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Aerosols affect the Earth's energy budget directly by scattering and absorbing radiation and indirectly by acting as cloud condensation nuclei and, thereby, affecting cloud properties. However, large uncertainties exist in current estimates of aerosol forcing because of incomplete knowledge concerning the distribution and the physical and chemical properties of aerosols as well as aerosol-cloud interactions. In recent years, a great deal of effort has gone into improving measurements and datasets. It is thus feasible to shift the estimates of aerosol forcing from largely model-based to increasingly measurement-based. Our goal is to assess current observational capabilities and identify uncertainties in the aerosol direct forcing through comparisons of different methods with independent sources of uncertainties. Here we assess the aerosol optical depth (tau;), direct radiative effect (DRE) by natural and anthropogenic aerosols, and direct climate forcing (DCF) by anthropogenic aerosols, focusing on satellite and ground-based measurements supplemented by global chemical transport model (CTM) simulations. The multi-spectral MODIS measures global distributions of aerosol optical depth (τ) on a daily scale, with a high accuracy of ±0.03±0.05τ over ocean. The annual average τ is about 0.14 over global ocean, of which about 21%±7% is contributed by human activities, as estimated by MODIS fine-mode fraction. The multiangle MISR derives an annual average AOD of 0.23 over global land with an uncertainty of ∼20% or ±0.05. These high-accuracy aerosol products and broadband flux measurements from CERES make it feasible to obtain observational constraints for the aerosol direct effect, especially over global the ocean. A number of measurement-based approaches estimate the clear-sky DRE (on solar radiation) at the top-of-atmosphere (TOA) to be about -5.5±0.2Wm-2 (median ± standard error from various methods) over the global ocean. Accounting for thin cirrus contamination of the satellite derived aerosol field will reduce the TOA DRE to -5.0Wm-2. Because of a lack of measurements of aerosol absorption and difficulty in characterizing land surface reflection, estimates of DRE over land and at the ocean surface are currently realized through a combination of satellite retrievals, surface measurements, and model simulations, and are less constrained. Over the oceans the surface DRE is estimated to be -8.8±0.7Wm-2. Over land, an integration of satellite retrievals and model simulations derives a DRE of -4.9±0.7Wm-2 and -11.8±1.9Wm-2 at the TOA and surface, respectively. CTM simulations derive a wide range of DRE estimates that on average are smaller than the measurement-based DRE by about 30-40%, even after accounting for thin cirrus and cloud contamination. A number of issues remain. Current estimates of the aerosol direct effect over land are poorly constrained. Uncertainties of DRE estimates are also larger on regional scales than on a global scale and large discrepancies exist between different approaches. The characterization of aerosol absorption and vertical distribution remains challenging. The aerosol direct effect in the thermal infrared range and in cloudy conditions remains relatively unexplored and quite uncertain, because of a lack of global systematic aerosol vertical profile measurements. A coordinated research strategy needs to be developed for integration and assimilation of satellite measurements into models to constrain model simulations. Enhanced measurement capabilities in the next few years and high-level scientific cooperation will further advance our knowledge. [ABSTRACT FROM AUTHOR]

The largest uncertainty in the radiative forcing of climate change over the industrial era is that due to aerosols, a substantial fraction of which is the uncertainty associated with scattering and absorption of shortwave (solar) radiation by anthropogenic aerosols in cloud-free conditions (IPCC, 2001). Quantifying and reducing the uncertainty in aerosol influences on climate is critical to understanding climate change over the industrial period and to improving predictions of future climate change for assumed emission scenarios. Measurements of aerosol properties during major field campaigns in several regions of the globe during the past decade are contributing to an enhanced understanding of atmospheric aerosols and their effects on light scattering and climate. The present study, which focuses on three regions downwind of major urban/population centers (North Indian Ocean (NIO) during INDOEX, the Northwest Pacific Ocean (NWP) during ACE-Asia, and the Northwest Atlantic Ocean (NWA) during ICARTT), incorporates understanding gained from field observations of aerosol distributions and properties into calculations of perturbations in radiative fluxes due to these aerosols. This study evaluates the current state of observations and of two chemical transport models (STEM and MOZART). Measurements of burdens, extinction optical depth (AOD), and direct radiative effect of aerosols (DRE -- change in radiative flux due to total aerosols) are used as measurement-model check points to assess uncertainties. In-situ measured and remotely sensed aerosol properties for each region (mixing state, mass scattering efficiency, single scattering albedo, and angular scattering properties and their dependences on relative humidity) are used as input parameters to two radiative transfer models (GFDL and University of Michigan) to constrain estimates of aerosol radiative effects, with uncertainties in each step propagated through the analysis. Constraining the radiative transfer calculations by observational inputs increases the clear-sky, 24-h averaged AOD (34±8%), top of atmosphere (TOA) DRE (32±12%), and TOA direct climate forcing of aerosols (DCF -- change in radiative flux due to anthropogenic aerosols) (37±7%) relative to values obtained with "a priori" parameterizations of aerosol loadings and properties (GFDL RTM). The resulting constrained clear-sky TOA DCF is -3.3±0.47, -14±2.6, -6.4±2.1Wm-2 for the NIO, NWP, and NWA, respectively. With the use of constrained quantities (extensive and intensive parameters) the calculated uncertainty in DCF was 25% less than the "structural uncertainties" used in the IPCC-2001 global estimates of direct aerosol climate forcing. Such comparisons with observations and resultant reductions in uncertainties are essential for improving and developing confidence in climate model calculations incorporating aerosol forcing. [ABSTRACT FROM AUTHOR]

Aerosol hygroscopicity plays a vital role in aerosol radiative forcing. One key parameter describing hygroscopicity is the scattering enhancement factor, f (RH), defined as the ratio of the scattering coefficient at humidified relative humidity (RH) to its dry value. Here, we utilize the f (80 %) from ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) 2016 and 2018 airborne measurements to investigate the hygroscopicity of aerosols, its vertical distribution, its relationship with chemical composition, and its sensitivity to organic aerosol (OA) hygroscopicity over the southeast Atlantic (SEA) Ocean during the biomass burning (BB) season. We found that aerosol hygroscopicity remains steady above 2 km, with a mean f (80 %) of 1.40 ± 0.17. Below 2 km, aerosol hygroscopicity increases with decreasing altitude, with a mean f (80 %) of 1.51 ± 0.22, consistent with higher values of BB aerosol hygroscopicity found in the literature. The hygroscopicity parameter of OA (κOA) is retrieved from the Mie model with a mean value of 0.11 ± 0.08, which is in the middle to upper range compared to the literature. Higher OA hygroscopicity is related to aerosols that are more aged, oxidized, and present at lower altitudes. The enhanced biomass burning aerosol (BBA) hygroscopicity at lower altitudes is mainly due to a lower OA fraction, increased sulfate fraction, and greater κOA at lower altitudes. We propose a parameterization that quantifies f (RH) with chemical composition and κOA based on Mie simulation of internally mixed OA–(NH4)2SO4–BC mixtures. The good agreement between the predictions and the ORACLES measurements implies that the aerosols in the SEA during the BB season can be largely represented by the OA–(NH4)2SO4–BC internal mixture with respect to the f (RH) prediction. The sensitivity of f (RH) to κOA indicates that applying a constant κOA is only suitable when the OA fraction is low and κOA shows limited variation. However, in situations deviating these two criteria, κOA can notably impact scattering coefficients and aerosol radiative effect; therefore, accounting for κOA variability is recommended. [ABSTRACT FROM AUTHOR]

Assessing aerosol mixing states, which primarily depend on aerosol chemical compositions, is indispensable to estimate direct and indirect effects of aerosols. The limitations of the direct measurements of aerosol chemical composition and mixing states necessitate modeling approaches to infer the aerosol mixing states. The Optical Properties of Aerosols and Clouds (OPAC) model has been extensively utilized to construct optically equivalent aerosol chemical compositions from measured aerosol optical properties using Mie inversion. However, the representation of real atmospheric aerosol mixing scenarios in OPAC has perennially been challenged by the exclusive assumption of external mixing. A Python successor to the aerosol module of the OPAC model is developed, named AeroMix, with novel capabilities to (1) model externally and core–shell mixed aerosols, (2) simulate optical properties of aerosol mixtures constituted by any number of aerosol components, and (3) define aerosol composition and relative humidity in up to six vertical layers. Designed as a versatile open-source aerosol optical model framework, AeroMix is tailored for sophisticated inversion algorithms aimed at modeling aerosol mixing states and also their physical and chemical properties. AeroMix's performance is demonstrated by modeling the probable aerosol mixing states over Kanpur (urban) and the Bay of Bengal (marine) in south Asia. The modeled mixing states are consistent with independent measurements using a single-particle soot photometer (SP2) and transmission electron microscopy (TEM), substantiating the potential capability of AeroMix to model complex aerosol mixing scenarios involving multiple internally mixed components in diverse environments. This work contributes a valuable tool for modeling aerosol mixing states to assess their impact on cloud-nucleating properties and radiation budget. [ABSTRACT FROM AUTHOR]

This study focuses on the comparison of aerosol columnar aerosol optical depth (AOD) and lidar ratios together with vertical profiles of aerosol extinction and backscatter at 532 nm retrieved over the King Abdullah University of Science and Technology (KAUST) campus observation site for the period of 2019–2022 using the Generalized Retrieval of Atmosphere and Surface Properties (GRASP) and Micro-Pulse Lidar Network (MPLNET) approaches. An emphasis is placed on independent analysis of daylight and nighttime retrievals to estimate how strongly the differences in the assumptions of both methods made in the absence of nighttime AOD observations influence the retrieval results. Additionally, two aerosol products provided by GRASP excluding and including the volume depolarization observations at 532 nm provided by MPLNET are analyzed to estimate the potential benefits of usage of depolarization data in aerosol profile retrievals. Overall, both columnar and vertical MPLNET and GRASP products demonstrated a better agreement for daytime retrievals for the GRASP product that excluded the depolarization information. At the same time, inclusion of the volume depolarization observations improved the agreement between MPLNET- and GRASP-estimated values at nighttime, both columnar and vertical. In addition, estimated values of daytime extinction profiles at ground level were compared to assess the impact of the assumption of a constant aerosol vertical distribution in the cutoff zone of lidar observations implied in GRASP. The values estimated by GRASP demonstrated a good agreement with MPLNET, for retrievals both including and excluding volume depolarization information. A seasonal variability in the diurnal cycle of aerosol properties estimated by GRASP over the KAUST site for the period 2019–2022 is presented, analyzed and discussed. [ABSTRACT FROM AUTHOR]

A new four-dimensional, multiyear, and near-global climate data record of the fine-mode (submicrometer in terms of diameter) and coarse-mode (supermicrometer in terms of diameter) components of atmospheric pure dust is presented. The separation of the two modes of dust in detected atmospheric dust layers is based on a combination of (1) the total pure-dust product provided by the well-established European Space Agency (ESA) "LIdar climatology of Vertical Aerosol Structure" (LIVAS) database and (2) the coarse-mode component of pure dust provided by the first step of the two-step POlarization LIdar PHOtometer Networking (POLIPHON) technique, developed in the framework of the European Aerosol Research Lidar Network (EARLINET). Accordingly, the fine-mode component of pure dust is extracted as the residual between the LIVAS total pure dust and the coarse-mode component of pure dust. Intermediate steps involve the implementation of regionally dependent lidar-derived lidar ratio values and AErosol RObotic NETwork (AERONET)-based climatological extinction-to-volume conversion factors, facilitating conversion of dust backscatter into extinction and subsequently extinction into mass concentration. The decoupling scheme is applied to observations from the Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) at 532 nm. The final products consist of the fine mode and coarse mode of atmospheric pure dust, quality-assured profiles of backscatter coefficient at 532 nm, extinction coefficient at 532 nm, and mass concentration for each of the two components. The datasets are established primarily with the original L2 horizontal (5 km) and vertical (60 m) resolution of the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) along the CALIPSO orbit path and secondly in averaged profiles of seasonal–temporal resolution, 1° × 1° spatial resolution, and the original vertical resolution of CALIPSO, focusing on the latitudinal band extending between 70° S and 70° N and covering more than 15 years of Earth observations (June 2006–December 2021). The quality of the CALIPSO-based fine-mode and coarse-mode dust products is assessed through the use of AERONET fine-mode and coarse-mode aerosol optical thickness (AOT) interpolated to 532 nm and the AERosol properties – Dust (AER-D) campaign airborne in situ particle size distributions (PSDs) as reference datasets during atmospheric conditions characterized by dust presence. The near-global fine-mode and coarse-mode pure-dust climate data record is considered unique with respect to a wide range of potential applications, including climatological, time series, and trend analysis over extensive geographical domains and temporal periods, validation of atmospheric dust models and reanalysis datasets, assimilation activities, and investigation of the role of airborne dust in radiation and air quality. [ABSTRACT FROM AUTHOR]

An uncrewed aerial system (UAS) has been developed for observations of aerosol and cloud properties relevant to aerosol direct and indirect forcing in the marine atmosphere. The UAS is a Hybrid Quadrotor–fixed-wing aircraft designed for launch and recovery from a confined space such as a ship deck. Two payloads, clear sky and cloudy sky, house instrumentation required to characterize aerosol radiative forcing effects. The observing platform (UAS plus payloads) has been deployed from a ship and from a coastal site for observations in the marine atmosphere. We describe here details of the UAS, the payloads, and first observations from the TowBoatU.S. Richard L. Becker (March 2022) and from the Tillamook UAS Test Range (August 2022). The development of this UAS technology for flights from ships and coastal locations is expected to greatly increase observations of aerosol radiative effects in the marine boundary layer over both temporal and spatial scales. [ABSTRACT FROM AUTHOR]

Ice-nucleating particles (INPs) are an essential class of aerosols found worldwide that have far-reaching but poorly quantified climate feedback mechanisms through interaction with clouds and impacts on precipitation. These particles can have highly variable physicochemical properties in the atmosphere, and it is crucial to continuously monitor their long-term concentration relative to total ambient aerosol populations at a wide variety of sites to comprehensively understand aerosol–cloud interactions in the atmosphere. Hence, our study applied an in situ forced expansion cooling device to measure ambient INP concentrations and test its automated continuous measurements at atmospheric observatories, where complementary aerosol instruments are heavily equipped. Using collocated aerosol size, number, and composition measurements from these sites, we analyzed the correlation between sources and abundance of INPs in different environments. Toward this aim, we have measured ground-level INP concentrations at two contrasting sites, one in the Southern Great Plains (SGP) region of the United States with a substantial terrestrially influenced aerosol population and one in the Eastern North Atlantic Ocean (ENA) region with a primarily marine-influenced aerosol population. These measurements examined INPs mainly formed through immersion freezing and were performed at a ≤ 12 min resolution and with a wide range of heterogeneous freezing temperatures (T s above - 31 °C) for at least 45 d at each site. The associated INP data analysis was conducted in a consistent manner. We also explored the additional offline characterization of ambient aerosol particle samples from both locations in comparison to in situ data. From our ENA data, on average, INP abundance ranges from ≈ 1 to ≈ 20 L -1 (- 30 °C ≤ T ≤ - 20 °C) during October–November 2020. Backward air mass trajectories reveal a strong marine influence at ENA with 75.7 % of air masses originating over the Atlantic Ocean and 96.6 % of air masses traveling over open water, but analysis of particle chemistry suggests an additional INP source besides maritime aerosols (e.g., sea spray aerosols) at ENA. In contrast, 90.8 % of air masses at the SGP location originated from the North American continent, and 96.1 % of the time, these air masses traveled over land. As a result, organic-rich SGP aerosols from terrestrial sources exhibited notably high INP abundance from ≈ 1 to ≈ 100 L -1 (- 30 °C ≤ T ≤ - 15 °C) during October–November 2019. The probability density function of aerosol surface area-scaled immersion freezing efficiency (ice nucleation active surface site density; ns) was assessed for selected freezing temperatures. While the INP concentrations measured at SGP are higher than those of ENA, the ns(T) values of SGP (≈ 10 5 to ≈ 10 7 m -2 for - 30 °C ≤ T ≤ - 15 °C) are reciprocally lower than ENA for approximately 2 orders of magnitude (≈ 10 7 to ≈ 10 9 m -2 for - 30 °C ≤ T ≤ - 15 °C). The observed difference in ns(T) mainly stems from varied available aerosol surface areas, Saer , from two sites (Saer,SGP > Saer,ENA). INP parameterizations were developed as a function of examined freezing temperatures from SGP and ENA for our study periods. [ABSTRACT FROM AUTHOR]

Aerosol optical depth was retrieved from two airborne remote sensing instruments, the Research Scanning Polarimeter (RSP) and Second Generation High Spectral Resolution Lidar (HSRL-2), during the National Aeronautics and Space Administration (NASA) Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE). The field campaign offers a unique opportunity to evaluate an extensive 3-year dataset under a wide range of meteorological conditions from two instruments on the same platform. However, a long-standing issue in atmospheric field studies is that there is a lack of reference datasets for properly validating field measurements and estimating their uncertainties. Here we address this issue by using the triple collocation method, in which a third collocated satellite dataset from the Moderate Resolution Imaging Spectroradiometer (MODIS) is introduced for comparison. HSRL-2 is found to provide a more accurate retrieval than RSP over the study region. The error standard deviation of HSRL-2 with respect to the ground truth is 0.027. Moreover, this approach enables us to develop a simple, yet efficient, quality control criterion for RSP data. The physical reasons for the differences in two retrievals are determined to be cloud contamination, aerosols near the surface, multiple aerosol layers, absorbing aerosols, non-spherical aerosols, and simplified retrieval assumptions. These results demonstrate the pathway for optimal aerosol retrievals by combining information from both lidars and polarimeters for future airborne and satellite missions. [ABSTRACT FROM AUTHOR]

Most of the dust models underestimate the load of the large dust particles, consider spherical shapes instead of irregular ones, and have to deal with a wide range of the dust refractive index (RI) to be used. This leads to an incomplete assessment of the dust radiative effects and dust-related impacts on climate and weather. The current work aims to provide an assessment, through a sensitivity study, of the limitations of models to calculate the dust direct radiative effect (DRE) due to the underrepresentation of its size, RI, and shape. We show that the main limitations stem from the size and RI, while using a more realistic shape plays only a minor role, with our results agreeing with recent findings in the literature. At the top of the atmosphere (TOA) close to dust sources, the underestimation of size issues an underestimation of the direct warming effect of dust of ∼ 18–25 W m -2 , for DOD = 1 (dust optical depth) at 0.5 µ m, depending on the solar zenith angle (SZA) and RI. The underestimation of the dust size in models is less above the ocean than above dust sources, resulting in an underestimation of the direct cooling effect of dust above the ocean by up to 3 W m -2 , for aerosol optical depth (AOD) of 1 at 0.5 µ m. We also show that the RI of dust may change its DRE by 80 W m -2 above the dust sources and by 50 W m -2 at downwind oceanic areas for DOD = 1 at 0.5 µ m at TOA. These results indicate the necessity of including more realistic sizes and RIs for dust particles in dust models, in order to derive better estimations of the dust DRE, especially near the dust sources and mostly for studies dealing with local radiation effects of dust aerosols. [ABSTRACT FROM AUTHOR]

Inadequate knowledge about the complex microphysical and optical processes of the aerosol–cloud system severely restricts our ability to quantify the resultant impact on climate. Contrary to the negative radiative forcing (cooling) exerted by aerosols in cloud-free skies over dark surfaces, the absorbing aerosols, when lofted over the clouds, can potentially lead to significant warming of the atmosphere. The sign and magnitude of the aerosol radiative forcing over clouds are determined mainly by the amount of aerosol loading, the absorption capacity of aerosols or single-scattering albedo (SSA), and the brightness of the underlying cloud cover. In satellite-based algorithms that use measurements from passive sensors, the assumption of aerosol SSA is known to be the largest source of uncertainty in quantifying above-cloud aerosol optical depth (ACAOD). In this paper, we introduce a novel synergy algorithm that combines direct airborne measurements of ACAOD and the top-of-atmosphere (TOA) spectral reflectance from Ozone Monitoring Instrument (OMI) and Moderate Resolution Imaging Spectroradiometer (MODIS) sensors of NASA's A-train satellites to retrieve (1) SSA of light-absorbing aerosols lofted over the clouds and (2) aerosol-corrected cloud optical depth (COD). Radiative transfer calculations show a marked sensitivity of the TOA measurements to ACAOD, SSA, and COD, further suggesting that the availability of accurate ACAOD allows retrieval of SSA for above-cloud aerosol scenes using the "color ratio" algorithm developed for satellite sensors carrying ultraviolet (UV) and visible-near-IR (VNIR) wavelength bands. The proposed algorithm takes advantage of airborne measurements of ACAOD acquired from the High Spectral Resolution Lidar-2 (HSRL-2) and Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) sun photometer operated during the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) field campaign (September 2016, August 2017, and October 2018) over the southeastern Atlantic Ocean and synergizes them with TOA reflectance from OMI and MODIS to derive spectral SSA in the near-UV (354–388 nm) and VNIR (470–860 nm), respectively. When compared against the ORACLES airborne remote sensing and in situ measurements and the inversion dataset of the ground-based Aerosol Robotic Network (AERONET) over land, the retrieved spectral SSAs from the satellites, on average, were found to be within agreement of ∼ 0.01 – the difference well within the uncertainties involved in all these inversion datasets. The retrieved SSA above the clouds at UV–Vis-NIR wavelengths shows a distinct increasing trend from August to October, which is consistent with the ORACLES in situ measurements, AERONET inversions, and previous findings. The sensitivity analysis quantifying theoretical uncertainties in the retrieved SSA shows that errors in the measured ACAOD, aerosol layer height, and the ratio of the imaginary part of the refractive index (spectral dependence) of aerosols by 20 %, 1 km, and 10 %, respectively, produce an error in the retrieved SSA at 388 nm (470 nm) by 0.017 (0.015), 0.008 (0.002), and 0.03 (0.005). The development of the proposed aerosol–cloud algorithm implies a possible synergy of Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) and OMI–MODIS passive sensors to deduce a global product of ACAOD and SSA. Furthermore, the presented synergy algorithm assumes implications for future missions, such as the Atmosphere Observing System (AOS) and the Earth Cloud Aerosol and Radiation Explorer (EarthCARE). The availability of the intended global dataset can help constrain climate models with the much-needed observational estimates of the radiative effects of aerosols in cloudy regions and expand our ability to study aerosol effects on clouds. [ABSTRACT FROM AUTHOR]

In order to improve aerosol representation in the NASA Goddard Earth Observing System (GEOS) model, we evaluated simulations of the transport and properties of aerosols from southern African biomass burning sources that were observed during the first deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) field campaign in September 2016. An example case study of 24 September was analyzed in detail, during which aircraft-based in situ and remote sensing observations showed the presence of a multi-layered smoke plume structure with significant vertical variation in single scattering albedo (SSA). Our baseline GEOS simulations were not able to represent the observed SSA variation or the observed organic aerosol-to-black-carbon ratio (OA : BC). Analyzing the simulated smoke age suggests that the higher-altitude, less absorbing smoke plume was younger (∼4 d), while the lower-altitude and more absorbing smoke plume was older (∼7 d). We hypothesize a chemical or microphysical loss process exists to explain the change in aerosol absorption as the smoke plume ages, and we apply a simple loss rate to the model hydrophilic biomass burning OA to simulate this process. We also utilized the ORACLES airborne observations to better constrain the simulation of aerosol optical properties, adjusting the assumed particle size, hygroscopic growth, and absorption. Our final GEOS model simulation with additional OA loss and updated optics showed better performance in simulating aerosol optical depth (AOD) and SSA compared to independent ground- and space-based retrievals for the entire month of September 2016, including the Ozone Monitoring Instrument (OMI) Aerosol Index. In terms of radiative implications of our model adjustments, the final GEOS simulation suggested a decreased atmospheric warming of about 10 % (∼2 W m -2) over the southeastern Atlantic region and above the stratocumulus cloud decks compared to the model baseline simulations. These results improve the representation of the smoke age, transport, and optical properties in Earth system models. [ABSTRACT FROM AUTHOR]

Marine aerosol affects the global energy budget and regional weather. The production of marine aerosol is primarily driven by wind at the sea–air interface. Previous studies have explored the effects of wind on marine aerosol, mostly by examining the relationships between aerosol optical depth (AOD) and surface wind speed. In this paper, utilizing the synergy of aerosol and wind observations from Aeolus, the relationships between the marine aerosol optical properties at 355 nm and the instantaneous co-located wind speeds of remote oceans are investigated at two vertical layers (within and above the marine atmospheric boundary layer (MABL)). The results show that the enhancements of the extinction and backscatter coefficients caused by wind are larger within the MABL than above it. The correlation models between extinction and backscatter with wind speed were established using power-law functions. The slope variation points occur during extinction and backscatter coefficients increasing with wind speed, indicating that the wind-driven enhancement of marine aerosol involves two phases: a rapid-growth phase with high wind dependence, followed by a slower-growth phase after the slope variation points. We also compared the AOD–wind relationship acquired from Aeolus with CALIPSO-derived results from previous research. The variation in the lidar ratio with wind speed is examined, suggesting a possible "increasing–decreasing–increasing" trend of marine aerosol particle size as wind speed increases. This study enhances the comprehension of the correlation between marine aerosol optical properties and wind speed by providing vertical information and demonstrating that their relationships are more complex than a linear or exponential relation. [ABSTRACT FROM AUTHOR]

Airborne dust aerosols impact negatively the climate, ecosystems, air quality, and human health. To mitigate these impacts, it is crucial to identify their three–dimensional spatiotemporal distribution, transport pathways and driving factors. In this study, the three–dimensional spatiotemporal variations and distribution of dust aerosols in China from 2007 to 2021 were first analyzed using multiple dust datasets, including Modern Era Retrospective Analysis for Research and Applications version 2 (MERRA–2) dust aerosol optical depth (DAOD) data, ultraviolet aerosol index (UVAI) data from the Ozone Monitoring Instrument (OMI), and the Vertical Feature Mask (VFM) product of Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP). Also, the transport pathways and potential source regions for dust haze in principle provincial capital cities of West and North China in spring were identified using the Hybrid Single–Particle Lagrangian Integrated Trajectory (HYSPLIT) model and Potential Source Contribution Function (PSCF). Additionally, DAOD variations over different land cover types and the impacts of meteorological driving factors were discussed with geographic detectors. Results indicate that: (1) The multi–year average of DAOD in China from 2007 to 2021 was 0.076. A mutation in annual average DAOD occurred between 2010 and 2011, with an insignificant increasing trend between 2007–2010, a downward trend between 2011–2021 and a significant downward trend between 2014–2017. (2) The Taklamakan Desert exhibited the highest DAOD for the entire China during spring throughout the years, with DAOD values ranging from 0.4 to 0.6 and UVAI values exceeding 2.0. The highest frequency of dust occurrence in the northwest and northern regions is at an altitude of 2–4 km in spring and summer, and of 0–2 km in autumn and winter, while it is at an altitude of 4–6 km for the Qinghai–Tibet region. (3) The dust transport routes for the provincial capital cities can be primarily divided into: western, northwestern, northern, southwestern, and local. Northwest cities are notably affected by dust from surrounding deserts. Dust originating from the Qaidam Basin and the Hexi Corridor can be carried further downwind to inland cities, such as Xining and Lanzhou. A dust backflow was found in Beijing and Tianjin. Moreover, the discussion revealed that barren and cropland had the highest DAOD and additionally precipitation, evaporation, and soil moisture were identified as the strongest driving factors affecting dust aerosol variations. The combination effect of precipitation and temperature had the highest explanatory power, ranging from 0.72–0.84, followed by 0.75–0.81 for precipitation and U10m wind speed and 0.67–0.75 for temperature and evaporation. [ABSTRACT FROM AUTHOR]

More than 2 decades ago, aerosol remote sensing underwent a revolution with the launch of the Terra and Aqua satellites. Advancement continued via additional launches carrying new passive and active sensors. Capable of retrieving parameters characterizing aerosol loading, rudimentary particle properties and in some cases aerosol layer height, the satellite view of Earth's aerosol system came into focus. The modeling communities have made similar advances. Now the efforts have continued long enough that we can see developing trends in both the remote sensing and modeling communities, allowing us to speculate about the future and how the community will approach aerosol remote sensing 20 years from now. We anticipate technology that will replace today's standard multi-wavelength radiometers with hyperspectral and/or polarimetry, all viewing at multiple angles. These will be supported by advanced active sensors with the ability to measure profiles of aerosol extinction in addition to backscatter. The result will be greater insight into aerosol particle properties. Algorithms will move from being primarily physically based to include an increasing degree of machine-learning methods, but physically based techniques will not go extinct. However, the practice of applying algorithms to a single sensor will be in decline. Retrieval algorithms will encompass multiple sensors and all available ground measurements in a unifying framework, and these inverted products will be ingested directly into assimilation systems, becoming "cyborgs": half observations, half model. In 20 years we will see a true democratization in space with nations large and small, private organizations, and commercial entities of all sizes launching space sensors. With this increasing number of data and aerosol products available, there will be a lot of bad data. User communities will organize to set standards, and the large national space agencies will lead the effort to maintain quality by deploying and maintaining validation ground networks and focused field experiments. Through it all, interest will remain high in the global aerosol system and how that system affects climate, clouds, precipitation and dynamics, air quality, the environment and public health, transport of pathogens and fertilization of ecosystems, and how these processes are adapting to a changing climate. [ABSTRACT FROM AUTHOR]

We investigated long-term changes using a harmonised 22-year data set of aerosol light absorption measurements, in conjunction with air mass history and aerosol source analysis. The measurements were performed at Zeppelin Observatory, Svalbard, from 2002 to 2023. We report a statistically significant decreasing long-term trend for the light absorption coefficient. However, the last 8 years of 2016–2023 showed a slight increase in the magnitude of the light absorption coefficient for the Arctic haze season. In addition, we observed an increasing trend in the single-scattering albedo from 2002 to 2023. Five distinct source regions, representing different transport pathways, were identified. The trends involving air masses from the five regions showed decreasing absorption coefficients, except for the air masses from Eurasia. We show that the changes in the occurrences of each transport pathway cannot explain the reductions in the absorption coefficient observed at the Zeppelin station. An increase in contributions of air masses from more marine regions, with lower absorption coefficients, is compensated for by an influence from high-emission regions. The proportion of air masses en route to Zeppelin, which have been influenced by active fires, has undergone a noticeable increase starting in 2015. However, this increase has not impacted the long-term trends in the concentration of light-absorbing aerosol. Along with aerosol optical properties, we also show an increasing trend in accumulated surface precipitation experienced by air masses en route to the Zeppelin Observatory. We argue that the increase in precipitation, as experienced by air masses arriving at the station, can explain a quarter of the long-term reduction in the light absorption coefficient. We emphasise that meteorological conditions en route to the Zeppelin Observatory are critical for understanding the observed trends. [ABSTRACT FROM AUTHOR]

Retrieval of aerosol properties near clouds from passive remote sensing is challenging. Sunlight scattered by clouds into nearby clear regions can effectively enhance the clear area reflectance. These cloud 3D radiative effects may lead to large biases in aerosol retrievals if uncorrected, risking the incorrect interpretation of satellite observations for aerosol-cloud interaction in a cloudy atmosphere. In earlier studies, we developed a simple two-layer model (2LM) to estimate the cloud-induced clear-sky radiance enhancements in cloud fields. In this study, we take advantage of CALIPSO lidar observations, which should not be affected by the 3D radiative effect, to study passive aerosol retrievals in cloud fields in the Amazon region, specifically those produced by the operational Dark Target algorithm applied to Aqua-MODIS. From 2 years' worth of co-located CALIPSO/MODIS aerosol retrievals, we find a larger increase in operationally retrieved MODIS AOD from clear to cloudy regions (~0.075 or ~40%) than for the CALIPSO AOD (~0.021 or ~20%). The much larger increase in MODIS AOD is mainly due to the 3D radiative effects. After using the 2LM model to account for cloud 3D radiative effects, the clear to cloudy increase in MODIS AOD was reduced to ~0.043 (~23%), which is much closer to CALIPSO observations. The 3D corrected average MODIS AOD for cloudy conditions is significantly larger than AOD for clear conditions, even for cloud fraction (CF) less than 0.1, suggesting aerosols in cloudy conditions are characteristically different from aerosols in clear conditions. Furthermore, the 3D correction of AOD (i.e., τ1D - τ3D) increases linearly with CF for a large range of CF. We have also examined the impact of the 3D effect on aerosol Ångström Exponent (AE) and fine model fraction (FMF) of AOD. We found that the uncorrected average AE and FMF depend strongly on CF, ~25% increase in AE (decrease in particle size) and ~60% increase in FMF as CF increases from 0.05 to 0.45. The 3D correction leads to smaller average AE (bigger particle size) and FMF that are almost independent of CF. Thus, the 3D corrected aerosol properties are expected to provide more accurate information for better understanding aerosol-cloud interactions. [ABSTRACT FROM AUTHOR]

The south-central interior of Andalusia experiences intricate precipitation patterns as a result of its semi-arid Mediterranean climate and the impact of Saharan dust and human-made pollutants. The primary aim of this study is to monitor the inter-relations between various factors, such as aerosols, clouds, and meteorological variables, and precipitation systems in Granada using ground-based remote sensing and in situ instruments including a microwave radiometer, ceilometer, cloud radar, nephelometer, and weather station. Over an 11-year period, we detected rain events using a physical retrieval method that employed microwave radiometer measurements. A composite analysis was applied to them to construct a climatology of the temporal evolution of precipitation. It was found that convective rain is the dominant precipitation type in Granada, accounting for 68 % of the rain events. The height of the cloud base is mainly distributed at an altitude of 2 to 7 km. Integrated water vapor (IWV) and integrated cloud liquid water (ILW) increase rapidly before the onset of rain. Aerosol scattering at the surface level and hence the aerosol concentration are reduced during rain, and the predominant mean size distribution of aerosol particles before, during, and after rain is almost the same. A meteorological environment favorable for virga formation is observed in Granada. The surface weather station detected rainfall later than the microwave radiometer, indicating virga according to ceilometer and cloud radar data. We used 889 rain-day events identified by weather station data to determine precipitation intensity classes and found that light rain is the main precipitation intensity class in Granada, accounting for 72 % of the rain-day events. This can be a result of the high tropospheric temperature induced by the Andalusian climate and the reduction of cloud droplet size by the high availability of aerosol particles in the urban atmosphere. This study provides evidence that aerosols, clouds, and meteorological variables have a combined impact on precipitation which can be considered for water resource management and improving rain forecasting accuracy. [ABSTRACT FROM AUTHOR]

The vertical distribution of biomass burning aerosol (BBA) is important in regulating their impacts on weather and climate. The plume‐rise process affects the injection height of BBA and interacts with the air parcel lifting and cloud processes. However, these processes are not represented in most global climate models. In this study, we replaced the fixed vertical profiles of monthly BBA emissions in the Department of Energy's Energy Exascale Earth System Model version 1 (E3SMv1) with an interactive fire plume‐rise model. The vertical distribution of BBA emissions was calculated as a function of ambient thermodynamic conditions from the host E3SMv1, with distributions of fire sizes and sensible heat fluxes derived from the observations. The maximum fire radiative power (FRP) technique was used to determine the fire size. Scaling‐FRP technique is used to calculate the wildfire heat release. Daily BBA emission, superimposed with a fire diurnal cycle retrieved from the satellite observation, was included in model simulations. The model shows improved agreement with satellite retrievals and in situ measurement during the National Oceanic and Atmospheric Administration Wildfire Experiment for Cloud chemistry, Aerosol absorption, and Nitrogen campaign. The model‐observation comparison demonstrates the importance of the plume‐rise model and fire diurnal cycle assumption in determining the BBA fields. We also find that E3SMv1 with new features produces a larger carbonaceous aerosol burden, leading to 0.13 W m−2 warming at the top of atmosphere compared to the default E3SMv1. This highlights the importance of accurately representing the BBA injection height and indicates a no‐linear nature in the BBA‐induced radiative effect. Plain Language Summary: In this study, we replaced fixed vertical profiles of biomass burning aerosols (BBA) used in the default doe's Energy Exascale Earth System Model version 1 (E3SMv1) with an interactive fire plume‐rise model and fire diurnal cycle assumption. The BBA vertical profiles predicted by the model with the new features are in better agreement with the satellite observations and in situ aircraft observations compared to the default version. In addition, the inclusion of the plume‐rise model and fire diurnal assumption also lead to a warming effect as strong as 0.13 W m−2. Key Points: We incorporate an interactive fire plume‐rise model and fire diurnal cycle in the Energy Exascale Earth System Model version 1 (E3SMv1)The new features in E3SMv1 generate biomass burning aerosol vertical profiles that agree better with the observations than the default onesThe E3SMv1 with plume‐rise model and fire diurnal cycle causes a 0.13 W m−2 warming effect compared to the default one [ABSTRACT FROM AUTHOR]

In order to conduct accurate aerosol retrieval over snow, the Remote Sensing of Trace Gases and Aerosol Products (RemoTAP) algorithm developed by SRON Netherlands Institute for Space Research is extended with a bi-directional reflection distribution function (BRDF) for snow surfaces. The capability of the extended algorithm is validated with both synthetic measurements and real satellite measurements from the Polarization & Anisotropy of Reflectances for Atmospheric Sciences coupled with Observations from a Lidar (PARASOL), and a comparison has been made to retrievals with the baseline RemoTAP (without a snow kernel). For retrievals with real PARASOL observations, we use pixels over Aerosol Robotic Network (AERONET) stations for validation and we use the MODIS snow cover products to identify pixels over snow. We evaluate the retrieved aerosol optical thickness (AOT) at 550 nm (τ550) , single-scattering albedo (SSA) at 550 nm (ω550) and Ångström exponent (AE) for 440–870 nm (AE440-870). The experiments with both synthetic and real data show that the extended RemoTAP maintains capability for snow-free pixels and has obvious advantages in accuracy and the fraction of successful retrievals for retrieval over snow, especially over surfaces with snow cover >75 %. According to the real-data experiment, we find that the retrieval algorithm has difficulty in fitting the PARASOL 1020 nm band, where snow reflectance is significantly lower than that for the visible bands. When we perform a four-band retrieval (490, 565, 670, 865 nm) with the extended RemoTAP, we obtain a good retrieval result for τ550 , ω550 and AE440-870. Therefore, the four-band retrieval with the extended RemoTAP is recommended for aerosol retrieval over snow. [ABSTRACT FROM AUTHOR]

Atmospheric aerosols affect the Earth's climate in many ways, including acting as the seeds on which cloud droplets form. Since a large fraction of these particles is anthropogenic, the clouds' microphysical and radiative characteristics are influenced by human activity on a global scale leading to important climatic effects. The respective change in the energy budget at the top of the atmosphere is defined as the effective radiative forcing due to aerosol‐cloud interaction (ERFaci). It is estimated that the ERFaci offsets presently nearly 1/4 of the greenhouse‐induced warming, but the uncertainty is within a factor of two. A common method to calculate the ERFaci is by the multiplication of the susceptibility of the cloud radiative effect to changes in aerosols by the anthropogenic change of the aerosol concentration. This has to be done by integrating it over all cloud regimes. Here we review the various methods of the ERFaci estimation. Global measurements require satellites' global coverage. The challenge of quantifying aerosol amounts in cloudy atmospheres are met with the rapid development of novel methodologies reviewed here. The aerosol characteristics can be retrieved from space based on their optical properties, including polarization. The concentrations of the aerosols that serve as cloud drop condensation nuclei can be also estimated from their impact on the satellite‐retrieved cloud drop number concentrations. These observations are critical for reducing the uncertainty in the ERFaci calculated from global climate models (GCMs), but further development is required to allow GCMs to properly simulate and benefit these novel observables. Plain Language Summary: Aerosols affect the climate in many ways, including serving as the basis for the formation of cloud droplets. Therefore, aerosols have profound impacts on clouds and through that on the Earth's energy budget. Increasing aerosols leads to additional cloud droplets, changing cloud properties such that they reflect more solar radiation back to space and offset nearly 1/4 of the warming induced by greenhouse gases, but with a large uncertainty within a factor of two. Here we review the ways by which aerosols and their radiative effects are retrieved from space. A major challenge is to reduce the uncertainty by better retrieval methods of atmospheric aerosol and cloud properties. This challenge is met by rapid satellite retrieval methodological developments and numerous new satellite missions, which are described here. These new methodologies have to be matched with parallel development in the global circulation models for the improved estimation of the actual climatic impacts. Key Points: Calculating the susceptibility of clouds to aerosols has to include the cleanest conditions where measuring the aerosols is challengingThe definition and use of regimes to group clouds with similar responses to aerosol is vital for future observation‐based effective radiative forcing due to aerosol‐cloud interaction (ERFaci) estimatesNew observational tools are vital for reducing ERFaci uncertainty but require further global climate model development to simulate these novel observables [ABSTRACT FROM AUTHOR]

The all‐sky Aerosol Direct Radiative Effect (ADRE) varies considerably among global climate models (GCMs), which results from differences in aerosol and atmospheric states and ADRE sensitivity to aerosol‐related radiative processes. This study uses a regression method to analyze the inter‐model spread of ADRE among the GCMs of the Sixth Coupled Model Intercomparison Projects (CMIP6). The key state variables examined include scattering and absorbing aerosol optical depth, surface albedo, and shortwave cloud radiative effect. We find that differences in state variables and radiative sensitivity explain 67% and 17%, respectively, of the global ADRE anomaly. The ADRE anomaly in different models is dominated by different factors, which sometimes leads to compensating effects. For the global mean ADRE anomaly, aerosol optical depth differences dominate in CNRM‐ESM2‐1 and GFDL‐ESM4 models, while ADRE sensitivity variations to aerosol‐only scattering effect dominate in HadGEM3‐GC31‐LL, MPI‐ESM‐1‐2‐HAM, and MRI‐ESM2‐0 models. Plain Language Summary: Aerosols scatter and absorb solar radiation, impacting the Earth's climate. Global climate models differ in their quantification of this effect. The differences in quantification arise from different state variables, including the aerosol properties and atmospheric conditions. Additionally, the radiative sensitivity of aerosol effect to aerosol‐related physical processes varies with models. In this study, we identify the primary causes of the differences in aerosol radiative effect among climate models and quantify their respective impacts by using a regression method. We find that besides the aerosol optical depth, whose influence on aerosol radiative effect is well recognized, the radiative sensitivity of aerosol and surface interactions significantly contributes to the aerosol radiative effect differences in the latest climate models. Key Points: A regression model is used to dissect the inter‐model spread of the all‐sky Aerosol Direct Radiative Effect (ADRE) in Sixth Coupled Model Intercomparison Projects ModelsThe model explains 86% of ADRE inter‐model spread, with variances in state‐variable and radiative sensitivity contributing 67% and 17% eachDifferences in aerosol optical depth and ADRE sensitivity to aerosol‐surface interactions drive the spatial variance in global ADRE spread [ABSTRACT FROM AUTHOR]

The extinction-to-backscattering ratio, popularly known as lidar (light detection and ranging) ratio of atmospheric aerosols is an important optical property, which is essential to retrieve the extinction profiles of atmospheric aerosols. Lidar satellite observations can provide the global coverage of atmospheric aerosols along with their vertical extent. NASA's Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) on board the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite is the only space-based platform available, so far, that provides the vertical profiles of extinction due to atmospheric aerosols. A physics-based theoretical approach is presented in the present paper that estimates lidar ratio values for CALIPSO aerosol models, which can be used as inputs to determine the extinction profiles of aerosols using CALIPSO data. The developed methodology was also qualified by comparing it with the lidar ratio values derived using AERONET (AErosol RObotic NETwork) datasets. Lidar ratio values for CALIPSO aerosol models were estimated in the range of 38.72 to 85.98 sr at 532 nm, whereas at 1064 nm lidar ratio varied between 20.11 to 71.11 sr depending upon the aerosol type and their size distributions. Aerosols are compositions of various particles; thus, the presence of water vapour in the atmosphere can affect the optical properties of the aerosols. Thus, the effect of relative humidity on lidar ratio was studied using Optical Properties of Aerosols and Clouds (OPAC) aerosol models, which are the standard aerosol models against the cluster-classified AERONET and CALIPSO aerosol models. Water-soluble particles contribute substantially in clean continental, clean marine, tropical marine and desert aerosol models and are hygroscopic in nature. Hygroscopic sulfate particles dominate the Antarctic aerosols during summertime. In the presence of relative humidity between 0 %–80 %, the lidar ratio values were observed to decrease from 53.59 to 47.13, from 53.66 to 47.15, from 53.70 to 47.16, and from 55.32 to 48.78 sr at 532 nm for clean continental, clean marine, tropical marine, and desert aerosols, respectively, whereas lidar ratio gradually increased from 47.13 to 51, from 47.15 to 51, from 47.16 to 51, and from 48.78 to 51.68 sr, respectively, for these aerosol models when relative humidity was between 80 %–99 %, due to constituent hygroscopic particles. In the case of Antarctic aerosols, the lidar ratio was observed to increase from 57.73 to 97.64 sr due to hygroscopic sulfate particles that backscattered heavily in the presence of water vapour at 532 nm. The soot particles dominate the polluted continental and polluted marine particles, causing an increase in lidar ratio over its corresponding clean counterpart. Similar results were observed at 1064 nm for OPAC aerosol models. [ABSTRACT FROM AUTHOR]

Mixing state and density are two key parameters of aerosol particles affecting their impacts on radiative forcing and human health. Here a single-particle aerosol mass spectrometer in tandem with a differential mobility analyzer and an aerodynamic aerosol classifier was deployed during the Beijing 2022 Olympic Winter Games (OWG) to investigate the impacts of emission controls on particle mixing state and density. Our results show the dominance of carbonaceous particles comprising mainly total elemental carbon (Total-EC, 13.4 %), total organic carbon (Total-OC, 10.5 %) and Total-ECOC (47.1 %). Particularly, the particles containing organic carbon and sulfate were enhanced significantly during OWG, although those from primary emissions decreased. The composition of carbonaceous particles also changed significantly which was characterized by the decreases in EC mixed with nitrate and sulfate (EC-NS), EC mixed with potassium nitrate (KEC-N), and amine-containing particles and increase in ECOC mixed with nitrate and sulfate (ECOC-NS). This result indicates that emission controls during OWG reduced the mixing of EC with inorganic aerosol species and amines yet increased the mixing of EC with organic aerosol. The average effective density (ρeff) of aerosol particles (150–300 nm) was 1.15 g cm -3 during the non-Olympic Winter Games (nOWG), with higher values during OWG (1.26 g cm -3) due to the increase in secondary particle contribution. In addition, the ρeff of most particles increased with the increases in pollution levels and relative humidity, yet they varied differently for different types of particles, highlighting the impacts of aging and formation processes on the changes of particle density and mixing state. [ABSTRACT FROM AUTHOR]

Future change in sea surface temperature may influence climate via various air–sea feedbacks and pathways. In this study, we investigate the influence of surface seawater biogeochemical composition on the temperature dependence of number-based sea spray emission fluxes. The dependence of sea spray fluxes was investigated in different water masses (i.e., subantarctic, subtropical and frontal bloom) with contrasting biogeochemical properties across a temperature range from ambient (13–18 ∘ C) to 2 ∘ C using seawater circulating in a plunging jet sea spray generator. We observed a significant increase in the sea spray total concentration at temperatures below 8 ∘ C. Specifically, at 2 ∘ C, there was an average 4-fold increase compared to the initial concentration at ambient temperatures. This temperature dependence was more pronounced for smaller-sized sea spray particles (i.e., nucleation and Aitken modes). Moreover, the temperature dependence varied based on the seawater type and its biogeochemical properties. While the sea spray flux at moderate temperatures (8–11 ∘ C) was highest in frontal-bloom waters, the effect of low temperature on the sea spray flux was highest in subtropical seawaters. The temperature dependence of the sea spray flux was found to be inversely proportional to the abundance of the cyanobacterium Synechococcus in seawater. This relationship allows for parameterizing the temperature dependence of sea spray emission fluxes based on Synechococcus, which may be utilized in future modeling exercises. [ABSTRACT FROM AUTHOR]

Cyclones are expected to increase the vertical transport of sea spray aerosols (SSAs), which may significantly impact the climate by increasing the population of cloud condensation nuclei (CCN) and the cloud droplet number concentration (Nd). In this study, a high-time-resolution (1 h) aerosol monitoring was carried out in the middle and high Southern Hemisphere from 23 February to 4 March 2018. The characteristics of SSAs during three cyclones were observed during the cruise. The results showed that SSA level in the low atmosphere did not increase with the wind speed during cyclone processes, which was different from the anticipated scenario that SSA concentration would increase with wind speed. However, the size of SSA particles during cyclones was larger than that in the no-cyclone periods. It seems that the generation of SSAs was enhanced during cyclones, but SSA concentration near the sea surface increased scarcely. The upward-transport proportion was calculated according to the wind stress and sea salt flux between cyclone and non-cyclone periods. It indicated that more than 23.4 % of the SSAs were transported upwards by cyclone processes during event 1, and 36.2 % and 38.9 % were transported upwards in event 2 and event 3, respectively. The upward transport of SSAs was the main reason why SSA concentration did not increase in the low atmosphere. The transport of SSAs to the high atmosphere during cyclones may additionally increase the CCN burden in the marine boundary layer, which may affect the regional climate. This study highlights the importance of SSA transport to the high atmosphere by cyclones and extends the knowledge of SSA generation and the impact factor during the cyclone period in marine atmosphere. [ABSTRACT FROM AUTHOR]

The Radiative Forcing Model Intercomparison Project (RFMIP) allows estimates of effective radiative forcing (ERF) in the Coupled Model Intercomparison Project phase six (CMIP6). We analyze the RFMIP output, including the new experiments from models that use the same parameterization for anthropogenic aerosols (RFMIP‐SpAer), to characterize and better understand model differences in aerosol ERF. We find little changes in the aerosol ERF for 1970–2014 in the CMIP6 multi‐model mean, which implies greenhouse gases primarily explain the positive trend in the total anthropogenic ERF. Cloud‐mediated effects dominate the present‐day aerosol ERF in most models. The results highlight a regional increase in marine cloudiness due to aerosols, despite suppressed cloud lifetime effects in that RFMIP‐SpAer experiment. Negative cloud‐mediated effects mask positive direct effects in many models, which arise from strong anthropogenic aerosol absorption. The findings suggest opportunities to better constrain simulated ERF by revisiting the optical properties and long‐range transport of aerosols. Plain Language Summary: Aerosols are particles in the atmosphere with sizes ranging from nanometers to tens of micrometers, which are emitted by natural and anthropogenic processes or formed from gases in the atmosphere. The extent to which anthropogenic aerosols affect the radiation budget of Earth is important to better understand anthropogenic climate changes. Aerosol effects on the radiation budget are simulated by complex Earth system models that informed the Sixth Assessment Report of the Intergovernmental Panel on Climate Change. Our study addresses why such model experiments show different magnitudes for aerosol radiative effects. The results point to opportunities to further improve models with existing observations of aerosol optical properties and aerosol transport over oceans in addition to the much‐studied aerosol effects on clouds. Key Points: Coupled Model Intercomparison Project phase six (CMIP6) averaged trend in aerosol effective radiative forcing (ERF) is small for 1970–2014 and weakly positive for 2000–2014Positive direct aerosol radiative effects in CMIP6 models are associated with strong aerosol absorptionDiverse and often strong cloud‐mediated effects primarily determine the magnitude of aerosol ERF in CMIP6 [ABSTRACT FROM AUTHOR]

Between April 2002 and June 2017, the Global Monitoring Laboratory (GML) of the National Oceanic and Atmospheric Administration (NOAA) made continuous measurements of a suite of in situ aerosol optical properties at a long-term monitoring site near Trinidad Head (THD), California. In addition to aerosol optical properties, between 2002–2006 a scanning humidograph system was operated, and inorganic ion and total aerosol mass concentrations were obtained from filter measurements. A combined analysis of these datasets demonstrates consistent patterns in aerosol climatology and highlights changes in sources throughout the year. THD is predictably dominated by sea salt aerosols; however, marine biogenic aerosols are the largest contributor to PM 1 in the warmer months. Additionally, a persistent combustion source appears in the winter, likely a result of wintertime home heating. While the influences of local anthropogenic sources from vehicular and marine traffic are visible in the optical aerosol data, their influence is largely dictated by the wind direction at the site. Comparison of the THD aerosol climatology to that reported for other marine sites shows that the location is representative of clean marine measurements, even with the periodic influence of anthropogenic sources. [ABSTRACT FROM AUTHOR]

For the observation of the global three-dimensional distribution of aerosol composition and the evaluation of the shortwave direct radiative effect (SDRE) by aerosols, we developed a retrieval algorithm that uses observation data from the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) on board the Cloud–Aerosol Lidar Infrared Pathfinder Satellite Observations (CALIPSO) satellite and the Moderate Resolution Imaging Spectroradiometer (MODIS) on board Aqua. The CALIOP–MODIS retrieval optimizes the aerosol composition to both the CALIOP and MODIS observations in the daytime. Aerosols were assumed to be composed of four aerosol components: water-soluble (WS), light-absorbing (LA), dust (DS), and sea salt (SS) particles. The outputs of the CALIOP–MODIS retrieval are the vertical profiles of the extinction coefficient (αa), single-scattering albedo (ω0), asymmetry factor (g) of total aerosols (WS + LA + DS + SS), and αa of WS, LA, DS, and SS. Daytime observations of CALIOP and MODIS in 2010 were analyzed by the CALIOP–MODIS retrieval. The global means of the aerosol optical depth (τa) at 532 nm were 0.147±0.148 for total aerosols, 0.072±0.085 for WS, 0.027±0.035 for LA, 0.025±0.054 for DS, and 0.023±0.020 for SS. τa of the CALIOP–MODIS retrieval was between those of the CALIPSO and MODIS standard products and was close to the MODIS standard product. The global means of ω0 and g were 0.940±0.038 and 0.718±0.037 ; these values are in the range of those reported by previous studies. The horizontal distribution of each aerosol component was reasonable; for example, DS was large in desert regions, and LA was large in the major regions of biomass burning and anthropogenic aerosol emissions. The values of τa , ω0 , g , and fine and coarse median radii of the CALIOP–MODIS retrieval were compared with those of the AERONET products. τa at 532 and 1064 nm of the CALIOP–MODIS retrieval agreed well with the AERONET products. The ω0 , g , and fine and coarse median radii of the CALIOP–MODIS retrieval were not far from those of the AERONET products, but the variations were large, and the coefficients of determination for linear regression between them were small. In the retrieval results for 2010, the clear-sky SDRE values for total aerosols at the top and bottom of the atmosphere were -4.99±3.42 and -13.10±9.93 W m -2 , respectively, and the impact of total aerosols on the heating rate was from 0.0 to 0.5 K d -1. These results are generally similar to those of previous studies, but the SDRE at the bottom of the atmosphere is larger than that reported previously. Consequently, comparison with previous studies showed that the CALIOP–MODIS retrieval results were reasonable with respect to aerosol composition, optical properties, and the SDRE. [ABSTRACT FROM AUTHOR]

The NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) produced a unique dataset for research into aerosol–cloud–meteorology interactions, with applications extending from process-based studies to multi-scale model intercomparison and improvement as well as to remote-sensing algorithm assessments and advancements. ACTIVATE used two NASA Langley Research Center aircraft, a HU-25 Falcon and King Air, to conduct systematic and spatially coordinated flights over the northwest Atlantic Ocean, resulting in 162 joint flights and 17 other single-aircraft flights between 2020 and 2022 across all seasons. Data cover 574 and 592 cumulative flights hours for the HU-25 Falcon and King Air, respectively. The HU-25 Falcon conducted profiling at different level legs below, in, and just above boundary layer clouds (< 3 km) and obtained in situ measurements of trace gases, aerosol particles, clouds, and atmospheric state parameters. Under cloud-free conditions, the HU-25 Falcon similarly conducted profiling at different level legs within and immediately above the boundary layer. The King Air (the high-flying aircraft) flew at approximately ∼ 9 km and conducted remote sensing with a lidar and polarimeter while also launching dropsondes (785 in total). Collectively, simultaneous data from both aircraft help to characterize the same vertical column of the atmosphere. In addition to individual instrument files, data from the HU-25 Falcon aircraft are combined into "merge files" on the publicly available data archive that are created at different time resolutions of interest (e.g., 1, 5, 10, 15, 30, 60 s, or matching an individual data product's start and stop times). This paper describes the ACTIVATE flight strategy, instrument and complementary dataset products, data access and usage details, and data application notes. The data are publicly accessible through 10.5067/SUBORBITAL/ACTIVATE/DATA001 (ACTIVATE Science Team, 2020). [ABSTRACT FROM AUTHOR]

Estimation of aerosol radiative forcing continues to suffer from large uncertainties, partially from a lack of observations of aerosol optical properties. Limited measurements of the atmospheric aerosol imaginary refractive index (iRI) have been made, especially in some of the world's most polluted regions. In this study, we measured aerosol optical and micro‐physical properties at a regional site, Rohtak, India, representative of polluted cities in the Indo‐Gangetic plains in northern India. The average PM2.5 measured during the campaign was 163 μg/m3 with a single‐scatter albedo of 0.7, indicating the presence of strongly absorbing aerosol components. Measurements of aerosol absorption, scattering, and particle number size distributions were used to estimate the effective refractive index using an established Mie inversion technique. The calculated iRI was spectrally invariant in the visible region with values ranging between 0.076 and 0.145. Brown carbon absorption, estimated using an existing Mie optimization method, ranged 34–88 Mm−1, with strongly absorbing mass absorption cross‐sections (∼1.9 m2/g). Higher iRI were observed during periods with higher brown carbon absorption, which are likely directly emitted from combustion sources. Low volatility organic carbon fractions dominated during these periods, with likely persistence of atmospheric absorption. The iRI values are at the upper end of previously reported ranges of urban aerosol iRI. In a sensitivity analysis to measured parameters, the absorption had the dominant effect on estimated iRI. Measured single scatter albedos, were lower than those from climate model simulations over the region, demonstrating the need for intrinsic property measurements to evaluate and constrain climate models. Plain Language Summary: Particles in the atmosphere, called aerosol, can absorb or reflect/scatter sunlight to heat or cool the atmosphere, depending upon their physical and chemical properties. Climate models try to simulate these properties to understand their effect on the climate. The strength of the absorption is determined by the size of the particle (generally the diameter) and its refractive index (a complex number) which is a material property. In this study, we measure the refractive index of atmospheric aerosol at Rohtak, which lies in the highly polluted Indo‐Gangetic plains in India. We find that the aerosol are very absorbing in nature, that is, they are warming the atmosphere, and that the absorbing/imaginary part of the refractive index is in the higher range of previously reported values. The aerosol at the site are dominated by emissions from fossil fuel and biomass burning sources. On comparing these absorbing properties with those simulated by climate models, we find that the climate models are not able to simulate the absorbing nature of these aerosol well. Hence, there is a need for more such measurements of the aerosol refractive index to improve climate models and ultimately improve our understanding of the effect of aerosol on our climate. Key Points: Estimate the aerosol effective refractive index (RI); imaginary RI ranges 0.076–0.145, higher than previously reported valuesA single scatter albedo of 0.7 reveals strongly absorbing components, with brown carbon absorption of 34–88 Mm−1Imaginary RI correlates well with near‐UV absorption by brown carbon, which has low volatility and is likely emitted from combustion sources [ABSTRACT FROM AUTHOR]

By utilizing Level 2A products (particle optical properties and numerical weather prediction data) and Level 2C products (numerical weather prediction wind vector assimilated with observed wind component) provided by the Atmospheric Laser Doppler Instrument (ALADIN) onboard the Aeolus mission, and Level 2 vertical feature mask (VFM) products provided by Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) onboard Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission, three remote ocean areas are selected and the optical properties at 355 nm of marine aerosol are derived. The combined analysis of marine aerosol optical properties at 355 nm and instantaneous co-located wind speeds above the remote ocean areas are conducted. Eventually their relationships are explored and discussed at two sperate vertical atmospheric layers (0–1 km and 1–2 km, correspond to the heights within and above marine atmospheric boundary layer (MABL)), revealing the marine aerosol related atmospheric background states. Pure marine aerosol optical properties at 355 nm are obtained after quality control, cloud screening and backscatter coefficient correction from the ALADIN observations. The spatial distributions of marine aerosol optical properties and wind speed above the study areas are presented and analysed, respectively, at two vertical layers. The statistical results of the marine aerosol optical properties along with the wind speed grids at two vertical layers together with the corresponding regression curves fitted by power law functions are acquired and analysed, for each remote ocean area. The optical properties present increasing trends with wind speed in all cases, implying that the atmosphere of the two vertical layers will both receive the marine aerosol input produced and transported by the wind and the turbulence. The marine aerosol enhancement caused by the wind speed at the lower layer is more intensive than at the higher layer. As derived data from ALADIN, the averaged marine aerosol optical depth (AODmar) and the averaged marine aerosol lidar ratio (LRmar) at 355 nm are acquired and discussed along the wind speed range. The marine aerosol optical properties distributions, wind speed bins, and the marine aerosol variation tendencies along wind speed above the individual study areas are not totally similar, implying that the development and evolution of the marine aerosol above the ocean might not only be dominated by the drive of the wind, but also be impacted by other meteorological and environmental factors, e.g., atmospheric stability, sea and air temperature, or relative humidity. Combined analysis on the aerosol optical properties and wind with additional atmospheric parameters above the ocean might be capable to provide more detailed information of marine aerosol production, entrainment, transport and removal. [ABSTRACT FROM AUTHOR]

Reliable observations of aerosol optical properties are crucial for quantifying the radiative forcing of climate. The simultaneous measurements of aerosol optical properties at three wavelengths for PM 1 and PM 10 were conducted in urban Beijing from March 2018 to February 2022. The aerosol absorption coefficient (σab) at 550 nm of PM 10 and PM 1 decreased by 55.0 % and 53.5 % from 2018 to 2021. The significant reduction in σab may be related to reduced primary emissions caused by effective air pollution control measures. PM 2.5 mass concentration decreased by 34.4 % from 2018 to 2021. Single scattering albedo (SSA) increased from 0.89±0.04 for PM 10 (0.87±0.05 for PM 1) in 2018 to 0.93±0.03 for PM 10 (0.91±0.04 for PM 1) in 2021. Increasing SSA and decreasing PM 2.5 mass concentration suggest that the fraction of absorbing aerosols decreased with improved air quality due to pollution control measures being taken. The annual average submicron absorption ratio (Rab) increased from 86.1 % in 2018 to 89.2 % in 2021, suggesting that fine particles are the main contributors to total PM 10 absorption and that the contribution of fine particles to absorption became more important. The absorption Ångström exponent (AAE) in winter decreased from 2018 to 2021, implying a decreasing contribution from brown carbon to light absorption, which may relate to the reduced emissions of biomass burning and coal combustion. During the study period, aerosol radiative forcing efficiency became more negative, mainly influenced by increasing SSA and was -27.0 and -26.2 W m -2 per aerosol optical depth (AOD) for PM 10 and PM 1 in 2021. Higher σab and PM 2.5 mass concentrations were primarily distributed in clusters 4 and 5, transported from the south and the west of Beijing each year. σab and PM 2.5 corresponding to clusters 4 and 5 decreased evidently from 2018 to 2021, which may result from the control of source emissions in surrounding regions of Beijing. The 4-year data presented in this study provide critical optical parameters for radiative forcing assessment within two size ranges and are helpful for evaluating the effectiveness of clean air action. [ABSTRACT FROM AUTHOR]

The south-central interior of Andalusia experiences intricate precipitation patterns as a result of its semi-arid Mediterranean climate and the impact of Saharan dust and human-made pollutants. The primary aim of this study is to monitor the inter-relations between various factors, such as aerosols, clouds, and meteorological variables, and precipitation systems in Granada using ground-based remote sensing and in situ instruments including microwave radiometer, ceilometer, cloud radar, nephelometer, and weather station. The objective is to identify potential properties of precipitation in the region and in that way improve precipitation forecasting. Over an 11-year period, we detected rain events using a physical retrieval method that employed microwave radiometer measurements. A composite analysis was applied to them to construct a climatology of the temporal evolution of precipitation. It was found that convective rain is the dominant precipitation type in Granada, accounting for 68 % of the rain events. The height of the cloud base is mainly distributed at an altitude of 2 to 7 km. Integrated water vapor (IWV) and integrated cloud liquid water (ILW) increase rapidly before the onset of rain. Aerosol scattering at surface level and hence the aerosol concentration is reduced during rain, and the predominant mean size distribution of aerosol particles before, during, and after rain is almost the same. A meteorological environment favorable for virga formation is observed in Granada. The surface weather station detected rainfall later than the microwave radiometer, indicating virga according to ceilometer and cloud radar data. We used rain-day events identified by weather station data to determine precipitation intensity classes and found that light rain is the main precipitation intensity class in Granada, accounting for 72 % of the rain-day events. This can be a result of the high tropospheric temperature induced by the Andalusian climate and the reduction of cloud droplet size by the high availability of aerosol particles in the urban atmosphere. This study provides evidence that aerosols, clouds, and meteorological variables have a combined impact on precipitation which can be considered for water resource management and improving rain forecasting accuracy. [ABSTRACT FROM AUTHOR]

Aerosol over the remote southeastern Atlantic is some of the most sunlight-absorbing aerosol on the planet: the in situ free-tropospheric single-scattering albedo at the 530 nm wavelength (SSA 530nm) ranges from 0.83 to 0.89 within ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) aircraft flights from late August–September. Here we seek to explain the low SSA. The SSA depends strongly on the black carbon (BC) number fraction, which ranges from 0.15 to 0.4. Low organic aerosol (OA)-to-BC mass ratios of 8–14 and modified combustion efficiency values >0.975 point indirectly to the dry, flame-efficient combustion of primarily grass fuels, with back trajectories ending in the miombo woodlands of Angola. The youngest aerosol, aged 4–5 d since emission, occupied the top half of a 5 km thick plume sampled directly west of Angola with a vertically consistent BC:ΔCO (carbon monoxide) ratio, indicating a homogenization of the source emissions. The younger aerosol, transported more quickly off of the continent by stronger winds, overlaid older, slower-moving aerosol with a larger mean particle size and fraction of BC-containing particles. This is consistent with ongoing gas condensation and the coagulation of smaller non-BC particles upon the BC-containing particles. The particle volumes and OA:BC mass ratios of the older aerosol were smaller, attributed primarily to evaporation following fragmentation, instead of dilution or thermodynamics. The CLARIFY (CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017) aircraft campaign sampled aerosols that had traveled further to reach the more remote Ascension Island. CLARIFY reported higher BC number fractions, lower OA:BC mass ratios, and lower SSA yet larger mass absorption coefficients compared to this study's. Values from one ORACLES 2017 flight, held midway to Ascension Island, are intermediate, confirming the long-range changes. Overall the data are most consistent with continuing oxidation through fragmentation releasing aerosols that subsequently enter the gas phase, reducing the OA mass, rather than evaporation through dilution or thermodynamics. The data support the following best fit: SSA 530nm=0.801+0055⋅(OA:BC) (r=0.84). The fires of southern Africa emit approximately one-third of the world's carbon; the emitted aerosols are distinct from other regional smoke emissions, and their composition needs to be represented appropriately to realistically depict regional aerosol radiative effects. [ABSTRACT FROM AUTHOR]

The eastern North Atlantic (ENA) is a region dominated by pristine marine environment and subtropical marine boundary layer clouds. Under unperturbed atmospheric conditions, the regional aerosol regime in the ENA varies seasonally due to different seasonal surface-ocean biogenic emissions, removal processes, and meteorological regimes. However, during periods when the marine boundary layer aerosol in the ENA is impacted by particles transported from continental sources, aerosol properties within the marine boundary layer change significantly, affecting the concentration of cloud condensation nuclei (CCN). Here, we investigate the impact of long-range transported continental aerosol on the regional aerosol regime in the ENA using data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility on Graciosa Island in 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. We develop an algorithm that integrates number concentrations of particles with optical particle dry diameter (Dp) between 100 and 1000 nm, single scattering albedo, and black carbon concentration to identify multiday events (with duration >24 consecutive hours) of long-range continental aerosol transport in the ENA. In 2017, we detected nine multiday events of long-range transported particles that correspond to ∼ 7.5 % of the year. For each event, we perform HYSPLIT 10 d backward trajectories analysis, and we evaluate CALIPSO aerosol products to assess, respectively, the origins and compositions of aerosol particles arriving at the ENA site. Subsequently, we group the events into three categories, (1) mixture of dust and marine aerosols, (2) mixture of marine and polluted continental aerosols from industrialized areas, and (3) biomass burning aerosol from North America and Canada, and we evaluate their influence on aerosol population and cloud condensation nuclei in terms of potential activation fraction and concentrations at supersaturation of 0.1 % and 0.2 %. The arrival of plumes dominated by the mixture of dust and marine aerosol in the ENA in the winter caused significant increases in baseline Ntot. Simultaneously, the baseline particle size modes and CCN potential activation fraction remained almost unvaried, while cloud condensation nuclei concentrations increased proportionally to Ntot. Events dominated by a mixture of marine and polluted continental aerosols in spring, fall, and winter led to a statistically significant increase in baseline Ntot , a shift towards larger particular sizes, a higher CCN potential activation fractions, and cloud condensation nuclei concentrations of >170 % and up to 240 % higher than during baseline regime. Finally, the transported aerosol plumes characterized by elevated concentration of biomass burning aerosol from continental wildfires detected in the summertime did not statistically contribute to increase baseline aerosol particle concentrations in the ENA. However, particle diameters were larger than under baseline conditions, and CCN potential activation fractions were >75 % higher. Consequentially, cloud concentration nuclei concentrations increased by ∼ 115 % during the period affected by the biomass burning events. Our results suggest that, through the year, multiday events of long-range continental aerosol transport periodically affect the ENA and represent a significant source of CCN in the marine boundary layer. Based on our analysis, in 2017, the multiday aerosol plume transport dominated by a mixture of dust and marine aerosol, a mixture of marine and polluted continental aerosols, and biomass burning aerosols caused increases in the NCCN baseline regime of, respectively, 6.6 %, 8 %, and 7.4 % at SS 0.1 % (and, respectively, 6.5 %, 8.2 %, and 7.3 % at SS 0.2 %) in the ENA. [ABSTRACT FROM AUTHOR]

Sea salt aerosols (SSAs) often mix with organic matter via sea‐to‐air emission, photochemical oxidation, and atmospheric transport, which change particle hygroscopicity and real refractive index (RRI), thereby the radiative effects. However, the influence of water uptake and organic matters on radiative effects is not well understood. In this study, relative humidity (RH)‐dependent growth factor (GF), light scattering enhancement factor, RRI (nmea), and radiative forcing efficiency (RFE) in the visible spectrum of SSAs/malonic acid (MA) internally mixed aerosols were investigated. Our results showed that MA‐mediated SSAs readily absorbed water even at low RH but suppressed hygroscopic growth at high RH. The discrepancy between Zdanovskii‐Stokes‐Robinson predictions and measured GF indicated that the suppressing effect on size caused by produced malonate salts in chloride depletion became more evident as MA content increased. RRI in the visible spectrum decreased as MA got enriched and approached toward water's RRI at high RH, resulting in a less cooling effect. The increasing RH reduced RFE both by decreasing RRI and increasing particle size substantially. Ignoring the effect of MA on particle size and RRI under varied RH, errors in RFE at 525 nm up to 25% could be induced. Volume mixing rule performs well in predicting the RRI of mixed aerosols in dry conditions, while the retrieved difference of 0.061 between volume mixing RRI nvol and nmea would make the error in RFE up to 1.15 W·m−2·Aerosol optical depth−1 at 87% RH. Our study helps understand the impact of water content and dicarboxylic acids on the direct radiative effects of SSAs. Plain Language Summary: Sea salt aerosols often mix with organic matter during the process of generation and transportation, which changes particles' hygroscopicity and real refractive index (RRI), thereby the radiative effects. In this study, the hygroscopicity, scattering properties, RRI, and radiative forcing efficiency (RFE) in the visible spectrum of both sea salt aerosols and sea salt/malonic acid aerosols under varied relative humidity are investigated. It was found that malonic acid enhanced the water uptake of sea salt aerosols at low relative humidity but suppressed hygroscopic growth at high relative humidity. RRI of mixed aerosols decreased along with the increase in relative humidity and malonic acid content leading to a lower RFE. Ignoring the effect of malonic acid on particle size and RRI under varied relative humidity, large errors in RFE could be induced. The volume mixing rule used to calculate the RRI and thereby RFE performs well at low relative humidity but is invalid at high relative humidity. Our study helps understand the impact of water content and dicarboxylic acids on the direct radiative effects of sea slat aerosols. Key Points: The relative humidity‐dependent refractive index of submicron sea salt/malonic acid internally mixed aerosols was first retrievedThe interactions between sea salt and malonic acid are responsible for the change in water uptake and refractive indexIt is necessary to consider the impact of relative humidity on sea salt/malonic acid mixed aerosols in climate models [ABSTRACT FROM AUTHOR]

The remoteness and extreme conditions of the Southern Ocean and Antarctic region have meant that observations in this region are rare, and typically restricted to summertime during research or resupply voyages. Observations of aerosols outside of the summer season are typically limited to long-term stations, such as Kennaook / Cape Grim (KCG; 40.7 ∘ S, 144.7 ∘ E), which is situated in the northern latitudes of the Southern Ocean, and Antarctic research stations, such as the Japanese operated Syowa (SYO; 69.0 ∘ S, 39.6 ∘ E). Measurements in the midlatitudes of the Southern Ocean are important, particularly in light of recent observations that highlighted the latitudinal gradient that exists across the region in summertime. Here we present 2 years (March 2016–March 2018) of observations from Macquarie Island (MQI; 54.5 ∘ S, 159.0 ∘ E) of aerosol (condensation nuclei larger than 10 nm, CN 10) and cloud condensation nuclei (CCN at various supersaturations) concentrations. This important multi-year data set is characterised, and its features are compared with the long-term data sets from KCG and SYO together with those from recent, regionally relevant voyages. CN 10 concentrations were the highest at KCG by a factor of ∼50% across all non-winter seasons compared to the other two stations, which were similar (summer medians of 530, 426 and 468 cm-3 at KCG, MQI and SYO, respectively). In wintertime, seasonal minima at KCG and MQI were similar (142 and 152 cm-3 , respectively), with SYO being distinctly lower (87 cm-3), likely the result of the reduction in sea spray aerosol generation due to the sea ice ocean cover around the site. CN 10 seasonal maxima were observed at the stations at different times of year, with KCG and MQI exhibiting January maxima and SYO having a distinct February high. Comparison of CCN 0.5 data between KCG and MQI showed similar overall trends with summertime maxima and wintertime minima; however, KCG exhibited slightly (∼10%) higher concentrations in summer (medians of 158 and 145 cm-3 , respectively), whereas KCG showed ∼40% lower concentrations than MQI in winter (medians of 57 and 92 cm-3 , respectively). Spatial and temporal trends in the data were analysed further by contrasting data to coincident observations that occurred aboard several voyages of the RSV Aurora Australis and the RV Investigator. Results from this study are important for validating and improving our models and highlight the heterogeneity of this pristine region and the need for further long-term observations that capture the seasonal cycles. [ABSTRACT FROM AUTHOR]

The aerosol direct radiative effect (ADRE) is controlled by both aerosol distributions and environmental factors, making it interesting and important to quantitatively assess their effects on the ADRE inhomogeneity and climate trends. By analyzing the ADRE in the 21st century from a global reanalysis data set, we find that the spatial variability of the ADRE and its trends can be well explained by a linear regression model. In this model, scattering and absorbing aerosol optical depths (AODs) are used, along with critical environmental variables such as surface albedo and cloud radiative effect, as predictors. Based on this model, we find that approximately 70% of the ADRE inhomogeneity is due to the AOD distributions and the remainder is attributable to environmental factors. This study also shows that a stronger cooling effect of the scattering aerosols in the Northern Hemisphere drives northward cross‐equator meridional energy transport, although this transport exhibits a declining trend over the last two decades. The changes in surface albedo and cloud radiative effect strongly influence the trends in the regional ADRE and the meridional energy transport driven by them. In particular, the reduction of surface albedo (sea ice) is primarily responsible for the enhancement of the cooling ADRE, as well as an associated trend in meridional energy transport, in the Arctic. Plain Language Summary: Aerosols are particles produced by natural events such as volcanic eruptions and anthropogenic emissions such as fossil fuel combustion. They can scatter and absorb incoming solar radiation, leading to a strong local cooling or warming effect on the Earth's climate. The impact of aerosols on the Earth's radiative balance is known as the aerosol direct radiative effect (ADRE). Factors that can affect ADRE include the types and amounts of aerosols and the environmental conditions such as surface albedo and clouds. This study proposed a regression model to predict the distributions and trends of global ADRE. According to the results, 70% of the ADRE variability is contributed by aerosols, while the rest is influenced by surface albedo and clouds. The high aerosol concentrations in the Northern Hemisphere require energy to be transported from the South Hemisphere to the North. However, this demand has decreased over the past two decades. Changes in surface albedo and clouds have a significant impact on the ADRE trend. In particular, the retreating sea ice plays a major role in the ADRE trend in the Arctic. Key Points: Nonaerosol factors contribute significantly to the spatial inhomogeneity of the aerosol direct radiative effect (ADRE) and its trends in recent decadesThe hemispheric difference in scattering aerosols drives northward cross‐equator energy transport, which shows a declining trendChanges in the surface albedo due to sea ice melt strongly influence the ADRE trends in, and the energy transport to, the Arctic [ABSTRACT FROM AUTHOR]

Biomass burning (BB) aerosols exert a strong surface cooling effect over the southeast Atlantic (SEA) via aerosol‐radiation and aerosol‐cloud interactions. The reduction of the sea surface temperature (SST) can trigger the SST‐low cloud feedback. Whether this feedback can amplify the surface cooling effect is examined. The modeling results from the Community Earth System Model version 2 (CESM2) demonstrate that counterintuitively the cloud radiative effect (CRE) caused by the BB aerosols is weaker if SST‐low cloud feedback is considered compared to fixed‐SST simulation (−2.99 W m−2 vs. −4.79 W m−2). This is caused by (a) stronger sea breeze due to larger sea‐land temperature contrast causing less smoke transport over SEA and (b) less moisture supply from surface due to colder SST. Changes in SST also lead to counterclockwise rotation of ocean circulation anomalies. Consequently, the excess heat transport from the equator reverses the direction of SST‐cloud feedback in this region. Plain Language Summary: Biomass burning aerosols can modulate the cloud macro‐ and microphysical properties over the Southeast Atlantic and induce a strong cooling effect at the surface. As a result, sea surface temperature will decrease, which can further promote cloudiness in this region (a positive SST‐low cloud feedback). Our study demonstrates that the cooling effect caused by biomass burning aerosols is actually smaller when the SST‐low cloud feedback is considered, because of stronger sea breeze that reduces the transport of biomass burning aerosols and weaker surface moisture supply. In addition, the ocean current changes can determine the direction of this SST‐low cloud feedback. Key Points: Sea surface temperature‐low cloud feedback reduces the magnitude of the cloud radiative effect (CRE) caused by the BB aerosols over Southeast AtlanticWeaker CRE is due to stronger sea breeze and less moisture supply from the oceanThe excess heat transport associated with counterclockwise rotation of ocean circulation anomalies stops the amplification of CRE [ABSTRACT FROM AUTHOR]

We characterize the aerosol physical and optical properties of 13 transported biomass burning (BB) events. BB events included long-range influence from fires in Alaskan and Siberian boreal forests transported to Mt. Bachelor Observatory (MBO) in the free troposphere (FT) over 8– 14+ d and regional wildfires in northern California and southwestern Oregon transported to MBO in the boundary layer (BL) over 10 h to 3 d. Intensive aerosol optical properties and normalized enhancement ratios for BB events were derived from measured aerosol light scattering coefficients (σscat), aerosol light-absorbing coefficients (σabs), fine particulate matter (PM 1), and carbon monoxide (CO) measurements made from July to September 2019, with particle size distribution collected from August to September. The observations showed that the Siberian BB events had a lower scattering Ångström exponent (SAE), a higher mass scattering efficiency (MSE; Δσscat/ΔPM1), and a bimodal aerosol size distribution with a higher geometric mean diameter (Dg). We hypothesize that the larger particles and associated scattering properties were due to the transport of fine dust alongside smoke in addition to contributions from condensation of secondary aerosol, coagulation of smaller particles, and aqueous-phase processing during transport. Alaskan and Siberian boreal forest BB plumes were transported long distances in the FT and characterized by lower absorption Ångström exponent (AAE) values indicative of black carbon (BC) dominance in the radiative budget. Significantly elevated AAE values were only observed for BB events with <1 d transport, which suggests strong production of brown carbon (BrC) in these plumes but limited radiative forcing impacts outside of the immediate region. [ABSTRACT FROM AUTHOR]

The sub-micron (SM) aerosol optical depth (AOD) is an optical separation based on the fraction of particles below a specified cutoff radius of the particle size distribution (PSD) at a given particle radius. It is fundamentally different from spectrally separated FM (fine-mode) AOD. We present a simple (AOD-normalized) SM fraction versus FM fraction (SMF vs. FMF) linear equation that explains the well-recognized empirical result of SMF generally being greater than the FMF. The AERONET inversion (AERinv) products (combined inputs of spectral AOD and sky radiance) and the spectral deconvolution algorithm (SDA) products (input of AOD spectra) enable, respectively, an empirical SMF vs. FMF comparison at similar (columnar) remote sensing scales across a variety of aerosol types. SMF (AERinv-derived) vs. FMF (SDA-derived) behavior is primarily dependent on the relative truncated portion (εc) of the coarse-mode (CM) AOD associated with the cutoff portion of the CM PSD and, to a second order, the cutoff FM PSD and FM AOD (εf). The SMF vs. FMF equation largely explains the SMF vs. FMF behavior of the AERinv vs. SDA products as a function of PSD cutoff radius ("inflection point") across an ensemble of AERONET sites and aerosol types (urban-industrial, biomass burning, dust, maritime and a mixed class of Arctic aerosols). The overarching dynamic was that the linear SMF vs. FMF relation pivots clockwise about the approximate (SMF, FMF) singularity of (1, 1) in a "linearly inverse" fashion (slope and intercept of approximately 1-εc and εc) with increasing cutoff radius. SMF vs. FMF slopes and intercepts derived from AERinv and SDA retrievals confirmed the general domination of εc over εf in controlling that dynamic. A more general conclusion is the apparent confirmation that the optical impact of truncating modal (whole) PSD features can be detected by an SMF vs. FMF analysis. [ABSTRACT FROM AUTHOR]

The vertical distribution of aerosols in the lower troposphere is critically important for assessing their impact on Earth's radiation budget and modulation of cloud microphysics. This study analyzed cloud‐free aerosol extinction coefficient (βext), aerosol subtypes, and particulate depolarization ratios obtained from CALIOP (Cloud‐Aerosol Lidar with Orthogonal Polarization) over the six regions of India during 2008–2018. We investigated unprecedented climatology of the physical and optical characteristics of elevated aerosol layers (EALs) along with their source and formation mechanism. The key findings include: (a) EALs over the Indian region were persistent between 4 and 6 km during all seasons, (b) geometrical layer thickness of EALs increased up to 36.7% and 25% from the annual mean during summer and fall seasons, respectively, compared to that of spring and winter, (c) dust and polluted dust accounted for up to 50%–80% from near‐surface to 6 km and up to 80%–90% of the EALs between 4 and 6 km, respectively for all the seasons and regions, (d) we anticipated that locally confined recirculation coupled with stratified stable layer capped within turbulent layers could be a possible mechanism of formation of stratified EALs between 4 and 6 km during winter‐spring‐fall, while in summer, vertical transport of pollutants from the PBL to mid‐troposphere due to enhanced deep convection served as a key formation mechanism of the EALs, (e) the second Modern‐Era Retrospective analysis for Research and Applications Global Modeling Initiative model reasonably simulated the shape and vertical gradient of βext with significant differences in magnitude below 4 km; however, it fails to reproduce EALs for all seasons and regions during the study period. Plain Language Summary: Aerosols distributed in the troposphere can scatter and absorb solar radiation and modify the Earth's radiation budget and cloud properties. The combined effect of scattering and absorption by particles is defined as aerosol extinction coefficient, is a measure of the alteration of radiant energy as it passes through the atmosphere. The aerosol extinction coefficient was derived with the space‐borne lidar Cloud‐Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) over the Indian region during 2008–2018. The vertical profiles of aerosol extinction coefficient depicted persistent layers between 4 and 6 km over the Indian region named elevated aerosol layers (EALs). In the summer and fall seasons, the thickness of the EALs increased by 36.7% and 25% from the annual mean, respectively. Throughout the year, dust and polluted dust aerosols accounted for up to 50%–80% of the EALs composition between near‐surface and 6 km. Stratified EALs between 4 and 6 km were formed by locally confined wind recirculation coupled with stable atmospheric layers during the winter, spring, and fall seasons. In summer, the vertical transport of pollutants from the planetary boundary layer to the mid‐troposphere associated with enhanced deep convection played a crucial role in the formation of EALs. Key Points: Aerosol layers persisted between 4 and 6 km in the free troposphere during all seasons over the Indian regionElevated aerosol layers (EALs) between 4 and 6 km were formed due to confined anticyclonic circulation capped within turbulent layersSecond Modern‐Era Retrospective analysis for Research and Applications Global Modeling Initiative simulation fails to reproduce EALs for all seasons and regions during the study period [ABSTRACT FROM AUTHOR]

Airborne observations of vertical aerosol particle distributions are crucial for detailed process studies and model improvements. Tethered balloon systems represent a less expensive alternative to aircraft to probe shallow atmospheric boundary layers (ABLs). This study presents the newly developed cubic aerosol measurement platform (CAMP) for balloon-borne observations of aerosol particle microphysical properties. With an edge length of 35 cm and a weight of 9 kg, the cube is an environmentally robust instrument platform intended for measurements at low temperatures, with a particular focus on applications in cloudy Arctic ABLs. The aerosol instrumentation on board CAMP comprises two condensation particle counters with different lower detection limits, one optical particle size spectrometer, and a miniaturized absorption photometer. Comprehensive calibrations and characterizations of the instruments were performed in laboratory experiments. The first field study with a tethered balloon system took place at the Leibniz Institute for Tropospheric Research (TROPOS) station in Melpitz, Germany, in the winter of 2019. At ambient temperatures between - 8 and 15 ∘ C, the platform was operated up to a 1.5 km height on 14 flights under both clear-sky and cloudy conditions. The continuous aerosol observations at the ground station served as a reference for evaluating the CAMP measurements. Exemplary profiles are discussed to elucidate the performance of the system and possible process studies. Based on the laboratory instrument characterizations and the observations during the field campaign, CAMP demonstrated the capability to provide comprehensive aerosol particle measurements in cold and cloudy ABLs. [ABSTRACT FROM AUTHOR]

Measurement of light absorption of solar radiation by aerosols is vital for assessing direct aerosol radiative forcing, which affects local and global climate. Low-cost and easy-to-operate filter-based instruments, such as the Particle Soot Absorption Photometer (PSAP), that collect aerosols on a filter and measure light attenuation through the filter are widely used to infer aerosol light absorption. However, filter-based absorption measurements are subject to artifacts that are difficult to quantify. These artifacts are associated with the presence of the filter medium and the complex interactions between the filter fibers and accumulated aerosols. Various correction algorithms have been introduced to correct for the filter-based absorption coefficient measurements toward predicting the particle-phase absorption coefficient (Babs). However, the inability of these algorithms to incorporate into their formulations the complex matrix of influencing parameters such as particle asymmetry parameter, particle size, and particle penetration depth results in prediction of particle-phase absorption coefficients with relatively low accuracy. The analytical forms of corrections also suffer from a lack of universal applicability: different corrections are required for rural and urban sites across the world. In this study, we analyzed and compared 3 months of high-time-resolution ambient aerosol absorption data collected synchronously using a three-wavelength photoacoustic absorption spectrometer (PASS) and PSAP. Both instruments were operated on the same sampling inlet at the Department of Energy's Atmospheric Radiation Measurement program's Southern Great Plains (SGP) user facility in Oklahoma. We implemented the two most commonly used analytical correction algorithms, namely, Virkkula (2010) and the average of Virkkula (2010) and Ogren (2010)–Bond et al. (1999) as well as a random forest regression (RFR) machine learning algorithm to predict Babs values from the PSAP's filter-based measurements. The predicted Babs was compared against the reference Babs measured by the PASS. The RFR algorithm performed the best by yielding the lowest root mean square error of prediction. The algorithm was trained using input datasets from the PSAP (transmission and uncorrected absorption coefficient), a co-located nephelometer (scattering coefficients), and the Aerosol Chemical Speciation Monitor (mass concentration of non-refractory aerosol particles). A revised form of the Virkkula (2010) algorithm suitable for the SGP site has been proposed; however, its performance yields approximately 2-fold errors when compared to the RFR algorithm. To generalize the accuracy and applicability of our proposed RFR algorithm, we trained and tested it on a dataset of laboratory measurements of combustion aerosols. Input variables to the algorithm included the aerosol number size distribution from the Scanning Mobility Particle Sizer, absorption coefficients from the filter-based Tricolor Absorption Photometer, and scattering coefficients from a multiwavelength nephelometer. The RFR algorithm predicted Babs values within 5 % of the reference Babs measured by the multiwavelength PASS during the laboratory experiments. Thus, we show that machine learning approaches offer a promising path to correct for biases in long-term filter-based absorption datasets and accurately quantify their variability and trends needed for robust radiative forcing determination. [ABSTRACT FROM AUTHOR]

By analyzing observations and simulations from the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), we investigated instant and delayed responses of large-scale atmospheric circulations and precipitation to biomass burning (BB) aerosols over the Indochina Peninsula (ICP) in the peak emission of March. The results show that the BB aerosols inhibit precipitation over the ICP in March and promote precipitation from early April to mid April. Specifically, the March BB aerosols over the ICP can induce mid- to lower-tropospheric heating and planetary boundary layer cooling to enhance local atmospheric stability; meanwhile, the perturbation heating can trigger an anomalous low in the lower troposphere to moisten the mid troposphere. However, the convection suppression due to the stabilized atmosphere dominates over the favorable water-vapor condition induced by large-scale circulation responses, leading to overall reduced precipitation over the ICP in March. For the delayed effect, the anomalous low can provide more water vapor as the monsoon advances in early April, although it becomes much weaker without BB aerosols' strong heating. On the other hand, the convective instability above 850 hPa is enhanced by more water vapor, resulting in enhanced precipitation over the ICP, northern South China Sea, and southern China. Thereafter, the condensational latent heating gradually takes over from the BB aerosol radiative heating, acting as the main driver for maintaining the anomalous circulation and thus the delayed effect in mid April. [ABSTRACT FROM AUTHOR]

There exists a lack of aerosol absorption measurement techniques with low uncertainties and without artefacts. We have developed the two-wavelength Photothermal Aerosol Absorption Monitor (PTAAM- 2λ) , which measures the aerosol absorption coefficient at 532 and 1064 nm. Here we describe its design, calibration and mode of operation and evaluate its applicability, limits and uncertainties. The 532 nm channel was calibrated with ∼ 1 µmol mol -1 NO 2 , whereas the 1064 nm channel was calibrated using measured size distribution spectra of nigrosin particles and a Mie calculation. Since the aerosolized nigrosin used for calibration was dry, we determined the imaginary part of the refractive index of nigrosin from the absorbance measurements on solid thin film samples. The obtained refractive index differed considerably from the one determined using aqueous nigrosin solution. PTAAM-2 λ has no scattering artefact and features very low uncertainties: 4 % and 6 % for the absorption coefficient at 532 and 1064 nm, respectively, and 9 % for the absorption Ångström exponent. The artefact-free nature of the measurement method allowed us to investigate the artefacts of filter photometers. Both the Aethalometer AE33 and CLAP suffer from cross-sensitivity to scattering – this scattering artefact is most pronounced for particles smaller than 70 nm. We observed a strong dependence of the filter multiple scattering parameter on the particle size in the 100–500 nm range. The results from the winter ambient campaign in Ljubljana showed similar multiple scattering parameter values for ambient aerosols and laboratory experiments. The spectral dependence of this parameter resulted in AE33 reporting the absorption Ångström exponent for different soot samples with values biased 0.23–0.35 higher than the PTAAM-2 λ measurement. Photothermal interferometry is a promising method for reference aerosol absorption measurements. [ABSTRACT FROM AUTHOR]

We investigate and assess how well a global chemical transport model (GEOS‐Chem) simulates submicron aerosol mass concentrations in the remote troposphere. The simulated speciated aerosol (organic aerosol (OA), black carbon, sulfate, nitrate, and ammonium) mass concentrations are evaluated against airborne observations made during all four seasons of the NASA Atmospheric Tomography Mission (ATom) deployments over the remote Pacific and Atlantic Oceans. Such measurements over pristine environments offer fresh insights into the spatial (Northern [NH] and Southern Hemispheres [SH], Atlantic, and Pacific Oceans) and temporal (all seasons) variability in aerosol composition and lifetime, away from continental sources. The model captures the dominance of fine OA and sulfate aerosol mass concentrations in all seasons. There is a high bias across all species in the ATom‐2 (NH winter) simulations; implementing recent updates to the wet scavenging parameterization improves our simulations, eliminating the large ATom‐2 (NH winter) bias, improving the ATom‐1 (NH summer) and ATom‐3 (NH fall) simulations, but producing a model underestimate in aerosol mass concentrations for the ATom‐4 (NH spring) simulations. Following the wet scavenging updates, simulated global annual mean aerosol lifetimes vary from 1.9 to 4.0 days, depending on species. Aerosol lifetimes in each hemisphere vary by season, and are longest for carbonaceous aerosol during the southern hemispheric fire season. The updated wet scavenging parameterization brings simulated concentrations closer to observations and reduces global aerosol lifetime for all species, indicating the sensitivity of global aerosol lifetime and burden to wet removal processes. Plain Language Summary: Aerosols are a key constituent of the atmosphere. Their lifetime in the atmosphere controls their global distribution and the resulting air quality and climate impacts. We use a global model (GEOS‐Chem) to simulate their mass concentrations. To evaluate the model, we compare simulations against airborne measurements over the remote Pacific and Atlantic oceans made in all four seasons during the NASA Atmospheric Tomography Mission (ATom). The model generally reproduces organic and sulfate aerosols well, yet it over‐estimates all species in the Northern Hemispheric (NH) winter season. An updated wet deposition method, which provides more effective aerosol removal, reduced the overestimation in this season, improved the simulation in NH summer and fall as well, but underestimated the concentrations in NH spring. With the model update, aerosol lifetimes vary from 1.9 to 4.0 days and by species and seasons, with organic aerosols and black carbon having the longest lifetime during the Southern Hemispheric fire season. The updated wet deposition scheme reduces these lifetimes significantly, demonstrating the sensitivity of aerosol lifetime and concentration to the wet removal process. Key Points: Evaluating GEOS‐Chem aerosol simulations against remote observations from the ATom campaign shows a systematic NH winter high biasUpdating the wet scavenging scheme improves the model simulation, in particular eliminating a high bias during ATom‐2Global aerosol lifetime is reduced by 1–2 days for all aerosols [ABSTRACT FROM AUTHOR]