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At least 19 records

Observations of anthropogenic cloud condensation nuclei

Cloud Condensation Nuclei (CCN) concentrations and spectral measurements obtained with the DRI instantaneous CCN spectrometer (Hudson, 1989) over the last few years are presented. The climatic importance of cloud microphysics has been pointed out. The particles which affect cloud microphysics are cloud condensation nuclei (CCN). The commonly-observed order of magnitude difference in cloud droplet concentrations between maritime and continental air masses (i.e., Squires, 1958) was determined to be caused by systematic differences in the concentrations of CCN between continental and maritime air masses (e.g., Twomey and Wojciechowski, 1969). Twomey (1977) first pointed out that cloud microphysics also affects the radiative properties of clouds. Thus continental and anthropogenic CCN could affect global temperature. Resolution of this Twomey effect requires answers to two questions - whether antropogenic CCN are a significant contribution to atmospheric CCN, and whether they are actually affecting cloud microphysics to an extent which is of climatic importance. The reasons for the contrast between continental and maritime CCN concentration are not understood. The question of the relative importance of anthropogenic CCN is addressed. These observations should shed light on this complex question although further research is being conducted in order to produce more quantitative answers. Accompanying CN measurements made with a TSI 3020 condensation nucleus (CN) counter are also presented.

Hudson, James G.↗

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.↗

Vertical Profiles of Cloud Condensation Nuclei, Condensation Nuclei, Optical Aerosol, Aerosol Optical Properties, and Aerosol Volatility Measured from Balloons

Under the support of this grant a balloon-borne gondola containing a variety of aerosol instruments was developed and flown from Laramie, Wyoming, (41 deg N, 105 deg W) and from Lauder, New Zealand (45 deg S, 170 deg E). The gondola includes instruments to measure the concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), optically detectable aerosol (OA.) (r greater than or equal to 0.15 - 2.0 microns), and optical scattering properties using a nephelometer (lambda = 530 microns). All instruments sampled from a common inlet which was heated to 40 C on ascent and to 160 C on descent. Flights with the CN counter, OA counter, and nephelometer began in July 1994. The CCN counter was added in November 1994, and the engineering problems were solved by June 1995. Since then the flights have included all four instruments, and were completed in January 1998. Altogether there were 20 flights from Laramie, approximately 5 per year, and 2 from Lauder. Of these there were one or more engineering problems on 6 of the flights from Laramie, hence the data are somewhat limited on those 6 flights, while a complete data set was obtained from the other 14 flights. Good CCN data are available from 12 of the Laramie flights. The two flights from Lauder in January 1998 were successful for all measurements. The results from these flights, and the development of the balloon-bome CCN counter have formed the basis for five conference presentations. The heated and unheated CN and OA measurements have been used to estimate the mass fraction of the aerosol volatile, while comparisons of the nephelometer measurements were used to estimate the light scattering, associated with the volatile aerosol. These estimates were calculated for 0.5 km averages of the ascent and descent data between 2.5 km and the tropopause, near 11.5 km.

Deshler, T.↗

Use of In Situ Cloud Condensation Nuclei, Extinction, and Aerosol Size Distribution Measurements to Test a Method for Retrieving Cloud Condensation Nuclei Profiles From Surface Measurements

If the aerosol composition and size distribution below cloud are uniform, the vertical profile of cloud condensation nuclei (CCN) concentration can be retrieved entirely from surface measurements of CCN concentration and particle humidification function and surface-based retrievals of relative humidity and aerosol extinction or backscatter. This provides the potential for long-term measurements of CCN concentrations near cloud base. We have used a combination of aircraft, surface in situ, and surface remote sensing measurements to test various aspects of the retrieval scheme. Our analysis leads us to the following conclusions. The retrieval works better for supersaturations of 0.1% than for 1% because CCN concentrations at 0.1% are controlled by the same particles that control extinction and backscatter. If in situ measurements of extinction are used, the retrieval explains a majority of the CCN variance at high supersaturation for at least two and perhaps five of the eight flights examined. The retrieval of the vertical profile of the humidification factor is not the major limitation of the CCN retrieval scheme. Vertical structure in the aerosol size distribution and composition is the dominant source of error in the CCN retrieval, but this vertical structure is difficult to measure from remote sensing at visible wavelengths.

Ghan, Stephen J.↗

Impacts of Varying Concentrations of Cloud Condensation Nuclei On Deep Convective Cloud Updrafts – A Multimodel Assessment

This study presents results from a model intercomparison project, focusing on the range of responses in deep convective cloud updrafts to varying cloud condensation nuclei (CCN) concentrations amongst seven, state-of-the-art, cloud-resolving models. Simulations of scattered convective clouds near Houston, Texas are conducted, after being initialized with both relatively low and high CCN concentrations. Deep convective updrafts are identified, and trends in the updraft intensity and frequency are assessed. The factors contributing to the vertical velocity tendencies are examined to identify the physical processes associated with the CCN-induced, updraft changes. The models show several consistent trends. In general, the changes between the High- CCN and Low-CCN simulations in updraft magnitudes throughout the depth of the troposphere are within 15% for all of the models. All models produce stronger (~+5-15%) mean updrafts from ~4–7 km above ground level (AGL) in the High-CCN simulations, followed by a waning response up to ~8 km AGL in most of the models. Thermal buoyancy was more sensitive than condensate loading to varying CCN concentrations in most of the models and more impactful in the mean updraft responses. However, there are also differences between the models. The change in the amount of deep convective updrafts varies significantly. Furthermore, approximately half the models demonstrate neutral-to-weaker (~-5-0%) updrafts above ~8 km AGL, while the other models show stronger (~+10%) updrafts in the High-CCN simulations. The combination of the CCN-induced impacts on the buoyancy and vertical perturbation pressure gradient terms better explains these middle- and upper-tropospheric updraft trends than the buoyancy terms alone.

deep convective cloud updrafts↗

Evaluation of Global Simulations of Aerosol Particle and Cloud Condensation Nuclei Number, with Implications for Cloud Droplet Formation

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011-2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of -24% and -35% for particles with dry diameters > 50 and > 120nm, as well as -36% and -34% for CCN at supersaturations of 0.2% and 1.0%, respectively. However, they seem to behave differently for particles activating at very low supersaturations (< 0.1%) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN(0.2)) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40% during winter and 20% in summer.

cloud droplets↗

Measurements of cloud condensation nuclei spectra within maritime cumulus cloud droplets: Implications for mixing processes

In a cloud formed during adiabatic expansion, the droplet size distribution will be systematically related to the critical supersaturation of the cloud condensation nuclei (CNN), but this relationship can be complicated in entraining clouds. Useful information about cloud processes, such as mixing, can be obtained from direct measurements of the CNN involved in droplet nucleation. This was accomplished by interfacing two instruments for a series of flights in maritime cumulus clouds. One instrument, the counterflow virtual impactor, collected cloud droplets, and the nonvolatile residual nuclei of the droplets was then passed to a CCN spectrometer, which measured the critical supersaturation (S(sub c)) spectrum of the droplet nuclei. The measured S(sub c) spectra of the droplet nuclei were compared with the S(sub c) spectra of ambient aerosol particles in order to identify which CCN were actually incorporated into droplets and to determine when mixing processes were active at different cloud levels. The droplet nuclei nearly always exhibited lower median S(sub c)'s than the ambient aerosol, as expected since droplets nucleate perferentially on particles with lower critical supersaturations. Critical supersaturation spectra from nuclei of droplets near cloud base were similar to those predicted for cloud regions formed adiabatically, but spectra of droplet nuclei from middle cloud levels showed some evidence that mixing had occurred. Near cloud top, the greatest variation in the spectra of the droplet nuclei was observed, and nuclei with high S(sub c)'s were sometimes present even within relatively large droplets. This suggests that the extent of mixing increases with height in cumulus clouds and that inhomogeneous mixing may be important near cloud top. These promising initial results suggest improvements to the experimental technique that will permit more quantitative results in future experiments.

Twohy, Cynthia H.↗

A Large Source of Cloud Condensation Nuclei from New Particle Formation in the Tropics

Cloud condensation nuclei (CCN) can affect cloud properties and therefore the Earth’s radiative balance. New particle formation (NPF) from condensable vapours in the free troposphere has been suggested to contribute to CCN, especially in remote, pristine atmospheric regions, but direct evidence is sparse, and the magnitude of this contribution is uncertain. Here we use in-situ aircraft measurements of vertical profiles of aerosol size distributions to present a global-scale survey of NPF occurrence. We observed intense NPF occurring at high altitude in tropical convective regions over both the Pacific and Atlantic Oceans. Together with the results of chemical-transport models, our findings indicate that NPF persists at all longitudes as a global-scale band in the tropical upper troposphere, covering about 40% of the Earth’s surface. Furthermore, we find that this NPF in the tropical upper troposphere is a globally important source of CCN in the lower troposphere, where they can affect cloud properties. Our findings suggest that the production of CCN, as these new particles descend towards the surface, is currently not adequately captured in global models, because they tend to underestimate both the magnitude of tropical upper tropospheric NPF and the subsequent growth to CCN sizes. This has potential implications for cloud albedo and the global radiative balance.

Atmospheric chemistry↗

Cloud condensation nuclei near marine cumulus

Extensive airborne measurements of cloud condensation nucleus (CCN) spectra and condensation nuclei below, in, between, and above the cumulus clouds near Hawaii point to important aerosol-cloud interactions. Consistent particle concentrations of 200/cu cm were found above the marine boundary layer and within the noncloudy marine boundary layer. Lower and more variable CCN concentrations within the cloudy boundary layer, especially very close to the clouds, appear to be a result of cloud scavenging processes. Gravitational coagulation of cloud droplets may be the principal cause of this difference in the vertical distribution of CCN. The results suggest a reservoir of CCN in the free troposphere which can act as a source for the marine boundary layer.

Hudson, James G.↗

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.↗

Multi-Campaign Ship and Aircraft Observations of Marine Cloud Condensation Nuclei and Droplet Concentrations

In-situ marine cloud droplet number concentrations (CDNCs), cloud condensation nuclei (CCN), and CCN proxies, based on particle sizes and optical properties, are accumulated from seven field campaigns: ACTIVATE; NAAMES; CAMP2EX; ORACLES; SOCRATES; MARCUS; and CAPRICORN2. Each campaign involves aircraft measurements, ship-based measurements, or both. Measurements collected over the North and Central Atlantic, Indo-Pacific, and Southern Oceans, represent a range of clean to polluted conditions in various climate regimes. With the extensive range of environmental conditions sampled, this data collection is ideal for testing satellite remote detection methods of CDNC and CCN in marine environments. Remote measurement methods are vital to expanding the available data in these difficult-to-reach regions of the Earth and improving our understanding of aerosolcloud interactions. The data collection includes particle composition and continental tracers to identify potential contributing CCN sources. Several of these campaigns include High Spectral Resolution Lidar (HSRL) and polarimetric imaging measurements and retrievals that will be the basis for the next generation of space-based remote sensors and, thus, can be utilized as satellite surrogates.

Atmospheric chemistry↗

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 near marine stratus

Extensive airborne measurements of cloud condensation nucleus (CCN) spectra and concentrations of total particles, or condensation nuclei (CN), below, in, and above the stratus cloud decks off the southern California coast point to important aerosol-cloud interactions. Consistently low CCN concentrations below cloud appear to be due to cloud scavenging processes which include Brownian coagulation, nucleation, coalescence, and drizzle. The higher CCN and CN concentrations above cloud are associated with ambient ozone concentrations which suggest a link with continental, probably anthropogenic, sources, even at distances of 500 km from the California coast.

Hudson, James G.↗

Rapid Cloud Removal of Dimethyl Sulfide Oxidation Products Limits SO 2 and Cloud Condensation Nuclei Production in the Marine Atmosphere

Oceans emit large quantities of dimethyl sulfide (DMS) to the marine atmosphere. The oxidation of 60 DMS leads to the formation and growth of cloud condensation nuclei (CCN) with consequent effects on Earth’s radiation balance and climate. Quantitative assessment of the impact of DMS emissions on CCN concentrations necessitates a detailed description of the oxidation of DMS in the presence of existing aerosol particles and clouds. In the unpolluted marine atmosphere, DMS is efficiently oxidized to hydroperoxymethyl thioformate (HPMTF), a stable intermediate in the chemical trajectory towards sulfur dioxide (SO 2 ) and ultimately sulfate aerosol (Veres et al. 2020). Using direct airborne flux measurements, we demonstrate that irreversible loss of HPMTF to clouds in the marine boundary layer determines the HPMTF lifetime (τ HPMTF < 2 hours) and terminates DMS oxidation to SO 2 in the cloudy marine boundary layer. When accounting for HPMTF cloud loss in a global chemical transport model, we show that SO 2 production from DMS is reduced by 35% globally and near surface (0-3km) SO 2 concentrations over the ocean are lowered by 24%. This large, previously unconsidered loss process for volatile sulfur accelerates the timescale for conversion of DMS to sulfate, while limiting new particle formation in the marine atmosphere and changing the dynamics of aerosol growth. This loss process potentially reduces the spatial scale over which DMS emissions contribute to aerosol production and growth and weakens the link between DMS emission and marine CCN production with subsequent implications for cloud formation, radiative forcing, and climate.

dimethyl sulfide↗

Cloud Condensation Nuclei Prediction Error from Application of Kohler Theory: Importance for the Aerosol Indirect Effect

In situ observations of aerosol and cloud condensation nuclei (CCN) and the GISS GCM Model II' with an online aerosol simulation and explicit aerosol-cloud interactions are used to quantify the uncertainty in radiative forcing and autoconversion rate from application of Kohler theory. Simulations suggest that application of Koehler theory introduces a 10-20% uncertainty in global average indirect forcing and 2-11% uncertainty in autoconversion. Regionally, the uncertainty in indirect forcing ranges between 10-20%, and 5-50% for autoconversion. These results are insensitive to the range of updraft velocity and water vapor uptake coefficient considered. This study suggests that Koehler theory (as implemented in climate models) is not a significant source of uncertainty for aerosol indirect forcing but can be substantial for assessments of aerosol effects on the hydrological cycle in climatically sensitive regions of the globe. This implies that improvements in the representation of GCM subgrid processes and aerosol size distribution will mostly benefit indirect forcing assessments. Predictions of autoconversion, by nature, will be subject to considerable uncertainty; its reduction may require explicit representation of size-resolved aerosol composition and mixing state.

Sotiropoulou, Rafaella-Eleni P.↗

Cloud Condensation Nuclei in the Early Martian Atmosphere

Explanations for how early Mars supported warmer and wetter conditions 3.5 to 4 billion years ago have long been debated. A water cloud greenhouse has been proposed as a mechanism of warming early Mars, but modeling studies of these environments produce mixed results. Studies show that both H 2 O and CO 2 clouds are capable of influencing atmospheric and surface temperatures, but the amount of warming induced is very sensitive to the cloud physics assumptions made. Producing a strong water cloud greenhouse effect is dependent on forming clouds as high in the atmosphere as possible to maximize warming. However, the majority of studies of H 2 O and CO 2 clouds on early Mars assume that a constant number of seed nuclei are available at all altitudes for clouds to condense onto. Here we test the validity of this assumption in massive CO 2 atmospheres. Explaining how dust is lofted into the middle atmosphere to serve as seed nuclei for cloud formation is a challenge even for present day Mars. This problem may change in an early Mars environment where having a more massive atmosphere could result in differences in the general circulation, vertical transport, and settling time scales of dust. Here, we begin a first-ever study of the early Mars dust cycle and how it might couple to the water cycle. We present early Mars simulations in which dust is injected at the surface and can be transported throughout the atmosphere. We explore the resulting vertical and horizontal distributions of dust particles and their sizes with an emphasis on the maximum height of the dust. We aim to investigate what the distribution of cloud condensation nuclei may have been on early Mars and how this might impact cloud formation.

Kathryn Steakley↗

Cloud Condensation Nuclei in FIRE III

Yum and Hudson showed that the springtime Arctic aerosol is probably a result of long-range transport at high altitudes. Scavenging of particles by clouds reduces the low level concentrations by a factor of 3. This produces a vertical gradient in particle concentrations when low-level clouds are present. Concentrations are uniform with height when clouds are not present. Low-level CCN (cloud condensation nuclei) spectra are similar to those in other maritime areas as found by previous projects including FIRE 1 and ASTEX, which were also supported on earlier NASA-FIRE grants. Wylie and Hudson carried this work much further by comparing the CCN spectra observed during ACE with back trajectories of air masses and satellite photographs. This showed that cloud scavenging reduces CCN concentrations at all altitudes over the springtime Arctic, with liquid clouds being more efficient scavengers than frozen clouds. The small size of the Arctic Ocean seems to make it more susceptible to continental and thus anthropogenic aerosol influences than any of the other larger oceans.

Hudson, James G.↗

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.↗