol types in East Asia may have changed. The Ångström exponent of fine-mode particles increased in most regions (0.0008–0.0103 yr−1 for the wavelength range 440–870 nm), which means the mean size of the fine-mode pollution particles tended to decrease, even though τPF increased. The change in particle size might be caused by the decrease in primary emission sources due to the strong air pollution reduction policies in China, Korea, and Japan. Therefore, we need to focus on the change in aerosol properties not just on aerosol loadings.

Spatiotemporal changes in aerosol properties by hygroscopic growth and impacts on radiative forcing and heating rates during DISCOVER-AQ 2011

Abstract. This work focuses on the characterization of vertically resolved aerosol hygroscopicity properties and their direct radiative effects through a unique combination of ground-based and airborne remote sensing measurements during the Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) 2011 field campaign in the Baltimore–Washington DC metropolitan area. To that end, we combined aerosol measurements from a multiwavelength Raman lidar located at NASA Goddard Space Flight Center and the airborne NASA Langley High Spectral Resolution Lidar-1 (HSRL-1) lidar system. In situ measurements aboard the P-3B airplane and ground-based Aerosol Robotic Network – Distributed Regional Aerosol Gridded Observational Network (AERONET-DRAGON) served to validate and complement quantifications of aerosol hygroscopicity from lidar measurements and also to extend the study both temporally and spatially. The focus here is on 22 and 29 July 2011, which were very humid days and characterized by a stable atmosphere and increasing relative humidity with height in the planetary boundary layer (PBL). Combined lidar and radiosonde (temperature and water vapor mixing ratio) measurements allowed the retrieval of the Hänel hygroscopic growth factor which agreed with that obtained from airborne in situ measurements and also explained the significant increase of extinction and backscattering with height. Airborne measurements also confirmed aerosol hygroscopicity throughout the entire day in the PBL and identified sulfates and water-soluble organic carbon as the main species of aerosol particles. The combined Raman and HSRL-1 measurements permitted the inversion for aerosol microphysical properties revealing an increase of particle radius with altitude consistent with hygroscopic growth. Aerosol hygroscopicity pattern served as a possible explanation of aerosol optical depth increases during the day, particularly for fine-mode particles. Lidar measurements were used as input to the libRadtran radiative transfer code to obtain vertically resolved aerosol radiative effects and heating rates under dry and humid conditions, and the results reveal that aerosol hygroscopicity is responsible for larger cooling effects in the shortwave range (7–10 W m−2 depending on aerosol load) near the ground, while heating rates produced a warming of 0.12 K d−1 near the top of PBL where aerosol hygroscopic growth was highest.

Long-term changes in aerosol radiative properties over Ny-Ålesund: Results from Indian scientific expeditions to the Arctic

Continuous long-term monitoring of black carbon (BC) mass concentration and aerosol light scattering coefficient (σSCA), supplemented by number size distribution and chemical composition, are utilized in this study to understand the temporal changes in aerosol properties, associated source processes and radiative effects at Ny-Ålesund (79 oN) in the Svalbard Archipelago. A statistically significant decreasing trend in BC (- 24.7 ng m−3 decade−1) is observed during spring of 2010–2019. In contrast, σSCA depicted a general increasing trend (5.2 Mm−1 decade−1) during 2011–2016. BC and σSCA were higher during winter and spring. Aerosol single scattering albedo was highest in May ~ 0.95 (during spring) and lowest in September ~ 0.87 (during summer). Fractional share of BC to total aerosol mass was higher in winter and summer. Anthropogenic SO42− and NO3− (after ssNa+) species dominated the summer, when total number and mass concentrations of aerosols were at their minimum. Elemental Carbon (EC) and Organic Carbon (OC) showed higher concentrations in spring with EC-to-OC ratio ~ 0.08 - 0.22. The columnar AOD varied between 0.01 and 0.20 (annual mean ~ 0.09), resulting in aerosol radiative forcing (in the top of the atmosphere) ~ 0.15 - 2.69 Wm-2 in the month of April (during spring). Potential source contribution function (PSCF) revealed the dominant source areas to be over Europe and Russia in terms of contributing to the seasonal high BC mass concentrations at Ny-Ålesund. Our study has also revealed an unusual impact of biomass burning aerosols (advected from the Alaska wildfire) during July 2015.

Influence of aerosol copper on HO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt; uptake: a novel parameterized equation

Abstract. Heterogeneous uptake of hydroperoxyl radicals (HO2) onto aerosols has been proposed to be a significant sink of HOx, hence impacting the atmospheric oxidation capacity. Accurate calculation of the HO2 uptake coefficient γHO2 is key to quantifying the potential impact of this atmospheric process. Laboratory studies show that γHO2 can vary by orders of magnitude due to changes in aerosol properties, especially aerosol soluble copper (Cu) concentration and aerosol liquid water content (ALWC). In this study we present a state-of-the-art model called MARK to simulate both gas- and aerosol-phase chemistry for the uptake of HO2 onto Cu-doped aerosols. Moreover, a novel parameterization of HO2 uptake was developed that considers changes in relative humidity (RH) and condensed-phase Cu ion concentrations and which is based on a model optimization using previously published and new laboratory data included in this work. This new parameterization will be applicable to wet aerosols, and it will complement current IUPAC recommendations. The new parameterization is as follows (the explanations for symbols are in the Appendix): 1γHO2=1αHO2+3×υHO24×106×RdHcorrRT×(5.87+3.2×ln⁡(ALWC/[PM]+0.067))×[PM]-0.2×Cu2+eff0.65+υHO2l4RTHorgDorgε. All parameters used in the paper are summarized in Table A1. Using this new equation, field data from a field campaign were used to evaluate the impact of the HO2 uptake onto aerosols on the ROx (= OH + HO2 + RO2) budget. Highly variable values for HO2 uptake were obtained for the North China Plain (median value &lt; 0.1).

Characterization of aerosol hygroscopicity using Raman lidar measurements at the EARLINET station of Payerne

Abstract. This study focuses on the analysis of aerosol hygroscopicity using remote sensing techniques. Continuous observations of aerosol backscatter coefficient (βaer), temperature (T) and water vapor mixing ratio (r) have been performed by means of a Raman lidar system at the aerological station of MeteoSwiss at Payerne (Switzerland) since 2008. These measurements allow us to monitor in a continuous way any change in aerosol properties as a function of the relative humidity (RH). These changes can be observed either in time at a constant altitude or in altitude at a constant time. The accuracy and precision of RH measurements from the lidar have been evaluated using the radiosonde (RS) technique as a reference. A total of 172 RS profiles were used in this intercomparison, which revealed a bias smaller than 4 % RH and a standard deviation smaller than 10 % RH between both techniques in the whole (in lower) troposphere at nighttime (at daytime), indicating the good performance of the lidar for characterizing RH. A methodology to identify situations favorable to studying aerosol hygroscopicity has been established, and the aerosol hygroscopicity has been characterized by means of the backscatter enhancement factor (fβ). Two case studies, corresponding to different types of aerosol, are used to illustrate the potential of this methodology. The first case corresponds to a mixture of rural aerosol and smoke particles (smoke mixture), which showed a higher hygroscopicity (fβ355=2.8 and fβ1064=1.8 in the RH range 73 %–97 %) than the second case, in which mineral dust was present (fβ355=1.2 and fβ1064=1.1 in the RH range 68 %–84 %). The higher sensitivity of the shortest wavelength to hygroscopic growth was qualitatively reproduced using Mie simulations. In addition, a good agreement was found between the hygroscopic analysis done in the vertical and in time for Case I, where the latter also allowed us to observe the hydration and dehydration of the smoke mixture. Finally, the impact of aerosol hygroscopicity on the Earth's radiative balance has been evaluated using the GAME (Global Atmospheric Model) radiative transfer model. The model showed an impact with an increase in absolute value of 2.4 W m−2 at the surface with respect to the dry conditions for the hygroscopic layer of Case I (smoke mixture).

Sensitivity of aerosol radiative forcing to various aerosol parameters over the Bay of Bengal

In the shortwave solar spectrum ( $$0.25{-}5~\upmu \hbox {m}$$ ), radiation is affected by the change in various aerosol properties and also by water vapour and other gas molecules. The presence of a variety of aerosols over the Bay of Bengal (BoB) during different seasons results in a change in aerosol properties, including the aerosol layer height. The BoB is an integral part of the Indian monsoon, and hence it is essential to understand the radiation budget over the BoB. The sensitivity of the aerosol forcing due to the changes in aerosol properties and other parameters has been studied using the Santa Barbara discrete ordinates radiative transfer model. The aerosol forcing at the top of the atmosphere was found to depend on the aerosol loading (aerosol optical depth), aerosol type (single scattering albedo) and the angular distribution of the scattered radiation (asymmetry parameter). The analysis also shows the presence of a relationship between aerosol layer height and the total amount of water vapour present in the atmosphere. The present study highlights the need for better retrievals of vertical aerosol distribution and water vapour profiles for a better understanding of the role of aerosols in the climate.

Properties of Arctic Aerosol Based on Sun Photometer Long-Term Measurements in Ny-Ålesund, Svalbard

On the basis of sun photometer measurements located at the German-French polar research base AWIPEV in Ny-Ålesund ( 78.923 ° N, 11.928 ° E), Svalbard, long-term changes (2001–2017) of aerosol properties in the European Arctic are analyzed with the main focus on physical aerosol properties like Aerosol Optical Depth (AOD) and the Ångström exponent during the Arctic haze season in spring compared with summer and autumn months. In order to gain more information from the photometer data and to reduce the error of fitting the data to the Ångström law, a new approach with an Ångström exponent, which depends linearly on wavelength, is presented in this paper. With the Mie program of libRadtran, a calculator for long- and short-wave radiation through the Earth’s atmosphere, artificial aerosol size distributions were created to extend the physical understanding of this modified Ångström law. Monthly means of the measured AOD of the years 1994–2017 are presented to analyze long-term changes of aerosol properties and its load. Because photometer data in general have no height information, a comparison with a Lidar located at the same site is presented. The so-obtained data are then compared with the previous Mie calculus. More homogeneous aerosol properties were found during spring and more heterogeneous in summer. To study possible aerosol sources and sinks, five-day back-trajectories were calculated with the FLEXPART model at three different arriving heights at 11 UTC in the village Ny-Ålesund. Besides the pollution pathway of the aerosol into the European Arctic based on the calculated back-trajectories, the influence of the boundary layer parameterized by the lowermost 100 hPa atmospheric layer is analyzed and compared to the measured aerosol load by the photometer in Ny-Ålesund additionally. During spring, the open ocean acts as a sink for aerosols, whereas sea ice clearly reduces their sinks. Hence, trajectories over sea ice are correlated to higher aerosol loads. Thus, both sources and sinks must be considered to understand aerosol occurrences in the Arctic.

Shallow Convective Cloud Field Lifetime as a Key Factor for Evaluating Aerosol Effects

SummaryClouds control much of the Earth's energy and water budgets. Aerosols, suspended in the atmosphere, interact with clouds and affect their properties. Recent studies have suggested that the aerosol effect on warm convective cloud systems evolve in time and eventually approach a steady state for which the overall effects of aerosols can be considered negligible. Using numerical simulations, it was estimated that the time needed for such cloud fields to approach this state is >24 hr. These results suggest that the typical cloud field lifetime is an important parameter in determining the total aerosol effect. Here, analyzing satellite observations and reanalysis data (with the aid of numerical simulations), we show that the characteristic timescale of warm convective cloud fields is less than 12 hr. Such a timescale implies that these clouds should be regarded as transient-state phenomena and therefore can be highly susceptible to changes in aerosol properties.

Satellite Observations of Cloud-Related Variations in Aerosol Properties

This paper presents an overview of our efforts to characterize and better understand cloud-related changes in aerosol properties. These efforts primarily involved the statistical analysis of global or regional datasets of Moderate Resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aerosol and cloud observations. The results show that in oceanic regions, more than half of all aerosol measurements by passive satellite instruments come from near-cloud areas, where clouds and cloud-related processes may significantly modify aerosol optical depth and particle size. Aerosol optical depth is also shown to increase systematically with regional cloud amount throughout the Earth. In contrast, it is shown that effective particle size can either increase or decrease with increasing cloud cover. In bimodal aerosol populations, the sign of changes depends on whether coarse mode or small mode aerosols are most affected by clouds. The results also indicate that over large parts of Earth, undetected cloud particles are not the dominant reason for the satellite-observed changes with cloud amount, and that 3D radiative processes contribute about 30% of the observed near-cloud changes. The findings underline the need for improving our ability to accurately measure aerosols near clouds.

What drives changes in aerosol properties over the Yangtze River Basin in past four decades？

Since the Reform and Opening up in China, aerosols increasingly affect the country's climate change and human health. However, remote sensing studies have been inconclusive as to long-term trends in Chinese aerosol emissions. The newly-released MERRA-2 product provides a long-term (1980 onward) aerosol reanalysis dataset, and thus is used in this study for identifying trends in aerosol optical depth (AOD) and aerosol direct radiative effect (ADRE) in clear sky over the Yangtze River Basin (YRB) based on the MK nonparametric method. Results reveal that there is a notable turning point in AOD trends around 2008, i.e., significantly increasing by 0.0201 year−1 before 2008 and then deceasing by −0.0185 year−1. The reason may be the decreases of S02, NOx and soot (dust) emissions from major cities in the YRB since 2006. Likewise, the cooling (warming) effects at the top of atmosphere (TOA), surface (SFC) and atmosphere (ATM) strongly increase by −0.3744 and −0.5652 (0.2935) wm−2 year−1 before 2008, and then significantly decrease by 0.2731 and 0.5868 (−0.3145) wm−2 year−1. Trend analyses confirm that changes in AOD dominate ADRE trends. Furthermore, AOD is significantly negatively (positively) associated with NDVI and precipitation (GDP and Population density) over most areas of the YRB. Besides, similar spatial trends with AOD are also identified in GDP and NDVI. This indicates that increases in GDP and decreases in NDVI caused by rapid urbanization partly lead to the growth of AOD over the middle and lower reaches of the YRB. However, changes in precipitation and Population density alone may not be the main factors for the increasing AOD.

Modification of Local Urban Aerosol Properties by Long-Range Transport of Biomass Burning Aerosol

During August 2016, a quasi-stationary high-pressure system spreading over Central and North-Eastern Europe, caused weather conditions that allowed for 24/7 observations of aerosol optical properties by using a complex multi-wavelength PollyXT lidar system with Raman, polarization and water vapour capabilities, based at the European Aerosol Research Lidar Network (EARLINET network) urban site in Warsaw, Poland. During 24–30 August 2016, the lidar-derived products (boundary layer height, aerosol optical depth, Ångström exponent, lidar ratio, depolarization ratio) were analysed in terms of air mass transport (HYSPLIT model), aerosol load (CAMS data) and type (NAAPS model) and confronted with active and passive remote sensing at the ground level (PolandAOD, AERONET, WIOS-AQ networks) and aboard satellites (SEVIRI, MODIS, CATS sensors). Optical properties for less than a day-old fresh biomass burning aerosol, advected into Warsaw’s boundary layer from over Ukraine, were compared with the properties of long-range transported 3–5 day-old aged biomass burning aerosol detected in the free troposphere over Warsaw. Analyses of temporal changes of aerosol properties within the boundary layer, revealed an increase of aerosol optical depth and Ångström exponent accompanied by an increase of surface PM10 and PM2.5. Intrusions of advected biomass burning particles into the urban boundary layer seem to affect not only the optical properties observed but also the top height of the boundary layer, by moderating its increase.

Different trends in extreme and median surface aerosol extinction coefficients over China inferred from quality-controlled visibility data

Abstract. Although the temporal changes in aerosol properties have been widely investigated, the majority of studies has focused on average conditions without much emphasis on the extremes. However, the latter can be more important in terms of human health and climate change. This study uses a previously validated, quality-controlled visibility dataset to investigate the long-term trends (expressed in terms of relative changes) in extreme surface aerosol extinction coefficient (AEC) over China and compares them with the median trends. Two methods are used to independently evaluate the trends, which arrive at consistent results. The signs of extreme and median trends are generally coherent, whereas their magnitudes show distinct spatial and temporal differences. In the 1980s, an overall positive trend is found throughout China with the extreme trend exceeding the mean trend, except for northwest China and the North China Plain. In the 1990s, AEC over northeast and northwest China started to decline while the rest of the country still exhibited an increase. The extreme trends continued to dominate in the south while they yielded to the mean trend in the north. After the year 2000, the extreme trend became weaker than the mean trend overall in terms of both the magnitude and significance level. The annual trend can be primarily attributed to winter and fall trends. The results suggest that the decadal changes in pollution in China may be governed by different mechanisms. Synoptic conditions that often result in extreme air quality changes might have dominated in the 1980s, whereas emission increase might have been the main factor for the 2000s.

Increase of surface solar irradiance across East China related to changes in aerosol properties during the past decade

Previously, it was widely documented that an overall decrease in surface solar radiation occurred in China at least until 2005, in contrast to the general background of ‘global brightening’. Increased anthropogenic aerosol emissions were speculated to be the source of the reduction. In this study, we extend the trend analysis to the most recent decade from 2005–2015 and find that surface solar radiation has shifted from ‘dimming’ to ‘brightening’ over East China, with the largest increase over the northeast and southeast parts. Meanwhile, satellite and ground observation both indicate a reduction in aerosol optical depth (AOD) during the same period, whereas no significant trends in cloud amount show up. Detailed analysis using co-located radiation and aerosol observation at the XiangHe station in North China suggests that both AOD and single scattering albedo (SSA) changes contribute to the radiation trends. AOD reduction contributes to the increase of direct solar radiation, also decreasing the diffuse radiation, while the increase of SSA serves to increase the diffuse fraction. Simple calculations using a radiative transfer model confirm that the two effects combined explain changes in the global solar radiation and its components effectively. Our results have implications for potential climate effects with the reduction of China’s aerosol emissions, and the necessity to monitor aerosol composition in addition to its loading.

Unveiling aerosol–cloud interactions – Part 2: Minimising the effects of aerosol swelling and wet scavenging in ECHAM6-HAM2 for comparison to satellite data

Abstract. Aerosol–cloud interactions (ACIs) are uncertain and the estimates of the ACI effective radiative forcing (ERFaci) magnitude show a large variability. Within the Aerosol_cci project the susceptibility of cloud properties to changes in aerosol properties is derived from the high-resolution AATSR (Advanced Along-Track Scanning Radiometer) data set using the Cloud–Aerosol Pairing Algorithm (CAPA) (as described in our companion paper) and compared to susceptibilities from the global aerosol climate model ECHAM6-HAM2 and MODIS–CERES (Moderate Resolution Imaging Spectroradiometer – Clouds and the Earth's Radiant Energy System) data. For ECHAM6-HAM2 the dry aerosol is analysed to mimic the effect of CAPA. Furthermore the analysis is done for different environmental regimes. The aerosol–liquid water path relationship in ECHAM6-HAM2 is systematically stronger than in AATSR–CAPA data and cannot be explained by an overestimation of autoconversion when using diagnostic precipitation but rather by aerosol swelling in regions where humidity is high and clouds are present. When aerosol water is removed from the analysis in ECHAM6-HAM2 the strength of the susceptibilities of liquid water path, cloud droplet number concentration and cloud albedo as well as ERFaci agree much better with those of AATSR–CAPA or MODIS–CERES. When comparing satellite-derived to model-derived susceptibilities, this study finds it more appropriate to use dry aerosol in the computation of model susceptibilities. We further find that the statistical relationships inferred from different satellite sensors (AATSR–CAPA vs. MODIS–CERES) as well as from ECHAM6-HAM2 are not always of the same sign for the tested environmental conditions. In particular the susceptibility of the liquid water path is negative in non-raining scenes for MODIS–CERES but positive for AATSR–CAPA and ECHAM6-HAM2. Feedback processes like cloud-top entrainment that are missing or not well represented in the model are therefore not well constrained by satellite observations. In addition to aerosol swelling, wet scavenging and aerosol processing have an impact on liquid water path, cloud albedo and cloud droplet number susceptibilities. Aerosol processing leads to negative liquid water path susceptibilities to changes in aerosol index (AI) in ECHAM6-HAM2, likely due to aerosol-size changes by aerosol processing. Our results indicate that for statistical analysis of aerosol–cloud interactions the unwanted effects of aerosol swelling, wet scavenging and aerosol processing need to be minimised when computing susceptibilities of cloud variables to changes in aerosol.

Effect of sea breeze circulation on aerosol mixing state and radiative properties in a desert setting

Abstract. Chemical composition, microphysical, and optical properties of atmospheric aerosol deep inland in the Negev Desert of Israel are found to be influenced by daily occurrences of sea breeze flow from the Mediterranean Sea. Abrupt increases in aerosol volume concentration and shifts of size distributions towards larger sizes, which are associated with increase in wind speed and atmospheric water content, were systematically recorded during the summertime at a distance of at least 80 km from the coast. Chemical imaging of aerosol samples showed an increased contribution of highly hygroscopic particles during the intrusion of the sea breeze. Besides a significant fraction of marine aerosols, the amount of internally mixed marine and mineral dust particles was also increased during the sea breeze period. The number fraction of marine and internally mixed particles during the sea breeze reached up to 88 % in the PM1–2. 5 and up to 62 % in the PM2. 5–10 size range. Additionally, numerous particles with residuals of liquid coating were observed by SEM/EDX analysis. Ca-rich dust particles that had reacted with anthropogenic nitrates were evidenced by Raman microspectroscopy. The resulting hygroscopic particles can deliquesce at very low relative humidity. Our observations suggest that aerosol hygroscopic growth in the Negev Desert is induced by the daily sea breeze arrival. The varying aerosol microphysical and optical characteristics perturb the solar and thermal infrared radiations. The changes in aerosol properties induced by the sea breeze, relative to the background situation, doubled the shortwave radiative cooling at the surface (from −10 to −20.5 W m−2) and increased by almost 3 times the warming of the atmosphere (from 5 to 14 W m−2), as evaluated for a case study. Given the important value of observed liquid coating of particles, we also examined the possible influence of the particle homogeneity assumption on the retrieval of aerosol microphysical characteristics. The tests suggest that sensitivity to the coating appears if backward scattering and polarimetric measurements are available for the inversion algorithm. This may have an important implication for retrievals of aerosol microphysical properties in remote sensing applications.

Transport of pollution to a remote coastal site during gap flow from California's interior: impacts on aerosol composition, clouds, and radiative balance

Abstract. During the CalWater 2015 field campaign, ground-level observations of aerosol size, concentration, chemical composition, and cloud activity were made at Bodega Bay, CA, on the remote California coast. A strong anthropogenic influence on air quality, aerosol physicochemical properties, and cloud activity was observed at Bodega Bay during periods with special weather conditions, known as Petaluma Gap flow, in which air from California's interior is transported to the coast. This study applies a diverse set of chemical, cloud microphysical, and meteorological measurements to the Petaluma Gap flow phenomenon for the first time. It is demonstrated that the sudden and often dramatic change in aerosol properties is strongly related to regional meteorology and anthropogenically influenced chemical processes in California's Central Valley. In addition, it is demonstrated that the change in air mass properties from those typical of a remote marine environment to properties of a continental regime has the potential to impact atmospheric radiative balance and cloud formation in ways that must be accounted for in regional climate simulations.

Effect of aerosol subgrid variability on aerosol optical depth and cloud condensation nuclei: implications for global aerosol modelling

Abstract. A fundamental limitation of grid-based models is their inability to resolve variability on scales smaller than a grid box. Past research has shown that significant aerosol variability exists on scales smaller than these grid boxes, which can lead to discrepancies in simulated aerosol climate effects between high- and low-resolution models. This study investigates the impact of neglecting subgrid variability in present-day global microphysical aerosol models on aerosol optical depth (AOD) and cloud condensation nuclei (CCN). We introduce a novel technique to isolate the effect of aerosol variability from other sources of model variability by varying the resolution of aerosol and trace gas fields while maintaining a constant resolution in the rest of the model. We compare WRF-Chem (Weather and Research Forecast model) runs in which aerosol and gases are simulated at 80 km and again at 10 km resolutions; in both simulations the other model components, such as meteorology and dynamics, are kept at the 10 km baseline resolution. We find that AOD is underestimated by 13 % and CCN is overestimated by 27 % when aerosol and gases are simulated at 80 km resolution compared to 10 km. The processes most affected by neglecting aerosol subgrid variability are gas-phase chemistry and aerosol uptake of water through aerosol–gas equilibrium reactions. The inherent non-linearities in these processes result in large changes in aerosol properties when aerosol and gaseous species are artificially mixed over large spatial scales. These changes in aerosol and gas concentrations are exaggerated by convective transport, which transports these altered concentrations to altitudes where their effect is more pronounced. These results demonstrate that aerosol variability can have a large impact on simulating aerosol climate effects, even when meteorology and dynamics are held constant. Future aerosol model development should focus on accounting for the effect of subgrid variability on these processes at global scales in order to improve model predictions of the aerosol effect on climate.

Effect of aerosol concentration and absorbing aerosol on the radiation fog life cycle

Analogous to cloud formation, the formation and life cycle of fogs is largely influenced by aerosol particles. The objective of this work is to analyze how changes in aerosol properties affect the fog life cycle, with special emphasis on how droplet concentrations change with cloud condensation nuclei (CCN) concentrations and on the effect that absorbing black carbon (BC) particles have on fog dissipation. For our simulation case study, we chose a typical fall time radiation fog at mid-latitudes (45° north) in fairly highly polluted conditions. Our results show that CCN concentrations have a strong influence on the fog lifetime. This is because the immediate effect of CCN on cloud droplet number concentrations (CDNC) is enhanced through two positive feedback loops: (1) Higher CDNC leads to more radiative cooling at the fog top, which leads to even stronger activation and (2) if CDNC is higher, the average droplet size is smaller, which slows down droplet removal through sedimentation. The effect that radiation fogs have on solar surface irradiation is large – the daily mean can change by 50% if CCN concentrations are doubled or halved (considering a reference CCN mixing ratio of 800 #/mg). With the same changes in CCN, the total fog lifetime increases 160 min or decreases 65 min, respectively. Although BC has a noticeable effect on fog height and dissipation time, its relative effect compared to CCN is small, even if BC concentrations are high. The fog formation is very sensitive to initial meteorological conditions which may be altered considerably if fog was present the previous day. This effect was neglected here, and future simulations, which span several days, may thus be a valuable extension of this study.