Microbiology and atmospheric processes: the role of biological particles in cloud physics

As part of a series of papers on the sources, distribution and potential impact of biological particles in the atmosphere, this paper introduces and summarizes the potential role of biological particles in atmospheric clouds. Biological particles like bacteria or pollen may be active as both cloud condensation nuclei (CCN) and heterogeneous ice nuclei (IN) and thereby can contribute to the initial cloud formation stages and the development of precipitation through giant CCN and IN processes. The paper gives an introduction to aerosol-cloud processes involving CCN and IN in general and provides a short summary of previous laboratory, field and modelling work which investigated the CCN and IN activity of bacterial cells and pollen. Recent measurements of atmospheric ice nuclei with a continuous flow diffusion chamber (CFDC) and of the heterogeneous ice nucleation efficiency of bacterial cells are also briefly discussed. As a main result of this overview paper we conclude that a proper assessment of the impact of biological particles on tropospheric clouds needs new laboratory, field and modelling work on the abundance of biological particles in the atmosphere and their CCN and heterogeneous IN properties

Ice nucleation by surrogates for atmospheric mineral dust and mineral dust/sulfate particles at cirrus temperatures

International audienceThis study examines the potential role of some types of mineral dust and mineral dust with sulfuric acid coatings as heterogeneous ice nuclei at cirrus temperatures. Commercially-available nanoscale powder samples of aluminum oxide, alumina-silicate and iron oxide were used as surrogates for atmospheric mineral dust particles, with and without multilayer coverage of sulfuric acid. A sample of Asian dust aerosol particles was also studied. Measurements of ice nucleation were made using a continuous-flow ice-thermal diffusion chamber (CFDC) operated to expose size-selected aerosol particles to temperatures between ?45 and ?60°C and a range of relative humidity above ice-saturated conditions. Pure metal oxide particles supported heterogeneous ice nucleation at lower relative humidities than those required to homogeneously freeze sulfuric acid solution particles at sizes larger than about 50 nm. The ice nucleation behavior of the same metal oxides coated with sulfuric acid indicate heterogeneous freezing at lower relative humidities than those calculated for homogeneous freezing of the diluted particle coatings. The effect of soluble coatings on the ice activation relative humidity varied with the respective uncoated core particle types, but for all types the heterogeneous freezing rates increased with particle size for the same thermodynamic conditions. For a selected size of 200 nm, the natural mineral dust particles were the most effective ice nuclei tested, supporting heterogeneous ice formation at an ice relative humidity of approximately 135%, irrespective of temperature. Modified homogeneous freezing parameterizations and theoretical formulations are shown to have application to the description of heterogeneous freezing of mineral dust-like particles with soluble coatings

Analysis of Ice Nucleating Aerosol Measurements during SUCCESS: April, May 1996

This section describes our research activities during year three of this effort. In the second year, preliminary archive data sets were submitted to the SUCCESS archive. After additional analyses, final versions were prepared and submitted. These are included on the SUCCESS CD-ROM data editions that were recently released by NASA Ames. Over the range of temperature and supersaturation conditions of our measurements (15 to -40 C, and from ice saturation to approximately 15% water supersaturation), IN concentrations ranged from less than 0.1 to approximately 500 per liter, being generally greater at colder temperatures and higher supersaturations. To estimate the potential of aircraft exhaust as a source of IN, we examined data from six days of the field project when the DC-8 was following closely behind other humidity conditions of our measurements. In April 1997, a microphysical workshop was convened at NCAR to select cases for in depth analyses and to address questions about the consistency of cloud ice crystal measurements (size distributions and mass concentrations) and aerosol size distributions. We attended this meeting and contributed to the discussions. A particular concern was identified in the CN measurements. On the DC-8, CN measurements were obtained by four different investigator groups, using commercially available instrumentation. The DC-8 SUCCESS CN data showed long periods where the measurements were in substantial agreement, but there were also periods with large discrepancies. Several possible factors were identified that could help explain these discrepancies, including minimum detectable particle size, response at reduced pressures, and location of sample inlet on the aircraft

Flight-based chemical characterization of biomass burning aerosols within two prescribed burn smoke plumes

Biomass burning represents a major global source of aerosols impacting direct radiative forcing and cloud properties. Thus, the goal of a number of current studies involves developing a better understanding of how the chemical composition and mixing state of biomass burning aerosols evolve during atmospheric aging processes. During the Ice in Clouds Experiment-Layer Clouds (ICE-L) in the fall of 2007, smoke plumes from two small Wyoming Bureau of Land Management prescribed burns were measured by on-line aerosol instrumentation aboard a C-130 aircraft, providing a detailed chemical characterization of the particles. After ~2–4 min of aging, submicron smoke particles, produced primarily from sagebrush combustion, consisted predominantly of organics by mass, but were comprised primarily of internal mixtures of organic carbon, elemental carbon, potassium chloride, and potassium sulfate. Significantly, the fresh biomass burning particles contained minor mass fractions of nitrate and sulfate, suggesting that hygroscopic material is incorporated very near or at the point of emission. The mass fractions of ammonium, sulfate, and nitrate increased with aging up to ~81–88 min and resulted in acidic particles. Decreasing black carbon mass concentrations occurred due to dilution of the plume. Increases in the fraction of oxygenated organic carbon and the presence of dicarboxylic acids, in particular, were observed with aging. Cloud condensation nuclei measurements suggested all particles >100 nm were active at 0.5% water supersaturation in the smoke plumes, confirming the relatively high hygroscopicity of the freshly emitted particles. For immersion/condensation freezing, ice nuclei measurements at −32 °C suggested activation of ~0.03–0.07% of the particles with diameters greater than 500 nm

Water activity and activation diameters from hygroscopicity data - Part I: Theory and application to inorganic salts

International audienceA method is described that uses particle hygroscopicity measurements, made with a humidified tandem differential mobility analyzer (HTDMA), to determine solution water activity as a function of composition. The use of derived water activity data in computations determining the ability of aerosols to serve as cloud condensation nuclei (CCN) is explored. Results for sodium chloride and ammonium sulfate are shown in Part I. The methodology yields solution water activities and critical dry diameters for ammonium sulfate and sodium chloride in good agreement with previously published data. The approach avoids the assumptions required for application of simplified and modified Köhler equations to predict CCN activity, most importantly, knowledge of the molecular weight and the degree of dissociation of the soluble species. Predictions of the dependence of water activity on the mass fraction of aerosol species are sensitive to the assumed dry density, but predicted critical dry diameters are not

Diagnosing ocean feedbacks to the MJO: SST-modulated surface fluxes and the moist static energy budget

The composite effect of intraseasonal sea surface temperature (SST) variability on the Madden-Julian Oscillation (MJO) is studied in the context of the column integrated moist static energy (MSE) budget using data from the European Centre for Medium-Range Weather Forecasts Interim Reanalysis (ERA-I). SST fluctuations influence the Delta-q and Delta-T parts of the bulk surface latent and sensible heat flux calculations, respectively, each of which influence column MSE. Reynolds decomposition of latent and sensible heat fluxes (LH and SH) reveal that the thermodynamic perturbations modestly offset the equatorial wind-driven perturbations and MSE, but strongly offset the subtropical wind-driven perturbations and MSE. Column moistening east of MJO convection is opposed by wind-driven perturbations and supported by thermodynamic perturbations. Impacts of intraseasonal SST fluctuations are analyzed by recomputing surface flux component terms using 61-day running-mean SST. Differences between "full SST" and "smoothed SST" projections onto MSE and its tendency yield the "SST effect" on the MJO MSE budget. Particularly in the Indian Ocean, intraseasonal SST fluctuations maintain equatorial MSE anomalies at a rate of 1%-2% per day, and damp subtropical MSE anomalies at a similar rate. Vertical advection exports 10%-20% of MSE per day, implying that the SST modulation of surface fluxes offsets roughly 10% of equatorial MSE export and amplifies by 10% the subtropical MSE export by vertical advection. SST fluctuations support MJO propagation by encouraging on-equator convection and the circulation anomalies that drive MJO propagation, and by contributing up to 10% of MSE tendencies across the Warm Pool

Water activity and activation diameters from hygroscopicity data - Part II: Application to organic species

International audienceA method has been developed for using particle hygroscopicity measurements made with a humidified tandem differential mobility analyzer (HTDMA) to determine water activity as a function of solute weight percent. In Part I, the method was tested for particles composed of sodium chloride and ammonium sulfate. Here, we report results for several atmospherically-relevant organic species: glutaric acid, malonic acid, oxalic acid and levoglucosan. Predicted water activities for aqueous dicarboxylic acid solutions are quite similar in some cases to published estimates and the simplified predictions of Köhler theory, while in other cases substantial differences are found, which we attribute primarily to the semivolatile nature of these compounds that makes them difficult to study with the HTDMA. In contrast, estimates of water activity for levoglucosan solutions compare very well with recently-reported measurements and with published data for aqueous glucose and fructose solutions. For all studied species, the critical dry diameters active at supersaturations between 0.2 and 1% that are computed with the HTDMA-derived water activities are generally within the experimental error (~20%) estimated in previously-published direct measurements using cloud condensation nuclei counters. For individual compounds, the variations in reported solution water activity lead to uncertainties in critical dry diameters of 5-25%, not significantly larger than the uncertainty in the direct measurements. To explore the impact of these uncertainties on modeled aerosol-cloud interactions, we incorporate the variations in estimates of solution water activities into the description of hygroscopic growth of aerosol particles in an adiabatic parcel model and examine the impact on the predicted drop number concentrations. For the limited set of initial conditions examined here, we find that the uncertainties in critical dry diameters for individual species lead to 0-21% changes in drop number concentration, with the largest effects at high aerosol number concentrations and slow updraft velocities. Ammonium sulfate, malonic acid and glutaric acid have similar activation behavior, while glutaric acid and levoglucosan are somewhat less hygroscopic and lead to lower drop number concentrations; sodium chloride is the most easily activated compound. We explain these behaviors in terms of a parameter that represents compound hygroscopicity, and conclude that this parameter must vary by more than a factor of 2 to induce more than a 15% change in activated drop number concentrations. In agreement with earlier studies, our results suggest that the number concentration of activated drops is more sensitive to changes in the input aerosol size and number concentrations and the applied updraft velocity than to modest changes in the aerosol composition and hygroscopic properties

Ice Initiation by Aerosol Particles: Measured and Predicted Ice Nuclei Concentrations versus Measured Ice Crystal Concentrations in an Orographic Wave Cloud

The initiation of ice in an isolated orographic wave cloud was compared with expectations based on ice nucleating aerosol concentrations and with predictions from new ice nucleation parameterizations applied in a cloud parcel model. Measurements of ice crystal number concentrations were found to be in good agreement both with measured number concentrations of ice nuclei feeding the clouds and with ice nuclei number concentrations determined from the residual nuclei of cloud particles collected by a counterflow virtual impactor. Using lognormal distributions fitted to measured aerosol size distributions and measured aerosol chemical compositions, ice nuclei and ice crystal concentrations in the wave cloud were reasonably well predicted in a 1D parcel model framework. Two different empirical parameterizations were used in the parcel model: a parameterization based on aerosol chemical type and surface area and a parameterization that links ice nuclei number concentrations to the number concentrations of particles with diameters larger than 0.5 μm. This study shows that aerosol size distribution and composition measurements can be used to constrain ice initiation by primary nucleation in models. The data and model results also suggest the likelihood that the dust particle mode of the aerosol size distribution controls the number concentrations of the heterogeneous ice nuclei, at least for the lower temperatures examined in this case

Size-resolved aerosol composition and its link to hygroscopicity at a forested site in Colorado

Aerosol hygroscopicity describes the ability of a particle to take up water and form a cloud droplet. Modeling studies have shown sensitivity of precipitation-producing cloud systems to the availability of aerosol particles capable of serving as cloud condensation nuclei (CCN), and hygroscopicity is a key parameter controlling the number of available CCN. Continental aerosol is typically assumed to have a representative hygroscopicity parameter, κ, of 0.3; however, in remote locations this value can be lower due to relatively large mass fractions of organic components. To further our understanding of aerosol properties in remote areas, we measured size-resolved aerosol chemical composition and hygroscopicity in a forested, mountainous site in Colorado during the six-week BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H₂O, Organics and Nitrogen–Rocky Mountain Biogenic Aerosol Study) campaign. This campaign followed a year-long measurement period at this site, and results from the intensive campaign shed light on the previously reported seasonal cycle in aerosol hygroscopicity. New particle formation events were observed routinely at this site and nucleation mode composition measurements indicated that the newly formed particles were predominantly organic. These events likely contribute to the dominance of organic species at smaller sizes, where aerosol organic mass fractions were between 70 and 90%. Corresponding aerosol hygroscopicity was observed to be in the range κ = 0.15–0.22, with hygroscopicity increasing with particle size. Aerosol chemical composition measured by an aerosol mass spectrometer and calculated from hygroscopicity measurements agreed very well during the intensive study, with an assumed value of κ_org = 0.13 resulting in the best agreement