Cloud Condensation Nuclei Concentrations Research Articles

Biomass burning aerosol as a modulator of the droplet number in the southeast Atlantic region

Abstract. The southeastern Atlantic (SEA) and its associated cloud deck, off the west coast of central Africa, is an area where aerosol–cloud interactions can have a strong radiative impact. Seasonally, extensive biomass burning (BB) aerosol plumes from southern Africa reach this area. The NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) study focused on quantitatively understanding these interactions and their importance. Here we present measurements of cloud condensation nuclei (CCN) concentration, aerosol size distribution, and characteristic vertical updraft velocity (w∗) in and around the marine boundary layer (MBL) collected by the NASA P-3B aircraft during the August 2017 ORACLES deployment. BB aerosol levels vary considerably but systematically with time; high aerosol concentrations were observed in the MBL (800–1000 cm−3) early on, decreasing midcampaign to concentrations between 500 and 800 cm−3. By late August and early September, relatively clean MBL conditions were sampled (<500 cm−3). These data then drive a state-of-the-art droplet formation parameterization from which the predicted cloud droplet number and its sensitivity to aerosol and dynamical parameters are derived. Droplet closure was achieved to within 20 %. Droplet formation sensitivity to aerosol concentration, w∗, and the hygroscopicity parameter, κ, vary and contribute to the total droplet response in the MBL clouds. When aerosol concentrations exceed ∼900 cm−3 and maximum supersaturation approaches 0.1 %, droplet formation in the MBL enters a velocity-limited droplet activation regime, where the cloud droplet number responds weakly to CCN concentration increases. Below ∼500 cm−3, in a clean MBL, droplet formation is much more sensitive to changes in aerosol concentration than to changes in vertical updraft. In the competitive regime, where the MBL has intermediate pollution (500–800 cm−3), droplet formation becomes much more sensitive to hygroscopicity (κ) variations than it does in clean and polluted conditions. Higher concentrations increase the sensitivity to vertical velocity by more than 10-fold. We also find that characteristic vertical velocity plays a very important role in driving droplet formation in a more polluted MBL regime, in which even a small shift in w∗ may make a significant difference in droplet concentrations. Identifying regimes where droplet number variability is driven primarily by updraft velocity and not by aerosol concentration is key for interpreting aerosol indirect effects, especially with remote sensing. The droplet number responds proportionally to changes in characteristic velocity, offering the possibility of remote sensing of w∗ under velocity-limited conditions.

Predicting cloud condensation nuclei number concentration based on conventional measurements of aerosol properties in the North China Plain

Cloud condensation nuclei (CCN) play an important role in the formation and evolution of cloud droplets. However, the dataset of global CCN number concentration (NCCN) is still scarce due to the lack of direct CCN measurements, hindering an accurate evaluation of its climate effects. Alternative approaches to determine NCCN have thus been proposed to calculate NCCN based on measurements of other aerosol properties, such as particle number size distribution, bulk aerosol chemical composition and aerosol optical properties. To better understand the interaction between haze pollution and climate, we performed direct CCN measurements in the winter of 2018 at the Gucheng site, a typical polluted suburban site in North China Plain (NCP). The results show that the average CCN concentrations were 3.81 × 103 cm−3, 5.35 × 103 cm−3, 9.74 × 103 cm−3, 1.27 × 104 cm−3, 1.44 × 104 cm−3 at measured supersaturation levels of 0.114%, 0.148%, 0.273%, 0.492% and 0.864%, respectively. Based on these observational data, we have further investigated two methods of calculating NCCN from: (1) bulk aerosol chemical composition and particle number size distribution; (2) bulk aerosol chemical composition and aerosol optical properties. Our results showed that both methods could well reproduce the observed concentration (R2 > 0.88) and variability of NCCN with a 9% to 23% difference in the mean value. Further error analysis shows that the estimated NCCN tends to be underestimated by about 20% during the daytime while overestimated by <10% at night compared with the measured NCCN. These results provide quantitative instructions for the NCCN prediction based on conventional aerosol measurements in the NCP.

Comparison of aircraft measurements during GoAmazon2014/5 and ACRIDICON-CHUVA

Abstract. The indirect effect of atmospheric aerosol particles on the Earth's radiation balance remains one of the most uncertain components affecting climate change throughout the industrial period. The large uncertainty is partly due to the incomplete understanding of aerosol–cloud interactions. One objective of the GoAmazon2014/5 and the ACRIDICON (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems)-CHUVA (Cloud Processes of the Main Precipitation Systems in Brazil) projects was to understand the influence of emissions from the tropical megacity of Manaus (Brazil) on the surrounding atmospheric environment of the rainforest and to investigate its role in the life cycle of convective clouds. During one of the intensive observation periods (IOPs) in the dry season from 1 September to 10 October 2014, comprehensive measurements of trace gases and aerosol properties were carried out at several ground sites. In a coordinated way, the advanced suites of sophisticated in situ instruments were deployed aboard both the US Department of Energy Gulfstream-1 (G1) aircraft and the German High Altitude and Long-Range Research Aircraft (HALO) during three coordinated flights on 9 and 21 September and 1 October. Here, we report on the comparison of measurements collected by the two aircraft during these three flights. Such comparisons are challenging but essential for assessing the data quality from the individual platforms and quantifying their uncertainty sources. Similar instruments mounted on the G1 and HALO collected vertical profile measurements of aerosol particle number concentrations and size distribution, cloud condensation nuclei concentrations, ozone and carbon monoxide mixing ratios, cloud droplet size distributions, and downward solar irradiance. We find that the above measurements from the two aircraft agreed within the measurement uncertainties. The relative fraction of the aerosol chemical composition measured by instruments on HALO agreed with the corresponding G1 data, although the total mass loadings only have a good agreement at high altitudes. Furthermore, possible causes of the discrepancies between measurements on the G1 and HALO are examined in this paper. Based on these results, criteria for meaningful aircraft measurement comparisons are discussed.

Aerosol Impacts on Mesoscale Convective Systems Forming Under Different Vertical Wind Shear Conditions

AbstractFollowing our previous study of wind shear effect on mesoscale convective system (MCS) organization under a clean atmospheric condition using the Weather Research and Forecasting model coupled with spectral‐bin microphysics, we conduct sensitivity simulations by increasing cloud condensation nuclei concentration to investigate aerosol impacts on MCSs forming under different wind shear conditions. We find that increased aerosols induce stronger updrafts and downdrafts in all MCSs. The stronger updrafts and enlarged convective core area contribute to larger vertical mass fluxes and enhance precipitation. The enhanced updrafts and vertical mass fluxes indicate convective invigoration. Increased updraft speed below 8‐km altitude is attributed to enhanced condensational heating, except for the weak wind shear and strong low‐level shear cases in which the enhanced low‐level convergence is another contributing factor. Interestingly, above 8‐km altitude, we see reduced updraft speed by the increased aerosols due to reduced vertical pressure perturbation gradient force. The accumulated rainfall and mean rain rate are increased with a greater occurrence frequency of heavy rain. Larger rain rate is seen in both convective and stratiform regions. In general, we see a higher frequency of deep clouds in the polluted condition because of invigorated convection, and more stratiform/anvil clouds, but a lower frequency of shallow warm clouds, with a larger significance for more organized MCSs. The consistently invigorated MCSs by aerosols under various wind shear conditions revealed by this study have important implications to weather and climate in warm and humid regions that are influenced by pollution.

Observations of Aerosol‐Cloud Interactions During the North Atlantic Aerosol and Marine Ecosystem Study

AbstractClouds and their response to aerosols constitute the largest uncertainty in our understanding of 20th‐century climate change. We present an investigation that determines linkages between remotely sensed marine cloud properties with in situ measurements of cloud condensation nuclei (CCN) and meteorological properties obtained during the North Atlantic Aerosols and Marine Ecosystems Study. The first two deployments of this campaign have geographically similar domains but occur in different seasons allowing the response of clouds to a range of CCN concentrations and meteorological conditions to be investigated. Well‐defined connections between CCN and cloud microphysical properties consistent with the indirect effect are observed, as well as complex, nonlinear secondary effects that are partially supported by previously proposed mechanisms. Using the Research Scanning Polarimeter's remotely sensed effective variance parameter, correlation is found with liquid water path. In general, cloud macrophysical properties are found to better correlate with atmospheric state parameters than changes in CCN concentrations.

The Role of Ice Splintering on Microphysics of Deep Convective Clouds Forming Under Different Aerosol Conditions: Simulations Using the Model With Spectral Bin Microphysics

AbstractObservations during the Ice in Clouds Experiment‐Tropical (ICE‐T) field experiment show that the ice particles concentration in a developing deep convective clouds at the level of T = −15 °C reached about 500 L−1, that is, many orders higher than that of ice‐nucleating particle. To simulate microphysics of these clouds, the 2‐D Hebrew University Cloud model (HUCM) with spectral bin microphysics was used in which two main types of ice multiplication mechanisms were included in addition to the Hallet‐Mossop mechanism. In the first ice multiplication mechanism ice splinters form by drop freezing and drop‐ice collisions. Ice multiplication of this type dominates during developing stage of cloud evolution, when liquid water content is significant. At later stage when clouds become nearly glaciated, ice crystals are produced largely by ice splintering during ice‐ice collisions (the second ice multiplication mechanism). Simulations show that droplet size distributions, as well as size distributions of ice particles, agree well with the measurements during ICE‐T. Simulations with different cloud condensation nuclei concentrations show the existence of the “optimum” cloud condensation nuclei concentration (or droplet concentration), at which concentration of ice splinters reaches maximum. In these simulations ice nucleation caused by the direct formation of ice crystals upon ice‐nucleating particles, as well as the Hallett‐Mossop process, has a negligible contribution to the ice crystal concentration.

Effect of Aerosol Particles on Orographic Clouds: Sensitivity to Autoconversion Schemes

Aerosol particles can serve as cloud condensation nuclei (CCN) to influence orographic clouds. Autoconversion, which describes the initial formation of raindrops from the collision of cloud droplets, is an important process for aerosol-cloud-precipitation systems. In this study, seven autoconversion schemes are used to investigate the impact of CCN on orographic warm-phase clouds. As the initial cloud droplet concentration is increased from 100 cm−3 to 1000 cm−3 (to represent an increase in CCN), the cloud water increases and then the rainwater is suppressed due to a decrease in the autoconversion rate, leading to a spatial shift in surface precipitation. Intercomparison of the results from the autoconversion schemes show that the sensitivity of cloud water, rainwater, and surface precipitation to a change in the concentration of CCN is different from scheme to scheme. In particular, the decrease in orographic precipitation due to increasing CCN is found to range from −87% to −10% depending on the autoconversion scheme. Moreover, the surface precipitation distribution also changes significantly by scheme or CCN concentration, and the increase in the spillover (ratio of precipitation on the leeward side to total precipitation) induced by increased CCN ranges from 10% to 55% under different autoconversion schemes. The simulations suggest that autoconversion parameterization schemes should not be ignored in the interaction of aerosol and orographic cloud.

Anthropogenic Effects on Cloud Condensation Nuclei Distribution and Rain Initiation in East Asia

Key Points The activated cloud condensation nuclei (CCN) into cloud droplets were nearly equally low (&lt;300 cm−3) in inland areas with little anthropogenic emissions Anthropogenic emissions were responsible to the greatly elevated concentrations of CCN over and downwind of urban agglomeration The enhanced CCN increased cloud depth for rain initiation up to 4 km, further delayed and suppressed the precipitation over the most polluted regions

Altitude profiles of cloud condensation nuclei characteristics across the Indo-Gangetic Plain prior to the onset of the Indian summer monsoon

Abstract. Concurrent measurements of the altitude profiles of the concentration of cloud condensation nuclei (CCN), as a function of supersaturation (ranging from 0.2 % to 1.0 %), and aerosol optical properties (scattering and absorption coefficients) were carried out aboard an instrumented aircraft across the Indo-Gangetic Plain (IGP) just prior to the onset of the Indian summer monsoon (ISM) of 2016. The experiment was conducted under the aegis of the combined South-West Asian Aerosol–Monsoon Interactions and Regional Aerosol Warming Experiment (SWAAMI–RAWEX) campaign. The measurements covered coastal, urban and arid environments. In general, the CCN concentration was highest in the central IGP, decreasing spatially from east to west above the planetary boundary layer (PBL), which is ∼1.5 km for the IGP during pre-monsoon period. Despite this, the CCN activation efficiency at 0.4 % supersaturation was, interestingly, the highest over the eastern IGP (∼72 %), followed by that in the west (∼61 %), and it was the least over the central IGP (∼24 %) within the PBL. In general, higher activation efficiency is noticed above the PBL than below it. The central IGP showed remarkably low CCN activation efficiency at all altitudes, which appears to be associated with high black carbon (BC) mass concentration there, indicating the role of anthropogenic sources in suppressing the CCN efficiency. These first-ever CCN measurements over the western IGP, encompassing “the Great Indian Desert” also known as “the Thar Desert”, showed high CCN efficiency, ∼61 % at 0.4 % supersaturation, indicating the hygroscopic nature of the dust. The vertical structure of CCN properties is found to be air mass dependent, with higher activation efficiency even over the central IGP during the prevalence of marine air mass. Wet scavenging associated with precipitation episodes seems to have reduced the CCN activation efficiency below cloud level. An empirical relation has emerged between the CCN concentration and the scattering aerosol index (AI), which would facilitate the prediction of CCN from aerosol optical properties.

Aerosols in the E3SM Version 1: New Developments and Their Impacts on Radiative Forcing

AbstractThe new Energy Exascale Earth System Model Version 1 (E3SMv1) developed for the U.S. Department of Energy has significant new treatments of aerosols and light‐absorbing snow impurities as well as their interactions with clouds and radiation. This study describes seven sets of new aerosol‐related treatments (involving emissions, new particle formation, aerosol transport, wet scavenging and resuspension, and snow radiative transfer) and examines how they affect global aerosols and radiative forcing in E3SMv1. Altogether, they give a reduced total aerosol radiative forcing (−1.6 W/m2) and sensitivity in cloud liquid water to aerosols, but an increased sensitivity in cloud droplet size to aerosols. A new approach for H2SO4 production and loss largely reduces a low bias in small particles concentrations and leads to substantial increases in cloud condensation nuclei concentrations and cloud radiative cooling. Emitting secondary organic aerosol precursor gases from elevated sources increases the column burden of secondary organic aerosol, contributing substantially to global clear‐sky aerosol radiative cooling (−0.15 out of −0.5 W/m2). A new treatment of aerosol resuspension from evaporating precipitation, developed to remedy two shortcomings of the original treatment, produces a modest reduction in aerosols and cloud droplets; its impact depends strongly on the model physics and is much stronger in E3SM Version 0. New treatments of the mixing state and optical properties of snow impurities and snow grains introduce a positive present‐day shortwave radiative forcing (0.26 W/m2), but changes in aerosol transport and wet removal processes also affect the concentration and radiative forcing of light‐absorbing impurities in snow/ice.

Downward Trend in the Frequency of Destructive Hailstorms and Maximum Hailstone Size in England and Wales

By their definition, destructive hailstorms cause a great deal of damage to property and have been known to be fatal to humans. At present the long term changes in the frequency of these storms are unknown. Records of destructive hailstorms from many different sources in England and Wales go back for several centuries. Recently discovered records of over 30 destructive hailstorms have allowed a better description of hailstorm history since 1780. The data were grouped into 30, 40, and 50 year non-overlapping time periods in relation to time. Increases in their frequency in the 17th and 18th centuries were probably due to an increase in population and better recording. Since 1900 the frequency has significantly declined so that in the present 50 year time period only 22 have been recorded as compared with an average of 49 in both halves of the 19th century. The decline in frequency may be partly due to the big increase in particulate matter from aviation, which leads to a much higher concentration of ice and cloud condensation nuclei, resulting in fewer destructive hailstorms.

Seasonal Variations in Western North Atlantic Remote Marine Aerosol Properties

AbstractThe impact of ocean ecosystems on marine boundary layer aerosols and clouds has been the subject of much research but remains uncertain. Five experiments were recently conducted in the western North Atlantic to assess if the seasonally recurring phytoplankton bloom affects aerosol properties. These experiments include the second Western Atlantic Climate Study and four North Atlantic Aerosols and Marine Ecosystem Study cruises. Measurements of unheated and heated number size distributions, cloud condensation nucleus (CCN) concentrations, and aerosol composition were used to identify primary and secondary aerosol components that could be related to the state of the bloom. Only periods of clean marine air, as defined by radon, particle number concentrations, aerosol light absorption coefficient, and back trajectories, were included in the analysis. Nonvolatile material was found to be prevalent in the Aitken mode size range after heating to 230°, likely due to downward mixing from the free troposphere. CCN concentrations at 0.1% supersaturation were best correlated (r2 = 0.73) with accumulation mode nss SO4=. Sea spray aerosol was only correlated with CCN during November when bloom accumulation had not yet occurred and dimethylsulfide concentrations were at a minimum. The fraction of CCN attributable to sea spray aerosol was less than 20% during March, May/June, and September, indicating the limited contribution of sea spray aerosol to the CCN population of the western North Atlantic atmosphere. The strongest link between the plankton bloom and aerosol and cloud properties appears to be due to biogenic non‐sea salt SO4=.

The Roles of Mineral Dust as Cloud Condensation Nuclei and Ice Nuclei During the Evolution of a Hail Storm

AbstractAerosols play important roles in the evolution of deep convective systems like hailstorms. In this study, the heterogeneous ice nucleation schemes have been improved in the Weather Research and Forecasting model coupled with a spectral bin microphysics (WRF‐SBM), which considered aerosols acting as ice nuclei (IN). A hail storm occurred around Tianshan mountains, northwestern China, was simulated with updated WRF‐SBM, and the results have been compared with satellite observations. Further, four sensitive simulation tests were conducted with different cloud condensation nuclei (CCN) and IN concentrations to investigate their respective roles during the evolution of the hailstorm. The increase in CCN concentration resulted in larger cloud droplet concentration and cloud water content, as well as enhanced condensational growth, which released more latent heat and led to stronger updraft at lower levels. The increase in IN number almost did not affect warm processes but led to larger ice crystal concentration and enhanced Bergeron process. Larger CCN concentration led to larger supercooled liquid water content, which in turn contributed to the enhanced hail growth by more efficient drop‐ice collisions and led to larger size of hail particles, while larger IN number reduced the size of graupel and suppressed the growth of hailstones. An analysis of the mobility of hail indicated increased frequency of larger hail with stronger sedimentation induced by more CCN. A further three ensemble runs with random perturbations on initial temperature and humidity were performed for each aerosol scenario, and the results suggested the robustness of simulated CCN and IN effects.

Estimating cloud condensation nuclei number concentrations using aerosol optical properties: role of particle number size distribution and parameterization

Abstract. The concentration of cloud condensation nuclei (CCN) is an essential parameter affecting aerosol–cloud interactions within warm clouds. Long-term CCN number concentration (NCCN) data are scarce; there are a lot more data on aerosol optical properties (AOPs). It is therefore valuable to derive parameterizations for estimating NCCN from AOP measurements. Such parameterizations have already been made, and in the present work a new parameterization is presented. The relationships between NCCN, AOPs, and size distributions were investigated based on in situ measurement data from six stations in very different environments around the world. The relationships were used for deriving a parameterization that depends on the scattering Ångström exponent (SAE), backscatter fraction (BSF), and total scattering coefficient (σsp) of PM10 particles. The analysis first showed that the dependence of NCCN on supersaturation (SS) can be described by a logarithmic fit in the range SS &lt;1.1 %, without any theoretical reasoning. The relationship between NCCN and AOPs was parameterized as NCCN≈((286±46)SAE ln(SS/(0.093±0.006))(BSF − BSFmin) + (5.2±3.3))σsp, where BSFmin is the minimum BSF, in practice the 1st percentile of BSF data at a site to be analyzed. At the lowest supersaturations of each site (SS ≈0.1 %), the average bias, defined as the ratio of the AOP-derived and measured NCCN, varied from ∼0.7 to ∼1.9 at most sites except at a Himalayan site where the bias was &gt;4. At SS &gt;0.4 % the average bias ranged from ∼0.7 to ∼1.3 at most sites. For the marine-aerosol-dominated site Ascension Island the bias was higher, ∼1.4–1.9. In other words, at SS &gt;0.4 % NCCN was estimated with an average uncertainty of approximately 30 % by using nephelometer data. The biases were mainly due to the biases in the parameterization related to the scattering Ångström exponent (SAE). The squared correlation coefficients between the AOP-derived and measured NCCN varied from ∼0.5 to ∼0.8. To study the physical explanation of the relationships between NCCN and AOPs, lognormal unimodal particle size distributions were generated and NCCN and AOPs were calculated. The simulation showed that the relationships of NCCN and AOPs are affected by the geometric mean diameter and width of the size distribution and the activation diameter. The relationships of NCCN and AOPs were similar to those of the observed ones.

The sensitivity of Southern Ocean aerosols and cloud microphysics to sea spray and sulfate aerosol production in the HadGEM3-GA7.1 chemistry–climate model

Abstract. With low concentrations of tropospheric aerosol, the Southern Ocean offers a “natural laboratory” for studies of aerosol–cloud interactions. Aerosols over the Southern Ocean are produced from biogenic activity in the ocean, which generates sulfate aerosol via dimethylsulfide (DMS) oxidation, and from strong winds and waves that lead to bubble bursting and sea spray emission. Here, we evaluate the representation of Southern Ocean aerosols in the Hadley Centre Global Environmental Model version 3, Global Atmosphere 7.1 (HadGEM3-GA7.1) chemistry–climate model. Compared with aerosol optical depth (AOD) observations from two satellite instruments (the Moderate Resolution Imaging Spectroradiometer, MODIS-Aqua c6.1, and the Multi-angle Imaging Spectroradiometer, MISR), the model simulates too-high AOD during winter and too-low AOD during summer. By switching off DMS emission in the model, we show that sea spray aerosol is the dominant contributor to AOD during winter. In turn, the simulated sea spray aerosol flux depends on near-surface wind speed. By examining MODIS AOD as a function of wind speed from the ERA-Interim reanalysis and comparing it with the model, we show that the sea spray aerosol source function in HadGEM3-GA7.1 overestimates the wind speed dependency. We test a recently developed sea spray aerosol source function derived from measurements made on a Southern Ocean research voyage in 2018. In this source function, the wind speed dependency of the sea spray aerosol flux is less than in the formulation currently implemented in HadGEM3-GA7.1. The new source function leads to good agreement between simulated and observed wintertime AODs over the Southern Ocean; however, it reveals partially compensating errors in DMS-derived AOD. While previous work has tested assumptions regarding the seawater climatology or sea–air flux of DMS, we test the sensitivity of simulated AOD, cloud condensation nuclei and cloud droplet number concentration to three atmospheric sulfate chemistry schemes. The first scheme adds DMS oxidation by halogens and the other two test a recently developed sulfate chemistry scheme for the marine troposphere; one tests gas-phase chemistry only, while the second adds extra aqueous-phase sulfate reactions. We show how simulated sulfur dioxide and sulfuric acid profiles over the Southern Ocean change as a result and how the number concentration and particle size of the soluble Aitken, accumulation and coarse aerosol modes are affected. The new DMS chemistry scheme leads to a 20 % increase in the number concentration of cloud condensation nuclei and cloud droplets, which improves agreement with observations. Our results highlight the importance of atmospheric chemistry for simulating aerosols and clouds accurately over the Southern Ocean.

A New Method for Distinguishing Unactivated Particles in Cloud Condensation Nuclei Measurements: Implications for Aerosol Indirect Effect Evaluation

AbstractAn ongoing challenge for cloud condensation nuclei (CCN) measurements is the inclusion of unactivated particles, which affects droplet activation parameterizations and aerosol indirect effects in models. For the first time, a reciprocal relationship between the critical diameter and critical supersaturation of activated droplets from the κ‐Köhler theory is derived to accurately count unactivated particles in CCN measurements. We conducted 4‐day continuous observations to simultaneously measure the number concentration of CCN (NCCN) and aerosol. The results show that as supersaturation (SS) decreases from 0.186% at 25 °C, the proportion of the unactivated particles in the CCN measurements increases, reaching 88% at SS of 0.07%. Owing to the NCCN overestimation caused by NCCN‐SS parameterizations with uncorrected NCCN, there is significant overestimation of aerosol indirect effects, especially under low SS conditions. After removing unactivated particles, NCCN‐SS parameterizations are adjusted accordingly, which can improve simulations of aerosol‐cloud‐radiation interactions in models.

Cloud Ice Processes Enhance Spatial Scales of Organization in Arctic Stratocumulus

AbstractStratocumulus clouds around the globe tend to organize into cellular patterns, a phenomenon that has been primarily studied for the subtropical trade wind region. However, stratocumulus are also prevalent in high latitudes, where they often occur as mixed‐phase clouds. Yet little research has been conducted regarding mechanisms of cloud organization in the mixed‐phase regime. In cloud‐resolving model simulations we investigate the processes driving organization in open‐cell mixed‐phase stratocumuli. Similar to warm‐phase clouds, mixed‐phase clouds develop a subcloud circulation of evaporated/sublimated precipitation, cold pool formation, and consecutive updrafts driving new convective cells. For a larger ice to liquid water ratio, we find locally stronger precipitation and larger cloud cells. Hence, a higher concentration of ice nucleating particles can induce a breakup of the stratocumulus organization, with implications for the radiative balance at the surface. A decrease in cloud condensation nuclei concentration is also found to intensify precipitation and impact cloud organization.

Improvement of aerosol activation/ice nucleation in a source-oriented WRF-Chem model to study a winter Storm in California

Abstract The source-oriented Weather Research and Forecasting chemistry (SOWC) model is modified to improve mixed-phase cloud parameterization by including aerosol aging processes (external mixture) in cloud activation/nucleation. The improved SOWC model is applied to investigate how aerosol mixing state influences cloud and ice formation and atmospheric optical properties during a winter storm. SOWC tracks 6-dimensional chemical variables (X, Z, Y, Size Bins, Source Types, Species) through an explicit simulation of atmospheric chemistry and physics. A new module is implemented into the enhanced SOWC model to simulate microphysics processes with all source-oriented hydrometeors (cloud, ice, rain, snow and graupel) by using the modified Morrison two-moment microphysics scheme. In this study, all aerosol source types can activate to form cloud droplets based on the Kohler theory, but the dust source type is the only source of ice nuclei (IN). The Goddard shortwave and longwave radiation schemes are modified to use a new geometric optics method to estimate cloud optical properties by considering the chemistry components and the physical shape of each hydrometeor. The improved SOWC model is used to study a winter storm event that occurred on 6 March 2011, along the western coast of the United States. Compared to ground-based observations, SOWC with the modified Morrison microphysics scheme and modified Goddard radiation schemes predicts reasonable rainfall but the onset of precipitation is delayed by 6 h. Contact freezing is the main mechanism for ice nuclei formation over the ocean because of the number of collisions and large radius gaps between cloud droplets and ice nuclei. However, immersion freezing becomes the dominant nucleation process when the storm approached over land due to increased CCN concentrations and smaller radius gaps between cloud droplets and ice nuclei, especially for the internally mixed simulation, as well as the orographic lifting effect. Increasing CCN and IN in the internal mixing experiment results in 1.7% less rainfall and snowfall over the western coast of the United States.

Polarimetric Radar Convective Cell Tracking Reveals Large Sensitivity of Cloud Precipitation and Electrification Properties to CCN

AbstractHypotheses have been proposed for decades about the effect of activated cloud condensation nuclei (CCN) on delaying the warm rain process, invigorating deep convective cloud vertical development, and enhancing mixed‐phase processes. Observational support has been only qualitative with mixed results due to the lack of regional measurements of CCN concentration (NCCN), while simulations have not produced a robust consensus. Quantitative assessments of these relationships became possible with the advent of NCCN retrievals from satellites; when combined with measurements by polarimetric radar and Lightning Mapping Array (LMA), tracking convective cells observed on radar and examining precipitation properties throughout the cells' life cycle has permitted the study of the impact of NCCN on cloud and precipitation characteristics. We composited more than 2,800 well‐tracked cells in the Houston region and stratified them by NCCN, convective available potential energy (CAPE), and urban/rural locations. The results show that increased NCCN invigorates the convection until saturation near NCCN = 1,000 cm3; increasing NCCN from ~400 to an optimum of ~1,000 cm3 increases lightning activity by an order of magnitude. A further increase in CCN decreases lightning rates. Adding CAPE enhances lightning only under low NCCN (e.g., less than 500 cm3). The presence of the urban area enhances lightning for similar NCCN concentrations, although this applies mainly under low NCCN conditions. The urban heat island as manifested by cloud base height cannot explain this observation. It is suspected that the urban ultrafine aerosols contribute to the storm electrification.

Profiles of cloud condensation nuclei, dust mass concentration, and ice-nucleating-particle-relevant aerosol properties in the Saharan Air Layer over Barbados from polarization lidar and airborne in situ measurements

Abstract. The present study aims to evaluate lidar retrievals of cloud-relevant aerosol properties by using polarization lidar and coincident airborne in situ measurements in the Saharan Air Layer (SAL) over the Barbados region. Vertical profiles of the number concentration of cloud condensation nuclei (CCN), large particles (diameter d&gt;500 nm), surface area, mass, and ice-nucleating particle (INP) concentration are derived from the lidar measurements and compared with CCN concentrations and the INP-relevant aerosol properties measured in situ with aircraft. The measurements were performed in the framework of the Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) in summer 2013. The CCN number concentrations derived from lidar observations were up to a factor of 2 higher than the ones measured in situ aboard the research aircraft Falcon. Possible reasons for the difference are discussed. The number concentration of particles with a dry radius of more than 250 nm and the surface-area concentration obtained from the lidar observations and used as input for the INP parameterizations agreed well (&lt;30 %–50 % deviation) with the aircraft measurements. In a pronounced lofted dust layer during summer (10 July 2013), the lidar retrieval yielded 100–300 CCN per cubic centimeter at 0.2 % water supersaturation and 10–200 INPs per liter at −25 ∘C. Excellent agreement was also obtained in the comparison of mass concentration profiles. During the SALTRACE winter campaign (March 2014), the dust layer from Africa was mixed with smoke particles which dominated the CCN number concentration. This example highlights the unique lidar potential to separate smoke and dust contributions to the CCN reservoir and thus to identify the sensitive role of smoke in trade wind cumuli developments over the tropical Atlantic during the winter season.