Droplet activation, separation, and compositional analysis: laboratory studies and atmospheric measurements [Discussion paper]

Droplets produced in a cloud condensation nucleus chamber as a function of supersaturation have been separated from unactivated aerosol particles using counterflow virtual impaction. Residual material after droplets were evaporated was chemically analyzed with an Aerodyne Aerosol Mass Spectrometer and the Particle Analysis by Laser Mass Spectrometry instrument. Experiments were initially conducted to verify activation conditions for monodisperse ammonium sulfate particles and to determine the resulting droplet size distribution as a function of supersaturation. Based on the observed droplet size, the counterflow virtual impactor cut-size was set to differentiate droplets from unactivated interstitial particles. Validation experiments were then performed to verify that only droplets with sufficient size passed through the counterflow virtual impactor for subsequent analysis. A two-component external mixture of monodisperse particles was also exposed to a supersaturation which would activate one of the types (ammonium sulfate) but not the other (polystyrene latex spheres). The mass spectrum observed after separation indicated only the former, validating separation of droplets from unactivated particles. Results from atmospheric measurements using this technique indicate that aerosol particles often activate predominantly as a function of particle size. Chemical composition is not irrelevant, however, and we observed enhancement of sulfate in droplet residuals using single particle analysis

Droplet activation, separation, and compositional analysis: laboratory studies and atmospheric measurements

Droplets produced in a cloud condensation nuclei chamber (CCNC) as a function of supersaturation have been separated from unactivated aerosol particles using counterflow virtual impaction. Residual material after droplets were evaporated was chemically analyzed with an Aerodyne Aerosol Mass Spectrometer (AMS) and the Particle Analysis by Laser Mass Spectrometry (PALMS) instrument. Experiments were initially conducted to verify activation conditions for monodisperse ammonium sulfate particles and to determine the resulting droplet size distribution as a function of supersaturation. Based on the observed droplet size, the counterflow virtual impactor cut-size was set to differentiate droplets from unactivated interstitial particles. Validation experiments were then performed to verify that only droplets with sufficient size passed through the counterflow virtual impactor for subsequent analysis. A two-component external mixture of monodisperse particles was also exposed to a supersaturation which would activate one of the types (hygroscopic salts) but not the other (polystyrene latex spheres or adipic acid). The mass spectrum observed after separation indicated only the former, validating separation of droplets from unactivated particles. Results from ambient measurements using this technique and AMS analysis were inconclusive, showing little chemical differentiation between ambient aerosol and activated droplet residuals, largely due to low signal levels. When employing as single particle mass spectrometer for compositional analysis, however, we observed enhancement of sulfate in droplet residuals

Wake Capture, Particle Breakup, and Other Artifacts Associated with Counterflow Virtual Impaction

Counterflow virtual impaction is used to inertially separate cloud elements from inactivated aerosol. Previous airborne, ground-based, and laboratory studies using this technique exhibit artifacts that are not fully explained by the impaction theory. We have performed laboratory studies that show small particles can be carried across the inertial barrier of the counterflow by collision and/or coalescence or riding the wake of larger particles with sufficient inertia. We have also performed theoretical calculations to show that aerodynamic forces associated with the requisite acceleration and deceleration of particles within a counterflow virtual impactor can lead to breakup. The implication of these processes on studies using this technique is discussed

Description of the RDCDS Meteorological Component

This report provides a detailed description of the Rapidly Deployable Chemical Defense System (RDCDS) Meteorological Component. The Meteorological Component includes four surface meteorological stations, miniSODAR, laptop computers, and communications equipment. This report describes the equipment that is used, explains the operation of the network, and gives instructions for setting up the Component and replacing defective parts. A detailed description of operation and use of the individual sensors, including the data loggers is not covered in the current document, and the interested reader should refer to the manufacturer’s documentation

Droplet activation, separation, and compositional analysis: laboratory studies and atmospheric measurements

Droplets produced in a cloud condensation nuclei chamber (CCNC) as a function of supersaturation have been separated from unactivated aerosol particles using counterflow virtual impaction. Residual material after droplets were evaporated was chemically analyzed with an Aerodyne Aerosol Mass Spectrometer (AMS) and the Particle Analysis by Laser Mass Spectrometry (PALMS) instrument. Experiments were initially conducted to verify activation conditions for monodisperse ammonium sulfate particles and to determine the resulting droplet size distribution as a function of supersaturation. Based on the observed droplet size, the counterflow virtual impactor cut-size was set to differentiate droplets from unactivated interstitial particles. Validation experiments were then performed to verify that only droplets with sufficient size passed through the counterflow virtual impactor for subsequent analysis. A two-component external mixture of monodisperse particles was also exposed to a supersaturation which would activate one of the types (hygroscopic salts) but not the other (polystyrene latex spheres or adipic acid). The mass spectrum observed after separation indicated only the former, validating separation of droplets from unactivated particles. Results from ambient measurements using this technique and AMS analysis were inconclusive, showing little chemical differentiation between ambient aerosol and activated droplet residuals, largely due to low signal levels. When employing as single particle mass spectrometer for compositional analysis, however, we observed enhancement of sulfate in droplet residuals.Pacific Northwest National Laboratory (U.S.) (Aerosol Climate Initiative)Universitat Frankfurt am Mai

Description of the Columbia Basin Wind Energy Study (CBWES)

The purpose of this Technical Report is to provide background information about the Columbia Basin Wind Energy Study (CBWES). This study, which was supported by the U.S. Department of Energy’s Wind and Water Power Program, was conducted from 16 November 2010 through 21 March 2012 at a field site in northeastern Oregon. The primary goal of the study was to provide profiles of wind speed and wind direction over the depth of the boundary layer in an operating wind farm located in an area of complex terrain. Measurements from propeller and vane anemometers mounted on a 62 m tall tower, Doppler Sodar, and Radar Wind Profiler were combined into a single data product to provide the best estimate of the winds above the site during the first part of CBWES. An additional goal of the study was to provide measurements of Turbulence Kinetic Energy (TKE) near the surface. To address this specific goal, sonic anemometers were mounted at two heights on the 62 m tower on 23 April 2011. Prior to the deployment of the sonic anemometers on the tall tower, a single sonic anemometer was deployed on a short tower 3.1 m tall that was located just to the south of the radar wind profiler. Data from the radar wind profiler, as well as the wind profile data product are available from the Atmospheric Radiation Measurements (ARM) Data Archive (http://www.arm.gov/data/campaigns). Data from the sonic anemometers are available from the authors

Elevated stratified layers observed during VTMX.

A suite of instrumentation including a minisodar, a low-frequency, single-axis sodar, a wind profiling radar and a tethersonde was used during the Vertical Transport and Mixing field study in Salt Lake City, UT, USA, to study the evolution and dynamics of stratified layers that commonly develop during nighttime. The month-long field study provided ten nights with good conditions for tethersonde flights. The real-time sodar display was used to place the tethersonde within and near the stratified layers and to make multiple transects, while atmospheric temperature, moisture, wind speed and wind direction were measured. Not surprisingly, the existence of layers with enhanced acoustic scattering correlated well with regions of potential temperature inversions; however, because wind speeds were invariably low, the Richardson number was rarely less than 0.25. The possible role of moisture in the dynamics of elevated stable layer is discussed

Aerosol Optical Hygroscopicity Measurements during the 2010 CARES Campaign

Measurements of the effect of water uptake on particulate light extinction or scattering made at two locations during the 2010 CARES study around Sacramento, CA are reported. The observed influence of water uptake, characterized through the dimensionless optical hygroscopicity parameter γ, is compared with calculations constrained by observed particle size distributions and size-dependent particle composition. A closure assessment has been carried out that allowed for determination of the average hygroscopic growth factors (GF) at 85% relative humidity and the dimensionless hygroscopicity parameter κ for oxygenated organic aerosol (OA) and for supermicron particles, yielding κ = 0.1–0.15 and 0.9–1.0, respectively. The derived range of oxygenated OA κ values are in line with previous observations. The relatively large values for supermicron particles is consistent with substantial contributions of sea salt-containing particles in this size range. Analysis of time-dependent variations in the supermicron particle hygroscopicity suggest that atmospheric processing, specifically chloride displacement by nitrate and the accumulation of secondary organics on supermicron particles, can lead to substantial depression of the observed GF

Aerosol optical hygroscopicity measurements during the 2010 CARES campaign

Measurements of the effect of water uptake on particulate light extinction or scattering made at two locations during the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES) study around Sacramento, CA are reported. The observed influence of water uptake, characterized through the dimensionless optical hygroscopicity parameter γ, is compared with calculations constrained by observed particle size distributions and size-dependent particle composition. A closure assessment has been carried out that allowed for determination of the average hygroscopic growth factors (GFs) at 85% relative humidity and the dimensionless hygroscopicity parameter κ for oxygenated organic aerosol (OA) and for supermicron particles (defined here as particles with aerodynamic diameters between 1 and 2.5 microns), yielding κ = 0.1–0.15 and 0.9–1.0, respectively. The derived range of oxygenated OA κ values are in line with previous observations. The relatively large values for supermicron particles is consistent with substantial contributions of sea-salt-containing particles in this size range. Analysis of time-dependent variations in the supermicron particle hygroscopicity suggest that atmospheric processing, specifically chloride displacement by nitrate and the accumulation of secondary organics on supermicron particles, can lead to substantial depression of the observed GF