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

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

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 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

Modeling regional aerosol variability over California and its sensitivity to emissions and long-range transport during the 2010 CalNex and CARES campaigns

Abstract. The performance of the Weather Research and Forecasting regional model with chemistry (WRF-Chem) in simulating the spatial and temporal variations in aerosol mass, composition, and size over California is quantified using measurements collected during the California Nexus of Air Quality and Climate Experiment (CalNex) and the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted during May and June of 2010. The extensive meteorological, trace gas, and aerosol measurements collected at surface sites and along aircraft and ship transects during CalNex and CARES were combined with operational monitoring network measurements to create a single dataset that was used to evaluate the one configuration of the model. Simulations were performed that examined the sensitivity of regional variations in aerosol concentrations to anthropogenic emissions and to long-range transport of aerosols into the domain obtained from a global model. The configuration of WRF-Chem used in this study is shown to reproduce the overall synoptic conditions, thermally-driven circulations, and boundary layer structure observed in region that controls the transport and mixing of trace gases and aerosols. However, sub-grid scale variability in the meteorology and emissions as well as uncertainties in the treatment of secondary organic aerosol chemistry likely contribute to errors at a primary surface sampling site located at the edge of the Los Angeles basin. Differences among the sensitivity simulations demonstrate that the aerosol layers over the central valley detected by lidar measurements likely resulted from lofting and recirculation of local anthropogenic emissions along the Sierra Nevada. Reducing the default emissions inventory by 50% led to an overall improvement in many simulated trace gases and black carbon aerosol at most sites and along most aircraft flight paths; however, simulated organic aerosol was closer to observed when there were no adjustments to the primary organic aerosol emissions. The model performance for some aerosol species was not uniform over the region, and we found that sulfate was better simulated over northern California whereas nitrate was better simulated over southern California. While the overall spatial and temporal variability of aerosols and their precursors were simulated reasonably well, we show cases where the local transport of some aerosol plumes were either too slow or too fast, which adversely affects the statistics regarding the differences between observed and simulated quantities. Comparisons with lidar and in-situ measurements indicate that long-range transport of aerosols from the global model was likely too high in the free troposphere even though their concentrations were relatively low. This bias led to an over-prediction in aerosol optical depth by as much as a factor of two that offset the under-predictions of boundary-layer extinction resulting primarily from local emissions. Lowering the boundary conditions of aerosol concentrations by 50% greatly reduced the bias in simulated aerosol optical depth for all regions of California. This study shows that quantifying regional-scale variations in aerosol radiative forcing and determining the relative role of emissions from local and distant sources is challenging during "clean" conditions and that a wide array of measurements are needed to ensure model predictions are correct for the right reasons. In this regard, the combined CalNex and CARES datasets are an ideal testbed that can be used to evaluate aerosol models in great detail and develop improved treatments for aerosol processes

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

Peer reviewe

Spatial and temporal variability of turbulence dissipation rate in complex terrain

To improve parameterizations of the turbulence dissipation rate (ϵ) in numerical weather prediction models, the temporal and spatial variability of ϵ must be assessed. In this study, we explore influences on the variability of ϵ at various scales in the Columbia River Gorge during the WFIP2 field experiment between 2015 and 2017. We calculate ϵ from five sonic anemometers all deployed in a ∼4&thinsp;km2 area as well as from two scanning Doppler lidars and four profiling Doppler lidars, whose locations span a ∼300&thinsp;km wide region. We retrieve ϵ from the sonic anemometers using the second-order structure function method, from the scanning lidars with the azimuth structure function approach, and from the profiling lidars with a novel technique using the variance of the line-of-sight velocity. The turbulence dissipation rate shows large spatial variability, even at the microscale, especially during nighttime stable conditions. Orographic features have a strong impact on the variability of ϵ, with the correlation between ϵ at different stations being highly influenced by terrain. ϵ shows larger values in sites located downwind of complex orographic structures or in wind farm wakes. A clear diurnal cycle in ϵ is found, with daytime convective conditions determining values over an order of magnitude higher than nighttime stable conditions. ϵ also shows a distinct seasonal cycle, with differences greater than an order of magnitude between average ϵ values in summer and winter.</p

Observational data from uncrewed systems over Southern Great Plains

Uncrewed Systems (UxS), including uncrewed aerial systems (UAS) and tethered balloon/kite systems (TBS), are significantly expanding observational capabilities in atmospheric science. Rapid adaptation of these platforms and the advancement of miniaturized instruments have resulted in an expanding number of datasets captured under various environmental conditions by the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility. In 2021, observational data collected using ARM UxS platforms, including seven TigerShark UAS flights and 133 tethered balloon system (TBS) flights, were archived by the ARM Data Center (https://adc.arm.gov/discovery/#/, last access: 11 February 2022) and made publicly available at no cost for all registered users (https://doi.org/10.5439/1846798) (Mei and Dexheimer, 2022). These data streams provide new perspectives on spatial variability of atmospheric and surface parameters, helping to address critical science questions in Earth system science research. This paper describes the DOE UAS/TBS datasets, including information on the acquisition, collection, and quality control processes, and highlights the potential scientific contributions using UAS and TBS platforms.</p

THE GREEN OCEAN AMAZON EXPERIMENT (GOAMAZON2014/5) OBSERVES POLLUTION AFFECTING GASES, AEROSOLS, CLOUDS, AND RAINFALL OVER THE RAIN FOREST

The susceptibility of air quality, weather, terrestrial ecosystems, and climate to human activities was investigated in a tropical environment.Peer reviewe