Cloud Interactions Research Articles

Radiation fog properties in two consecutive events under polluted and clean conditions in the Yangtze River Delta, China: a simulation study

Abstract. Aerosol–cloud interaction (ACI) in fog and planetary boundary layer (PBL) conditions plays critical roles in the fog life cycle. However, it is not clear how ACI in the first fog (Fog1) affects the PBL and subsequently affects ACI in the second fog (Fog2), which is important information for understanding the interaction between ACI and the PBL, as well as their effects on fog properties. To fill this knowledge gap, we simulate two successive radiation fog events in the Yangtze River Delta, China, using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). Our simulations indicate that the PBL conditions conducive to Fog2 formation are affected by ACI with high aerosol loading in Fog1; subsequently, the PBL promotes ACI in Fog2, resulting in a higher liquid water content, higher droplet number concentration, smaller droplet size, larger fog optical depth, wider fog distribution, and longer fog lifetime in Fog2 than in Fog1. This phenomenon is related to the following physical factors. The first factor involves meteorological conditions conducive to Fog2 formation, including low temperature, high humidity, and high stability. The second factor is the feedbacks between microphysics and radiative cooling. A higher fog droplet number concentration increases the liquid water path and fog optical depth, thereby enhancing long-wave radiative cooling and condensation near the fog top. The third factor is the feedbacks between macrophysics, radiation, and turbulence. A higher fog top presents stronger long-wave radiative cooling near the fog top than near the fog base, which weakens temperature inversion and strengthens turbulence, ultimately increasing the fog-top height and fog area. In summary, under polluted conditions, ACI postpones the dissipation of Fog1 owing to these two feedbacks and generates PBL meteorological conditions that are more conducive to the formation of Fog2 than those prior to Fog1. These conditions promote the earlier formation of Fog2, further enhancing the two feedbacks and strengthening the ACI in Fog2. Our findings are critical for studying the interaction between aerosols, fog, and the PBL; moreover, they shed new light on ACI.

Verification of satellite and model products against a dense rain gauge network for a severe flooding event in Kumasi, Ghana

AbstractFloods as a result of severe storms cause significant impacts on lives and properties. Therefore, timely and accurate forecasts of the storms will reduce the associated risks. In this study, we look at the characteristics of a storm on 28 June, 2018 in Kumasi from a rain gauge network and satellite data, and reanalysis data. The storm claimed at least 8 lives and displaced 293 people in Kumasi, Ghana. The ability of satellite and reanalysis data to capture the temporal variations of the storm was assessed using a high temporal resolution (accumulation per minute) rain gauge data. We employed the observation data from the Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa (DACCIWA) rain gauges to assess the storm's onset, duration, and cessation. Subsequently, the performance of the ERA5 reanalysis and Global Precipitation Measurement (GPM) satellite precipitation estimates in capturing the rainfall is assessed. Both GPM and the ERA5 had difficulty reproducing the hourly pattern of the rain. However, the GPM produced variability that is similar to the observed. Generally, the region of maximum rainfall was located in the southern parts of the study domain in ERA5, while GPM placed it in the northern parts. The study contributes a verification measure to improve weather forecasting in Ghana as part of the objectives of the GCRF African Science for Weather Information and Forecasting Techniques (SWIFT) project.

The global impact of the transport sectors on the atmospheric aerosol and the resulting climate effects under the Shared Socioeconomic Pathways (SSPs)

Abstract. A global aerosol–climate model is applied to quantify the impact of the transport sectors (land transport, shipping, and aviation) on aerosol and climate. Global simulations are performed for the present day (2015), based on the emission inventory of the Climate Model Intercomparison Project Phase 6 (CMIP6), and for near-term (2030) and mid-term (2050) future projections, under the Shared Socioeconomic Pathways (SSPs). The results for the present day show that land transport emissions have a large impact on near-surface concentrations of black carbon and aerosol nitrate over the most populated areas of the globe, but with contrasting patterns in terms of relative contributions between developed and developing countries. In spite of the recently introduced regulations to limit the fuel sulfur content in the shipping sector, shipping emissions are still responsible for a considerable impact on aerosol sulfate near-surface concentrations, about 0.5 to 1 µg m−3 in the most travelled regions, with significant effects on continental air pollution and in the northern polar regions as well. Aviation impacts on aerosol mass are found to be quite small, of the order of a few nanograms per cubic metre, while this sector considerably affects particle number concentrations, contributing up to 20 %–30 % of the upper-tropospheric particle number concentration at the northern mid-latitudes. The transport-induced impacts on aerosol mass and number concentrations result in a present-day radiative forcing of −164, −145, and −64 mW m−2 for land transport, shipping, and aviation, respectively, with a dominating contribution by aerosol–cloud interactions. These forcings represent a marked offset to the CO2 warming from the transport sectors and are therefore very relevant for climate policy. The projections under the SSPs show that the impact of the transport sectors on aerosol and climate are generally consistent with the narratives underlying these scenarios: the lowest impacts of transport on both aerosol and climate are simulated under SSP1, especially for the land transport sector, while SSP3 is generally characterized by the largest effects. Notable exceptions to this picture, however, exist, as the emissions of other anthropogenic sectors also contribute to the overall aerosol concentrations and thus modulate the relevance of the transport sectors in the different scenarios, not always consistently with their underlying storyline. On a qualitative level, the results for the present day mostly confirm the findings of our previous assessment for the year 2000, which used a predecessor version of the same model and the CMIP5 emission data. Some important quantitative differences are found, which can mostly be ascribed to the improved representation of aerosol background concentrations in the present study.

A first global height-resolved cloud condensation nuclei data set derived from spaceborne lidar measurements

Abstract. We present a global multiyear height-resolved data set of aerosol-type-specific cloud condensation nuclei concentrations (nCCN) estimated from the spaceborne lidar aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite. For estimating nCCN, we apply the recently introduced Optical Modelling of the CALIPSO Aerosol Microphysics (OMCAM) algorithm to the CALIPSO Level 2 Aerosol Profile product. The estimated nCCN are then gridded into a uniform latitude–longitude grid of 2∘×5∘, a vertical grid of resolution 60 m from the surface to an altitude of 8 km, and a temporal resolution of 1 month. The data span a total of 186 months, from June 2006 to December 2021. In addition, we provide a 3D aerosol-type-specific climatology of nCCN produced using the complete time series. We further highlight some potential applications of the data set in the context of aerosol–cloud interactions. The complete data set can be accessed at https://doi.org/10.1594/PANGAEA.956215 (Choudhury and Tesche, 2023).

Nonlinearity of the cloud response postpones climate penalty of mitigating air pollution in polluted regions

Aerosol–cloud interactions contribute substantially to uncertainties in anthropogenic forcing, in which the sensitivity of cloud droplet number concentration (Nd) to aerosol plays a central role. Here we use satellite observations to show that the aerosol–Nd relation (in log–log space) is not linear as commonly assumed. Instead, the Nd sensitivity decreases at large aerosol concentrations due to the transition from aerosol-limited to updraft-limited regime, making the widely used linear method problematic. A sigmoidal transition is shown to adequately fit the data. When using this revised relationship, the additional warming that arises from air pollution mitigation is delayed by two to three decades in heavily polluted locations, compared to the linear relationship. This cloud-mediated climate penalty will manifest markedly starting around 2025 in China and 2050 in India after applying the strongest air quality policy, underlining the urgency of mitigating greenhouse gas emissions.

Quantification of carbon monoxide emissions from African cities using TROPOMI

Abstract. Carbon monoxide (CO) is an air pollutant that plays an important role in atmospheric chemistry and is mostly emitted by forest fires and incomplete combustion in, for example, road transport, residential heating, and industry. As CO is co-emitted with fossil fuel CO2 combustion emissions, it can be used as a proxy for CO2. Following the Paris Agreement, there is a need for independent verification of reported activity-based bottom-up CO2 emissions through atmospheric measurements. CO can be observed daily at a global scale with the TROPOspheric Monitoring Instrument (TROPOMI) satellite instrument with daily global coverage at a resolution down to 5.5 × 7 km2. To take advantage of this unique TROPOMI dataset, we develop a cross-sectional flux-based emission quantification method that can be applied to quantify emissions from a large number of cities, without relying on computationally expensive inversions. We focus on Africa as a region with quickly growing cities and large uncertainties in current emission estimates. We use a full year of high-resolution Weather Research and Forecasting (WRF) simulations over three cities to evaluate and optimize the performance of our cross-sectional flux emission quantification method and show its reliability down to emission rates of 0.1 Tg CO yr−1. Comparison of the TROPOMI-based emission estimates to the Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa (DACCIWA) and Emissions Database for Global Atmospheric Research (EDGAR) bottom-up inventories shows that CO emission rates in northern Africa are underestimated in EDGAR, suggesting overestimated combustion efficiencies. We see the opposite when comparing TROPOMI to the DACCIWA inventory in South Africa and Côte d'Ivoire, where CO emission factors appear to be overestimated. Over Lagos and Kano (Nigeria) we find that potential errors in the spatial disaggregation of national emissions cause errors in DACCIWA and EDGAR respectively. Finally, we show that our computationally efficient quantification method combined with the daily TROPOMI observations can identify a weekend effect in the road-transport-dominated CO emissions from Cairo and Algiers.

Influence of natural and anthropogenic aerosols on cloud base droplet size distributions in clouds over the South China Sea and West Pacific

Abstract. Cumulus clouds are common over maritime regions. They are important regulators of the global radiative energy budget and global hydrologic cycle, as well as a key contributor to the uncertainty in anthropogenic climate change projections due to uncertainty in aerosol–cloud interactions. These interactions are regionally specific owing to their strong influences on aerosol sources and meteorology. Here, our analysis focuses on the statistical properties of marine boundary layer (MBL) aerosol chemistry and the relationships of MBL aerosol to cumulus cloud properties just above cloud base as sampled in 2019 during the NASA Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex). The aerosol and clouds were sampled by instruments on the NASA P-3 aircraft over three distinct maritime regions around the Philippines: the West Pacific, the South China Sea, and the Sulu Sea. Our analysis shows three primary sources influenced the aerosol chemical composition: clean marine (ocean source), industrial (Southeast Asia, Manila, and cargo and tanker ship emissions), and biomass burning (Borneo and Indonesia). The clean marine aerosol chemical composition had low values of all sampled chemical signatures, specifically median values of 2.2 µg m−3 of organics (ORG), 2.3 µg m−3 of SO4, 0.3 µg m−3 of NO3, 1.4 µg m−3 of NH4, 0.04 µg m−3 of Cl, and 0.0074 µg m−3 of refractory black carbon (BC). Chemical signatures of the other two aerosol source regions were industrial, with elevated SO4 having a median value of 6.1 µg m−3, and biomass burning, with elevated median concentrations of ORG 21.2 µg m−3 and BC 0.1351 µg m−3. Based on chemical signatures, the industrial component was primarily from ship emissions, which were sampled within 60 km of ships and within projected ship plumes. Normalized cloud droplet size distributions in clouds sampled near the MBL passes of the P-3 showed that clouds impacted by industrial and biomass burning contained higher concentrations of cloud droplets, by as much as 1.5 orders of magnitude for diameters < 13 µm compared to clean marine clouds, while at size ranges between 13.0–34.5 µm the median concentrations of cloud droplets in all aerosol categories were nearly an order of magnitude less than the clean marine category. In the droplet size bins centered at diameters > 34.5 µm concentrations were equal to, or slightly exceeded, the concentrations of the clean marine clouds. These analyses show that anthropogenic aerosols generated from industrial and biomass burning sources significantly influenced cloud base microphysical structure in the Philippine region enhancing the small droplet concentration and reducing the concentration of mid-sized droplets.

Characterization of a Low-Temperature Plasma (LTP) Ambient Ionization Source Using Temporally Resolved Monochromatic Imaging Spectrometry.

The low-temperature plasma (LTP) probe is a common plasma-based source used for ambient desorption-ionization mass spectrometry (MS). While the LTP probe has been characterized in detail with MS, relatively few studies have used optical spectroscopy. In this paper, two-dimensional (2D) imaging at selected wavelengths is used to visualize important species in the LTP plasma jet. First, 2D steady-state images of the LTP plume for N2+ (391.2 nm), He I (706.5 nm), and N2 (337.1 nm) emissions were recorded under selected plasma conditions. Second, time-resolved 2D emission maps of radiative species in the LTP plasma jet were recorded through the use of a 200 ns detection gate and varying gate delays with respect to the LTP trigger pulse. Emission from He I, N2+, and N2 in the plasma jet region was found to show a transient behavior (often referred to as plasma bullets) lasting only a few microseconds. The N2+ and He I maps were highly correlated in spatial and temporal structure. Further, emission from N2 showed two maxima in time, one before and one after the maximum emission for N2+ and He I, due to an initial electronic excitation wave and ion-electron recombination, respectively. Third, the interaction of the LTP probe with a sample substrate and an electrically grounded metallic needle was studied. Emission from a fluorophore on the sample substrate showed an initial photon-induced excitation from plasma-generated photons followed by electronic excitation by other plasma species. The presence of a grounded needle near the plasma jet significantly extended the plasma jet lifetime and also generated a long-lived corona discharge on the needle. The effect of LTP operating parameters on emission spectra was correlated with mass-spectral results including reagent-ion signals. Lastly, five movies provide a side-by-side comparison of the temporal behavior of emitting species and insights into the interactions of the emission clouds with a sample surface as well as an external needle. Temporally and spatially resolved imaging provided insights into important processes in the LTP plasma jet, which will help improve analyte ion sampling in LTP-MS.

Pollution slightly enhances atmospheric cooling by low-level clouds in tropical West Africa

Abstract. Reflection of solar radiation by tropical low-level clouds has an important cooling effect on climate and leads to decreases in surface temperatures. Still, the effect of pollution on ubiquitous tropical continental low-level clouds and the investigation of the related impact on atmospheric cooling rates are poorly constrained by in situ observations and modeling, in particular during the West African summer monsoon season. Here, we present comprehensive in situ measurements of microphysical properties of low-level clouds over tropical West Africa, measured with the Deutsches Zentrum für Luft- und Raumfahrt (DLR) aircraft Falcon 20 during the DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa) campaign in June and July 2016. Clouds below 1800 m altitude, identified as boundary layer clouds, were classified according to their carbon monoxide (CO) pollution level into pristine and less polluted clouds (CO < 135 ppbv) and polluted low-level clouds (CO > 155 ppbv) as confirmed by the linear CO to accumulation aerosol number concentration correlation. Whereas slightly enhanced aerosol background levels from biomass burning were measured across the entire area, clouds with substantially enhanced aerosol levels were measured in the outflow of major coastal cities, as well as over rural conurbations in the hinterlands. Here we investigate the impact of pollution on cloud droplet number concentration and size during the West African monsoon season. Our results show that the cloud droplet number concentration (CDNC) measured in the size range from 3 to 50 µm around noon increases by 26 % in the elevated aerosol outflow of coastal cities and conurbations with elevated aerosol loadings from median CDNC of 240 cm−3 (52 to 501 cm−3 interquartile range) to 324 cm−3 (60 to 740 cm−3 interquartile range). Higher CDNC resulted in a 17 % decrease in effective cloud droplet diameter from a median deff of 14.8 µm to a deff of 12.4 µm in polluted clouds. Radiative transfer simulations show a non-negligible influence of higher droplet number concentrations and smaller particle sizes on the diurnally averaged (noon) net radiative forcing at the top of atmosphere of −3.9 W m−2 (−16.3 W m−2) of polluted with respect to less polluted clouds and lead to a change in instantaneous heating rates of −22.8 K d−1 (−17.7 K d−1) at the top of clouds. Thus, the atmospheric cooling by low-level clouds increases only slightly in the polluted case due to the already elevated background aerosol concentrations. Additionally, the occurrence of mid- and high-level cloud layers atop buffer this effect further, so that the net radiative forcing and instantaneous heating rate of low-level clouds turn out to be less sensitive towards projected future increases in anthropogenic pollution in West Africa.

The Nature of γ-Ray Emission from HESS J1912+101

Since the discovery of HESS J1912+101 at teraelectronvolt energies, its nature has been extensively studied. Due to the absence of X-ray and radio counterparts, whether its γ-ray emission is produced by relativistic electrons or ions is still a matter of debate. We reanalyze its megaelectronvolt to gigaelectronvolt γ-ray emission using 14 yr of Pass 8 data of the Fermi-LAT, and find that the gigaelectronvolt γ-ray emission is more extended than the teraelectronvolt shell detected by H. E. S. S. and flux above 10 GeV from the northern half is much higher than that from the southern half, where there is evident interaction between shocks and molecular clouds. As a consequence, the gigaelectronvolt spectrum of the northern half (with an index of 2.19 ± 0.12) is much harder than that in the south (with an index of 2.72 ± 0.08), and the overall gigaelectronvolt spectrum shows a concave shape, which is distinct from most γ-ray supernova remnants (SNRs). In combination with the teraelectronvolt spectrum, the overall γ-ray spectrum can be fitted with a broken power-law model for trapped ions and a low energy component due to escaping ions. The diffusion coefficient for escaping ions however needs to be proportional to the energy, implying that the low energy component may also be attributed to ions accelerated via recent shock–cloud interactions. A hadronic origin for the γ-ray emission is therefore favored and the overall emission properties are consistent with ion acceleration by SNR shocks. On the other hand, it is still undeniable that stellar cluster or PWN may have some contribution in some parts of this extended source.

Understanding aerosol–climate–ecosystem interactions and the implications for terrestrial carbon sink using the Community Earth System Model

Anthropogenic aerosols exert significant effects on the terrestrial ecosystem carbon cycle by causing climate change and altering surface hydrological conditions through radiation and cloud interaction, but such aerosol–climate–ecosystem interactions are difficult to quantify using currently available observations. Here, we used the Community Earth System Model (CESM, version 2.1.3) to quantify the effects of anthropogenic aerosols on terrestrial ecosystem carbon fluxes during the period from 1980 to 2014. The results found that the response of temperature and radiation to anthropogenic aerosols in different regions shows considerable variability in the CESM. Anthropogenic aerosols caused a 0.26 Pg C (0.43%) reduction in cumulative net biome production (NBP) during the period 1980-2014. In Southeast China (SEC) and East United States (EUS), anthropogenic aerosols caused a net reduction in NBP of 0.27 and 0.09 Pg C, respectively. In India (IND) and Europe (EUR), anthropogenic aerosols caused an increase of NBP by 0.07 and 0.14 Pg C, respectively. In addition, the decrease of the carbon sink was mainly dominated by changes in TER and others (40.6%), and the increase of the carbon sink was mainly dominated by changes in gross primary production (GPP) (38.9%). We also found that temperature is the dominant climate variable controlling the carbon cycle with a relative contribution of about 38%. Finally, the carbon flux response at the global scale is significantly lower than at the regional scale, which in turn highlights the importance of the assessment of the regional carbon cycle.

Detection of large-scale cloud microphysical changes within a major shipping corridor after implementation of the International Maritime Organization 2020 fuel sulfur regulations

Abstract. New regulations from the International Maritime Organization (IMO) limiting sulfur emissions from the shipping industry are expected to have large benefits in terms of public health but may come with an undesired side effect: acceleration of global warming as the climate-cooling effects of ship pollution on marine clouds are diminished. Previous work has found a substantial decrease in the detection of ship tracks in clouds after the IMO 2020 regulations went into effect, but changes in large-scale cloud properties have been more equivocal. Using a statistical technique that estimates counterfactual fields of what large-scale cloud and radiative properties within an isolated shipping corridor in the southeastern Atlantic would have been in the absence of shipping, we confidently detect a reduction in the magnitude of cloud droplet effective radius decreases within the shipping corridor and find evidence for a reduction in the magnitude of cloud brightening as well. The instantaneous radiative forcing due to aerosol–cloud interactions from the IMO 2020 regulations is estimated as O(1 W m−2) within the shipping corridor, lending credence to global estimates of O(0.1 W m−2). In addition to their geophysical significance, our results also provide independent evidence for general compliance with the IMO 2020 regulations.

Airborne investigation of black carbon interaction with low-level, persistent, mixed-phase clouds in the Arctic summer

Abstract. Aerosol–cloud interaction is considered one of the largest sources of uncertainty in radiative forcing estimations. To better understand the role of black carbon (BC) aerosol as a cloud nucleus and the impact of clouds on its vertical distribution in the Arctic, we report airborne in situ measurements of BC particles in the European Arctic near Svalbard during the “Arctic CLoud Observations Using airborne measurements during polar Day” (ACLOUD) campaign held in the summer of 2017. BC was measured with a single-particle soot photometer aboard the Polar 6 research aircraft from the lowest atmospheric layer up to approximately 3500 m a.s.l (metres above sea level). During in-cloud flight transects, BC particles contained in liquid droplets (BC residuals) were sampled through a counterflow virtual impactor (CVI) inlet. Four flights, conducted in the presence of low-level, surface-coupled, inside-inversion, and mixed-phase clouds over sea ice, were selected to address the variability in BC above, below, and within the cloud layer. First, the increase in size and coating thickness of BC particles from the free troposphere to the cloud-dominated boundary layer confirmed that ground observations were not representative of upper atmospheric layers. Second, although only 1 % of liquid droplets contained a BC particle, the higher number concentration of BC residuals than BC particles sampled below cloud indicated that the totality of below-cloud BC was activated by nucleation scavenging but also that alternative scavenging processes such as the activation of free-tropospheric BC at the cloud top might occur. Third, the efficient exchange of aerosol particles at cloud bottom was confirmed by the similarity of the size distribution of BC residuals and BC particles sampled below cloud. Last, the increase in the BC residual number concentration (+31 %) and geometric mean diameter (+38 %) from the cloud top to the cloud bottom and the absolute enrichment in larger BC residuals compared with outside of the cloud supported the hypothesis of concomitant scavenging mechanisms but also suggested the formation of BC agglomerates caused by cloud processing. The vertical evolution of BC properties from inside the cloud and below the cloud indicated an efficient aerosol exchange at cloud bottom, which might include activation, cloud processing, and sub-cloud release of processed BC agglomerates. In the case of persistent low-level Arctic clouds, this cycle may reiterate multiple times, adding an additional degree of complexity to the understanding of cloud processing of BC particles in the Arctic.

Observational study of relationships between entrainment rate, homogeneity of mixing, and cloud droplet relative dispersion

The entrainment–mixing process is key to the cloud's dynamical and microphysical processes. However, to the best of our knowledge, no study has quantitatively linked entrainment rate and homogeneity of mixing. Additionally, their combined effects on cloud droplet relative dispersion and physical mechanisms are even more unclear. This study analyzed the aircraft measurements of cumulus clouds collected in the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems field campaign to identify these relationships. The relationship between the entrainment rate and homogeneous mixing degree was found to be moderately positive, and the underlying mechanisms related to mixing and evaporation time scales and environmental relative humidity were explored. The relationship between relative dispersion and entrainment rate changes from positive to negative with increasing entrainment rate, depending on the dominance of evaporation of large or small droplets. The relative dispersion first increases and then decreases with increasing homogeneous mixing degree, validating the results of previous model simulations. The results shed new light on understanding the interactions between cloud microphysics and cloud dynamics through turbulent entrainment and mixing processes.

Change from aerosol-driven to cloud-feedback-driven trend in short-wave radiative flux over the North Atlantic

Abstract. Aerosol radiative forcing and cloud–climate feedbacks each have a large effect on climate, mainly through modification of solar short-wave radiative fluxes. Here we determine what causes the long-term trends in the upwelling short-wave (SW) top-of-the-atmosphere (TOA) fluxes (FSW↑) over the North Atlantic region. Coupled atmosphere–ocean simulations from the UK Earth System Model (UKESM1) and the Hadley Centre General Environment Model (HadGEM3-GC3.1) show a positive FSW↑ trend between 1850 and 1970 (increasing SW reflection) and a negative trend between 1970 and 2014. We find that the 1850–1970 positive FSW↑ trend is mainly driven by an increase in cloud droplet number concentration due to increases in aerosol, while the 1970–2014 trend is mainly driven by a decrease in cloud fraction, which we attribute mainly to cloud feedbacks caused by greenhouse gas-induced warming. In the 1850–1970 period, aerosol-induced cooling and greenhouse gas warming roughly counteract each other, so the temperature-driven cloud feedback effect on the FSW↑ trend is weak (contributing to only 23 % of the ΔFSW↑), and aerosol forcing is the dominant effect (77 % of ΔFSW↑). However, in the 1970–2014 period the warming from greenhouse gases intensifies, and the cooling from aerosol radiative forcing reduces, resulting in a large overall warming and a reduction in FSW↑ that is mainly driven by cloud feedbacks (87 % of ΔFSW↑). The results suggest that it is difficult to use satellite observations in the post-1970 period to evaluate and constrain the magnitude of the aerosol–cloud interaction forcing but that cloud feedbacks might be evaluated. Comparisons with observations between 1985 and 2014 show that the simulated reduction in FSW↑ and the increase in temperature are too strong. However, the temperature discrepancy can account for only part of the FSW↑ discrepancy given the estimated model feedback strength (λ=∂FSW∂T). The remaining discrepancy suggests a model bias in either λ or in the strength of the aerosol forcing (aerosols are reducing during this time period) to explain the too-strong decrease in FSW↑, with a λ bias being the most likely. Both of these biases would also tend to cause too-large an increase in temperature over the 1985–2014 period, which would be consistent with the sign of the model temperature bias reported here. Either of these model biases would have important implications for future climate projections using these models.

Measurement of the collision rate coefficients between atmospheric ions and multiply charged aerosol particles in the CERN CLOUD chamber

Abstract. Aerosol particles have an important role in Earth's radiation balance and climate, both directly and indirectly through aerosol–cloud interactions. Most aerosol particles in the atmosphere are weakly charged, affecting both their collision rates with ions and neutral molecules, as well as the rates by which they are scavenged by other aerosol particles and cloud droplets. The rate coefficients between ions and aerosol particles are important since they determine the growth rates and lifetimes of ions and charged aerosol particles, and so they may influence cloud microphysics, dynamics, and aerosol processing. However, despite their importance, very few experimental measurements exist of charged aerosol collision rates under atmospheric conditions, where galactic cosmic rays in the lower troposphere give rise to ion pair concentrations of around 1000 cm−3. Here we present measurements in the CERN CLOUD chamber of the rate coefficients between ions and small (<10 nm) aerosol particles containing up to 9 elementary charges, e. We find the rate coefficient of a singly charged ion with an oppositely charged particle increases from 2.0 (0.4–4.4) × 10−6 cm3 s−1 to 30.6 (24.9–45.1) × 10−6 cm3 s−1 for particles with charges of 1 to 9 e, respectively, where the parentheses indicate the ±1σ uncertainty interval. Our measurements are compatible with theoretical predictions and show excellent agreement with the model of Gatti and Kortshagen (2008).

Influence of horizontal resolution and complexity of aerosol–cloud interactions on marine stratocumulus and stratocumulus‐to‐cumulus transition in HadGEM3‐GC3.1

AbstractStratocumulus (Sc) clouds and stratocumulus‐to‐cumulus transitions (SCTs) are challenging to represent in global models and they contribute to a large spread in modeled subtropical cloud feedbacks. We evaluate the impact of increasing the horizontal model resolution (∼135, 60 and 25 km, respectively) and increasing the complexity of the aerosol–cloud interaction parameterization (interactive versus non‐interactive at medium resolution) on springtime subtropical marine Sc properties and SCTs in the atmosphere‐only version of HadGEM3‐GC3.1. No significant impact on the spatial location of the SCT could be found between the different model versions. Increasing horizontal resolution led to small but significant increases in liquid water content and a stronger (more negative) shortwave (SW) cloud radiative effect (CRE), in particular over the southern‐hemisphere Sc regions. However, for two out of the four studied regions, the stronger SW CRE also brought the model outside the range of satellite‐derived values of the SW CRE. Applying non‐interactive aerosols instead of interactive aerosols also led to significantly higher liquid water content and a stronger SW CRE over the southern‐hemisphere Sc regions, while over the northern‐hemisphere Sc regions, a competition between a substantial increase in the cloud droplet number concentration and small changes in the liquid water content resulted in a weaker SW CRE or non‐significant changes. In general, using interactive instead of non‐interactive aerosol–cloud interactions brought the model closer to satellite‐retrieved mean values of the SW CRE. Our results suggest that increasing the horizontal resolution or the complexity of the aerosol–cloud parameterization has a small but statistically significant effect on the SW CRE of marine Sc, in particular over regions with high liquid water content. For these regions, the effect of introducing non‐interactive versus interactive aerosol–cloud interactions is about as large as increasing the horizontal resolution from medium to high.

ЧИСЛЕННОЕ МОДЕЛИРОВАНИЕ ВЛИЯНИЯ АЭРОЗОЛЬНОГО СОСТАВА АТМОСФЕРЫ НА ФОРМИРОВАНИЕ МАКРО- И МИКРОСТРУКТУРНЫХ ХАРАКТЕРИСТИК КОНВЕКТИВНЫХ ОБЛАКОВ

Currently, the physics of clouds and active impacts on them is gradually moving from thestage of studying "elementary" cloud processes to the stage of studying clouds as a whole, takinginto account their systemic properties. One of the directions of research at this stage is the study ofthe role of the system properties of clouds in the formation of their macro- and microstructuralcharacteristics. These properties are the main factors influencing the formation of the cloud structure.The article presents some results of research on the role of one of these properties of clouds,namely the interaction of clouds with their surrounding atmosphere (the property of the hierarchyof systems). The mechanism caused by the aerosol composition of the atmosphere is considered asa method of their interaction. The research methodology is based on the assumption that the intensityof crystal formation in clouds is influenced by the content of aerosol particles of sufficientconcentration in the atmosphere with ice-forming properties (sublimation nuclei). A threedimensional unsteady model of convective clouds was used for calculations. The intensity of crystalformation in the cloud was changed by varying the value of the parameter in the expression forthe crystal source in the model equations for the cloud environment. The paper also discusses thecurrent state of the problem of active impacts on convective clouds in order to control precipitationprocesses. In order to carry out successful active exposure, it is necessary to determine thelocal area in the cloud in which conditions are favorable for exposure and the concentration ofreagent particles that should be provided in this area at any given time. Model calculationsshowed that a slight increase in the content of aerosol particles in the atmosphere led to an increasein the values of maximum ice content and total water content, as well as ice content, whilesimultaneously reducing the maximum water content in the cloud. At the same time, its macrostructuralcharacteristics have practically not changed. Further solving the problems requires thedevelopment of effective methodologies for modeling active exposure to convective clouds.

Chemical identification of new particle formation and growth precursors through positive matrix factorization of ambient ion measurements

Abstract. In the lower troposphere, rapid collisions between ions and trace gases result in the transfer of positive charge to the highest proton affinity species and negative charge to the lowest proton affinity species. Measurements of the chemical composition of ambient ions thus provide direct insight into the most acidic and basic trace gases and their ion–molecule clusters – compounds thought to be important for new particle formation and growth. We deployed an atmospheric pressure interface time-of-flight mass spectrometer (APi-ToF) to measure ambient ion chemical composition during the 2016 Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) campaign at the United States Department of Energy Atmospheric Radiation Measurement facility in the Southern Great Plains (SGP), an agricultural region. Cations and anions were measured for alternating periods of ∼ 24 h over 1 month. We use binned positive matrix factorization (binPMF) and generalized Kendrick analysis (GKA) to obtain information about the chemical formulas and temporal variation in ionic composition without the need for averaging over a long timescale or a priori high-resolution peak fitting. Negative ions consist of strong acids including sulfuric and nitric acid, organosulfates, and clusters of NO3- with highly oxygenated organic molecules (HOMs) derived from monoterpene (MT) and sesquiterpene (SQT) oxidation. Organonitrates derived from SQTs account for most of the HOM signal. Combined with the diel profiles and back trajectory analysis, these results suggest that NO3 radical chemistry is active at this site. SQT oxidation products likely contribute to particle growth at the SGP site. The positive ions consist of bases including alkyl pyridines and amines and a series of high-mass species. Nearly all the positive ions contained only one nitrogen atom and in general support ammonia and amines as being the dominant bases that could participate in new particle formation. Overall, this work demonstrates how APi-ToF measurements combined with binPMF analysis can provide insight into the temporal evolution of compounds important for new particle formation and growth.

Aerosol first indirect effect of African smoke at the cloud base of marine cumulus clouds over Ascension Island, southern Atlantic Ocean

Abstract. The interactions between aerosols and clouds are among the least understood climatic processes and were studied over Ascension Island. A ground-based UV polarization lidar was deployed on Ascension Island, which is located in the stratocumulus-to-cumulus transition zone of the southeastern Atlantic Ocean, to infer cloud droplet sizes and droplet number density near the cloud base of marine boundary layer cumulus clouds. The aerosol–cloud interaction (ACI) due to the presence of smoke from the African continent was determined during the monsoonal dry season. In September 2016, a cloud droplet number density ACIN of 0.3 ± 0.21 and a cloud effective radius ACIr of 0.18 ± 0.06 were found, due to the presence of smoke in and under the clouds. Smaller droplets near the cloud base makes them more susceptible to evaporation, and smoke in the marine boundary layer over the southeastern Atlantic Ocean will likely accelerate the stratocumulus-to-cumulus transition. The lidar retrievals were tested against more traditional radar–radiometer measurements and shown to be robust and at least as accurate as the lidar–radiometer measurements. The lidar estimates of the cloud effective radius are consistent with previous studies of cloud base droplet sizes. The lidar has the large advantage of retrieving both cloud and aerosol properties using a single instrument.