Condensation Nuclei Concentrations Research Articles

Source Contribution of Firecrackers Burst vs. Long-Range Transport of Biomass Burning Emissions Over an Urban Background

This study reports on the high-resolution data set of ground-level O3, surface-bound polycyclic aromatic hydrocarbons (SB-PAHs), and particle's number concentrations (range: 10 to 1,000 nm, referred to as condensation nucleus concentration: CNC) during a Diwali festival campaign (conducted from 08th to 16th Nov.2015) at Kanpur location. In this study, we have made an attempt to assess the change in atmospheric composition and chemistry (based on SB-PAHs, O3, and CNC) during Diwali festival (11th Nov.) and compared the results with pre-Diwali (08th−10th Nov.) and post-Diwali (12th−16th Nov.) scenarios. The wind pattern and cluster analysis have revealed a quite similar feature that from 10th to 16th of November the prevailed winds were north-westerly (NW). It is noteworthy that NW-winds during post-monsoon season (Oct–Nov) favors the long-range transport of biomass burning emissions (LRT-BB) from its source region in upwind Indo-Gangetic Plain (IGP). The influence of LRT-BB emissions at the receptor site during Diwali and post-Diwali period was reflected by the substantial increase in average concentrations of PM2.5, O3 and CNC (difference has been ascertained from a two-tailed t-test). The Lenshchow-type analysis revealed that the firecrackers (FC) burst and LRT-BB emissions have lead to increase the concentrations of CNC by 54% and 86%, respectively over the urban background level. On the other hand, the FC burst and LRT-BB increased the concentrations of O3 by 12% and 31% (over the urban background), respectively. Lenschow-type analysis revealed that FC burst and LRT-BB increased the daily PM2.5 concentration by 11% and 36%, respectively over its urban background level (286 μg m−3). However, the SB-PAHs concentrations were found to be decreased by 6% and 2%, respectively, during the FC burst activity and LRT-BB emissions. Based on the observations pertaining to the decrease in SB-PAHs concentrations from the Lenschow-type analysis and anti-correlation between SB-PAHs and O3 the heterogeneous-phase chemical reactivity and loss of SB-PAHs has been inferred in this study.

Optimization of the sulfate aerosol hygroscopicity parameter in WRF-Chem

Abstract. A new sulfate aerosol hygroscopicity parameter (κSO4) parameterization is suggested that is capable of considering the two major sulfate aerosols, H2SO4 and (NH4)2SO4, using the molar ratio of ammonium to sulfate (R). An alternative κSO4 parameterization method is also suggested that utilizes typical geographical distribution patterns of sulfate and ammonium, which can be used when ammonium data are not available for model calculation. Using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), the impacts of different κSO4 parameterizations on cloud microphysical properties and cloud radiative effects in East Asia are examined. Comparisons with the observational data obtained from an aircraft field campaign suggest that the new κSO4 parameterizations simulate more reliable aerosol and cloud condensation nuclei concentrations, especially over the sea in East Asia, than the original κSO4 parameterization in WRF-Chem that assumes sulfate aerosols as (NH4)2SO4 only. With the new κSO4 parameterizations, the simulated cloud microphysical properties and precipitation became significantly different, resulting in a greater cloud albedo effect of about −1.5 W m−2 in East Asia than that with the original κSO4 parameterization. The new κSO4 parameterizations are simple and readily applicable to numerical studies investigating the impact of sulfate aerosols in aerosol–cloud interactions without additional computational expense.

The dual-field-of-view polarization lidar technique: a new concept in monitoring aerosol effects in liquid-water clouds – case studies

Abstract. In a companion article (Jimenez et al., 2020), we introduced a new lidar method to derive microphysical properties of liquid-water clouds (cloud extinction coefficient, droplet effective radius, liquid-water content, cloud droplet number concentration Nd) at a height of 50–100 m above the cloud base together with aerosol information (aerosol extinction coefficients, cloud condensation nuclei concentration NCCN) below the cloud layer so that detailed studies of the influence of given aerosol conditions on the evolution of liquid-water cloud layers with high temporal resolution solely based on lidar observations have become possible now. The novel cloud retrieval technique makes use of lidar observations of the volume linear depolarization ratio at two different receiver field of views (FOVs). In this article, Part 2, the new dual-FOV polarization lidar technique is applied to cloud measurements in pristine marine conditions at Punta Arenas in southern Chile. A multiwavelength polarization Raman lidar, upgraded by integrating a second polarization-sensitive channel to permit depolarization ratio observations at two FOVs, was used for these measurements at the southernmost tip of South America. Two case studies are presented to demonstrate the potential of the new lidar technique. Successful aerosol–cloud-interaction (ACI) studies based on measurements with the upgraded aerosol–cloud lidar in combination with a Doppler lidar of the vertical wind component could be carried out with 1 min temporal resolution at these pristine conditions. In a stratocumulus layer at the top of the convective boundary layer, we found values of Nd and NCCN (for 0.2 % water supersaturation) ranging from 15–100 and 75–200 cm−3, respectively, during updraft periods. The studies of the aerosol impact on cloud properties yielded ACI values close to 1. The impact of aerosol water uptake on the ACI studies was analyzed with the result that the highest ACI values were obtained when considering aerosol proxies (light-extinction coefficient αpar or NCCN) measured at heights about 500 m below the cloud base (and thus for dry aerosol conditions).

The dual-field-of-view polarization lidar technique: a new concept in monitoring aerosol effects in liquid-water clouds – theoretical framework

Abstract. In a series of two articles, a novel, robust, and practicable lidar approach is presented that allows us to derive microphysical properties of liquid-water clouds (cloud extinction coefficient, droplet effective radius, liquid-water content, cloud droplet number concentration) at a height of 50–100 m above the cloud base. The temporal resolution of the observations is on the order of 30–120 s. Together with the aerosol information (aerosol extinction coefficients, cloud condensation nucleus concentration) below the cloud layer, obtained with the same lidar, in-depth aerosol–cloud interaction studies can be performed. The theoretical background and the methodology of the new cloud lidar technique is outlined in this article (Part 1), and measurement applications are presented in a companion publication (Part 2) (Jimenez et al., 2020a). The novel cloud retrieval technique is based on lidar observations of the volume linear depolarization ratio at two different receiver fields of view (FOVs). Extensive simulations of lidar returns in the multiple scattering regime were conducted to investigate the capabilities of a dual-FOV polarization lidar to measure cloud properties and to quantify the information content in the measured depolarization features regarding the basic retrieval parameters (cloud extinction coefficient, droplet effective radius). Key simulation results and the overall data analysis scheme developed to obtain the aerosol and cloud products are presented.

Constraining the Twomey effect from satellite observations: issues and perspectives

Abstract. The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (ΔNd, ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol–cloud interactions, but rapid adjustments also contribute. These adjustments are essentially the responses of cloud fraction and liquid water path to ΔNd, ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (Nd) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large-scale (hundreds of kilometres) perturbation, ΔNd, ant, remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and updraught velocity and by droplet sink processes. These operate at scales on the order of tens of metres at which only localised observations are available and at which no approach yet exists to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are four key uncertainties in determining ΔNd, ant, namely the quantification of (i) the cloud-active aerosol – the cloud condensation nuclei (CCN) concentrations at or above cloud base, (ii) Nd, (iii) the statistical approach for inferring the sensitivity of Nd to aerosol particles from the satellite data and (iv) uncertainty in the anthropogenic perturbation to CCN concentrations, which is not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: in terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, non-direct relation to the concentration of aerosols, difficulty to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilising co-located polarimeter and lidar instruments, ideally including high-spectral-resolution lidar capability at two wavelengths to maximise vertically resolved size distribution information content. In terms of Nd, a key problem is the lack of operational retrievals of this quantity and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the Nd-to-CCN sensitivity, key issues are the updraught distributions and the role of Nd sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect.

First surface measurement of variation of Cloud Condensation Nuclei (CCN) concentration over the Pristine Himalayan region of Garhwal, Uttarakhand, India

A Droplet Measurement Technology (DMT) Cloud Condensation Nuclei Counter (CCNC) was deployed to measure cloud condensation nuclei (CCN) for the first time in the pristine Himalayan region at Himalayan Clouds Observatory (HCO), Swami Ram Tirtha (SRT) Campus (30°34′ N, 78°41′ E, 1706 m AMSL), Hemvati Nandan Bahuguna (HNB) Garhwal University, Badshahithaul, Tehri Garhwal, Uttarakhand, India. The CCN concentration (NCCN) was observed at four supersaturation levels (SS: 0.2, 0.5, 0.8, and 1.0%). In this study, we reported CCN concentration at 0.5% SS in different weather conditions from Aug 01, 2018 to Jun 30, 2019. During this observation period, the monthly averaged value of CCN concentration ranged between 1098.3 ± 448.9 cm−3 (mean ± SD) and 3842.9 ± 2512.9 cm−3. It covers a significantly wide range of daily averaged concentrations from the minimum concentration of 43.84 cm−3 (during heavy wet scavenging due to snowfall) to maximum concentration of 17000 cm−3 (during the events of a forest fire) at the observation site. The highest CCN concentration is observed at the time of sunrise (~07:00 a.m.) and after the sunset (~07:00 p.m.) for the diurnal variation of monsoon, post-monsoon, and winter season. Pre-monsoon season shows peak values at 10:00 a.m. and at 07:00 p.m. with higher concentrations at night hours. The possible reasons for maximum concentration in morning and evening time could be upliftment and settlement of CCN because of the convection process, anthropogenic emission, vehicular emission, and biomass burning in the residential area and valley region adjacent to HCO, Badshahithaul. The highest CCN concentration (3842.9 ± 2513 cm−3) values of the whole observation period were observed in May 2019. It was significantly affected by the heavy fire activities over the Uttarakhand and nearby IGP regions. Diurnal variation of CCN concentration during the HFAD shows higher values in the night time differing from the diurnal pattern of CCN for other months of the observation period. The long-range transport of air mass could also contribute to the high CCN concentration values, as found through the five-day air mass backward trajectory analysis. The lowest value of CCN concentration corresponds to the heavy rains and snowfall days, possibly caused by extensive wet scavenging. Cluster analysis of the air mass trajectories used for the allocation and classification of the possible sources of pollutants reaching the observation site. The highest fraction of CCN concentration (more than 2000 cm−3) corresponds to the air mass from the arid and semi-arid regions of Asian countries. Large air mass fraction (~40–60%) with moderate CCN concentration was received from northwestern IGP region and foothills of central Himalaya.

The evolution of cloud and aerosol microphysics at the summit of Mt. Tai, China

Abstract. The influence of aerosols, both natural and anthropogenic, remains a major area of uncertainty when predicting the properties and the behaviours of clouds and their influence on climate. In an attempt to better understand the microphysical properties of cloud droplets, the simultaneous variations in aerosol microphysics and their potential interactions during cloud life cycles in the North China Plain, an intensive observation took place from 17 June to 30 July 2018 at the summit of Mt. Tai. Cloud microphysical parameters were monitored simultaneously with number concentrations of cloud condensation nuclei (NCCN) at different supersaturations, PM2.5 mass concentrations, particle size distributions and meteorological parameters. Number concentrations of cloud droplets (NC), liquid water content (LWC) and effective radius of cloud droplets (reff) show large variations among 40 cloud events observed during the campaign. The low values of reff and LWC observed at Mt. Tai are comparable with urban fog. Clouds on clean days are more susceptible to the change in concentrations of particle number (NP), while clouds formed on polluted days might be more sensitive to meteorological parameters, such as updraft velocity and cloud base height. Through studying the size distributions of aerosol particles and cloud droplets, we find that particles larger than 150 nm play important roles in forming cloud droplets with the size of 5–10 µm. In general, LWC consistently varies with reff. As NC increases, reff changes from a trimodal distribution to a unimodal distribution and shifts to smaller size mode. By assuming a constant cloud thickness and ignoring any lifetime effects, increase in NC and decrease in reff would increase cloud albedo, which may induce a cooling effect on the local climate system. Our results contribute valuable information to enhance the understanding of cloud and aerosol properties, along with their potential interactions on the North China plain.

Evaluation of Orographic Cloud Seeding Using a Bin Microphysics Scheme: Three-Dimensional Simulation of Real Cases

AbstractThe University of Pécs and NCAR Bin (UPNB) microphysical scheme was implemented into the mesoscale Weather Research and Forecast (WRF) Model that was used to study the impact of silver iodide (AgI) seeding on precipitation formation in winter orographic clouds. Four different experimental units were chosen from the Wyoming Weather Modification Pilot Project to simulate the seeding effect. The results of the numerical experiments show the following: (i) Comparisons with the soundings, snow gauges, and microwave radiometer data indicate that the three-dimensional simulations with detailed microphysics reasonably represent both the dynamics and the microphysics of real clouds. (ii) The dispersion of the AgI particles from the simulated ground-based seeding was effective because of turbulent mixing. (iii) In the investigated cases (surface temperature is less than 0°C), surface precipitation and precipitation efficiency show low susceptibility to the concentrations of cloud condensation nuclei and natural ice nucleating particles. (iv) If the available liquid water content promotes the enhancement of the number of snowflakes by diffusional growth, the surface precipitation can be increased by more than 5%. A novel parameter relevant to orographic clouds, horizontally integrated liquid water path (LWP), was evaluated to find the relation between seeding efficiency and liquid water content. The impact of seeding is negligible if the horizontal LWP is less than 0.1 mm and is apparent if the horizontal LWP is larger than 1 mm, as based on the cases investigated in this study.

Variations in <i>N</i><sub>cn</sub> and <i>N</i><sub>ccn</sub> over marginal seas in China related to marine traffic emissions, new particle formation and aerosol aging

Abstract. In this study, a cruise campaign was conducted over marginal seas in China to measure the concentrations of condensation nuclei (Ncn), cloud condensation nuclei (Nccn) and other pollutants from day of year (DOY) 110 to DOY 135 of 2018. The ship self-emission signals were exhaustively excluded, and the mean values of Nccn during the cruise campaign were found to slightly increase from 3.2±1.1×103 cm−3 (mean ± standard deviation) at supersaturation (SS) of 0.2 % to 3.9±1.4×103 cm−3 at SS of 1.0 %, and the mean value for Ncn was 8.1±4.4×103 cm−3. Data analysis showed that marine traffic emissions apparently largely contributed to the increase in Ncn in the daytime, especially in the marine atmospheres over heavily traveled sea zones; however, the fresh sources made no clear contribution to the increase in Nccn. This finding was supported by the quantitative relations between Ncn and Nccn at SS = 0.2 %–1.0 % against the mixing ratios of SO2 in the ship self-emission plumes – i.e., a 1 ppb increase in SO2 corresponded to a 1.4×104 cm−3 increase in Ncn but only a 30–170 cm−3 increase in Nccn, possibly because of abundant organics in the aerosols. Smooth growth can be observed in the marine-traffic-derived particles, reflecting aerosol aging. The estimated hygroscopicity parameter (κ) values were generally as high as 0.46–0.55 under the dominant onshore winds, suggesting that inorganic ammonium aerosols likely acted as the major contributor to Nccn largely through aerosol aging processes of decomposing organics. Moreover, the influences of the new transported particles from the continent on the Ncn and Nccn in the marine atmosphere were investigated.

Satellite Retrieval of Cloud Condensation Nuclei Concentrations in Marine Stratocumulus by Using Clouds as CCN Chambers

AbstractA new methodology for the satellite retrieval of cloud condensation nuclei (CCN) in shallow marine boundary layer clouds is developed and validated in this study. The methodology is based on retrieving cloud base drop concentrations (Nd) and updrafts (Wb), which are used for calculating the supersaturation (S). The Nd is then defined as the CCN at that S. The accuracy of the satellite retrievals was validated against ship‐borne measurements of CCN done in recent campaigns in the Southern Oceans (ACE‐SPACE, MARCUS, & PEGASO [2015–2018]) and in the subtropics (MAGIC [2012–2013]). The satellite‐retrieved Nd and S at cloud base were validated against the measured CCN at sea surface. The main findings show that (a) coupled clouds have good agreement between satellite retrievals and ship measurements of CCN; (b) the best agreement is achieved when using the brightest 10% of the clouds and accounting for their adiabatic fraction; (c) most of the decoupled clouds had much lower CCN than were present at the underlying surface. This means that most CCN in the coupled clouds originate from the surface and not from the free troposphere. This study validates the satellite retrievals of CCN and allows us to further quantify the relationships between CCN and cloud microphysical properties.

Global and Arctic effective radiative forcing of anthropogenic gases and aerosols in MRI-ESM2.0

The effective radiative forcing (ERF) of anthropogenic gases and aerosols under present-day conditions relative to preindustrial conditions is estimated using the Meteorological Research Institute Earth System Model version 2.0 (MRI-ESM2.0) as part of the Radiative Forcing Model Intercomparison Project (RFMIP) and Aerosol and Chemistry Model Intercomparison Project (AerChemMIP), endorsed by the sixth phase of the Coupled Model Intercomparison Project (CMIP6). The global mean total anthropogenic net ERF estimate at the top of the atmosphere is 1.96 W m−2 and is composed primarily of positive forcings due to carbon dioxide (1.85 W m−2), methane (0.71 W m−2), and halocarbons (0.30 W m−2) and negative forcing due to the total aerosols (− 1.22 W m−2). The total aerosol ERF consists of 23% from aerosol-radiation interactions (− 0.32 W m−2), 71% from aerosol-cloud interactions (− 0.98 W m−2), and slightly from surface albedo changes caused by aerosols (0.08 W m−2). The ERFs due to aerosol-radiation interactions consist of opposing contributions from light-absorbing black carbon (BC) (0.25 W m−2) and from light-scattering sulfate (− 0.48 W m−2) and organic aerosols (− 0.07 W m−2) and are pronounced over emission source regions. The ERFs due to aerosol-cloud interactions (ERFaci) are prominent over the source and downwind regions, caused by increases in the number concentrations of cloud condensation nuclei and cloud droplets in low-level clouds. Concurrently, increases in the number concentration of ice crystals in high-level clouds (temperatures < –38 °C), primarily induced by anthropogenic BC aerosols, particularly over tropical convective regions, cause both substantial negative shortwave and positive longwave ERFaci values in MRI-ESM2.0. These distinct forcings largely cancel each other; however, significant longwave radiative heating of the atmosphere caused by high-level ice clouds suggests the importance of further studies on the interactions of aerosols with ice clouds. Total anthropogenic net ERFs are almost entirely positive over the Arctic due to contributions from the surface albedo reductions caused by BC. In the Arctic, BC provides the second largest contribution to the positive ERFs after carbon dioxide, suggesting a possible important role of BC in Arctic surface warming.

Estimation of cloud condensation nuclei number concentrations and comparison to in situ and lidar observations during the HOPE experiments

Abstract. Atmospheric aerosol particles are the precondition for the formation of cloud droplets and therefore have large influence on the microphysical and radiative properties of clouds. In this work, four different methods to derive or measure number concentrations of cloud condensation nuclei (CCN) were analyzed and compared for present-day aerosol conditions: (i) a model parameterization based on simulated particle concentrations, (ii) the same parameterization based on gravimetrical particle measurements, (iii) direct CCN measurements with a CCN counter, and (iv) lidar-derived and in situ measured vertical CCN profiles. In order to allow for sensitivity studies of the anthropogenic impact, a scenario to estimate the maximum CCN concentration under peak aerosol conditions of the mid-1980s in Europe was developed as well. In general, the simulations are in good agreement with the observations. At ground level, average values between 0.7 and 1.5×109 CCN m−3 at a supersaturation of 0.2 % were found with the different methods under present-day conditions. The discrimination of the chemical species revealed an almost equal contribution of ammonium sulfate and ammonium nitrate to the total number of CCN for present-day conditions. This was not the case for the peak aerosol scenario, in which it was assumed that no ammonium nitrate was formed while large amounts of sulfate were present, consuming all available ammonia during ammonium sulfate formation. The CCN number concentration at five different supersaturation values has been compared to the measurements. The discrepancies between model and in situ observations were lowest for the lowest (0.1 %) and highest supersaturations (0.7 %). For supersaturations between 0.3 % and 0.5 %, the model overestimated the potentially activated particle fraction by around 30 %. By comparing the simulation with observed profiles, the vertical distribution of the CCN concentration was found to be overestimated by up to a factor of 2 in the boundary layer. The analysis of the modern (year 2013) and the peak aerosol scenario (expected to be representative of the mid-1980s over Europe) resulted in a scaling factor, which was defined as the quotient of the average vertical profile of the peak aerosol and present-day CCN concentration. This factor was found to be around 2 close to the ground, increasing to around 3.5 between 2 and 5 km and approaching 1 (i.e., no difference between present-day and peak aerosol conditions) with further increasing height.

Disdrometer, Polarimetric Radar, and Condensation Nuclei Observations of Supercell and Multicell Storms on 11 June 2018 in Eastern Nebraska

Disdrometer and condensation nuclei (CN) data are compared with operational polarimetric radar data for one multicell and one supercell storm in eastern Nebraska on 11 June 2018. The radar was located ~14.3 km from the instrumentation location and provided excellent observation time series with new low-level samples every 1–2 min. Reflectivity derived by the disdrometer and radar compared well, especially in regions with high number concentration of drops and reflectivity &lt;45 dBZ. Differential reflectivity also compared well between the datasets, though it was most similar in the supercell storm. Rain rate calculated by the disdrometer closely matched values estimated by the radar when reflectivity and differential reflectivity were used to produce the estimate. Concentration of CN generally followed precipitation intensity for the leading convective cell, with evidence for higher particle concentration on the edges of the convective cell associated with outflow. The distribution of CN in the supercell was more complex and generally did not follow precipitation intensity.

Marine productivity and synoptic meteorology drive summer-time variability in Southern Ocean aerosols

Abstract. Cloud–radiation interactions over the Southern Ocean are not well constrained in climate models, in part due to uncertainties in the sources, concentrations, and cloud-forming potential of aerosol in this region. To date, most studies in this region have reported measurements from fixed terrestrial stations or a limited set of instrumentation and often present findings as broad seasonal or latitudinal trends. Here, we present an extensive set of aerosol and meteorological observations obtained during an austral summer cruise across the full width of the Southern Ocean south of Australia. Three episodes of continental-influenced air masses were identified, including an apparent transition between the Ferrel atmospheric cell and the polar cell at approximately 64∘ S, and accompanied by the highest median cloud condensation nuclei (CCN) concentrations, at 252 cm−3. During the other two episodes, synoptic-scale weather patterns diverted air masses across distances greater than 1000 km from the Australian and Antarctic coastlines, respectively, indicating that a large proportion of the Southern Ocean may be periodically influenced by continental air masses. In all three cases, a highly cloud-active accumulation mode dominated the size distribution, with up to 93 % of the total number concentration activating as CCN. Frequent cyclonic weather conditions were observed at high latitudes and the associated strong wind speeds led to predictions of high concentrations of sea spray aerosol. However, these modelled concentrations were not achieved due to increased aerosol scavenging rates from precipitation and convective transport into the free troposphere, which decoupled the air mass from the sea spray flux at the ocean surface. CCN concentrations were more strongly impacted by high concentrations of large-diameter Aitken mode aerosol in air masses which passed over regions of elevated marine biological productivity, potentially contributing up to 56 % of the cloud condensation nuclei concentration. Weather systems were vital for aerosol growth in biologically influenced air masses and in their absence ultrafine aerosol diameters were less than 30 nm. These results demonstrate that air mass meteorological history must be considered when modelling sea spray concentrations and highlight the potential importance of sub-grid-scale variability when modelling atmospheric conditions in the remote Southern Ocean.

Airborne bacteria confirm the pristine nature of the Southern Ocean boundary layer

Microorganisms are ubiquitous and highly diverse in the atmosphere. Despite the potential impacts of airborne bacteria found in the lower atmosphere over the Southern Ocean (SO) on the ecology of Antarctica and on marine cloud phase, no previous region-wide assessment of bioaerosols over the SO has been reported. We conducted bacterial profiling of boundary layer shipboard aerosol samples obtained during an Austral summer research voyage, spanning 42.8 to 66.5°S. Contrary to findings over global subtropical regions and the Northern Hemisphere, where transport of microorganisms from continents often controls airborne communities, the great majority of the bacteria detected in our samples were marine, based on taxonomy, back trajectories, and source tracking analysis. Further, the beta diversity of airborne bacterial communities varied with latitude and temperature, but not with other meteorological variables. Limited meridional airborne transport restricts southward community dispersal, isolating Antarctica and inhibiting microorganism and nutrient deposition from lower latitudes to these same regions. A consequence and implication for this region's marine boundary layer and the clouds that overtop it is that it is truly pristine, free from continental and anthropogenic influences, with the ocean as the dominant source controlling low-level concentrations of cloud condensation nuclei and ice nucleating particles.

Parameter sensitivity analysis of the theoretical model of a CR-39-based direct 222Rn/220Rn progeny monitor

Abstract The deposition-based direct indoor 222Rn and 220Rn progeny measurement techniques are mostly affected by the indoor environmental conditions, such as the ventilation, concentration of condensation nuclei, and reactions with the structure and its furnishings. In this study, a theoretical model of a direct 222Rn and 220Rn progeny monitor based on allyl diglycol carbonate (ADC or CR-39) was established to analyse the factors that influence the detection process by using the parameter sensitivity analysis. The aerosol parameters contributed the highest to the variance, followed by the aerodynamic parameters. With respect to the result of the Spearman’s correlation analysis, the aerosol-related and the room-related parameters are positive, whereas the aerodynamic parameters – which affect the turbulence of indoor deposition – are negative. It means that both the attachment process and the deposition process of 222Rn and 220Rn progenies are important to the performance of the progeny monitor.

Hygroscopic properties and cloud condensation nuclei activity of atmospheric aerosols under the influences of Asian continental outflow and new particle formation at a coastal site in eastern Asia

Abstract. The chemical composition of fine particulate matter (PM2.5), the size distribution and number concentration of aerosol particles (NCN), and the number concentration of cloud condensation nuclei (NCCN) were measured at the northern tip of Taiwan during an intensive observation experiment from April 2017 to March 2018. The parameters of aerosol hygroscopicity (i.e., activation ratio, activation diameter and kappa of CCN) were retrieved from the measurements. Significant variations were found in the hygroscopicity of aerosols (kappa – κ – of 0.18–0.56, for water vapor supersaturation – SS – of 0.12 %–0.80 %), which were subject to various pollution sources, including aged air pollutants originating in eastern and northern China and transported by the Asian continental outflows and fresh particles emitted from local sources and distributed by land–sea breeze circulations as well as produced by processes of new particle formation (NPF). Cluster analysis was applied to the back trajectories of air masses to investigate their respective source regions. The results showed that aerosols associated with Asian continental outflows were characterized by lower NCN and NCCN values and by higher kappa values of CCN, whereas higher NCN and NCCN values with lower kappa values of CCN were observed in the aerosols associated with local air masses. Besides, it was revealed that the kappa value of CCN exhibited a decrease during the early stage of an event of new particle formation, which turned to an increasing trend over the later period. The distinct features in the hygroscopicity of aerosols were found to be consistent with the characteristics in the chemical composition of PM2.5. This study has depicted a clear seasonal characteristic of hygroscopicity and CCN activity under the influence of a complex mixture of pollutants from different regional and/or local pollution sources. Nevertheless, the mixing state and chemical composition of the aerosols critically influence the aerosol hygroscopicity, and further investigations are necessary to elucidate the atmospheric processing involved in the CCN activation in coastal areas.

A First Case Study of CCN Concentrations from Spaceborne Lidar Observations

We present here the first cloud condensation nuclei (CCN) concentration profiles derived from measurements with the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO), for different aerosol types at a supersaturation of 0.15%. CCN concentrations, along with the corresponding uncertainties, were inferred for a nighttime CALIPSO overpass on 9 September 2011, with coincident observations with the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 research aircraft, within the framework of the Evaluation of CALIPSO’s Aerosol Classification scheme over Eastern Mediterranean (ACEMED) research campaign over Thessaloniki, Greece. The CALIPSO aerosol typing is evaluated, based on data from the Copernicus Atmosphere Monitoring Service (CAMS) reanalysis. Backward trajectories and satellite-based fire counts are used to examine the origin of air masses on that day. Our CCN retrievals are evaluated against particle number concentration retrievals at different height levels, based on the ACEMED airborne measurements and compared against CCN-related retrievals from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensors aboard Terra and Aqua product over Thessaloniki showing that it is feasible to obtain CCN concentrations from CALIPSO, with an uncertainty of a factor of two to three.

Reactive VOC Production from Photochemical and Heterogeneous Reactions Occurring at the Air-Ocean Interface.

The ocean surface serves as a source and sink for a diverse set of reactive trace gases in the atmosphere, including volatile organic compounds (VOCs), reactive halogens, and oxidized and reduced nitrogen compounds. The exchange of reactive trace gases between the atmosphere and ocean has been shown to alter atmospheric oxidant concentrations and drive particle nucleation and growth. Uncertainties in cloud radiative forcing and aerosol-cloud interactions are among the largest uncertainties in current global climate models. Climate models are particularly sensitive to cloud cover over the remote ocean due to large changes in albedo between the ocean surface and cloud tops. Oceanic emissions contribute to cloud condensation nuclei concentrations, either through the direct emission of particles during wave breaking or through the formation of secondary aerosol particles following the emission of reactive gas-phase compounds. Despite generally small and diffuse oceanic emission rates for reactive trace gases, it has been shown that oxidant and particle number concentrations are acutely sensitive to air-sea trace gas exchange rates and the chemical composition of emitted species. To date, field measurements of air-sea reactive gas exchange have focused primarily on the emission of gases of biological origin, such as dimethyl sulfide (DMS). While DMS emissions are relatively well constrained, the gas-phase oxidation that connects DMS to sulfate aerosol is less well understood. Recent laboratory measurements suggest that heterogeneous and photochemical reactions occurring at the air-sea interface can also lead to the production and emission of a wide array of reactive VOC. When laboratory-based measurements are used to derive global scale emissions, the calculated sea-to-air fluxes of reactive VOC generated from heterogeneous and photochemical processes are comparable or larger in magnitude to the sea-to-air flux of DMS. It is not yet clear how the mechanisms proposed in these laboratory experiments translate to atmospheric conditions. The proposed abiotic emissions are also a potential source of VOC in regions of low biological activity, which carries important implications for regional and global modeling.This Account reviews recent laboratory and field experiments of biotic and abiotic ocean VOC emissions, with a specific focus on exploring open questions related to proposed abiotic reactive VOC emissions and the impact of including a large, abiotic VOC emission source on atmospheric oxidants and aerosol particles. To date, abiotic emissions are not typically included in global chemical transport models. The proposed abiotic emissions mechanisms discussed here have the potential to drive significant changes to current understanding of chemistry in the marine atmosphere if present at the magnitudes suggested by laboratory studies. In order to validate their proposed significance, a coordinated set of laboratory, field, and modeling studies under ocean-relevant conditions are necessary.

Atmospheric aerosol properties at a semi-rural location in southern India: particle size distributions and implications for cloud droplet formation

Particle number size distributions in the diameter range of 5 nm–34 µm were measured in tropical southern India during the transition season from May (pre-monsoon) to June–July (monsoon). Averaged over the entire measurement period, the particle number size distributions were bimodal with a total particle number concentration of NTot = (4.5 ± 2.7) × 103 cm−3 (arithmetic mean ± standard deviation). The ratio of Aitken to accumulation mode particle number concentrations (NAit/NAcc) ranged from 1.06 to 2.07, increasing from May to June–July due to a pronounced decrease in the accumulation mode particles with the onset of the monsoon. Cloud condensation nuclei concentrations at 0.4% supersaturation (CCN0.4) were calculated under the assumption of an average continental hygroscopicity parameter of κ = 0.3. The calculated CCN0.4 concentrations are mostly sensitive to variations in NAcc and vary accordingly between the May and June–July. Using a cloud parcel model, we investigated the formation of cloud droplets using the measured average particle number size distributions, updraft velocities up to 20 m s−1, and initial aerosol particle number concentrations up to 25,000 cm−3. We found different regimes of CCN activation and cloud formation for the month of May (shifting from aerosol-limited regime to transitional regime) and for June–July (transitional regime), which was primarily due to the variability of particle number concentrations in the accumulation mode.