Source Of Cloud Condensation Nuclei Research Articles

"Sizing" Heterogeneous Chemistry in the Conversion of Gaseous Dimethyl Sulfide to Atmospheric Particles.

The oxidation of biogenic dimethyl sulfide (DMS) emissions is a global source of cloud condensation nuclei. The amounts of the nucleating H2SO4(g) species produced in such process, however, remain uncertain. Hydrophobic DMS is mostly oxidized in the gas phase into H2SO4(g) + DMSO(g) (dimethyl sulfoxide), whereas water-soluble DMSO is oxidized into H2SO4(g) in the gas phase and into SO4(2-) + MeSO3(-) (methanesulfonate) on water surfaces. R = MeSO3(-)/(non-sea-salt SO4(2-)) ratios would therefore gauge both the strength of DMS sources and the extent of DMSO heterogeneous oxidation if Rhet = MeSO3(-)/SO4(2-) for DMSO(aq) + ·OH(g) were known. Here, we report that Rhet = 2.7, a value obtained from online electrospray mass spectra of DMSO(aq) + ·OH(g) reaction products that quantifies the MeSO3(-) produced in DMSO heterogeneous oxidation on aqueous aerosols for the first time. On this basis, the inverse R dependence on particle radius in size-segregated aerosol collected over Syowa station and Southern oceans is shown to be consistent with the competition between DMSO gas-phase oxidation and its mass accommodation followed by oxidation on aqueous droplets. Geographical R variations are thus associated with variable contributions of the heterogeneous pathway to DMSO atmospheric oxidation, which increase with the specific surface area of local aerosols.

Mechanism of New Particle Formation and Growth as well as Environmental Effects under Complex Air Pollution in China

New particle formation (NPF) and its subsequent growth plays a key role in air quality and climate change at regional and global scales. Especially under complex air pollution in China, nucleation and growth can be highly efficient, claimed to be a main source of cloud condensation nuclei (CCN) and an important cause of secondary aerosol pollution. Cur- rently, the mechanism of particle formation and growth as well as its environmental effects are still poorly understood. Thereby, fully understanding of the atmospheric nucleation and subsequent growth still presents a big challenge to atmos- pheric chemistry researches. This study reviews the current results from studies on mechanisms and environmental effects of atmospheric nucleation and growth. We summarize that traditional nucleation theories such as binary nucleation of H2SO4-H2O, ternary nucleation of H2SO4-NH3-H2O, ion-induced nucleation are not capable in explaining new particle for- mation under complex air pollution, while newly proposed mechanisms such as organic acids and amine induced nucleation were not verified because of technique limitation. We propose that the future researches should focus on identifying the key chemical precursor response for driving nucleation and initial and subsequent growth, and understand the physical and chem- ical processing of new particle formation and growth. In particularly, application and development of novel techniques, such as APi-TOF-CIMS, PSM, Nano-HTDMA in new particle formation study is very important. Also, future researches should establish whole process tracking on new particle formation, from precursor, nucleation, growth till the environmental effects, by integrating field observation, chamber simulation, and modelling. Currently, the mechanism of highly efficient nucleation and rapid growth taking place under complex air pollution in China is urgently needed to be in-depth studied in order to im- prove our understanding of regional haze formation. This could be helpful to understand the similarity and difference in the nucleation mechanism between clean and polluted atmospheric environments. Keywords new particle formation; particle growth; transformation mechanism; environmental impact; complex air pollu- tion

Some insights into the condensing vapors driving new particle growth to CCN sizes on the basis of hygroscopicity measurements

Abstract. New particle formation (NPF) and growth is an important source of cloud condensation nuclei (CCN). In this study, we investigated the chemical species driving new particle growth to the CCN sizes on the basis of particle hygroscopicity measurements carried out at the research station Melpitz, Germany. Three consecutive NPF events occurred during summertime were chosen as examples to perform the study. Hygroscopicity measurements showed that the (NH4)2SO4-equivalent water-soluble fraction accounts for 20 and 16 % of 50 and 75 nm particles, respectively, during the NPF events. Numerical analysis showed that the ratios of H2SO4 condensational growth to the observed particle growth were 20 and 13 % for 50 and 75 nm newly formed particles, respectively. Aerosol mass spectrometer measurements showed that an enhanced mass fraction of sulfate and ammonium in the newly formed particles was observed when new particles grew to the sizes larger than 30 nm shortly after the particle formation period. At a later time, the secondary organic species played a key role in the particle growth. Both hygroscopicity and aerosol mass spectrometer (AMS) measurements and numerical analysis confirmed that organic compounds were major contributors driving particle growth to CCN sizes. The critical diameters at different supersaturations estimated using AMS data and κ-Köhler theory increased significantly during the later course of NPF events. This indicated that the enhanced organic mass fraction caused a reduction in CCN efficiency of newly formed particles. Our results implied that the CCN production associated with atmospheric nucleation may be overestimated if assuming that newly formed particles can serve as CCN once they grow to a fixed particle size, an assumption made in some previous studies, especially for organic-rich environments. In our study, the enhancement in CCN number concentration associated with individual NPF events were 63, 66, and 69 % for 0.1, 0.4, and 0.6 % supersaturation, respectively.

Atmospheric new particle formation as a source of CCN in the eastern Mediterranean marine boundary layer

Abstract. While cloud condensation nuclei (CCN) production associated with atmospheric new particle formation (NPF) is thought to be frequent throughout the continental boundary layers, few studies on this phenomenon in marine air exist. Here, based on simultaneous measurement of particle number size distributions, CCN properties and aerosol chemical composition, we present the first direct evidence on CCN production resulting from NPF in the eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles to CCN sizes in this environment during the summertime. Sub-100 nm particles were found to be substantially less hygroscopic than larger particles during the period with active NPF and growth (the value of κ was lower by 0.2–0.4 for 60 nm particles compared with 120 nm particles), probably due to enrichment of organic material in the sub-100 nm size range. The aerosol hygroscopicity tended to be at minimum just before the noon and at maximum in the afternoon, which was very likely due to the higher sulfate-to-organic ratios and higher degree of oxidation of the organic material during the afternoon. Simultaneous with the formation of new particles during daytime, particles formed during the previous day or even earlier were growing into the size range relevant to cloud droplet activation, and the particles formed in the atmosphere were possibly mixed with long-range-transported particles.

Investigating the significance of zero-point motion in small molecular clusters of sulphuric acid and water

The nucleation of particles from trace gases in the atmosphere is an important source of cloud condensation nuclei, and these are vital for the formation of clouds in view of the high supersaturations required for homogeneous water droplet nucleation. The methods of quantum chemistry have increasingly been employed to model nucleation due to their high accuracy and efficiency in calculating configurational energies; and nucleation rates can be obtained from the associated free energies of particle formation. However, even in such advanced approaches, it is typically assumed that the nuclei have a classical nature, which is questionable for some systems. The importance of zero-point motion (also known as quantum nuclear dynamics) in modelling small clusters of sulphuric acid and water is tested here using the path integral molecular dynamics method at the density functional level of theory. The general effect of zero-point motion is to distort the mean structure slightly, and to promote the extent of proton transfer with respect to classical behaviour. In a particular configuration of one sulphuric acid molecule with three waters, the range of positions explored by a proton between a sulphuric acid and a water molecule at 300 K (a broad range in contrast to the confinement suggested by geometry optimisation at 0 K) is clearly affected by the inclusion of zero point motion, and similar effects are observed for other configurations.

Free troposphere as a major source of CCN for the equatorial pacific boundary layer: long-range transport and teleconnections

Abstract. Airborne aerosol measurements in the central equatorial Pacific during PASE (Pacific Atmospheric Sulfur Experiment) revealed that cloud condensation nuclei (CCN) activated in marine boundary layer (MBL) clouds were strongly influenced by entrainment from the free troposphere (FT). About 65% entered at sizes effective as CCN in MBL clouds, while ~25% entered the MBL too small to activate but subsequently grew via gas to particle conversion. The remaining ~10% were inferred to be sea salt aerosol. FT aerosols at low carbon monoxide (CO) mixing ratios (< 63 ppbv) were mostly volatile at 360 °C with a number mode peak of around 30–40 nm dry diameter and tended to be associated with cloud outflow from distant (3000 km or more) deep convection. Higher CO concentrations were commonly associated with trajectories from South America and the Amazon region (ca. ~10 000 km away) and occurred in layers indicative of combustion sources (biomass burning season) partially scavenged by precipitation. These had number modes near 60–80 nm dry diameter with a large fraction of CCN.2 (those activated at 0.2% supersaturation and representative of MBL clouds) prior to entrainment into the MBL. Flight averaged concentrations of CCN.2 were similar for measurements near the surface, below the inversion and in the FT just above the inversion, confirming that subsidence and entrainment of FT aerosol strongly influenced MBL CCN.2. Concurrent flight-to-flight variations of CCN.2 at all altitudes below 3 km also imply MBL CCN.2 concentrations were in quasi-equilibrium with the FT over a 2–3 day timescale. The observed FT transport over thousands of kilometers indicates teleconnections between MBL CCN and cloud-scavenged sources of both natural and/or residual combustion origin. Nonetheless, in spite of its importance, this source of CCN number is not well represented in most current models and is generally not detectable by satellite because of the low aerosol scattering in such layers as a result of cloud scavenging. In addition, our measurements confirm nucleation in the MBL was not evident during PASE and argue against a localized linear relation in the MBL between dimethyl sulfide (DMS) and CCN suggested by the CLAW hypothesis. However, when the FT is not impacted by long-range transport, sulfate aerosol derived from DMS pumped aloft in the ITCZ (Inter-Tropical Convergence Zone) can provide a source of CCN to the boundary layer via FT teleconnections involving more complex non-linear processes.

Aircraft Measurements of Atmospheric Aerosol over North China in Autumn

Using an aircraft equipped with Passive Cavity Aerosol Spectrum Probe (PCASP-100X) and streamwise thermal gradient cloud condensation nuclei (CCN) counter, six flight measurements of atmospheric aerosol and CCN were conducted over North China in autumn. Five flight observations over Shijiazhuang urban area show that there is great difference of aerosol microphysical character between clear day and haze day. Vertical distributions show that aerosols mainly concentrated on the levels from near surface to the low level of troposphere and the concentration generally decreased with height increasing. The max aerosol concentration was 8110 cm-3on haze day and 1614 cm-3on clear day. There was more than 4 times difference in concentration of aerosol in boundary layer between haze day and clear day. CCN has the similar vertical distributions as aerosol. Most CCN concentrated on the boundary layer suggesting that the main source of CCN is from surface. Observation over Bohai Bay shows that the marine aerosol and CCN were greatly influenced by anthropogenic emissions.

Spatial and Temporal Distribution of Clouds Observed by MODIS Onboard the Terra and Aqua Satellites

Cloud properties have been retrieved from the Moderate Resolution Imaging Spectroradiometer (MODIS) over 12 years of continuous observations from Terra and over nine years from Aqua. Results include the spatial and temporal distribution of cloud fraction, the cloud top pressure and cloud top temperature, and the cloud optical thickness and effective radius of both liquid water and ice clouds. Globally, the cloud fraction derived by the MODIS cloud mask is ~ 67%, with somewhat more clouds over land during the afternoon and less clouds over ocean in the afternoon, with very little difference in global cloud cover between Terra and Aqua. Overall, the cloud fraction over land is ~ 55%, with a distinctive seasonal cycle, whereas the ocean cloudiness is much higher, around 72%, with much reduced seasonal variation. Aqua and Terra have comparable zonal cloud top pressures, with Aqua having somewhat higher clouds (cloud top pressures lower by 100 hPa) over land due to afternoon deep convection. The coldest cloud tops (colder than 230 K) generally occur over Antarctica and the high clouds in the tropics. The cloud effective particle radius of liquid water clouds is significantly larger over ocean (mode 12-13 μm) than land (mode 10-11 μm), consistent with the variation in hygroscopic aerosol concentrations that provide cloud condensation nuclei necessary for cloud formation. We also find the effective radius to be 2-3 μm larger in the southern hemisphere than in the northern hemisphere, likely reflecting differences in sources of cloud condensation nuclei.

Comparison between summertime and wintertime Arctic Ocean primary marine aerosol properties

Abstract. Primary marine aerosols (PMAs) are an important source of cloud condensation nuclei, and one of the key elements of the remote marine radiative budget. Changes occurring in the rapidly warming Arctic, most importantly the decreasing sea ice extent, will alter PMA production and hence the Arctic climate through a set of feedback processes. In light of this, laboratory experiments with Arctic Ocean water during both Arctic winter and summer were conducted and focused on PMA emissions as a function of season and water properties. Total particle number concentrations and particle number size distributions were used to characterize the PMA population. A comprehensive data set from the Arctic summer and winter showed a decrease in PMA concentrations for the covered water temperature (Tw) range between −1°C and 15°C. A sharp decrease in PMA emissions for a Tw increase from −1°C to 4°C was followed by a lower rate of change in PMA emissions for Tw up to about 6°C. Near constant number concentrations for water temperatures between 6°C to 10°C and higher were recorded. Even though the total particle number concentration changes for overlapping Tw ranges were consistent between the summer and winter measurements, the distribution of particle number concentrations among the different sizes varied between the seasons. Median particle number concentrations for a dry diameter (Dp< 0.125μm measured during winter conditions were similar (deviation of up to 3%), or lower (up to 70%) than the ones measured during summer conditions (for the same water temperature range). For Dp > 0.125μm, the particle number concentrations during winter were mostly higher than in summer (up to 50%). The normalized particle number size distribution as a function of water temperature was examined for both winter and summer measurements. An increase in Tw from −1°C to 10°C during winter measurements showed a decrease in the peak of relative particle number concentration at about a Dp of 0.180μm, while an increase was observed for particles with Dp > 1μm. Summer measurements exhibited a relative shift to smaller particle sizes for an increase of Tw in the range 7–11°C. The differences in the shape of the number size distributions between winter and summer may be caused by different production of organic material in water, different local processes modifying the water masses within the fjord (for example sea ice production in winter and increased glacial meltwater inflow during summer) and different origin of the dominant sea water mass. Further research is needed regarding the contribution of these factors to the PMA production.

Simple Field Device for Measurement of Dimethyl Sulfide and Dimethylsulfoniopropionate in Natural Waters, Based on Vapor Generation and Chemiluminescence Detection

A small, simple device was developed for trace analysis of dimethyl sulfide (DMS) and dimethylsulfoniopropionate (DMSP) in natural waters. These compounds are known to be the major sources of cloud condensation nuclei in the oceanic atmosphere and ideally should be measured onsite because of their volatility and instability. First, chemical and physical vapor generations were examined, and simple pressurizing by injection of 30 mL of air using a syringe was adopted. Pressurized headspace air above a 10 mL water sample was introduced to a detection cell as a result of the pressure differential and mixed with ozone to induce chemiluminescence. Although the measurement procedure was simple, the method was very sensitive: sharp peaks appeared within seconds for nanomolar levels of DMS, and the limit of detection was 0.02 nmol L(-1) (1 ng L(-1)). Although interference from methanethiol was significant, this was successfully addressed by adding a small amount of Cd(2+) before DMS vapor generation. DMSP was also measured after hydrolysis to DMS, as previously reported. Pond water and seawater samples were analyzed, and DMS was found in both types of sample, whereas DMSP was observed only in seawater. The DMS/DMSP data obtained using the developed method were compared with data obtained by purge/trap and gas chromatography-mass spectrometry, and the data from the two methods agreed, with good correlation (R(2) = 0.9956). The developed device is inexpensive, light (5 kg), simple to use, can be applied in the field, and is sensitive enough for fresh- and seawater analysis.

Impacts of aerosol particles on the microphysical and radiative properties of stratocumulus clouds over the southeast Pacific Ocean

Abstract. The southeast Pacific Ocean is covered by the world's largest stratocumulus cloud layer, which has a strong impact on ocean temperatures and climate in the region. The effect of anthropogenic sources of aerosol particles on the stratocumulus deck was investigated during the VOCALS field experiment. Aerosol measurements below and above cloud were made with a ultra-high sensitivity aerosol spectrometer and analytical electron microscopy. In addition to more standard in-cloud measurements, droplets were collected and evaporated using a counterflow virtual impactor (CVI), and the non-volatile residual particles were analyzed. Many flights focused on the gradient in cloud properties on an E-W track along 20° S from near the Chilean coast to remote areas offshore. Mean statistics, including their significance, from eight flights and many individual legs were compiled. Consistent with a continental source of cloud condensation nuclei, below-cloud accumulation-mode aerosol and droplet number concentration generally decreased from near shore to offshore. Single particle analysis was used to reveal types and sources of the enhanced particle number that influence droplet concentration. While a variety of particle types were found throughout the region, the dominant particles near shore were partially neutralized sulfates. Modeling and chemical analysis indicated that the predominant source of these particles in the marine boundary layer along 20° S was anthropogenic pollution from central Chilean sources, with copper smelters a relatively small contribution. Cloud droplets were smaller in regions of enhanced particles near shore. However, physically thinner clouds, and not just higher droplet number concentrations from pollution, both contributed to the smaller droplets. Satellite measurements were used to show that cloud albedo was highest 500–1000 km offshore, and actually slightly lower closer to shore due to the generally thinner clouds and lower liquid water paths there. Thus, larger scale forcings that impact cloud macrophysical properties, as well as enhanced aerosol particles, are important in determining cloud droplet size and cloud albedo. Differences in the size distribution of droplet residual particles and ambient aerosol particles were observed. By progressively excluding small droplets from the CVI sample, we were able to show that the larger drops, some of which may initiate drizzle, contain the largest aerosol particles. Geometric mean diameters of droplet residual particles were larger than those of the below-cloud and above cloud distributions. However, a wide range of particle sizes can act as droplet nuclei in these stratocumulus clouds. A detailed LES microphysical model was used to show that this can occur without invoking differences in chemical composition of cloud-nucleating particles.

New particle formation and growth in biomass burning plumes: An important source of cloud condensation nuclei

Experiments were performed in an environmental chamber to characterize the effects of photo‐chemical aging on biomass burning emissions. Photo‐oxidation of dilute exhaust from combustion of 12 different North American fuels induced significant new particle formation that increased the particle number concentration by a factor of four (median value). The production of secondary organic aerosol caused these new particles to grow rapidly, significantly enhancing cloud condensation nuclei (CCN) concentrations. Using inputs derived from these new data, global model simulations predict that nucleation in photo‐chemically aging fire plumes produces dramatically higher CCN concentrations over widespread areas of the southern hemisphere during the dry, burning season (Sept.–Oct.), improving model predictions of surface CCN concentrations. The annual indirect forcing from CCN resulting from nucleation and growth in biomass burning plumes is predicted to be −0.2 W m−2, demonstrating that this effect has a significant impact on climate that has not been previously considered.

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.

Simulation of particle formation and number concentration over the Eastern United States with the WRF-Chem + APM model

Abstract. Aerosol nucleation events, widely observed at various locations around the globe, are a significant source of cloud condensation nuclei (CCN) which determines aerosol indirect radiative forcing. In this study, a size-resolved, computationally efficient, advanced particle microphysics (APM) model, which has been previously incorporated into a global chemistry transport model (GEOS-Chem), is integrated into the Weather Research and Forecast model coupled with Chemistry (WRF-Chem) to study new particle formation and its contribution to particle number concentration and CCN abundance over the Eastern United States. Size- and composition-resolved aerosol properties from GEOS-Chem + APM simulations are used to initialize and provide boundary conditions for the WRF-Chem + APM model. The modeling results have been evaluated with the relevant measurements obtained during the INTEX-A field campaign in the summer of 2004. Model simulation captures the high concentrations of SO2 and CN10 at surface layer and source regions but underpredicts the values in the upper troposphere. The particle formation and number concentrations simulated by WRF-Chem + APM are generally consistent with those based on GEOS-Chem + APM over the Eastern United States, but the WRF-Chem + APM simulation has a much higher spatial resolution and can reveal urban and even plume scale processes. Our simulations show that high values of nucleation rates are largely confined to the regions of high SO2 emissions and that aerosol nucleation dominates the spatial and temporal distributions of condensation nuclei lager than 10 nm (CN10). Similarly, high concentrations of CCN at supersaturation of 0.4% (CCN0.4) are generally confined to SO2 source regions, with the highest monthly (July) mean CCN0.4 value exceeding 1600 # cm−3 in the lower troposphere over Indiana and Ohio. Nucleation and subsequent growth of secondary particles are important sources of CCN0.4, accounting for more than 80% in most parts of the Eastern United States.

Marine microgels as a source of cloud condensation nuclei in the high Arctic.

Marine microgels play an important role in regulating ocean basin-scale biogeochemical dynamics. In this paper, we demonstrate that, in the high Arctic, marine gels with unique physicochemical characteristics originate in the organic material produced by ice algae and/or phytoplankton in the surface water. The polymers in this dissolved organic pool assembled faster and with higher microgel yields than at other latitudes. The reversible phase transitions shown by these Arctic marine gels, as a function of pH, dimethylsulfide, and dimethylsulfoniopropionate concentrations, stimulate the gels to attain sizes below 1 μm in diameter. These marine gels were identified with an antibody probe specific toward material from the surface waters, sized, and quantified in airborne aerosol, fog, and cloud water, strongly suggesting that they dominate the available cloud condensation nuclei number population in the high Arctic (north of 80°N) during the summer season. Knowledge about emergent properties of marine gels provides important new insights into the processes controlling cloud formation and radiative forcing, and links the biology at the ocean surface with cloud properties and climate over the central Arctic Ocean and, probably, all oceans.

Modeling chemical and aerosol processes in the transition from closed to open cells during VOCALS-REx

Abstract. Chemical and aerosol processes in the transition from closed- to open-cell circulation in the remote, cloudy marine boundary layer are explored. It has previously been shown that precipitation can initiate a transition from the closed- to the open-cellular state, but that the boundary layer cannot maintain this open-cell state without a resupply of cloud condensation nuclei (CCN). Potential sources of CCN include wind-driven production of sea salt from the ocean, nucleation from the gas phase, and entrainment from the free troposphere. In order to investigate CCN sources in the marine boundary layer and their role in supplying new particles, we have coupled in detail chemical, aerosol, and cloud processes in the WRF/Chem model, and added state-of-the-art representations of sea salt emissions and aerosol nucleation. We conduct numerical simulations of the marine boundary layer in the transition from a closed- to an open-cell state. Results are compared with observations in the Southeast Pacific boundary layer during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx). The transition from the closed- to the open-cell state generates conditions that are conducive to nucleation by forming a cloud-scavenged, ultra-clean layer below the inversion base. Open cell updrafts loft dimethyl sulfide from the ocean surface into the ultra-clean layer, where it is oxidized during daytime to SO2 and subsequently to H2SO4. Low H2SO4 condensation sink values in the ultra-clean layer allow H2SO4 to rise to concentrations at which aerosol nucleation produces new aerosol in significant numbers. The existence of the ultra-clean layer is confirmed by observations. We find that the observed DMS flux from the ocean in the VOCALS-REx region can support a nucleation source of aerosol in open cells that exceeds sea salt emissions in terms of the number of particles produced. The freshly nucleated, nanometer-sized aerosol particles need, however, time to grow to sizes large enough to act as CCN. In contrast, mechanical production of particles from the ocean surface by near-surface winds provides a steady source of larger particles that are effective CCN at a rate exceeding a threshold for maintenance of open-cell circulation. Entrainment of aerosol from the free troposphere contributes significantly to boundary layer aerosol for the considered VOCALS-REx case, but less than sea salt aerosol emissions.

Isoprene suppression of new particle formation in a mixed deciduous forest

Abstract. Production of new particles over forests is an important source of cloud condensation nuclei that can affect climate. While such particle formation events have been widely observed, their formation mechanisms over forests are poorly understood. Our observations made in a mixed deciduous forest with large isoprene emissions during the summer displayed a surprisingly rare occurrence of new particle formation (NPF). Typically, NPF events occur around noon but no NPF events were observed during the 5 weeks of measurements. The exceptions were two evening ultrafine particle events. During the day, sulfuric acid concentrations were in the 106 cm−3 range with very low preexisting aerosol particles, a favorable condition for NPF to occur even during the summer. The ratio of emitted isoprene carbon to monoterpene carbon at this site was similar to that in Amazon rainforests (ratio >10), where NPF events are also very rare, compared with a ratio <0.5 in Finland boreal forests, where NPF events are frequent. Our results suggest that large isoprene emissions can suppress NPF formation in forests although the underlying mechanism for the suppression is unclear. The two evening ultrafine particle events were associated with the transported anthropogenic sulfur plumes and ultrafine particles were likely formed via ion-induced nucleation. Changes in landcover and environmental conditions could modify the isoprene suppression of NPF in some forest regions resulting in a radiative forcing that could have influence on the climate.

The use of algorithms to predict surface seawater dimethyl sulphide concentrations in the SE Pacific, a region of steep gradients in primary productivity, biomass and mixed layer depth

Abstract. Dimethyl sulphide (DMS) is an important precursor of cloud condensation nuclei (CCN), particularly in the remote marine atmosphere. The SE Pacific is consistently covered with a persistent stratocumulus layer that increases the albedo over this large area. It is not certain whether the source of CCN to these clouds is natural and oceanic or anthropogenic and terrestrial. This unknown currently limits our ability to reliably model either the cloud behaviour or the oceanic heat budget of the region. In order to better constrain the marine source of CCN, it is necessary to have an improved understanding of the sea-air flux of DMS. Of the factors that govern the magnitude of this flux, the greatest unknown is the surface seawater DMS concentration. In the study area, there is a paucity of such data, although previous measurements suggest that the concentration can be substantially variable. In order to overcome such data scarcity, a number of climatologies and algorithms have been devised in the last decade to predict seawater DMS. Here we test some of these in the SE Pacific by comparing predictions with measurements of surface seawater made during the Vamos Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) in October and November of 2008. We conclude that none of the existing algorithms reproduce local variability in seawater DMS in this region very well. From these findings, we recommend the best algorithm choice for the SE Pacific and suggest lines of investigation for future work.

Strong air pollution causes widespread haze‐clouds over China

North China (Huabei in Chinese) is a geographical region located between 32°N and 42°N latitude in eastern China, including several provinces and large municipalities (e.g., Beijing and Tianjin). In the past decades the region has experienced dramatic changes in air quality and climate. Among the multiple causes aerosol pollution is expected to play a particularly important role. To investigate this, a field measurement campaign was performed in April–May 2006 as part of the project Influence of Pollution on Aerosols and Cloud Microphysics in North China. Here we report the first aircraft measurements of atmospheric trace gases, aerosols, and clouds over this part of China, a region strongly affected by both natural desert dust and pollution smog. We observed very high concentrations of gaseous air pollutants and haze particles, partly together with nonprecipitating stratiform clouds. The clouds were characterized by numerous droplets, much smaller than in a less‐polluted atmosphere. Our data reveal that the highly efficient coating of dust particles by pollution acids provides the predominant source of cloud condensation nuclei. The pollution‐enhanced activation of dust particles into droplets is shown to be remarkably efficient so that clouds even form below 100% relative humidity. Contrary to previous analyses, we find that the haze particles influence the spectral shape of the cloud droplet size distribution such that the indirect climate cooling effect of aerosols on clouds is increased. The widespread haze, combined with low clouds, diminishes air quality and exerts an unusually strong cooling forcing on climate.

The impact of the 1783–1784 AD Laki eruption on global aerosol formation processes and cloud condensation nuclei

Abstract. The 1783–1784 AD Laki flood lava eruption commenced on 8 June 1783 and released 122 Tg of sulphur dioxide gas over the course of 8 months into the upper troposphere and lower stratosphere above Iceland. Previous studies have examined the impact of the Laki eruption on sulphate aerosol and climate using general circulation models. Here, we study the impact on aerosol microphysical processes, including the nucleation of new particles and their growth to cloud condensation nuclei (CCN) using a comprehensive Global Model of Aerosol Processes (GLOMAP). Total particle concentrations in the free troposphere increase by a factor ~16 over large parts of the Northern Hemisphere in the 3 months following the onset of the eruption. Particle concentrations in the boundary layer increase by a factor 2 to 5 in regions as far away as North America, the Middle East and Asia due to long-range transport of nucleated particles. CCN concentrations (at 0.22% supersaturation) increase by a factor 65 in the upper troposphere with maximum changes in 3-month zonal mean concentrations of ~1400 cm−3 at high northern latitudes. 3-month zonal mean CCN concentrations in the boundary layer at the latitude of the eruption increase by up to a factor 26, and averaged over the Northern Hemisphere, the eruption caused a factor 4 increase in CCN concentrations at low-level cloud altitude. The simulations show that the Laki eruption would have completely dominated as a source of CCN in the pre-industrial atmosphere. The model also suggests an impact of the eruption in the Southern Hemisphere, where CCN concentrations are increased by up to a factor 1.4 at 20° S. Our model simulations suggest that the impact of an equivalent wintertime eruption on upper tropospheric CCN concentrations is only about one-third of that of a summertime eruption. The simulations show that the microphysical processes leading to the growth of particles to CCN sizes are fundamentally different after an eruption when compared to the unperturbed atmosphere, underlining the importance of using a fully coupled microphysics model when studying long-lasting, high-latitude eruptions.