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Environmental effects on aerosol–cloud interaction in non-precipitating marine boundary layer (MBL) clouds over the eastern North Atlantic

Abstract. Over the eastern North Atlantic (ENA) ocean, a total of 20 non-precipitating single-layer marine boundary layer (MBL) stratus and stratocumulus cloud cases are selected to investigate the impacts of the environmental variables on the aerosol–cloud interaction (ACIr) using the ground-based measurements from the Department of Energy Atmospheric Radiation Measurement (ARM) facility at the ENA site during 2016–2018. The ACIr represents the relative change in cloud droplet effective radius re with respect to the relative change in cloud condensation nuclei (CCN) number concentration at 0.2 % supersaturation (NCCN,0.2 %) in the stratified water vapor environment. The ACIr values vary from −0.01 to 0.22 with increasing sub-cloud boundary layer precipitable water vapor (PWVBL) conditions, indicating that re is more sensitive to the CCN loading under sufficient water vapor supply, owing to the combined effect of enhanced condensational growth and coalescence processes associated with higher Nc and PWVBL. The principal component analysis shows that the most pronounced pattern during the selected cases is the co-variations in the MBL conditions characterized by the vertical component of turbulence kinetic energy (TKEw), the decoupling index (Di), and PWVBL. The environmental effects on ACIr emerge after the data are stratified into different TKEw regimes. The ACIr values, under both lower and higher PWVBL conditions, more than double from the low-TKEw to high-TKEw regime. This can be explained by the fact that stronger boundary layer turbulence maintains a well-mixed MBL, strengthening the connection between cloud microphysical properties and the below-cloud CCN and moisture sources. With sufficient water vapor and low CCN loading, the active coalescence process broadens the cloud droplet size spectra and consequently results in an enlargement of re. The enhanced activation of CCN and the cloud droplet condensational growth induced by the higher below-cloud CCN loading can effectively decrease re, which jointly presents as the increased ACIr. This study examines the importance of environmental effects on the ACIr assessments and provides observational constraints to future model evaluations of aerosol–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

Evaluation of aerosol–cloud interactions in E3SM using a Lagrangian framework

A Lagrangian framework is used to evaluate aerosol–cloud interactions in the U.S. Department of Energy's Energy Exascale Earth System Model (E3SM) version 1 (E3SMv1) for measurements taken at Graciosa Island in the Azores where a U.S. Department of Energy Atmosphere Radiation Measurement (ARM) site is located. This framework uses direct measurements of cloud condensation nuclei (CCN) concentration (instead of relying on satellite retrievals of aerosol optical depth) and incorporates a suite of ground-based ARM measurements, satellite retrievals, and meteorological reanalysis products that when applied to over a 1500 trajectories provides key insights into the evolution of low-level clouds and aerosol radiative forcing that is not feasible from a traditional Eulerian analysis framework. Significantly lower concentrations (40 %) of surface CCN concentration are measured when precipitation rates in 48 h back trajectories average above 1.2 mm d -1 in the Integrated Multi-satellitE Retrievals for Global Precipitation Measurement (IMERG) product. The depletion of CCN concentration when precipitation rates are elevated is nearly twice as large in the ARM observations compared to E3SMv1 simulations. The model CCN concentration bias remains significant despite modifying the autoconversion and accretion rates in warm clouds. As the clouds in trajectories associated with larger surface-based CCN concentration advect away from Graciosa Island, they maintain higher values of droplet number concentrations (N d ) over multiple days in observations and E3SM simulations compared to trajectories that start with lower CCN concentrations. The response remains robust even after controlling for meteorological factors such as lower troposphere stability, the degree of cloud coupling with the surface, and island wake effects. E3SMv1 simulates a multi-day aerosol effect on clouds and a Twomey radiative effect that is within 30 % of the ARM and satellite observations. However, the mean cloud droplet concentration is more than 2–3 times larger than in the observations. While Twomey radiative effects are similar amongst autoconversion and accretion sensitivity experiments, the liquid water path and cloud fraction adjustments are positive when using a regression model as opposed to negative when using the present-day minus pre-industrial aerosol emissions approach. This result suggests that tuning the autoconversion and accretion alone is unlikely to produce the desired aerosol susceptibilities in E3SMv1.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

African smoke particles act as cloud condensation nuclei in the wintertime tropical North Atlantic boundary layer over Barbados

Abstract. The number concentration and properties of aerosol particles serving as cloud condensation nuclei (CCN) are important for understanding cloud properties, including in the tropical Atlantic marine boundary layer (MBL), where marine cumulus clouds reflect incoming solar radiation and obscure the low-albedo ocean surface. Studies linking aerosol source, composition, and water uptake properties in this region have been conducted primarily during the summertime dust transport season, despite the region receiving a variety of aerosol particle types throughout the year. In this study, we compare size-resolved aerosol chemical composition data to the hygroscopicity parameter κ derived from size-resolved CCN measurements made during the Elucidating the Role of Clouds–Circulation Coupling in Climate (EUREC4A) and Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) campaigns from January to February 2020. We observed unexpected periods of wintertime long-range transport of African smoke and dust to Barbados. During these periods, the accumulation-mode aerosol particle and CCN number concentrations as well as the proportions of dust and smoke particles increased, whereas the average κ slightly decreased (κ=0.46±0.10) from marine background conditions (κ=0.52±0.09) when the submicron particles were mostly composed of marine organics and sulfate. Size-resolved chemical analysis shows that smoke particles were the major contributor to the accumulation mode during long-range transport events, indicating that smoke is mainly responsible for the observed increase in CCN number concentrations. Earlier studies conducted at Barbados have mostly focused on the role of dust on CCN, but our results show that aerosol hygroscopicity and CCN number concentrations during wintertime long-range transport events over the tropical North Atlantic are also affected by African smoke. Our findings highlight the importance of African smoke for atmospheric processes and cloud formation over the Caribbean.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Improving the Confidence in Retrievals of Vertical Distributions of Cloud Condensation Nuclei Number Concentration from ARM Supported by Aircraft In Situ Observations

Accurate quantification of the vertical distribution of cloud condensation nuclei (CCN) number concentrations is critical for improving our understanding of aerosol–cloud interactions. Ground-based Raman lidars operated by the Atmospheric Radiation Measurement (ARM) program, together with surface CCN measurements, are used to retrieve vertically resolved CCN number concentrations (Retrieved Number concentration of CCN, RNCCN). These retrievals rely on several assumptions, including that aerosol composition is vertically homogeneous. To assess this assumption, we developed and tested a framework to infer the dominant aerosol classes/types at different altitudes. This was done by applying a k-Nearest-Neighbors (kNN) algorithm to lidar ratio and linear depolarization ratio measurements from Raman lidar. We evaluated the framework using aircraft aerosol and CCN measurements from the ARM Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) field campaign. The results show that RNCCN performance degrades as vertical aerosol complexity increases, i.e., RNCCN agrees with the aircraft CCN in vertically homogeneous conditions, but closure decreases in layered aerosol structures. To generalize beyond individual examples, we introduce a metric (heterogeneity index) that quantifies the vertical complexity by assessing the variation of inferred aerosol classes/types. Case-level statistics show a tendency for RNCCN and aircraft differences to increase with this metric. By detecting retrievals that are likely compromised by aerosol vertical heterogeneity, the proposed framework improves the interpretability and effective use of RNCCN used for long-term evaluation of models and aerosol–cloud interactions.

Tian, Jingjing↗

The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

Cloud microphysics are inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e.,pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.A spectral-bin microphysical model is very expensive from a from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Besides the initial differences in aerosol concentration, preliminary results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CCN case but has less cloud water mass aloft. Because the spectral-bin model explicitly calculates and allows for the examination of both the mass and number concentration of species in each size categor, a detailed analysis of the instantaneous size spectrum can be obtained for the two cases. It is shown that since the low CCN case produces fewer droplets, larger sized develop due to the greater condensational and collectional growth, leading to a broader size spectrum in comparison to the high CCN case.

Tao, Wei-Kuo↗

The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

Cloud microphysics are inevitable affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distribution parameterized as spectral bin microphysics are needed to explicitly study the effect of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensembel (GCE) model. The formulation for the explicit spectral-bim microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e., pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), groupel and frozen drops/hall] Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep cloud systems in the west Pacific warm pool region and in the mid-latitude using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Besides the initial differences in aerosol concentration, preliminary results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CCN case but has less cloud water mass aloft. Because the spectral-bim model explicitly calculates and allows for the examination of both the mass and number concentration of cpecies in each size category, a detailed analysis of the instantaneous size spectrum can be obtained for the two cases. It is shown that since the low CCN case produces fever droplets, larger size develop due to greater condencational and collectional growth, leading to a broader size spectrum in comparison to the high CCN case.

Tao, Wei-Kuo↗

On the Effect of Dust Particles on Global Cloud Condensation Nuclei and Cloud Droplet Number

Aerosol-cloud interaction studies to date consider aerosol with a substantial fraction of soluble material as the sole source of cloud condensation nuclei (CCN). Emerging evidence suggests that mineral dust can act as good CCN through water adsorption onto the surface of particles. This study provides a first assessment of the contribution of insoluble dust to global CCN and cloud droplet number concentration (CDNC). Simulations are carried out with the NASA Global Modeling Initiative chemical transport model with an online aerosol simulation, considering emissions from fossil fuel, biomass burning, marine, and dust sources. CDNC is calculated online and explicitly considers the competition of soluble and insoluble CCN for water vapor. The predicted annual average contribution of insoluble mineral dust to CCN and CDNC in cloud-forming areas is up to 40 and 23.8%, respectively. Sensitivity tests suggest that uncertainties in dust size distribution and water adsorption parameters modulate the contribution of mineral dust to CDNC by 23 and 56%, respectively. Coating of dust by hygroscopic salts during the atmospheric aging causes a twofold enhancement of the dust contribution to CCN; the aged dust, however, can substantially deplete in-cloud supersaturation during the initial stages of cloud formation and can eventually reduce CDNC. Considering the hydrophilicity from adsorption and hygroscopicity from solute is required to comprehensively capture the dust-warm cloud interactions. The framework presented here addresses this need and can be easily integrated in atmospheric models.

Karydis, V. A.↗

Retrieved Number concentration of Cloud Condensation Nuclei (RNCCN) Value-Added Product (VAP)

The objective of Retrieved Number concentration of Cloud Condensation Nuclei (RNCCN) Value-Added Product (VAP) is to provide the vertical distribution of cloud condensation nuclei (CCN) number concentrations to better represent aerosol indirect effects in climate models. The RNCCN VAP allows to collect a large number of independent samples of vertical CCN measurements at various supersaturation values from the ground. This helps to avoid the high cost of aircraft and increases the temporal distribution of retrieved CCN in the planetary boundary layer. The VAP method is based on Ghan and Collins (2004) and Ghan et al. (2006) proposed parameterizations that retrieve the vertical profiles of CCN directly from the ground level CCN, humidification factor, and in-situ lidar measurements. Further, the VAP accuracy is improved by using the quality controlled data that ensures that the boundary layer is well mixed.

54 ENVIRONMENTAL SCIENCES↗

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

Abstract The maximum supersaturation ( S x ) in clouds is a key parameter affecting the cloud's microphysical and radiative properties. We investigate the S x of the marine boundary layer clouds by combining airborne and surface observations in the Eastern North Atlantic. The cloud droplet number concentration ( N c ) 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 S x 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 S x 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 S x . The influence of CCN concentration on S x leads to a buffered response of N c to aerosol perturbations. The response of N c to low aerosol concentration during winter is further buffered by the high w . The global Community Earth System Model (CESM) simulated S x values in the Azores have a positive bias compared to measured S x , likely due to overestimated w and underestimated CCN concentration. The CESM simulated S x exhibits higher values further north over the North Atlantic Ocean, which is attributed to stronger w . The suppression of S x by aerosol is also evident in regions with high CCN concentrations.

54 ENVIRONMENTAL SCIENCES↗

Peak Rain Rate Sensitivity to Observed Cloud Condensation Nuclei and Turbulence in Continental Warm Shallow Clouds During CACTI

Abstract Warm clouds strongly affect Earth's energy budget but remain imperfectly represented in climate models, partly due to the complexity and covariability of relevant processes influencing warm rain. This work presents a detailed analysis of different factors affecting rain rate peak intensity (RR) in continental warm clouds. Clouds were identified with vertically pointing radar and lidar observations and categorized via a temperature‐based cloud type classification algorithm from which warm clouds were isolated. Observations and retrievals of liquid water path (LWP), cloud condensation nuclei concentration (N CCN ), cloud depth, and cloud duration of more than 3,000 separate warm clouds sampled during the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign are analyzed in this work. Multiple linear regression (MLR) and random forest (RF) models are applied to assess the relative impact of these variables on RR. Overall, RR tends to increase as cloud depth, LWP, and cloud duration increase, or N CCN decreases. Cloud depth affects RR the most while N CCN impacts it the least. When considering over 170 warm clouds observed at least 1 hr in which in‐cloud turbulence is retrieved, the effect of N CCN on RR remains most likely suppressive, but it is not significant at a 75% level for MLR and is highly uncertain for RF. The impact of in‐cloud turbulence depends on the moment and location it is sampled. Cloud base turbulence around the time of RR suppresses RR, while cloud top turbulence effects are inconclusive. Possible difficulties in isolating robust CCN and turbulence effects on RR are discussed.

54 ENVIRONMENTAL SCIENCES↗

Impact of Anthropogenic Aerosol Transport on Cloud Condensation Nuclei Activity During Summertime in Qilian Mountain, in the Northern Tibetan Plateau

Here in this study, we conducted field campaigns at two mountain-top observatories on the Qilian Mountains (QLM) in the northeastern Tibetan Plateau of China, which plays a vital role in sustaining water resources for the downstream arid and semi-arid regions. The two observatories, Waliguan Baseline Observatory (WLG) and Laohugou station (LHG), are situated on the eastern and western edge of the QLM, respectively. The objectives of this study were to examine the properties of atmospheric aerosols, CCN concentrations (NCCN) at varying supersaturation levels (SS = 0.2%–1.0%), and the hygroscopic nature of aerosols in the QLM, especially during the formation of orographic cloud. Notably, the average aerosol concentration and N CCN was approximately 2–3 factors higher at WLG compared to LHG. The chemical compositions of aerosols were primarily dominated by sulfate and organic aerosol (OA) at these two sites. A very high hygroscopicity parameter of aerosol calculated using chemical composition was observed at these two sites (0.37 ± 0.03 at LHG vs. 0.30 ± 0.04 at WLG). Enhanced aerosol loading episodes impacted by anthropogenic emission were observed at these two sites. Exploration on high-loading cases at each site, we found that the CCN activity was dominated by aerosol size, but the chemical processes of aerosol during the formation of orographic cloud could also be important in CCN activity, especially for low SS conditions. These findings collectively underscore the significant impact of anthropogenic air plumes on CCN concentrations in the QLM and their potential influence on precipitation patterns.

54 ENVIRONMENTAL SCIENCES↗

Vertical Aerosol Profiling during SAIL (VAPS) Field Campaign Report

To more fully address the science goals of the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility’s Surface Atmosphere Integrated Field Laboratory (SAIL) campaign, particularly the key science question of “How strongly do aerosols affect the surface energy and water balance by altering clouds, precipitation, and surface albedo, and how do these impacts vary seasonally?”, our campaign added instrumentation to planned tethered balloon system (TBS) flights in May and July of 2022. A key aspect of aerosol-cloud interactions is understanding cloud condensation nuclei (CCN) and ice nucleating particle (INP) populations, and how they vary seasonally and spatially. Because the interactions between aerosols and clouds is the target of this work, vertical distributions are particularly important to evaluate. Measurements of aerosol at ground level, below-cloud, and in-cloud will allow a better understanding of the airmasses that are feeding cloud-active particles into low- and mid-level clouds. Measurements of INP and aerosol populations often differ between the ground and aloft, with relationships that likely depend on regional and seasonal. Because of this, collocated measurements of aerosol, CCN, and INP, across different seasons, are crucial to reducing uncertainties in relationships between ground-level and cloud-base aerosol populations. Our campaign added online measurements of CCN using a compact CCN counter and offline filter collections for measurement of INP populations to the SAIL campaign TBS flights in May and July of 2022. The CCN instrument, the CloudPuck, flew and successfully collected data for a total of eight flights across both campaign periods. The IcePuck flew for most flights during the same period. Both instruments have continued to be used for other campaign requests in the SAIL domain. Analysis of this data was proposed through a concurrent DOE Atmospheric System Research (ASR) project submission, which was not funded in 2022. A similar proposal, which would involve analysis of the samples and data collected from this campaign, has been resubmitted in 2023 but a funding decision has not yet been made. If the proposal is again declined, we will seek other resources to ensure that this data can be analyzed.

54 ENVIRONMENTAL SCIENCES↗

Long-range transported continental aerosol in the eastern North Atlantic: three multiday event regimes influence cloud condensation nuclei

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

54 ENVIRONMENTAL SCIENCES↗

Dimethylsulfide/cloud condensation nuclei/climate system - Relevant size-resolved measurements of the chemical and physical properties of atmospheric aerosol particles

The mass and number relationships occurring within the atmospheric dimethylsulfide/cloud condensation nuclei (CCN)/climate system, using simultaneous measurements of particulate phase mass size distributions of nss SO4(2-), methanesulfonic acid (MSA), and NH4(+); number size distributions of particles having diameters between 0.02 and 9.6 microns; CCN concentrations at a supersaturation of 0.3 percent; relative humidity; and temperature, obtained for the northeastern Pacific Ocean in April and May 1991. Based on these measurements, particulate nss SO4(2-), MSA, and NH4(+) mass appeared to be correlated with both particle effective surface area and number in the accumulation mode size range (0.16 to 0.5 micron). No correlations were found in the size range below 0.16 micron. A correlation was also found between nss SO4(2-) mass and the CCN number concentration, such that a doubling of the SO4(2-) mass corresponded to a 40 percent increase in the CCN number concentration. However, no correlation was found between MSA mass and CCN concentration.

Quinn, P. K.↗

A Balloon-Borne Cloud Condensation Nuclei Counter

A balloon-borne instrument was constructed for observations of vertical profiles of cloud condensation nucleus (CCN) concentrations, active at 1% supersaturation. Droplet concentration in the static thermal-gradient diffusion chamber is deduced from the amount of scattered laser light detected by a photodetector. The photodetector is calibrated using a video camera and computer system to count the number of droplets produced from NaCl aerosol. Preliminary data are available from nine early morning profiles obtained at Laramie, Wyoming, between June 1995 and January 1997. To complement the CCN measurements, instruments that measure condensation nuclei (CN) and aerosols with diameter greater than 0.30 micrometers (D(sub 0.3) were also included on the balloon package. CCN concentrations exhibited a general decrease from the surface to the top of the boundary layers, were generally uniform through well-mixed layers, and show variability above well-mixed layers. In general, the structure of the CCN profile appears to be closely related to the structure in the CN and D(sub 0.3) profiles. Summer profiles generally have CCN concentration greater than 200/cu cm up to 500 mbar, whereas winter profiles are less than 200/cu cm at all levels.

Delene, David J.↗

Radiative Importance of Aerosol-Cloud Interaction

Aerosol particles are input into the troposphere by biomass burning, among other sources. These aerosol palls cover large expanses of the earth's surface. Aerosols may directly scatter solar radiation back to space, thus increasing the earth's albedo and act to cool the earth's surface and atmosphere. Aerosols also contribute to the earth's energy balance indirectly. Hygroscopic aerosol act as cloud condensation nuclei (CCN) and thus affects cloud properties. In 1977, Twomey theorized that additional available CCN would create smaller but more numerous cloud droplets in a cloud with a given amount of liquid water. This in turn would increase the cloud albedo which would scatter additional radiation back to space and create a similar cooling pattern as the direct aerosol effect. Estimates of the magnitude of the aerosol indirect effect on a global scale range from 0.0 to -4.8 W/sq m. Thus the indirect effect can be of comparable magnitude and opposite in sign to the estimates of global greenhouse gas forcing Aerosol-cloud interaction is not a one-way process. Just as aerosols have an influence on clouds through the cloud microphysics, clouds have an influence on aerosols. Cloud droplets are solutions of liquid water and CCN, now dissolved. When the cloud droplet evaporates it leaves behind an aerosol particle. This new particle does not have to have the same properties as the original CCN. In fact, studies show that aerosol particles that result from cloud processing are larger in size than the original CCN. Optical properties of aerosol particles are dependent on the size of the particles. Larger particles have a smaller backscattering fraction, and thus less incoming solar radiation will be backscattered to space if the aerosol particles are larger. Therefore, we see that aerosols and clouds modify each other to influence the radiative balance of the earth. Understanding and quantifying the spatial and seasonal patterns of the aerosol indirect forcing may have even greater consequences. Presently we know that through the use of fossil fuel and land-use changes we have increased the concentration of greenhouse gases in the atmosphere. In parallel, we have seen a modest increase of global temperature in the last century. These two observations have been linked as cause and effect by climate models, but this connection is still experimentally not verified. The spatial and seasonal distribution of aerosol forcing is different from that of greenhouse gases, thus generating a different spatial fingerprint of climate change. This fingerprint was suggested as a method to identify the response of the climate system to anthropogenic forcing of greenhouse gases and aerosol. The aerosol fingerprint may be the only way to firmly establish the presence (or absence) of human impact on climate. Aerosol-cloud interaction through the indirect effect will be an important component of establishing this fingerprint.

Tsay, Si-Chee↗

Cloud Condensation Nuclei in Fire-3

The centerpiece of this research was the cloud condensation nuclei (CCN) measurements of the Desert Research Institute (DRI) CCN spectrometers on board the NCAR C-130 aircraft during the Arctic Cloud Experiment (ACE) in May, 1998. These instruments operated successfully throughout all eight 10-hour research flights based in Fairbanks and the two ferry flights between Colorado and Fairbanks. Within a few months of completion of ACE the CCN data was edited and put into the archives. A paper was completed and published on the CCN climatology during the previous two FIRE field projects-FIRE 1 based in San Diego in June and July, 1987 and ASTEX based in the Azores Islands in June, 1992. This showed distinct contrasts in concentrations and spectra between continental and maritime CCN concentrations, which depended on air mass trajectories. Pollution episodes from Europe had distinct influences on particle concentrations at low altitudes especially within the boundary layer. At higher altitudes concentrations were similar in the two air mass regimes. Cloudier atmospheres showed lower concentrations especially below the clouds, which were a result mostly of coalescence scavenging.

Source record↗

Cloud Condensation Nuclei Measurements in Tropical Cyclones

The first measurements of cloud condensation nuclei (CCN) within and around tropical cyclones were made with the Desert Research Institute (DRI) CCN spectrometer (Hudson 1909) from a NOAA P-3 Hurricane Hunter aircraft throughout the 2001 season. Two penetrations of the closed eye of Hurricane Erin off the northeast US coast on Sept. 10 showed concentrations consistently well in excess of 1000 per cubic cm at approximately 1.4% supersaturation. Simultaneous condensation nuclei (CN--total particle) concentrations were consistently well in excess of 2000 per cubic cm throughout these closed eye penetrations. These within eye measurements at 4 km altitude for exceeded CCN and CN measurements just outside of the storm at similar altitudes--300 and 600 per cubic cm respectively. These CCN and CN concentrations within this closed eye were far above concentrations in maritime air masses; they are characteristic of continental or polluted air masses. Although there was a possibility that Saharan duct may have gotten into this storm these sub tenth micrometer particles are much too small and much too numerous to be dust. Such high concentrations may have originated from European air pollution, which may have been transported by similar airflow patterns to those that carry Saharan dust across the Atlantic. These high concentrations may be a manifestation of descending air that brings higher concentrations that are often characteristic of the upper troposphere (Clarke and Kapustin 2002). Later in the month measurements in Humberto showed highly variable CCN and CN concentrations that ranged from lots than 5 per cubic cm to more than 1000 per Cubic cm over km scale distances within and around the open eye of this tropical storm/hurricane. These very low concentrations suggest strong cloud scavenging.

Hudson, J. G.↗