Cloud Droplet Number Research Articles

Impact of acidity and surface-modulated acid dissociation on cloud response to organic aerosol

Abstract. Acid dissociation of the organic aerosol fraction has the potential to impact cloud-activating properties by altering aqueous-phase H+ concentrations and water activity but is currently overlooked in most atmospheric aerosol models. We implemented a simple representation of organic acid dissociation in the aerosol–chemistry–climate box model ECHAM6.3–HAM2.3 and investigated the impact on aerosol-forming aqueous sulfur chemistry, cloud droplet number concentrations, and the shortwave radiative effect. Many atmospheric organic acids are also surface-active and may be strongly adsorbed at the surface of small aqueous droplets. The degree of dissociation has recently been observed for several atmospheric surface-active organics with Brönsted acid character to be significantly shifted in the surface, compared to the bulk aqueous solution. In addition to the well-known bulk acidity, we therefore introduced an empirical account of this surface-modulated dissociation to further explore the potential impact on aerosol climate effects. Malonic acid and decanoic acid were used as proxies for atmospheric organic aerosols of different surface-active and acid strengths. Both acids were found to yield sufficient hydrogen ion concentrations from dissociation in an aqueous droplet population to strongly influence aqueous aerosol sulfur chemistry, leading to enhanced cloud droplet number concentrations and a cooling shortwave radiative effect. Further considering the surface modulation of organic acid dissociation, the impact on cloud microphysics was smaller than according to the well-known bulk solution acidity but still significant. Our results show that organic aerosol acid dissociation can significantly influence predictions of aerosol and cloud droplet formation and aerosol–cloud–climate effects and that, even for a well-known bulk solution phenomenon such as acidity, it may be important to also consider the specific influence of surface effects when surface-active acids comprise a significant fraction of the total organic aerosol mass.

New Particle Formation Events Can Reduce Cloud Droplets in Boundary Layer Clouds at the Continental Scale

AbstractNew particle formation (NPF) substantially contributes to global cloud condensation nuclei (CCN), and their climate impacts. Individual NPF events are also thought to increase local CCN, cloud droplet number (CDN), and cloud albedo. High resolution simulations however go against the latter, showing that radiatively important stratiform clouds can experience a systematic and substantial decrease in CDN during and after NPF events. CDN drops because particles too small to act as CCN uptake condensable material, and stunt the growth of particles that would otherwise form droplets. Convective clouds however experience modest increases in CDN—consistent with established views on the NPF‐cloud link. Together, these results reshape our conceptual understanding of NPF impacts on clouds, as the newly discovered duality of responses would drive cloud systems in a fundamentally different manner than thought.

Causes of Reduced Climate Sensitivity in E3SM From Version 1 to Version 2

AbstractThe effective climate sensitivity in the Department of Energy's Energy Exascale Earth System Model (E3SM) has decreased from 5.3 K in version 1 to 4.0 K in version 2. This reduction is mainly due to a weaker positive cloud feedback that leads to a stronger negative radiative feedback. Present‐day atmosphere‐only experiments with uniform 4 K sea surface temperature warming are used to separate the contributions of individual model modifications to the reduced cloud feedback. We find that the reduced cloud feedback is mostly driven by changes over the tropical marine low cloud regime, mainly related to a new trigger function for the deep convection scheme and modifications in the cloud microphysics scheme. The new trigger function helps weaken the low cloud reduction by increasing the cloud water detrainment at low levels from deep convection under warming. Changes to the formula of autoconversion rate from liquid to rain and an introduced minimum cloud droplet number concentration threshold in cloud microphysical calculations help sustain clouds against dissipation by suppressing precipitation generation with warming. In the midlatitudes, the increased Wegener‐Bergeron‐Findeisen (WBF) efficiency strongly reduces present‐day liquid water and leads to a stronger negative cloud optical depth feedback. The reduced trade cumulus cloud feedback in v2 is closer to estimates from recent observational and large‐eddy modeling studies but might not be due to the right physical reasons. The reduced mid‐latitude cloud feedback may be more plausible because more realistic present‐day mixed‐phase clouds are produced through the change in the WBF efficiency.

Understanding the Effects of Aerosols on Electrification and Lightning Polarity in an Idealized Supercell Thunderstorm via Model Emulation

AbstractAerosol effects on the lightning intensity and polarity of a continental supercell storm were investigated using a three‐dimensional lightning scheme within the Weather Research and Forecasting model. We find that both intra‐cloud (IC) and cloud‐to‐ground (CG) flashes are enhanced by the increasing number of cloud condensation nuclei (CCN), especially the percentage of positive CG (+CG) strokes peaking at 42%. Electrical characteristics of the storm varied in different aerosol scenarios through microphysical processes. Added aerosols increase the number of cloud droplets and ice‐phase hydrometeors. The greater ice‐crystal concentration and larger graupel size ensure sufficient charge separation, leading to higher charge density and more lightning discharges. In addition, an inverted polarity charge structure with a strong positive‐charge region in the mid‐levels was formed mainly due to the positively charged graupel in the presence of higher supercooled cloud water content. Positive lightning channels originating from this positive‐charge region propagated to the ground, producing more +CG strokes. When the aerosol concentration was low, the charge density in the upper positive‐charge region was much lower due to smaller ice‐particle content. Consequently, there were barely any +CG strokes. Most of the negative CG flashes deposited positive charge in the lower negative‐charge region.

Retrieving Cloud Sensitivity to Aerosol Using Ship Emissions in Overcast Conditions

AbstractThe interaction between aerosols and clouds is one of the major uncertainties in past climate change, affecting the accuracy of future climate projections. Ship tracks, trails left in clouds through the addition of aerosol in the ship exhaust plume, have become a key observational tool for constraining aerosol‐cloud interactions. However, many expected tracks remain undetected, presenting a significant gap in current knowledge of aerosol forcing. Here we leverage a plume‐parcel model to simulate the impact of aerosol dispersion for 2,957 cases off California's coast on cloud droplet number concentration (CDNC) enhancements. Plume‐parcel models show a large sensitivity to updraft uncertainties, which are found to be a primary control on track formation. Using these plume‐parcel models, updraft values consistent with observed CDNC enhancements are recovered, suggesting that relying solely on cloud‐top radiative cooling may overestimate in‐cloud updrafts by around 50%, hence overstating the cloud sensitivity to aerosols.

Secondary droplet activation during condensational growth in convective clouds and its detection from satellites

By acting as cloud condensation nuclei (CCN), aerosol particles play a key role in the climate system. The CCN can be activated into cloud droplets at the cloud base (i.e., primary activation), or above it (i.e., secondary activation). This study shows the conditions required for secondary activation during the condensational growth phase in convective clouds. It also proposes a methodology for detecting this secondary activation from satellites. Using a spectral bin adiabatic parcel model, we simulate the vertical profile of cloud microphysical properties and demonstrate how different aerosol size distributions and updraft velocities greatly affect the secondary activation initiation and the cloud properties. The secondary activation slows down the cloud drop effective radius (re) growth rate with increasing height, and decreasing temperature (T), due to the relatively larger population of smaller droplets in the cloud parcel. Therefore, the vertical profile of re growth with height is slower than the adiabatic rate when the secondary activation occurs.The proposed physical principle was verified by satellite-retrieved T-re profiles and adiabatic cloud drop number concentrations (Nd) over the Amazon region. The results obtained from this study can be utilized to identify the secondary droplet activation during the condensational growth phase, which can lead to an overestimation of the retrieved Nd as well as suppression of warm rain. This improves our knowledge and observational capabilities of the role of aerosol particles in the microphysics, dynamics, and precipitation behavior of convective clouds. Plain text summarySmall particles serve as sites for cloud droplets' condensation at the cloud base (primary droplet activation) or above it (secondary activation). Once a droplet is activated at the cloud base, the surrounding water vapor condenses on it and the droplet grows - this is called condensational growth. The cloud droplet number concentrations (Nd) can be obtained by the satellite-retrieved vertical growth rate of droplet size in the condensational growth phase. However, new small droplets formed during this phase (i.e., secondary activation), might cause an overestimate in the retrieved Nd. This study presents the physical principle of secondary activation during condensational growth. Using a model, we simulate the condensational growth of aerosol particles, which act as cloud condensation nuclei (CCN), for different particle size distributions and thermodynamic conditions (i.e., vertical velocities). Our simulations show that secondary activation slows the cloud droplet growth rate with height due to the larger competition for the available water vapor promoted by the new drops. Comparisons between satellite-retrieved Nd of convective clouds and in-situ measurements show that the satellite retrievals overestimate Nd when the secondary activation of droplets is neglected. Our findings improve the understanding of aerosols' role in the condensational growth of droplets in convective clouds.

Effects of Wind Shear and Aerosol Conditions on the Organization of Precipitating Marine Stratocumulus Clouds

AbstractThis study examines how wind shear affects precipitating marine stratocumulus clouds under different cloud droplet number concentrations (Nd). We performed a series of large eddy simulations (LES) of nocturnal marine stratocumulus clouds using Cloud Model 1 (CM1). The simulations show that Nd is the dominant factor for cloud cellular organization in this cloud regime rather than wind shear. Low Nd characterizes the open cellular structure with a high in‐cloud liquid water path (LWP). When wind shear is increased, the cloud fraction tends to decrease along with LWP, suggesting the cloud top region is significantly influenced by the entrainment and mixing of dry air from the free troposphere. We also examine cold pools in open and closed cellular clouds. Open‐cell clouds produce larger and deeper cold pools compared to closed‐cell clouds. Interestingly, cold pools can exist without surface precipitation and are produced by evaporation of light precipitation (drizzle) below the cloud base with weak downdrafts. The evaporation of raindrops and drizzle play an important role in initiating new convection, particularly where colliding outflows occur downstream of the cloud. This secondary convection contributes to the development and maintenance of the cloud cellular organization and formation.

Evaluation of four ground-based retrievals of cloud droplet number concentration in marine stratocumulus with aircraft in situ measurements

Abstract. Cloud droplet number concentration (Nd) is crucial for understanding aerosol–cloud interactions (ACI) and associated radiative effects. We present evaluations of four ground-based Nd retrievals based on comprehensive datasets from the Atmospheric Radiation Measurement (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. The Nd retrieval methods use ARM ENA observatory ground-based remote sensing observations from a micropulse lidar, Raman lidar, cloud radar, and the ARM NDROP (Droplet Number Concentration) value-added product (VAP), all of which also retrieve cloud effective radius (re). The retrievals are compared against aircraft measurements from the fast cloud droplet probe (FCDP) and the cloud and aerosol spectrometer (CAS) obtained from low-level marine boundary layer clouds on 12 flight days during summer and winter seasons. Additionally, the in situ measurements are used to validate the assumptions and characterizations used in the retrieval algorithms. Statistical comparisons of the probability distribution function (PDF) of the Nd and cloud re retrievals with aircraft measurements demonstrate that these retrievals align well with in situ measurements for overcast clouds, but they may substantially differ for broken clouds or clouds with low liquid water path (LWP). The retrievals are applied to 4 years of ground-based remote sensing measurements of overcast marine boundary layer clouds at the ARM ENA observatory to find that Nd (re) values exhibit seasonal variations, with higher (lower) values during the summer season and lower (higher) values during the winter season. The ensemble of various retrievals using different measurements and retrieval algorithms such as those in this paper can help to quantify Nd retrieval uncertainties and identify reliable Nd retrieval scenarios. Of the retrieval methods, we recommend using the micropulse lidar-based method. This method has good agreement with in situ measurements, less sensitivity to issues arising from precipitation and low cloud LWP and/or optical depth, and broad applicability by functioning for both daytime and nighttime conditions.

The Effects of Aerosol on Small‐Scale Cloud‐Environment Mixing: Implications for Simulating and Observing Inhomogeneous Mixing

AbstractEntrainment‐mixing modulates the number and size of cloud droplets, and thus affects the optical properties of clouds and their role in the climate system. Using a statistical turbulence model coupled with Lagrangian cloud microphysics, we analyze the role of aerosol in the entrainment‐mixing process, which, for instance, prevent the full evaporation of cloud droplets, leaving behind haze particles. To test a commonly applied indicator for inhomogeneous mixing, a set of different mixing scenarios is simulated. We conclude that if a hard separation radius between cloud droplets and haze particles is chosen, the typical classification into homogeneous and inhomogeneous mixing can be wrong because larger haze particles might be misidentified as cloud droplets, making the mixing appear more homogeneous. Furthermore, we show that the growth of cloud droplets on the expense of other hydrometeors due to differences in aerosol loading and particle curvature (Ostwald ripening) can produce cloud microphysical signatures indistinguishable from inhomogeneous mixing. Finally, we investigate how the consideration of haze particles can mitigate the previously reported negative impacts of inhomogeneous mixing on the cloud albedo. These findings should be considered when interpreting observations and simulations of small‐scale entrainment‐mixing.

Robust Susceptibility of Cloud Cover and Radiative Effects to Biases in Retrieved Droplet Concentrations

AbstractThe quantification of cloud droplet number concentration (Nd) is essential in gaining insights into the aerosol‐cloud interactions (ACI), contributing to the most significant source of anthropogenic climate forcing uncertainty. This study compared the retrieved Nd from Moderate Resolution Imaging Spectroradiometer (MODIS) and Visible Infrared Imaging Radiometer Suite (VIIRS) at pixel and scene levels and analyzed the changes in the susceptibility of cloud albedo (CA), cloud fraction (CF), and cloud radiative effect (CRE) to Nd. The results show that the differences between the pixel‐level cloud products from VIIRS and MODIS are caused by a combination of factors including cloud detectability, spatial resolution, and wavelengths of channels. As cloud top inhomogeneity increases, the differences become more significant. This deviation finally results in VIIRS achieving a global average of 40% higher Nd than MODIS. Although the non‐systematic differences cause an inevitable variability in the dependence of CA, CF, and CRE on Nd, the strong susceptibilities of these cloud properties to Nd are similar for both VIIRS and MODIS. This study found minimal impact on the susceptibilities, whether using the average Nd or that of the top 10% reflective clouds. This study further supports the conclusion that cloud cover and radiative effect are highly susceptible to variations in Nd, which can reduce uncertainty when evaluating the cooling effect of ACI in the context of global warming.

Maximum Supersaturation in the Marine Boundary Layer Clouds Over the North Atlantic

AbstractThe maximum supersaturation (Sx) in clouds is a key parameter affecting the cloud's microphysical and radiative properties. We investigate the Sx of the marine boundary layer clouds by combining airborne and surface observations in the Eastern North Atlantic. The cloud droplet number concentration (Nc) in the least diluted cloud cores agrees well with the number concentration of particles larger than the Hoppel Minimum (HM) (N>HM) below clouds, indicating that the HM represents the average size threshold above which particles are activated to form cloud droplets. The Sx values derived from surface observations vary from 0.10% to 0.50% from June 2017 to June 2018, with a clear seasonal variation exhibiting higher values during winter. Most of the Sx variance (∼60%) can be explained by the cloud condensation nuclei (CCN) concentration and updraft velocity (w), with the CCN concentration playing a more important role than w in explaining the variation of Sx. The influence of CCN concentration on Sx leads to a buffered response of Nc to aerosol perturbations. The response of Nc to low aerosol concentration during winter is further buffered by the high w. The global Community Earth System Model (CESM) simulated Sx values in the Azores have a positive bias compared to measured Sx, likely due to overestimated w and underestimated CCN concentration. The CESM simulated Sx exhibits higher values further north over the North Atlantic Ocean, which is attributed to stronger w. The suppression of Sx by aerosol is also evident in regions with high CCN concentrations.

Observational evidence of strong forcing from aerosol effect on low cloud coverage.

Aerosols cool Earth's climate indirectly by increasing low cloud brightness and their coverage (Cf), constituting the aerosol indirect forcing (AIF). The forcing partially offsets the greenhouse warming and positively correlates with the climate sensitivity. However, it remains highly uncertain. Here, we show direct observational evidence for strong forcing from Cf adjustment to increased aerosols and weak forcing from cloud liquid water path adjustment. We estimate that the Cf adjustment drives between 52% and 300% of additional forcing to the Twomey effect over the ocean and a total AIF of -1.1 ± 0.8 W m-2. The Cf adjustment follows a power law as a function of background cloud droplet number concentration, Nd. It thus depends on time and location and is stronger when Nd is low. Cf only increases substantially when background clouds start to drizzle, suggesting a role for aerosol-precipitation interactions. Our findings highlight the Cf adjustment as the key process for reducing the uncertainty of AIF and thus future climate projections.

Earth System Model Aerosol–Cloud Diagnostics (ESMAC Diags) package, version 2: assessing aerosols, clouds, and aerosol–cloud interactions via field campaign and long-term observations

Abstract. Poor representations of aerosols, clouds, and aerosol–cloud interactions (ACIs) in Earth system models (ESMs) have long been the largest uncertainties in predicting global climate change. Huge efforts have been made to improve the representation of these processes in ESMs, and the key to these efforts is the evaluation of ESM simulations with observations. Most well-established ESM diagnostics packages focus on the climatological features; however, they lack process-level understanding and representations of aerosols, clouds, and ACIs. In this study, we developed the Earth System Model Aerosol–Cloud Diagnostics (ESMAC Diags) package to facilitate the routine evaluation of aerosols, clouds, and ACIs simulated the Energy Exascale Earth System Model (E3SM) from the US Department of Energy (DOE). This paper documents its version 2 functionality (ESMAC Diags v2), which has substantial updates compared with version 1 (Tang et al., 2022a). The simulated aerosol and cloud properties have been extensively compared with in situ and remote-sensing measurements from aircraft, ship, surface, and satellite platforms in ESMAC Diags v2. It currently includes six field campaigns and two permanent sites covering four geographical regions: the eastern North Atlantic, the central US, the northeastern Pacific, and the Southern Ocean. These regions produce frequent liquid- or mixed-phase clouds, with extensive measurements available from the DOE Atmospheric Radiation Measurement user facility and other agencies. ESMAC Diags v2 generates various types of single-variable and multivariable diagnostics, including percentiles, histograms, joint histograms, and heatmaps, to evaluate the model representation of aerosols, clouds, and ACIs. Select examples highlighting the capabilities of ESMAC Diags are shown using E3SM version 2 (E3SMv2). In general, E3SMv2 can reasonably reproduce many observed aerosol and cloud properties, with biases in some variables such as aerosol particle and cloud droplet sizes and number concentrations. The coupling of aerosol and cloud number concentrations may be too strong in E3SMv2, possibly indicating a bias in processes that control aerosol activation. Furthermore, the liquid water path response to a perturbed cloud droplet number concentration behaves differently in E3SMv2 and observations, which warrants further study to improve the cloud microphysics parameterizations in E3SMv2.

Aerosol and dynamical contributions to cloud droplet formation in Arctic low-level clouds

Abstract. The Arctic is one of the most rapidly warming regions of the globe. Low-level clouds and fog modify the energy transfer from and to space and play a key role in the observed strong Arctic surface warming, a phenomenon commonly termed “Arctic amplification”. The response of low-level clouds to changing aerosol characteristics throughout the year is therefore an important driver of Arctic change that currently lacks sufficient constraints. As such, during the NASCENT campaign (Ny-Ålesund AeroSol Cloud ExperimeNT) extending over a full year from October 2019 to October 2020, microphysical properties of aerosols and clouds were studied at the Zeppelin station (475 m a.s.l.), Ny-Ålesund, Svalbard, Norway. Particle number size distributions obtained from differential mobility particle sizers as well as chemical composition derived from filter samples and an aerosol chemical speciation monitor were analyzed together with meteorological data, in particular vertical wind velocity. The results were used as input to a state-of-the-art cloud droplet formation parameterization to investigate the particle sizes that can activate to cloud droplets, the levels of supersaturation that can develop, the droplet susceptibility to aerosol and the role of vertical velocity. We evaluate the parameterization and the droplet numbers calculated through a droplet closure with in-cloud in situ measurements taken during nine flights over 4 d. A remarkable finding is that, for the clouds sampled in situ, closure is successful in mixed-phase cloud conditions regardless of the cloud glaciation fraction. This suggests that ice production through ice–ice collisions or droplet shattering may have explained the high ice fraction, as opposed to rime splintering that would have significantly reduced the cloud droplet number below levels predicted by warm-cloud activation theory. We also show that pristine-like conditions during fall led to clouds that formed over an aerosol-limited regime, with high levels of supersaturation (generally around 1 %, although highly variable) that activate particles smaller than 20 nm in diameter. Clouds formed in the same regime in late spring and summer, but aerosol activation diameters were much larger due to lower cloud supersaturations (ca. 0.5 %) that develop because of higher aerosol concentrations and lower vertical velocities. The contribution of new particle formation to cloud formation was therefore strongly limited, at least until these newly formed particles started growing. However, clouds forming during the Arctic haze period (winter and early spring) can be limited by updraft velocity, although rarely, with supersaturation levels dropping below 0.1 % and generally activating larger particles (20 to 200 nm), including pollution transported over a long range. The relationship between updraft velocity and the limiting cloud droplet number agrees with previous observations of various types of clouds worldwide, which supports the universality of this relationship.

Surface-Area-to-Volume Ratio Determines Surface Tensions in Microscopic, Surfactant-Containing Droplets.

The surface composition of aerosol droplets is central to predicting cloud droplet number concentrations, understanding atmospheric pollutant transformation, and interpreting observations of accelerated droplet chemistry. Due to the large surface-area-to-volume ratios of aerosol droplets, adsorption of surfactant at the air-liquid interface can deplete the droplet's bulk concentration, leading to droplet surface compositions that do not match those of the solutions that produced them. Through direct measurements of individual surfactant-containing, micrometer-sized droplet surface tensions, and fully independent predictive thermodynamic modeling of droplet surface tension, we demonstrate that, for strong surfactants, the droplet's surface-area-to-volume ratio becomes the key factor in determining droplet surface tension rather than differences in surfactant properties. For the same total surfactant concentration, the surface tension of a droplet can be >40 mN/m higher than that of the macroscopic solution that produced it. These observations indicate that an explicit consideration of surface-area-to-volume ratios is required when investigating heterogeneous chemical reactivity at the surface of aerosol droplets or estimating aerosol activation to cloud droplets.

The impact of aerosols on stratiform clouds over southern West Africa: a large-eddy-simulation study

Abstract. Low-level stratiform clouds (LLSCs) covering a large area appear frequently during the wet monsoon season in southern West Africa. This region is also a place where different types of aerosols coexist, including biomass burning aerosols coming from central and southern Africa and aerosols emitted by local anthropogenic activities. We investigate the indirect and semi-direct effects of these aerosols on the life cycle of LLSCs by conducting a case study based on airborne and ground-based observations from the field campaign of Dynamic-Aerosol-Chemistry-Cloud-Interaction in West Africa (DACCIWA). This case is modeled using a large-eddy-simulation (LES) model with fine resolution and in situ aerosol measurements, including size distribution and chemical composition. The model has successfully reproduced the observed life cycle of the LLSC, from stratus formation to stabilization during the night and to upward development after sunrise until break-up of the cloud deck in the late afternoon. Additional sensitivity simulations using different measured aerosol profiles also suggest that aerosols can affect the cloud life cycle through both the indirect and semi-direct effects. As expected, modeled cloud microphysical features, including cloud droplet number concentration, mean radius, and thus cloud reflectivity, are all controlled by aerosol concentration. However, it is found that the variation in cloud reflectivity induced by different aerosol profiles is not always the only factor in determining the incoming solar radiation at the ground and thus for the cloud life cycle after sunrise. Instead, the difference in cloud fraction brought by dry-air entrainment from above and thus the speed of consequent evaporation – also influenced by aerosol concentration – is another important factor to consider. Clouds influenced by higher aerosol concentrations and thus with a higher number concentration and smaller sizes of cloud droplets are found to evaporate more easily and thus impose a lower cloud fraction. In addition, our sensitivity runs including versus excluding aerosol direct radiative effects have also demonstrated the impacts specifically of solar absorption by black carbon on the cloud life cycle. The semi-direct effect resulting from an excessive atmospheric heating of up to 12 K d−1 by black carbon in our modeled cases is found to lower the cloud top as well as the liquid water path, reducing surface incoming solar radiation and dry entrainment and increasing the cloud fraction.

Global observations of aerosol indirect effects from marine liquid clouds

Abstract. Interactions between aerosols and liquid clouds are one of the largest sources of uncertainty in the historical radiative forcing of climate. One widely shared goal to reduce this uncertainty is to decompose radiative anomalies arising from aerosol–cloud interactions into components associated with changes in cloud-droplet number concentration (Twomey effect), liquid-water-path adjustments, and cloud-fraction adjustments. However, there has not been a quantitative foundation for simultaneously estimating these components with global satellite observations. Here we present a method for assessing shortwave radiative flux anomalies from the Twomey effect and cloud adjustments over ocean between 55∘ S and 55∘ N. We find that larger aerosol concentrations are associated with widespread cloud brightening from the Twomey effect, a positive radiative adjustment from decreasing liquid water path in subtropical stratocumulus regions, and a negative radiative adjustment from increasing cloud fraction in the subtropics and midlatitudes. The Twomey effect and total cloud adjustment have contributed −0.77 ± 0.25 and −1.02 ± 0.43 W m−2, respectively, to the effective radiative forcing since 1850 over the domain (95 % confidence). Our findings reduce uncertainty in these components of aerosol forcing and suggest that cloud adjustments make a larger contribution to the forcing than is commonly believed.

Rapid saturation of cloud water adjustments to shipping emissions

Abstract. Human aerosol emissions change cloud properties by providing additional cloud condensation nuclei. This increases cloud droplet numbers, which in turn affects other cloud properties like liquid-water content and ultimately cloud albedo. These adjustments are poorly constrained, making aerosol effects the most uncertain part of anthropogenic climate forcing. Here we show that cloud droplet number and water content react differently to changing emission amounts in shipping exhausts. We use information about ship positions and modeled emission amounts together with reanalysis winds and satellite retrievals of cloud properties. The analysis reveals that cloud droplet numbers respond linearly to emission amount over a large range (1–10 kg h−1) before the response saturates. Liquid water increases in raining clouds, and the anomalies are constant over the emission ranges observed. There is evidence that this independence of emissions is due to compensating effects under drier and more humid conditions, consistent with suppression of rain by enhanced aerosol. This has implications for our understanding of cloud processes and may improve the way clouds are represented in climate models, in particular by changing parameterizations of liquid-water responses to aerosol.

Vertical Motions in Orographic Cloud Systems over the Payette River Basin. Part IV: Controls on Supercooled Liquid Water Content and Cloud Droplet Number Concentrations

Abstract This paper examines the controls on supercooled liquid water content (SLWC) and drop number concentrations (Nt,CDP) over the Payette River basin during the Seeded and Natural Orographic Wintertime Clouds: The Idaho Experiment (SNOWIE) campaign. During SNOWIE, 27.4% of 1-Hz in situ cloud droplet probe samples were in an environment containing supercooled liquid water (SLW). The interquartile range of SLWC, when present, was found to be 0.02–0.18 g m−3 and 13.3–37.2 cm−3 for Nt,CDP, with the most extreme values reaching 0.40–1.75 g m−3 and 150–320 cm−3 in isolated regions of convection and strong shear-induced turbulence. SLWC and Nt,CDP distributions are shown to be directly related to cloud-top temperature and ice particle concentrations, consistent with past research over other mountain ranges. Two classes of vertical motions were analyzed as potential controls on SLWC and Nt,CDP, the first forced by the orography and fixed in space relative to the topography (stationary waves) and the second transient, triggered by vertical shear and instability within passing synoptic-scale cyclones. SLWC occurrence and magnitudes, and Nt,CDP associated with fixed updrafts were found to be normally distributed about ridgelines when SLW was present. SLW was more likely to form at low altitudes near the terrain slope associated with fixed waves due to higher mixing ratios and larger vertical air parcel displacements at low altitudes. When considering transient updrafts, SLWC and Nt,CDP appear more uniformly distributed over the flight track with little discernable terrain dependence as a result of time and spatially varying updrafts associated with passing weather systems. The implications for cloud seeding over the basin are discussed.

Impacts of marine cloud brightening scheme on climatic extremes in the Tibetan Plateau

Abstract As an ecologically fragile plateau and major water source in Asia, the Tibetan Plateau (TP) has grown warmer over recent decades, contributing to frequent occurrence of extreme climate events. It is urgently needed to find a suitable option to mitigate climate change impacts in the TP. The marine cloud brightening (MCB) scheme is proposed to mitigate global warming through the increasing cloud droplet number concentration of low marine clouds to reflect some solar radiation back into space. Until now, impacts of MCB scheme on the TP have not been investigated. In this study, we utilized 13 Expert Team on Climate Change Detection and Indices to assess the evolution of climate extremes over the TP with/without MCB implementation. We found that although the MCB is implemented over ocean only, it would cause significant changes on climate extremes in the TP which is very far from oceans and much higher than sea level. During 2030–2059, MCB implementation can decrease warm temperature extremes, leading to a significant decrease in the TXx index by 6–18°C, the TX90p index by 15–45 days, and the TN90p index by 15–50 days. MCB implementation would also have some cooling effects on cold temperature extremes, leading to an increase in the ID index by 30–80 days, the TX10p index by 22–32 days, and the TN10p index by about 12 days and a decrease in the TNn index by 0.5–1.5°C. Although MCB implementation would not have much impacts on precipitation extremes, it would significantly increase the area of the region with <10% drought frequency, and increase the drought intensity in the west of Lhasa city.