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 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

Airborne Aerosol in Situ Measurements during TCAP: A Closure Study of Total Scattering

We present a framework for calculating the total scattering of both non-absorbing and absorbing aerosol at ambient conditions from aircraft data. Our framework is developed emphasizing the explicit use of chemical composition data for estimating the complex refractive index (RI) of particles, and thus obtaining improved ambient size spectra derived from Optical Particle Counter (OPC) measurements. The feasibility of our framework for improved calculations of total scattering is demonstrated using three types of data collected by the U.S. Department of Energy’s (DOE) aircraft during the Two-Column Aerosol Project (TCAP). Namely, these data types are: (1) size distributions measured by a suite of OPC’s; (2) chemical composition data measured by an Aerosol Mass Spectrometer and a Single Particle Soot Photometer; and (3) the dry total scattering coefficient measured by a integrating nephelometer and scattering enhancement factor measured with a humidification system. We demonstrate that good agreement (~10%) between the observed and calculated scattering can be obtained under ambient conditions (RH < 80%) by applying chemical composition data for the RI-based correction of the OPC-derived size spectra. We also demonstrate that ignoring the RI-based correction or using non-representative RI values can cause a substantial underestimation (~40%) or overestimation (~35%) of the calculated scattering, respectively

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

Airborne flux measurements of ammonia over the southern Great Plains using chemical ionization mass spectrometry

Peer reviewe

Impact of model improvements on 80 m wind speeds during the second Wind Forecast Improvement Project (WFIP2)

During the second Wind Forecast Improvement Project (WFIP2; October 2015&ndash;March 2017, held in the Columbia River Gorge and Basin area of eastern Washington and Oregon states), several improvements to the parameterizations used in the High Resolution Rapid Refresh (HRRR &ndash; 3&thinsp;km horizontal grid spacing) and the High Resolution Rapid Refresh Nest (HRRRNEST &ndash; 750&thinsp;m horizontal grid spacing) numerical weather prediction (NWP) models were tested during four 6-week reforecast periods (one for each season). For these tests the models were run in control (CNT) and experimental (EXP) configurations, with the EXP configuration including all the improved parameterizations. The impacts of the experimental parameterizations on the forecast of 80&thinsp;m wind speeds (wind turbine hub height) from the HRRR and HRRRNEST models are assessed, using observations collected by 19 sodars and three profiling lidars for comparison. Improvements due to the experimental physics (EXP vs. CNT runs) and those due to finer horizontal grid spacing (HRRRNEST vs. HRRR) and the combination of the two are compared, using standard bulk statistics such as mean absolute error (MAE) and mean bias error (bias). On average, the HRRR 80&thinsp;m wind speed MAE is reduced by 3&thinsp;%&ndash;4&thinsp;% due to the experimental physics. The impact of the finer horizontal grid spacing in the CNT runs also shows a positive improvement of 5&thinsp;% on MAE, which is particularly large at nighttime and during the morning transition. Lastly, the combined impact of the experimental physics and finer horizontal grid spacing produces larger improvements in the 80&thinsp;m wind speed MAE, up to 7&thinsp;%&ndash;8&thinsp;%. The improvements are evaluated as a function of the model's initialization time, forecast horizon, time of the day, season of the year, site elevation, and meteorological phenomena. Causes of model weaknesses are identified. Finally, bias correction methods are applied to the 80&thinsp;m wind speed model outputs to measure their impact on the improvements due to the removal of the systematic component of the errors. </div

Pulse Jet Mixing Tests With Noncohesive Solids

This report summarizes results from pulse jet mixing (PJM) tests with noncohesive solids in Newtonian liquid conducted during FY 2007 and 2008 to support the design of mixing systems for the Hanford Waste Treatment and Immobilization Plant (WTP). Tests were conducted at three geometric scales using noncohesive simulants. The test data were used to independently develop mixing models that can be used to predict full-scale WTP vessel performance and to rate current WTP mixing system designs against two specific performance requirements. One requirement is to ensure that all solids have been disturbed during the mixing action, which is important to release gas from the solids. The second requirement is to maintain a suspended solids concentration below 20 weight percent at the pump inlet. The models predict the height to which solids will be lifted by the PJM action, and the minimum velocity needed to ensure all solids have been lifted from the floor. From the cloud height estimate we can calculate the concentration of solids at the pump inlet. The velocity needed to lift the solids is slightly more demanding than "disturbing" the solids, and is used as a surrogate for this metric. We applied the models to assess WTP mixing vessel performance with respect to the two perform¬ance requirements. Each mixing vessel was evaluated against these two criteria for two defined waste conditions. One of the wastes was defined by design limits and one was derived from Hanford waste characterization reports. The assessment predicts that three vessel types will satisfy the design criteria for all conditions evaluated. Seven vessel types will not satisfy the performance criteria used for any of the conditions evaluated. The remaining three vessel types provide varying assessments when the different particle characteristics are evaluated. The assessment predicts that three vessel types will satisfy the design criteria for all conditions evaluated. Seven vessel types will not satisfy the performance criteria used for any of the conditions evaluated. The remaining three vessel types provide varying assessments when the different particle characteristics are evaluated. The HLP-022 vessel was also evaluated using 12 m/s pulse jet velocity with 6-in. nozzles, and this design also did not satisfy the criteria for all of the conditions evaluated