Search for: All records

According to recent field studies, almost half of the New Particle Formation (NPF) events occur aloft, in a residual layer, near the top of the boundary layer. Therefore, measurements of the meteorological parameters, precursor gas concentrations, and aerosol loadings conducted at the ground level are often not representative of the conditions where the NPFs take place. This paper presents new measurements obtained during the Turbulent Flux Measurements of the Residual Layer Nucleation Particles, conducted at the Southern Great Plains research site. Vertical turbulent fluxes of 3–10 nm‐sized particles were measured using a sonic anemometer and two condensation particle counters with nominal cutoff diameters of3 nm and10 nm mounted at the top of the 10‐m telescoping tower. Aerosol number size distribution (5–300 nm) was determined through the ground‐based Scanning Mobility Particle Sizers. The size selected (15–50 nm) particle hygroscopicity was derived with the Humidified Tandem Differential Mobility Analyzer. The ground level observations were supplemented by vertically‐resolved measurements of horizontal and vertical wind speeds and aerosol backscatter. The data analysis suggests that (a) turbulent flux measurements of 3–10 nm particles can distinguish between near‐surface and residual‐layer small particle events; (b) sub‐50 nm particles had a hygroscopicity value of 0.2, suggesting that organic compounds dominate atmospheric nanoparticle chemical composition at the site; and (c) current methodologies are inadequate for estimating the dry deposition velocity of sub‐10 nm particles because it is not feasible to measure particle concentration very near the surface, in the diffusion sublayer.

 

Abstract. Relationships between critical supersaturation required for activation and particle dry diameter have been the primary means for experimentally characterizing cloud condensation nuclei (CCN) activity; however, use of the dry diameter inherently limits the application to cases where the dry diameter can be used to accurately estimate solute volume. This study challenges the requirement and proposes a new experimental approach, Wet CCN, for studying CCN activity without the need for a drying step. The new approach directly measures the subsaturated portion of the Köhler curves. The experimental setup consists of a humidity-controlled differential mobility analyzer and a CCN counter; wet diameter equilibrated at known relative humidity is used to characterize CCN activity instead of the dry diameter. The experimental approach was validated against ammonium sulfate, glucose, and nonspherical ammonium oxalate monohydrate. Further, the approach was applied to a mixture of nonspherical iodine oxide particles. The Wet CCN approach successfully determined the hygroscopicity of nonspherical particles by collapsing them into spherical, deliquesced droplets. We further show that the Wet CCN approach offers unique insights into the physical and chemical impacts of the aqueous phase on CCN activity; a potential application is to investigate the impact of evaporation/co-condensation of water-soluble semivolatile species on CCN activity.

 

Data from both laboratory studies and atmospheric measurements are used to develop an empirical parameterization for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RH_w) are taken as a measure of the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterization developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A calibration factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RH_w of 105% vs. maximum fractions active at higher RH_w. Instrumental factors that affect activation behavior vs. RH_w in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this calibration factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization, including calibration correction, to predictions of the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first-order approximation in numerical modeling investigations.